Research Journal of Chemical Sciences ______________________________________________ ISSN 2231-606X Vol. 4(1), 91-102, January (2014) Res. J. Chem. Sci. International Science Congress Association 91 Review Paper Removal of Methylene Blue Using Low Cost Adsorbent: A ReviewMohammed M.A., Shitu A. and Ibrahim A. Department of Chemical and Environmental Engineering,Faculty of Engineering, Universiti Putra Malaysia, 43400, UPM, Serdang, Selangor Darul Ehsan, MALAYSIAAvailable online at: www.isca.in, www.isca.me Received 3rd December 2013, revised 6th January 2014, accepted 14th January 2014Abstract In this article, adsorption process has been found to be one of the best treatment methods for Methylene blue (MB) removals. As the control of water pollution has become an increasing importance in recent years, the use of physical/chemical treatments such as membrane filtration, reverse osmosis, coagulation/flocculation and fenton reagents are not economically feasible. The use of different biosorbent as an alternative low cost adsorbent in the removal of methylene blue has been extensively studied and compiled, together with their adsorption capacities and experimental conditions such as adsorbent dose, pH of the solution, temperature and equilibrium time. But, there are issues as regards to draw back in the use of activated sorbents which were also discussed briefly. However, it is evident from the results of experiments in the literatures surveyed that various low-cost adsorbents have shown good potential for MB. Keywords: Adsorption, methylene blue, waste water, low-cost adsorbent. Introduction Methylene blue is a common dye mostly used by industries involve in textile, paper, rubber, plastics, leather, cosmetics, pharmaceutical and food industries. Effluents discharged from such industries contain residues of dyes. Consequently, the presence of very low concentrations in effluent is highly visible1,2. Discharge of colored wastewater without proper treatment can results in numerous problems such as chemical oxygen demand (COD) by the water body, and an increase in toxicity. Currently, there are about 10,000 different commercial dyes and pigments exist and over 7x10tones of synthetic dyes are produced annually world-wide. It is estimated that 10–15% of the dyes are lost in the effluent during the dyeing processes. Major problems associated with colored effluent is lowering light penetration, photosynthesis and damages the aesthetic nature of the water surface4-6. Moreover, their degradation products may be mutagenic and carcinogenic7-9. Many dyes may cause allergic dermatitis, skin irritation, dysfunction of kidney, liver, brain, reproductive and central nervous system10. Organic dyes are harmful to human beings, the need to remove color from wastewater Effluents become environmentally important. It is rather difficult to treat dye effluents because of their synthetic origins and mainly aromatic structures, which are biologically non-degradable. Among several chemical and physical methods, adsorption process is one of the effective techniques that have been successfully employed for color removal from wastewater11. There are currently numerous treatment processes for effluent discharged from industrial processes containing dyes; amongst which we can mention biodegradation12, chemical oxidation13,14, foam flotation15, electrolysis16, adsorption17, electro-coagulation18 and photocatalysis19. Major aim of this review is to provide a summary of recent information concerning the use of low-cost materials as sorbents. For this, an extensive list of sorbent literature on methylene blue has been compiled. Nomenclature: T o C Temperature S Sips Isotherm mode Initial Concentration (Mg/l) Te Temkin isotherm models. T(min) Equilibrium Contact Time TY Thomas and Yoon–Nelson models, A.D Adsorbent dosage (g/l) K1 Pseudo first order kinetic model L Langumuir isotherm model K2 Pseudo second order kinetic model F Freundlich Isotherm model SDS sodium dodecylsulfate R Redlich–Peterson isotherm model MB Methylene blue Current treatment technologies for