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Progress in Chemistry 2020, Vol. 32 Issue (7): 950-965 DOI: 10.7536/PC191106 Previous Articles   Next Articles

Special Issue: 锂离子电池

• Review •

The Recovery and Recycling of Cathode Materials and Electrolyte from Spent Lithium Ion Batteries in Full Process

Deying Mu1,3, Zhu Liu1, Shan Jin1, Yuanlong Liu1, Shuang Tian2,**(), Changsong Dai1,**()   

  1. 1. School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China
    2. Ningbo Institute of Materials Technology & Engineering, Chinese Academy of Sciences, Ningbo 315201, China
    3. School of Food Science and Engineering, Harbin University of Commerce, Harbin 150076, China
  • Received: Online: Published:
  • Contact: Shuang Tian, Changsong Dai
  • About author:
    ** e-mail: (Shuang Tian);
    .(Changsong Dai)
  • Supported by:
    Foundation of Key Program of Sci-Tech Innovation in Ningbo(2019B10114); University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(UNPYSCT-2018138)
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As a new type of energy storage devices with rapid development momentum, lithium ion batteries(LIBs)alleviate the dependence on fossil fuels in energy field and reduce the increasingly severe environmental pressure. A large number of spent lithium ion batteries are not only hazardous wastes, but also resources with high added value from different perspectives. Therefore, it is of great challenge and practical significance to realize high-efficient recycling and reuse of spent lithium ion batteries with progressively diverse components through innovation and combination of different technical means. Starting from the pretreatment process, the technical means and requirements of a series of processes such as deactivation and discharge, dismantling and classification, crushing and sieving, separation process, acid leaching and impurity removal are described in detail. This review discusses the typical strategies of reuse from three aspects and analyzes the advantages and disadvantages of various techniques in the process of material regeneration, structural repair and re-synthesis of cathode materials. In addition, the harmless treatment and recovery of spent electrolyte are discussed, especially the application of supercritical CO2 extraction process. Finally, the outlook is put forward in view of the existing problems at the present stage to provide references for subsequent research and industrial applications of spent lithium ion battery recycling.

Contents

1 Introduction

2 Overview of spent lithium ion battery recycling

3 Pretreatment of spent lithium ion batteries

3.1 Discharge and deactivation

3.2 Dismantling and classification

3.3 Crushing and sieving

3.4 Separation

4 Dissolution and purification of spent materials

4.1 Acid leaching process

4.2 Removal of impurities

5 Recycle and reuse of spent materials

5.1 Recovery of metals and raw materials

5.2 Direct regeneration of cathode materials

5.3 Re-synthesis of cathode materials

6 Non-hazardous treatment and recovery of spent electrolyte

6.1 Harmless disposal by conventional physical and chemical methods

6.2 Reclamation by supercritical CO2 extraction

7 Conclusion and outlook

Key words: spent lithium ion batteries, recovery and recycling, pretreatment, material synthesis, electrolyte, supercritical CO2 extraction
Fig.1 Daily averaged CO2 from four global monitoring division baseline observatories and CO2 radiative forcing[3]
Fig.2 Classification of battery recycling processes and final reused products
Fig.3 Simplified diagram of whole pretreatment processes for spent lithium ion batteries
Table 1 Typical research works about the inorganic and organic acid leaching for spent lithium-ion batteries in recent years
work group raw material reagent leaching conditions leaching efficiency ref
Barik S P(2017) Spent LIBs 1.75 mol/L HCl 50 ℃, 120 min 99.2%Li, 98%Co, 99%Mn 22
He L P(2017) Spent LIBs
(LiNi1/3Co1/3Mn1/3O2)		 1 mol/L H2SO4 + 1 vol% H2O2 40 ℃, 60 min 99.7%Li, 99.7%Co
99.7%Mn, 99.7%Ni		 38
Chen X P(2018) Spent LIBs(LiCoO2) 1 mol/L H2SO4 + 0.4 g/g Glucose 95 ℃, 120 min 96%Li, 98%Co 39
Guan J(2017) Spent LIBs 1 mol/L HNO3 250 min(grinding)+
550 rpm(rotation)		 77.15% Li, 91.25%Co
100%Mn, 99.9%Ni		 40
Chen X P(2017) Spent LIBs(LiCoO2) 0.7 mol/L H3PO4 + 4 vol% H2O2 40 ℃, 60 min 99%Li, 99%Co 41
Meng Q(2017) Spent LIBs(LiCoO2) 1.5 mol/L H3PO4 + 0.02 mol/L Glucose 80 ℃, 120 min 100%Li, 98%Co 42
Li L(2019) Spent LIBs(LiFePO4) 20 g/g Citric Acid + H2O 460 min(grinding)
+300 rpm(rotation)		 97.8%Li, 95.6%Fe 43
Yu M(2019) LiCoO2 1.0 mol/L Citric Acid + 8 vol% H2O2 70 ℃, 70 min 99% 44
Gao W F(2018) Spent LIBs
(LiNi x Co y Mn1- x - y O2)		 3.5 mol/L Acetic Acid + 4 vol% H2O2 60 ℃, 60 min 99.97%Li, 93.62%Co
96.32% Mn, 92.67% Ni		 45
He L P(2017) Spent LIBs(LiCoO2 and
LiNi0.5Co0.2Mn0.3O2)		 2 mol/L L-tartaric Acid + 4 vol% H2O2 70 ℃, 30 min 99.1%Li, 98.6%Co
99.3%Mn, 99.3%Ni		 46
Zhuang L Q
(2019)		 Spent LIBs
(LiNi0.5Co0.2Mn0.3O2)		 0.2 M Phosphoric acid +0.4 M Citric acid 90 ℃, 30 min 100% Li, 91.63%Co
92.00% Mn, 93.38%Ni		 47
Fig.4 Effect on leaching efficiency of (a) initial acid concentration, (b) solid/liquid ratio, (c) amount of H2O2, and (d) metal leaching efficiencies under optimized conditions[48]
Fig.5 The changing concentrations of metal ions in the solution through adjusting pH value of leaching solution(a, b) and the effect of different pH buffer(c, d) [55]
Fig.6 Mechanism and process of direct regeneration in spent cathode materials[70,71]
Fig.7 Schematic diagram of supercritical CO2 extraction of spent electrolyte(a), the components (b, c) and electrochemical window (d) of recovered electrolyte[100]
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