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Article history: The readily available, highly efficient and relatively inexpensive adsorbents of Cerastoderma lamarcki shell
Received 14 April 2015 (CLS) was applied for removal of dye as pollutant using the Taguchi design as an optimization strategy.
Received in revised form The Taguchi design was utilized to find out the influencing optimization conditions. As expected, the C.
24 November 2015
lamarcki waste shell is mainly composed of mineral component, so powdered CLS applied for removal of
Accepted 8 December 2015
dye pollutant. The pH of solution, CLS particle size, adsorbent dose, contact time, temperature and initial
Available online 24 December 2015
dye concentration were studied as the affecting factors on the adsorption process. The experimental
results showed that maximum adsorption occurs in pH about 5. The equilibrium was attained for dyes in
Keywords:
Pollutant
60 min. Adsorption isotherm well fitted to the Freundlich and kinetics of the adsorption reaction followed
Cerastoderma lamarcki shell the pseudo second-order. The maximum adsorption capacity for malachite green was 35.84 mg/g at
Adsorbent 303 K. The morphology of the surface of adsorbent was studied before and after the adsorption by SEM
Malachite green micrograph. It was concluded that CLS powder has a great potential to be applied as an adsorbent for
Taguchi design removal of malachite green.
© 2015 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.ecoleng.2015.12.020
0925-8574/© 2015 Elsevier B.V. All rights reserved.
S.Y. Kazemi et al. / Ecological Engineering 88 (2016) 82–89 83
osmosis-ion exchange apparatus. Malachite green (MG) was pur- The optimization of obtained results was analyzed using MINITAB
chased from Merck (Darmstadt, Germany). The chemical structure, 16 for windows. (Daneshvar et al., 2007; Ross, 1996; Moghaddam
properties and absorption spectrum of Malachite green have been et al., 2006)
presented in Fig. 3. MG is an extensively used biocide in the aqua-
culture industry world-wide and is also as a medical disinfectant 3. Result and discussion
(Chowdhury et al., 2010; Saha et al., 2010). The initial pH of solution
was adjusted by the addition of 0.01 M NaOH and 0.01 M HCl and All experiments were done as: 50 mL of MG solution added to the
measured by pH meter (Metrohm, Switzerland) 1 g of CLS in a100 mL Erlenmeyer flask and UV–vis spectrophotome-
ter was used to study the adsorption performance under different
2.3. Adsorption experiments experimental conditions. All the r results show the percent of the
adsorption of dye in the surface of CLS.
The equilibrium time was determined from kinetic data. A 50 mL Amount of adsorbed dye qe (mg/g) was determination by the
of varying concentration malachite green (10, 15, 25, 50, 100, and following equation:
150 mg/L) solution was added to 1 g of CLS in a Erlenmeyer flask (C0 − Ce ) V
and then mixed at 250 rpm for 60 min. The aqueous samples were qe = (1)
M
centrifuged (Hettich, Tuttlingen, Germany) at 4000 rpm for 1 min to
in which C0 and Ce are initial and equilibrium concentration of
remove the adsorbent. Dye concentration was measured via UV–vis
dye in liquid phase, respectively. V and M are solution volume
spectrophotometer GBC modelCintra-101 (Sydney, Australia) at
and adsorbent (g). Percentage of dye removing is obtained by the
617 nm. The adsorption of MG was studied after adding (0.1–1 g/L)
following equation:
of the adsorbent with size of adsorbent (mesh: 40, 60, 80, 120,
200), pH of solution (4–8), contact time (20, 30, 40, 50, 60 min) (C0 − Ce )
R% = × 100 (2)
and temperature (10–30 ◦ C). C0
C0 and Ce are initial and final dye concentration.
