June 2011, Volume 2, No.

3 International Journal of Chemical and Environmental Engineering

Modelling for capture of carbon dioxide using aqueous ammonia from flue gases of a brick kiln
S. Nazir-1a, M. Tufail, W. Nisa,, M. Ghauri,, Biomass Conversion Research Center Department of Chemical Engineering COMSATS Institute of Information Technology (CIIT) M.A. Jinnah Building, Defence Road, Off Raiwind Road, Lahore-Pakistan a Salman Nazir E-mail: salmannazir@ciitlahore.edu.pk
Abstract Different sources are responsible for the addition of green house gases to the environment. Carbon dioxide in flue gasses from brick manufacturing industry is a considerable cause among them, especially in developing countries like Pakistan. Firewood and coal both are commonly used as primary fuel for a brick kiln manufacturing in Pakistan. The carbon emissions from brick kilns must be captured for carbon controlled environment. The objective of this research is the development of a simulation model in order to mitigate carbon emissions from the Brick Kiln. The statistical data of flue gases of a brick kiln situated near Lahore (Pakistan) has been identified and a model for the absorption of carbon dioxide prior to entrance in environment is proposed. It is widely accepted that the post combustion carbon capture technique is most feasible among the rest of the methods available; therefore, aqueous ammonia is employed in our research as a post combustion carbon capture technique. This technique has never been employed before on brick industry of Pakistan. The carbon dioxide recovered can be consumed by using it for beverages and also for oil fields. This development not only earns pollution control but also substantial carbon neutrality. Keywords: Brick industry of Pakistan, Brick kiln, Carbon capture techniques, Modeling, Aqueous ammonia

1. Introduction
Reduction of green house effect gases (GHGs) has taken the attention of researchers and scientists around the globe. In recent years, these concerns have risen than ever before. In 1997, world community including Pakistan accepted Kyoto Protocol. Its importance and possible implementation was emphasized in 2005. The objective was to address the problem of climate changes occurring due to human activities. Protocols were defined to follow the footwork of UN Framework Convention on Climate Change (UNFCCC) [1]. All the signatories agreed to take legal obligation for the reduction of green house gases by 5.2% of the emissions by 2012. Pakistan has to take actions to fulfill this commitment. Therefore it is obligatory to review and mitigate the greenhouse gases emissions in all industrial sectors including brick industry. Other than power plants and automobiles brick kilns, are also contributing in environmental pollution. According to our estimation there are more than 1000 brick kilns working in the vicinity of Lahore. The annual production of bricks is approximately 46 million per year from more than 6000 brick kilns in Pakistan. It has been estimated that approximately 533019 tons of untreated greenhouse gases are emitted from these kilns on annual basis which contribute in various environmental problems [2]. The height of chimney is also not high enough because of which the gloom leans downwards to the land, ultimately polluting the area. Since birth man has urged to adopt a better lifestyle with better living conditions. To satisfy this desire the concept of urbanization appeared. Various activities influence the demand of building materials which include new construction ideas, renovations, congestion of population, and other such technological advancements. In densely populated countries, like Pakistan, continuous urbanization and increased buying power of people have played significant role in the increase of production of construction materials like fired clay bricks. Many houses of 170 million people living in Pakistan are being constantly constructed by the orthodox fired clay bricks, but this almost invisible process tends to be underestimated. Fired clay bricks have been the preferred and reliable construction material of mankind for centuries. For several thousands of years even in 20th century, the technology for brick-making changed very little. Bricks were made by hand, dried under the sun and then fired in clamps or kiln using firewood or coal. During the last fifty years, the brick industry in Europe has gone through a revolution and thousands of small brickworks that existed at the beginning of the 20th century have been replaced by a few hundred large-scale, capital-intensive, highly mechanized brick works.

