skip to main content

Utilization of the spent catalyst as a raw material for rechargeable battery production: The effect of leaching time, type, and concentration of organic acids

1Department of Chemical Engineering, Faculty of Industrial Technology, Parahyangan Catholic University, Bandung, Indonesia

2Research Unit for Mineral Technology, National Research and Innovation Agency, Tanjung Bintang, Indonesia

3Department of Chemical Engineering, Faculty of Engineering, Universitas Gadjah Mada, Yogyakarta, Indonesia

Received: 31 Dec 2022; Revised: 3 Feb 2023; Accepted: 24 Feb 2023; Available online: 24 Mar 2023; Published: 15 May 2023.
Editor(s): Rock Keey Liew
Open Access Copyright (c) 2023 The Author(s). Published by Centre of Biomass and Renewable Energy (CBIORE)
Creative Commons License This work is licensed under a Creative Commons Attribution-ShareAlike 4.0 International License.

Citation Format:
This study examines the potential use of the spent catalyst as a raw material for rechargeable batteries. The spent catalyst Ni/γ-Al2O3 still contains relatively high amounts of nickel. This indicates the potential use of the spent catalyst to be leached and purified for synthesizing nickel-based compounds so that it can be applied to rechargeable battery cathodes. In this study, the spent catalyst leaching process employed four types of organic acids: citric acid, lactic acid, oxalic acid, and acetic acid. The spent catalyst was leached under atmospheric conditions and room temperature. Organic acid concentrations were also varied at 0.1, 0.5, 1, and 2 M. The leaching process took place for 240 minutes, where sampling was conducted periodically at 30, 60, 120, 180, and 240 minutes. Experimental results showed that Ni (II) and Al (III) ions were successfully leached to the maximum when using 2M citric acids at a leaching time of 240 minutes. The conditions succeeded in leaching Ni (II) and Al (III) ions of 357.8 and 1,975.4 ppm, respectively. Organic acid, notably citric acid, has excellent potential for further development. Citric acid, as a solvent, has the ability to leach metal ions with high recovery. In addition, this acid is categorized as an eco-friendly and green solvent compared to inorganic acid. Thus, the leaching process can take place without harming the environment.
Fulltext View|Download
Keywords: Batteries; organic acid; spent catalyst; nickel; aluminum

Article Metrics:

