In situ electrochemical modification of the Li/Li1.3Al0.3Ti1.7(PO4)3 interface in solid lithium metal batteries via an electrolyte additive

Yadong Xu; Meng Tian; Yi Rong; Chengyi Lu; Zhengyi Lu; Ruhua Shi; Tianyi Gu; Qian Zhang; Chengchang Jin; Ruizhi Yang

doi:10.1016/j.jcis.2023.03.069

In situ electrochemical modification of the Li/Li_1.3Al_0.3Ti_1.7(PO₄)₃ interface in solid lithium metal batteries via an electrolyte additive

J Colloid Interface Sci. 2023 Jul:641:396-403. doi: 10.1016/j.jcis.2023.03.069. Epub 2023 Mar 13.

Authors

Yadong Xu¹, Meng Tian¹, Yi Rong¹, Chengyi Lu¹, Zhengyi Lu¹, Ruhua Shi¹, Tianyi Gu¹, Qian Zhang¹, Chengchang Jin², Ruizhi Yang³

Affiliations

¹ College of Energy, Soochow Institute for Energy and Materials Innovations, Soochow University, Suzhou 215006, China.
² College of Energy, Soochow Institute for Energy and Materials Innovations, Soochow University, Suzhou 215006, China. Electronic address: jinchengchang@suda.edu.cn.
³ College of Energy, Soochow Institute for Energy and Materials Innovations, Soochow University, Suzhou 215006, China. Electronic address: yangrz@suda.edu.cn.

PMID: 36948096
DOI: 10.1016/j.jcis.2023.03.069

Abstract

Solid-state Li batteries employing Li-metal anodes and solid Li/Li_1.3Al_0.3Ti_1.7(PO₄)₃ (LATP) electrolytes have emerged as promising next-generation energy storage devices due to their high energy density and safety. However, their performance is seriously limited by the irreversible reactivity of LATP with the Li-metal anode and the poor solid-solid interfacial contact between them, which result in relatively low ionic conductivity at the interface. The present work addresses these issues by presenting a method for modifying the Li/LATP interface in situ by applying 2-(trimethylsilyl) phenyl trifluoromethanesulfonate (2-(TMS)PTM) as a new type of electrolyte additive between the Li anode and the LATP electrolyte when assembling the battery, and then forming a uniform and thin interfacial layer via redox reactions occurring during the application of multiple charge-discharge cycles to the resulting battery. As a result of the significantly improved chemical compatibility between the Li anode and the LATP electrolyte, an as-assembled battery delivers a high reversible capacity of 165.7 mAh g^-1 and an outstanding capacity retention of 86.2% after 300 charge-discharge cycles conducted at a rate of 0.2C and a temperature of 30 °C. Accordingly, this work provides a new strategy for developing advanced solid-state Li metal batteries by tailoring the interface between the Li anode and the solid electrolyte.

Keywords: Electrolyte additive; Interfacial modification; LATP; Li metal anode; Solid-state battery.