Lithium Recovery from NCM Lithium-ion Battery by Carbonation Roasting with Graphite Followed by Water Leaching

So-Yeon Lee; Dae-Hyeon Lee; So-Yeong Lee; Ho-Sang Sohn

doi:10.7844/kirr.2022.31.4.26

All Issue

2022 Vol.31, Issue 4 Preview Page Next Page

Research Paper

Lithium Recovery from NCM Lithium-ion Battery by Carbonation Roasting with Graphite Followed by Water Leaching NCM계 리튬이온 배터리 양극재의 그라파이트 첨가 탄산화 배소와 수침출에 의한 Li 회수

31 August 2022. pp. 26-33

PDF XML

Abstract

Owing to the demand for lithium-ion batteries, the recovery of valuable metals from waste lithium-ion batteries is required in future. A pyrometallurgical treatment is appropriate for recycling a large number of waste lithium-ion batteries, but Li loss to slag and dust present a significant challenge. This research investigated carbonation roasting and water leaching behaviors in Li-ion batteries by graphite addition to recover Li from the NCM-based cathode materials of waste Li-ion batteries. When 10 wt% of graphite was added, CO and CO₂ gases were emitted with a rapid weight reduction at apporoximately 850 K, when heated in Ar and CO₂ atmosphere. After the rapid weight reduction, NCM was decomposed and reduced to metal oxides and pure metals. In the carbonation roasting of black powder (NCM+graphite), O₂ is generated via the decomposition of NCM, and an oxides, such as Li₂O and NiO were were also generated. Subsequently, Li₂O reacts with CO₂ to generate Li₂CO₃, and a part of NiO was reduced by graphite to produce metal Ni. In addition, up to 94.5 % Li₂CO₃ with ~99.95 % purity was recovered via water leaching after carbonation roasting.

Keywords

lithium-ion battery

graphite

carbonation

lithium carbonate

water leaching

리튬이온배터리의 수요가 증가함에 따라 향후 발생할 폐리튬이온배터리 중의 유가금속 회수가 필요하다. 대량의 폐리튬이온배터리 리사이클링에는 건식제련이 적합하지만 Li이 슬래그나 분진으로 손실되는 문제점이 있다. 본 연구에서는 폐리튬이온배터리의 NCM계 양극재로부터 Li을 회수하기 위해 그라파이트 첨가에 따른 탄산화 배소와 수침출 거동에 대해 조사하였다. 그라파이트를 10 wt% 첨가 시, Ar 및 CO₂ 분위기에서 승온 중 약 850 K에서 급격한 무게 감소와 함께 CO 및 CO₂ 가스가 배출되었다. 급격한 무게 감소 후 NCM은 금속 산화물 및 순금속으로 분해되고 환원되었다. 따라서 블랙파우더(NCM+그라파이트)의 탄산화 배소에서는 NCM의 분해에 의해 O₂가 발생하면서 Li₂O, NiO 등의 산화물이 생성되고, 이어서 Li₂O가 CO₂와 반응하여 Li₂CO₃를 생성하며, NiO의 일부는 그라파이트에 의해 환원되어 금속 Ni을 생성한다. 그리고 탄산화 배소 후 수침출에 의해 약 99.95 % 순도의 Li₂CO₃를 최대 94.5 %까지 회수하였다.

키워드

리튬이온배터리

그라파이트

탄산화

탄산리튬

수침출

References

Sohn, Ho-Sang, 2022 : Extractive Metallurgy of Lithium, Resources Recycling, 31(3), pp.3-15. 10.7844/kirr.2022.31.3.3

Nayaka, G. P., Pai, K. V., Santhosh, G., et al., 2016 : Recovery of cobalt as cobalt oxalate from spent lithium ion batteries by using glycine as leaching agent, Journal of Environmental Chemical Engineering, 4(2), pp.2378-2383. 10.1016/j.jece.2016.04.016

Huang, Z., Liu, F., Makuza, B., et al., 2022 : Metal Reclamation from Spent Lithium-Ion Battery Cathode Materials: Directional Conversion of Metals Based on Hydrogen Reduction, ACS Sustainable Chemistry & Engineering, 10(2), pp.756-765. 10.1021/acssuschemeng.1c05721

Gao, W., Zhang, X., Zheng, X., et al., 2017 : Lithium carbonate recovery from cathode scrap of spent lithium- ion battery: a closed-loop process. Environmental Science & Technology, 51(3), pp.1662-1669. 10.1021/acs.est.6b0332028081362

Higuchi, A., Ankei, N., Nishihama, S., et al., 2016 : Selective recovery of lithium from cathode materials of spent lithium ion battery, The Journal of Minerals, Metals & Materials Society, 68, pp.2624-2631. 10.1007/s11837-016-2027-6

Georgi-Maschler, T., Friedrich, B., Weyhe, R., et al., 2012 : Development of a recycling process for Li-ion batteries, Journal of Power Sources, 207, pp.173-182. 10.1016/j.jpowsour.2012.01.152

Xiao, J., Niu, B., Xu, Z., 2021 : Highly efficient selective recovery of lithium from spent lithium-ion batteries by thermal reduction with cheap ammonia reagent, Journal of Hazardous Materials, 418, p.126319. 10.1016/j.jhazmat.2021.12631934329006

Pyo, Je-Jung and Wang, Jei-Pil, 2019 : Recovery of Lithium Carbonate and Nickel from Cathode Active Material LNO (Li₂NiO₂) of Precursor Process Byproducts, J. of Korean Inst. of Resources Recycling, 28(4), pp.30-36.

Sohn, Hosang, 2019 : Engineering of Resources Recycling, p.355, KNU Press, Daegu, Korea.

Sohn, Hosang, 2020 : Recycling of Common Metals, p.315, KNU Press, Daegu, Korea.

Information

Publisher :The Korean Institute of Resources Recycling
Publisher(Ko) :한국자원리싸이클링학회
Journal Title :Resources Recycling
Journal Title(Ko) :자원리싸이클링
Volume : 31
No :4
Pages :26-33
Received Date : 2022-07-20
Revised Date : 2022-07-29
Accepted Date : 2022-08-01
DOI :https://doi.org/10.7844/kirr.2022.31.4.26

Resources Recycling ISSN:2765-3439(Print) 2765-3447(Online) 자원리싸이클링

All Issue