  1. Allen, J. A. (1953). The precipitation of nickel oxalate. J. Phys. Chem., 57(7), 715–716.
  2. Angumeenal, A. R., & Venkappayya, D. (2013). An overview of citric acid production. LWT - Food Science and Technology, 50(2), 367–370;
  3. Arslanoğlu, H., & Yaraş, A. (2019). Recovery of precious metals from spent Mo–Co–Ni/Al2O3 catalyst in organic acid medium: Process optimization and kinetic studies. Petroleum Science and Technology, 37(19), 2081–2093;
  4. Ash, B., Nalajala, V. S., Popuri, A. K., Subbaiah, T., & Minakshi, M. (2020). Perspectives on nickel hydroxide electrodes suitable for rechargeable batteries: Electrolytic vs. chemical synthesis routes. Nanomaterials, 10(9), 1–22;
  5. Astuti, W., Hirajima, T., Sasaki, K., & Okibe, N. (2016). Comparison of effectiveness of citric acid and other acids in leaching of low-grade Indonesian saprolitic ores. Minerals Engineering, 85, 1–16;
  6. Astuti, W., Mufakhir, F. R., Setiawan, F. A., Wanta, K. C., & Petrus, H. T. B. M. (2022). Leaching characteristics of lanthanum from a secondary resource using inorganic and organic acids: Emphasizing the citric acid kinetics. Circular Economy and Sustainability;
  7. Behera, S. K., & Mulaba-Bafubiandi, A. F. (2015). Advances in microbial leaching processes for nickel extraction from lateritic minerals - A review. Korean Journal of Chemical Engineering, 32(8), 1447–1454;
  8. Behera, S. S., & Parhi, P. K. (2016). Leaching kinetics study of neodymium from the scrap magnet using acetic acid. Separation and Purification Technology, 160, 59–66.
  9. Benayed, A., Gasbaoui, B., Bentouba, S., & Soumeur, M. A. (2021). Movement of a solar electric vehicle controlled by ANN-based DTC in hot climate regions. International Journal of Renewable Energy Development, 10(1), 61–70;
  10. Chen, Y., & Nielsen, J. (2016). Biobased organic acids production by metabolically engineered microorganisms. Current Opinion in Biotechnology, 37, 165–172;
  11. Cheng, F., Liang, J., Tao, Z., & Chen, J. (2011). Functional materials for rechargeable batteries. Advanced Materials, 23(15), 1695–1715;
  12. Cui, Z., Xie, Q., & Manthiram, A. (2021). Zinc-doped high-nickel, low-cobalt layered oxide cathodes for high-energy-density lithium-ion batteries. ACS Applied Materials and Interfaces, 13(13), 15324–15332;
  13. Demarco, J., Cadore, J. S., Veit, H. M., Madalosso, H. B., Tanabe, E. H., & Bertuol, D. A. (2020). Leaching of platinum group metals from spent automotive catalysts using organic acids. Minerals Engineering, 159;
  14. Esmaeili, M., Rastegar, S. O., Beigzadeh, R., & Gu, T. (2020). Ultrasound-assisted leaching of spent lithium ion batteries by natural organic acids and H2O2. Chemosphere, 254, 126670;
  15. Gaber, M. A. F. M. (2019). Extraction of nickel from spent catalyst of primary reformer. Recent Advances in Petrochemical Science, 6(3), 64–69;
  16. Garole, D. J., Hossain, R., Garole, V. J., Sahajwalla, V., Nerkar, J., & Dubal, D. P. (2020). Recycle, recover and repurpose strategy of spent li-ion batteries and catalysts: Current status and future opportunities. ChemSusChem, 13(12), 3079–3100;
  17. General Chemistry Laboratory, Eastern Michigan University. (2018). Experiment 3: Analysis of aluminum (III) in water.
  18. Goel, S., Pant, K. K., & Nigam, K. D. P. (2009). Extraction of nickel from spent catalyst using fresh and recovered EDTA. Journal of Hazardous Materials, 171(1–3), 253–261;
  19. Golmohammadzadeh, R., Faraji, F., & Rashchi, F. (2018). Recovery of lithium and cobalt from spent lithium ion batteries (LIBs) using organic acids as leaching reagents: A review. Resources, Conservation and Recycling, 136, 418–435;
  20. Haar, K. T., & Westerveld, W. (1948). The colorimetric determination of nickel, as Ni(4) dimethylglyoxime. Recueil, 67, 71–81;
  21. Hosseini, S. A., Raygan, S., Rezaei, A., & Jafari, A. (2017). Leaching of nickel from a secondary source by sulfuric acid. Journal of Environmental Chemical Engineering, 5(4), 3922–3929;
  22. Khalid, M. M., & Athraa, B.A. (2017). Experimental study on factors affecting the recovery of nickel from spent catalyst. Journal of Powder Metallurgy & Mining, 6(1);
  23. Kiani, M. A., Mousavi, M. F., & Ghasemi, S. (2010). Size effect investigation on battery performance: Comparison between micro- and nano-particles of β-Ni(OH)2 as nickel battery cathode material. Journal of Power Sources, 195(17), 5794–5800;
  24. Le, M. N. L. & Lee, M. S. (2020). Separation of Al(III), Mo(VI), Ni(II), and V(V) from model hydrochloric acid leach solutions of spent petroleum catalyst by solvent extraction. Journal of Chemical Technology & Biotechnology, 95(11), 2886–2897;
  25. Li, L., Ge, J., Chen, R., Wu, F., Chen, S., & Zhang, X. (2010). Environmental friendly leaching reagent for cobalt and lithium recovery from spent lithium-ion batteries. Waste Management, 30(12), 2615–2621;
  26. Li, L., Qu, W., Zhang, X., Lu, J., Chen, R., Wu, F., & Amine, K. (2015). Succinic acid-based leaching system: A sustainable process for recovery of valuable metals from spent Li-ion batteries. Journal of Power Sources, 282, 544–551;