color removal involving physical and/or chemical and biological processes: The main components of dye molecules are: the chromophores, which are responsible for producing the color, and the auxochromes, which can not only supplement the chromophore but also render the molecule soluble in water and give enhanced affinity (to attach) toward the fibers20. The conventional methods for the treatment of colored wastewater are physical, chemical and biological treatments. However, these technologies have advantage and disadvantages. At large scale, most of these conventional methods are not applicable Because of the high cost anddisposal problems as large amount of sludge is been generated at the end of the process21. Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(1), 91-102, January (2014) Res. J. Chem. Sci. International Science Congress Association 92 Physical methods: Physical treatment includes membrane –filtration process, reverse osmosis, electrolysis and adsorption techniques. The major drawback in this technology, especially membrane filtration is limited life time before membrane fouling occurs and as such the cost of periodic replacement must thus be included in any analysis of their economic viability. Among all the physical treatments, adsorption process has been reported to be the most effective method for water decontamination22. Adsorption is known to be a promising technique, which has great importance due to the ease of operation and comparable low cost of application in the decoloration process. Commercially activated carbon is a remarkable highly adsorbent material with a large number of applications in the remediation of contaminated groundwater and industrial wastes such as colored effluents. However, activated carbon is an expensive adsorbent due to its high costs of manufacturing and regeneration. For the purpose of removing unwanted hazardous compounds from contaminated water at a low cost, much attention has been focused on various naturally occurring adsorbents such as chitosan, zeolites, fly ash, coal, paper mill sludge, and various clay minerals23,24. The use of activated carbon, however, is restricted due to its high cost. An attempt to develop cheaper and effective adsorbents and many non-conventional low-cost adsorbents such as clay materials, zeolites, siliceous material, agricultural wastes and industrial waste products have also been suggested25,26. Chemical treatment: The major agents of chemical treatment of dye wastewater are coagulants/ flocculants27,28,. It involves the addition of substances such as calcium, aluminum, or ferric ions in to the effluent, as such flocculation is induced29. Furthermore, Mishara30 and Yue15have report the use of other agents for chemical processes such as, ferric sulphate, and some synthetic organic polymers. While Shi et al27suggests the combination of the two methods may also be added to enhance the process. Generally, chemical treatment has economic feasibility and efficiency, but major drawback is that, the cost of chemical are expensive and price fluctuation in market due to high demand and the rate at which chemicals are being produced. Moreover, even though it’s efficient, the overall disadvantage of chemical treatment is the production of sludge at the final stage of the treatment which is pH dependent and brings about disposalproblems31. Biological methods: Biological treatment of wastewater is an alternative and most economical method as compare to physical and chemical methods. Biodegradation methods such as adsorption by (living or dead) microbial biomass, fungal decolorization, bioremediation systems and microbial degradation are commonly used in the treatment of industrial effluents. Microorganism such as yeasts, bacteria, fungi and algae are able to accumulate and degrade different pollutants, but due to some technical constraints their applications is often restricted32,33,34. Biological treatment may be aerobic and anaerobic35. But the major drawback is that, it requires substantial land area and is constrained by sensitivity toward diurnal