Modeling for capture of carbon dioxide using aqueous ammonia from flue gases of a brick kiln Contrary to the situation in rural areas of developing countries like Pakistan, in terms of both brick-making technology and the organization of work, there have been no major changes. In villages small-scale brick-making, is organized in family-owned enterprises serving local markets. The traditional technology of hand-molding, sun drying and firing in clamps is still being used. In this work the need of developing a model to update the brick manufacturing industry in a way that the continous poisoning of environment can be reduced thereby controlling the amount of CO2 being added continuously. The process which is commonly used for the production of brick in Pakistan is shown in Fig. 1. Clay operation, shaping, drying and firing operations are the important steps in the formation of brick as shown in the Fig. 1. Bricks are made from clay, soft slate and calcium silicate with the addition of water to give it a uniform shape.
Clay

It is very understandable that Pakistan a country of over 170 million people (ref) and with one of the highest growth rate per year have a high demand of brick per year which is rising on consistent basis. Table 1 shows the emissions of GHGs produced by the Brick Industry in all provinces of Pakistan. 1.3 Emissions: The emissions from Brick Kiln industry in Pakistan is at frightening level. The values of GHGs release calculated from the up corresponding to 6000 brick units established in the country are 139600, 19600, 495200, 2100, 360, 17 and 540 t respectively for total carbon (C), carbon dioxide (CO), carbon dioxide (CO2), methane CH4, nitrous oxide (NO), nitrogen dioxide (N2O) and NOx. It is evident that GHGs emissions are dominated by carbon dioxide (CO2) followed by CO and other non-CO2 gases. Projected contributions of GHGs from the Punjab province to the countrys total emissions are highest which can be observed in the Table 1. [2].

2. Carbon Dioxide Capture Techniques

There are mainly three major routes of capturing carbon dioxide namely (i) Post-combustion (ii) Precombustion and (iii) Oxy-combustion as shown in Fig. 1. Post combustion capturing methods involve removal of CO2 from gases produced by combustion after the combustion reactions. In Pre-combustion methods CO2 is absorbed before the fuel is burnt. Fuel is first oxidized to produce synthesis gas by the gasification reactions then the water gas shift reaction takes place to form CO2 concentrated streams and H2 gas from where CO2 is absorbed and H2 is burnt. In oxy-combustion processes the fuel is burnt with almost pure oxygen (95%) and a cryogenic unit is normally used to supply such high purity oxygen [4]. Table 1 discusses the salient features of the technologies and some of their limitations. The tree diagram shows the options for capturing CO2 with major focus on post combustion techniques because of retrofit ability of these processes [4]. Post Combustion Techniques: Post-combustion process involves removal of CO2 from the flue gas. Combustion units generate flue gases that are at atmospheric pressure and have CO2 concentration between 5 to 15%. It has the greatest potential for reducing emissions, because it can be integrated to existing plants which majorly contribute in CO2 emissions. Some of the methods used for CO2 capture are disused in the following sections.

Brick Shaping

Water

Brick Shaping

Solar Energy

Firing

Fuel

Fig. 1: Brick manufacturing process

It starts with the raw clay, preferably in a mix with 2530% sand to reduce shrinkage. The clay is first ground and mixed with water to the desired consistency. The clay is then pressed into steel moulds with a hydraulic press. The shaped clay is then fired at 900-1000 C to achieve strength [3]. 1.1 Bull's Trench Kilns In Pakistan, brick making is classically a manual process. The only type of brick kiln in use is Bull's Trench Kiln (BTK), based on a design developed by British engineer W. Bull in the late nineteenth century [3]. 1.2 GHG Emissions The combustion of coal and wood release carbon dioxide, methane, carbon particle, nitrous oxide and a variety of manufactured chemicals that do not occur in nature like CFCs, ozone, carbon monoxide, non-methane hydrocarbons, (NMHCs) and nitrogen oxides [2].

