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化学进展 2023, Vol. 35 Issue (2): 287-301 DOI: 10.7536/PC220727 前一篇   后一篇

• 综述 •

废旧锂离子电池选择性提锂

朱国辉1,2, 还红先1,2, 于大伟1,2,*(), 郭学益1,2, 田庆华1,2   

  1. 1 中南大学 冶金与环境学院 长沙 410083
    2 有色金属资源循环利用国家地方联合工程研究中心 长沙 410083
  • 收稿日期:2022-07-20 修回日期:2022-09-30 出版日期:2023-02-24 发布日期:2022-10-30
  • 基金资助:
    湖南省自然科学基金(2021JJ30854); 国家自然科学基金(52274413)
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Selective Recovery of Lithium from Spent Lithium-Ion Batteries

Guohui Zhu1,2, Hongxian Huan1,2, Dawei Yu1,2(), Xueyi Guo1,2, Qinghua Tian1,2   

  1. 1 School of Metallurgy and Environment, Central South University,Changsha 410083, China
    2 National and Regional Joint Engineering Research Centre of Nonferrous Metal Resource Recycling,Changsha 410083, China
  • Received:2022-07-20 Revised:2022-09-30 Online:2023-02-24 Published:2022-10-30
  • Contact: *e-mail: dawei.yu@csu.edu.cn
  • About author:
    †These authors contributed equally to this work.
  • Supported by:
    Natural Science Foundation of Hunan Province(2021JJ30854); National Natural Science Foundation of China(52274413)

新能源汽车行业的蓬勃发展不仅使锂离子电池需求量激增,大批锂离子电池在达到一定循环次数后也会因无法继续使用而报废。目前研究者们已经对废旧锂离子电池中有价金属的提取方法进行了许多研究,但回收过程中重点关注的对象是钴和镍,锂作为锂离子电池中的主要成分没有给予足够的重视。随着锂资源供需关系的日趋紧张,近年来通过将废旧锂离子电池中的锂优先选择性提取以提高其回收效率的研究不断增多。基于此,本文系统梳理了从不同正极材料(如钴酸锂、锰酸锂、镍钴锰酸锂和磷酸铁锂)中选择性提锂的方法,包括高温转型、选择性浸出、机械化学及电化学法,为后续有关退役锂离子电池选择性提锂的研究及产业实践提供参考。

关键词： 电池回收, 锂离子电池, 选择性提锂, 循环利用

The transition towards electric vehicles (EVs) has resulted in a proliferating demand for lithium-ion batteries (LIBs). The continuous growth in the EV industry results in a colossal number of LIBs being discarded after reaching their end-of-life. Researchers have carried out numerous investigations on the extraction of valuable metals from spent LIBs. The recycling processes have mainly been concerned with the recovery of the valuable metals of cobalt and nickel, with less attention being placed on lithium recovery. With the imbalance of the supply and demand of lithium resources, research on selective recovery of lithium from spent LIBs has increased in recent years. This paper provides a comprehensive overview of the high-temperature selective conversion, selective leaching, mechanical and electrochemical recycling methods that facilitate selective lithium recovery. It provides recommendations for future research and development to enhance the selective extraction of lithium from spent LIBs.

