Research Journal of Recent Sciences ________________________________________________ ISSN 2277 - 2502 Vol. 1(ISC-2011), 434-443 (2012) Res.J.Recent.Sci. Review Paper Recovery of Nickel from Spent Ni/Al2O3 Catalysts using Acid Leaching, Chelation and Ultrasonication Oza R.* and Patel S. Chemical Engineering Department, Institute Of Technology, Nirma University, Ahmedabad–382 481, INDIA Available online at: www.isca.in (Received 7th November 2011, revised 13th January 2012, accepted 30th March 2012) Abstract Supported nickel catalysts, containing 2.5% to 20% of nickel metal, are widely used in chemical industry for hydrogenation, hydrotreating, and steam-reforming reaction. These catalysts have specific life and are subsequently discarded due to its deactivation owing to coke deposition on its surface. Disposal of spent catalyst is a problem as it falls under the category of hazardous industrial waste and also it requires compliance with stringent environmental regulations. Also the cost and demand of nickel has been rising significantly. In this context recovery of nickel can serve both of the important issues. This review cum research work focuses on the recovery of nickel from spent nitrogenous catalyst using conventional acid leaching & chelation route and a novel technique Ultrasonication developed & implemented successfully by the authors. Using ultrasonication technique significantly faster recovery of nickel salt (50 minutes) was accomplished compared to chelation route (7-8 h) and acid leaching (5-6 h). The %recovery and purity is significantly high for ultrasonication route compared to conventional acid leaching and chelation technique. The recovered nickel salts can be recycled for the preparation of fresh catalysts and promises to be a good industrial process for handling 1-2 t per batch of spent nickel catalyst. Keywords: Spent catalyst, ultrasonication, chelation, leaching, nickel recovery. References 1. Singh B., Treatment of spent catalyst from the nitrogenous fertilizer industry - A review of the available methods of regeneration, recovery and disposal, J. Hazard. Mater., 167(1-3), 24-37 (2009) 2. Oza R. Shah N. and Patel S., Removal of Nickel from Spent Catalysts using Ultrasonication Assisted Leaching, J. Chem. Technol. Biotechnol., 86(10), 1276-1281 (2011) 3. Oza R. Shah N. and Patel S., Nickel Recovery from Spent Ni/Al2O3 Catalysts using Nitric Acid Solution, Asian J. Water, Environ. Pollut,. 8(3), 29-35 (2011) 4. Oza R. Shah N. and Patel S., Extraction of Nickel from Spent Catalyst using EDTA as Chelating Agent, Nat. Environ. Pollut. Technol., 10(2), 197-200 (2011) 5. Vuyyuru K. R. Pant K. K. Krishnan V. V. and Nigam K. D. P., Recovery of Nickel from Spent Industrial Catalysts Using Chelating Agents, Ind. Eng. Chem. Res., 49(5), 2014– 2024 (2010) 6. Kolosnitsyn V. S. Kosternova S. P. Yapryntseva O. A. Ivashchenko A. A. and Alekseev S. V., Recovery of nickel with sulfuric acid solutions from spent catalysts for steam conversion of methane, Russian J. Appl. Chem., 79, 539–543 (2006) 7. Ivascan S. and Roman O., Nickel recovery from spent catalyst. I Solvation process, Bu1 Inst Politeh Iasi Sect 22, 47–51 (1975) 8. Sinka G. Vigvari M. Koracsi G. Legal T. Gyalasi I. and Gabor G., Recovery of Ni from spent catalyst, Hung Teljes HU, 46, 556 (1988) 9. Al-Mansi