2.4. Optimization method (Taguchi design) Taguchi design was used in order to select the factors that
have influence on removal of dye. The dye removal percentage
Taguchi experimental design, which is developed by Taguchi, was selected as a response and experimental data were considered
is one of the most common ways to optimize adsorption param- as S/N ratio. With envisaging the characteristics, three S/N ratios
eters. In addition, simultaneous study of several parameters and exist; higher is better (HB), normal is best (NB) and lower is better
minimal number of experiments were achieved by this method. (LB) (Elizalde-González and García-Díaz, 2010; Engina et al., 2008;
S.Y. Kazemi et al. / Ecological Engineering 88 (2016) 82–89 85
Table 1 Table 2
parameter settings used in the experiments. Different parameter variables and their levels.
1 pH 4 5 6 7 8 1 1 1 5 3 1
2 Temperature 10 15 20 25 30 2 1 2 1 4 2
3 Adsorbent dosage 0.1 0.3 0.5 0.7 1 3 1 3 2 5 3
4 Time 20 30 40 50 60 4 1 4 3 1 4
5 Mesh 40 60 80 120 200 5 1 5 5 4 3
6 2 1 1 5 4
7 2 2 2 1 5
Wang et al., 2009). Since the high removal rate of dye is desired so 8 2 3 3 2 1
9 2 4 4 3 2
the larger is better was used. Response of this design depends on
10 2 5 5 3 1
the parameters and levels of experimental. Initially, we selected five 11 3 1 1 4 2
factors while they were potentially affecting the removal. Effective 12 3 2 2 5 3
parameters and considered parameters for every Taguchi design 13 3 3 3 1 4
are recorded in Table 1. Considering the mentioned factors and their 14 3 4 5 4 3
15 3 5 1 5 4
levels, 25 experiments have been designed (Table 2). 16 4 1 2 1 5
Obtained results were introduced to the software and the output 17 4 2 3 2 1
was evaluated an all Taguchi diagrams, longitudinal axis is related 18 4 3 4 3 2
to the investigating factors and transverse axis is related to S/N 19 4 4 5 3 1
20 4 5 1 4 2
proportion.
21 5 1 2 5 3
22 5 2 3 1 4
3.1. Effect of pH 23 5 3 5 4 3
24 5 4 1 5 4
25 5 5 2 1 5
As expected, pH is one of the most important parameters that
can affect adsorption process. The removal efficiency of dye was
examined in the pH range of 4.0 to 8.0 (Fig. 4a). Due to the malachite
green instability in pH of higher than 8, the effect of pH solution adsorptive process through dissociation of functional groups on
beyond 8 was not investigated. The results strongly verified that the active sites of the adsorbent. pH is, also, known to affect the
removal of dye from solution is influenced by pH, so the optimum structural stability of MG, and therefore, its color intensity.
pH is 5. This is likely because of adsorption process is affected by the
surface charge of adsorbent, the degree of ionization and speciation 3.2. Effect of temperature
of the adsorbent. The hydrogen ion and hydroxyl ions are adsorbed
quite strongly, and therefore, the adsorption of other ions is affected The influence of temperature on dye adsorption by CLS was
by the pH of the solution. And also the change of pH affects the studied (Fig. 4b). As seen, the percentage of dye adsorption
Fig. 4. (a) The effect of temperature on the removal of Malachite green by Cerastoderma lamarcki shell, initial Malachite green concentration = 20 mg/L, adsorbent dose = 1 g/L.
(b) The effect of adsorbent dose on the removal of Malachite green by Cerastoderma lamarcki shell, initial Malachite green concentration = 20 mg/L, adsorbent dose = 1 g/L. (c)
The effect of time on the removal of Malachite green by Cerastoderma lamarcki shell, initial Malachite green concentration = 20 mg/L, adsorbent dose = 1 g/L. (d) The effect of
particle size on the removal of Malachite green by Cerastoderma lamarcki shell, initial Malachite green concentration = 20 mg/L, adsorbent dose = 1 g/L. (e) The effect of pH on
the removal of Malachite green by Cerastoderma lamarcki shell, initial Malachite green concentration = 20 mg/L, adsorbent dose = 1 g/L.
86 S.Y. Kazemi et al. / Ecological Engineering 88 (2016) 82–89
Concentraon(mg/L)
considered as the optimum temperature.
