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Progress in Chemistry 2023, Vol. 35 Issue (2): 287-301 DOI: 10.7536/PC220727 Previous Articles   Next Articles

• Review •

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: Revised: Online: Published:
  • 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)
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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
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
Fig.1 Schematic diagram of selective lithium extraction from electrode material and lithium-bearing slag by high temperature transition
Fig.2 Solubility of lithium carbonate in water at different temperatures[37]
Fig.3 Schematic diagram of selective lithium extraction from LCO cathode by aluminothermic reduction[52], Copyright 2019, American Chemical Society
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
Fig.4 Schematic diagram of the selective chlorination of the NCM cathode using CaCl2[64]
Fig.5 Schematic diagram of selective lithium extraction from spent LCO batteries by sulfation roasting[68]. Copyright 2019, RSC
Fig.6 Process for recovering lithium from spent LFP by the H2O2-CH3COOH system[76]
Fig.7 Selective recovery of lithium from spent LFP by mechanical activation[80]
Fig.8 Schematic illustration of the selective recovery of Li from LFP by electrochemical treatment[82]. Copyright 2020, Elsevier
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
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
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
Fig.10 Flowsheet for lithium recovery from electrolyte
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