N. M. and Abdel Monem N. M., Recovery of nickel oxide from spent catalyst, Waste Manage., 22, 85–90 (2002) 10. Pamela A. Mukharjee T. K. and Sundaresan A. M., Reduction roasting – sulphuric acid leaching of nickel from a spent catalyst, Metal Mineral. Process., 3, 81–92 (1991) 11. Sahu K. K. Agarwal A. and Pandey B. D., Nickel recovery from spent nickel catalyst, J. Waste Manage. Res., 23, 148–154 (2005) 12. Matkovic V. Markovic B. Sokic M. and Vuckovic N., Recycling of spent nickel based catalysts, Acta Metallurgica Slovaca., 12, 284–288 (2006) 13. Chaudhary A. J. Donaldson J. D. Boddington S. C. and Grimes S.G., Heavy metals in environment: part II. A hydrochloric acid leaching process for the recovery of nickel value from a spent catalyst, Hydrometall., 34,137–150 (1993) 14. Bosio V. and Vierra M. and Donati E., Integrated bacterial process for the treatment of a spent nickel catalyst, J. Hazard. Mater., 154(1-3), 804-810 (2008) 15. Santhiya D. and Ting Y., Bioleaching of spent refinery processing catalyst using Aspergillus niger with high-yield oxalic acid, J. Biotechnol., 116(2), 171-184 (2005) 16. Shinohara Y. and Mitsuhasli M., Leaching of valuable metal in waste desulfurization catalyst, Japan kokai, 76 82–86 (1976) 17. Floarea O. Mihai M. Morarus M. Kohn D. and Sora M., Filtration: physical models and operating conditions, Rev Chim (Bucharest), 42 553 (1991) 18. Vicol M. Heves A. and Potoroaca M., Recovery of nickel from spent catalysts, CombinatuldeIngrasaminteChimicePiatraNeamt, 112, 832 (1986) 19. Manoliu C. Olara I. Zugravescu P. Serdaru M. and Popescu E., Metal recovery from spent Ni/AlO3 catalyst, Rom. Ro., 87, 980 (1985) 20. Ghanem R. Farag H. Eltaweel Y. and Ossman E., Recovery of nickel from spent catalyst by single and multi-stage leaching process, Int. J. Environ. Waste Manag., 2(6), 540–548 (2008) 21. Molnar L. Sinka G. Szentgyorgyi G. and Lukacs P., Ni recovery from spent hydrocracking catalyst, Hung Teljes HU, 46, 565 (1988). 22. Kitakatsu N. Maurice V. Hinnen C. and Marcus P., Surface hydroxylation and local structure of NiO thin films formed on Ni(111), Surf. Sci., 407(1-3), 36-58 (1998) 23. Kitakatsu N. Maurice V. and Marcus P., Local decomposition of NiO ultra-thin films formed on Ni(111), Surf. Sci., 411(1-2), 215 (1998) 24. Jesus J. C. Carrazza J. Pereira P. and Zaera F., Hydroxylation of NiO films: the effect of water and ion bombardment during the oxidation of nickel foils with O2 under vacuum, Surf. Sci., 397(1-3), 34-47(1998) 25. Christel L. Pierre A. and Abel D. A-M. P., Temperature programmed reduction studies of nickel manganite spinels, Thermochim Acta., 306(1-2), 51-59 (1997) 26. Richardson J. T. Scates R. and Twigg M. V., X-ray diffraction study of nickel oxide reduction by hydrogen, Appl. Catal. A:Gen., 246(1), 137-150 (2003) 27. Sharma S. K. Vastola F. J. Walker P. L. Jr., Reduction of nickel oxide by carbon: I. Interaction between nickel oxide and pyrolytic graphite, Carbon., 34(11), 1407-1412 (1996) 28. Liu S. Xu L. Xie S. Wang Q. and Xiong G., Partial oxidation of propane to syngas over nickel supported catalysts modified by alkali metal oxides and rare-earth metal oxides, Appl. Catal. A:Gen., 211(2), 145-152 (2001) 29. Sehested J. Carlsson A. Janssens T. V. W. Hansen P. L. and Datye A. K., Sintering of Nickel Steam-Reforming