Steering Surface Reaction at Specific Sites with Self-Assembly Strategy

Xiong Zhou; Fabian Bebensee; Mingmei Yang; Regine Bebensee; Fang Cheng; Yang He; Qian Shen; Jian Shang; Zhirong Liu; Flemming Besenbacher; Trolle R. Linderoth; Kai Wu

doi:10.1021/acsnano.7b04900

Steering Surface Reaction at Specific Sites with Self-Assembly Strategy

Xiong Zhou, Fabian Bebensee, Mingmei Yang, Regine Bebensee, Fang Cheng, Yang He, Qian Shen, Jian Shang, Zhirong Liu, Flemming Besenbacher, Trolle R. Linderoth^*, Kai Wu

^*Corresponding author for this work

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

39 Citations (Scopus)

Abstract

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.

Original language	English
Journal	A C S Nano
Volume	11
Issue	9
Pages (from-to)	9397-9404
Number of pages	8
ISSN	1936-0851
DOIs	https://doi.org/10.1021/acsnano.7b04900
Publication status	Published - 26 Sept 2017

Keywords

steering surface reaction
self-assembly strategy
active site
Ullmann coupling
scanning tunneling microscopy
ULLMANN COUPLING REACTION
SCANNING TUNNELING MICROSCOPE
DENSITY-FUNCTIONAL THEORY
AUGMENTED-WAVE METHOD
GRAPHENE NANORIBBONS
HYBRID CHAINS
C-C
HALOGEN
NANOARCHITECTURES
POLYMERIZATION

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10.1021/acsnano.7b04900

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title = "Steering Surface Reaction at Specific Sites with Self-Assembly Strategy",

abstract = "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.",

keywords = "steering surface reaction, self-assembly strategy, active site, Ullmann coupling, scanning tunneling microscopy, ULLMANN COUPLING REACTION, SCANNING TUNNELING MICROSCOPE, DENSITY-FUNCTIONAL THEORY, AUGMENTED-WAVE METHOD, GRAPHENE NANORIBBONS, HYBRID CHAINS, C-C, HALOGEN, NANOARCHITECTURES, POLYMERIZATION",

author = "Xiong Zhou and Fabian Bebensee and Mingmei Yang and Regine Bebensee and Fang Cheng and Yang He and Qian Shen and Jian Shang and Zhirong Liu and Flemming Besenbacher and Linderoth, {Trolle R.} and Kai Wu",

year = "2017",

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doi = "10.1021/acsnano.7b04900",

language = "English",

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T1 - Steering Surface Reaction at Specific Sites with Self-Assembly Strategy

AU - Zhou, Xiong

AU - Bebensee, Fabian

AU - Yang, Mingmei

AU - Bebensee, Regine

AU - Cheng, Fang

AU - He, Yang

AU - Shen, Qian

AU - Shang, Jian

AU - Liu, Zhirong

AU - Besenbacher, Flemming

AU - Linderoth, Trolle R.

AU - Wu, Kai

PY - 2017/9/26

Y1 - 2017/9/26

N2 - 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.

AB - 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.

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KW - scanning tunneling microscopy

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KW - SCANNING TUNNELING MICROSCOPE

KW - DENSITY-FUNCTIONAL THEORY

KW - AUGMENTED-WAVE METHOD

KW - GRAPHENE NANORIBBONS

KW - HYBRID CHAINS

KW - C-C

KW - HALOGEN

KW - NANOARCHITECTURES

KW - POLYMERIZATION

U2 - 10.1021/acsnano.7b04900

DO - 10.1021/acsnano.7b04900

M3 - Journal article

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SN - 1936-0851

VL - 11

SP - 9397

EP - 9404

JO - A C S Nano

JF - A C S Nano

IS - 9

ER -

Steering Surface Reaction at Specific Sites with Self-Assembly Strategy

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Keywords

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