Available online at http://www.urpjournals.com International Journal of Research in Pure and Applied Microbiology Universal Research Publications. All rights reserved ISSN 2277–3843 Original Article BIOADSORPTION OF THE TOXIC HEAVY METAL CHROMIUM BY USING Pseudomonas putida R.Sadeeshkumar1*, P.Saranraj2 and D.Annadurai3 1,3 Centre of Advanced Study of Marine Biology, Annamalai University, Parangipettai – 608 502, Tamil Nadu, India. 2 Department of Microbiology, Annamalai University, Chidambaram – 608 002, Tamil Nadu, India. E.mail: sadeesh86@gmail.com Received 11 September 2012; accepted 27 September 2012 Abstract Elimination of heavy metals from industrial wastewater is important for preserving the quality of aquatic systems, streams, and groundwaters. Contaminated waters are generally cleaned by precipitation of a metallic oxyhydroxide sludge or by ion exchange with synthetic resins. Various types of nonliving biomass, bacteria, filamentous fungi, algae and higher plants can be profitably used in alternative metal removal processes because of their low cost and the high ion exchange capacity of cell walls. Bioadsorption, bioaccumulation and enzymatic reduction are the processes by which the microorganisms interact with the toxic metals, enabling their removal or recovery. In the present study, a bacterial strain was isolated from tannery effluent and identified as Pseudomonas putida. It showed a high level resistance of 800 µg/ml chromium. The minimal inhibitory concentration of chromium was found to be 512 µg/ml of potassium dichromate in Nutrient broth medium. The chromium adsorption was more significant by the live cells than killed cells at different time intervals. It was observed that, the inoculation of Pseudomonas putida reduced the BOD and COD values of tannery effluent. © 2011 Universal Research Publications. All rights reserved Key words: Tannery effluent, Chromium, Bioadsorption and Pseudomonas putida. 1. INTRODUCTION Industrial pollution has been and continues to be a major factor causing the degradation of the environment around us, affecting the water we use, the air we breathe and the soil we live on. But of these, the pollution of water is arguably the most serious threat to current human welfare. Water is polluted not only by industries but also by households. Both industries and household wastewater contain chemicals and biological matter that impose high demands on the oxygen present in water. Polluted water thus contains low levels of dissolved oxygen as a result of the heavy biological oxygen demand (BOD) and chemical oxygen demand (COD) placed by industrial and household waste materials discharged into water bodies and water systems, both above and below the earth’s surface. In addition to low levels of dissolved oxygen in water, industrial wastes also contain chemicals and metals that are directly harmful to human health and the ecosystem. The pollution of the aquatic environment with heavy metals has become a worldwide problem during recent years, because they are indestructible and most of them have toxic effects on organisms [1]. Among environmental pollutants, metals are of particular concern, due to their potential toxic effect and ability to bioaccumulate in aquatic ecosystems [2]. 32 Tanning is a process of making leather from skin and hides. The process involves a complex combination of mechanical and chemical practices as a result of which organic and inorganic materials become chemically bound to the protein component of the hides and preserve it from deterioration. A significant number of operations within a tannery industry are wet operations consuming large amounts of water, chemicals and energy leading to large amounts of polluted water. Leather industries and tanneries generate massive by-products, solid wastes, high amounts of wastewater rich in organic wastes with different loads of pollutants and emissions into the air. Majority of tanneries worldwide use chromium salts which are highly toxic and possess a serious threat to the environment upon improper disposal of their wastewaters. Even in low concentrations, these salts have a toxic effect upon daphnia, thus