Transition metal-functionalized hexagonal bipyramidal boron clusters as high-performance electrocatalysts for hydrogen evolution reaction: A DFT study

IF 8.3 2区工程技术 Q1 CHEMISTRY, PHYSICAL International Journal of Hydrogen Energy Pub Date : 2025-05-13 Epub Date: 2025-04-19 DOI:10.1016/j.ijhydene.2025.04.092

Chou-Yi Hsu , Ali B.M. Ali , Zainab H. Jamal , Mustafa Mudhafar , Hasan Ali Alsailawi , Dilsora Abduvalieva , A.M.A. Mohamed , S.K. Adil , Hamad M. Alkahtani , Ibrahm Mahariq

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Abstract

This present study investigates the electrocatalytic activity of transition metal-functionalized TaB₆ hexagonal bipyramidal boron cluster (M -TaB₆: M = Ta, Hf, Ir, Re, W) systems for hydrogen evolution reaction (HER) within the framework of density functional theory (DFT) at the PBE-D3/GenECP/Def2-SVP/LanL2DZ computational method. The study concludes that transition metal modifications significantly contribute to hydrogen chemisorption and catalytic efficiency. Most significantly, Re-TaB₆ (−0.765 eV) and W–TaB₆ (−0.768 eV) hexagonal bipyramidal surfaces possess nearly ideal Gibbs free energy (

{Δ G}_{H}

) for HER, indicating excellent catalytic activity. Calculation of adsorption energy further reveals Hf-TaB₆ (−0.829 eV) and B₆ (−0.587 eV) with the highest hydrogen interaction, favoring strong chemisorption behavior. The study highlights how transition metal doping enhances catalytic activity by stabilizing hydrogen adsorption and breaking, optimizing the efficiency of HER.

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过渡金属功能化六方双锥体硼团簇作为析氢反应高性能电催化剂的DFT研究

本研究在密度泛函理论（DFT）框架内，采用 PBE-D3/GenECP/Def2-SVP/LanL2DZ 计算方法，研究了过渡金属功能化的 TaB6 六方双锥硼簇（M -TaB6：M = Ta、Hf、Ir、Re、W）体系在氢气进化反应（HER）中的电催化活性。研究得出结论，过渡金属修饰对氢的化学吸附和催化效率有显著的促进作用。最重要的是，Re-TaB6（-0.765 eV）和 W-TaB6（-0.768 eV）六角双锥体表面对 HER 具有近乎理想的吉布斯自由能 (ΔGH)，这表明它们具有出色的催化活性。对吸附能的计算进一步表明，Hf-TaB6（-0.829 eV）和 B6（-0.587 eV）具有最高的氢相互作用，有利于强烈的化学吸附行为。该研究强调了过渡金属掺杂如何通过稳定氢吸附和断裂来增强催化活性，从而优化 HER 的效率。

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来源期刊

International Journal of Hydrogen Energy 工程技术-环境科学

CiteScore

13.50

自引率

25.00%

发文量

3502

审稿时长

60 days

期刊介绍： The objective of the International Journal of Hydrogen Energy is to facilitate the exchange of new ideas, technological advancements, and research findings in the field of Hydrogen Energy among scientists and engineers worldwide. This journal showcases original research, both analytical and experimental, covering various aspects of Hydrogen Energy. These include production, storage, transmission, utilization, enabling technologies, environmental impact, economic considerations, and global perspectives on hydrogen and its carriers such as NH3, CH4, alcohols, etc. The utilization aspect encompasses various methods such as thermochemical (combustion), photochemical, electrochemical (fuel cells), and nuclear conversion of hydrogen, hydrogen isotopes, and hydrogen carriers into thermal, mechanical, and electrical energies. The applications of these energies can be found in transportation (including aerospace), industrial, commercial, and residential sectors.