Theoretical evidence of self-intercalated 2D materials for battery and electrocatalytic applications

Abstract

Covalently bonded two-dimensional (2D) self-intercalated transition metal chalcogenides (i.e., ic-2Ds) have been recently fabricated experimentally, and their properties are highly tunable by stoichiometry and composition. Inspired by this progress, we focus on the applications of ic-2Ds in the field of electrochemistry and systematically investigate their performance in lithium-ion batteries (LIBs) and electrocatalytic hydrogen evolution reactions (HER). By means of density functional theory calculations, seven 3d-metal ic-2Ds are confirmed to be thermodynamically, mechanically, and thermally stable. The metallicity and abundant active sites endow these ic-2Ds with the potential as excellent electrode materials and HER catalysts. Among them, Ti₇S₁₂ and V₇S₁₂ exhibit the potential as anode materials for LIBs, showing low Li diffusion energy barriers, suitable open-circuit voltages, and ultrahigh capacity of 745.6 and 723.9 mA hg^-1, respectively; Cr₇S₁₂ and Co₇S₁₂ show promises for HER with moderate hydrogen adsorption strengths. This theoretical study provides a new avenue for the application of newly reported ic-2Ds in various electrochemical energy conversion and storage applications.

Keywords

Self-intercalated 2D materials / transition metal chalcogenides / lithium-ion batteries / hydrogen evolution reaction

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