50ppm
100
3.3. Effect of adsorbent dose
100ppm
80
The effect of adsorbent dose in solution on the malachite green
150ppm
adsorption was investigated and the results are shown in Fig. 4c. As
60
seen, the percentage of MG removal increases with an increase in
adsorbent amount in solution. It means that increasing adsorbent
40
mass provides the more available pores and surface for adsorption.
Maximum removal occurs when amount of CLS is 1 g.
20
Table 3
Isotherm constants for Malachite green onto Cerastoderma lamarcki shell.
1
ln qe = ln KF + ln Ce (4)
nF
Table 4
The calculated kinetic parameters for pseudo first-order and pseudo second-order models for the adsorptions of Malachite green onto Cerastoderma lamarcki shell.
Table 5 Chowdhury, S., Saha, P., 2010. Sea shell powder as a new adsorbent to remove Basic
Comparison of MG adsorption capacity of Cerastoderma lamarcki shell with other Green 4 (Malachite Green) from aqueous solutions: equilibrium, kinetic and
reported low-cost adsorbents. thermodynamic studies. J. Chem. Eng. 164, 168–177.
Daneshvar, N., Khataee, A.R., Rasoulifard, M.H., Pourhassan, M., 2007. Biodegradation
Sorbent qmax(mgg−1 ) Reference of dye solution containing malachite green: optimization of effective parameters
using Taguchi method. J. Hazard. Mater. 143, 214–219.
Bentonite 7.72 Tahir and Rauf (2006)
Elizalde-González, M.P., García-Díaz, L.E., 2010. Application of a Taguchi L16 ortho-
Sugarcane dust 4.88 Khattri and Singh (1999) gonal array for optimizing the removal of Acid Orange 8 using carbon with a low
Cellulose 2.422 Sekhar et al. (2009) specific surface area. J. Chem. Eng. 163, 55–61.
Treated sawdust 65.8 Garg et al. (2003) Engina, A.B., Ozdemirb, O., Turanb, M., Turanc, A.Z., 2008. Color removal from textile
Sea shell powder 42.3 Chowdhury and Saha (2010) dye bath effluents in a zeolite fixed bed reactor: determination of optimum
Hen feathers 26.1 Mittal (2006) process conditions using Taguchi method. J. Hazard. Mater. 159, 348–353.
Zeolite 19.70 Wang and Ariyanto (2007) Eren, Z., Acar, F.N., 2006. Adsorption of Reactive Black 5 from an aqueous solution:
Arundo donax root 8.69 Zhang and Li (2008) equilibrium and kinetic studies. Desalination 194, 1–10.
carbon (ADRC) Eren, Z., Acar, F.N., 2007. Equilibrium and kinetic mechanism for Reactive Black 5
Marine alga 66.6 Kannan et al. (2010) sorption onto high lime Soma fly ash. J. Hazard. Mater. 143, 226.
Iron humate 19.2 Janos (2003) Garg, V.K., Gupta, R., Yadav, A.B., Kumar, R., 2003. Dye removal from aqueous solution
Cerastoderma lamarcki 35.84 Present study by adsorption on treated sawdust. Bioresour. Technol. 89, 121–124.
Haddad, M.E., Regti, A., Laamari, R., Slimani, R., Mamouni, R., EAntri, S., Lazar, S.,
shell
2014. Calcined mussel shells as a new and eco-friendly biosorbent to remove
textile dyes from aqueous solutions. J. Taiwan. Inst. Chem. Eng. 45, 533–540.
Ho, Y.S., McKay, G., 1999a. Pseudo-second order model for sorption processes. Pro-
3.8. Comparison of Cerastoderma lamarcki shell with other cess Biochem. 34, 451–465.
sorbents Ho, Y.S., McKay, G., 1999b. The sorption of lead (II) ions on peat. Water Res. 33,
578–584.
