Activating Honeycomb Borophene for Efficient Hydrogen Evolution via Substrate-Induced p -Band Center Modulation

作者：Wenjun Tang, Haiyuan Chen, Xiaobin Niu · 发表于：ACS Applied Materials & Interfaces · 年份：2025 · DOI：10.1021/acsami.5c12479 · 被引用次数：2 · 研究领域：Electrocatalysts for Energy Conversion、Advanced Photocatalysis Techniques、Hydrogen Storage and Materials

Developing efficient and stable electrocatalysts for the hydrogen evolution reaction (HER) is crucial for enabling sustainable hydrogen production through water electrolysis. Two-dimensional (2D) boron allotropes, particularly honeycomb borophene (hc-B), have emerged as promising candidates due to their electron-deficient nature and rich active sites. However, this same electron deficiency compromises their structural stability, limiting practical applications. In this study, we employ first-principles calculations to investigate a donor–acceptor hc-B/V 2 CS 2 heterostructure, where the V 2 CS 2 substrate plays a dual role in stabilizing hc-B and modulating its catalytic properties. Machine learning-accelerated molecular dynamics simulations in an explicit water environment confirm the heterostructure’s exceptional structural integrity and aqueous tolerance over 50 ps. Remarkably, the hc-B side of the heterostructure exhibits hydrogen adsorption Gibbs free energy values near the thermoneutral point, outperforming benchmark catalysts such as Pt and the MoS 2 S-edge. Electronic structure analyses reveal that the enhanced HER activity arises from substrate-induced modulation of the boron p -band center, which promotes an optimal binding environment for H intermediates through interfacial orbital hybridization and stabilized B–H coordination. Furthermore, reaction pathway analysis incorporating explicit solvation identifies the Volmer–Tafel mechanism as the kinetically preferred ...