Enabling a Co-Free, High-Voltage LiNi0.5Mn1.5O4 Cathode in All-Solid-State Batteries with a Halide Electrolyte

作者：Jihyun Jang, Yu‐Ting Chen, Grayson Deysher, Diyi Cheng, So‐Yeon Ham, Ashley Cronk, Phillip Ridley, Hedi Yang, Baharak Sayahpour, Bing Han, Weikang Li, Weiliang Yao, Erik A. Wu, Jean‐Marie Doux, Long H. B. Nguyen, Jin An Sam Oh, Darren H. S. Tan, Ying Shirley Meng · 发表于：ACS Energy Letters · 年份：2022 · DOI：10.1021/acsenergylett.2c01397 · 被引用次数：114 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Thermal Expansion and Ionic Conductivity

High Resolution Image Download MS PowerPoint Slide One approach to increase the energy density of all-solid-state batteries (ASSBs) is to use high-voltage cathode materials. The spinel LiNi 0.5 Mn 1.5 O 4 (LNMO) cathode is one such example, as it offers a high reaction potential (close to 5 V). Moreover, it is a Co-free cathode system, which makes it an environmentally friendly and a low-cost alternative. However, several challenges must be addressed before it can be properly adopted in ASSB technologies. Herein, we reveal that lithium argyrodite (Li 6 PS 5 Cl), a sulfide solid-state electrolyte (SSE), possesses intrinsic chemical incompatibility with the LNMO cathode. We demonstrate the necessity of using a halide SSE, Li 3 YCl 6 (LYC), through careful analysis of the LNMO/SSE interface. Moreover, we emphasize the necessity of applying a protective coating layer to LNMO particles, even when halide SSEs are used. Furthermore, the chemical phenomena involving LYC in the oxidative environment of LNMO are analyzed, including a comparison between coated and uncoated LNMO particles.