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Accepted Manuscript

Utilizations of agricultural waste as adsorbent for the removal of contaminants: A


review

Yingjie Dai, Qiya Sun, Wensi Wang, Lu Lu, Mei Liu, Jingjing Li, Shengshu Yang, Yue
Sun, Kexin Zhang, Jiayi Xu, Wenlei Zheng, Zhaoyue Hu, Yahan Yang, Yuewen Gao,
Yanjun Chen, Xu Zhang, Feng Gao, Ying Zhang
PII: S0045-6535(18)31254-2
DOI: 10.1016/j.chemosphere.2018.06.179
Reference: CHEM 21711

To appear in: ECSN

Received Date: 5 May 2018


Revised Date: 28 June 2018
Accepted Date: 29 June 2018

Please cite this article as: Dai, Y., Sun, Q., Wang, W., Lu, L., Liu, M., Li, J., Yang, S., Sun, Y., Zhang,
K., Xu, J., Zheng, W., Hu, Z., Yang, Y., Gao, Y., Chen, Y., Zhang, X., Gao, F., Zhang, Y., Utilizations of
agricultural waste as adsorbent for the removal of contaminants: A review, Chemosphere (2018), doi:
10.1016/j.chemosphere.2018.06.179.

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ACCEPTED MANUSCRIPT

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1 Utilizations of agricultural waste as adsorbent for the removal of


2 contaminants: A review

4 Yingjie Dai Qiya Sun, Wensi Wang, Lu Lu, Mei Liu, Jingjing Li, Shengshu Yang,

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5 Yue Sun, Kexin Zhang, Jiayi Xu, Wenlei Zheng, Zhaoyue Hu, Yahan Yang, Yuewen Gao,

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6 Yanjun Chen, Xu Zhang, Feng Gao and Ying Zhang*

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8 Laboratory of Environmental Remediation, College of Resources and Environment, Northeast Agricultural

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9 University, No.600 Changjiang Road, Xiangfang District, Harbin 150030, China
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11 Abstract

12 In recent years, various industrial activities have caused serious pollution to the environment. Due to the
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13 low operating costs and high flexibility, adsorption is considered as one of the most effective technologies for
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14 pollutant management. Agricultural waste has loose and porous structures, and contains functional groups

15 such as the carboxyl group and hydroxyl group, so it can be invoked as biological adsorption material.
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16 Agricultural waste gets the advantages of a wide range of sources, low cost, and renewable. It has a good

17 prospect for the comprehensive utilization of resources when used for environmental pollution control. This
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18 article summarized the current research status of agricultural waste in adsorbing pollutants, which pointed out
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19 the influencing factors of adsorption, expounded the adsorption mechanism of biological adsorption and

20 introduced the related parameters of adsorption, proposed the application of adsorbents in engineering

21 including adsorption in liquid and gas phases, at the same time it gave the future development prospect of

22 agricultural waste as adsorbent.

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24 Keywords: Agricultural waste; Contaminant; Removal; Adsorption

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26 *Corresponding author. Tel.: +86 451 5519 0993; Fax: +86 451 5519 0993.

27 E-mail address: zhangyinghr@hotmail.com (Y. Zhang)

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28

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30 Contents

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31 1. Introduction ...................................................................................................................................................... 3

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32 2. Types, structures and resource utilization of agricultural waste ....................................................................... 6
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33 2.1. Types and structures of agricultural wastes ........................................................................................... 6

34 2.2. The resource utilization of agricultural waste........................................................................................ 7


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35 3. Remove inorganic contaminants ...................................................................................................................... 8


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36 3.1. Heavy metal ........................................................................................................................................... 8


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37 3.1.1. Lead ............................................................................................................................................ 8


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38 3.1.2. Cadmium .................................................................................................................................... 9

39 3.1.3. Copper ...................................................................................................................................... 10


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40 3.1.4. Nickel ....................................................................................................................................... 11


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41 3.1.5. Other heavy metal..................................................................................................................... 11

42 3.2. Nitrogen and Phosphorus .................................................................................................................... 12

43 4. Remove organic contaminants........................................................................................................................ 13

44 4.1. Dyes ..................................................................................................................................................... 14


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45 4.1.1. Anionic dyes ............................................................................................................................. 15

46 4.1.2. Cationic dyes ............................................................................................................................ 17

47 4.1.3. Non-ionic dyes.......................................................................................................................... 17

48 4.2. Drugs ................................................................................................................................................... 18

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49 4.2.1. Antibiotics................................................................................................................................. 18

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50 4.2.2. Other Drugs .............................................................................................................................. 19

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51 4.3. Pesticides ............................................................................................................................................. 20

52 4.4. Aromatic compounds ........................................................................................................................... 21

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4.5. Oil substances ...................................................................................................................................... 22
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54 4.6. Adsorption mechanisms for organic pollutant removal ....................................................................... 23
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55 5. Get rid of the gas ............................................................................................................................................ 24


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56 6. Application of adsorbents in engineering ....................................................................................................... 26


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57 6.1. Adsorption in liquid phase ................................................................................................................... 26

58 6.2. Adsorption in the gas phase ................................................................................................................. 27


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59 7. Adsorbent regeneration................................................................................................................................... 27
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60 8. Future perspectives ......................................................................................................................................... 28


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61 9. Conclusions .................................................................................................................................................... 29

62 Acknowledgement .............................................................................................................................................. 30

63 References .......................................................................................................................................................... 30

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65 1. Introduction

66 Agricultural waste is a general term for organic substances discarded by human beings in the process of

67 agricultural production. It mainly includes plant waste, livestock and poultry manure, agricultural and sideline

68 products processing waste, rural household waste (Wang et al., 2016). Agricultural waste, which originates

69 from our life, mainly refers to crop stalks and animal manure (Liu, 2017). It is characterized by a wide range

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70 of sources, large quantity, reproducible, biodegradable and environmental-friendly. Research showed that the

71 total agricultural wastes in 2013 was 1.75×109 tons in China, of which crop straw was 9.93×108 tons,

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72 accounting for 56.82%, livestock and poultry manure was 4.52×108 tons, accounting for 25.85%, forest

73 residues were 3.03×108 tons, accounting for 17.33% (Zuo, 2015). Fig. 1 shows the proportion of agricultural

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74 wastes. In addition, with the rapid development of social economy and the increase of population, total waste

75 production will increase at a rate of 5% to 10% a year and the annual output of waste is estimated to exceed

76 5.00×109 tons in China (Tao, 2013).


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77 With the rapid development of industry and the over-exploitation of natural resources, environmental
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78 pollution has caused serious harm to human health, so it is urgent to solve ecological problems. Conventional

79 methods for removing contaminants from gaseous and aqueous phases are mainly biological treatment,
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80 flocculation (Jawad et al., 2015), membrane separation processes, chemical precipitation, adsorption (utilizing

81 activated carbon) and ion exchange (Rosales et al., 2017). Among these methods, adsorption has been shown
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82 to be an effective and cost-effective method for removing many pollutants (Ashrafi et al., 2015). In adsorbents,

83 activated carbon adsorption is an effective and reliable method. Activated carbon has the benefits of high
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84 surface area, micro-porous structure, uniform pore size distribution, high porosity, high surface reactivity,

85 superior mechanical strength and strong adsorption capacity (Mashhadi et al., 2016). However, the high cost
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86 of this approach has prompted the search for alternative industries (Jawad et al., 2015). Agricultural waste has
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87 a loose, porous structure and contains carboxyl, hydroxyl and other reactive groups, can be used as a biomass

88 adsorption material in the field of pollution control, which can not only reduce the environmental burden but

89 also achieve the effect of "treating waste by waste" (Huang, 2017). The agricultural wastes used for distortion

90 mainly include straw (Salem and Yakoot, 2016), wheat straw (Shang et al., 2015), bagasse (Rattanachueskul et

91 al., 2016), banana skin (Gupta and Gupta, 2015), walnut shell (Tonucci et al., 2015), coconut shell (Tang et al.,

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92 2017), avocado skin (Marahel et al., 2013; Palma et al., 2016), olive powder (Gámiz et al., 2016;

93 López-Cabeza et al., 2017; Peña et al., 2016), mustard (Safa, 2016; Trivedi et al., 2016), linen (Safa, 2016;

94 Sharma et al, 2016), cucumber (Lee et al., 2015; Smitha et al., 2012), waste tea (Zhou et al., 2015), earthworm

95 feces (Wang et al., 2017).

96 At present, a great deal of researches has been made at home and abroad on taking advantage of agricultural

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97 wastes as biomass adsorbents for the treatment of pollutants. Numerous researchers have done a lot of

98 research on the use of agricultural waste to adsorb heavy metals. Salmania et al. (2017) studied the removal of

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99 cadmium ions by magnetized biochar based on orange peel and conventional orange peel (Salmania et al.,

100 2017). Houda and Moussa (2017) studied that using banana waste to remove zinc ions from aqueous solutions.

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101 In addition, many researchers studied to remove extra dense metal (Houda and Moussa, 2017). In organic

102 adsorption, Djelloul and Hamdaoui (2015) researched the kinetic adsorption of methylene blue (MB) by

103
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melon peel in packed columns (Djelloul and Hamdaoui, 2015). Shang et al. (2015) studied the use of
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104 thermally activated pinecone as a low cost adsorbent to remove dimethyl trisulfide from aqueous solutions

105 (Shang et al., 2015). Currently adsorption has been successfully employed to remove inorganic, organic
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106 pollutants and gases in the environment. However, research on gas is comparatively fewer.
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107 In recent years, a great deal of agricultural waste has been generated every year around the world. At

108 present, extensive agricultural waste disposal methods not only fail to effectively convert and utilize
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109 agricultural resources, but also cause serious environmental pollution. A large amount of N2O, SO2, CH4 and

110 smoke are generated during the process of fecal burning and rice straw incineration, which seriously pollutes
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111 the atmosphere (Wei, 2013). In addition to organic matter in livestock and poultry manure, there are mass

112 pathogenic bacteria, parasitic eggs and heavy metal (Zhang and Wu, 2016). They are given directly into the
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113 water without proper treatment, causing serious contamination of groundwater and surface water systems (Wei,
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114 2013). Traditional organic fertilizers have been gradually superseded by chemical fertilizers and other

115 chemical materials, due to the widespread use of pesticides. Fertilizers greatly narrows the quality of the soil

116 and the soil buffer capacity. Therefore, improving the reuse of agricultural wastes could effectively replenish

117 soil nutrients enhances the quality of arable land (Liu, 2017). In the face of agricultural waste and ecological

118 environmental damage caused by agricultural waste, researching on the utilization of agricultural waste has

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119 caused widespread concern. The rationalization of agricultural wastes is of profound significance to

120 effectively alleviate the environmental pollution and improve the ecological environment.

