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In Situ Raman Monitoring and Manipulating of Interfacial Hydrogen Spillover by Precise Fabrication of Au/TiO 2 /Pt Sandwich Structures
Author(s) -
Wei Jie,
Qin SiNa,
Liu JingLi,
Ruan XiangYu,
Guan Zhiqiang,
Yan Hao,
Wei DiYe,
Zhang Hua,
Cheng Jun,
Xu Hongxing,
Tian ZhongQun,
Li JianFeng
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202000426
Subject(s) - hydrogen spillover , catalysis , hydrogen , selectivity , raman spectroscopy , materials science , spillover effect , in situ , fabrication , chemical engineering , nanotechnology , photochemistry , chemistry , organic chemistry , optics , physics , economics , microeconomics , engineering , medicine , alternative medicine , pathology
The spillover of hydrogen species and its role in tuning the activity and selectivity in catalytic hydrogenation have been investigated in situ using surface‐enhanced Raman spectroscopy (SERS) with 10 nm spatial resolution through the precise fabrication of Au/TiO 2 /Pt sandwich nanostructures. In situ SERS study reveals that hydrogen species can efficiently spillover at Pt‐TiO 2 ‐Au interfaces, and the ultimate spillover distance on TiO 2 is about 50 nm. Combining kinetic isotope experiments and density functional theory calculations, it is found that the hydrogen spillover proceeds via the water‐assisted cleavage and formation of surface hydrogen–oxygen bond. More importantly, the selectivity in the hydrogenation of the nitro or isocyanide group is manipulated by controlling the hydrogen spillover. This work provides molecular insights to deepen the understanding of hydrogen activation and boosts the design of active and selective catalysts for hydrogenation.