Ho, Y.S., 2004. Citation review of Lagergren kinetic rate equation on adsorption
Table 5 shows summarize the comparison data for the removal reactions. Scientometrics 59, 171–177.
capacity of MG by several adsorbents including CLS. This com- Hsu, T.C., 2009. Experimental assessment of adsorption of Cu2+ and Ni2+ from aque-
ous solution by oyster shell powder. J. Hazard. Mater. 171, 995–1000.
parison of sorption capacity of CLS used in this study with those Janos, P., 2003. Sorption of basic dyes onto iron humate. Environ. Sci. Technol. 37,
obtained in the literature shows that this shell is an effective adsor- 5792–5798.
bent for the removal of MG from aqueous solutions. Jung, J.H., Shon, B.H., Yoo, K.S., Oh, K.J., 2000. Physicochemical characteristics of waste
sea shells for acid gas cleaning absorbent. Korean J. Chem. Eng. 17, 585–592.
Kannan, R.R., Rajasimman, M., Rajamohan, N., Sivaprakash, B., 2010. Brown marine
4. Conclusions algae turbinaria conoides as biosorbent for Malachite green removal: equilib-
rium and kinetic modeling. Front. Environ. Sci. Engin. 4, 116–122.
Karatas, M., Argun, Y.A., Argun, M.E., 2012. Decolorization of antraquinonic dye.
The purpose of the present study was to evaluate the removal Reactive Blue 114 from synthetic wastewater by Fenton process: kinetics and
efficiency of dye from aqueous solutions by Taguchi design. thermodynamics. J. Ind. Eng. Chem. 18, 1058–1062.
The operational parameters such as pH, particle size, adsorbent Kazemi, S.Y., Hamidi, A.S., Asanjarani, N., Zolgharnein, J., 2010. Optimization of a
new polymeric chromium(III) membrane electrode based on methyl violet by
dose, contact time, temperature and initial dye concentration were using experimental design. Talanta 81, 1681–1687.
found to have effects on the adsorption efficiency. Kazemi, S.Y., Hamidi, A.S., Asanjarani, N., Zolgharnein, J., Lakouraj, M.M., 2014.
Experimental as an designs optimization approach for fabrication a new
selective sensor for thallium based on calix[6]arene. Russ. Anal. Chem. 69,
(1) The CLS used in this study was mainly composed of calcium 715–724.
carbonate. This is easy to access, non-toxic and used in an ani- Khattri, S.D., Singh, M.K., 1999. Colour removal from dye wastewater using sugar
mal husbandry industry. It is an inexpensive adsorbent found cane dust as an adsorbent. Adsorpt. Sci. Technol. 17, 269–282.
Kim, Y.S., Choi, Y.M., Noh, D.O., Cho, S.Y., Suh, H.J., 2007. The effect of oyster shell
worldwide in the oceans and seas. powder on the extension of the shelf life of tofu. Food Chem. 103, 155–160.
(2) The kinetics of MG adsorption on CLS follows the pseudo Lagergren, S., 1898. About the theory of so-called adsorption of soluble substances.
second order model. The correlation coefficient for the K. Sven. Vet. Akad. Handl. 24, 1–39.
Lee, D.Y., Jing, S.R., Lin, Y.F., 2001. Using seafood waste as sludge conditioners. Water
Freundlich model was significantly better than the Langmuir Sci. Technol. 44, 301–307.
isotherm. Maximum adsorption capacity for malachite green Lima, E.C., Royer, B., Vaghetti, J.C.P., Simon, N.M., Cunha, B.M., Pavan, F.A., Benvenutti,
was 35.84 mg/g on CLS. E.V., CatalunaVeses, R., Airoldi, C., 2008. Application of Brazilian pine-fruit shell
as a biosorbent to removal of reactive red 194 textile dye from aqueous solution
(3) The adsorption was highly dependent on particle size, adsor-
Kinetics and equilibrium study. J. Hazard. Mater. 155, 536–550.
bent dose, reaction temperature and pH. Lima, R.O.A.D., Bazo, A.P., Salvadori, D.M.F., Rech, C.M., Oliveira, D.P., Umbuzeiro,
(4) Thus, this present study showed that CLS could be used as an G.A., 2007. Mutagenic and carcinogenic potential of a textile azo dye processing
plant effluent that impacts a drinking water source. Mutat. Res.: Genet. Toxicol.
adequate adsorbent for dye effluent treatment.