121 In order to comprehend the research progress of agricultural wastes as adsorbents, this paper reviews the

122 literature in recent years. At present, Zhou et al. (2015) reviewed the removal of organic pollutants on

123 agricultural wastes. Nguyen et al. (2013) summarized the removal of heavy metals from water using

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124 agricultural waste. Rosales et al. (2017) reviewed the development of biochar as a low cost adsorbent.

125 However, there was not any comprehensive review on the application (remove organic, inorganic and gas) of

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126 agricultural waste as adsorbent. The main purpose of this paper was to present a summary of the latest

127 information on the use of agricultural waste as an adsorbent in environmental management (see Fig. 2). The

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128 article (i) introduced the mechanism of removing inorganic (heavy metals, N and P), organic matter (dyes,

129 drugs, pesticides, aromatic compounds, and oil substances) and gases respectively; (ii) listed the adsorption

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parameters of typical agricultural wastes under the experimental conditions; (iii) analyzed the factors affecting
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131 the adsorption process; (iv) made a forecast on the future development of agricultural waste.
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132

133 2. Types, structures and resource utilization of agricultural waste


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134 2.1. Types and structures of agricultural wastes


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135 Agricultural wastes are lignocellulosic materials and the main structural components are lignin, cellulose
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136 and hemicellulose (Salleh et al., 2011). Lignin is only an aromatic polymer, which consists of carbonyl,

137 hydroxyl, methyl and other functional groups. Both hemicellulose and cellulose contain oxygen functional
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138 groups including carbonyl groups, hydroxyl groups and ether. These functional groups can bind heavy metal
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139 ions and organic small molecule contaminants by cheating, completing, coordinating, hydrogen bonding and

140 the like, which play an important part in the preparation of adsorbents (Zhou et al., 2015). Chemical

141 composition analysis of conventional agricultural wastes is presented in Fig. 3. When agricultural waste

142 absorbed heavy metal ions, the dynamic functional groups took an important role, in which O element can

143 form coordination bonds with heavy metals (Wen et al., 2017). The focal mechanism, by which agricultural

144 wastes adsorb dyes was generally influenced by several processes (Shah et al., 2016). In general, agricultural

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145 waste directly acts as an adsorbent and researchers are now paying much attention to increase the adsorption

146 capacity of cultivated waste through modification (chemical and physical). Ashrafi et al. (2015) optimized

147 adsorption conditions for basic blue 41 based on the Box-Behnken design response surface methodology

148 using NaOH-modified rice husk. It is shown that the method of NaOH modification can be used to improve

149 the rice husk to raise the adsorption capacity (Ashrafi et al., 2015). Abdelwahab et al. (2016) separated the oil

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150 from water through polymer coated partially esterified sugarcane bagasse (Abdelwahab et al., 2016). In

151 general, modification can improve the adsorption capacity of agricultural wastes.

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152

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153 2.2. The resource utilization of agricultural waste

154 Agricultural waste is highly available and is utilized in a variety of ways. At present, there are mostly five

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aspects of resource utilization of agricultural waste. Fertilizer utilization, making the waste into fertilizer and
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156 soil conditioner by using agricultural waste fertilizer technology, which can lead to the return of organic

157 fertilizer to the soil, increase the organic content of the soil, ensure the organic minerals need for the growth of
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158 the plant, improve the soil structure and reduce the application of chemical fertilizers and pesticides (Deng,

159 2017). Feed utilization, using the crop straws as feed, which will help animal digestion and absorption. It can
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160 largely curb the burning of straw and reduce greenhouse gas emissions. The industrialization and construction
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161 raw materials of agricultural waste mean that is used as a raw material for paper making and the output of

162 polymer panels instead of wood. Energy utilization of agricultural wastes mainly includes anaerobic
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163 fermentation and direct pyrolysis. Converting agricultural waste into electricity is direct combustion pyrolysis.

164 It largely contained open-air straw burning and coal combustion. So it can hold back the occurrence of acid
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165 rain, to a certain extent. Optimization is utilizing the proper treatment of agricultural waste as a substrate
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166 material for mushrooms, vegetables production (Chen and Shi, 2017). In addition, agricultural waste is a

167 natural, environmental and economic adsorbent source. Because of its loose surface, porous, superior

168 mechanical strength and chemical stability, it is appropriate for the restoration of ecological pollution.

169 However, there is poorly researched on agricultural wastes as adsorbents at present, so it is of great

170 significance to consider the application of agricultural wastes as adsorbents.

171
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172 3. Remove inorganic contaminants

173 3.1. Heavy metal

174 The rapid advance of industrialization and rapid urbanization has resulted in the excessive discharge of

175 heavy metal-containing wastewater into the environment, seriously affecting human health (Zhang et al.,

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176 2016). These metallic elements have been defined as mutagenic and carcinogenic agents, and may be toxic to

177 aquatic life (EPA, 2017). Over decades, numerous cadmium remediation techniques, broadly classified into

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178 chemical precipitation, flotation, ion exchange, adsorption and membrane filtration, have been established for

179 cadmium removal (Kurniawan et al., 2006; Pehlivan and Altun, 2006). These methods have significant

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180 disadvantages, including elevated energy requirements, incomplete metal removal, generation of toxic sludge,

181 demanding treatment and expensive equipment (Farhan et al., 2012). In this context, proscription has proved

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182 to be a promising method, with such benefits as: (1) the minimization of chemical sludge; (2) low cost of
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183 promotion and without detrimental effects on the environment (Du et al., 2016). Fig. 4 accurately describes

184 the mechanisms of adsorption of heavy metal ions in agricultural wastes including chemical adsorption,
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185 physical adsorption, ion exchange, membrane diffusion, particle diffusion, chelation, electrostatic attraction,

186 surface complexation, ligand exchange and internal complexation. An increasing number of studies have
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187 shown that agricultural waste can contribute to immobilization of heavy metals (Qian and Chen, 2013; Qian et

188 al., 2016). This section will describe in the adsorption of several archetypal heavy metal ions by agricultural
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189 waste.
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190

191 3.1.1. Lead


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192 Lead is detrimental heavy metal to the body. Lead and its compounds enter the body that will do harm to

193 the nervous, cardiovascular, hematopoietic, kidney, digestive and endocrine and other systems. If the content

194 is overproof, it will cause lead poisoning. With the rapid progress of the industrial market, lead has been

195 widely used in all walks of life. Simultaneously, it causes environmental pollution and health hazards to the

196 human body. At present, lead affects human health mainly through food, drinking water, air and other

197 approaches (http://baike.asianmetal.cn/metal/pb/health.shtml). The maximum allowable concentration of lead

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198 in drinking water is 15.00×10-3 mg/L (EPA, 2017). Amer et al. (2017) has been established that rice husk was

199 an efficient adsorbent for adsorbing Pb (II) in experiments (Amer et al., 2017). The disruption was due to

200 multiple mechanisms: Surface complexation with carboxylic and hydroxyl functional groups, ion exchange

201 with Ca (II), Mg (II), and physical forces of attraction. They found the benefits of rice husk as an adsorbent.

202 Pb (II) can be marked by using an acid and eventually recovered. Rice straw can be regenerated for a certain

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203 number of cycles. So the resources can be stored. El-Deen and El-Deen (2016) did some experiments and

204 found the phosphoric acid activated coconut shell (ACS) adsorbed more Pb (II) than inactivated coconut shell

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205 (CS) (El-Deen and El-Deen, 2016). They operated a series of adsorption experiments to measure the use of the

206 ACS as a dissolution agent for the absorption of lead in wastewater and to compare it with pyrolysis of CS.

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207 The results demonstrate that the biological adsorbent (ACS) is under a high surface area and functional groups.

208 Table 1 shows the adsorption of lead by other agricultural wastes. As can be seen from the figure, there are

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209 many kinds of agricultural wastes that can absorb lead ions, which is a method worthy of being promoted to
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210 handle heavy metal ion pollution.

211
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212 3.1.2. Cadmium


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213 Cadmium (Cd) is seen as an extremely toxic metal without a known biological function (Wang et al., 2010).
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214 Cadmium accumulates in the human body, especially in the kidneys and it can lead to insufficiency of renal

215 function. Being dependent on the World Health Organization and its recommended standard values, the
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216 permissible limit of cadmium in drinking water was 0.005 mg/L. Cadmium is widely used in various kinds of

217 industrial activities (e.g., pigment manufacture, refining of non-ferrous metals), and the subsequent release of
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218 cadmium-containing wastewater into the environment has become a focus of global concern over the past
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219 years, due to its high toxicity, environmental accumulation and non-biodegradable characteristic (Park et al.,

220 2017). Gondhalekar and Shukla (2015) studied the principal mechanism for Cd (II) removal utilizing raw

221 walnut shell was ion exchange (Gondhalekar and Shukla, 2015). Because the ester and acetyl operative groups

222 have been changed to carboxylate, the ability of dissolution increased. Singha and Guleria (2014) used

223 succinylated cellulosic biomass as adsorbent to remove heavy metal ions (Singha and Guleria, 2014). Studies

224 have found that ion exchange is the main mechanism. The possible mechanism is shown in Fig. 5. Two

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225 adjacent carboxyl and hydroxyl groups are attached by a divalent heavy metal ion, and two pairs of electrons

226 can be given to the metal ion to form four coordination number compounds and release the two sodium ions

227 and protons into the solution. Farasati et al. (2015) compared the adsorption ability of Phragmites australis (P.

228 australis) with sugarcane stalks on cadmium ions (Farasati et al., 2015). They discovered the reason why

229 sugarcane stalks adsorbed more Cd (II) than P. australis were the most extended surface area and softer

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230 surface. Chen et al. (2015a) evaluated biochar derived from geophysical dried sewage sludge through

231 pyrolysis at 1173K (Chen et al., 2015a). The results showed a minimal contribution of organic matters on

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232 cadmium removal whereas alkaline earth metals such as calcium was in charge of the adsorption process

233 owing to cation exchange and surface precipitation by the formation of insoluble cadmium salt under alkaline

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234 conditions. In addition, there is ample data in Table 2 indicating that agricultural waste can absorb cadmium as

235 an adsorbent. Consequently, agricultural waste will be a popular cheap adsorption in the future according to its

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236 non-pollution exchange progress and high removal rate. At present, there is less research on cadmium ion
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237 adsorption in agricultural waste, and more research is needed.

