Insight into the Microstructure and Ionic Conductivity of Cold Sintered NASICON Solid Electrolyte for Solid-State Batteries

Yulong Liu; Jingru Liu; Qian Sun; Dawei Wang; Keegan R Adair; Jianneng Liang; Cheng Zhang; Li Zhang; Shigang Lu; Huan Huang; Xiping Song; Xueliang Sun

doi:10.1021/acsami.9b08132

Insight into the Microstructure and Ionic Conductivity of Cold Sintered NASICON Solid Electrolyte for Solid-State Batteries

ACS Appl Mater Interfaces. 2019 Aug 7;11(31):27890-27896. doi: 10.1021/acsami.9b08132. Epub 2019 Jul 24.

Authors

Yulong Liu¹, Jingru Liu², Qian Sun¹, Dawei Wang¹, Keegan R Adair¹, Jianneng Liang¹, Cheng Zhang², Li Zhang³, Shigang Lu³, Huan Huang⁴, Xiping Song², Xueliang Sun¹

Affiliations

¹ Department of Mechanical and Materials Engineering , The University of Western Ontario , London , Ontario N6A 5B9 , Canada.
² State Key Laboratory for Advance Metal and Materials , University of Science and Technology Beijing , Beijing 100083 , China.
³ China Automotive Battery Research Institute Co., Ltd , Beijing 100088 , China.
⁴ Glabat Solid-State Battery Inc. , 700 Collip Circle, Suite 211 , London , Ontario N6G 4X8 , Canada.

PMID: 31298519
DOI: 10.1021/acsami.9b08132

Abstract

Li_1.3Al_0.3Ti_1.7(PO₄)₃ (LATP) is a popular solid electrolyte used in solid-state lithium batteries due to its high ionic conductivity. Traditionally, the densification of LATP is achieved by a high-temperature sintering process (about 1000 °C). Herein, we report the compaction of LATP by a newly developed cold sintering process and post-annealing. LATP pellets are first densified at 120 °C and then annealed at 650 °C, yielding an ionic conductivity of 8.04 × 10^-5 S cm^-1 at room temperature and a relative density of 93% with a low activation energy of 0.37 eV. High-resolution transmission electron microscopy of the cold sintered pellets is investigated as well, showing that the particles are interconnected with some nanoprecipitates at the grain boundaries. Such nanocrystalline-enriched grain boundaries are beneficial for lithium-ion transportation, which leads to higher ionic conductivity of the cold sintered sample. This new sintering process can direct new horizons for development of all solid-state batteries due to its simplicity.

Keywords: HRTEM; LATP; cold sintering process; ionic conductivity; solid-state electrolyte.