variation as well as toxicity of chemicals 25. Moreover, contradictory findings were reported in review of current technologies36 which states that, with current conventional technology, biological treatment is incapable of obtaining satisfactory color elimination. Furthermore, dyes such as (azo dyes) are not easily degradable due to their complex chemical structure, synthetic organic origin and xenobiotic nature37. The table below, shows the advantage and disadvantages of physical and chemical treatments. Table-1 Existing and Emerging processes for dyes removal38Physical/chemical Methods Method description Advantages Disadvantages Fenton reagents Oxidation reaction using mainly 2 O 2 -Fe(II) Effective decolorization of both soluble and insoluble dyes Sludge generation Ozonation Oxidation reaction using ozone gas Application in gaseous state: no alteration of volume Short half-life (20 min) Photochemical Oxidation reaction using mainly 2 O-UV No sludge production Formation of by-products NaCl Oxidation reaction using Cl+ to attack the amino group Initial and acceleration of azo bond cleavage Release of aromatic amines Electrochemical destruction Oxidation reaction using electricity Breakdown compounds are non-hazardous High cost of electricity Activated carbon Dye removal by adsorption Good removal of a wide variety of dyes Regeneration difficulties Membrane filtration Physical separation Removal of all dye types Concentrated sludge Production Ion exchange Ion exchange resin Regeneration: no adsorbent loss Not effective for all dyes Electrokinetic coagulation Addition of ferrous sulphate and ferric chloride Economically feasible High sludge production Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(1), 91-102, January (2014) Res. J. Chem. Sci. International Science Congress Association 93 Despite the development of various technologies for dye waste water treatment, economic, effectiveness and rapid water treatment at a commercial level is still a challenging problem. Previous research efforts have focused on the adsorption technology for the dye remediation from wastewater39. This technique can handle fairly large flow rates, producing a high-quality effluent that does not result in the formation of harmful substances, such as ozone and free radicals40. Moreover, it can remove or minimize different types of organic and inorganic pollutants and thus has a wider applicability in pollution control. Adsorption is hence recognized as the most versatile process used in lesser developing countries and is currently being used extensively for the removal of organic pollutants from the aqueous media41,42. Natural adsorbents used for color removal Clay: Clay are natural adsorbent classified based on their difference in layered structure.The available classes of clay materials include smectites (montmorillonite, saponite), mica (illite), kaolinite, serpentine, pylophyllite (talc), vermiculite and sepiolite43. The process by which adsorption takes place is as a result of net negative charge on the structure of minerals, and it’s this negative charge that gives the clay mineral the capability to adsorb positively charged species. Most of Their sorption properties depends their high surface area and high porosity44. Siliceous materials: Natural Siliceous materials are one of the most availability and low price adsorbent. It includessilica beads, perlite and dolomite, aluniteand glasses. The use of these minerals was based on chemical reactivity of their hydrophilic surface and mechanically stable, which results from the presence of silanol groups. But among all this, silica beads is given particular attention in the use of the material as adsorbent45,25,46 . However, Ahmed47 reports that, a major problem with this kind of application is their low resistance toward alkaline solutions their usage is limited to media of pH less than 8. Zeolites: Zeolites occur naturally as porous aluminosilicates consisting of different cavity structures and are linked together by shared oxygen atoms48. Zeolite has a wide variety of species. More than 40 