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化学进展 2020, Vol. 32 Issue (7): 950-965 DOI: 10.7536/PC191106 前一篇   后一篇

所属专题： 锂离子电池

• 综述 •

废旧锂离子电池正极材料及电解液的全过程回收及再利用

穆德颖1,3, 刘铸1, 金珊1, 刘元龙1, 田爽2,**(), 戴长松1,**()   

  1. 1. 哈尔滨工业大学化工与化学学院 哈尔滨 150001
    2. 中国科学院宁波材料技术与工程研究所 宁波 315201
    3. 哈尔滨商业大学食品工程学院 哈尔滨 150076
  • 收稿日期:2019-11-08 出版日期:2020-07-24 发布日期:2020-07-10
  • 通讯作者: 田爽, 戴长松
  • 基金资助:
    宁波市科技创新2025重大专项(2019B10114); 黑龙江省教育厅创新人才培养计划项目(UNPYSCT-2018138)
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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:2019-11-08 Online:2020-07-24 Published:2020-07-10
  • 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)

作为发展势头迅猛的新型储能形式,锂离子电池缓解了能源领域对化石燃料的依赖,同时减轻了日益严峻的环境压力,但是数量巨大的废旧锂离子电池具有危险废弃物和高附加值可用资源的双重属性。因此,通过不同技术手段的创新和组合,实现组成成分日益多样化的废旧锂离子电池的高效回收和再利用具有巨大的挑战和特殊重要的现实意义。本文从预处理工艺出发,详细阐述了放电失活、分类拆解、粉碎筛分、酸浸除杂等一系列过程的技术手段和要求;从原料再生、结构修复以及再制备三个方面探讨了具有代表性的再利用思路,分析了各技术方法的优势和存在的问题。此外,对废旧电解液的无害化处理和回收进行了专题讨论,重点介绍了超临界CO2萃取工艺。最后,针对现阶段存在的问题提出展望,为后续开展废旧锂离子电池回收的相关研究及工业应用提供参考。

关键词： 废旧锂离子电池, 回收再利用, 预处理, 材料合成, 电解液, 超临界CO2萃取

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
()
图1 全球日平均CO2含量及CO2辐射强迫[3]
Fig.1 Daily averaged CO2 from four global monitoring division baseline observatories and CO2 radiative forcing[3]
图2 废旧锂离子电池回收处理的分类及再利用最终产物
Fig.2 Classification of battery recycling processes and final reused products
图3 废旧锂离子电池预处理全过程分类简图
Fig.3 Simplified diagram of whole pretreatment processes for spent lithium ion batteries
表1 近三年利用有机和无机酸浸出废旧锂离子电池的代表性研究工作
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
图4 不同条件对浸出效率的影响:(a)初始乳酸浓度,(b)固液比,(c)双氧水用量,(d)在优化条件下,各金属的浸出效率[48]
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]
图5 在不同pH条件下,浸出溶液中金属离子的浓度变化及不同缓冲液的影响[55]
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]
图6 废旧正极材料直接修复的原理与过程[70,71]
Fig.6 Mechanism and process of direct regeneration in spent cathode materials[70,71]
图7 超临界CO2萃取废旧锂离子电池电解液过程演示(a)及再利用电解液成分(b和c)及电化学窗口(d)[100]
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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