3. Absorption
Absorption processes are being commercially employed to overcome acid gas from natural gas and to

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Modeling for capture of carbon dioxide using aqueous ammonia from flue gases of a brick kiln remove CO2 from synthesis gas in the production of hydrogen, ammonia and methanol. CO2 from brick kiln can be captured by such absorption mechanisms. Various types of amine solutions are being used to scrub CO2 from natural gas which is an example of CO2 absorption route. CO2 is absorbed in a solvent and this process is temperature and pressure dependent. Removal of CO2 by absorption processes is based on the solubility of CO2 within the solvents. The solubility depends on the partial pressure and on the temperature of the gas. High CO2 partial pressure and low temperature favor the solubility of CO2 in the absorbent. The solvents are then regenerated by heating or by reducing pressure. Monoethanolamine solution is one of the majorly used solvent for CO2 absorption. Amines have a property to react with CO2 and form water soluble compounds. Because of this compound formation, amines are able to capture CO2 from streams with a low CO2 partial pressure. Amine-based systems, such as Monoethanolamine (MEA), are able to capture CO2 from the flue gases. This method has been used for years to remove CO2 from sources of natural gas. There have been many improvements in amine absorption systems for capture of CO2, and NOx from flue gases. It is currently used for comparing other CO2 capture technologies [5]. Aqueous ammonia based absorption unit is similar in operation to amine systems such as MEA. Ammonia and its derivatives react with CO2 through various mechanisms, out of which one is the reaction of ammonium carbonate, CO2, and water to give ammonium bicarbonate. This has a significantly lower heat of reaction than amine-based systems, which saves energy. CO2 when absorbed in ammonia forms carbonates and other by-products like ammonium sulfate and ammonium nitrate after reacting with NOx and SOx in the flue gases which is a significant feature of this system. The absorber in this case works best within the temperature range of 16 to 27 oC to enhance CO2 absorption in ammonium compounds. Within these temperatures vapor emissions during regeneration step are also minimized. Another process with lesser escape of ammonia vapors is called Chilled Ammonia Process (CAP). Same compounds of ammonium carbonate and ammonium bicarbonate are formed just like the aqueous ammonia system discussed. In this case no fertilizer is produced but only a slurry containing aqueous ammonium carbonate and ammonium bicarbonate solids is used to absorb carbon dioxide. In this process flue gas has to be cooled down to the temperature range of 32 to 50 C for which direct heat transfer by chilled water is required [6].
Table 1: CO2 Emissions of provinces of Pakistan [2] Province Provincial Division Green House Gases Emission (tons/year) 91335 81929 60130 80487 51552 45440 42692 25902 479467 9542 14020 3409 7361 34332 8463 Green House Gasses Emission %age 17.16 15.37 11.28 15.10 9.67 8.52 8.00 4.86 89.96 1.79 2.63 0.64 1.38 6.44 1.59

Punjab

Lahore Faisal Abad Multan Gujranwala Sargodha Rawalpindi Bahawalpur D.G.Khan Total

Sindh

Hyderabad Karachi Mir Pur Khas Sakhar Total

Khyber Pakhtunkh wa

Peshawar

D.I.Khan Kohat Total Balochista n Kalat Naseer Abad Quetta Total Grand Total

3726 2556 14745 614 1181 2680 4475 533019

0.69 0.48 2.76 0.11 0.22 0.51 0.84 100

There are few technical hurdles for chilled ammonia process in terms of energy consumption to run this plant but it gives 90% efficiency of carbon dioxide capture and there is no problem of ammonium bicarbonates deposition which causes fouling [5].

3.1. Membrane Separation

A relatively new capture concept is the use of selective membranes to separate CO2 from a flue gas stream. Membranes are semi-permeable barriers which separate substances by various mechanisms namely: solution/diffusion, adsorption/diffusion, molecular sieve and ionic transport, etc [7]. They are available in different organic and inorganic materials. Polymeric membranes are organic whereas carbon, zeolite, ceramic and metallic membranes are categorized as inorganic membranes. These membranes can be both, porous or nonporous.

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Modeling for capture of carbon dioxide using aqueous ammonia from flue gases of a brick kiln research is going on for stability and the effect of impurities at various temperatures and pressures. Ideally an MOF should have low energy requirement for regeneration, good thermal stability, tolerance to contaminants, attrition resistance, and low cost [9]. Current status of CO2 capturing technologies: Systems like Integrated Gasification Combined Cycle (IGCC) and ammonia production are well established processes for CO2 capture. Solvents used in these processes are effectively separated [5]. The only requirement is that the gas turbines must be capable of using H2-rich fuel. According to latest technological developments MEA Solution, one of the solvents for chemical absorption, is being commercially used for CO2 capture from flue gases. Other commercially available technologies include CO2 capture using membranes and cryogenic process [5].

