Transition metal-anchored WS2 nanosheets as efficient electrocatalysts for hydrogen evolution reaction: A first-principles study

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis Pub Date : 2025-10-10 DOI:10.1016/j.mcat.2025.115519

Rui Sun, Zhongxu Wang, Jingxiang Zhao

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Abstract

The development of efficient, low-cost, and stable electrocatalysts remains a central challenge for sustainable hydrogen production. In this work, we systematically designed a series of single transition metal (TM) atoms (including Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zr, Nb, Mo, Ru, Rh, Pd, Ag, Hf, Ta, W, Os, Ir, Pt, and Au) anchored on a WS₂ monolayer, and investigated their catalytic activity for the hydrogen evolution reaction (HER) using density functional theory (DFT) calculations. The comprehensive results reveal that TM atoms can effectively tune the electronic structure, electrical conductivity, and hydrogen adsorption behavior of WS₂. In particular, Cr@WS₂, Fe@WS₂, Mo@WS₂, and Ru@WS₂ catalysts exhibit Gibbs free energies of hydrogen adsorption close to zero, indicating their promising HER activity. Further crystal orbital Hamilton population (COHP) analyses and Bader charge calculations demonstrate that the chemical bonding characteristics and charge transfer between the TM atoms and the WS₂ substrate play a pivotal role in tuning adsorption strength and catalytic performance. This work provides a theoretical foundation for optimizing WS₂-based single-atom catalysts and opens new avenues for the design of highly efficient HER electrocatalysts based on two-dimensional materials.

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过渡金属锚定WS2纳米片作为析氢反应的高效电催化剂：第一线原理研究

开发高效、低成本、稳定的电催化剂仍然是可持续制氢的核心挑战。在这项工作中，我们系统地设计了一系列单一过渡金属（TM）原子（包括Ti、V、Cr、Mn、Fe、Co、Ni、Cu、Zr、Nb、Mo、Ru、Rh、Pd、Ag、Hf、Ta、W、Os、Ir、Pt和Au）锚定在WS2单层上，并使用密度泛函理论（DFT）计算研究了它们对析氢反应（HER）的催化活性。综合结果表明，TM原子可以有效调节WS2的电子结构、电导率和氢吸附行为。特别是Cr@WS2， Fe@WS2， Mo@WS2和Ru@WS2催化剂的氢吸附吉布斯自由能接近于零，表明它们具有良好的HER活性。进一步的晶体轨道汉密尔顿族（COHP）分析和Bader电荷计算表明，TM原子与WS2衬底之间的化学键特性和电荷转移在调节吸附强度和催化性能方面起着关键作用。本研究为优化基于ws2的单原子催化剂提供了理论基础，为设计基于二维材料的高效HER电催化剂开辟了新的途径。

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来源期刊

Molecular Catalysis Chemical Engineering-Process Chemistry and Technology

CiteScore

6.90

自引率

10.90%

发文量

700

审稿时长

40 days

期刊介绍： Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods