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Middle-East Journal of Scientific Research 11 (6): 828-832, 2012 ISSN 1990-9233 IDOSI Publications, 2012

Comparative Study of Adsorptive Removal of Congo Red and Brilliant Green Dyes from Water Using Peanut Shell
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Aadil Abbas, 1Shahzad Murtaza, 2Kashif Shahid, 1Muhammad Munir, 1Rabia Ayub and 1Saba Akber
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Department of Chemistry, University of Gujrat, Gujrat, Pakistan 2 Student Service Center, University of Gujrat, Gujrat, Pakistan

Abstarct: Aqueous toxicity is a burning issue of the current era with rapidly growing industrialization and urbanization, especially in the developing countries where no proper treatment of the waste effluents is regulated. Present was a comparative study involving removal of congo red and brilliant green, two toxic dyes of different chemical origin, by biosorption using peanut shell as biosorbent. Effect of various factors on biosorption process such as contact time, pH, agitation speed, biosorption dose, particle size was studied. Study revealed that peanut shell adsorbs dyes by both chemisorption and physiorption. Removal efficiency of congo red was 15.09 mg/g and that of brilliant green 19.92 mg/g. Negative values of thermodynamical parameters ( G) showed that it was an exothermic process. Key words: Adsorptive Removal Congo Red Brilliant Green Dyes Peanut Shell

INTRODUCTION The potable water used by every human being for drinking and cooking should be uncontaminated and pure [1]. Waste water from the textile, cosmetics, printing, dying, food coloring and paper-making industries is polluted by dyes [2]. More than 80% of their production is utilized by the textile industries. A huge amount of water is necessary by these industries for the cleaning and washing purposes and they discharge highly colored effluents containing different dyes [3]. These colored effluents can be mixed in surface water and ground water system. Then they may also transfer to drinking water. In literature, almost 40,000 dyes and pigments are listed which consist of over 7000 diverse chemical structures [4-6]. Industrial effluents discharged from dyeing industries are highly colored with a large amount of suspended organic solid. These effluents are discharge into rivers make water unfit for domestic, agricultural and industrial purposes. Many dyes and their break down products may be toxic for living organisms. Dyes even in low concentrations are visually detected and meanwhile affect the aquatic life. A very small amount of dye in water is highly visible. Further, discharging even a small amount of dye into water can affect aquatic life and food webs due to the carcinogenic and mutagenic effects of synthetic dyes [7]. The various textile dyes rank 1st in usage of dyes for coloration of fiber. It is estimated that

about 10-15% dyes are released into processing water during this procedure. It is broadcasted that more than 60% of the dyes world production is consumed by textiles industries. [8].Dyes according to their structure as anionic and cationic. In aqueous solution, anionic dyes carry a net negative charge due to the presence of sulphonate (SO 3-) groups, while cationic dyes carry a net positive charge due to the presence of protonated amine or sulfur containing groups. Dyes are chemicals, which on binding with a material will give color to them [9-10]. Congo red dye is benzedene based dye. This dye has been known to cause an allergic reaction and to be metabolized to Benzedrine. Its decomposition results in carcinogenic products. It acts as a skin, eye and gastrointestinal irritant. It impresses blood factors such as clotting and induces drowsiness and respiratory problems [11-12].

Fig. 1: Molecular Formula of Congo Red

Corresponding Author: Aadil Abbas, Department of Chemistry, University of Gujrat, Gujrat, Pakistan .

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Middle-East J. Sci. Res., 11 (6): 828-832, 2012

Experimental Work Processing of Adsorbent: The peanut shell was collected from rural district council Gujrat. It was ground to powder and washed with double distilled water to remove dust particles. Then powder was kept in air to dry and placed in oven at 30C for one hour. Biosorbent was ready. Fig. 2: Molecular structure of Brilliant Green dye. Brilliant green is hazardous triphenyl nitrogen containing cationic dye. About 0.8 to 1.0 kg of this dye is used per ton of paper produced. It is utilized in the manufacturing of green ink, as an indicator, which changes its color from yellow to green at pH 2.6. Its contact with skin results in irritation with redness and pain. It can causes irritation to the respiratory tract and gastrointestinal tract that leads to cough, shortness of breath, symptoms of nausea, vomiting and diarrhea in human beings [13,14]. Although contaminated waste water may be treated with conventional physicalchemical methods like reverse osmosis, ion exchange, chemical precipitation or lime coagulation and oxidation, the application of these techniques has been restricted due to high energy consumptions or expensive synthetic resins and chemicals. Moreover, these methods generate large amount of toxic sludge and are ineffective at lower concentrations of dye. Therefore, there is an urgent requirement for development of innovative, but low cost processes, by which dye molecules can be removed. Adsorption technique is quite popular due to simplicity and high efficiency, as well as the availability of a wide range of adsorbents. It has proved to be an effective method for removal of dye from wastewater. A number of non-conventional, low cost adsorbents such as, rice hull ash, leaf, fly ash, activated red mud, rice husk and fungi have been used for the removal of dyes from aqueous solutions. Various adsorbents have been tried for removal of Brilliant Green dye from water. The peanut, or groundnut (Arachis hypogaea), is a species in the legume or "bean" family (Fabaceae). It is an annual herbaceous plant growing 30 to 50 cm (1.0 to 1.6 ft) tall. The leaves are opposite; pinnate with four leaflets and flowers are a typical pea flower in shape, yellow with reddish veining. Peanuts are known by many other local names such as earthnuts, ground nuts, goober peas, monkey nuts, pygmy nuts and pig nuts. In order to design adsorption treatment systems, knowledge of kinetic and mass transfer processes is essential [15-16]. 829 Procedure: Standard solutions from 1000ppm stock solution of both the dyes of concentrations (3-15ppm for CR and 2-10ppm for BG) were prepared. Mesh Size: The batch adsorption was carried out on a thermostat shaker at100rpm and 25C using flasks containing 25ml of dye solution and 0.5g of biosorbent of mesh size ranging from 20-100 micron meter. Biosorbent Dose: Biosorbent of different doses from 0.5 to 3.0g having difference of 0.5g each in 25ml dye solution was stirred at 100rpm for 10min. Contact Time: The batch absorption for contact time was carried out on stirrers at 100rpm with time varying from 1060min. Agitation Speed: For agitation speed, sorption experiments were conducted by agitating 0.5g of the biosorbent with 25ml of the solution in a shaking thermostatic water bath varying agitating speed from 50300rpm. Temperature: The batch sorption of flasks was conducted on stirrers containing 25ml dye solution and 0.5g biosorbent varying temperature ranging from 10-60C having a difference of 10C each. pH: For pH, adsorption was carried out in flasks containing 25ml dye solution and 0.5g biosorbent having pH ranging from 2-8 for congo red and 5-12 for brilliant green. RESULTS AND DISCUSSION Comparative study was conducted using peanut shell powder surface as biosorbent for the adsorptive removal of congo red (anionic dye) and brilliant green (cationic dye) dye from its aqeous solution. Operational conditions such as biosorbent dose, agitation speed, contact time, pH, temperature and particle size were optimized for both the dyes.

Middle-East J. Sci. Res., 11 (6): 828-832, 2012

Fig. 1: Comparative graph showing effect of temprature on %age removal of CR and BG.

Fig. 3: Comparative graph showing effect of agitation speed on %age removal of CR and BG. Migration of dye from bulk of the solution to the surface of the adsorbent Diffusion of dye through the boundary layer to the surface of the adsorbent Intra-particle diffusion of dye into the interior pores of the adsorbent particle. The boundary layer resistance will be affected by the rate of adsorption and increase in contact time, which will reduce the resistance and increase the mobility of dye during adsorption [18]. Effect of Agitation Speed: Agitation is an important parameter I n adsorption phenomenon, influencing the distribution of the solute in the bulk solution and formation of the external boundary film. The effect of variation in the agitation speed on the adsorption of brilliant green and congo red was studied. The results are shown in Fig. 3. For brilliant green maximum %age removal efficiency was observed at an agitation rate of 250rpm and for congo red it was at 150rpm. An increasing agitation rate may reduce the film boundary layer, surrounding the sorbent particles, thus increasing the external film diffusion rate and the uptake rate. Effect of Biosorbent Dose: The study of biosorbent dose for the removal of the dyes from aqueous solution was carried out using peanut shell powder with their amount varying from 0.5 to 3.0g. The maximum % age of dye removal for brilliant green was 97.53% and 87.2% for congo red attained for biosorbent dose of 1.0g as shown in Fig. 4. The percentages of the dye removal decreases with increase in biosorbent dose because of all available sites were covered and no active site available for further binding of dye molecules to biosorbent surface. 830

Fig. 2: Comparative graph showing effect of contact time on %age removal of CR and BG. Effect of Temperature: Temperature has a pronounced effect on the adsorption capacity of various adsorbents. The temperature effect was investigated for temperatures ranging 10-60C. The results are shown in Fig. 1. The maximum % age removal efficiency of biosorbent was 85.94% for congo red at 40C and 98.91% for brilliant green at 30C. Since adsorption is an exothermic process, it would be expected that an increase in temperature of the adsorbateadsorbent system would result in decreased adsorption capacity. Thus the adsorption of dyes is leading to a decrease in the residual forces on the surface of the biosorbent and hence causing a decrease in the surface energy of the biosorbent [17]. Effect of Contact Time: The time-dependent behaviour of dye adsorption was examined by varying the contact time between biosorbate and biosorbent in the range of 10-60 min. The results are shown in Fig. 2. The adsorption of brilliant green dye increased with increasing contact time due to larger surface area available of the adsorbent. The maximum %age removal efficiency was 97.50% at 60min for brilliant green and 88.21% at 40min for congo red. The mechanism for the removal of dye by adsorption may be assumed to involve:

Middle-East J. Sci. Res., 11 (6): 828-832, 2012

Fig. 4: Comparative graph showing effect of biosorbent dose on %age removal of CR and BG.

