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Vol. 14 (2022)

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

https://doi.org/10.1007/s40820-022-00952-z
Xinyang Li
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
Yong Wang
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
Kai Xi
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
Wei Yu
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
Jie Feng
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
Guoxin Gao
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
Hu Wu
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
Qiu Jiang
Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou, Zhejiang 313001, People’s Republic of China
Amr Abdelkader
Faculty of Science and Technology, Bournemouth University, Talbot Campus, Fern Barrow, Poole BH12 5BB, UK
Weibo Hua
Institute for Applied Materials-Energy Storage Systems (IAM-ESS), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein‑Leopoldshafen, Germany
Guiming Zhong
Laboratory of Advanced Spectroelectrochemsitry and Li‑ion Batteries, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
Shujiang Ding
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

Corresponding Author: Shujiang Ding

dingsj@mail.xjtu.edu.cn

Nano-Micro Letters, Vol. 14 (2022), Article Number: 210

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.


Highlights:


1 The composite gel electrolyte with low tortuosity ion-conducting arrays (GPE/ICAs) exhibiting high room-temperature ionic conductivity (1.08 mS cm−1) was successfully prepared by directionally growing ice crystals and in-situ polymerization.
2 The stable and rapid Li+ migration through ICAs in the GPE is proved by 6Li solid-state nuclear magnetic resonance and synchrotron radiation X-ray diffraction combined with computer simulations.
3 Li/LiFePO4 full cells using GPE/ICAs exhibit excellent cycle performance and high-capacity retention at wide temperature (0–60 °C), which has the potential towards all-weather practical solid-state batteries.

Keywords

Solid-state batteries Composite electrolytes Vertical-aligned ion-conducting arrays Interfacial ion-conduction mechanism All-weather practical electrolyte design
Li, Xinyang, Yong Wang, Kai Xi, Wei Yu, Jie Feng, Guoxin Gao, Hu Wu, Qiu Jiang, Amr Abdelkader, Weibo Hua, Guiming Zhong, and Shujiang Ding. 2022. “Quasi-Solid-State Ion-Conducting Arrays Composite Electrolytes With Fast Ion Transport Vertical-Aligned Interfaces for All-Weather Practical Lithium-Metal Batteries”. Nano-Micro Letters 14 (October):210. https://doi.org/10.1007/s40820-022-00952-z.
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