Quasi-Solid-State Ion-Conducting Arrays Composite Electrolytes with Fast Ion Transport Vertical-Aligned Interfaces for All-Weather Practical Lithium-Metal Batteries

Xinyang Li; Yong Wang; Kai Xi; Wei Yu; Jie Feng; Guoxin Gao; Hu Wu; Qiu Jiang; Amr Abdelkader; Weibo Hua; Guiming Zhong; Shujiang Ding

doi:10.1007/s40820-022-00952-z

Quasi-Solid-State Ion-Conducting Arrays Composite Electrolytes with Fast Ion Transport Vertical-Aligned Interfaces for All-Weather Practical Lithium-Metal Batteries

Nanomicro Lett. 2022 Oct 31;14(1):210. doi: 10.1007/s40820-022-00952-z.

Authors

Xinyang Li¹, Yong Wang^{1

2}, Kai Xi¹, Wei Yu¹, Jie Feng¹, Guoxin Gao^{1

3}, Hu Wu¹, Qiu Jiang^{4

5}, Amr Abdelkader⁶, Weibo Hua^{7

8}, Guiming Zhong⁹, Shujiang Ding¹⁰

Affiliations

¹ School of Chemistry, Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, State Key Laboratory of Electrical Insulation and Power Equipment, Xi'an Jiaotong University, Xi'an, 710049, People's Republic of China.
² State Key Laboratory for Mechanical Behaviour of Materials, Xi'an Jiaotong University, Xi'an, 710049, People's Republic of China.
³ State Key Laboratory of Organic-inorganic Composites, Beijing University of Chemical Technology, Beijing, 100029, People's Republic of China.
⁴ Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou, Zhejiang, 313001, People's Republic of China.
⁵ School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 610054, People's Republic of China.
⁶ Faculty of Science and Technology, Bournemouth University, Talbot Campus, Fern Barrow, Poole, BH12 5BB, UK.
⁷ Institute for Applied Materials-Energy Storage Systems (IAM-ESS), Karlsruhe Institute of Technology (KIT), 76344, Eggenstein-Leopoldshafen, Germany.
⁸ School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, Shaanxi, 710049, People's Republic of China.
⁹ Laboratory of Advanced Spectroelectrochemsitry and Li-ion Batteries, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, People's Republic of China.
¹⁰ School of Chemistry, Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, State Key Laboratory of Electrical Insulation and Power Equipment, Xi'an Jiaotong University, Xi'an, 710049, People's Republic of China. dingsj@mail.xjtu.edu.cn.

Abstract

The rapid improvement in the gel polymer electrolytes (GPEs) with high ionic conductivity brought it closer to practical applications in solid-state Li-metal batteries. The combination of solvent and polymer enables quasi-liquid fast ion transport in the GPEs. However, different ion transport capacity between solvent and polymer will cause local nonuniform Li⁺ distribution, leading to severe dendrite growth. In addition, the poor thermal stability of the solvent also limits the operating-temperature window of the electrolytes. Optimizing the ion transport environment and enhancing the thermal stability are two major challenges that hinder the application of GPEs. Here, a strategy by introducing ion-conducting arrays (ICA) is created by vertical-aligned montmorillonite into GPE. Rapid ion transport on the ICA was demonstrated by ⁶Li solid-state nuclear magnetic resonance and synchrotron X-ray diffraction, combined with computer simulations to visualize the transport process. Compared with conventional randomly dispersed fillers, ICA provides continuous interfaces to regulate the ion transport environment and enhances the tolerance of GPEs to extreme temperatures. Therefore, GPE/ICA exhibits high room-temperature ionic conductivity (1.08 mS cm^-1) and long-term stable Li deposition/stripping cycles (> 1000 h). As a final proof, Li||GPE/ICA||LiFePO₄ cells exhibit excellent cycle performance at wide temperature range (from 0 to 60 °C), which shows a promising path toward all-weather practical solid-state batteries.

Keywords: All-weather practical electrolyte design; Composite electrolytes; Interfacial ion-conduction mechanism; Solid-state batteries; Vertical-aligned ion-conducting arrays.