pH‐Dependent Behavior of Ru‐Based Hydrogen‐Oxidation Electrocatalysis by a Reconstructed Hydrogen‐Bond Network

, releasing more free water molecules into the gap region and restructuring interfacial hydrogen-bond network, as confirmed by in situ surface-enhanced infrared absorption spectroscopy. Consequently, these synergistic effects promote proton-coupled electron transfer (PCET) at the electrode-electrolyte interface, thereby markedly accelerating the alkaline HOR kinetics and even resulting in the reversed pH effect. This work elucidates the pivotal roles of oxophilic promoters in synergistically modulating intermediate behavior and interfacial microenvironment, especially, in restructuring the hydrogen-bond network, which provides strategies for designing high-performance Ru-based HOR electrocatalysts and fundamental insights into pH-dependent electrocatalytic reactions.