Kang, L;
Wang, B;
Thetford, A;
Wu, K;
Danaie, M;
He, Q;
Gibson, EK;
... Wang, FR; + view all
(2021)
Design, Identification, and Evolution of a Surface Ruthenium(II/III) Single Site for CO Activation.
Angewandte Chemie
, 133
(3)
pp. 1232-1239.
10.1002/ange.202008370.
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Abstract
An air-stable surface [bipy-RuII(CO)2Cl2] single site is designed towards CO oxidation, while all other RuIII single sites are not active. The methodology is further extended to nine transition-metal single-site systems, enabling the use of surface coordination chemistry in heterogeneous catalysis. // 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.
| Type: | Article |
|---|---|
| Title: | Design, Identification, and Evolution of a Surface Ruthenium(II/III) Single Site for CO Activation |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/ange.202008370 |
| Publisher version: | https://doi.org/10.1002/ange.202008370 |
| Language: | English |
| Additional information: | Copyright © 2020 The Authors. Published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/), which permits use, distribution and reproduction in any medium, provided the original work is properly cited. |
| Keywords: | heterogeneous catalysis, ruthenium(II/III) complexes, single site, surface coordination chemistry, X-ray absorption spectroscopy |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10128875 |
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