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Design, identification and evolution of surface ruthenium (II/III) single-site for CO activation

Kang, Liqun, Wang, Bolun, Thetford, Adam, Wu, Ke, Danaie, Mohsen, He, Qian, Gibson, Emma, Sun, Ling-Dong, Asakura, Hiroyuki, Catlow, Richard and Wang, Feng Ryan 2020. Design, identification and evolution of surface ruthenium (II/III) single-site for CO activation. Angewandte Chemie International Edition 10.1002/anie.202008370

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Abstract

Ru(II) compounds are widely used in catalysis, photocatalysis and medical applications. They are usually obtained in reductive environment as molecular O 2 can oxidize Ru(II) to Ru(III) and Ru(IV). Here we report the design, identification and evolution of an air‐stable surface ‐[bipy‐Ru(II)(CO) 2 Cl 2 ] site that is covalently mounted onto a polyphenylene framework. Such Ru(II) site was obtained by reduction of ‐[bipy‐Ru(III)Cl 4 ] ‐ 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‐Ru(II)(CO) 2 Cl 2 ] site enables oxidation of CO with a turnover frequency of 0.73 × 10 ‐2 s ‐1 at 462 K, while the Ru(III) site is completely inert. This work contributes to the studies of structure‐activity relationship by demonstrating a practical control over both geometric and electronic structures of single‐site catalysts at molecular level, which can be further applied in other single site catalyst researches.

Item Type: Article
Date Type: Published Online
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Wiley
ISSN: 1433-7851
Funders: EPSRC and Royal Society
Date of First Compliant Deposit: 22 October 2020
Date of Acceptance: 21 September 2020
Last Modified: 19 Jan 2021 13:51
URI: http://orca.cardiff.ac.uk/id/eprint/135851

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