Abstract
Metal-support electronic interactions play crucial roles in triggering the hydrogen spillover (HSo) to boost hydrogen evolution reaction (HER). It requires the supported metal of electron-rich state to facilitate the proton adsorption/spillover. However, this electron-rich metal state contradicts the traditional metal→support electron transfer protocol and is not compatible with the electron-donating oxygen evolution reaction (OER), especially in proton-poor alkaline conditions. Here we profile an Ir/NiPS3 support structure to study the Ir electronic states and performances in HSo/OER-integrated alkaline water electrolysis. The supported Ir is evidenced with Janus electron-rich and electron-poor states at the tip and interface regions to respectively facilitate the HSo and OER processes. Resultantly, the water electrolysis (WE) is efficiently implemented with 1.51 V at 10 mA cm-2 for 1000 h in 1 M KOH and 1.44 V in urea-KOH electrolyte. This research clarifies the Janus electronic state as fundamental in rationalizing efficient metal-support WE catalysts.