A Comparative Study of LiNCA Cathode Recycled from Spent Lithium-Ion Batteries and Synthesized from Metal Precursor
Arif Jumari(1*), Enni Apriliani(2), Cornelius Satria Yudha(3), Agus Purwanto(4), Anne Zulfia Syahrial(5), Wara Dyah Pita Rengga(6)
(1) Department of Chemical Engineering, Faculty of Engineering, Universitas Sebelas Maret, Jl. Ir. Sutami 36A, Kentingan, Surakarta 57126, Indonesia; Center of Excellence for Electrical Energy Storage Technology, Universitas Sebelas Maret, Jl. Slamet Riyadi No. 435, Surakarta 57126, Indonesia
(2) Center of Excellence for Electrical Energy Storage Technology, Universitas Sebelas Maret, Jl. Slamet Riyadi No. 435, Surakarta 57126, Indonesia
(3) Center of Excellence for Electrical Energy Storage Technology, Universitas Sebelas Maret, Jl. Slamet Riyadi No. 435, Surakarta 57126, Indonesia
(4) Department of Chemical Engineering, Faculty of Engineering, Universitas Sebelas Maret, Jl. Ir. Sutami 36A, Kentingan, Surakarta 57126, Indonesia; Center of Excellence for Electrical Energy Storage Technology, Universitas Sebelas Maret, Jl. Slamet Riyadi No. 435, Surakarta 57126, Indonesia
(5) Department of Metallurgical and Material Engineering, Faculty of Engineering, Universitas Indonesia, Jl. Prof. Dr. Sumitro Djojohadikusumo, Depok 16424, Indonesia
(6) Department of Chemical Engineering, Faculty of Engineering, Universitas Negeri Semarang, Kampus Sekaran, Gunung Pati, Semarang 50229, Indonesia
(*) Corresponding Author
Abstract
Spent lithium NCA (LiNCA) battery was recycled using organic and inorganic acids and the performances were compared against the cathode synthesized from precursor. The metals in the spent cathode were leached using sulfuric or citric acid and coprecipitated into ternary metal oxalate (TMO) after reduction and lithium separation. Subsequently, the coprecipitated solution was used for cathode synthesis. Leaching efficiencies for nickel, cobalt and aluminum using citric acid were 85.6, 94.1, and 99%, respectively, while the efficiencies using sulfuric acid were 96, 98, and 100%, respectively. TMO produced from coprecipitation had the same physical characteristics. It was important to acknowledge that all cathodes also had similar physical characteristics. The electrochemical tests showed that commercial cathodes had the highest capacity of 150 mAh/g. This was followed by those from precursors, sulfuric acid leaching, and citric acid leaching, which recorded 142, 135, and 130 mAh/g, respectively. Based on the cycle test at 1C, the sample from citric acid leaching was 86% after 20 cycles compared to others at 82–83%. The results suggested that spent LiNCA could be regenerated into new cathodes using acid with performance comparable to those synthesized from precursor. This presented a viable alternative for LiNCA cathode synthesis.
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[1] Neumann, J., Petranikova, M., Meeus, M., Gamarra, J.D., Younesi, R., Winter, M., and Nowak, S., 2022, Recycling of lithium-ion batteries—Current state of the art, circular economy, and next generation recycling, Adv. Energy Mater., 12 (17), 2102917
[2] Mrozik, W., Rajaeifar, M.A., Heidrich, O., and Christensen, P., 2021, Environmental impacts, pollution sources and pathways of spent lithium-ion batteries, Energy Environ. Sci., 14 (12), 6099–6121.
[3] Steward, D., Mayyas, A., and Mann, M., 2021, Economics and challenges of li-ion battery recycling from end-of-life vehicles, Procedia Manuf., 33, 272–279.
[4] Melin, E., 2019, State-of-the-art in reuse and recycling of lithium-ion batteries - A research review, https://www.energimyndigheten.se/globalassets/forskning--innovation/overgripande/state-of-the-art-in-reuse-and-recycling-of-lithium-ion-batteries-2019.pdf, accessed on March 15, 2022.
[5] Alipanah, M., Saha, A.K., Vahidi, E., and Jin, H., 2021, Value recovery from spent lithium-ion batteries: A review on technologies, environmental impacts, economics, and supply chain, Clean Technol. Recycl., 1 (2), 152–184.
[6] Asadi Dalini, E., Karimi, G., Zandevakili, S., and Goodarzi, M., 2021, A review on environmental, economic and hydrometallurgical processes of recycling spent lithium-ion batteries, Miner. Process. Extr. Metall. Rev., 42 (7), 451–472.
