Plasma Coupled Electrolyte Additive Strategy for Construction of High‐Performance Solid Electrolyte Interphase on Li Metal Anodes

Author:

Liu Ping12,Shen Shenghui3,Qiu Zhong1,Yang Tianqi2,Liu Yaning2,Su Han1,Zhang Yongqi4,Li Jingru1,Cao Feng5,Zhong Yu1,Liang Xinqi46,Chen Minghua6,He Xinping2,Xia Yang2,Wang Chen7,Wan Wangjun7,Tu Jiangping1,Zhang Wenkui2,Xia Xinhui12ORCID

Affiliation:

1. State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province, and Department of Materials Science and Engineering Zhejiang University Hangzhou 310027 P. R. China

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

3. School of Materials Science and Engineering Zhejiang Sci‐Tech University Hangzhou 310018 China

4. Institute of Fundamental and Frontier Science University of Electronic Science and Technology of China Chengdu 611371 China

5. Department of Engineering Technology Huzhou College Huzhou 313000 P. R. China

6. Key Laboratory of Engineering Dielectric and Applications (Ministry of Education) School of Electrical and Electronic Engineering Harbin University of Science and Technology Harbin 150080 P. R. China

7. Zhejiang Academy of Science and Technology for Inspection & Quarantine Hangzhou Zhejiang 311215 P. R. China

Abstract

AbstractHigh‐performance lithium metal anodes are crucial for the development of advanced Li metal batteries. Herein, this work reports a novel plasma coupled electrolyte additive strategy to prepare high‐quality composite solid electrolyte interphase (SEI) on Li metal to achieve enhanced performance and stability. With the guidance of calculations, this work selects diethyl dibromomalonate (DB) as an additive to optimize the solvation structure of electrolytes to modify the SEI. Meanwhile, this work groundbreakingly develops DB plasma technology coupled with DB electrolyte additive to construct a combinatorial SEI: inner plasma‐induced SEI layer composed of LiBr and Li2CO3 plus additive‐reduced SEI containing LiBr/Li2CO3/organic lithium compounds as an outer compatible layer. The optimized hybrid SEI has strong affinity toward Li+ and good mechanical properties, thereby inducing horizontal dispersion and uniform deposition of Li+ and keep structure stable. Accordingly, the symmetrical cells exhibit enhanced cycling stability for 1200 h at an overpotential of 23.8 mV with average coulombic efficiency (99.51%). Additionally, the full cells with LiNi0.8Co0.1Mn0.1O2 cathode deliver a capacity retention of 81.7% after 300 cycles at 0.5 C, and the pouch cell achieves a volumetric specific energy of ≈664 Wh L‒1. This work provides new enlightenment on plasma technology for fabrication of advanced metal anodes for energy storage.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Zhejiang Province

Key Laboratory of Engineering Dielectrics and Its Application (Harbin University of Science and Technology), Ministry of Education

Publisher

Wiley

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