Engineering Cathode-Electrolyte Interface of High-Voltage Spinel LiNi0.5Mn1.5O4 via Halide Solid-State Electrolyte Coating

Jheng-Yi Huang; Ching-Yun Cheng; Yan-Ming Lai; Kevin Iputera; Ren-Jei Chung; Ru-Shi Liu

doi:10.1021/acsami.3c08517

Engineering Cathode-Electrolyte Interface of High-Voltage Spinel LiNi_0.5Mn_1.5O₄ via Halide Solid-State Electrolyte Coating

ACS Appl Mater Interfaces. 2023 Aug 30;15(34):40648-40655. doi: 10.1021/acsami.3c08517. Epub 2023 Aug 16.

Authors

Jheng-Yi Huang¹, Ching-Yun Cheng², Yan-Ming Lai¹, Kevin Iputera¹, Ren-Jei Chung², Ru-Shi Liu¹

Affiliations

¹ Department of Chemistry and Advanced Research Center for Green Materials Science and Technology, National Taiwan University, Taipei 106, Taiwan.
² Department of Chemical Engineering and Biotechnology, National Taipei University of Technology, Taipei 106, Taiwan.

PMID: 37584718
DOI: 10.1021/acsami.3c08517

Abstract

The high-voltage spinel LiNi_0.5Mn_1.5O₄ (LNMO) cathode material with high energy density, low cost, and excellent rate capability has grabbed the attention of the field. However, a high-voltage platform at 4.7 V causes severe oxidative side reactions when in contact with the organic electrolyte, leading to poor electrochemical performance. Furthermore, the contact between the liquid electrolyte and LNMO leads to Mn dissolution during cycles. In this work, we applied the sol-gel method to prepare Li₃InCl₆-coated LNMO (LIC@LNMO) to address the mentioned problems of LNMO. By introducing a protective layer of halide-type solid-state electrolyte on LNMO, we can prevent direct contact between LNMO and electrolyte while maintaining good ionic conductivity. Thus, we could demonstrate that 5 wt % LIC@LNMO exhibited a good cycle performance with a Coulombic efficiency of 99% and a capacity retention of 80% after the 230th cycle at the 230th cycle at 1C at room temperature.

Keywords: Li3InCl6; LiNi0.5Mn1.5O4; coating method; interface improvement; sol−gel method.