[7] Islam, M.T., and Iyer-Raniga, U., 2022, Lithium-ion battery recycling in the circular economy: A review, Recycling, 7 (3), 33.
[8] Nitta, N., Wu, F., Lee, J.T., and Yushin, G., 2015, Li- Li-ion battery materials: Present and future, Mater. Today, 18 (5), 252–264.
[9] Lai, Y.Q., Xu, M., Zhang, Z.A., Gao, C.H., Wang, P., and Yu, Z.Y., 2016, Optimized structure stability and electrochemical performance of LiNi0.8Co0.15Al0.05O2 by sputtering nanoscale ZnO film, J. Power Sources, 309, 20–26.
[10] Yudha, C.S., Muzayanha, S.U., Rahmawati, M., Widiyandari, H., Sutopo, W., Nizam, M., Santosa, S.P., and Purwanto, A., 2020, Fast production of high performance LiNi0.815Co0.15Al0.035O2 cathode material via urea-assisted flame spray pyrolysis, Energies, 13 (11), 2757.
[11] Purwanto, A., Yudha, C.S., Ikhwan Muhammad, K., Algifari, B.G., Widiyandari, H., and Sutopo, W., 2020, Synthesis of LiNi0.8Co0.15Al0.05O2 cathode material via flame-assisted spray pyrolysis method, Adv. Powder Technol., 31 (4), 1674–1681.
[12] Zhang, J., Xu, S., Hamad, K.I., Jasim, A.M., and Xing, Y., 2020, High retention rate NCA cathode powders from spray drying and flame assisted spray pyrolysis using glycerol as the solvent, Powder Technol., 363, 1–6.
[13] Ghosh, S., Bhattacharjee, U., Bhowmik, S., and Martha, S.K., 2022, A review on high-capacity and high-voltage cathodes for next-generation lithium-ion batteries, J. Energy Power Technol., 4 (1), 002.
[14] Purwanto, A., Yudha, C.S., Ubaidillah, U., Widiyandari, H., Ogi, T., and Haerudin, H., 2018, NCA cathode material: Synthesis methods and performance enhancement efforts, Mater. Res. Express, 5 (12), 122001.
[15] Zhu, J., Cao, G., Li, Y., Xi, X., Jin, Z., Xu, B., and Li, W., 2020, Efficient utilisation of rod-like nickel oxalate in lithium-ion batteries: A case of NiO for the anode and LiNiO2 for the cathode, Scr. Mater., 178, 51–56.
[16] Petranikova, M., Naharro, P.L., Vieceli, N., Lombardo, G., and Ebin, B., 2022, Recovery of critical metals from EV batteries via thermal treatment and leaching with sulphuric acid at ambient temperature, Waste Manage., 140, 164–172.
[17] Chiu, K.L., Shen, Y.H., Chen, Y.H., and Shih, K.Y., 2019, Recovery of valuable metals from spent lithium ion batteries (LIBs) using physical pretreatment and a hydrometallurgy process, Adv. Mater., 8 (1), 12–20.
[18] Velázquez-Martínez, O., Valio, J., Santasalo-Aarnio, A., Reuter, M., and Serna-Guerrero, R., 2019, A critical review of lithium-ion battery recycling processes from a circular economy perspective, Batteries, 5 (4), 68.
[19] Sun, L., Liu, B., Wu, T., Wang, G., Huang, Q., Su, Y., and Wu, F., 2021, Hydrometallurgical recycling of valuable metals from spent lithium-ion batteries by reductive leaching with stannous chloride, Int. J. Miner., Metall. Mater., 28 (6), 991–1000.
[20] Petranikova, M., Naharro, P.L., Vieceli, N., Lombardo, G., and Ebin, B., 2022, Recovery of critical metals from EV batteries via thermal treatment and leaching with sulphuric acid at ambient temperature, Waste Manage., 140, 164–172.
[21] Wang, S., Wang, C., Lai, F., Yan, F., and Zhang, Z., 2020, Reduction-ammoniacal leaching to recycle lithium, cobalt, and nickel from spent lithium-ion batteries with a hydrothermal method: Effect of reductants and ammonium salts, Waste Manage., 102, 122–130.
[22] Zhang, Y., Wang, W., Fang, Q., and Xu, S., 2020, Improved recovery of valuable metals from spent lithium-ion batteries by efficient reduction roasting and facile acid leaching, Waste Manage., 102, 847–855.
[23] Liu, P., Xiao, L., Tang, Y., Chen, Y., Ye, L., and Zhu, Y., 2019, Study on the reduction roasting of spent LiNixCoyMnzO2 lithium-ion battery cathode materials, J. Therm. Anal. Calorim., 136 (3), 1323–1332.