Fig. 2: CO2 Capture Techniques

Membranes act as filters to separate one or more gases from a feed mixture and generate a specific gas rich permeate. A membrane is mainly characterized on two fundamental parameters which are permeability and selectivity. For instance when flue gas is passed through membrane tubes and amine solution is in the shell side, CO2 would pass through the membrane and be absorbed in the amine, while impurities would be blocked from the amine. There is a variety of options for using membranes to recover CO2 from flue gas which is absorbed in MEA solution. After the membrane separation, the amine would be regenerated before being recycled. For better results increased membrane selectivity and permeability is required. Studies are being carried to develop such membranes which enhanced selectivity and permeability. Another concept under development is the use of an inorganic membrane [4].

4. MaterialandMethod
4.1 Aqueous Ammonia Process: Ammonia-based wet scrubbing is similar in operation to amine systems. Ammonia and its derivatives react with CO2 to give ammonium carbonate which then further reacts with CO2 and water to form ammonium bicarbonate. The heat of reaction for this change is lower than the amine absorbers. An ammonia based absorption unit because of its multiple advantages over MEA and that is why has more potential to be considered for CO2 absorption under the controlled conditions. Ammonia-based absorption has some advantages over amine systems. For instance, aqueous ammonia is capable of absorbing more CO2. There is less degradation of solvent during absorption and regeneration. It has tolerance to oxygen in the flue gas and can be regenerated at high pressures. There is more capacity of CO2 absorption as compared to the MEA system which is up till now taken as a reference model to assess the absorption characteristics of different solvents. It also reacts with SOx and NOx, the criteria pollutants found in flue gas, to form fertilizers which are ammonium sulfate and ammonium nitrate respectively. These by products have potential to generate profit and fulfill local exigencies [5]. There are some concerns regarding ammonia. It has higher volatility compared to that of MEA but to overcome this issue flue gas needs to be cooled so that absorber operates within the temperature range of 15 to 25 0C. This enhances formation of ammonium compounds and helps to minimize emissions of ammonia vapors. Same concern rises during regeneration but since ammonia regenerates at lower temperature that is why altogether its emission is lower than MEA absorber. More research is carried out to further optimize the process for

3.2. Adsorption
Another way of capturing CO2 is by adsorption route. In this mechanism the separation relies on the thermodynamic properties of the substance to shift from the gas phase to attach itself to a solid material. This attachment can be physical (physisorption) or chemical (chemisorption). Adsorption encompasses the selective removal of CO2 from a gas stream to the adsorbents like zeolite or charcoal. This is followed by regeneration (desorption), which is carried out mainly by reducing pressure or by increasing temperature. Sometimes an electric current is also passed through the adsorbent. Some of the adsorbents are washed to separate the attached species [8]. Metal organic frameworks (MOFs) are a new class of hybrid material built from metal ions with well-defined coordination geometry and organic bridging ligands. They are extended structures with carefully sized cavities that can absorb CO2. High storage capacity is possible, and the heat required for recovery of the adsorbed CO2 is low.Over 600 chemically and structurally diverse MOFs have been developed over the past several years. More

216

Modeling for capture of carbon dioxide using aqueous ammonia from flue gases of a brick kiln
Table 1: Carbon dioxide Capture technologies: Advantages and disadvantages Capture Technology Postcombustion Pre-combustion Advantages This technology can be integrated to existing power plants and there is comparatively more removal of NOx and SOx Low CO2 partial pressure. Significant cost savings are possible. Very low GHG emissions Gives higher CO2 concentration and partial pressure as compared to post-combustion capture hence higher CO2 separation from flue gases. For coal plants, efficiency and cost are generally lower than for post-combustion capture. Very high CO2 concentration in flue gases Conventional commercially available combustors are used. Need to recycle large quantities of flue gas to avoid excessively high combustion temperatures. CO2 is recycled to the compressor to provide the expansion medium, instead of air. Retrofit and repowering technology option. Potential for advanced oxygen separation membranes with low energy consumption Limitations More energy is consumed due to solvent regeneration step and some loss in the solvent also occurs. Significantly high circulation volume is required for high capture levels. Cooling of gas to capture CO2 is necessary Efficiency loss in water gas shift reaction Fuel processing and extensive supporting systems are required Barriers to commercial application of gasification are common Large cryogenic O2 production requirement may be cost prohibitive Large cryogenic oxygen production requirement Cooled CO2 recycle required to maintain temperatures within limits of combustor materials. Decreased process efficiency High energy input for air separation Combustion in pure Oxygen is complicated and sophisticated

