Steering Surface Reaction at Specific Sites with Self-Assembly Strategy
Autor: | Kai Wu, Trolle R. Linderoth, Jian Shang, Zhirong Liu, Qian Shen, Mingmei Yang, Yang He, Fang Cheng, Regine Bebensee, Xiong Zhou, Fabian Bebensee, Flemming Besenbacher |
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Jazyk: | angličtina |
Rok vydání: | 2017 |
Předmět: |
NANOARCHITECTURES
General Physics and Astronomy 02 engineering and technology 010402 general chemistry 01 natural sciences AUGMENTED-WAVE METHOD Catalysis law.invention Ullmann coupling SCANNING TUNNELING MICROSCOPE DENSITY-FUNCTIONAL THEORY HYBRID CHAINS X-ray photoelectron spectroscopy Computational chemistry law Atom General Materials Science HALOGEN steering surface reaction biology Chemistry General Engineering Active site self-assembly strategy 021001 nanoscience & nanotechnology active site 0104 chemical sciences Crystallography GRAPHENE NANORIBBONS POLYMERIZATION Catalytic cycle C-C biology.protein ULLMANN COUPLING REACTION scanning tunneling microscopy Density functional theory Self-assembly Scanning tunneling microscope 0210 nano-technology |
Zdroj: | Zhou, X, Bebensee, F, Yang, M, Bebensee, R, Cheng, F, He, Y, Shen, Q, Shang, J, Liu, Z, Besenbacher, F, Linderoth, T R & Wu, K 2017, ' Steering Surface Reaction at Specific Sites with Self-Assembly Strategy ', A C S Nano, vol. 11, no. 9, pp. 9397-9404 . https://doi.org/10.1021/acsnano.7b04900 |
DOI: | 10.1021/acsnano.7b04900 |
Popis: | 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. |
Databáze: | OpenAIRE |
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