Please use this identifier to cite or link to this item: https://doi.org/10.1002/anie.202008370
Title: Design, Identification, and Evolution of a Surface Ruthenium(II/III) Single Site for CO Activation
Authors: Kang, Liqun
Wang, Bolun
Thetford, Adam
Wu, Ke
Danaie, Mohsen
He, Qian 
Gibson, Emma K
Sun, Ling-Dong
Asakura, Hiroyuki
Catlow, C Richard A
Wang, Feng Ryan
Keywords: Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry
heterogeneous catalysis
ruthenium(II) complexes
single sites
surface coordination chemistry
X-ray absorption spectroscopy
POLYPYRIDYL COMPLEXES
ELECTRONIC-STRUCTURE
METAL
CATALYSIS
METHANOL
SPECTRA
EDGES
WATER
CL
Issue Date: 13-Nov-2020
Publisher: WILEY-V C H VERLAG GMBH
Citation: Kang, Liqun, Wang, Bolun, Thetford, Adam, Wu, Ke, Danaie, Mohsen, He, Qian, Gibson, Emma K, Sun, Ling-Dong, Asakura, Hiroyuki, Catlow, C Richard A, Wang, Feng Ryan (2020-11-13). Design, Identification, and Evolution of a Surface Ruthenium(II/III) Single Site for CO Activation. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 60 (3) : 1212-1219. ScholarBank@NUS Repository. https://doi.org/10.1002/anie.202008370
Abstract: RuII compounds are widely used in catalysis, photocatalysis, and medical applications. They are usually obtained in a reductive environment as molecular O2 can oxidize RuII to RuIII and RuIV. Here we report the design, identification and evolution of an air-stable surface [bipy-RuII(CO)2Cl2] site that is covalently mounted onto a polyphenylene framework. Such a RuII site was obtained by reduction of [bipy-RuIIICl4]− with simultaneous ligand exchange from Cl− to CO. This structural evolution was witnessed by a combination of in situ X-ray and infrared spectroscopy studies. The [bipy-RuII(CO)2Cl2] site enables oxidation of CO with a turnover frequency of 0.73×10−2 s−1 at 462 K, while the RuIII site is completely inert. This work contributes to the study of structure–activity relationship by demonstrating a practical control over both geometric and electronic structures of single-site catalysts at molecular level.
Source Title: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
URI: https://scholarbank.nus.edu.sg/handle/10635/216456
ISSN: 14337851
15213773
DOI: 10.1002/anie.202008370
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