金属锂负极失效机制及其先进表征技术

doi:10.3866/PKU.WHXB202005012

物理化学学报 >> 2021, Vol. 37 >> Issue (2): 2005012.doi: 10.3866/PKU.WHXB202005012

所属专题：金属锂负极

金属锂负极失效机制及其先进表征技术

岳昕阳¹, 马萃¹, 包戬¹, 杨思宇², 陈东¹, 吴晓京¹, 周永宁¹^,*()

¹ 复旦大学材料科学系，上海 200433
² 复旦大学化学系，上海 200433

收稿日期:2020-05-06 录用日期:2020-06-04 发布日期:2020-06-10
通讯作者: 周永宁 E-mail:ynzhou@fudan.edu.cn
作者简介:周永宁，复旦大学青年研究员。2010年在复旦大学材料科学系获得博士学位；2010–2011年复旦大学化学系从事博士后研究；2012–2015年在美国布鲁克海文国家实验室任助理研究员；2015年回国加入复旦大学材料科学系，任青年研究员。主要从事新型电池材料设计及机理研究第一联系人：
^†These authors contributed equally to this work.
基金资助:
上海市自然科学基金(19ZR1404200)

Failure Mechanisms of Lithium Metal Anode and Their Advanced Characterization Technologies

Xinyang Yue¹, Cui Ma¹, Jian Bao¹, Siyu Yang², Dong Chen¹, Xiaojing Wu¹, Yongning Zhou¹^,*()

¹ Department of Materials Science, Fudan University, Shanghai 200433, China
² Department of Chemistry, Fudan University, Shanghai 200433, China

Received:2020-05-06 Accepted:2020-06-04 Published:2020-06-10
Contact: Yongning Zhou E-mail:ynzhou@fudan.edu.cn
About author:Yongning Zhou, Email: ynzhou@fudan.edu.cn; Tel.: +86-21-65642685
Supported by:
the Science & Technology Commission of Shanghai Municipality, China(19ZR1404200)

摘要/Abstract

摘要：

尽管传统的石墨负极在商业化锂离子电池中取得了成功，但其理论容量低(372 mAh·g^-1)、本身不含锂的先天缺陷限制了其在下一代高比能量锂电池体系中的应用，特别是在需要锂源的锂-硫和锂-空气电池体系中。金属锂因其极高的理论比容量(3860 mAh·g^-1)和低氧化还原电势(相对于标准氢电极为-3.040 V)，被认为是下一代锂电池负极材料的最佳选择之一。但是，金属锂负极存在库伦效率低、循环性能差、安全性差等一系列瓶颈问题亟待解决，而循环过程中锂枝晶的生长、巨大的体积变化、以及电极界面不稳定等是导致这些问题的关键因素。本文综述了近年来关于金属锂负极瓶颈问题及其机理，包括金属锂电极表面固态电解质界面膜的形成，锂枝晶的生长行为，以及惰性死锂的形成。同时，本文还介绍了目前用于研究金属锂负极的先进表征技术，这些技术为研究人员深入认识金属锂负极的失效机制提供了重要信息。

关键词: 锂电池, 金属锂负极, 失效机制, 先进表征技术

Abstract:

Although traditional graphite anodes ensure the cycling stability and safety of lithium-ion batteries, the inherent drawbacks, particularly low theoretical specific capacity (372 mAh·g^-1) and Li-free character, of such anodes limit their applications in high energy density battery systems, especially in lithium-sulfur and lithium-air batteries. Lithium metal has been considered as one of the best next-generation anode materials due to its extremely high theoretical specific capacity (3860 mAh·g^-1) and low redox potential (-3.04 V vs. the standard hydrogen electrode). The first generation of commercial rechargeable lithium metal batteries were developed by Moli Energy in the late 1980s and were not widely used due to several problems, including low coulombic efficiency, poor cycle stability, and safety hazards. These problems associated with the Li metal anode are mainly caused by lithium dendrite growth, electrode volume changes, and interface instability. During the charge and discharge processes, Li deposition is not uniform across the electrode surface. Due to the low surface energy and high migration energy of Li metal, dendrites are preferentially formed during Li deposition. These dendrites proceed to grow with successive battery cycling, penetrate the separator, and eventually reach the cathode, thereby causing short circuits and thermal runaway. Additionally, the growth of the lithium dendrite is inherently correlated with the reaction interface structure, and dendrite growth results in inhomogeneity of the SEI (solid electrolyte interface) which is inevitably formed on the Li metal surfaces. Moreover, the volume change of lithium metal anodes is of importance, particularly during battery cycling and Li stripping/deposition processes which make the SEI layers considerably unstable. SEI layers usually cannot withstand the mechanical deformation caused by volume changes; such layers continuously break and repair during cycling and consume large amounts of the electrolyte. Additionally, some Li dendrites could break and become wrapped by SEI layers to form electrically isolated "dead" Li, which results in the loss of active Li in the Li metal anode. All these factors are responsible for the failure of Li metal anodes. Herein, recent investigations on the failure mechanisms of lithium metal anodes are reviewed and summarized, including the formation of SEI layers on the surface of Li metal anodes, the behavior and mechanism of lithium dendrite growth, and the mechanism of "dead" lithium formation. Additionally, some advanced characterization techniques for investigating lithium metal anodes are introduced, including in situ tools, cryo-electron microscopy, neutron depth analysis technology, and solid state nuclear magnetic resonance technology. These techniques enable researchers to gain in-depth insights into the failure mechanisms of Li metal anodes.

Key words: Lithium battery, Lithium metal anode, Failure mechanism, Advanced characterization technology

岳昕阳, 马萃, 包戬, 杨思宇, 陈东, 吴晓京, 周永宁. 金属锂负极失效机制及其先进表征技术[J]. 物理化学学报, 2021, 37(2), 2005012. doi: 10.3866/PKU.WHXB202005012

Xinyang Yue, Cui Ma, Jian Bao, Siyu Yang, Dong Chen, Xiaojing Wu, Yongning Zhou. Failure Mechanisms of Lithium Metal Anode and Their Advanced Characterization Technologies[J]. Acta Phys. -Chim. Sin. 2021, 37(2), 2005012. doi: 10.3866/PKU.WHXB202005012

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202005012

https://www.whxb.pku.edu.cn/CN/Y2021/V37/I2/2005012

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金属锂负极失效机制及其先进表征技术

Failure Mechanisms of Lithium Metal Anode and Their Advanced Characterization Technologies

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