Decoupling the crucial architectures of carbon support governing Pt nanoparticle anchoring behaviour for electrocatalytic hydrogen evolution

Abstract

Porous carbons have garnered broad attention as catalyst supports for maximizing Pt utilization. However, significant challenges persist in systematic decoupling crucial carbon architectures governing nanocatalyst anchoring behavior, due to highly correlated nature of multiple carbon structures. Herein, we precisely engineered various carbons with well-defined architectures to isolate and evaluate individual structural contribution to Pt nanoparticle anchoring. Experimental results reveal three key structure-performance relationships: (1) While increasing specific surface area (SSA) effectively enhances Pt dispersion, this SSA-driven dispersion strategy becomes ineffective in microporous systems, where the pore accessibility—rather than total SSA—governs Pt dispersion quality. (2) Nanopore engineering enables effective Pt nanoparticle stabilization through confinement effects, significantly enhancing catalyst durability, while this stabilization follows pronounced pore-size-dependent mechanism, with micro-mesopores (1–10 nm) exhibiting optimal effects. (3) Oxygen functionalities own superior Pt-anchoring capability than vacancy defects, with C=O groups triggering stronger metal-support interactions via C=O-Pt coordination than C-O species, while excessive C=O-Pt coordination may compromise catalytic activity, revealing an important stability-activity balance. Consequently, rational design of carbon support with well-engineered micro-mesopores and C=O-dominant functionalities, enables exceptional catalytic activity and durability. This investigation systematically decouples crucial carbon architectures governing Pt nanoparticle anchoring, providing guidance for engineering carbon-supported catalysts with enhanced catalytic performance.