Mixed‐Dimensional Partial Dealloyed PtCuBi/C as High‐Performance Electrocatalysts for Methanol Oxidation with Enhanced CO Tolerance

Abstract Developing efficient electrocatalysts for methanol oxidation reaction (MOR) is crucial in advancing the commercialization of direct methanol fuel cells (DMFCs). Herein, carbon‐supported 0D/2D PtCuBi/C (0D/2D PtCuBi/C) catalysts are fabricated through a solvothermal method, followed by a partial electrochemical dealloying process to form a novel mixed‐dimensional electrochemically dealloyed PtCuBi/C (0D/2D D‐PtCuBi/C) catalysts. Benefiting from distinctive mixed‐dimensional structure and composition, the as‐obtained 0D/2D D‐PtCuBi/C catalysts possess abundant accessible active sites. The introduction of Cu as a water‐activating element weakens the CO_ads, and oxophilic metal Bi facilitates the OH_ads, thereby enhancing its tolerance to CO poisoning and promoting MOR activity. The X‐ray photoelectron spectroscopy (XPS) and X‐ray absorption fine structure spectroscopy (XAFS) collectively reveal the electron transfer from Cu and Bi to Pt, the electron‐enrichment effect induced by dealloying, and the strong interactions among Pt‐M (Cu, Pt, and Bi) multi‐active sites, which improve the tuning of the electronic structure and enhancement of electron transfer ability. Impressively, the optimized 0D/2D D‐PtCuBi/C catalysts exhibit the superior mass activity (MA) of 17.68 A mg_Pt⁻¹ for MOR, which is 14.86 times higher than that of commercial Pt/C. This study offers a proposed strategy for Pt‐based alloy catalysts, enabling their use as efficient anodic materials in fuel cell applications.