Bond selectivity in electron-induced reaction due to directed recoil on an anisotropic substrate

Kelvin Anggara; Kai Huang; Lydie Leung; Avisek Chatterjee; Fang Cheng; John C. Polanyi

doi:10.1038/ncomms13690

Bond selectivity in electron-induced reaction due to directed recoil on an anisotropic substrate

Kelvin Anggara, Kai Huang, Lydie Leung, Avisek Chatterjee, Fang Cheng, John C. Polanyi^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

14 Scopus citations

Abstract

Bond-selective reaction is central to heterogeneous catalysis. In heterogeneous catalysis, selectivity is found to depend on the chemical nature and morphology of the substrate. Here, however, we show a high degree of bond selectivity dependent only on adsorbate bond alignment. The system studied is the electron-induced reaction of meta-diiodobenzene physisorbed on Cu(110). Of the adsorbate's C-I bonds, C-I aligned € Along' the copper row dissociates in 99.3% of the cases giving surface reaction, whereas C-I bond aligned € Across' the rows dissociates in only 0.7% of the cases. A two-electronic-state molecular dynamics model attributes reaction to an initial transition to a repulsive state of an Along C-I, followed by directed recoil of C towards a Cu atom of the same row, forming C-Cu. A similar impulse on an Across C-I gives directed C that, moving across rows, does not encounter a Cu atom and hence exhibits markedly less reaction.

Original language	English
Article number	13690
Journal	Nature Communications
Volume	7
DOIs	https://doi.org/10.1038/ncomms13690
State	Published - 9 Dec 2016
Externally published	Yes

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title = "Bond selectivity in electron-induced reaction due to directed recoil on an anisotropic substrate",

abstract = "Bond-selective reaction is central to heterogeneous catalysis. In heterogeneous catalysis, selectivity is found to depend on the chemical nature and morphology of the substrate. Here, however, we show a high degree of bond selectivity dependent only on adsorbate bond alignment. The system studied is the electron-induced reaction of meta-diiodobenzene physisorbed on Cu(110). Of the adsorbate's C-I bonds, C-I aligned € Along' the copper row dissociates in 99.3% of the cases giving surface reaction, whereas C-I bond aligned € Across' the rows dissociates in only 0.7% of the cases. A two-electronic-state molecular dynamics model attributes reaction to an initial transition to a repulsive state of an Along C-I, followed by directed recoil of C towards a Cu atom of the same row, forming C-Cu. A similar impulse on an Across C-I gives directed C that, moving across rows, does not encounter a Cu atom and hence exhibits markedly less reaction.",

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T1 - Bond selectivity in electron-induced reaction due to directed recoil on an anisotropic substrate

AU - Anggara, Kelvin

AU - Huang, Kai

AU - Leung, Lydie

AU - Chatterjee, Avisek

AU - Cheng, Fang

AU - Polanyi, John C.

PY - 2016/12/9

Y1 - 2016/12/9

N2 - Bond-selective reaction is central to heterogeneous catalysis. In heterogeneous catalysis, selectivity is found to depend on the chemical nature and morphology of the substrate. Here, however, we show a high degree of bond selectivity dependent only on adsorbate bond alignment. The system studied is the electron-induced reaction of meta-diiodobenzene physisorbed on Cu(110). Of the adsorbate's C-I bonds, C-I aligned € Along' the copper row dissociates in 99.3% of the cases giving surface reaction, whereas C-I bond aligned € Across' the rows dissociates in only 0.7% of the cases. A two-electronic-state molecular dynamics model attributes reaction to an initial transition to a repulsive state of an Along C-I, followed by directed recoil of C towards a Cu atom of the same row, forming C-Cu. A similar impulse on an Across C-I gives directed C that, moving across rows, does not encounter a Cu atom and hence exhibits markedly less reaction.

AB - Bond-selective reaction is central to heterogeneous catalysis. In heterogeneous catalysis, selectivity is found to depend on the chemical nature and morphology of the substrate. Here, however, we show a high degree of bond selectivity dependent only on adsorbate bond alignment. The system studied is the electron-induced reaction of meta-diiodobenzene physisorbed on Cu(110). Of the adsorbate's C-I bonds, C-I aligned € Along' the copper row dissociates in 99.3% of the cases giving surface reaction, whereas C-I bond aligned € Across' the rows dissociates in only 0.7% of the cases. A two-electronic-state molecular dynamics model attributes reaction to an initial transition to a repulsive state of an Along C-I, followed by directed recoil of C towards a Cu atom of the same row, forming C-Cu. A similar impulse on an Across C-I gives directed C that, moving across rows, does not encounter a Cu atom and hence exhibits markedly less reaction.

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Bond selectivity in electron-induced reaction due to directed recoil on an anisotropic substrate

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