Ultra‐thin and Mechanically Stable LiCoO2‐Electrolyte Interphase Enabled by Mg2+ Involved Electrolyte

Author:

Liu Pei1,Huang Tao2,Xiao Biwei3,Zou Lianfeng4,Wang Kai4,Wang Kuan3,Wang Kai5,Yao Xiangming5,Liu Yuying1,Huang Zhencheng1,Wang Hongbin1,Liu Mijie6,Ren Xiaodi7,Ren Xiangzhong1,Ouyang Xiaoping1,Liu Jianhong18,zhang Qianling1,Hu Jiangtao1ORCID

Affiliation:

1. Graphene Composite Research Center College of Chemistry and Environmental Engineering Shenzhen University Shenzhen 518060 China

2. College of Energy Engineering Zhejiang University Hangzhou Zhejiang 310027 China

3. GRINM (Guangdong) Institute for Advanced Materials and Technology Foshan Guangdong 528051 China

4. Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 China

5. School of Advanced Materials Peking University Shenzhen Graduate School Shenzhen 518055 China

6. BASIS Bilingual School Shenzhen Nanshan District Shenzhen 518067 China

7. School of Chemistry and Materials Science University of Science and Technology of China Hefei 230026 China

8. Shenzhen Eigen‐Equation Graphene Technology Co. Ltd Shenzhen 518000 China

Abstract

AbstractLiCoO2 (LCO) cathode materials have attracted significant attention for its potential to provide higher energy density in current Lithium‐ion batteries (LIBs). However, the structure and performance degradation are exacerbated by increasing voltage due to the catastrophic reaction between the applied electrolyte and delithiated LCO. The present study focuses on the construction of physically and chemically robust Mg‐integrated cathode‐electrolyte interface (MCEI) to address this issue, by incorporating Magnesium bis(trifluoromethanesulfonyl)imide (Mg[TFSI]2) as an electrolyte additive. During formation cycles, the strong MCEI is formed and maintained its 2 nm thickness throughout long‐term cycling. Notably, Mg is detected not only in the robust MCEI, but also imbedded in the surface of the LCO lattice. As a result, the parasitic interfacial side reactions, surface phase reconstruction, particle cracking, Co dissolution and shuttling are considerably suppressed, resulting in long‐term cycling stability of LCO up to 4.5 V. Therefore, benefit from the double protection of the strong MCEI, the Li||LCO coin cell and the Ah‐level Graphite||LCO pouch cell exhibit high capacity retention by using Mg‐electrolyte, which are 88.13% after 200 cycles and 90.4% after 300 cycles, respectively. This work provides a novel approach for the rational design of traditional electrolyte additives.

Funder

National Natural Science Foundation of China

Publisher

Wiley

Subject

Biomaterials,Biotechnology,General Materials Science,General Chemistry

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