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

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-01-26 DOI:10.1016/j.apcata.2025.120137

Kaicheng Qian , Yuezhou Li , Yupeng Lou , Tong Wei , Xiaoqing Yan , Hisayoshi Kobayashi , Dongming Qi , Mingwu Tan , Renhong Li

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引用次数: 0

Abstract

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.

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.