Gold-decorated Pt bimetallic nanoparticles on sulfur vacancy-rich MoS2 for aqueous phase reforming of methanol into hydrogen at low temperature and atmospheric pressure

Aqueous phase reforming of methanol (APRM) into H₂ at low temperature is a sustainable methodology to the efficient generation and safe storage of hydrogen. Herein, we demonstrate that Pt-Au bimetallic nanoparticles supported on sulfur vacancy (S_v)-controllable MoS₂ nanosheets (Pt-Au/MoS₂-TH) enable high-efficiency H₂ production via APRM at 70 °C and atmospheric pressure. The Au species modifies the valence electron environment of neighboring Pt and functions as a “pump” to drive the electron migration from Pt to MoS₂. Meanwhile, the S_v created by H₂ thermal reduction acts as the “electrons reservoir” to increase the electron density at the valence band top of MoS₂, thus forming S_v-rich Pt^δ+Au−S_v−Mo^<4+ interface sites. Mechanistic investigations elucidate that the Pt^δ+Au−S_v and S_v−Mo^<4+ sites are responsible for cleaving C−H and O−H bonds in CH₃OH and HO−HCHO−H, respectively, accounting for the significantly enhanced catalytic performance. The optimal Pt-Au/MoS₂-500H catalyst with the most S_v and the strongest electronic interaction, exhibits an APRM TOF up to 10.9 h⁻¹, surpassing the Pt-Au/MoS₂-500N calcined under N₂ by 12 times and Pt/MoS₂-500H by 34 times. This discovery not only presents a promising avenue for versatile H₂ utilization via APRM, but holds potential for a variety of hydrogen-involved energy and environmental applications.