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

Haikuo Zhang; Ruhong Li; Long Chen; Yingzhu Fan; Hao Zhang; Ruixin Zhang; Lei Zheng; Junbo Zhang; Shouhong Ding; Yongjian Wu; Baochen Ma; Shuoqing Zhang; Tao Deng; Lixin Chen; Yanbin Shen; Xiulin Fan

doi:10.1002/anie.202218970

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

Angew Chem Int Ed Engl. 2023 Mar 6;62(11):e202218970. doi: 10.1002/anie.202218970. Epub 2023 Feb 6.

Authors

Haikuo Zhang¹, Ruhong Li¹, Long Chen^{1

2}, Yingzhu Fan³, Hao Zhang⁴, Ruixin Zhang⁴, Lei Zheng³, Junbo Zhang^{1

5}, Shouhong Ding⁴, Yongjian Wu⁴, Baochen Ma¹, Shuoqing Zhang¹, Tao Deng⁶, Lixin Chen^{1

7}, Yanbin Shen³, Xiulin Fan¹

Affiliations

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.

PMID: 36688728
DOI: 10.1002/anie.202218970

Abstract

Although 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.

Keywords: Bottom-up Design; Hyperconjugative Electrolyte; Lithium Metal Battery; Molecule Descriptor.

Abstract

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