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:
Abstract
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. https://doi.org/10.1021/j150508a027
  2. Angumeenal, A. R., & Venkappayya, D. (2013). An overview of citric acid production. LWT - Food Science and Technology, 50(2), 367–370; https://doi.org/10.1016/j.lwt.2012.05.016
  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; https://doi.org/10.1080/10916466.2019.1618867
  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; https://doi.org/10.3390/nano10091878
  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; https://doi.org/10.1016/j.mineng.2015.10.001
  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; https://doi.org/10.1007/s43615-022-00183-9
  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; https://doi.org/10.1007/s11814-015-0085-z
  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. https://doi.org/10.1016/j.seppur.2016.01.014
  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; https://doi.org/10.14710/ijred.2021.18596
  10. Chen, Y., & Nielsen, J. (2016). Biobased organic acids production by metabolically engineered microorganisms. Current Opinion in Biotechnology, 37, 165–172; https://doi.org/10.1016/j.copbio.2015.11.004
  11. Cheng, F., Liang, J., Tao, Z., & Chen, J. (2011). Functional materials for rechargeable batteries. Advanced Materials, 23(15), 1695–1715; https://doi.org/10.1002/adma.201003587
  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; https://doi.org/10.1021/acsami.1c01824
  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; https://doi.org/10.1016/j.mineng.2020.106634
  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; https://doi.org/10.1016/j.chemosphere.2020.126670
  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; https://doi.org/10.19080/RAPSCI.2019.06.555690
  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; https://doi.org/10.1002/cssc.201903213
  17. General Chemistry Laboratory, Eastern Michigan University. (2018). Experiment 3: Analysis of aluminum (III) in water. https://canvas.emich.edu/courses/48894
  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; https://doi.org/10.1016/j.jhazmat.2009.05.131
  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; https://doi.org/10.1016/j.resconrec.2018.04.024
  20. Haar, K. T., & Westerveld, W. (1948). The colorimetric determination of nickel, as Ni(4) dimethylglyoxime. Recueil, 67, 71–81; https://doi.org/10.1002/recl.19480670112
  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; https://doi.org/10.1016/j.jece.2017.07.059
  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); https://doi.org/10.4172/2168-9806.1000146
  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; https://doi.org/10.1016/j.jpowsour.2010.03.080
  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; https://doi.org/10.1002/jctb.6448
  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; https://doi.org/10.1016/j.wasman.2010.08.008
  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; https://doi.org/10.1016/j.jpowsour.2015.02.073
  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; https://doi.org/10.1002/inf2.12000
  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; https://doi.org/10.1039/c0jm01921f
  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; https://doi.org/10.1007/s11356-021-13027-0
  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; https://doi.org/10.14710/ijred.2022.40090
  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; https://doi.org/10.1016/j.wasman.2015.12.018
  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; https://doi.org/10.1080/08827508.2018.1514300
  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; https://doi.org/10.1088/1757-899X/478/1/012013
  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; https://doi.org/10.1080/10643389.2019.1709399
  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; https://doi.org/10.1016/j.minpro.2016.01.006
  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; https://doi.org/10.1016/j.jtice.2012.08.003
  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; https://doi.org/10.1016/j.hydromet.2010.03.012
  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; https://doi.org/10.1016/j.hydromet.2019.105122
  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; https://doi.org/10.14710/ijred.2021.34484
  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; https://doi.org/10.1002/ejic.200500348
  41. Ucyildiz, A., & Girgin, I. (2017). High pressure sulphuric acid leaching of lateritic nickel ore. Physicochemical Problems of Mineral Processing, 53(1), 475–488; https://doi.org/10.5277/ppmp170137
  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; https://doi.org/10.1007/s10665-020-10061-8
  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; https://doi.org/10.3390/min10070613
  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); https://doi.org/10.1088/1757-899X/742/1/012025
  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); https://doi.org/10.14203/metalurgi.v36i2.591
  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; https://doi.org/10.14716/ijtech.v13i2.4641
  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; https://doi.org/10.1021/acs.chemmater.8b03900
  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; https://doi.org/10.1038/s41560-018-0191-3
  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; https://doi.org/10.1002/cnma.201800078

Last update:

No citation recorded.

Last update: 2024-04-24 03:41:16

No citation recorded.