natural species are available which includes clinoptilolite and chabazite. But, clinoptilolite, a mineral of the heulandite group is the most and frequently studied material, due to its have high selectivity for certain pollutants. Intensive research has been done on the use and application of zeolite as adsorbent in removing trace quantities of pollutants such as heavy metal ions and phenols with regards to their cage-like structures suitable for ion exchange49-51 . Color removal using activated carbons from solid waste: Activated carbons are derived from natural materials such as wood, lignite or coal, which are commercially available. But almost any carbonaceous material may be used as precursor for the preparation of carbon adsorbents52-54. Coal is the most commonly used precursor for AC production Because of its availability and cost effective55,56. Coal comprises of different mixtures of carbonaceous materials and mineral matter, which results from the degradation of plants. The nature, origin and the extent of the physical–chemical changes occurring after deposition of vegetation, determines the sorption properties of each individual coal. In a research conducted by Karaka et al 57attention has been drawn onthe use of coal as a successful sorbents for dye removal. Additionally, coal is not a pure material, and thus will have different sorption properties due to its large variety of surface properties. Recently there has been report on the use of activated carbon in the treatment of dye and heavy effluents. Material such as peanut shell58, bael shell carbon59, raw pine and acid-treated pine cone powder60, Calotropis procera61, Neem Leaf62, Coconut Shell63, Super paramagnetic PVA-Alginate Microspheres64 were able to reduce the concentration of pollutants in wastewater successfully. Their sorption capacity increases with increasing in adsorbent dosage. Agricultural waste materials used as low cost adsorbent: The use of biomass (dead or living), fungi, algae and other microbial cultures in the removal of methylene blue was the subject of many recent researches. Biological materials used to accumulate and concentrate dyes from aqueous solution are termed as bioadsorbents. Major disadvantage in these biomaterials is its non-selective (i.e. it cannot isolate each pollutant and get it removed independently of one another) all the target and non-target contaminants if present are concentrated on the surface of the adsorbent. Unlike the conventional ion exchange the process are selective to the ions it needs to adsorb by selecting the ion in such a way that it is having affinity only that ion. Bioadsorption is a novel approach, and considered to be relatively superior to other techniques because of its low cost, simplicity of design high efficiency, availability and ability to separate wide65. Recent literature on the methods of removal of dye from wastewater focuses on MB adsorption. Adsorption capacities of different biosorbent for the removal of MB from wastewater; The excellent ability and economic promise of adsorbents prepared from biomass exhibited high sorption properties from selected literatures in the last one decade are summarized in the tables below. With the recent development on the use of low cost adsorbent, this review has made tremendous effort to cover a wide range of current researches on nonconventional adsorbents in order to enlighten researchers on the adsorption capacities of different biological material used in recent times as shown from the tables above. In all the studies compiled, it was observed that Equilibrium isotherms and kinetic studies were all determined as observed. Different adsorption isotherm models ranging from lagmuir, freundlich, BET, Temkin and Redlich- peterson were used during to analysed the fittness. Furthermore, based on the knowledged acquired so far, the process of studies on biosorption shuould further be widen in the light of Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(1), 91-102, January (2014) Res. J. Chem. Sci. International Science Congress Association 94 regeneration