disrupting the food chain for fish life and possibly inhibiting photosynthesis of aquatic plants [3]. Effluents from raw hide processing tanneries contain compounds of Cr III and sulphides in most cases with a major proportion of dyes. Release of these effluents into aquatic ecosystems alters the pH, increases the BOD and COD and gives the water intense colourations [4]. However, the toxicity of effluents depends on operations employed in each tannery. International Journal of Research in Pure and Applied Microbiology 2012; 2(4): 32-36 Chromium, a priority pollutant is well known for its mutagenicity, carcinogenicity and teratogenicity in humans, experimental animals and plants. Extensive use of chromium in industries such as leather tanning, stainlesssteel production, electroplating and wood preservatives have resulted in chromium contaminated soil and ground water at production sites [5] which pose a serious threat to human health. The hexavalent chromium compounds are comparatively more toxic than trivalent chromium compounds due to their higher solubility in water, rapid permeability through biological membranes and subsequent interaction with intracellular proteins and nucleic acids [6]. A maximum acceptable concentration of 0.05 mg/l for hexavalent chromium in drinking water has been established on basis of health considerations. However, its high toxicity, mutagenicity and carcinogenicity renders it hazardous even at very low concentration. In general, treatment of effluents includes physiochemical methods such as filtration, specific coagulation, use of activated carbon and chemical flocculation [7]. Conventional treatment of tannery effluents for the purpose of detoxification requires application of physical and chemical methods which involves the chrome precipitation and sulphide treatment. Due to associated problems in these treatments such as cost and intense experimental set-up [8, 9], biological treatment methods using various bacteria and fungi have been widely studies. Recent developments in biology have provided new tools and approaches for monitoring the environment and engineering organisms with the capacity to degrade environmental pollutants. Different types of organisms can be bioremediation agents. Considering the enormous biodiversity and biological wealth in this country, basic research and modern biology, product oriented research for new generation of vaccines, diagnostics, recombinant products and other bio products specially the eco-friendly technologies would be the priority agenda for future. The present study is focused on isolation, identification of chromium resistant Pseudomonas putida and its ability to remove chromium contaminants in tannery effluents. 2. MATERIALS AND METHODS 2.1. Sample collection Tannery effluents were collected from leather industry at Aambur in Vellore district. The sample was collected after the primary treatment in Leather industry. 2.2. Isolation and identification of Pseudomonas putida from Tannery effluent The tannery effluent sample was taken and diluted in water and was isolated by Serial dilution technique followed by Spread plate method. The isolated colony was sub-cultured in Minimal salt agar medium supplemented with hexavalent chromium 100µg/ml (hexavalent chromium was supplemented in the form of potassium dichromate) and also in Nutrient agar with Potassium dichromate medium 50mg/100ml, and incubated at 37°C for 2 days. Identification of the bacterial isolates was carried out by the routine bacteriological methods i.e., By the colony morphology, preliminary tests like Gram staining, motility, plating on selective medias and performing biochemical tests. 33 2.3. Evaluation of chromium tolerance The isolated bacterium (Pseudomonas putida) was tested for their resistance to chromate both by Agar dilution method and Broth dilution method. 2.3.1. Agar dilution method The test organism inoculating into Nutrient broth and incubated at 37°C in a shaker incubator at 150 rpm till the concentration of the test organisms matched with 0.5 McFarland standards. In this method, Pseudomonas putida was aseptically streaked into freshly prepared Nutrient agar plates amended with hexavalent chromium as dichromate at various concentrations ranging from 100 – 1500 µg/ml. Plates were then incubated at 37°C for 24 hours. 