  27. Liang, Y., Zhao, C.-Z., Yuan, H., Chen, Y., Zhang, W., Huang, J.-Q., Yu, D., Liu, Y., Titirici, M.-M., Chueh, Y.-L., Yu, H., & Zhang, Q. (2019). A review of rechargeable batteries for portable electronic devices. InfoMat, 1(1), 6–32;
  28. Liu, Y., Pan, H., Gao, M., & Wang, Q. (2011). Advanced hydrogen storage alloys for Ni/MH rechargeable batteries. Journal of Materials Chemistry, 21(13), 4743–4755;
  29. Liu, R., Tian, Z., Cheng, H., Zhou, H., & Wang, Y. (2021). Organic acid leaching was an efficient approach for detoxification of metal-containing plant incineration ash. Environmental Science and Pollution Research, 28(25), 32721–32732;
  30. Maddu, A., Sulaeman, A. S., Wahyudi, S. T., & Rifai, A. (2022). Enhancing ionic conductivity of carboxymethyl cellulose-lithium perchlorate with crosslinked citric acid as solid polymer electrolytes for lithium polymer batteries. International Journal of Renewable Energy Development, 11(4), 1002–1011;
  31. Meshram, P., Pandey, B. D., & Mankhand, T. R. (2016). Process optimization and kinetics for leaching of rare earth metals from the spent Ni-metal hydride batteries. Waste Management, 51, 196–203;
  32. Meshram, P., Abhilash, & Pandey, B. D. (2018). Advanced review on extraction of nickel from primary and secondary sources. In Mineral Processing and Extractive Metallurgy Review, 40(3), 157–193;
  33. Oediyani, S., Ariyanto, U., & Febriana, E. (2019). Effect of concentration, agitation, and temperature of Pomalaa limonitic nickel ore leaching using hydrochloric acid. IOP Conf. Series: Materials Science and Engineering, 478(012013), 1–8;
  34. Pathak, A., Vinoba, M., & Kothari, R. (2020). Emerging role of organic acids in leaching of valuable metals from refinery-spent hydroprocessing catalysts, and potential techno-economic challenges: A review. Critical Reviews in Environmental Science and Technology, 51(1), 1–43;
  35. Ramos-Cano, J., González-Zamarripa, G., Carrillo-Pedroza, F. R., Soria-Aguilar, M. D. J., Hurtado-Macías, A., & Cano-Vielma, A. (2016). Kinetics and statistical analysis of nickel leaching from spent catalyst in nitric acid solution. International Journal of Mineral Processing, 148, 41–47;
  36. Sheik, A. R., Ghosh, M. K., Sanjay, K., Subbaiah, T., & Mishra, B. K. (2013). Dissolution kinetics of nickel from spent catalyst in nitric acid medium. Journal of the Taiwan Institute of Chemical Engineers, 44(1), 34–39;
  37. Simate, G. S., Ndlovu, S., & Walubita, L. F. (2010). The fungal and chemolithotrophic leaching of nickel laterites - Challenges and opportunities. Hydrometallurgy, 103(1–4), 150–157;
  38. Srichandan, H., Mohapatra, R. K., Parhi, P. K., & Mishra, S. (2019). Bioleaching approach for extraction of metal values from secondary solid wastes: A critical review. Hydrometallurgy, 189;
  39. Thiruvonasundari, D., & Deepa, K. (2021). Evaluation and comparative study of cell balancing methods for lithium-ion batteries used in electric vehicles. International Journal of Renewable Energy Development, 10(3), 471–479;
  40. Trueba, M., & Trasatti, S. P. (2005). γ-alumina as a support for catalysts: A review of fundamental aspects. European Journal of Inorganic Chemistry, 17, 3393–3403;
  41. Ucyildiz, A., & Girgin, I. (2017). High pressure sulphuric acid leaching of lateritic nickel ore. Physicochemical Problems of Mineral Processing, 53(1), 475–488;
  42. Vynnycky, M., & Assunção, M. (2020). On the significance of sulphuric acid dissociation in the modelling of vanadium redox flow batteries. Journal of Engineering Mathematics, 123(1), 173–203;
  43. Wanta, K. C., Astuti, W., Perdana, I., & Petrus, H. T. B. M. (2020). Kinetic study in atmospheric pressure organic acid leaching: Shrinking core model versus lump model. Minerals, 10(7), 1–10;
  44. Wanta, K. C., Gunawan, W. T., Susanti, R. F., Gemilar, G. P., Petrus, H. T. B. M., & Astuti, W. (2020). Subcritical water as a solvent for extraction of nickel and aluminum ions from reforming spent catalysts. IOP Conference Series: Materials Science and Engineering, 742(1);
  45. Wanta, K. C., Natapraja, E. Y., Susanti, R. F., Gemilar, G. P., Astuti, W., & Petrus, H. T. B. M. (2021). Increasing of metal recovery in leaching process of spent catalyst at low temperature: The addition of hydrogen peroxide and sodium chloride. Metalurgi, 36(2);
  46. Wanta, K. C., Astuti, W., Petrus, H. T. B. M., & Perdana, I. (2022). Product diffusion-controlled leaching of nickel laterite using low concentration citric acid leachant at atmospheric condition. International Journal of Technology, 13(2), 410–421;
  47. Xie, Q., Li, W., & Manthiram, A. (2019). A Mg-doped high-nickel layered oxide cathode enabling safer, high-energy-density li-ion batteries. Chemistry of Materials, 31(3), 938–946;
  48. Yan, P., Zheng, J., Liu, J., Wang, B., Cheng, X., Zhang, Y., Sun, X., Wang, C., & Zhang, J. G. (2018). Tailoring grain boundary structures and chemistry of Ni-rich layered cathodes for enhanced cycle stability of lithium-ion batteries. Nature Energy, 3(7), 600–605;
  49. Zhang, H., Wang, R., Lin, D., Zeng, Y., & Lu, X. (2018). Ni-based nanostructures as high-performance cathodes for rechargeable Ni−Zn battery. ChemNanoMat, 4(6), 525–536;

Last update:

No citation recorded.

Last update: 2023-09-26 08:56:00

No citation recorded.