Regeneration of LiNi1/3Co1/3Mn1/3O2cathode active materials from end-of-life lithium-ion batteries through ascorbic acid leaching and oxalic acid coprecipitation processes
Refly S.a, Floweri O.a, Mayangsari T.R.b, Sumboja A.a, Santosa S.P.a, Ogi T.c, Iskandar F.a
a Department of Physics, Faculty of Mathematics and Natural Sciences, Institut Teknologi Bandung, Bandung, 40132, Indonesia
b Department of Chemistry, Universitas Pertamina, Simprug, Jakarta, 12220, Indonesia
c Chemical Engineering Program, Graduate School of Advanced Science and Engineering, Hiroshima University, Hiroshima, 739-8527, Japan
Abstract
© One of the emerging issues in solving the electronic waste problem is to address the growing amount of end-of-life Li-ion battery (LIB) waste. In this work, the regeneration of LiNi1/3Co1/3Mn1/3O2 (NCM 111) cathode active materials from end-of-life LIBs was successfully carried out via an easy, fast, and environmentally friendly recycling process that comprised three main stages, i.e., ascorbic acid leaching, oxalate coprecipitation process, and heat treatment. Ascorbic acid was able to leach Li, Ni, Co, and Mn ions from the spent NCM 111 cathode material with a relatively high leaching efficiency up to 90%. The following oxalic acid coprecipitation method has effectively recovered the transition metal ions in the leachate in the form of the metal oxalates MC2O4·2H2O (M = Ni, Mn, and Co), as confirmed by the result of X-ray diffraction characterization. The quantitative analysis of metal ions using X-ray fluorescence revealed that the ratio of Ni, Co, and Mn in the precipitate was approximately 1:1:1, with a slightly lower amount of Mn. Regeneration of NCM 111 via the heat treatment of metal oxalates at temperatures of 800-950 °C successfully reproduced the material (R-NCM) with an R3m hexagonal-layered structure, which could be reemployed as the cathode in LIBs. Charge-discharge characterization of the as-fabricated LIB at 2.5-4.3 V revealed that the battery with the R-NCM cathode synthesized at 900 °C exhibited a slightly higher initial specific discharge capacity (164.9 mAh/g at 0.2 C) than that of commercial NCM (157.4 mAh/g at 0.2 C). Moreover, the Li-ion battery also showed a very stable performance with a capacity retention of 91.3% after 100 cycles at 0.2 C.
Author keywords
Capacity retention,Cathode active material,Co-precipitation process,Coprecipitation method,Hexagonal layered structure,Oxalate coprecipitation process,Specific discharge capacity,Stable performance
Indexed keywords
Ascorbic acid leaching,End-of-life Li-ion battery,Li-ion battery,Oxalic acid coprecipitation,Recycle
Funding details
This work was supported by USAID through Sustainable Higher Education Research Alliances (SHERA) Program – Centre for Collaborative (CCR) National Center for Sustainable Transportation Technology (NCSTT) and by the Ministry of Research and Technology/National Agency for Research and Innovation through Post-Doctoral Research Program. This research was also partially funded by the Indonesian Ministry of Research and Technology/National Agency for Research and Innovation, and Indonesian Ministry of Education and Culture under World Class University (WCU) Program managed by Institut Teknologi Bandung. S. R. would like to thank the Indonesia Endowment Fund for Education (LPDP) of the Ministry of Finance of Indonesia for the master scholarship and research grant. O. F. would like to thank ITB World Class University (WCU) post-doctoral program.