Simultaneous Stabilization of Lithium Anode and Cathode using Hyperconjugative Electrolytes for High‐voltage Lithium Metal Batteries

Author:

Zhang Haikuo1,Li Ruhong1,Chen Long12,Fan Yingzhu3,Zhang Hao4,Zhang Ruixin4,Zheng Lei3,Zhang Junbo15,Ding Shouhong4,Wu Yongjian4,Ma Baochen1,Zhang Shuoqing1,Deng Tao6,Chen Lixin17,Shen Yanbin3,Fan Xiulin1ORCID

Affiliation:

1. State Key Laboratory of Silicon Materials School of Materials Science and Engineering Zhejiang University Hangzhou 310027 China

2. Polytechnic Institute Zhejiang University Hangzhou 310027 China

3. i-Lab CAS Center for Excellence in Nanoscience Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO) Chinese Academy of Sciences Suzhou 215123 P. R. China

4. Youtu Lab Tencent, No. 397 Tianlin Road Xuhui District Shanghai 200233 China

5. Shenyang National Laboratory for Materials Science Northeastern University Shenyang 110819 China

6. Department of Chemical and Biomolecular Engineering University of Maryland College Park MD 20742 USA

7. Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province Hangzhou 310013 China

Abstract

AbstractAlthough great progress has been made in new electrolytes for lithium metal batteries (LMBs), the intrinsic relationship between electrolyte composition and cell performance remains unclear due to the lack of valid quantization method. Here, we proposed the concept of negative center of electrostatic potential (NCESP) and Mayer bond order (MBO) to describe solvent capability, which highly relate to solvation structure and oxidation potential, respectively. Based on established principles, the selected electrolyte with 1.7 M LiFSI in methoxytrimethylsilane (MOTMS)/ (trifluoromethyl)trimethylsilane (TFMTMS) shows unique hyperconjugation nature to stabilize both Li anode and high‐voltage cathode. The 4.6 V 30 μm Li||4.5 mAh cm−2 lithium cobalt oxide (LCO) (low N/P ratio of 1.3) cell with our electrolyte shows stable cycling with 91 % capacity retention over 200 cycles. The bottom‐up design concept of electrolyte opens up a general strategy for advancing high‐voltage LMBs.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Zhejiang Province

Publisher

Wiley

Subject

General Medicine

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