Fig. 6: Comparative graph showing effect of particle size on %age removal of CR and BG. biosorbent surface. Generally, the net positive charge decreases with increasing pH value resulting in the decrease in repulsion between the adsorbent surface and the dye, thus improving the biosorption capacity [19]. Effect of Particle Size: Removal is directly related with surface area of biosorbent; therefore, the effect of particle size (Figure 6) was studied. The size of the biosorbent has a greater influence on the rate of biosorption. It was found that %age removal efficiency of congo red dye was 90.86% for 40-60micron and 96.34% for 60-80micron for brilliant green. The reduction in size resulted in increased %age removal efficiency. This of course related to high surface area of the adsorbent with much smaller size and high availability of function groups, which are responsible for dye adsorption over biosorbent [20]. Date Evaluation by Isothermal Modeling: So the above broad outcome of this comparison was that the peanut shell powder can actively adsorb congo red and brilliant green from its aqueous solution. Optimized conditions of adsorption for congo red dye were: 40 minute contact time, 8.0 pH, 1g biosorbent dose, 40-60 microns mesh sized particles, 150 rpm agitation speed and

Fig. 5: Comparative graph showing effect of pH on %age removal of CR and BG. Effect of pH: Figure 5 clearly showed the influence of the initial solution pH on the biosorption extent of brilliant green and congo red on to peanut shell. The maximum % age removal of congo red was 86.48% at pH 8.0 and 96.54% at pH 9.0 for brilliant green. In general, initial pH value may enhance or depress the uptake. This is attributed to the charge of the adsorbent surface with the change in pH value. It can be seen from the figure that as the solution pH increases, the adsorption capacity increases. Increasing solution pH increases the number of hydroxyl groups thus, increases the number of negatively charge sites and enlarges the attraction between dye and

Table 1: Langmuir modeling of equilibrium data for adsorption of congo red and brilliant green by peanut shell powder Langmuir Isotherm Parameter ----------------------------------------------------------------------------------------------------------Slope Intercept R2 qm(mg/g) b(L/g) 11.919 1.174 0.034 0.850 0.899 0.912 15.09 19.92 0.066 0.050 Separation Factor RL 0.78 0.19 Thermodynamical Parameters g (kJ/mol) -06.33 -16.51

Dye Congo Red Brilliant Green

Table 2: Freundlich modeling of equilibrium data for adsorption of congo red and brilliant green by peanut shell powder Freundlich Isotherm Parameters ----------------------------------------------------------------------------------------------------------------------------------------------------------------Slope Intercept R2 KF (mg1-1/n L1/n g-1) n 0.485 0.893 +0.921 -1.347 0.859 0.978 0.110 0.978 1.038 1.117

Dye Congo Red Brilliant Green

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Middle-East J. Sci. Res., 11 (6): 828-832, 2012

40C temperature. Whereas for brilliant green optimized conditions were: 60 minute contact time, 9.0 pH, 1g adsorbent dose, 60-80 microns mesh sized particles, 250 rpm agitation speed and 30C temperature. Suitability of equilibrium data was modulated with Langmuir and Freundlich isotherms and found that both physiosorption and chemisorption processes plays important role in adsorption of these dyes by peanut shell powder. Maximum biosorption capacity for congo red and brilliant green dyes were 15.09 and 19.92 mg/g respectively. The feasibility of adsorption system was supported by separation factor RL, adsorption intensity n and thermodynamic parameter G. Exothermic nature of the process suggested that peanut shell can be used as a potential adsorbent for dyes removal from waste water by using this method. REFERENCES 1. Jayaraj, R., P.J. Thanaraj, S.N. Thillai, P.M. Deva Prasath, 2011. Removal of Congo Red dye from aqueous solution using acid activated eco-friendly low cost carbon prepared from marine algae Valoria bryopsis. J. Chem. Pharm. Res., 3(3): 389-396. Jayarajan, M., R. Arunachalam and G. Annadurai, 2011. Agriculture wastes of Jackfruite Peel NanoPorous adsorbent for removal of Rhodamine Dye. Asian Journal of applied sciences, 4(3): 263-270. King, P., V.K. Parasanna and V.S.R.K. Prasad, 2005. Studies on adsorption isotherms for removal of fluorides using conventional and non-conventional adsorbents. Journal of Industrial Pollution Control, 21(1): 155-162. Acemioglu, B., 2004. Adsorption of Congo red from aqueous solution on to calcium-rich fly ash. Journal of Colloid and Interface Science, 274(2): 371-379. Noroozi, B., G.A. Sorial, H. Bahrami and M. Arami, 2008. Adsorption of binary mixtures of cationic dyes. Dyes and Pigments, 76(3): 784-791. Moussavi, G. and M. Mahmoudi, 2009. Removal of azo and anthraquinone reactive dyes from industrial waste waters using MgO nanoparticles. Journal of Hazardous Materials, 168(2-3): 806-812. Patil, A.K. and V.S. Shrivastava, 2010. Alternanthera bettzichiana plant powder as low cost adsorbent for removal of Congo red from aqueous Solution. J. International Journal of Chem Tech Research, 2(2): 842-850. Gharbani, P., S.M. Tabatabaii and A. Mehrizad, 2008. Removal of Congo red from textile waste water by ozonation. J. Environ. Sci. Tech., 5(4): 495-500. 832

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