[24] He, L.P., Sun, S.Y., Mu, Y.Y., Song, X.F., and Yu, J.G., 2017, Recovery of lithium, nickel, cobalt, and manganese from spent lithium-ion batteries using L-tartaric acid as a leachant, ACS Sustainable Chem. Eng., 5 (1), 714–721.
[25] Fan, B., Chen, X., Zhou, T., Zhang, J., and Xu, B., 2016, A sustainable process for the recovery of valuable metals from spent lithium-ion batteries, Waste Manage. Res., 34 (5), 474–481.
[26] Bae, H., and Kim, Y., 2021, Technologies of lithium recycling from waste lithium ion batteries: A review, Mater. Adv., 2 (10), 3234–3250.
[27] Peng, C., Liu, F., Wang, Z., Wilson, B.P., and Lundström, M., 2019, Selective extraction of lithium (Li) and preparation of battery grade lithium carbonate (Li2CO3) from spent Li-ion batteries in nitrate system, J. Power Sources, 415, 179–188.
[28] Zhang, N., 2022, Efficient Methods for Recycling Cathodes of Spent Lithium-Ion Batteries, Thesis, University of Alberta, Alberta, Edmonton, Canada.
[29] Zheng, H., Dong, T., Sha, Y., Jiang, D., Zhang, H., and Zhang, S., 2021, Selective extraction of lithium from spent lithium batteries by functional ionic liquid, ACS Sustainable Chem. Eng., 9 (20), 7022–7029.
[30] Refly, S., Floweri, O., Mayangsari, T.R., Aimon, A.H., and Iskandar, F., 2021, Green recycle processing of cathode active material from LiNi1/3Co1/3Mn1/3O2 (NCM 111) battery waste through citric acid leaching and oxalate co-precipitation process, Mater. Today: Proc., 44, 3378–3380.
[31] Vieceli, N., Casasola, R., Lombardo, G., Ebin, B., and Petranikova, M., 2021, Hydrometallurgical recycling of EV lithium-ion batteries: Effects of incineration on the leaching efficiency of metals using sulfuric acid, Waste Manage., 125, 192–203.
[32] Guimarães, L.F., Botelho Junior, A.B., and Espinosa, D.C.R., 2022, Sulfuric acid leaching of metals from waste Li-ion batteries without using reducing agent, Miner. Eng., 183, 107597.
[33] Beaudet, A., Larouche, F., Amouzegar, K., Bouchard, P., and Zaghib, K., 2020, Key challenges and opportunities for recycling electric vehicle battery materials, Sustainability, 12 (14), 5837.
[34] Meshram, P., Mishra, A., Abhilash; A., and Sahu, R., 2020, Environmental impact of spent lithium ion batteries and green recycling perspectives by organic acids – A review, Chemosphere, 242, 125291.
[35] Cheng, Q., Chirdon, W.M., Lin, M., Mishra, K., and Zhou, X., 2019, Characterization, modeling, and optimization of a single-step process for leaching metallic ions from LiNi1/3Co1/3Mn1/3O2 cathodes for the recycling of spent lithium-ion batteries, Hydrometallurgy, 185, 1–11.
[36] Chen, X., Chen, Y., Zhou, T., Liu, D., Hu, H., and Fan, S., 2015, Hydrometallurgical recovery of metal values from sulfuric acid leaching liquor of spent lithium-ion batteries, Waste Manage., 38, 349–356.
[37] Muzayanha, S.U., Yudha, C.S., Nur, A., Widiyandari, H., Haerudin, H., Nilasary, H., Fathoni, F., and Purwanto, A., 2019, A fast metals recovery method for the synthesis of lithium nickel cobalt aluminum oxide material from cathode waste, Metals, 9 (5), 615.
[38] Li, L., Fan, E., Guan, Y., Zhang, X., Xue, Q., Wei, L., Wu, F., and Chen, R., 2017, Sustainable recovery of cathode materials from spent lithium-ion batteries using lactic acid leaching system, ACS Sustainable Chem. Eng., 5 (6), 5224–5233.
[39] Yudha, C.S., Muzayanha, S.U., Widiyandari, H., Iskandar, F., Sutopo, W., and Purwanto, A., 2019, Synthesis of LiNi0.85Co0.14Al0.01O2 cathode material and its performance in an NCA/graphite full-battery, Energies, 12 (10), 1886.