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239 3.1.3. Copper


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240 Copper and its alloys (brass and bronze) have been used in ordinary household wiring, photovoltaic cells
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241 and phytotherapy products as fungicides, fertilizers, algicides and insecticides. The EPA has set the acceptable

242 limit of copper in drinking water at 1.30 mg/L. Table 3 shows manifold groups of cultivated waste adsorbed
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243 copper ion data. Removal of Cu (II) from aqueous solution via adsorption has been extensively employed in

244 the wastewater treatment plant (Jin et al., 2016). When a large amount of dense metal remains in the human
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245 body, it is not hard to make the body's organs heavy burden especially the liver and gall bladder. When these
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246 two organs appeared problems, the body's metabolism would be frightened. Guechi et al. (2015) studied the

247 adsorption of copper ions by potato peel (PP) (Guechi et al., 2015). They found that the adsorption kinetics

248 absorption of Cu (II) at different initial metal ions was analyzed by pseudo level, pseudo two levels and

249 particle internal diffusion model. It was pointed out that the maximum adsorption capacity (qm) was 84.74

250 mg/g at 298K. The thermodynamic parameters of Cu (II) adsorption on PP were also calculated. The results

251 showed that PP was a type of adsorbent suitable for removing Cu (II) from aqueous solution. Mokkapati et al.

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252 (2016) also studied difference among three kinds of agricultural waste (banana stem powder, casuarinas fruit

253 powder, sorghum stem powder) (Mokkapati et al., 2016). They did a lot of experiments to study the impact of

254 different factors on the adsorption effect. The qm for the three adsorbents for Cu (II) was 6.50 mg/g, 4.50 mg/g

255 and 7.90 mg/g, respectively. The mechanism of banana stem powder and casuarinas fruit powder is

256 chemisorptions, and the mechanism of sorghum stem powder is the combination of both physisorption and

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257 chemical attachment. So they affirmed the three adsorbents could remove Cu (II) from aqueous environment.

258

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259 3.1.4. Nickel

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260 Nickel is the human body essential life element, and in the human body content is extremely tiny. Under

261 normal circumstances, the human body contains the nickel to 10.00mg and the blood normal concentration is

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0.11 mg/L. Nickel is also the most widespread sensitization of metal. Nickel ions can penetrate through the
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263 pores and sebaceous glands inside the skin, leading to allergic inflammation of the skin. Once into

264 sensitization symptoms, nickel allergy can be indefinitely sustained. More worrying thing is the poisoning
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265 resulted from excessive intake of nickel. The mortal body is daily intake of soluble nickel 250.00mg will

266 cause poisoning. And the peculiar symptoms are dermatitis, respiratory disorders and respiratory tract cancer
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267 (http://baike.asianmetal.cn/metal/ni/health.shtml). Many experiments in Table 4 showed that nickel ions could
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268 be absorbed by a variety of agricultural wastes. Singh and Shukla (2017) proved that the waste citrus limits

269 peel was a cheap and abundantly available biomass, which showed excellent potential for adsorbing Ni (II)
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270 (Singh and Shukla, 2017). Ion exchange mechanism was involved in dissolution which receives the support of

271 FTIR, isotherm and desorption studies. Under the most suitable physical and chemical conditions, qm was
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272 27.78 mg/g. Desorption studies using HCl showed almost complete recovery of Ni (II) ions. Hence, citrus
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273 limits peels owing to its porous structure, high sorption rate, low cost, and comparatively high uptake capacity

274 for Ni (II) ions, is a promising bioscience for commercial applications.

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276 3.1.5. Other heavy metal

277 In addition to the above mentioned abundant heavy metal ions, there are many other heavy metal ions that
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278 can also have an influence on human health, for example, Mercury has chronic toxicity to human. Song et al.

279 (2015) found rice husk and rice straw could absorb Hg (II) by ion exchange (Song et al., 2015). Chromium

280 can cause dermatitis, eczema, bronchitis and rhinitis, causing allergic reactions and carcinogenic effects. Ding

281 et al. (2016) conducted a series of experiments and found that the rice husk had the qm of rice husk for Cr (VI)

282 adsorption was 18.20 mg/g at pH 6.0 and room temperature. Too much zinc can cause poisoning, for example,

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283 excessive intake of zinc can cause acute zinc poisoning, vomiting, diarrhea and other gastrointestinal

284 symptoms, chronic zinc poisoning may have anemia and other symptoms (Ding et al., 2016). Najam and

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285 Andrabi (2016) using experimental data showed that the walnut shell adsorbed Zn (II) through the mechanism

286 of ion exchange (Najam and Andrabi, 2016). Table 5 and Table 6 shows in the adsorption of metal ions by

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287 multiple sets of data. However, there becomes less research on these kinds of heavy metal ions in agricultural

288 wastes, and the research on these metals can be deepened in the future.

289
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290 3.2. Nitrogen and Phosphorus
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291 Agricultural waste cannot be only adsorb heavy metal, but also adsorb nitrogen and phosphorus (NO3-,

292 PO43-, NH4+-N). This section summarizes the data on the adsorption of Nitrogen and phosphorus from
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293 agricultural wastes through the literature search in Table 7. Generally, the surfaces of most carbon-rich and
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294 low-mineral biochars are negatively charged and have little or no ability to delete anions, particularly PO43-

295 (Jung et al., 2015; Yao et al., 2011). For example, Kizito et al. (2015) has studied wood and rice husk
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296 adsorption of ammonium ions in NH4Cl solution and slurry solutions (Kizito et al., 2015). It was noted that

297 the adsorption effect was accomplished in the case of chemisorption and physisorption, and qm reached 133.33
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298 mg/g, 78.06 mg/g, 71.94 mg/g and 59.56 mg/g, respectively. In addition, Zhu et al. (2016) studied the avocado
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299 seed at 298K, pH of 5.0 by an ion exchange mechanism reached the gm of 5.40 mg/g (Zhu et al., 2016). Jung

300 et al. (2015) discovered that biochars derived from soybean stover, bamboo wood, and maize residue showed

301 no sorption capacity for PO43- removal and even released inherent PO43- into the solution (Jung et al., 2015).

302 Nguyen et al. (2015) modified to study the adsorption of zirconium loaded Okara to PO43-, and the

303 experimental results showed that at room temperature, when zirconium loaded okara in acidic environment

304 with pH of 3.0, its qm was 16.43 mg/g (Nguyen et al., 2015). In short, agricultural waste can absorb N and P,

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305 through chemisorption and physisorption, ion exchange mechanism, and the enriched bio-carbon obtained

306 after adsorption can be used as slow-release fertilizer for horticulture and agriculture (Nguyen et al., 2015).

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308 4. Remove organic contaminants

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309 In recent years, with the continuous use of emerging organic products, it has caused pollution problems

310 such as water and soil. At present, the application of agricultural waste as adsorbent in water and soil to

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311 remove all kinds of organic pollutants has been a great effort. Among them, the studies of pollutants are

312 mainly dyes (methylene blue (MB), rhodamine B, crystal violet, malachite green, Congo red) (Chebli et al.,

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313 2015; Feng et al., 2015; Nayak and Pal, 2017; Ren et al., 2016; Smitha et al., 2012; Wang et al., 2017), drugs

314 (tetracycline, caffeine, tylosin) (Chen et al., 2016; Portinho et al., 2017; Yin et al., 2016), pesticides (metalaxyl,

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metribuzin, 2,4-dichlorophenoxyacetic acid) (Gámiz et al., 2016; Peña et al., 2016; Trivedi et al., 2016),
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316 aromatic compounds (polycyclic aromatic hydrocarbons, phenol) (Gupta and Gupta, 2015; Karri et al., 2017)

317 and oil substances (emulsified oil, diesel oil, lubricating oil) (Abdelwahab et al., 2016; Chai et al., 2015;
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318 Pachathu et al., 2016).


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319 A number of treatment techniques have been developed to remove organics, such as flocculation (Guan and

320 Tian, 2017), sedimentation (Wen et al., 2017), light treatment (Deng et al., 2017), membrane processes
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321 (Sarasidis et al., 2017), chemical oxidant oxidation (Gayathri et al., 2017), biological oxidation (Chen et al.,

322 2017), photo-catalytic oxidation/degradation (Janssens et al., 2017), adsorption (Huang et al., 2017) and
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323 combined methods (Sandoval et al., 2017; Zhou et al., 2015). Among them, adsorption is the most concerned

324 because of its high removal rate and simple operation. However, conventional adsorbents such as activated
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325 carbon are cost-effective, and it is not economically viable to achieve their widespread use in the removal of
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326 organic contaminants. Therefore, the bio-adsorbent prepared by theunassuming, easy and low-cost agricultural

327 waste has become the focus of the researchers. At present, various biosorbents prepared from agricultural

328 waste can be effectively used to remove different types of organic pollutants, such as cationic dyes (Amela et

329 al., 2012; Zhu et al., 2016), azo dyes (Tomczak and Tosik, 2017), direct dyes (Karthick et al., 2017), active

330 dyes (Hong and Wang, 2017; Tunç et al., 2009), vulcanization dyes and reduction dyes (Tran et al., 2017).

331 Furthermore, the functional groups of these agricultural wastes such as carbonyl (Bouguettoucha et al., 2016;
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332 Zhu et al., 2016), hydroxyl (Inam et al., 2015; Shang et al., 2015; Zhu et al., 2016), carboxyl (Bouguettoucha

333 et al., 2016; Inam et al., 2015), amine (Inam et al., 2015), amide (Sohrabi and Ameri, 2015), alcohols (Chebli

334 et al., 2015) and phenols (Bouguettoucha et al., 2016; Feng et al., 2015; Gülen et al., 2015) contribute to the

335 adsorption of dyes by various binding mechanisms (Lee et al., 2015). Thus, ion exchange (Charles et al.,

336 2016), complexation/coordination (Ji et al., 2007), adsorption (Sharma et al., 2016), electrostatic interaction

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337 (Safa, 2016), hydrogen bonding (Ahmad et al., 2014) and π-π stacking interaction (Wang et al., 2017)

338 adsorption mechanisms have been proposed. Safa (2016) found that mustard and linseed oil cakes can make

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339 use of electrostatic interaction to remove the acid dyes (Safa, 2016), and Marahel et al. (2013) also found this

340 mechanism when avocado integument removed basic red 2 (BR2) dye (Marahel et al., 2013).

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341 This section summarizes and comments on the application of agricultural wastes in the preparation of

342 adsorbents for adsorption of organic pollutants from five aspects of dyes, drugs, pesticides, aromatic

343 compounds and oily substances.


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344
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345 4.1. Dyes


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346 Growing demand for commercial dyes in various industries has led to the mass production of dyes. More

347 than 1.00×105 types of commercial dyes are available, with annual output exceeding 7.00×105 tons, most of
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348 them are directly discharged into the aqueous medium (Ansari et al., 2016). Water pollution can cause

349 numerous side effects such as mutagenicity, embryo toxicity, teratogenicity and carcinogenicity as well as
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350 damage to the liver, brain and central nervous and reproductive system resulting in abnormal renal function

351 (Tran et al., 2017). Dyes in natural water because of their content in aromatic hydrocarbons, metals, chlorides
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352 can lead to reduced transparency, damage to photosynthesis, damage to animals and plant growth, and affect
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353 the solubility of oxygen and self-cleaning process (Bouguettoucha et al., 2016; Tomczak and Tosik, 2017).

354 And because of its high water solubility, the dyes can be moved into the river affecting the water quality

355 (Dardouri and Sghaier, 2017).

356 In general, dyes are mainly anionic dyes (direct, acid and reactive dyes), cationic dyes (alkaline dyes) and

357 non-ionic dyes (disperse dyes) (Chebli et al., 2015; Zhou et al., 2015). At present, due to the harmfulness of

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358 dyes, many researchers are increasingly concerned about the removal of dyes, they choose to use simple and

359 easy agricultural waste (such as: rice husk, straw, coconut shell, olive powder) as adsorbent to study the

360 removal of different types of dyes.

361

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362 4.1.1. Anionic dyes

363 Anion dyes is dependent on negative ions. They include many compounds from different types of dyes,

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364 structural differences (azo, anthraquinone, triphenyl methane and nitro dyes). For them, however, there is a

365 shared trait: water-soluble ionic substituents. Acidic dyes, direct dyes and reactive dyes are anionic dyes

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366 (Zhou et al., 2015).

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367 AN
368 4.1.1.1. Acid dyes

369 Acid dyes, acidic dyes have azo type, anthraquinone type, travel type, and most belong to azo dyes
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370 (https://baike.so.com/doc/5630201-5842822.html). Such as naphthol blue black (Palma et al., 2016), methyl

371 orange (Hosseinzadeh and Mohammadi, 2016; Mahmoud et al., 2017), acid blue 40 (Oei et al., 2009), amido
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372 black 10B (Ojha and Bulasara, 2015). The adsorption balance experiment was carried out by Safa (2015)
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373 through studying the dissolution of the new biomass oil mustard cake and flaxseed cake with Synolon black

374 HWF-FS and Synolon Red 3HF dye in batches. It found that the qm was 37.04 mg/g and 6.89 mg/g,
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375 respectively, and found its electrostatic interaction mechanism (Safa, 2015). Lee et al. (2017) found that the qm

376 of acid blue 113 dye adsorbed by Cucumis serious skin was 59.80 mg/g under the optimal conditions of pH
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377 6.0 and temperature 323K (Lee et al., 2017). The studies show that agricultural waste is a friendly and
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378 effective alternative to reduce the environmental pollution of acidic dyes. Although there are not a few studies

379 on this aspect, but it need to pay more attention.

380

381 4.1.1.2. Direct dyes

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382 The researchers explored the ability and mechanism of using agricultural waste as an adsorbent to eliminate

383 direct dyes through various experiments. Among them, Chebli et al. (2015) studied the use of a new low-cost

384 disorient Stipa tenassicima fibers that removed Congo red (CR) dye in aqueous solution, studied the

385 influencing factors and at pH 4.0, temperature 298K found that its qm was 7.93 mg/g. Its mechanisms of action

386 were: antiparticle diffusion, strong protonation and electrostatic interactions (Chebli et al., 2015). Shang et al.

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387 (2015) also tested for CR adsorption by using polyethyleneimine-modified straw to improve the adsorption

388 capacity. The results showed that at 303K, its qm was 89.70 mg/g through the Langmuir model. And it found

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389 that its mechanisms of action were mainly ion exchange and hydrogen bonding (Shang et al., 2015). In

390 addition, direct dyes include direct red 23 dyes (DR23). Fathi et al. (2015) evaluated the applicability and

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391 efficiency of corn stover (CS) removal of DR23 using isotherms, kinetics and thermodynamic models and

392 found it was very effective. And it is good to conclude that CS was a friendly adsorbent which removed DR23

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393 and it was easy to get (Fathi et al., 2015). According to different experimental studies, agricultural waste can
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394 be used for direct dyes adsorption effectively (Chebli et al., 2015). However, there is not much research on the

395 adsorbent of agricultural waste as a direct dye, so more research is needed.


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396
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397 4.1.1.3. Reactive dyes


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398 Reactive dyes include reactive black 5 (RB5) (Palma et al., 2016), reactive blue 5G (RB5G) (Módenes et al.,

399 2015), reactive red 141 (Sreelatha et al., 2011), and reactive blue 21 (Sreelatha et al., 2011). Researchers
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400 studied the adsorption performance of different adsorbents on reactive dyes. For example, in the case of RB5

401 adsorption, Palma et al. (2016) explored the production of carbonaceous material in avocado skin by assessing
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402 the carbonization temperature and time effect, and by acid, alkali, reactive dye adsorption contrast, to explore
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403 the feasibility of carbonization materials (Palma et al., 2016). However, Oei et al. (2009) modified the barley

404 straw by nitrogen adsorption, titration and FTIR analysis, through the investigation of influencing factors

405 (adsorbent dosage, initial dye concentration, pH and temperature) to find the most suitable conditions (Oei et

406 al., 2009). Módenes et al. (2015) studied the removal of RB5G by drying biomass of low cost biosorbent

407 prepared from banana pseudostem (BPS). The results showed that the adsorption of RB5G dye was the

408 process of physical adsorption (Módenes et al., 2015). Reactive dyes are mainly used in dyeing and printing of

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409 cotton, hemp, viscose, silk, wool and other fibers and their blended fabrics, so for the removal of the research

410 is very important. Many studies have shown that agricultural waste, as a simple biological adsorbent, can

411 effectively remove reactive dyes, but more research is needed (Palma et al., 2016).

412

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413 4.1.2. Cationic dyes

414 Common cationic dyes include malachite green (MG) (Agarwal et al., 2016; Ren et al., 2016), BR2

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415 (Marahel et al., 2013), basic blue 41 (Palma et al., 2016), crystal violet (Smitha et al., 2012; Wang et al., 2017),

416 rhodamine B (Smitha et al., 2012; Wang et al., 2017), methylene green (Tran et al., 2017; Tran et al., 2017)

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417 and MB (Djelloul and Hamdaoui, 2015; Gülen et al., 2015; Zhu et al., 2016). Among them, MB is a cationic

418 dye that researchers are more concerned about, for example: using the rind as adsorbent to remove MB

419

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(Djelloul and Hamdaoui, 2015), sumac leaves as a low cost and effective biological adsorbent to remove MB
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420 (Gülen et al., 2015), using citric acid to repair the gas tea as MB adsorbent (Zhou et al., 2016). The

421 experiment using different agricultural wastes as adsorbents to adsorb MB concluded that the adsorption
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422 mechanism were mainly electrostatic interaction (Gülen et al., 2015; Nayak and Pal, 2017), particle internal

423 diffusion (Gülen et al., 2015; Nayak and Pal, 2017; Sharma et al., 2016; Zhu et al., 2016; Zhou et al., 2016),
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424 ion exchange (Nayak and Pal, 2017), boundary layer diffusion (Nayak and Pal, 2017; Sharma and Tiwari,
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425 2016; Zhu et al., 2016). In addition, Ren et al. (2016) used agricultural waste garlic as a adsorbent to remove

426 malachite green, through the Langmuir model, and found that at pH 8.0, temperature 298K, adding 2.00×103
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427 mg/L gallon particles, adsorption capacity was the largest 232.56 mg/g. And it was proved that garlic root can

428 be used as adsorbent which is low-cost, and can be used to remove dyes from industrial waste water (Ren et
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429 al., 2016). It is very necessary to reduce the pollution of the environment in the age when the dye is widely
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430 used. According to the recent research, agricultural waste as an environment-friendly adsorbent can effectively

431 adsorb cationic dye. However, there is no reason to stop exploring and further strengthen agricultural waste as

432 adsorbents for the removal of dyes.

433

434 4.1.3. Non-ionic dyes

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435 Non-ionic dyes also refer to disperse dyes. At present, there are few studies on the removal of non-ionic

436 dyes from agricultural wastes as adsorbents. Bamboo stalk as precursor, pretreated activated carbon (AC) by

437 low-temperature chemical activation, and used AC to remove azo disperse red 167 (Zhou et al., 2015). Dyes

438 as a substance that is colored and harmful to human, other animals and plants, deserve greater attention from

439 researchers. More agricultural waste should be used to remove such substances as an adsorbent. The

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440 corresponding adsorption parameters of dyes are shown in the Table 8.

441

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442 4.2. Drugs

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443 Drugs are dangerous environmental contaminants around the world (Kyzas and Deliyanni, 2015). As a

444 newly recognized category of environmental pollutants, drugs have received considerable attention in terms of

445

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their environmental fate and toxicological nature (Kyzas and Deliyanni, 2015; Portinho et al., 2017). Drugs
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446 are made by humans and animals, unchanged or in metabolite form through urine and feces (Portinho et al.,

447 2017). Drugs bring convenience to humans, but they also cause pollution, and improper handling can lead to
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448 water, soil and other pollution. Therefore, the treatment of drugs is particularly important, especially

449 agricultural waste as adsorbent to remove drugs. The studies show that agricultural waste is an
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450 environmentally friendly adsorbent Portinho et al., 2017 .


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451
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452 4.2.1. Antibiotics

453 Antibiotics can control infectious diseases and be used as feed additives to promote healthy growth (Wang
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454 et al., 2017). Since the introduction of penicillin into drug therapy in 1942, hundreds of other antibiotics have
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455 been isolated or synthesized for the treatment of human and animal infections (Qiao et al., 2018).With the

456 increasing use of antibiotics, environmental problems have gradually emerged. Researchers are also paying

457 more attention to the removal of antibiotics, which are the focus of researchers attention by using agricultural

458 waste as adsorbent to adsorb antibiotics. Yin et al. (2016) used iron ore to alter straw biomass (MSF) to

459 improve the ability of adsorbing the tylosin (TYL). The results showed that the main adsorption mechanism

460 was attributed to electrostatic interaction and hydrophobic interaction, in addition, it might be related to
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461 H-bonding and surface complexation. As a result, MSF was considered to be the removal of TYL scavengers

462 and had great potential for removing organic contaminants from aqueous solutions (Yin et al., 2016).

463 In antibiotics, tetracycline (TC) is a concern for researchers. TC is one of the most widely used antibiotics

464 and is often used in animal husbandry (Wang et al., 2017). Therefore, the removal of tetracycline is very

465 necessary. The study was designed to investigate the feasibility of removing TC from rice husk ash (RHA) as

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466 a new adsorbent, and the results showed that RHA was a cheap adsorbent for removing TC and reached the qm

467 8.37 mg/g at 313K (Chen et al., 2016). The experiment was a magnetic carbon composite with layered

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468 structure, which was used to prepare TC adsorption of bagasse by hydrothermal carbonation and simple heat

469 treatment process, the magnetic carbon composites exhibited qm 48.35 mg/g, and the chemical and mechanical

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470 properties were stable and the magnetic properties were good. The adsorption of TC by magnetic adsorbent

471 was mainly attributed to H-bonding and α-β interaction. The results showed that sugarcane bagasse in the

472
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sugar industry could be effectively converted into magnetic adsorbent to remove TC by environmental
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473 friendly methods (Rattanachueskul et al., 2016). The use of agricultural waste to absorb antibiotics will have a

474 great impact on human development. Therefore, researchers should devote more energy to the removal of
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475 antibiotics and other methods to explore. The use of antibiotics is one of the greatest advances in human

476 history, but at the same time it has brought harm to human beings and the environment. And if not
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477 governed,there will be unimaginable crises. At present, there are many experiments on the removal of
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478 antibiotics. Among them, agricultural waste as adsorbent has brought hope to researchers, which will have a

479 great impact on human development. Although there are many studies on the removal of antibiotics,
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480 researchers need to explore more accurate and effective ways to mitigate environmental pollution.