2.3.2. Broth dilution method The test organism was inoculated into Nutrient broth and incubated at 37°C in a shaker incubator at 150 rpm till the concentration of the test organisms matched with 0.5 McFarland standard. A stock solution of chromium was prepared (50 mg/100ml). Two fold dilutions of this solution were prepared in Nutrient broth medium. A standard suspension of Pseudomonas putida was inoculated onto the medium with one control chromium solution free medium. The inoculated medium was then incubated at 37°C for 24 hours. 2.4. Bioadsorption studies 2.4.1. Estimation of standard chromium: (Diphenyl carbazide method) A standard curve for the reaction between chromium and its binding dye, 1,5 – diphenyl carbazide was added to determine the chromium concentration. The diphenyl carbazide forms a pink complex with hexavalent chromium but not with trivalent chromium. [10]. 50 mg of potassium dichromate was dissolved in 100 ml of sterile distilled water, in standard flask. From this standard, 0.02, 0.04, 0.06, 0.08 and 0.1 ml of chromium was added into different tubes, then the volume was made upto 2 ml. 2 ml of distilled water was taken as blank. To all the above tubes, 0.04 µl of diphenyl carbazide and one drop of sulphuric acid were added and the residual hexavalent chromium content was determined at 540nm in colorimeter. 2.4.2. Chromium uptake 24 hours old culture of Pseudomonas putida was prepared in Nutrient broth. To 50 ml of Nutrient broth, 50 µg/ml of potassium dichromate was added and sterilized. Similarly another set was prepared. To the first set, 10 ml of overnight broth culture i.e., live cells were added. To the second set, 10 ml of 24 hours culture was autoclaved at 121ºC for 15 minutes i.e., killed cells was added. From above, 10 ml of samples were removed at different time intervals and centrifuged at 8000 rpm for 20 minutes. Then the pellet obtained was homogenized in 2 ml of phosphate buffer. To this 0.04 µl of diphenyl carbazide and one drop of sulphuric acid was added to the homogenate. Chromium uptake was estimated using diphenyl carbazide method at 540 nm in colorimeter. 2.4.3. Chromium reduction Reduction of chromium was determined by growing the Pseudomonas putida in Nutrient broth supplemented with hexavalent chromium as dichromate at a concentration of 50 µg/ml. Cells were grown on a shaker incubator (150 International Journal of Research in Pure and Applied Microbiology 2012; 2(4): 32-36 rpm) for 24 hours. Supernatant obtained after centrifugation was used for chromate reductase assay. Chromate reductase activity was estimated as the decrease in chromium concentration with time using hexavalent chromium specific colorimetric reagent 1,5-diphenyl carbazide (DPC) 0.5% (vol/vol) prepared in acetone. To 1 ml of supernatant, 1 ml of phosphate buffer (pH 7.2) with chromium was added and incubated for 1 hour. After incubation, 1 drop of 0.1 M sulphuric acid and 0.04 µl of 1,5 diphenyl carbazide was added. The readings were taken in colorimeter (540nm). 2.5. Physico-chemical analysis of tannery effluent Physico-chemical characteristics of tannery effluent was analyzed before and after treatment. 3. RESULTS AND DISCUSSION Hexavalent chromium [Cr(VI)] has many industrial applications and often causes environmental contamination in marine and freshwater sediments from urban and industrial discharges. Chromate is a strong oxidizing agent that is reduced intracellularly to Cr 5+ and reacts with nucleic acids and other cell components to produce mutagenic and carcinogenic effects on biological systems [11]. Although reduction to Cr5+ is responsible for chromate toxicity, further reduction to trivalent chromium leads to the formation of stable, less soluble, and less toxic Cr (III). Reduction of Cr (VI) to Cr (III) is therefore a potentially useful process for remediation of Cr (VI)-affected environments [12]. Bioreduction of Cr (VI) can occur directly as a result of microbial metabolism (enzymatic) or indirectly, mediated