This study uses first-principles calculations to investigate the asymmetric Zr₂CO/VSe₂ heterostructure for hydrogen evolution reaction (HER) applications, focusing on its interlayer interactions, electronic structures, and HER performance across six stacking angles. Our findings demonstrate remarkable structural stability, characterized by interlayer distances of 2.1 Å to 2.7 Å and binding energies from −150.521 to −257.939 meV Å⁻². Band structure analyses highlight the heterostructures' exceptional conductivity, essential for catalytic efficiency. Additionally, charge density difference calculations reveal significant charge transfer and redistribution at the interface, providing insights into the interlayer interactions and their influence on catalytic activity. Notably, the Gibbs free energy of hydrogen adsorption (ΔG_H*) remains within ±0.1 eV across all configurations, indicating superior HER activity. Further analysis shows that the work function (Φ) serves as a critical electronic structure descriptor, influencing HER performance. The relationship between work function and ΔG_H* across different interlayer distances underscores the predictive value of the work function for HER activity. These insights provide a theoretical foundation for developing advanced and effective non-noble metal HER catalysts, paving the way for innovations in sustainable energy technologies.

中文翻译：

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不对称 Zr2CO/VSe2 异质结构作为析氢反应的高效电催化剂


本研究采用第一性原理计算来研究不对称 Zr ₂ CO/VSe ₂ 异质结构在析氢反应 (HER) 中的应用，重点关注其层间相互作用、电子结构和 HER六个堆叠角度的性能。我们的研究结果表明其具有显着的结构稳定性，其特征在于层间距离为 2.1 Å 至 2.7 Å，结合能为 -150.521 至 -257.939 meV Å ⁻² 。能带结构分析强调了异质结构卓越的导电性，这对于催化效率至关重要。此外，电荷密度差计算揭示了界面处显着的电荷转移和重新分布，从而深入了解层间相互作用及其对催化活性的影响。值得注意的是，在所有配置中，氢吸附的吉布斯自由能 (ΔG _H* ) 保持在 ±0.1 eV 范围内，表明 HER 活性优异。进一步分析表明，功函数 (Φ) 作为关键的电子结构描述符，影响 HER 性能。不同层间距离的功函数和 ΔG _H* 之间的关系强调了功函数对 HER 活性的预测价值。这些见解为开发先进有效的非贵金属析氢催化剂提供了理论基础，为可持续能源技术的创新铺平了道路。