481
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482 4.2.2. Other Drugs

483 In addition to antibiotics, there are anti-inflammatory drugs (diclofenac, ketoprofen, naproxen, nimesulide,

484 ibuprofen, diclofenac sodium) and other medications (Zhou et al., 2015). Portinho et al. (2017) investigated

485 the availability of caffeine from aqueous solution on grape stalk, observed better adsorption ability in acidic

486 solution, assessed balance by adsorption isotherm structure, and found the qm 916.70 mg/g (Portinho et al.,

487 2017). As one of the most dangerous contaminants, drugs need to be solved and removed. Experimental study
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488 using various agricultural wastes to remove drugs showed that agricultural waste is a good adsorbent and has

489 great potential. The corresponding adsorption parameters are shown in the Table 9.

490

491 4.3. Pesticides

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492 Pesticides can kill organisms that cause disease and can prevent, kill weeds, pests, fungi or microorganisms

493 (viruses and bacteria) (Trivedi et al., 2016). At present, the synthetic chemical pesticides are about 500 species.

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494 The widespread use of these pesticides, not only causes serious environmental pollution, but also hazards

495 human health (https://zhidao.baidu.com/question/292778191.html). Pesticides affect humans and the

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496 environment including air, soil and water (Peña et al., 2016). As an effective method of pesticide removal,

497 adsorption is favored by researchers, especially agricultural waste as adsorbent. For example, Gámiz et al.

498

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(2016) investigated how to repair agricultural soil with 2% of compost from olive mill waste or its biochar
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499 (BC), affecting the adsorption, degradation and leaching of two enantiomers of choral fungicide a cream. It

500 concluded that when BC was applied to soil, it can reduce pollution in agriculture and reduce the mobility of
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501 highly polar chiral pesticides (Gámiz et al., 2016). In addition, BC can be used as a fixed correction in soil

502 remediation and groundwater pollution prevention strategies. Peña et al. (2016) also conducted experiments
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503 on the adsorption of pesticides, which evaluated the effects of de-oiled two-phase olive mill waste on the
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504 behavior of metribuzin in the Mediterranean agricultural soil and assessed the effects of these wastes on the

505 conversion of organic matter in situ conditions (Peña et al., 2016).


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506 2,4-dichlorophenoxyacetic acid (2,4-D) is a systematic, selective and popular herbicide and plant growth

507 regulator, and is widely used in broad-leaved plants worldwide. It is highly toxic and may be harmful to
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508 humans and animals (López-Cabeza et al., 2017). It was also reported by the International Agency for Cancer
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509 Research as carcinogenic and mutagenic agents (Trivedi et al., 2016). Therefore, the removal of 2,4-D has

510 become the focus of researchers. The H3PO4 -activated langsat empty fruit bunch was used by Njoku et al.

511 (2015) as a chelating agent for the production of AC to remove 2,4-D. It found the qm 332.00 mg/g and the

512 internal diffusion of particles was the main control mechanism (Njoku et al., 2015). Deokar et al. (2016) used

513 bagasse fly ash (BFA) as adsorbent to remove 2,4-D. The results showed that BFA can be an adsorbent which

514 is low cost and efficient (Deokar et al., 2016).


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515 Pesticides are characterized by high efficiency and high residual or low residue, among which many species

516 have high acute toxicity to mammals. So the hazards of pesticide use are not to be underestimated. Although

517 researchers have done a lot of research on the removal of pesticides, this is far from enough. In recent years,

518 the studies of agricultural waste as an adsorbent to remove pesticides have brought dawn to the researchers,

519 but further research is also needed to achieve more efficient and accurate. The corresponding adsorption

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520 parameters are in the Table 9.

521

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522 4.4. Aromatic compounds

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523 Organic Pollutants in addition to dyes, pesticides, pharmaceuticals and other organic compounds, there is a

524 class of the material-aromatic compounds that the researchers should pay attention to. Many aromatic

525

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compounds contain a benzene ring, which binds to one or more substituent groups (Ouellette and Rawn, 2015).
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526 Among them, polycyclic aromatic hydrocarbon is a kind of matter of concern. It is a toxic pollutant which is

527 produced in the process of fossil fuel combustion, which is a toxic, mutagenic, carcinogenic, almost
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528 biodegradable organic compound (Kronenberg et al., 2017; Lamichhane et al., 2017; Yang et al., 2017).

529 Aromatic compounds are classified by the United States Environmental Protection Agency and the European
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530 commission (Gupta and Gupta, 2015). They can be released in the water system through various sources, such
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531 as industrial waste water, agricultural runoff and polluted air deposition (Gupta and Gupta, 2015). And they

532 pose a great threat to the human body and the environment. Gupta and Gupta (2015) synthesized activated
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533 carbon from waste banana peel, aimed to remove polycyclic aromatic hydrocarbons from the water system,

534 established Langmuir and Freundlich model, and calculated characteristic parameters of adsorption isotherm.
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535 It concluded that the adsorbent prepared from banana peel can be easily used in industrial processing plants to
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536 remove polycyclic aromatic hydrocarbons (Gupta and Gupta, 2015). And the authors found that the removal

537 of sugar or hydrolytic biomass was a promising biological adsorbent for the removal of polycyclic aromatic

538 hydrocarbons (Tran et al., 2015).

539 In addition, aromatic compounds include phenols and their derivatives (phenol, chlorophenol,

540 para-chlorophenol, ortho-Chlorophenol). Phenolic compounds have a water-soluble, highly toxic, adverse

541 impact on aquatic organisms and the environment (Karri et al., 2017). Phenolic compounds are highly mobile
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542 and soluble in water capacity, which can be mixed by natural drinking water downstream, causing serious

543 harm and health hazards to the human body (Karri et al., 2017). Therefore, the treatment of phenolic

544 compounds and their compounds is the key to ensure environmental and human health. At present, many

545 researchers have carried out studies on the removal of phenolic compounds from agricultural wastes as

546 adsorbents, and the main adsorption mechanisms are hydrogen bonding, hydrophobic interaction, π-π

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547 interaction, ion exchange, electronic sharing and exchange, electrostatic interaction, boundary layer diffusion,

548 particle internal diffusion (Feng et al., 2015; Shah et al., 2016; Tonucci et al., 2015; Tran et al., 2015). Feng et

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549 al. (2015) passed from cattails (Asha Orientalis Presl)preparation of activated carbon and evaluated the ability

550 of removing phenol, and the adsorption experiment found that the ionic strength of the effect of phenol

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551 removal was minimal, and concluded that Asha Orientalis Presl has great potential, and was an economic and

552 effective adsorbent (Feng et al., 2015).

553
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Aromatic compounds, which are characterized by stable structure, easy decomposition and strong toxicity,
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554 cause serious pollution to the environment and cause great harm to human body. Therefore, the study of its

555 removal is particularly important. In recent years, researchers have done a lot of research, in which
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556 agricultural waste as adsorbent to remove aromatic compounds is a friendly and effective method.For its

557 removal, there have been great achievements.. But researchers cannot stop there and should continue to
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558 explore ways to be more efficient and green and apply them to industry. The corresponding adsorption
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559 parameters are shown in the Table 9.

560
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561 4.5. Oil substances


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562 Oil pollution poses a serious threat to the environment. When oil floating into water, it can spread hundreds
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563 of miles, form thin layers and prevent oxygen moving from the atmosphere to aquatic organisms (Abdelwahab

564 et al., 2016). The largest source of pollution is oil substances (Zhou et al., 2015). In recent years, more and

565 more research has focused on agricultural waste as an adsorbent to remove oil, such as barley straw, coconut

566 shells, garlic and onion skins (Ibrahim et al., 2010; Zhou et al., 2015). Abdelwahab et al. (2016) modified the

567 bagasse by esterification and coating of polyacrylonitrile and used as a hydrophobic adsorbent to remove

568 diesel from man-made seawater. The adsorption mechanism is chemical adsorption, and it found that the
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569 maximum absorption of oil on all adsorbents can be arranged as follows: paraffin oil > vegetable oil > diesel

570 oil > petrol. The results showed that the prepared adsorbent can be actively involved in solving environmental

571 problems (Abdelwahab et al., 2016). In addition to petroleum products, emulsified oil is also a material

572 affecting the environment. Pachathu et al. (2015) studied the modified bagasse and straw as emulsified oil

573 absorption agent through the microwave-assisted technology. Under 313K, the maximum oil removal ratio of

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574 microwave-assisted bagasse and straw were 98.07% and 98.72%, respectively. It can be seen that the qm of

575 modified bagasse and rice straw were 192.58 mg/g and 276.82 mg/g, respectively (Pachathu et al., 2015). The

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576 research results showed that agricultural waste can be used as an effective adsorbent for oil products. In recent

577 years, the study on the adsorption of oil substances by agricultural waste as adsorbent was not much, so it

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578 should be further studied.

579

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580 4.6. Adsorption mechanisms for organic pollutant removal

581 The adsorption mechanism of organic pollutant removal depends on the nature of the pollutant and the
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582 chemical properties of the agricultural waste surface (Rosales et al. 2017). And it is also accompanied by a

583 variety of factors that affect each other. In the batch mode, the adsorption experiment of the
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584 polyethyleneimine-modified wheat straw (NWS) on CR was carried out by Shang et al. (2015). The
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585 experiment has shown that in NWS there were varieties of floristic fibers and some functional groups

586 including carboxyl, hydroxy and amides, which can be used for adsorption process. H-bonding was the
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587 principal adsorption mechanism of the adsorption process, and it also accompanied with a variety of

588 mechanisms (Shang et al., 2015). Wang et al. (2017) studied the adsorption of tetracycline by activated carbon
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589 prepared by straw at different temperatures and found that the π–π electron-donor acceptor and the high
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590 surface area of the biochar samples derived from rice straw that were pyrolyzed at 973K made its high

591 adsorption capacity (Wang et al., 2017). Scholar studied the magnetic composite materials prepared by

592 bagasse to remove tetracycline, and found that the oxygen-containing functional groups on the surface of the

593 adsorbent played a dominant role in the adsorption of TC. The oxygen-containing groups on the complex

594 adsorbent and the -OH, C=O and -NH2 on the TC molecule form H bonds. In addition, the surface of the

595 composite has a partially aromatic characteristics, indicating that an electron donor-acceptor (EDA)

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596 interaction, or cation-bonding, can form a cationic bond with the conjugate in the TC molecule ring. The

597 specific mechanism of the adsorbent and TC is shown in Fig. 6 (Rattanachueskul et al., 2016). Shah et al.

