Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries

Qian Wu; Mandi Fang; Shizhe Jiao; Siyuan Li; Shichao Zhang; Zeyu Shen; Shulan Mao; Jiale Mao; Jiahui Zhang; Yuanzhong Tan; Kang Shen; Jiaxing Lv; Wei Hu; Yi He; Yingying Lu

doi:10.1038/s41467-023-41808-3

Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries

Nat Commun. 2023 Oct 9;14(1):6296. doi: 10.1038/s41467-023-41808-3.

Authors

Qian Wu^{1

2}, Mandi Fang³, Shizhe Jiao⁴, Siyuan Li^{1

2}, Shichao Zhang^{1

2}, Zeyu Shen^{1

2}, Shulan Mao^{1

2}, Jiale Mao^{1

2}, Jiahui Zhang^{1

2}, Yuanzhong Tan⁵, Kang Shen⁵, Jiaxing Lv⁵, Wei Hu⁴, Yi He^{3

6}, Yingying Lu^{7

8}

Affiliations

¹ State Key Laboratory of Chemical Engineering, Institute of Pharmaceutical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 310027, Hangzhou, Zhejiang, China.
² ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, 311215, Hangzhou, China.
³ College of Chemical and Biological Engineering, Zhejiang University, 310058, Hangzhou, Zhejiang, China.
⁴ School of Future Technology, Department of Chemical Physics, and Anhui Center for Applied Mathematics, University of Science and Technology of China, 230026, Hefei, China.
⁵ Innovation Research Institute of Technology Center, Zhejiang Xinan Chemical Industrial Group Co. ltd, 311600, Hangzhou, Zhejiang, China.
⁶ Department of Chemical Engineering, University of Washington, Seattle, WA, 98195, USA.
⁷ State Key Laboratory of Chemical Engineering, Institute of Pharmaceutical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 310027, Hangzhou, Zhejiang, China. yingyinglu@zju.edu.cn.
⁸ ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, 311215, Hangzhou, China. yingyinglu@zju.edu.cn.

Abstract

Solid polymer electrolytes with large-scale processability and interfacial compatibility are promising candidates for solid-state lithium metal batteries. Among various systems, poly(vinylidene fluoride)-based polymer electrolytes with residual solvent are appealing for room-temperature battery operations. However, their porous structure and limited ionic conductivity hinder practical application. Herein, we propose a phase regulation strategy to disrupt the symmetry of poly(vinylidene fluoride) chains and obtain the dense composite electrolyte through the incorporation of MoSe₂ sheets. The electrolyte with high dielectric constant can optimize the solvation structures to achieve high ionic conductivity and low activation energy. The in-situ reactions between MoSe₂ and Li metal generate Li₂Se fast conductor in solid electrolyte interphase, which improves the Coulombic efficiency and interfacial kinetics. The solid-state Li||Li cells achieve robust cycling at 1 mA cm^-2, and the Li||LiNi_0.8Co_0.1Mn_0.1O₂ full cells show practical performance at high rate (3C), high loading (2.6 mAh cm^-2) and in pouch cell.

Grants and funding

22022813 and 21878268/National Natural Science Foundation of China (National Science Foundation of China)