An atomically dispersed Pt/γ-Mo2N(O0.3) catalyst for hydrogen production via aqueous-phase reforming of methanol

Abstract

Aqueous-phase reforming (APR) of alcohols has emerged as a promising approach for hydrogen production. The APR of methanol (APRM) is particularly important, given its cost-effectiveness and high hydrogen yield. Hence, the development of high-performance interfacial catalysts for APRM necessitates the rational integration of reactive supports to achieve optimal dispersion of active metallic species, thereby enhancing catalytic efficacy. Herein, we demonstrate that a stable atomically dispersed Pt/γ-Mo₂N(O_0.3) catalyst exhibits exceptional activity for hydrogen production in APRM. Under the optimized reaction conditions, the 0.2 wt% Pt/γ-Mo₂N(O_0.3) catalyst achieved an intrinsic activity (ATOF = 14 813 h⁻¹). The superior hydrogen evolution performance originates from the synergistic catalytic interplay between atomically dispersed Pt species and the γ-Mo₂N(O_0.3) support, wherein the latter represents a γ-Mo₂N framework surface-modified with partial MoO_x species. Notably, the atomically dispersed Pt species, stably anchored on the unique γ-Mo₂N(O_0.3) surface, govern methanol activation and reforming processes, while the distinctive Pt/γ-Mo₂N(O_0.3) interfacial architecture plays a pivotal role in accelerating water dissociation kinetics. These concerted synergistic mechanisms collectively drive a marked enhancement in the overall catalytic efficiency.