The dynamic evolution of aggregated lithium dendrites in lithium metal batteries

doi:10.1016/j.cjche.2021.05.008

中国化学工程学报 ›› 2021, Vol. 37 ›› Issue (9): 137-143.DOI: 10.1016/j.cjche.2021.05.008

• Energy Science and Technology • 上一篇下一篇

The dynamic evolution of aggregated lithium dendrites in lithium metal batteries

Xin Shen¹, Rui Zhang², Shuhao Wang³, Xiang Chen¹, Chuan Zhao³, Elena Kuzmina⁴, Elena Karaseva⁴, Vladimir Kolosnitsyn⁴, Qiang Zhang¹

1. Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China;
2. Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, China;
3. School of Chemistry, The University of New South Wales, Sydney, NSW 2052, Australia;
4. Ufa Institute of Chemistry UFRC RAS, Ufa, 450054, Russia

收稿日期:2021-01-27 修回日期:2021-04-16 出版日期:2021-09-28 发布日期:2021-11-02
通讯作者: Qiang Zhang
基金资助:
This work was supported by the National Natural Science Foundation of China (22061132002, U1801257, and 21825501), Russell Sage Foundation project (21-43-00006), the National Key Research and Development Program (2016YFA0200102 and 2016YFA0202500), Beijing Municipal Natural Science Foundation (Z20J00043), and the Tsinghua University Initiative Scientific Research Program.

The dynamic evolution of aggregated lithium dendrites in lithium metal batteries

Xin Shen¹, Rui Zhang², Shuhao Wang³, Xiang Chen¹, Chuan Zhao³, Elena Kuzmina⁴, Elena Karaseva⁴, Vladimir Kolosnitsyn⁴, Qiang Zhang¹

1. Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China;
2. Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, China;
3. School of Chemistry, The University of New South Wales, Sydney, NSW 2052, Australia;
4. Ufa Institute of Chemistry UFRC RAS, Ufa, 450054, Russia

Received:2021-01-27 Revised:2021-04-16 Online:2021-09-28 Published:2021-11-02
Contact: Qiang Zhang
Supported by:
This work was supported by the National Natural Science Foundation of China (22061132002, U1801257, and 21825501), Russell Sage Foundation project (21-43-00006), the National Key Research and Development Program (2016YFA0200102 and 2016YFA0202500), Beijing Municipal Natural Science Foundation (Z20J00043), and the Tsinghua University Initiative Scientific Research Program.

摘要/Abstract

摘要： Lithium (Li) metal anodes promise an ultrahigh theoretical energy density and low redox potential, thus being the critical energy material for next-generation batteries. Unfortunately, the formation of Li dendrites in Li metal anodes remarkably hinders the practical applications of Li metal anodes. Herein, the dynamic evolution of discrete Li dendrites and aggregated Li dendrites with increasing current densities is visualized by in-situ optical microscopy in conjunction with ex-situ scanning electron microscopy. As revealed by the phase field simulations, the formation of aggregated Li dendrites under high current density is attributed to the locally concentrated electric field rather than the depletion of Li ions. More specifically, the locally concentrated electric field stems from the spatial inhomogeneity on the Li metal surface and will be further enhanced with increasing current densities. Adjusting the above two factors with the help of the constructed phase field model is able to regulate the electrodeposited morphology from aggregated Li dendrites to discrete Li dendrites, and ultimately columnar Li morphology. The methodology and mechanistic understanding established herein give a significant step toward the practical applications of Li metal anodes.

关键词: Electrochemistry, Li dendrites, Rechargeable Li batteries, In-situ optical microscopy, Phase field model, Electrochemical engineering

Abstract: Lithium (Li) metal anodes promise an ultrahigh theoretical energy density and low redox potential, thus being the critical energy material for next-generation batteries. Unfortunately, the formation of Li dendrites in Li metal anodes remarkably hinders the practical applications of Li metal anodes. Herein, the dynamic evolution of discrete Li dendrites and aggregated Li dendrites with increasing current densities is visualized by in-situ optical microscopy in conjunction with ex-situ scanning electron microscopy. As revealed by the phase field simulations, the formation of aggregated Li dendrites under high current density is attributed to the locally concentrated electric field rather than the depletion of Li ions. More specifically, the locally concentrated electric field stems from the spatial inhomogeneity on the Li metal surface and will be further enhanced with increasing current densities. Adjusting the above two factors with the help of the constructed phase field model is able to regulate the electrodeposited morphology from aggregated Li dendrites to discrete Li dendrites, and ultimately columnar Li morphology. The methodology and mechanistic understanding established herein give a significant step toward the practical applications of Li metal anodes.

Key words: Electrochemistry, Li dendrites, Rechargeable Li batteries, In-situ optical microscopy, Phase field model, Electrochemical engineering

Xin Shen, Rui Zhang, Shuhao Wang, Xiang Chen, Chuan Zhao, Elena Kuzmina, Elena Karaseva, Vladimir Kolosnitsyn, Qiang Zhang. The dynamic evolution of aggregated lithium dendrites in lithium metal batteries[J]. 中国化学工程学报, 2021, 37(9): 137-143.

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The dynamic evolution of aggregated lithium dendrites in lithium metal batteries

The dynamic evolution of aggregated lithium dendrites in lithium metal batteries

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