Insight into Controllable Metal–Support Interactions in Metal/Metal Electrocatalysts for Efficient Energy-Saving Hydrogen Production

Controllable metal–support interaction (MSI) modulations have long been studied for improving the performance of catalysts supported on metal oxides. However, the corresponding in-depth study for metal 1 -metal 2 (M 1 -M 2 ) composited configurations is rarely achieved due to the lack of reliable models and manipulation mechanisms of MSI modifications. We modeled ruthenium on copper support (Ru–Cu) metal catalysts with negligible interfacial contact potential (e0.06 V) and investigated MSI-dependent hydrogen evolution reaction (HER) catalysis kinetics induced by an electronic hydroxyl (HO-) modifier. Comprehensive simulations and characterizations confirmed that adjusting the HO- coverage can readily realize the tailorable improvement of MSI, facilitating charge migration at the Ru–Cu interface and optimizing the overall HER pathway on active Ru. As a result, a 5/10 monolayer (ML) HO-modified catalyst (5/10 ML) exhibits superior HER activity and durability owing to the relatively stronger MSI. This catalyst also ensured sustainable and efficient hydrogen generation in a urea electrolyzer with significant energy savings. Our work provides a valuable reference for optimizing the MSI-activity relationship in M 1 -M 2 catalysts that target more than just HER.