Two-Dimensional Transition Metal Phosphides As Cathode Additive in Robust Lithium-Sulfur Batteries.

Zhang, Jie; Yang, Dawei; Li, Canhuang; Gong, Qianhong; Bi, Wei; Zheng, Xuejiao; Arbiol, Jordi; Li, Shengjun et al. · Nano Lett · 2024

basic_science · Level V

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Abstract

The development of advanced cathode materials able to promote the sluggish redox kinetics of polysulfides is crucial to bringing lithium-sulfur batteries to the market. Herein, two electrode materials: namely, Zr<sub>2</sub>PS<sub>2</sub> and Zr<sub>2</sub>PTe<sub>2</sub>, are identified through screening several hundred thousand compositions in the Inorganic Crystal Structure Database. First-principles calculations are performed on these two materials. These structures are similar to that of the classical MXenes. Concurrently, calculations show that Zr<sub>2</sub>PS<sub>2</sub> and Zr<sub>2</sub>PTe<sub>2</sub> possess high electrical conductivity, promote Li ion diffusion, and have excellent electrocatalytic activity for the Li-S reaction and particularly for the Li<sub>2</sub>S decomposition. Besides, the mechanisms behind the excellent predicted performance of Zr<sub>2</sub>PS<sub>2</sub> and Zr<sub>2</sub>PTe<sub>2</sub> are elucidated through electron localization function, charge density difference, and localized orbital locator. This work not only identifies two candidate sulfur cathode additives but may also serve as a reference for the identification of additional electrode materials in new generations of batteries, particularly in sulfur cathodes.