Engineering a Dynamic Solvent-Phobic Liquid Electrolyte Interphase for Long-Life Lithium Metal Batteries

Qi Kang; Yong Li; Zechao Zhuang; Huijun Yang; Liuxuan Luo; Jie Xu; Jian Wang; Qinghua Guan; Han Zhu; Yinze Zuo; Dong Wang; Fei Pei; Lianbo Ma; Jin Zhao; Pengli Li; Ying Lin; Yijie Liu; Kunming Shi; Hongfei Li; Yingke Zhu; Jie Chen; Fei Liu; Guangning Wu; Jun Yang; Pingkai Jiang; Xingyi Huang

doi:10.1002/adma.202308799

Engineering a Dynamic Solvent-Phobic Liquid Electrolyte Interphase for Long-Life Lithium Metal Batteries

Adv Mater. 2024 Jan 25:e2308799. doi: 10.1002/adma.202308799. Online ahead of print.

Authors

Qi Kang¹, Yong Li², Zechao Zhuang³, Huijun Yang⁴, Liuxuan Luo⁵, Jie Xu⁶, Jian Wang⁷, Qinghua Guan⁷, Han Zhu⁸, Yinze Zuo⁹, Dong Wang¹⁰, Fei Pei¹¹, Lianbo Ma⁶, Jin Zhao¹², Pengli Li¹, Ying Lin¹, Yijie Liu¹, Kunming Shi¹, Hongfei Li¹, Yingke Zhu¹, Jie Chen¹, Fei Liu¹, Guangning Wu¹³, Jun Yang¹⁴, Pingkai Jiang¹, Xingyi Huang^{1

15}

Affiliations

¹ Department of Polymer Science and Engineering, Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
² Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology, University of Bremen, 28359, Bremen, Germany.
³ Department of Chemical Engineering, Columbia University, New York, NY, 10027, USA.
⁴ Graduate School of System and Information Engineering, University of Tsukuba, 1-1-1, Tennoudai, Tsukuba, 305-8573, Japan.
⁵ Department of Chemical and Biological Engineering, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, 999077, China.
⁶ School of Materials Science and Engineering, Anhui University of Technology, Ma'anshan, 243002, China.
⁷ School of Nano Technology and Nano Bionics, University of Science and Technology of China, Hefei, Anhui, 230026, China.
⁸ Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi, 214122, China.
⁹ School of Materials Science & Engineering, Fuzhou University, Fuzhou, Fujian, 350108, China.
¹⁰ Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, and Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials, Jilin University, Changchun, 130013, China.
¹¹ State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China.
¹² State Key Laboratory of Organic Electronics and Information Displays (KLOEID) and Jiangsu Key Laboratory for Biosensors, Institute of Advanced Materials (IAM), Nanjing University of Posts and Telecommunications, 9 Wenyuan Road, Nanjing, 210023, China.
¹³ Research Institute of Future Technology, School of Electrical Engineering, Southwest Jiaotong University, Chengdu, 611756, China.
¹⁴ Shanghai Electrochemical Energy Devices Research Center, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
¹⁵ Department of Electrical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.

PMID: 38270498
DOI: 10.1002/adma.202308799

Abstract

The heterogeneity, species diversity, and poor mechanical stability of solid electrolyte interphases (SEIs) in conventional carbonate electrolytes result in the irreversible exhaustion of lithium (Li) and electrolytes during cycling, hindering the practical applications of Li metal batteries (LMBs). Herein, this work proposes a solvent-phobic dynamic liquid electrolyte interphase (DLEI) on a Li metal (Li-PFbTHF (perfluoro-butyltetrahydrofuran)) surface that selectively transports salt and induces salt-derived SEI formation. The solvent-phobic DLEI with C-F-rich groups dramatically reduces the side reactions between Li, carbonate solvents, and humid air, forming a LiF/Li₃ PO₄ -rich SEI. In situ electrochemical impedance spectroscopy and Ab-initio molecular dynamics demonstrate that DLEI effectively stabilizes the interface between Li metal and the carbonate electrolyte. Specifically, the LiFePO₄ ||Li-PFbTHF cells deliver 80.4% capacity retention after 1000 cycles at 1.0 C, excellent rate capacity (108.2 mAh g^-1 at 5.0 C), and 90.2% capacity retention after 550 cycles at 1.0 C in full-cells (negative/positive (N/P) ratio of 8) with high LiFePO₄ loadings (15.6 mg cm^-2 ) in carbonate electrolyte. In addition, the 0.55 Ah pouch cell of 252.0 Wh kg^-1 delivers stable cycling. Hence, this study provides an effective strategy for controlling salt-derived SEI to improve the cycling performances of carbonate-based LMBs.

Keywords: air tolerance; dynamic liquid electrolyte interphase; high loading; long-life; solvent-phobic.

Abstract

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