598 (2016) studied the adsorption of chlorine-chlorophenol on zeolite composites derived from bagasse fly ash.

599 The experimental results shown that the adsorption process were dominated by π-π interaction and affinity

600 formation of donor acceptor complexes on the adsorbent surface (Shah et al., 2016). Electrostatic effect is also

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601 the main mechanism of agricultural waste adsorption organic pollutants. Many researchers had come to the

602 same conclusion by experiments (Fathi et al., 2015; Krishna et al., 2017; Mashhadi et al., 2016). In addition,

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603 Deokar et al. (2016) used bagasse fly ash as an adsorbent to remove 2,4-dichlorophenoxyacetic acid. The

604 result shown that the molecules form of 2,4-D mainly due to Van Der Waals interaction was adsorbed on the

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605 surface of BFA, while the anionic form may be due to electrostatic interaction was adsorbed (Deokar et al.,

606 2016). Fan et al. (2016) used the activated carbon derived from hazelnut shell to remove tetracycline

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607 antibiotics, indicating that electron donor–acceptor, hydrogen bonding, and π-π dispersion interaction between
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608 the aromatic ring of three antibiotics are the main adsorption mechanisms. And the kinetic analysis shown that

609 the adsorption process can ascribe to external transfer and intraparticle diffusion (Fan et al., 2016). On the
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610 other hand, the adsorption mechanism of MB onto adsorbent including physical adsorption and chemical

611 adsorption was studied (Fan et al., 2016). Due to the different chemical composition of various agricultural
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612 wastes, the surface active groups and functional groups are different, which results in different mechanisms of
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613 the adsorption organics by various agricultural wastes (see Fig. 7). In this paper, the qm and mechanisms of

614 agricultural waste under different experimental conditions are listed.


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615

616 5. Get rid of the gas


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617 With the increasingly serious environmental problems, in addition to inorganic and organic pollutants,

618 harmful gases have become the focus of global attention. At present, global warming and climate change are

619 already a major threat to human survival, and human beings are facing melting glaciers, rising sea levels and

620 other problems. The rapid increase of greenhouse gases is one of the reasons. Two main types of greenhouse

621 gases include carbon dioxide (CO2) and nitrous oxide (N2O). In 2017, the concentration of CO2 in the

622 atmosphere was 406 mg/L (Ramphull and Surroop, 2017).

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623 Excessive CO2 stimulates the human respiratory center, causing shortness of breath and headaches,

624 confusion and other symptoms. N2O greenhouse effect was about 300 times serious than CO2 (Yan et al.,

625 2016). Dizziness, loss of direction and balance, memory loss, cognitive impairment, and weakness in the legs

626 are all the side effects of N2O. Severe or prolonged use of N2O can cause vitamin B12 inactivation, leading to

627 functional vitamin B12 deficiency, initial finger numbness, and possibly further development of peripheral

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628 neuropathy and giant cell anemia (Amsterdam and Nabben, 2015). Currently, research on greenhouse gases

629 mainly focuses on the capture and storage of gas. In recent researches, adsorption has the characteristics of

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630 high efficiency and low pollution, so it is a suitable technology for this pollution. Moreover, biochar is a cheap

631 and easily available adsorbent. Nowadays, many agricultural wastes are used for adsorb harmful gases.

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632 Through the activation of CO2, ammonification with ammonia (NH3) and the treatment of soybean straw with

633 CO2 and NH3 at high temperature, Zhang et al. (2016) found that the optimum activation conditions were

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634 obtained and the qm was 49.87 mg/g (Zhang et al., 2016). Erto et al. (2016) pointed out that the removal of
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635 CO2 by pyrolysis and steam-activated agricultural waste mainly relied on the high micropore volume and

636 narrow pore size distribution (Erto et al., 2016). Shahkarami et al. (2015) identified the main differences of the
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637 surface chemistry, porous structure and morphology of activated carbon obtained through rapid and slow

638 pyrolysis of agricultural waste, and obtained the qm 78.10 mg/g (Shahkarami et al., 2015). A research about
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639 the adsorption of 16 volatile organic compounds in the gas phase by activated carbon from waste rice hulls,
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640 and proposed the adsorption mechanism were hydrogen bonding and non-specific interaction (Li et al., 2016).

641 Scholar also made use of rice husk as adsorbent, and developed an effective adsorbent of flue gas removal by
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642 modification (Zhu et al., 2016). These studies show that agricultural waste can play a significant role in the

643 removal of greenhouse gases, and its adsorption mechanism mainly depends on the high micropore volume,
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644 narrow pore size distribution, hydrogen bonding and non-specific interaction. Harmful gases in a certain

645 extent will endanger the survival of mankind. The problem of accumulation for agricultural wastes is also
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646 urgent to be solved. The use of waste as an adsorbent to remove greenhouse gases can solve both problems.

647 However, there are still few researches in this area, which still need to be further explored by researchers.

648

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649 6. Application of adsorbents in engineering

650 6.1. Adsorption in liquid phase

651 The use of agricultural waste as adsorbent for fixed bed adsorbers removes organic substances in water, and

652 is often used in drinking water treatment, groundwater remediation, and swimming pool water treatment

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653 (Shao, 2013). The current adsorber for treating the water phase is designed as a closed pressure filter or an

654 open gravity filter. The material of the filter is usually corrosion-resistant steel or concrete. The adsorbent in a

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655 fixed bed adsorber is located at the bottom of the perforation, and water typically flows down through the

656 adsorbent bed. Between the activated carbon and the bottom there is a small layer of sand used to remove the

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657 toner(see Fig. 8). As the most common adsorbent for water treatment, agricultural waste exists in two forms:

658 powdered and granular. Granular agricultural waste is used in fixed bed adsorbers.

659

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In a wastewater treatment plant, multiple adsorbers in series can make the fixed bed adsorption process a
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660 continuous process, reducing capacity loss. In principle, there are two ways to connect a single fixed bed

661 adsorber to a multiple adsorber system: series and parallel. The total sorbent mass was divided into four
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662 adsorbers, only three adsorbers were running, and the other was stopped to regenerate the adsorbent. The time

663 t1 indicates the time point at which the adsorber 1 is inactive and the mass transfer zone (MTZ) is located
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664 between the adsorbers 3 and 4 . As the MTZ has left the adsorber 2, the adsorbent in the adsorber is fully
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665 saturated to equilibrium. Therefore, the adsorber 2 will be the next stop. The time t2 indicates a later time. So

666 on and so forth. In an ideal situation, all adsorbers can be operated until the entire adsorbent bed reaches the
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667 equilibrium load. The total flow to be treated is divided into a plurality of substreams which are supplied to a

668 plurality of adsorbers operating in parallel. Different adsorbers are put into use at different starting times.
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669 Therefore, at a given time, the travel distance of MTZ in different adsorbers is different, so the breakthrough
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670 time is also different. Different concentrations of different sorbent effluents are mixed to obtain a total effluent

671 stream. The main advantage of parallel connections is that the total cross-sectional area increases with the

672 number of adsorbers. Therefore, this multi-adsorber system is very flexible and can be adjusted according to

673 the different requirements of the amount of water that needs to be treated. It is particularly suitable for

674 handling large amounts of water.

675
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676 6.2. Adsorption in the gas phase

677 The use of bio-carbon derived from agricultural waste such as sugarcane bagasse (Youssef, 1981) as Carbon

678 Molecular Sieve (CMS) to isolate gas is another important application of agricultural waste in industry.

679 Researcher found three fluxes in the hole through the "selective surface Flow" carbon film: flux, Knudsen flux,

680 and diffusion through the surface (Rao and Sircar, 1993a). Surface diffusion can be the main flux of pore

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681 diffusion when the surface concentration is high or when other fluxes are low (Kapoor et al., 1989). Moreover,

682 when the pore size is about twice times that of the strongly adsorbed molecule, the adsorbed molecule

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683 effectively reduces the pore openings, thereby eliminating or hindering the fluxes of other adsorbed or weakly

684 adsorbed molecules, and eventually enhancing the separation. The successful application of the separation

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685 principle depends on the fabrication of a membrane with controllable and uniform aperture, through the poly

686 (two) vinyl chloride controlled pyrolysis experiment supported on the macroporous alumina tube(Golden et al.,

687
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1998). The principle of CMS membrane is shown in Fig. 9 (Golden et al., 1998).
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688 CMS membrane has a relatively unique distribution of molecular size of the membrane hole, good
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689 separation and mechanical properties as well as high stability. Therefore, the CMS membrane can be used in

690 air O2/N2 separation, H2 recovery, CO2 enrichment, low carbon hydrocarbon separation and He recovery, and
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691 has a good application prospects.


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692

693 7. Adsorbent regeneration


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694 The study of adsorbent regeneration can effectively prevent secondary pollution caused by waste adsorbents
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695 (Anirudhan and Sreekumari, 2011). At present, commonly used adsorbent regeneration methods include
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696 solvent extraction, calcination, and biological methods. The solvent extraction method uses an appropriate

697 solvent to extract the adsorbate from the adsorbent. The calcination method is to adsorb the adsorbed

698 adsorbent at a high temperature to convert the adsorbate into a gas or a volatile substance, thereby recovering

699 the adsorbent's adsorption capacity. Emerging bioremediation utilizes microorganisms to desorb the adsorbent

700 and achieve desorption and regeneration of the adsorbent, which is characterized by simple operation, low

701 cost, and low environmental impact (Zhang et al., 2009).

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702 In the experiment, hydrochloric acid, sulfuric acid, and nitric acid are commonly used to desorb the heavy

703 metal ions adsorbed by the biomass adsorbent by placing an adsorbent that has adsorbed heavy metal ions in

704 an acidic solution and competitively adsorbing the heavy metal ions by H+ ions to make the heavy metal ions.

705 Replace it for regeneration. The experiment was carried out by using 0.1 mol/L hydrochloric acid to

706 desorption of algae Oedogonium sp. which adsorbed Cd2+. The adsorption capacity of algae in 4 cycles was

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707 42.8 mg/g, 40.1 mg/g, 38.8 mg/g, 36.5 mg/g and 34.2 mg/g, respectively (Gupta and Rastogi, 2008). Another

708 study was carried out used a 0.1 mol/L hydrochloric acid solution as a desorption agent. The desorption humic

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709 acid adsorbent was activated with 0.1 mol/L NaOH solution, and then the adsorbent was washed with

710 ultrapure water. The next cycle of adsorption experiments was performed with propargite adsorbents.

