Stable Interface Chemistry and Multiple Ion Transport of Composite Electrolyte Contribute to Ultra-long Cycling Solid-State LiNi0.8 Co0.1 Mn0.1 O2 /Lithium Metal Batteries

Ke Yang; Likun Chen; Jiabin Ma; Chen Lai; Yanfei Huang; Jinshuo Mi; Jie Biao; Danfeng Zhang; Peiran Shi; Heyi Xia; Guiming Zhong; Feiyu Kang; Yan-Bing He

doi:10.1002/anie.202110917

Stable Interface Chemistry and Multiple Ion Transport of Composite Electrolyte Contribute to Ultra-long Cycling Solid-State LiNi_0.8 Co_0.1 Mn_0.1 O₂ /Lithium Metal Batteries

Angew Chem Int Ed Engl. 2021 Nov 8;60(46):24668-24675. doi: 10.1002/anie.202110917. Epub 2021 Oct 7.

Authors

Ke Yang^{1

2}, Likun Chen^{1

2}, Jiabin Ma^{1

2}, Chen Lai³, Yanfei Huang⁴, Jinshuo Mi^{1

2}, Jie Biao^{1

2}, Danfeng Zhang^{1

2}, Peiran Shi^{1

2}, Heyi Xia¹, Guiming Zhong⁵, Feiyu Kang^{1

2}, Yan-Bing He¹

Affiliations

¹ Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR), Tsinghua Shenzhen International Graduate School, Shenzhen, 518055, P. R. China.
² School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, P. R. China.
³ Key Lab of Advanced Functional Materials, Ministry of Education, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100084, P. R. China.
⁴ College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518055, P. R. China.
⁵ Laboratory of Advanced Spectro-electrochemistry and Li-ion Batteries, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China.

PMID: 34498788
DOI: 10.1002/anie.202110917

Abstract

Severe interfacial side reactions of polymer electrolyte with LiNi_0.8 Co_0.1 Mn_0.1 O₂ (NCM811) cathode and Li metal anode restrict the cycling performance of solid-state NCM811/Li batteries. Herein, we propose a chemically stable ceramic-polymer-anchored solvent composite electrolyte with high ionic conductivity of 6.0×10^-4 S cm^-1 , which enables the solid-state NCM811/Li batteries to cycle 1500 times. The Li_1.4 Al_0.4 Ti_1.6 (PO₄ )₃ nanowires (LNs) can tightly anchor the essential N, N-dimethylformamide (DMF) in poly(vinylidene fluoride) (PVDF), greatly enhancing its electrochemical stability and suppressing the side reactions. We identify the ceramic-polymer-liquid multiple ion transport mechanism of the LNs-PVDF-DMF composite electrolyte by tracking the ⁶ Li and ⁷ Li substitution behavior via solid-state NMR. The stable interface chemistry and efficient ion transport of LNs-PVDF-DMF contribute to superior performances of the solid-state batteries at wide temperature range of -20-60 °C.

Keywords: composite electrolytes; interface chemistry; multiple ion transport; solid-state lithium metal batteries.

Abstract

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