Environ. Mutagen. 626, 53–60.
Liu, Y.X., Yang, T.O., Yuan, D.X., Wu, X.Y., 2010. Study of municipal wastewater treat-
Acknowledgment ment with oyster shell as biological aerated filter medium. Desalination 254,
149–153.
Mittal, A., 2006. Adsorption kinetics of removal of a toxic dye, malachite green, from
The partial support of this work by Sari Agricultural Sciences wastewater by using hen feathers. J. Hazard. Mater. 133, 196–202.
and Natural Resources University is acknowledged. Moghaddam, J., Sarraf-Mamoory, R., Abdollahy, M., Yamini, Y., 2006. Purification of
zinc ammoniacal leaching solution by cementation: determination of optimum
process conditions with experimental design by Taguchi’s method. Sep. Purif.
References Technol. 51, 157–164.
Namasivayam, C., Sakoda1, A., Suzuki, M., 2005. Removal of phosphate by adsorp-
Birshtain, Y.A., Vinogradova, L.G., Kondakov, N.N., Koon, M.S., Astakhova, T.V., tion onto oyster shell powder—kinetic studies. J. Chem. Technol. Biotechnol. 80,
Romanova, N.N., 1968. Invertebrate Atlas Caspian Sea. Industry Food, Moscow, 356–358.
Russia. Nigam, P., Armour, G., Banat, I.M., Singh, D., Marchant, R., 2000. Physical removal of
Blais, J.F., Shen, S., Meunier, N., Tyagi, R.D., 2003. Comparison of natural adsorbents textile dyes from eluents and solid-state fermentation of dye-adsorbed agricul-
for metal removal from acidic effluent. Environ. Technol. 24, 205–215. tural residues. Bioresour. Technol. 72, 219–226.
Brookstein, D.S., 2009. Factors associated with textile pattern dermatitis caused by Pan, S.C., Lin, C.C., Tseng, D.H., 2003. Reusing sewage sludge ash as adsorbent for
contact allergy to dyes, finishes, foams, and preservatives. Dermatol. Clin. 27, copper removal from wastewater. Resour. Conserv. Recycl. 39, 79–90.
309–322. Raghu, S., Basha, C.A., 2007. Chemical or electrochemical techniques, followed by ion
Carneiro, P.A., Umbuzeiro, G.A., Oliveira, D.P., Zanoni, M.V.B., 2010. Assessment of exchange, for recycle of textile dye wastewater. J. Hazard. Mater. 149, 324–330.
water contamination caused by a mutagenic textile effluent/dyehouse effluent Ross, P., 1996. Taguchi Techniques for Quality Engineering. McGraw-Hill Interna-
bearing disperses dyes. J. Hazard. Mater. 174, 694–699. tional Editions, Singapore.
Chowdhury, S., Mishra, R., Saha, P., Kushwaha, P., 2010. Adsorption thermodynamics, Royer, B., Cardoso, N.F., Lima, E.C., Macedo, T.R., Airoldi, C., 2010. A useful organofunc-
kinetics and isosteric heat of adsorption of Malachite Green onto chemically tionalized layered silicate for textile dye removal. J. Hazard. Mater. 181,
modified rice husk. Desalination 265, 159–168. 366–374.
