Reconstruction of Solid Electrolyte Interphase with SrI2 Reactivates Dead Li for Durable Anode-Free Li-Metal Batteries

Liwei Dong; Shijie Zhong; Botao Yuan; Yaqiang Li; Jipeng Liu; Yuanpeng Ji; Dongjiang Chen; Yuanpeng Liu; Chunhui Yang; Jiecai Han; Weidong He

doi:10.1002/anie.202301073

Reconstruction of Solid Electrolyte Interphase with SrI₂ Reactivates Dead Li for Durable Anode-Free Li-Metal Batteries

Angew Chem Int Ed Engl. 2023 Jun 5;62(23):e202301073. doi: 10.1002/anie.202301073. Epub 2023 Apr 26.

Authors

Liwei Dong^{1

2

3}, Shijie Zhong¹, Botao Yuan¹, Yaqiang Li³, Jipeng Liu², Yuanpeng Ji^{2

4}, Dongjiang Chen⁴, Yuanpeng Liu¹, Chunhui Yang^{2

3}, Jiecai Han¹, Weidong He^{1

4

5}

Affiliations

¹ National Key Laboratory of Science and Technology on Advanced Composites in Special Environments, and Center for Composite Materials and Structures, Harbin Institute of Technology, Harbin, 150080, China.
² MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150080, China.
³ State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin, 150080, China.
⁴ Chongqing Research Institute, Harbin Institute of Technology, Chongqing, 401151, China.
⁵ School of Mechanical Engineering, Chengdu University, Chengdu, 610106, China.

PMID: 37011095
DOI: 10.1002/anie.202301073

Abstract

Without excess Li, anode-free Li-metal batteries (AFLMBs) have been proposed as the most likely solution to realizing highly-safe and cost-effective Li-metal batteries. Nevertheless, short cyclic life puzzles conventional AFLMBs due to anodic dead Li accumulation with a local current concentration induced by irreversible electrolyte depletion, insufficient active Li reservoir and slow Li⁺ transfer at the solid electrolyte interphase (SEI). Herein, SrI₂ is introduced into carbon paper (CP) current collector to effectively suppress dead Li through synergistic mechanisms including reversible I^- /I₃ ^- redox reaction to reactivate dead Li, dielectric SEI surface with SrF₂ and LiF to prevent electrolyte decomposition and highly ionic conductive (3.488 mS cm^-1 ) inner layer of SEI with abundant LiI to enable efficient Li⁺ transfer inside. With the SrI₂ -modified current collector, the NCM532/CP cell delivers unprecedented cyclic performances with a capacity of 129.2 mAh g^-1 after 200 cycles.

Keywords: Anode-Free Li-Metal Batteries; Current Collector; Dead Li; SrF2; SrI2.

Abstract

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