Steering Surface Reaction at Specific Sites with Self-Assembly Strategy

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  • Xiong Zhou, Peking University
  • ,
  • Fabian Bebensee, Sino-Danish Center for Molecular Nanostructures on Surfaces
  • ,
  • Mingmei Yang, Peking University
  • ,
  • Regine Bebensee, Sino-Danish Center for Molecular Nanostructures on Surfaces
  • ,
  • Fang Cheng, Peking University
  • ,
  • Yang He, Peking University
  • ,
  • Qian Shen, Peking University
  • ,
  • Jian Shang, Peking University
  • ,
  • Zhirong Liu, Peking University
  • ,
  • Flemming Besenbacher
  • Trolle R. Linderoth
  • Kai Wu, Peking University

To discern the catalytic activity of different active sites, a self-assembly strategy is applied to confine the involved species that are "attached" to specific surface sites. The employed probe reaction system is the Ullmann coupling of 4-bromobiphenyl, C6H5C6H4Br, on an atomically flat Ag(111) surface, which is explored by combined scanning tunneling microscopy, synchrotron X-ray photoelectron spectroscopy, and density functional theory calculations. The catalytic cycle involves the detachment of the Br atom from the initial reactant to form an organometallic intermediate, C6H5C6H4AgC6H4C6H5, which subsequently self-assembles with its central Ag atom residing either on 2-fold bridge or 3-fold hollow sites at full coverage. The hollow site turns out to be catalytically more active than the bridge one, allowing us to achieve site-steered reaction control from the intermediate to the final coupling product, p-quaterphenyl, at 390 and 410 K, respectively.

OriginalsprogEngelsk
TidsskriftA C S Nano
Vol/bind11
Nummer9
Sider (fra-til)9397-9404
Antal sider8
ISSN1936-0851
DOI
StatusUdgivet - 26 sep. 2017

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