Oxy-combustion

increased loading capacity of CO2 and decreased losses of ammonia vapors [5]. 4.2 CO2 Ammonia Absorption Chemistry: Following reactions take place during the capturing process:
CO2 + H2O
CO2 + NH3

nitrogen fertilizers, like ammonium bicarbonate and urea [5]. It is known that carbonates can react with alkaline earth metals such as calcium and magnesium, and be deposited as carbonate minerals [6]. Ammonium bicarbonate can neutralize alkaline species and reduce salt content by forming stable compounds shown in the equations below:

HCO3- +H+
NH2COO - +H+

(1) (2) (3) (4)

HCO3- + Ca2+ + OHHCO3 + Mg

2+

H2O + CaCO3

(8)

NH2COO - + H2O

NH3 + HCO3-

+ OH

H2O + MgCO3 (9)

NH3 + H+
CO3 + H
2+

NH4+
HCO3
-

(5) CO2 reacts with water to form bicarbonate and ammonia to form a carbamate. The carbamate undergo hydrolysis to release ammonia and bicarbonate. Sprinkling aqueous ammonia into flue gas not only reacts with CO2 but also absorbs traces of SOx and NOx from the flue gas in accordance with the following chemical equations [6]:
NOx + SOx + H2O HNO3 + H2SO4

These solid products, calcium carbonate and magnesium carbonate are undoubtedly stable form of sequestered CO2. The purpose of this work is to mitigate the emission of CO2 from a brick kiln, as this gas is among the major culprits causing green-house effect which has ultimately resulted in drastic and disastrous weather changes and temperature-rise to alarming levels across the globe. Each year the addition of CO2 solely from the brick industry of Pakistan is 533019 tons.
Table 2: Flue gas composition from brick kiln Sr. Number Component N2 CO2 CO NO2 H2O H2 SO2 Mole Percentage 71 6.06 3.94 8.89 3.11 2.12 4.88

(6)

NH4NO3 + (NH4)2SO4 (7) The solid ammonium carbonate and bicarbonate hence formed can either be dried or exist in an aqueous solution as crystalline solids. The ammonium bicarbonate (NH4HCO3) is being used in china for more than 30 years from now as a nitrogen fertilizer. It has been experienced when NH4HCO3 is placed into deep soil; its nitrogen contents effect on crops similar to other well known

HNO3 + H2SO4+ NH3

1 2 3 4 5 6 7

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Modeling for capture of carbon dioxide using aqueous ammonia from flue gases of a brick kiln Gas absorption has so far been the most useful and advantageous technique which has been covered in detail in the section post carbon techniques. Different models and methods have been proposed and tested. In our model, we have chosen Aqueous Ammonia as the solvent. The model was developed on HYSYS 7.1. General NRTL was selected as the fluid package. This fluid package is quite versatile and it not only accommodates the properties of our system components but also the aqueous and mixed solvent systems. The flow-sheet of our model is shown in Fig. 3. The temperature of gases emitting from top of the brick kilns is in the range of 120 to 150 C. The composition of these gases is dependent on different parameters and also the composition of CO2 varies from 3-15%. The composition of the flue gesses were found using industrial combustion and emission analyzer (E8500, USA) which is shown in Table 2. Aqueous ammonia solution introduced from top of the column absorbed most of the CO2 and the treated gas contained almost negligible amount of CO2. In order to make the process economical, a stripper was installed after the absorber. By the virtue of stripper, not only Ammonia solution was recovered but also CO2 was regenerated. The recovered MEA solution was then recycled to the top of While simulating absorber and stripper, special attention was paid to find a workable temperature and pressure range because too much high pressure and low temperature in absorber can lead to condensation of feed gas. Whereas in stripper, high temperature and low pressure can result in vaporization of liquid feed. The tables and graphs resulted from this simulation of our proposed model are shown in results and discussion section.

5. ResultsandDiscussion
The rate of absorption is affected by variables such as

Fig. 3: Effect of Flowrate

temperature, pressure, flow-rate, solvent percentage etc. all these variables were manipulated to study their effect on absorption with the help of resulting tables and trends. The results of all these parametric changes are discussed one by one.

