The realization of the hydrogen spillover effect in metal-supported catalysts is an effective strategy for enhancing the performance of hydrogen evolution reactions (HERs). However, regulating the interaction between the substrate and the metal to promote the spillover process remains challenging. In this study, we construct a Pt nanoparticle catalyst supported by molybdenum oxide rich in oxygen vacancies (Pt-NP/MoO_x). Enhanced hydrogen transfer is achieved by regulating the microenvironment of the substrate surface. Specific experiments and theoretical analyses demonstrate that the reduction treatment of the substrate induces the formation of oxygen vacancies, valence gradients, and amorphous–crystalline interfaces, resulting in strong interactions and electron transfer to Pt nanoparticles, thus ensuring efficient hydrogen spillover at the interface. Consequently, Pt-NP/MoO_x exhibits excellent HER activity of −24 mV at 10 mA cm⁻². This study offers a proof-of-concept for comprehending the influence of the substrate surface environment on the performance of noble metal-based catalysts.

中文翻译：

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价梯度诱导电荷转移，在析氢中实现高效的氢溢出


在金属负载催化剂中实现氢溢出效应是提高析氢反应 （HER） 性能的有效策略。然而，调节基材和金属之间的相互作用以促进溢出过程仍然具有挑战性。在这项研究中，我们构建了一种由富含氧空位 （Pt-NP/MoO_x） 的氧化钼负载的 Pt 纳米颗粒催化剂。通过调节衬底表面的微环境来实现增强的氢转移。具体实验和理论分析表明，衬底的还原处理诱导氧空位、价梯度和非晶-结晶界面的形成，导致强相互作用和电子转移到 Pt 纳米颗粒，从而确保在界面处有效的氢溢出。因此，Pt-NP/MoO_x 在 10 mA ^cm-2 处表现出 -24 mV 的优异 HER 活性。本研究为理解衬底表面环境对贵金属基催化剂性能的影响提供了概念验证。