The hydrogen evolution reaction (HER) under neutral conditions is highly important for achieving practical hydrogen production. However, catalysts often exhibit lower activity under neutral conditions, the cause of which remains an unsolved puzzle. By employing ab initio molecular dynamics and in situ surface-enhanced Raman spectroscopy, we investigated the regulatory role of Nb₂O₅ on interfacial water molecules, which determines the activity of neutral HER. The rigid interfacial water layer in a neutral medium inhibits the transport of intermediates (H₂O*/OH*) at the interface between Ru nanoclusters and the electrolyte. However, electron-rich Nb₂O₅ can overcome this challenge by altering the orientation of H₂O molecules to disrupt the H-bond network, thereby increasing the availability of H₂O on the surface of catalyst. Finally, Ru/Nb₂O₅ exhibited excellent activity, even surpassing that of commercial Pt/C catalysts at higher current density. This study provides new avenues for constructing coupled catalysts to activate interfacial water and enhance neutral HER.

中文翻译：

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通过 Nb2O5 介导的水重新取向破坏 Ru 纳米团簇上的刚性氢键网络，从而增强中性氢的产生


中性条件下的析氢反应（HER）对于实现实际的氢气生产非常重要。然而，催化剂在中性条件下往往表现出较低的活性，其原因仍然是一个未解之谜。通过从头算分子动力学和原位表面增强拉曼光谱，我们研究了 Nb ₂ O ₅ 对界面水分子的调节作用，界面水分子决定了中性 HER 的活性。中性介质中的刚性界面水层抑制了Ru纳米团簇和电解质之间界面处的中间体（H ₂ O*/OH*）的传输。然而，富电子的 Nb ₂ O ₅ 可以通过改变 H ₂ O 分子的方向来破坏氢键网络来克服这一挑战，从而增加催化剂表面 H ₂ O 的可用性。最后，Ru/Nb ₂ O ₅ 表现出优异的活性，甚至在更高的电流密度下超过了商业Pt/C催化剂。这项研究为构建耦合催化剂来活化界面水和增强中性析氢反应提供了新途径。