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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 |
Appears in Collections: | Staff Publications Elements |
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