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711 Repeatedly for 5 cycles, the adsorption of Cd2+ were 20.12 mg/g, 19.35 mg/g, 18.96 mg/g, 18.52 mg/g, and

712 18.13 mg/g, respectively (Chen et al., 2014). It can be seen that the biomass adsorbent can be used repeatedly

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713 and has good practical application value.
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714
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715 8. Future perspectives

716 At present, China is the country with the largest output of agricultural waste all over the world. When its
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717 agricultural waste in the process of not being effective use, to a certain extent, increased the burden of rural
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718 agricultural production, more importantly, also caused the pollution of the rural environment. Therefore,

719 increasing the reuse of agricultural wastes can effectively reduce the air pollution caused by plant incineration.
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720 The soil pollution caused by the residues of heavy metals and pesticides in plants, fixed N/P to replenish soil

721 nutrients and improve soil quality of cultivated land. Meanwhile, it also can prevent the water pollution
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722 caused by livestock manure and the spread of bacteria and viruses caused by the long-term decay of
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723 agricultural wastes, and improve the ecological environment (Liu, 2017).

724 From domestic and international studies, it can be seen that agricultural waste is an ideal choice to deal with

725 pollutants and improve its adsorption effect by modifying their properties. However, researchers often ignore

726 the size of environmental pollution caused by the modification process, the complexity of the modified

727 process and the level of the modified cost. Biochar is an idiographic renewable resource and has great

728 potential to solve several environmental problems in recent years, including remediation of contaminants in
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729 soil, water and gaseous media (Rosales et al., 2017). The utilization of agricultural wastes for bio-carbon is the

730 core international competitive technology of green low-carbon agriculture, which is the current international

731 agricultural soil carbon sequestration, waste environmental management, resource recycling and energy

732 saving and emission reduction, and tackling climate change. This technology is to research and develop

733 various types of carbonization technology of agricultural waste biomass and promote the industrialization of

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734 biochar, which can effectively alleviate a series of realistic ecological and environmental problems, such as

735 the increase of carbon emissions caused by the rapid economic development, the increase of environmental

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736 pollution and the increase of greenhouse gas emissions.

737 This paper argues that the future directions of agricultural waste as adsorbent are:

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738 (1) Research and develop of agricultural waste biomass carbonization technology to promote the

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739 industrialization of biomass carbon.
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740 (2) Development of high efficiency green modifier and modification process will be the development

741 direction of biological adsorption.


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742 (3) Future research should also extend to the use of agricultural waste adsorbents to deal with the
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743 engineering problems of pollution scaling.


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744 In summary, biomass adsorbents based on agricultural waste show significant advantages and can be used

745 to replace expensive commercial activated carbon for environmental pollution control. This provides a broad
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746 application prospect for the utilization of agricultural waste.

747
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748 9. Conclusions
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749 With the development of economy, regional environmental pollution and large-scale ecological destruction

750 have become increasingly serious, threatening the survival and development of all mankind. Wide range of

751 sources, low-cost, renewable biosorbents is becoming more and more popular. Agricultural wastes with loose

752 and porous structure contain carboxyl, hydroxyl and other active groups, which can remove pollutants better.

753 Its adsorption is effected by the pH, temperature, initial concentration and other factors. Modified agricultural
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754 waste can get a better adsorption effect. Its main mechanisms of adsorbing pollutants are ion exchange,

755 electrostatic interaction, complex adsorption and others are still under further exploration. This paper believes

756 that the development of efficient green modifier and technology will be the development direction of

757 biological adsorption. Using agricultural waste as biomass adsorbent can not only reduce the environmental

758 burden but also achieve the goal of "treating waste by waste". In the future environmental governance, it will

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759 have broad space for development.

760

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761 Acknowledgement

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762 This work was supported by Program of Student Innovation Practice Training (SIPT) of Northeast

763 Agricultural University (201810224031;201810224356;201810224357).

764
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765 References
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1187 bioethanol production by rice straw. Energy 135, 32–39.Zhou, R.S., Zhou, R.W., Zhang X.H., Tu, S., Yin

1188 Y.W., Yang, S.Z., Ye, L.Y., 2016. An efficient bio-adsorbent for the removal of dye: Adsorption studies and

1189 cold atmospheric plasma regeneration. J. Taiwan Inst. Chem. Eng. 68, 372-378.

1190 Zhang, T., Li, W. L., Tang, H., Xing, J. M., Liu, H. Z., 2009. Bioregeneration: a novel regeneration method for

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1191 adsorbents. CIESC J. 60(9), 2145-2152.

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1192 Zhang, W.X., Gao, H.L., Jiang, H.T., Wang, Z.W., Wu, Q.T., 2016. Research progress in agricultural wastes

1193 for adsorbing heavy metals. Ind. Water Treat. 36(2), 10-14.

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1194 Zhang, X., Wu, J., Yang, H., Shao, J., Wang, X., Chen, Y.Q., Zhang, S., Chen H., 2016. Preparation of

1195 nitrogen-doped microporous modified biochar by high temperature CO2–NH3 treatment for

1196

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CO2 adsorption: effects of temperature. RSC Adv. 100, 98157-98166.
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1197 Zhou, Y., Zhang, L., Cheng, Z.J., 2015. Removal of organic pollutants from aqueous solution using

1198 agricultural wastes: A review. J. Mol. Liq. 212, 739-762.


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1199 Zhu, C., Duan, Y.F., Wu, C.Y., Zhou, Q., She, M., Yao, T., Zhang, J., 2016. Mercury removal and synergistic
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1200 capture of SO2/NO by ammonium halides modified rice husk char. Fuel 172, 160-169.
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1201 Zhu, L., Wang, Y., He, T.T., You, L.J., Shen, X.Q., 2016. Assessment of potential capability of water bamboo

1202 leaves on the adsorption removal efficiency of cationic dye from aqueous solutions. J. Polym. Environ. 24
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1203 (2), 148-158.


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1204 Zhu, N.Y., Yan, T.M., Qiao, J., Cao, H.L., 2016. Adsorption of arsenic, phosphorus and chromium by bismuth

1205 impregnated biochar: Adsorption mechanism and depleted adsorbent utilization. Chemosphere 164, 32-40.
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1206 Zhu, Y.Y., Kolar, P., Shah, S.B., Cheng, J.J., Lim, P.K., 2016. Avocado seed-derived activated carbon for

1207 mitigation of aqueous ammonium. Ind. Crop. Prod. 92, 34-41.

1208 Zuo, X., 2015. A research on the development and utilization of the agricultural residues as new sources

1209 energy in China. Ph. D. Dissertation, Chinese Academy of Agricultural Sciences.

48
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Grain crop straw
production

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Forest residues, Vegetable melons
17.33% vines and residue

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42.47% production
Oil crop straw yield

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Crop straw,
56.82%
4.74% Cotton stalk yield
Livestock and

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poultry manure,
25.85% 4.53% Others

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3.28%
1.80%

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Fig. 1. The agricultural wastes’ output of China in 2013.


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Fig. 2. Agricultural waste as adsorbent application.

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100

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Chemical composition (%)
Others
75

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Lignin

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Hemicellulos
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Cellulose
25

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CEP
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Fig. 3. Chemical composition of some typical agriculture waste (% dry weight ).

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(Chan et al., 2015; Chen et al., 2016; Chen et al., 2017; Heng et al., 2017; Hesami et al., 2015;

Katsimpouras et al., 2016; Robl et al., 2016; Rohowsky et al., 2013; Wang et al., 2011; Zhang et al., 2017)

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Fig. 4. The adsorption mechanism of inorganic pollutants on agricultural waste.

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Fig. 5. The possible mechanism of heavy metal ion adsorption (Singha and Guleria, 2014)

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Fig. 6. The adsorption mechanism of TC on a magnetic composite derived from sugarcane bagasse

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(Rattanachueskul et al., 2016)

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Fig. 7. The adsorption mechanism of organic pollutants on agricultural waste.


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Fig. 8. Typical fixed-bed adsorbers in water treatment: (a) pressure GAC filter made
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of corrosion-resistant steel and (b) rectangular gravity concrete filter.

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(Worch, 2012)

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Fig. 9. Schematic of exclusive surface diffusion CMS membrane


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(Golden et al., 1998)

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Table 1 Maximum adsorption capacity and mechanism of Pb (II) on different agricultural wastes

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Pollutant Agricultural waste pH Temperature(K) qm (mg/g) Sorption mechanism Reference

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Andes Salsa Inch shell biomass 3.0 323 17.07 Electrostatic attraction Kumar et al., 2016

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6.0 298 18.98 Monolayer chemisorption Guo et al., 2015
Acid-modified rice straw

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and ion exchanges

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Coconut shell 26.14

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5.5 298 Chemisorption El-Deen et al., 2016
Pb (II) Activated coconut shell 49.92
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Rice straw 5.5 298 42.55 Electrostatic attraction and
Amer et al., 2017
physical adsorption
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Plantain peels 6.0 50.51 _ Omidvar-Hosseini and


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Moeinpour., 2016

Plum stone 5.5 298 80.65 _ Parlayıcı et al., 2017


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Hazelnut husk 5.0 298 109.90 _ Imamoglu et al., 2016

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Alkali-treated persimmon fallen 5.0 303 256.00 Electrostatic attraction, ion
Fan et al., 2016
leaves exchange and chelation

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Table 2 Maximum adsorption capacity and mechanism of Cd (II) on different agricultural wastes
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Pollutant Agricultural waste pH Temperature (K) qm (mg/g) Sorption mechanism Reference


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Cd (II) Phragmites australis 6.0 _ 5.41 Film diffusion Farasati et al., 2015
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Sugarcane straw 4.0 _ 8.00

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6.0 313 7.29 Share or exchange electronics Najam et al., 2016
Raw walnut shell
and chemisorption

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Alkali treated walnut shell 6.0 303 14.29 Ion exchange Gondhalekar et al., 2015

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Salix matsudana carbon 5.0 298 40.98
Chemisorption and
Tang et al., 2017

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Typha angustifolia carbon 5.0 298 48.08

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Sesame 6.0 298 84.74 Chemisorption Cheraghi et al., 2015

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Succinate-bonded pullulan 7.0 298 476.20 Ion exchange Abbas et al., 2015

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Table 3 Maximum adsorption capacity and mechanism of Cu (II) on different agricultural wastes

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Sorption
Pollutant Agricultural waste pH Temperature(K) qm (mg/g) Reference
mechanism

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Casuarinas fruit powder 4.55

