Interfacial Microenvironment Modulation Boosts Efficient Hydrogen Evolution Reaction in Neutral and Alkaline

Abstract

AbstractThe design of highly efficient and stable electrocatalysts in hydrogen evolution reaction over a wide range of pH, especially in neutral or alkaline conditions, is of great significance but remains· challenging. Herein, a family of single‐atoms and clusters inside the N‐doped porous carbon matrix (NDPCM) are encapsulated. Specifically, the single‐atom platinum (PtSA) and cluster platinum (PtC) in NDPCM exhibited ultralow overpotentials of 20 and 14 mV at −10 mA cm−2 under neutral and alkaline conditions, respectively and superior long‐term durability. Theoretical calculations and operando Raman measurements revealed that the coexistence of PtSA and PtC can provide multiple H adsorption sites, contributing to the extremely low |ΔGH*| of H adsorption and constructing a local acidic microenvironment to trigger a unique H3O+‐induced water reduction in neutral and alkaline conditions This unique configuration significantly promotes the catalytic activity and opens a new avenue for the crafted design of electrocatalysts.