A Quasi-Double-Layer Solid Electrolyte with Adjustable Interphases Enabling High-Voltage Solid-State Batteries

Jun Pan; Yuchen Zhang; Jian Wang; Zhongchao Bai; Ruiguo Cao; Nana Wang; Shixue Dou; Fuqiang Huang

doi:10.1002/adma.202107183

A Quasi-Double-Layer Solid Electrolyte with Adjustable Interphases Enabling High-Voltage Solid-State Batteries

Adv Mater. 2022 Mar;34(10):e2107183. doi: 10.1002/adma.202107183. Epub 2022 Jan 30.

Authors

Jun Pan¹, Yuchen Zhang², Jian Wang³, Zhongchao Bai⁴, Ruiguo Cao², Nana Wang⁵, Shixue Dou⁵, Fuqiang Huang^{1

6}

Affiliations

¹ State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Science, Shanghai, 200050, P. R. China.
² Hefei National Laboratory for Physical Science at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, P. R. China.
³ School of Life Science and Technology, ShanghaiTech University, Shanghai, 200050, P. R. China.
⁴ College of Mechanical and Electronic Engineering, Shandong University of Science and Technology, Qingdao, 266590, P. R. China.
⁵ Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Innovation Campus, North Wollongong, New South Wales, 2500, Australia.
⁶ State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.

PMID: 34699655
DOI: 10.1002/adma.202107183

Abstract

Increasing the energy density and long-term cycling stability of lithium-ion batteries necessitates the stability of electrolytes under high/low voltage application and stable electrode/electrolyte interfacial contact. However, neither a single polymer nor liquid electrolyte can realize this due to their limited internal energy gap, which cannot avoid lithium-metal deposition and electrolyte oxidation simultaneously. Herein, a novel type of quasi-double-layer composite polymer electrolytes (QDL-CPEs) is proposed by using plasticizers with high oxidation stability (propylene carbonate) and high reduction stability (diethylene glycol dimethyl ether) in a poly(vinylidene fluoride) (PVDF)-based electrolyte composites. In-situ-polymerized propylene carbonate can function as a cathode electrolyte interface (CEI) film, which can enhance the antioxidant ability. The nucleophilic substitution reaction between diethylene glycol dimethyl ether and PVDF increases the reduction stability of the electrolyte on the anodic side, without the formation of lithium dendrites. The QDL-CPEs has high ionic conductivity, an enhanced electrochemical reaction window, adjustable electrode/electrolyte interphases, and no additional electrolyte-electrolyte interfacial resistance. Thus, this ingenious design of the QDL-CPEs improves the cycling performance of a fabricated LiNi_0.8 Co_0.1 Mn_0.1 O₂ (NCM811)//QDL-CPEs//hard carbon full cell at room temperature, paving a new way for designing solid-state battery systems accessible for practical applications.

Keywords: artificial cathode electrolyte interface; high redox stability; polymer solid-state lithium-ion batteries; quasi-double-layer solid electrolytes; stable interfacial contact.

Abstract

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