Single‐Atom Platinum Immobilized on Polyimide for Highly Efficient and Durable Hydrogen Evolution Electrocatalysis

Abstract Electrocatalytic hydrogen evolution reaction (HER) is widely regarded as a promising approach to convert renewable electricity into hydrogen. Platinum (Pt) based catalysts demonstrate superior activity toward acidic HER, but the scarcity of Pt metal presents obstacles for large‐scale application. Therefore, constructing Pt single‐atom catalysts (SACs) with maximum metal‐atom‐utilization efficiency renders a feasible strategy, which however is critically hindered by an unsatisfactory catalyst lifetime. Here, a general strategy is reported to develop novel HER catalysts with Pt single atoms immobilized on polyimide support, which can display an exceptional activity toward acidic HER while achieving an outstandingly high durability with negligible activity decay for 760 h of continuous operation at 100 mA cm −2 . The detailed experimental and theoretical results unravel that, the polyimide support lowers the d‐band level of Pt site with a reduced energy barrier for acidic HER and simultaneously promotes the proton concentration near Pt site, leading to appreciably improved HER kinetics. Additionally, the polyimide support is versatile toward immobilizing ruthenium, palladium, and other single metal atoms, providing an alternative approach to develop SACs with superior catalytic activity and durability.