Contents

1 Introduction

2 Selective lithium extraction from spent LIBs cathode material

2.1 High-temperature transition

2.2 Selective leaching

2.3 Mechanical/electrochemical extraction

2.4 Comparison of advantages and shortcomings of different treatments

2.5 Influence of impurities

3 Recovery of lithium from electrolyte

4 Conclusion and outlook

Key words: batteries recycling, spent lithium-ion batteries, selective lithium recovery, sustainable recycling
()
表1 不同类型正极材料组成、结构、锂含量、主要用途、市场份额及回收经济效益对比[4,16,29]
Table 1 Comparison of different types of cathode composition, structure, proportion of lithium, typical use, market share and recycling economic benefits[4,16,29]
Cathode types LCO NCM LMO LFP
Chemical formular LiCoO2 LiNi0.33Co0.33Mn0.33O2 (NCM111)
LiNi0.5Co0.3Mn0.2O2(NCM532)
LiNi0.6Co0.2Mn0.2O2(NCM622)
LiNi0.8Co0.1Mn0.1O2(NCM811)		 LiMn2O4 LiFePO4
Structure Layered Layered Spinel Olivine
Theoretical
lithium content		 7.09 wt% 7.65 wt%
(NCM111)		 3.84 wt% 5.74 wt%
Typical use Portable electronic
devices and electric tools		 Portable electronic devices and EVs Electric tools and bikes Electric bikes, large EVs and power tools
Characteristics Low safety,
high cost,
medium
performance		 Medium safety, medium cost,
higher energy density,
high lifetime		 Medium safety,
low cost,
medium energy
density,
low lifetime		 Good safety,
low cost,
high thermal stability, medium energy
density
Market share Steady Growing Small Growing
Recycling
economic benefits		 LCO > NCM > LMO > LFP
图1 通过高温转型实现电极活性材料/含锂熔渣选择性提锂示意图
Fig.1 Schematic diagram of selective lithium extraction from electrode material and lithium-bearing slag by high temperature transition
图2 不同温度下碳酸锂在水中的溶解度[37]
Fig.2 Solubility of lithium carbonate in water at different temperatures[37]
图3 LCO正极材料铝热还原选择性提锂示意图[52]
Fig.3 Schematic diagram of selective lithium extraction from LCO cathode by aluminothermic reduction[52], Copyright 2019, American Chemical Society
表2 不同硝酸盐分解温度对比[58]
Table 2 Comparison of the decomposition temperatures of relevant nitrate compounds[58]
Sample Decomposition Temperature (K)
LiNO3 913 ± 100
Ni(NO3)2 580 ± 25
Co(NO3)2 515 ± 30
Mn(NO3)2 480 ± 20
Cu(NO3)2 520 ± 30
Fe(NO3)3 465 ± 20
Al(NO3)3 440 ± 25
图4 CaCl2氯化NCM选择性提锂过程示意图[64]
Fig.4 Schematic diagram of the selective chlorination of the NCM cathode using CaCl2[64]
图5 硫酸化焙烧法从废LCO电池选择性提锂示意图[68]
Fig.5 Schematic diagram of selective lithium extraction from spent LCO batteries by sulfation roasting[68]. Copyright 2019, RSC
图6 H2O2-CH3COOH体系从废旧LFP回收锂的流程[76]
Fig.6 Process for recovering lithium from spent LFP by the H2O2-CH3COOH system[76]
图7 机械活化法从废旧LFP选择性回收锂的流程[80]
Fig.7 Selective recovery of lithium from spent LFP by mechanical activation[80]
图8 电化学法从LFP中选择性回收Li的示意图[82]
Fig.8 Schematic illustration of the selective recovery of Li from LFP by electrochemical treatment[82]. Copyright 2020, Elsevier
图9 不同高温转型方法适用的正极材料类型、焙烧温度及焙烧产物所需浸出体系对比
Fig.9 Comparison of high temperature processes for the treatment of different cathode materials with regard to the roasting temperature and required leaching conditions for the roasted products
表3 选择性浸出使用试剂对比
Table 3 Comparison of leaching reagent and reduction/oxidation agent in selective leaching
Leaching Reagent Reduction/Oxidation Agent Cathode Material Ref
H2SO4 H2O2 LFP 73
H3PO4 H2O2 LCO, NCM, LMO, LFP 19
H2C2O4 - LCO 75
CH3COOH H2O2 LFP 76
Na2S2O8 Na2S2O8 LFP 77
表4 选择性提锂不同方法的能量消耗、试剂成本、尾气排放、浸出体系、处理能力对比
Table 4 Comparision of various process treatments in terms of the required energy, reagent costs, exhaust gas emission, acid/alkaline leaching, and processing capacity
Process
Treatments		 Required Energy Reagent Costs Exhaust Gas
Emission		 Acid/Alkaline
Reagent Leaching		 Processing Capacity
High temperature transition High Medium Yes No
(Except in-situ reduction and oxidation roasting)		 High
Selective leaching Medium High No Yes High
Mechanical
chemistry		 High High No No Low
Electrochemical
treatment		 Medium Low No No Low
图10 电解液中回收锂流程图
Fig.10 Flowsheet for lithium recovery from electrolyte
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摘要

废旧锂离子电池选择性提锂