by a bacterial metabolite. A number of chromium-resistant microorganisms have been reported, including Pseudomonas spp. [13], Microbacterium [14], Desulfovibrio, Enterobacter spp., Escherichia coli, Shewanella alga [15], Bacillus sp. [16], and several other bacterial isolates [17]. However, most of them have been isolated from tannery sludge, industrial sewage, evaporation ponds, or discharge water, or were purchased from culture collections. With the increasing demand for leather and leather products, both for indigenous use as well as for export, large number of vegetable and chrome tanneries have mushroomed in India, especially in states like Tamil Nadu, Uttar Pradesh and West Bengal. Tannery wastewater is characterized by its strong colour, high COD, high BOD, and TDS. The levels of pollutants in tannery wastewater also vary depending upon the process adopted in leather making. The unplanned manner in which these units have come up forces to think about their disposal of liquid effluents. The quality of discharged waters from tanneries is far from the desired level of acceptance into waterways. As a result, the tanneries are forced to construct a Common Effluent Treatment Plant (CETP). Tamil Nadu Pollution Control Board accorded permission to resume the operation of those tanneries, which put up full-fledged Effluent Treatment Plant (ETP) or CETP. The treatment of tannery effluent depends on the efficiency with which the CETP functions. Hence, the continuous evaluation is a prerequisite for up keeping of efficiency with which the CETP functions [18]. The chromium resistant bacterium from tannery effluent 34 was identified by preliminary tests, cultivating on selective media and standard biochemical tests. Based on the conventional biochemical tests, the organism was identified as Pseudomonas aeruginosa. The isolation of chromium resistant bacteria from tannery effluents and identified as Brevibacterium sp. and Brucella sp. respectively. In Agar dilution method, the bacterial isolate (Pseudomonas putida) was resistant to hexavalent chromium level at 800 µg/ml. Above 800 µg/ml of chromium, the growth was inhibited. In Broth dilution method, the bacterial isolate (Pseudomonas putida) was resistant to hexavalent chromium level at 512 µg/ml. Growth was inhibited at above 512 µg/ml of hexavalent chromium level. Shahida Hasnain and Indu Shekhar Thakur [19] found that Brevibacterium sp. showed high level – resistance of chromium upto 40 mg/ml by Agar dilution method. Megharaj and Naidu [20] examined that Bacillus sp. tolerated hexavalent chromium at 100 mg/ml on a minimal medium supplemented with 0.5% glucose. Table-1: Estimation of standard chromium by Diphenyl carbazide method Concentration of chromium Optical density (in µg) (in nm) 10 0.30 20 0.60 30 0.90 40 1.20 50 1.50 In this study, the standard chromium was estimated by Diphenyl carbazide method and the results were showed in Table – 1. Bioadsorption studies were done to test the ability of cells (both live and dead cells) to accumulate chromium at different time intervals 15 minutes, 5 and 24 hours. The results were shown in Table-2. The living cells accumulated 22, 30 and 38 µg/ml of chromium and the killed cells accumulated 8, 10 and 10 µg/ml of chromium. The rate of chromium accumulation was rapid. It showed that the living cells exhibited better chromium uptake compared to heat killed cells. The ability of Pseudomonas putida to reduce chromium at different time intervals 15, 30 and 60 minutes was 19, 18 and 18 µg/ml of chromium. Pseudomonas putida has not shown significant chromium reduction in the supernatants. Kader et al. [21] showed that the rate of chromium accumulation by active cells was also faster compared to chromium reduction. The maximum amount of chromium accumulated by consortia was 6.4 mg/L and the reduction of chromium was 1.8 mg/L. Shahida Hasnain and Indu Shekhar Thakur [22] found that Brevibacterium sp. living cells pellet showed higher chromium uptake than killed cells pellet when time intervals increased. Table – 2: Estimation of Chromium uptake Time (in hours) 15 minutes 5 24 Chromium uptake in whole cells (µg) Live pellet Killed pellet 22 8 30 10 38 10 The ability of Pseudomonas putida to reduce chromium at different time intervals 15, 30 and 60 minutes was 19, 18 International Journal of Research in Pure and Applied Microbiology 2012; 2(4): 32-36 Table-3: Estimation of chromium reduction Time Reduction of chromium level in (Min) supernatant (µg) 15 19 30 18 60 18 and 18 µg/ml of chromium and the chromium reduction is showed in Table -3. Pseudomonas putida has not shown significant chromium reduction in the supernatants. Kader et al. [23] showed that the rate of chromium accumulation by active cells was also faster compared to chromium reduction. The maximum amount of chromium accumulated by consortia was 6.4 mg/L and the reduction of chromium was 1.8 mg/L. Shahida Hasnain and Indu Shekhar Thakur [24] found that Brevibacterium sp. living cells pellet showed higher chromium uptake than killed cells pellet when time intervals increased. Physico-chemical analysis of tannery effluent was analyzed before and after treatment. After the inoculation of Pseudomonas putida in tannery effluents, the pH of the tannery effluents was brought down from 11.6 to7.The BOD mg/lit of the tannery effluents was reduced from 8000 to 6400. The COD mg/lit of the tannery effluents was reduced from 5000 to 2500. Chromium content level was reduced from 38 µg- 25 µg/ml. Duangporn Kantachote et al. [25] identified the reduction of biological oxygen demand in tannery effluents from 4967 mg/L to 1010 mg/ml after inoculation of Rhodopseudomonas blastica. He also found the reduction of chemical oxygen demand from 7328 mg/L to 3371 mg/L in tannery effluents. Saranraj et al. [26] isolated a bacterial strain from tannery effluent and identified as Enterococcus casseliflavus. It showed a high level resistance of 800 µg/ml chromium. The minimal inhibitory concentration of chromium was found to be 512 µg/ml of potassium dichromate in Nutrient broth medium. The chromium adsorption was more significant by the live cells than killed cells at different time intervals. It was observed that, the inoculation of Enterococcus casseliflavus reduced the BOD and COD values of tannery effluent. The maximum adsorption of chromium was at a temperature of 35ºC to 45ºC and at a pH of 7.0 to 7.5. 4. CONCLUSION The chromium uptake from tannery effluents was significantly found in live pellet cells than killed pellet cells of Pseudomonas putida. Irrespective of the pH of the tannery effluent, Pseudomonas putida has shown significant chromium adsorption by bringing down the pH of tannery effluent to neutral pH 7. Application of traditional wastewater treatment requires enormous cost and continuous input of chemicals which becomes uneconomical and causes further environmental damage. Hence easy effective economical and ecofriendly techniques such as utilization of bacteria can be applied for fine tuning of wastewater treatment. 5. REFERENCE 1) MacFarlane, G. B. Ajayi, S.O., Osibanjo, O. 1980. The state of environment in Nig. Pollution studies of textile industries in Nigeria. Monogra, 1: 76-86. 35 2) Burchettt, M. D. 2000. Cellular distribution of Cu, Pb, and Zn in the Grey Mangrove Avicemnia marina (Forsk.). Vierh Aquatic Botanic, 68: 45–59. 3) Censi, P., Spoto, S. E., Saiano, F., Sprovieri, M., Mazzola, S., Nardone, G., Di Geronimo, S. I., Punturo, R., Ottonello, D. 2006. Heavy metals in coastal water systems. A case study from the Northwestern Gulf of Thailand. Chemosphere, 64: 1167–1176. 4) Bosnic, M., Buljan, J., Daniels, R.P. 2000. Pollutants in tannery effluents. United Nations Industrial Development Organization: 1-26. 5) Turick and Carmiol. 1996. Isolation of Cr VI reducing anaerobes from Cr contaminated and non contaminated areas. Applied Biotechnology and Microbiology, 44(5): 683-688. 6) Sultan and Hasnain. 2005. Isolation of hexavalent chromium-reducing Cr-tolerant facultative anaerobes from tannery effluent. Journal of General Applied Microbiology, 47: 307-312. 7) Olukanni, O.D., Osuntoki, A.A and Gbenle, G.O. 2006. Textile effluent biodegradation potentials of textile effluent-adapted and non-adapted bacteria. African Journal of Biotechnology, 5 (20): 1980-1984. 