[40] Li, L., Bian, Y., Zhang, X., Guan, Y., Fan, E., Wu, F., and Chen, R., 2018, Process for recycling mixed-cathode materials from spent lithium-ion batteries and kinetics of leaching, Waste Manage., 71, 362–371.
[41] Hu, J., Zhang, J., Li, H., Chen, Y., and Wang, C., 2017, A promising approach for the recovery of high value-added metals from spent lithium-ion batteries, J. Power Sources, 351, 192–199.
[42] Yi, W., Yan, C., Ma, P., Li, F., and Wen, X., 2007, Refining of crude Li2CO3 via slurry phase dissolution using CO2, Sep. Purif. Technol., 56 (3), 241–248.
[43] Liu, B., Huang, Q., Su, Y., Sun, L., Wu, T., Wang, G., Kelly, R.M., and Wu, F., 2019, Maleic, glycolic and acetoacetic acids-leaching for recovery of valuable metals from spent lithium-ion batteries: leaching parameters, thermodynamics and kinetics, R. Soc. Open Sci., 6 (9), 191061.
[44] Krüger, S., Hanisch, C., Kwade, A., Winter, M., and Nowak, S., 2014, Effect of impurities caused by a recycling process on the electrochemical performance of Li[Ni0.33Co0.33Mn0.33]O2, J. Electroanal. Chem., 726, 91–96.
[45] Li, J., Li, X., Hu, Q., Wang, Z., Zheng, J., Wu, L., and Zhang, L., 2009, Study of extraction and purification of Ni, Co and Mn from spent battery material, Hydrometallurgy, 99 (1-2), 7–12.
[46] Petrović, S.J., Bogdanović, G.D., and Antonijević, M.M., 2018, Leaching of chalcopyrite with hydrogen peroxide in hydrochloric acid solution, Trans. Nonferrous Met. Soc. China, 28 (7), 1444–1455.
[47] Yao, X., Xu, Z., Yao, Z., Cheng, W., Gao, H., Zhao, Q., Li, J., and Zhou, A., 2019, Oxalate co-precipitation synthesis of LiNi0.6Co0.2Mn0.2O2 for low-cost and high-energy lithium-ion batteries, Mater. Today Commun., 19, 262–270.
[48] Li, J., Zhang, N., Li, H., Liu, A., Wang, Y., Yin, S., Wu, H., and Dahn, J.R., 2018, Impact of the synthesis conditions on the performance of LiNixCoyAlzO2 with high Ni and low Co content, J. Electrochem. Soc., 165 (14), A3544.
[49] Li, J., Chen, B.R., and Zhou, H.M., 2016, Effects of washing and heat-treatment on structure and electrochemical charge/discharge property of LiNi0.8Co0.15Al0.05O2 powder, J. Inorg. Mater., 31 (7), 773–778.
[50] Li, Y., Tan, Z., Liu, Y., Lei, C., He, P., Li, J., He, Z., Cheng, Y., Wu, F., and Li, Y., 2024, Past, present and future of high-nickel materials, Nano Energy, 119, 109070.
[51] Zhang, J., Hu, J., Zhang, W., Chen, Y., and Wang, C., 2018, Efficient and economical recovery of lithium, cobalt, nickel, manganese from cathode scrap of spent lithium-ion batteries, J. Cleaner Prod., 204, 437–446.
[52] Yang, Y., Huang, G., Xie, M., Xu, S., and He, Y., 2016, Synthesis and performance of spherical LiNixCoyMn1-x-yO2 regenerated from nickel and cobalt scraps, Hydrometallurgy, 165, 358–369.
[53] Yao, L., Yao, H., Xi, G., and Feng, Y., 2016, Recycling and synthesis of LiNi1/3Co1/3Mn1/3O2 from waste lithium ion batteries using D,L-malic acid, RSC Adv., 6 (22), 17947–17954.
[54] Shan, M., Dang, C., Meng, K., Cao, Y., Zhu, X., Zhang, J., Xu, G., and Zhu, M., 2024, Recycling of LiFePO4 cathode materials: From laboratory scale to industrial production, Mater. Today, 73, 130–150.
[55] Xavier, L.H., Ottoni, M., and Abreu, L.P.P., 2023, A comprehensive review of urban mining and the value recovery from e-waste materials, Resour., Conserv. Recycl., 190, 106840.
[56] Gomes, N., Garjulli, F., Botelho Junior, A.B., Espinosa, D.C.R., and Baltazar, M.P.G., 2024, Recycling of spent catalysts from the petrochemical industry by hydrometallurgy to obtain high-purity nickel products for electroplating, JOM, 76 (3), 1372–1382.
DOI: https://doi.org/10.22146/ijc.98276
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