Kang, L;
Wang, B;
Thetford, A;
Wu, K;
Danaie, M;
He, Q;
Gibson, E;
... Wang, FR; + view all
(2021)
Design, Identification, and Evolution of a Surface Ruthenium(II/III) Single Site for CO Activation.
Angewandte Chemie: International Edition
, 60
(3)
pp. 1212-1219.
10.1002/anie.202008370.
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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.
| Type: | Article |
|---|---|
| Title: | Design, Identification, and Evolution of a Surface Ruthenium(II/III) Single Site for CO Activation |
| Location: | Germany |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/anie.202008370 |
| Publisher version: | https://doi.org/10.1002/anie.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, 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 UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10110980 |
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