8) Do, T., Shen, J., Cawood, G., Jeckins, R. 2002. Biotreatment of textile effluent using Pseudomonas spp. Immobilized on polymer supports. In: Advances in biotreatment for textile processing. (Hardin, I.R; Akin D.E & Wilson J.S, eds). University of Georgia Press. 9) Maier, J., Kandelbauer, A., Erlacher, A., CavacoPaulo, A., Gubits, G.M. 2004. A new alkalithermostable azoreductase from bacillus sp. Strain SF. Applied Environmental Microbiology, 70:837-844. 10) Young Hak, Kwak and Han Bok Kim. 2003. Vibrio harveyi is also a chromate reductase. Applied Environmental and Microbiology, 69: 4390-4395. 11) McLean, J and T.J. Beveridge. 2001. Chromate reduction by a pseudomonad isolated from a site contaminated with chromated copper arsenate. Applied Environmental Microbiology, 67:1076–1084. 12) Michel, C., M. Brugma, C. Aubert, A. Bernadac, and M. Bruschi. 2001. Enzymatic reduction of chromate: Comparative studies using sulfate-reducing bacteria. Applied Microbiology and Biotechnology, 55:95–100. 13) Alvarez, A.H., R. Moreno-Sanchez, and C. Cervantes. 1999. Chromate efflux by means of the chrA chromate resistance protein from Pseudomonas aeruginosa. Journal of Bacteriology, 181:7398–7400. 14) Pattanapipitpaisal, P., N.L. Brown, and L.F. Macaskie. 2001. Chromate reduction and 16S rRNA identification of bacteria isolated from a Cr (VI)contaminated site. Applied Microbiology and Biotechnology, 57:257–261 15) Guha, H., K. Jayachandran, and F. Maurrasse. 2001. Kinetics of chromium (VI) reduction by a type strain Shewanella alga under different growth conditions. Environmental Pollution, 115: 209 – 218. 16) Campos, J., M. Martinez-Pacheco, and C. Cervantes. 1995. Hexavalent-chromium reduction by a chromateresistant Bacillus sp. strain. Antonie Van Leeuwenhoek, 68: 203–208. International Journal of Research in Pure and Applied Microbiology 2012; 2(4): 32-36 17) Holman, H.-Y.N., D.L. Perry, M.C. Martin, G. 1999. Real-time characterization of biogeochemical reduction of Cr (VI) on basalt surfaces by SR-FTIR imaging. Geomicrobiology Journal, 16: 307–323. 18) Prasad, B.G.S and B.V.S Gurunatha Rao. 1981. Studies on the treatment and disposal of tannery wastewater, Part 1, Leather Science, 28, 221. 19) Shahida Hasnain and Indu Shekhar Thakur. 2007. Evaluation of biosorption potency of Acinetobacter sp. for removal of hexavalent chromium from tannery effluent. Journal of Earth and Environmental Science, 18(5): 637-646.. 20) Megharaj and Naidu. 2003. Toxicity of Cr VI and its reduction by bacteria isolated from soil contaminated with tannery waste. Journal of Earth and Environmental Science, 47(1): 51-4. 21) Kader, P. Sannasi, O. Othman, B.S. Ismail and S. Salmijah. 2007. Removal of Cr (VI) from Aqueous Solutions by Growing and Non-growing Populations of Environmental Bacterial Consortia. Global Journal of Environmental Research, 1(1): 12-17. 22) Shahida Hasnain and Indu Shekhar Thakur. 2007. Evaluation of biosorption potency of Acinetobacter sp. 23) 24) 25) 26) Lamble, W.R. McKinney, and J.C. Hunter-Cevera. for removal of hexavalent chromium from tannery effluent. Journal of Earth and Environmental Science, 18(5): 637-646. Kader, P. Sannasi, O. Othman, B.S. Ismail and S. Salmijah. 2007. Removal of Cr(VI) from Aqueous Solutions by Growing and Non-growing Populations of Environmental Bacterial Consortia. Global Journal of Environmental Research, 1(1): 12-17. Shahida Hasnain and Indu Shekhar Thakur. 2007. Evaluation of biosorption potency of Acinetobacter sp. for removal of hexavalent chromium from tannery effluent. Journal of Earth and Environmental Science, 18(5): 637-646.. Duangporn Kantachote, Salwa Torpee, Kamontam Umsakul. 2005. The potential use anoxygenic phototrophic bacteria for treating latex rubber sheet wastewater. Electronic Journal of Biotechnology, 8(3): 11 – 17. Saranraj.P., Stella.D., Reetha.D and Mythili.K. 2010. Bioadsorption of chromium resistant Enterococcus casseliflavus isolated from tannery effluent. Journal of Ecobiotechnology, 2 (7): 17 – 22. Source of support: Nil; Conflict of interest: None declared 36 International Journal of Research in Pure and Applied Microbiology 2012; 2(4): 32-36