of bioadsorbents and recovery. Directional modeling, and disposal of the waste material in order to achieve high efficiency. Moreover, it is also observed that most of the studies were reported in batch process, and as such this will provide a room for continuous flow systems design with viable industrial applications, which can be more economical and efficient at commercial level. Having done this, we hope Such a strategy will fulfill the goal of a zero waste. Table-2 2003-2006 Biosorbent Q max(mg/g) pH Experimental Parameters/ Result Source T(C) (mg/l) T (min) AD (g/l) Best fitted model Modified polysaccharide 48 8 25 50 150 0.5 - 66 Mango seed kernel powder 142.86 8 30 100 0.02 L and K1 67 wheat shells 21.50 6.5 50 100 60 1.0 L 68 Neem leaf powder 8.76 5-8 30 40 240 2 L and F 69 jute fibre carbon: 22.5 5-10 28 50-200 250 1 L 70 Rice husk 40.58 8 32 100 40 0.12 L and K2 71 Giant duckweed 144.93 9 25 300 144 0.2 K1 72 Date pit 80.3 8 25 5 NA NA K2 and L 34 Wool Fibre (sheep wool) 94.3% 5 5g 30 1.0 F and L 73 Cotton Fibre 97% 5 3.5 10 1.50 Table-3 2007 Biosorbent Q max(mg/g) pH Experimental Parameters/ Result Source T( O C) C(mg/l) T (min) AD (g/l) Best fitted model Rattan sawdust 294.14 30 100-200 300 0.1 L and k2 74 Guava Seeds 198.12 8-8.3 500 40 L 75 Dehydrated wheat bran carbon 99.84 2.5 45 200 300 2 L and K2 76 bamboo-based activated carbon: 454.2 7 30 100-500 0.2 L and K2 77 Dehydrated peanut hull 161.30 3.5 50 400 150 1.0 L an K2 78 Paspalum notatum 31 8 30 100 300 1.33 L and K2 79 Rice husk (Coir pith carbon) 5.87 6.8 10-20 60 2 L 80 Wheat Bran 3.08 2.97 20-50 5-20 180 - K2 81 Table-3 2008 Biosorbent Q max(mg/g) pH Experimental Parameters/ Result Source T(C) C (mg/l) T (min) AD (g/l) Best fitted model Yellow passion fruit waste 44.70 7-10 25 28.7 2880 10 F,R,Land S. K1 and K3 82 leaf powder: 295 7.5 30 517 120 2 L and K2 83 Banana Stalk waste 243.90 4-12 30 50-500 330 1.0 L, F and T and K2 84 Hevea brasiliensis seed coat 227.27 30 50-500 300 0.1 F and K2 85 activated desert plant 23 3-8 24 150 65 4 NA 86 periwinkle shells 500 7 25 400-500 360 0.2 L and K2 87 Sesame stalk 502.68 NA NA NA 410 2 NA 88 Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(1), 91-102, January (2014) Res. J. Chem. Sci. International Science Congress Association 95 Table-4 2009 Biosorbent Q max(mg/g) pH Experimental Parameters/ Result Source T(C) C (mg/l) T (min) AD (g/l) Best fitted model Grass waste 457.64. 3-10 380 70 0.05–1.20 L and k2 89 Pummelo peel 390.6 8 30 300 30 2 L and K1 90 Gulmohar plant leaf powder 186.22 7.5 30 10-100 0.5-2.5 L and K2 91 Guava seed 0.10 6 25 50 0.03 - 92 Meranti sawdust 120.48 9-12 60 50-200 180 0.1-1.2 L and K2 93 Tea waste 85.16 4.3+0.2 27+2 20-50 300 0.2 L and K2 94 Garlic peel, 142.86 4-12 50 25–200 210 F and K2 95 Carica papaya seeds 1250 6.25 30 10 120 1.5 96 Pineapple stem waste 119.05 9 30 250 330 03 L and K2 97 Jackfruit peel 285.713 2-11 30 35-400 0.05-1.20 L and K2 98 Papaya seeds (PS) 555.557 3-10 30 50-360 0.05-1.0 L and K2 99 Water hyacinth 426.9 8 30 250 2.0 L 100 Hydrolyzed Oak sawdust 67.78 8 25 300 90 2.5 L and K2 101 Table-4 2010 Biosorbent Q max(mg/g) pH Experimental Parameters/ Result Source T (C) (mg/l) T (min) AD (g/l) Best fitted model Rhizopus arrhizus 370.3 10 25 50 240 1 F and K2 11 Rhizopus with SDS 1666.6 10 288.4 Brazil nut shells 7.81 3-10 30 1100 120 L and K2 102 Bamboo 286.1 3.7 25 400 1440 0.1 F, L and K2 103 Activated carbons from walnut shells 315 7.0 25 200 1440 0.75 R, L and F 104 Pretreated rice husk (RH) and rice husk ash (RHA) 1347.7 and 1455.6 7 150 NA 30 NA L and F 105 Modified sugarcane bagasse 115.3 8 106 Walnut shells via vacuum chemical activation 315 177 0.75 R, L and F 107 Algal biomass 860 4 -10 L 108 Treated sawdust 263.16 7 25 300 480 0.2 L and K2 109 Activated carbon 8.77 6.8 25 25 120 5.0 L and F 110 Table-4 2011 Biosorbent Q max(mg/g) pH Experimental Parameters/ Result Source T(C) (mg/l) T (min) AD (g/l) Best fitted model Date Stones and Palm-Tree Waste 43.47, 39.47 6.3 20-70 100 240 10 K2 111 NaOH modified rejected tea 242.11 7 30 50-100 0.5 L and K2 112 teak tree bark powder ( Tectonagrandis) 333.33 7 50 300 30 1 L ,F and K2 113 Cold plasma-treated and formaldehyde-treated onion skins 250, 166.67. 