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Insights into the Active Sites and Kinetics of Double-site Catalysts for Semi-hydrogenation under Hydrogen Spillover
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  • Shuai Wang,
  • Yipin Lv,
  • Xilong Wang,
  • Daowei Gao,
  • Aijun Duan,
  • Huaiqing Zhao,
  • Peng Zheng,
  • Guozhu Chen
Shuai Wang
University of Jinan
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Yipin Lv
University of Jinan
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Xilong Wang
King Abdullah University of Science and Technology
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Daowei Gao
University of Jinan
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Aijun Duan
China University of Petroleum Beijing
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Huaiqing Zhao
University of Jinan
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Peng Zheng
China University of Petroleum Beijing
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Guozhu Chen
University of Jinan

Corresponding Author:[email protected]

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Abstract

A well-defined catalyst with platinum (Pt) and gold (Au) encapsulated in micropore and mesopore of micro-mesoporous zeolite (TMSN), respectively, was designed to investigate the original active sites and kinetics of semi-hydrogenation. Specifically, hydrogen molecules are dissociated on Pt nanoclusters (NCs) to form hydrogen atoms that migrate to the surfaces of TMSN zeolite and Au nanoparticles (NPs). Meanwhile, the Au NPs with inferior H2 dissociation capability in the mesopore can be served as the detector and controller of hydrogen spillover. The Pt NCs in micropore act as H2 dissociation sites while both the Au NPs and zeolite surface are identified as the semi-hydrogenation sites. Noteworthy, the Pt-Au/TMSN catalyst with double active sites exhibits higher selectivity and rate constant ratio for semi-hydrogenation than Pt/TMSN, as well as higher turnover frequency (TOF) than Au/MSN. This work creates an effective regulation strategy of hydrogen spillover for improving active sites and kinetics of semi-hydrogenation.