5.1. Effect of Temperature on CO2 Absorption

It is a well known fact that temperature is inversely related to the rate of absorption, our model also gives the similar results. The system temperature was varied from 20C to 50C and there was a mark decrease in absorption rate with the increasing temperature. The resulting graph is shown in Fig. 4.

Fig. 3: Process flow diagram

the absorber. In our model as shown in Fig. 3, kinetic and hydrodynamic aspects were also considered so the results of our model depicted realistic values. These values were then compared and verified by the reported values. In order to recover the adsorbate or the solute-gas (CO2 in our case) and to regenerate the adsorbent or liquid solvent (Ammonia solution in our case), a stripper was also installed next to the absorber. The stripping was done with steam at low pressure. In our HYSYS model, we varied different parameters (i.e. Temperature, Pressure, Flow-rate, MEA concentration etc.) and examined the resulting percentage of CO2 absorbed.

218

Modeling for capture of carbon dioxide using aqueous ammonia from flue gases of a brick kiln Pakistan 35818 tons per year of CO2can be saved from entering in the environment. As mentioned earlier that the total amount of flue gases emitting from the Brick Industry is 533019 tons per annum. This means that every year 37311 tons (from Table 4) of CO2 are gifted to the environment by only brick kilnFig. 4: Effect However, if our Ammonia model is industry. of Concentration of proposed installed throughout the country, only 1492 tons/year of CO2 will be added to environment, as shown in the Table 4. The amount of CO2 captured annually will be 35819 tons. This amount of CO2 could be further utilized to the advantage of industrial processes. These findings are identified for the first time for the Brick industry of Pakistan.

It can be seen from Fig. 4 that our model follows standard pattern of increase in absorption with decrease in temperature. Moreover, for better validation of our proposed model we have completed the simulation using solvents of different flow rates which is clearly depicted in the figure.

5.2. Effect of Flow rate on Rate of Absorption

The results obtained by simulation of our HYSYS model show agreement with the standard findings that there is increase in absorption with that of increase in flow rate. In our HYSYS model, we used different flowrates and the results showed that the rate of absorption increased with flow-rate as shown in Figure. The effect of number of stages in the absorber was also studied which
Fig. 4: Effect of Temperature

6. Conclusions
In this work, a model has been developed and simulated, which aims at the control of CO2 gas which is continuously entering to the environment from the brick industry in Pakistan. It is for the first time that the brick industry in Pakistan has been analyzed with this perspective and a model is proposed for the mitigation of major GHGs i.e. CO2. With the implementation of our model, the result showed that 96% of CO2 emitting from Brick kiln is captured. If all the brick Kilns in Pakistan employ the proposed model then 35818 tons of CO2 can be captured. Moreover the proposed model follows the exact trends regarding the absorption of CO2 of the dependency of absorption with the change in temperature, pressure, and flowrate with that of the reported values in the literature. In future work the authors plan to carry out the comparison of economic feasibility of proposed work with the idea of the replacement of BTK with Vertical Shaft Brick Kiln (VSBK).

is shown in the Fig.5.

5.3. Effect of Ammonia Percentage on Rate of Absorption

The percentage of Aqueous Ammonia was varied from 3 to 15 %. The HYSYS model showed that the percentage of CO2 absorbed increased with the decreasing Ammonia percentage. The percentage of CO2 absorbed increased more rapidly from 15 to 7% but after 7%, the percentage of CO2 absorbed did not increase with the
Table 3: Comparison of Carbon Dioxide emission before and after employing proposed Model Province CO2 at CO2 Captured CO2 Present (tons/yr) Released (tons/yr) (tons/yr) 33562.70 32220.19 1342.50 Punjab 2403.12 2307.00 96.12 Sindh 1032.18 990.89 41.28 Khyber P. 313.31 300.78 12.53 Balochistan Total 37311.33 35818.87 1492.45

same rate. Therefore, 7% Ammonia solution was selected as the optimum solution. The reported values suggested that higher percentage of Aqueous Ammonia can lead to corrosion of absorber. Hence, a model with 7 % Aqueous Ammonia solution is identified as the best choice. The temperature of Aqueous Ammonia solution entering from the top in to the absorber is 15 C. The simulation results exhibits that with the use of proposed model from the brick industry in

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