Stable Operation of Lithium Metal Batteries with Aggressive Cathode Chemistries at 4.9 V

Author:

Piao Zhihong1,Ren Hong‐Rui1,Lu Gongxun12,Jia Kai1,Tan Junyang1,Wu Xinru1,Zhuang Zhaofeng1,Han Zhiyuan1,Li Chuang1,Gao Runhua1,Tao Xinyong2,Zhou Guangmin1,Cheng Hui‐Ming13ORCID

Affiliation:

1. Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 P. R. China

2. College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

3. Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 P. R. China

Abstract

AbstractHigh‐voltage lithium metal batteries (LMBs) pose severe challenges for the matching of electrolytes with aggressive electrodes, especially at low temperatures. Here, we report a rational modification of the Li+solvation structure to extend the voltage and temperature operating ranges of conventional electrolytes. Ion‐ion and ion‐dipole interactions as well as the electrochemical window of solvents were tailored to improve oxidation stability and de‐solvation kinetics of the electrolyte. Meanwhile, robust and elastic B and F‐rich interphases are formed on both electrodes. Such optimization enables Li||LiNi0.5Mn1.5O4cells (90.2 % retention after 400 cycles) and Li||LiNi0.6Co0.2Mn0.2O2(NCM622) cells (74.0 % retention after 200 cycles) to cycle stably at an ultra‐high voltage of 4.9 V. Moreover, NCM622 cells deliver a considerable capacity of 143.5 mAh g−1at −20 °C, showing great potential for practical uses. The proposed strategy sheds light on further optimization for high‐voltage LMBs.

Funder

National Key Research and Development Program of China

National Natural Science Foundation of China

Guangdong Province Introduction of Innovative R&D Team

Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute

Publisher

Wiley

Subject

General Chemistry,Catalysis

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