S.Y. Kazemi et al. / Ecological Engineering 88 (2016) 82–89 89
Royer, B., Cardoso, N.F., Lima, E.C., Vaghetti, J.C.P., Simon, N.M., Calvete, Wu, D., Zhang, B., Li, C., Zhang, Z., Kong, H., 2006. Simultaneous removal of ammo-
T., Veses, R.C., 2009. Applications of Brazilian-pine fruit shell in natural nium and phosphate by zeolite synthesized from fly ash as influenced by salt
and carbonized forms as adsorbents to removal of methylene blue from treatment. J. Colloid Interface Sci. 304, 300–306.
aqueous solutions—kinetic and equilibrium study. J. Hazard. Mater. 164, Wu, J., Eiteman, M., Law, S., 1998. Evaluation of membrane filtration and ozona-
1213–1222. tion processes for treatment of reactive-dye wastewater. J. Environ. Eng. 124,
Saha, P., Chowdhury, S., Gupta, S., Kumar, I., Kumar, R., 2010. Assessment on the 272–277.
removal of Malachite Green using tamarind fruit shell as biosorbent. CLEAN: Yoon, H., Park, S., Lee, K., Park, J., 2004. Oyster shell as substitute for aggregate in
Soil Air Water 38, 437–445. mortar. Waste Manage. Res. 22, 158–170.
Sekhar, C.P., Kalidhasan, S., Rajesh, V., Rajesh, N., 2009. Bio-polymer adsorbent Zhang, J., Li, Y., 2008. Adsorption of malachite green from aqueous solution onto
for the removal of malachite green from aqueous solution. Chemosphere 77, carbon prepared from Arundo donax root. J. Hazard. Mater. 150, 774–778.
842–847. Zhu, M.X., Lee, L., Wang, H.H., Wang, Z., 2007. Removal of an anionic dye by adsorp-
Siboni, M.S., Khataee, A., Joo, S.W., 2014. Kinetics and equilibrium studies of removal tion/precipitation processes using alkaline white mud. J. Hazard. Mater. 49,
of an azodye from aqueous solution by adsorption onto scallop. J. Ind. Eng. Chem. 735–741.
20, 610–615. Zolgharnein, J., Shahmoradi, A., Sangi, M.R., 2008. Optimization of Pb(II) biosorp-
Tahir, S.S., Rauf, N., 2006. Removal of a cationic dye from aqueous solutions by tion by Robinia tree leaves using statistical design of experiments. Talanta 76,
adsorption onto bentonite clay. Chemosphere 63, 1842–1848. 528–532.
Tsai, W.T., Chen, H.R., Kuo, K.C., Lai, C.Y., Su, T.C., Chang, Y.M., Yang, J.M., 2009. The
adsorption of methylene blue from aqueous solution using waste aquacultural
shell powders. J. Environ. Eng. Manage. 19, 65–172. Further reading
Tsai, W.T., Chen, H.R., 2010. Removal of malachite green from aqueous solution using
low cost chlorella-based biomass. J. Hazard. Mater. 175, 844–849. Chen, C.C., Lu, C.S., Chung, Y.C., Jan, J.L., 2007. UV light induced photodegradation of
Walker, G.M., Hansen, L., Hanna, J.A., Allen, S.J., 2003. Kinetics of a reactive dye malachite green on TiO2 nanoparticles. J. Hazard. Mater. 141, 520–528.
adsorption onto dolomitic sorbents. Water Res. 37, 2081–2089. Hameed, B.H., El-Khaiary, M.I., 2008. Batch removal of malachite green from aqueous
Wang, C.C., Chow, H.M., Yang, L.D., Lu, C.T., 2009. Recast layer removal after electrical solutions by adsorption on oil palm trunk fibre: equilibrium isotherm and kinetic
discharge machining via Taguchi analysis: a feasibility study. J. Mater. Process. studies. J. Hazard. Mater. 154, 237–244.
Technol. 209, 4134–4140. Pan, B., Huang, P., Wu, M., Wang, Z., Wang, P., Jiao, X., Xing, B., 2012. Physicochem-
Wang, S., Ariyanto, E., 2007. Competitive adsorption of malachite green and Pb ions ical and sorption properties of thermally-treated sediments with high organic
on natural zeolite. J. Colloid Interface Sci. 314, 25–31. matter content. Bioresour. Technol. 103, 367–373.