Matchmaker of Marriage between a Li Metal Anode and NASICON-Structured Solid-State Electrolyte: Plastic Crystal Electrolyte and Three-Dimensional Host Structure

Zizheng Tong; Shu-Bo Wang; Anirudha Jena; Chia-Erh Liu; Shih-Chieh Liao; Jin-Ming Chen; Ho Chang; Shu-Fen Hu; Xiangxin Guo; Ru-Shi Liu

doi:10.1021/acsami.0c12962

Matchmaker of Marriage between a Li Metal Anode and NASICON-Structured Solid-State Electrolyte: Plastic Crystal Electrolyte and Three-Dimensional Host Structure

ACS Appl Mater Interfaces. 2020 Oct 7;12(40):44754-44761. doi: 10.1021/acsami.0c12962. Epub 2020 Sep 25.

Authors

Zizheng Tong¹, Shu-Bo Wang¹, Anirudha Jena^{1

2}, Chia-Erh Liu³, Shih-Chieh Liao³, Jin-Ming Chen³, Ho Chang², Shu-Fen Hu⁴, Xiangxin Guo⁵, Ru-Shi Liu¹

Affiliations

¹ Department of Chemistry, National Taiwan University, Taipei 106, Taiwan.
² Department of Mechanical Engineering and Graduate Institute of Manufacturing Technology, National Taipei University of Technology, Taipei 106, Taiwan.
³ Material and Chemical Research Laboratories, Industrial Technology Research Institute, Hsinchu 300, Taiwan.
⁴ Department of Physics, National Taiwan Normal University, Taipei 116, Taiwan.
⁵ College of Physics, Qingdao University, Qingdao 266071, China.

PMID: 32917086
DOI: 10.1021/acsami.0c12962

Abstract

The marriage between a Li metal anode and the solid-state electrolyte is expected to limit the safety risk of secondary batteries. However, dendrites and interfacial stability hinder the combination of Li metal anode and solid-state electrolyte. Herein, a plastic crystal electrolyte (PCE) and three-dimensional (3D) host structure played the role of a matchmaker in combining the solid-state electrolyte and Li metal anode. Succinonitrile cooperated with Li salt and Li_6.4La₃Zr_1.4Ta_0.6O₁₂ nanosize powder and built a PCE interphase, which enhanced the interfacial stability between Li_1.5Al_0.5Ge_1.5(PO₄)₃ and Li metal anode. To protect the soft PCE from the dendrite penetration, commercially sold Super P, carbon nanotube, KS6, and Ketjen black were co-heated with the melted Li metal. However, only KS6 built a 3D host in Li metal successfully because of its high graphitization and layered structure. Benefitting from the matchmakers, the solid-state batteries exhibited enhanced cycling stability.

Keywords: LAGP; plastic crystal electrolyte; solid-state battery; solid-state electrolyte; three-dimensional host structure.