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Chemisorption and

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Banana stem powder 5.0 303 6.49 Mokkapati et al., 2016
physical adsorption
Sorghum stem powder 7.97
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Cu (II)
Watermelon shells 8.0 298 9.54 _ Mohammed et al., 2016
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Andes Salsa Inch shell 6.0 323 9.70 Electrostatic Kumar et al., 2016
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biomass
attraction
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Walnut shell 5.0 313 14.54 _ Najam et al., 2016

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Raw pomegranate peel 5.8 323 21.37

Ion exchange Ali et al., 2017


Platanus orientalis leaf 6.0 333 49.94

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powder

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Chemically Treated Potato 6.5 298 42.74 _ Moyo et al., 2016

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Plum stone 5.5 298 48.31 _ Parlayıcı et al., 2017

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Potato peel 5.0 298 84.74 Particle diffusion Guechi et al., 2015

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Table 4 Maximum adsorption capacity and mechanism of Ni (II), Zn (II) and Mg (II) on different agricultural wastes
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Pollutants Agricultural waste pH Temperature(K) qm (mg/g) Sorption mechanism Reference

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Litrus limetta Peel
27.07
(Nonlinear)
Singh and Shukla,

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6.0 _ Ion exchange
2017
Litrus limetta Peel
27.78

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(Linear)

Apple pomace 5.0 303 83.33

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Chelation Chand et al., 2014

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Chemically modified 6.0 256.40
apple pomace

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Tabacco stem 5.3 298 97.32 _ Rao et al., 2014
Ni (II)

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Cocoa shell-prepared at 97.59

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ambient temperature
6.0 303 Intra-particle diffusion Kalaivani et al., 2014
Cocoa shell-prepared at 158.80
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Hemp shive 160.00


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Hemp fiber 6.0 293 206.00 Intra-particle diffusion Kyzas et al., 2015

Treated hemp shive 237.00


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Treated hemp fiber 242.00

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5.0 313 7.48 Ion exchange Najam and Andrabi,
Walnut shell
2016
Zn (II)

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Fennel seeds 6.5 293 _ _ Laskar et al., 2016

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Mg (II) Raw date pits 5.0 293 38.50 Ion exchange Rezgui et al., 2016

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Table 5 Maximum adsorption capacity and mechanism of Cr (VI) on different agricultural wastes

Pollutant Agricultural waste pH Temperature (K) qm (mg/g) Sorption mechanism Reference


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Teff straw 2.0 298 3.51 Chemisorption Tadesse et al., 2014
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Cr (VI) Rice husk 6.0 298 18.20 Metal reduction and ion exchange Ding et al., 2016
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Raw Sterculia guttata shell 2.0 333 45.45 Electrostatic attraction Prasanthi et al., 2016
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ZnCl2 activated Sterculia


90.90
guttata shell waste

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Polypyrrole modified natural
3.5 298 84.70 Ion exchange Zhang et al., 2016

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corncob-core sponge

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Table 6 Maximum adsorption capacity and mechanism of Hg (II), As (III) and As (V) on different agricultural wastes

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Pollutants Agricultural waste pH Temperature(K) qm (mg/g) Sorption mechanism Reference

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Peanut shell 6.0 308 6.60 Surface complexation Bai et al., 2015

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Raw date pits 5.0 293 52.63 Ion exchange Rezgui et al., 2017

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Unmodified rice husk 75.19

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Hg (II) Unmodified rice straw 91.74

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6.5 303 Ion exchange Song et al., 2015
Sulfur-fuctionalized rice husk 98.33
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Sulfur-fuctionalized rice straw 125.00
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Rice straw 5.0 313 500.00 _ Mashhadi et al., 2016


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As (III) Bi impregnation-wheat straw 4.0 298 43.15 Ligand exchange


Zhu et al., 2016
As (V) 9.3 318 0.27 Electrostatic attraction
Magnetic gelatin-modified
and innersphere
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chestnut shell complexation

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Table 7 Maximum adsorption capacity and mechanism of NH4+, NO3- and PO43- by different agricultural wastes in varying pH and temperature

Pollutant Agricultural waste pH Temperature(K) qm(mg/g) Sorption mechanism Reference


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Avocado seed-derived 5 298 5.40 Ion exchange Zhu et al., 2016


NH4+
Rice husk (adsorption from slurry 7.8 318 59.56 Chemisorption and Kizito et al., 2015
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solutions) physical adsorption

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Rice husk (adsorption from pure NH4Cl) 303 71.94

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Wood (adsorption from slurry solutions) 318 78.06
9.8

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Wood (adsorption from pure NH4Cl) 303 133.33

SB-AE (Sugarcane bagasse) 73.40

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7 298 Ion exchange Mao et al., 2015

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PSBMIHM-AE 100.2

Amine-grafted corn cob 49.90 _

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6.5 297 Kalaruban et al., 2016
NO3- Amine-grafted coconut copra 59.20 _

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Quaternary Starch 6.5 303 205.00 Ion exchange Chauhan et al., 2016

Corncob TE
5.65 297 0.04 Ion exchange
Micháleková-Richveisová
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PO43-
Activated Rice Husk Ash 6 303 0.74 Physical adsorption Mor et al., 2016
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Zirconium loaded okara 3 298 16.43 _ Nguyen et al., 2015


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Table 8 Maximum adsorption capacity and mechanism of dyes on different agricultural wastes

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Camelina-derived Methylene blue 6.0 323 5.08
Intraparticle diffusion, Surface adsorption Sharma and Tiwari, 2016

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Sapindus-derived Methylene blue 6.0 323 50.76

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Chemisorption, Physisorption, Electrostatic Gülen et al., 2016
Sumac leaves Methylene blue 5.0 298 5.80

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Interactions

Synolon black
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Linseed oil cake 2.0 6.89
HWF-FS
_ Electrostatic Interactions Safa, 2016
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Mustard oil cake Synolon red 3HF 1.0 37.04


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Stipa tenassicima fibers Congo red 4.0 298 7.93 Strong protonation, Electrostatic Interactions Chebli et al., 2015

Earthworm manure Rhodamine B 2.0 600 21.60 Ion exchange, Hydrogen bonding, Electrostatic Wang et al., 2017
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interaction, π-π stacking interaction driven

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Malachite green 27.00
Stem of Solanum tuberosum

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Methylene blue 41.60
7.0 303 Physisorption Gupta et al., 2016
Malachite green 33.30

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Leaves of Solanum tuberosum
Methylene blue 52.60

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Sesame waste Reactive red 141 1.1 293 27.55 Electrostatic Interactions Sohrabi and Ameri, 2015

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Bengal gram fruit shell (BGFS) Acid blue 25 2.0 308 29.41 Electrostatic Interactions, Intraparticle diffusion Krishna et al., 2017

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Coconut coir dust Cationic dye 6.0 303 29.50 Interaction, Electrostatic force Etim et al., 2016

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Crystal violet 33.22

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Cucumis sativus 7.0 300
Rhodamine B 35.33
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Boundary layer diffusion, Intraparticle diffusion Smitha et al., 2012
Crystal violet 40.82
Sulfuric acid-Cucumis sativus 6.3 300
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Rhodamine B 34.01
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Table 8 Continued

Banana pseudostem Reactive blue 5G 1.0 303 37.01 Ion exchange, Physisorption Módenes et al., 2015
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Corn stalks Direct Red 23 3.0 318 51.87 Electrostatic Interactions Fathi et al., 2015

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Water Bamboo Leaves Methylene blue 6.8 283 54.17 Intraparticle diffusion , Electrostatic Interactions Zhu et al., 2016

Walnut Shell Methylene blue 6.0 318 56.13 Chemical reaction Tang et al., 2017

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Cucumis sativus peel Acid Blue 113 6.0 323 59.81 Chemisorption Lee et al., 2015

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Rice straw-Microwave induced
Methylene blue 7.0 298 62.50 H-bonding, Electrostatic attraction Mashhadi et al., 2016

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-H2SO4 activation

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Ion exchange, Chemical reaction, Electrostatic
Avocado integument BR2 dye 7.0 303 102.45 Marahel et al., 2013
Interactions, Protonation of surface groups

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Potato (Solanum tuberosum)

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Methylene blue 6.2 298 105.26 Physisorption, Electrostatic Interactions Guechi et al., 2015
peel

Polyethyleneimine-
Congo red 5.0 TE
313 118.00
H-bonding, Van Der Waals, π-π conjugate, Ion
Shang et al., 2015
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modified wheat straw exchange

Citric acid modified peanut shell Methylene blue 303 120.48 Electrostatic attraction Wang et al., 2015
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Abelmoschus esculentus seed Methylene blue 6.7 600 168.63 Ion exchange, Chemisorption Nayak and Pal, 2017

Chemically modified pine nut Methylene blue 5.9 328 182.08 Dipole-dipole interaction, π-π interaction Naushad et al., 2015
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Ion exchange, Chemical reaction, Electrostatic
Alfa grass Methylene blue 12.0 293 200.00 Toumi et al., 2015
Interactions, External diffusion

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Aminated pumpkin seed Methylorange 3.0 318 200.30 Electrostatic Interactions Subbaiah and Kim, 2016

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Durian Seed - KOH Synthetic Dye 2.0 303 357.14 H-bonding Ahmad et al., 2014

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Complexes adsorption, Ion exchange,
Fe3O4-wheat straw Basic Blue 9 7.0 323 627.10 Pirbazari et al., 2014

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Deprotonation

Table 9 Maximum adsorption capacity and mechanism of other organic pollutants on different agricultural wastes

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Agricultural wastes Organic contaminants pH Temperature(K) qm(mg/g) Sorption mechanism Reference

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2,4-dichlorophenoxyacetic
Bagasse fly ash 3.5 328 7.14 Van Der Waals Deokar et al., 2016
acid
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Electrostatic Interactions, The sharing or
Typha orientalis Presl Phenol 5.0 313 7.23 Feng et al., 2015
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π-π electron donor-acceptor, H-bonding,


Rice straw Tetracycline 5.5 298 14.16 Wang et al., 2017
Hydrophobic, Electrostatic interactions
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Modified sugarcane
Tetracycline 6.8 303 48.35 H-bonding, π-π interaction Rattanachueskul et al., 2016
bagasse

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Rice husk 63.50

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Fluoroquinolone 5.1 309 H-bonding Ashrafi et al., 2015
NaOH-modified rice husk 241.00

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Tetracycline (TC) 312.50
Hazelnut shell derived H-bonding, π-π electron donor-acceptor,

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Oxytetracycline (OTC) 5.0 293 322.60 Fan et al., 2016
activated carbons p–p dispersion interaction

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Chlortetracycline (CTC) 333.30

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HIGHLIGHTS

Summarized the research progress of adsorbing inorganics, organics and gases on

agricultural wastes.

Expounded the mechanism of adsorption inorganics and organics by agricultural wastes.

The application of agricultural waste as adsorbents in engineering was introduced.

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Future prospects of agricultural wastes as adsorbents were discussed.

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