Catalysts on MgAl2O4 Spinel Supports, J. Catal., 197(1), 200-209 (2001) 30. Pfender E., Thermal Plasma Technology: Where Do We Stand and Where Are We Going?, Plasma Chem. Plasma Process, 19(1), 1-31 (1999) 31. Tanahashi N. Takeuchi A. and Tanaka K., Metal Recovery From the Waste MagnesiaChromia Bricks With Arc Plasmas, J. Eng. Res. Technol., 123(1), 76-80 (2001) 32. Chatterjee P. K, Datta A. B and Kundu K. M., Fluidized bed gasification of coal, Can. J. Chem. Eng., 73(2), 204-210 (1995) 33. Herguido J. Corella J. and Gonzalez-Saiz J., Steam gasification of lignocellulosic residues in a fluidized bed at a small pilot scale. Effect of the type of feedstock, Ind. Eng. Chem. Res., 31(5), 1274-1282 (1992) 34. Judd M. R., In: 2nd International Coal & Gas Conversion Conference, Pretoria, 23 (1987) 35. Liu S. Xiong G. Yang W. Xu L. Xiong G. and Li C., Partial oxidation of ethane to syngas over nickel‐based catalysts modified by alkali metal oxide and rare earth metal oxide, Catal. Lett. 63(3-4), 167-171 (1999) 36. Huff M. Torniainen P. M. and Schmidt L.D., Partial oxidation of alkanes over noble metal coated monoliths, Catal. Today, 21(1), 113- 128 (1994) 37. Wong F. F. Lin C. M. Chang C. P. Huang J. R. Yeh M. Y. and Huang J. J., Recovery and Reduction of Spent Nickel Oxide Catalyst via Plasma Sintering Technique, Plasma Chem. Plasma Process., 26(6), 585-595 (2006) 38. Fischer K. Bipp H. P. Riemschneider P. Leidmann P. Bieniek D. and Kettrup A., Utilization of biomass residues for the remediation of metal-polluted soils, Environ. Sci. Technol., 32(14), 2154–2161 (1998) 39. Steele M.C. and Pichtel J., Ex-situ remediation of a metal contaminated superfund soil using selective extractants, J. Environ. Eng., 124(7), 639–645 (1998) 40. Papassiopi N. Tambouris S. and Kontopoulos A., Removal of heavy metals from calcareous contaminated soil by edta leaching, Water Air Soil Pollut., 109(1-4), 1–15 (1999) 41. Garrabrants A. C. and Kosson D. S., Use of a chelating agent to determine the metal availability for leaching from soils and wastes, Waste Manage., 20(2-3), 155–165 (2000) 42. Kim C. and Ong S. K., Recycling of leadcontaminated EDTA wastewater, J. Hazard. Mater., 69(3), 273–286 (1999) 43. Wasay S. A. Barrington S. and Tokunaga S., Organic acids for the in situ remediation of soils polluted by heavy metals: soil flushing columns, Water Air Soil Pollut., 127(1-4), 301–314 (2001) 44. Bergers P. J. M. and de Groot A. C., The analysis of EDTA in water by HPLC, Water Res., 28(3), 639–642 (1994). 45. Kari F. G. and Giger W., Modeling the photochemical degradation of ethylenediaminetetraacetate in the river Glatt, Environ. Sci. Technol., 29(11), 2814–2827 (1995) 46. Goel S. Nigam K. D. P and Pant K, K,, Extraction of Nickel from spent catalyst using fresh and recovered EDTA, J. Hazard. Mater., 171(1-3), 253-261 (2009) 47. Vadamalar R. Mani D. and Balakrishnan R., Ultrasonic Study of Binary Liquid Mixtures of Methyl Methacrylate with Alcohols, Res.J.Chem.Sci., 1(9), 79-82 (2011) 48. Mason T.J., Advances in Sonochemistry, Elsevier Science Publishers, New York, 1–6 (1990–2001) 49. Suslick K. S., Ultrasound: its Chemical, Physical and Biological Effects. VCH, New York (1988) 50. Crum L. A., Mason T.J., Reisse J. and Suslick K. S., Sonochemistry and Sonoluminescence, Kluwer Academic Publishers (1999)