10 50 150 0.15 L and K1 114 oil palm (Elaeis) empty fruit bunch 344.8 2-12 30 200 15 0.1 L 115 Date stones 316.11 2-12 30 300 8 0.1 F, L and T 116 cotton stalk 111.3586 7 35 ± 2 825 120 4 L and K2 117 sulphuric acid treated cotton stalk 381.68 7 35 ± 2 4 F and K2 and phosphoric acid treated cotton stalk 242.13 7 35 ± 2 4 L and K2 peanut husk 72.13 80 20 NA L and K2 118 lotus leaf 221.7 7 20 50-150 1 L, F and Koble–Corrigan 119 palm kernel fibre 95.4 10-11 55 20-160 60 0.4 L, F and T 120 Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(1), 91-102, January (2014) Res. J. Chem. Sci. International Science Congress Association 96 Table-4 2012 Biosorbent Q max(mg/g) pH Experimental Parameters/ Result Source T(C) (mg/l) T (min) AD (g/l) Best fitted model Pink Guava 250 30 50–500 300 - L and K2 121 Alkali-modified malted sorghum mash 357.1 7.3 33 18 0.1 L 122 sugar extracted spent rice biomass 8.13 5.2 25 50 0.5 L and K2 123 Water Hyacinth Root Powder 8.04 8 20-10 80 1 L,F and K2 4 Date stones 398.19 7 30 450 270 0.5 S and K2 124 Oil palm shell 133.13 30 150 10 TY 125 Swede rape straw 246.4 L 126 bio-char from pyrolysis of wheat straw 12.03 8-9 20 100 50 S 127 Table-4 2013 Biosorbent Q max(mg/g) pH Experimental Parameters/ Result Source T(C) (mg/l) T (min) AD (g/l) Best fitted model Pea shells (Pisum sativum) 246.91 2 and 11.5 25 100-350 180 1 L 128 coconut husk 500 7.8 30 100-200 30 o.o3 L and K2 129 papaya leaf 231.65 2-10 30 200 300 L 130 Coconut fiber 50 0.6 131 untreated Alfa grass 200 12 20 10–150 180 0.25–12.5 L and K2 132 Neem leaf powder (Azadirachta indica) activated NLP and NLP 401.6 , 352.6 7 87 200 60 3 F and K2 133 Corn husk byZnCl2 activation(CHACZ) 662.25 4 25 50 120 0.4 F 134 HCl Treated SawDust (Lagerstroemia microcarpa): 229.8 30 50-200 360 1.0 L and K2 135 sugarcane bagasse: 95.19% NA 72 0.18 NA 136 watermelon (Citrullus lanatus) 489.80 NA 30 50 30 0.5 L and K2 137 Artocarpus odoratissimus (Tarap) skin 184.6 4.4 0.577 2010 L ,S and K2 138 Sugarcanebagasse: 95.19% 8.76 25 72 193 0.19 Na 139 Fallen leaves of platanus 145.62 7 50-500 300 0.5 Te, L andF and Ho 140 Pine sawdust 16.75 35 20-50 180 L and F 141 ConclusionBased on the literature reviewed so far, it is evident that, recently, there has been an increase in production and utilization of dyes, resulting in an increase in environmental pollution. Various techniques have been utilized in the removal of dyes. However, practically a successful methodology for removal of all types of dyes at low cost has not been established. The results of the literatures above and methods employed during the researches lead to a conclusion that for removal of MB using bio-materials, a collection or combination of different processes involving adsorption yields a rewarding results, but it is also observed that there exist some drawback in biosorption as the cost becomes higher when it is activated. Moreover, despite their upright efficiency and applicability, an economic consideration has restricted the use of some varieties, because Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(1), 91-102, January (2014) Res. J. Chem. Sci. International Science Congress Association 97 substantial amount of adsorbent is loss during regeneration processes. Treatment of industrial wastewater has gained so much importance in recent years, regulations become stricter and researchers have shown clearly for many years, its health, safety and environmental problems if not properly treated before final discharge. Finally, from the data available in literatures, these suggest that MB removal can be achieved to some extent by low cost adsorbent, as some have advantages where by many of them are renewable and available natural resources which are currently under use. References1.Alkan M., Demirbas O., CelikcΈapa S., Dogan M., Sorption of acid red 57 from aqueous solutions onto sepiolite, J Hazard. 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