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Tunable catalysis by reversible switching between Ru(III) single sites and Ru0 clusters in solid micelles

Qiyan Wang, Catarina Martins De Brito Mendes (UGent) , Olga V. Safonova, Walid Baaziz, César A. Urbina-Blanco (UGent) , Danielle Wuyts (UGent) , Maya Marinova, Ovidiu Ersen, Mickael Capron, Andrei Y. Khodakov, et al.
(2023) JOURNAL OF CATALYSIS. 426. p.336-344
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Abstract
Traditionally, catalytic active sites are robust; they do not change after a reaction. We show here that the Ru(III) active sites in a solid micellar Ru(III)@MCM catalyst can be controllably switched to Ru0 nanoclusters and vice versa by a mild treatment. The Ru(III) single-sites selectively catalyze the hydrogenation of functional groups such as carbonyl, and double and triple bonds in aromatic compounds via heterolytic H2 activation. The Ru0 nanoclusters in contrast are very active for hydrogenating aromatic rings. Ru0 nanoclusters are reversibly formed from the Ru(III) sites via hydrolysis and reduction as shown by XAS, HRTEM, CO adsorption, and DFT calculations. The reported strategy offers reversible switching between oxidized and metallic states of Ru to perform different chemical transformations, achieving on-demand active sites.
Keywords
Physical and Theoretical Chemistry, Catalysis, Ruthenium, Solid Micelles, Single-site, Cluster, Switching Catalysis, Arene hydrogenation, RING-OPENING POLYMERIZATION, NANOPARTICLES, TIO2

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MLA
Wang, Qiyan, et al. “Tunable Catalysis by Reversible Switching between Ru(III) Single Sites and Ru0 Clusters in Solid Micelles.” JOURNAL OF CATALYSIS, vol. 426, 2023, pp. 336–44, doi:10.1016/j.jcat.2023.07.022.
APA
Wang, Q., Martins De Brito Mendes, C., Safonova, O. V., Baaziz, W., Urbina-Blanco, C. A., Wuyts, D., … Ordomsky, V. V. (2023). Tunable catalysis by reversible switching between Ru(III) single sites and Ru0 clusters in solid micelles. JOURNAL OF CATALYSIS, 426, 336–344. https://doi.org/10.1016/j.jcat.2023.07.022
Chicago author-date
Wang, Qiyan, Catarina Martins De Brito Mendes, Olga V. Safonova, Walid Baaziz, César A. Urbina-Blanco, Danielle Wuyts, Maya Marinova, et al. 2023. “Tunable Catalysis by Reversible Switching between Ru(III) Single Sites and Ru0 Clusters in Solid Micelles.” JOURNAL OF CATALYSIS 426: 336–44. https://doi.org/10.1016/j.jcat.2023.07.022.
Chicago author-date (all authors)
Wang, Qiyan, Catarina Martins De Brito Mendes, Olga V. Safonova, Walid Baaziz, César A. Urbina-Blanco, Danielle Wuyts, Maya Marinova, Ovidiu Ersen, Mickael Capron, Andrei Y. Khodakov, Mark Saeys, and Vitaly V. Ordomsky. 2023. “Tunable Catalysis by Reversible Switching between Ru(III) Single Sites and Ru0 Clusters in Solid Micelles.” JOURNAL OF CATALYSIS 426: 336–344. doi:10.1016/j.jcat.2023.07.022.
Vancouver
1.
Wang Q, Martins De Brito Mendes C, Safonova OV, Baaziz W, Urbina-Blanco CA, Wuyts D, et al. Tunable catalysis by reversible switching between Ru(III) single sites and Ru0 clusters in solid micelles. JOURNAL OF CATALYSIS. 2023;426:336–44.
IEEE
[1]
Q. Wang et al., “Tunable catalysis by reversible switching between Ru(III) single sites and Ru0 clusters in solid micelles,” JOURNAL OF CATALYSIS, vol. 426, pp. 336–344, 2023.
@article{01H90T1Z2JBNYJ3N62NB7RGF1K,
  abstract     = {{Traditionally, catalytic active sites are robust; they do not change after a reaction. We show here that the Ru(III) active sites in a solid micellar Ru(III)@MCM catalyst can be controllably switched to Ru0 nanoclusters and vice versa by a mild treatment. The Ru(III) single-sites selectively catalyze the hydrogenation of functional groups such as carbonyl, and double and triple bonds in aromatic compounds via heterolytic H2 activation. The Ru0 nanoclusters in contrast are very active for hydrogenating aromatic rings. Ru0 nanoclusters are reversibly formed from the Ru(III) sites via hydrolysis and reduction as shown by XAS, HRTEM, CO adsorption, and DFT calculations. The reported strategy offers reversible switching between oxidized and metallic states of Ru to perform different chemical transformations, achieving on-demand active sites.}},
  author       = {{Wang, Qiyan and Martins De Brito Mendes, Catarina and Safonova, Olga V. and Baaziz, Walid and Urbina-Blanco, César A. and Wuyts, Danielle and Marinova, Maya and Ersen, Ovidiu and Capron, Mickael and Khodakov, Andrei Y. and Saeys, Mark and Ordomsky, Vitaly V.}},
  issn         = {{0021-9517}},
  journal      = {{JOURNAL OF CATALYSIS}},
  keywords     = {{Physical and Theoretical Chemistry,Catalysis,Ruthenium,Solid Micelles,Single-site,Cluster,Switching Catalysis,Arene hydrogenation,RING-OPENING POLYMERIZATION,NANOPARTICLES,TIO2}},
  language     = {{eng}},
  pages        = {{336--344}},
  title        = {{Tunable catalysis by reversible switching between Ru(III) single sites and Ru0 clusters in solid micelles}},
  url          = {{http://doi.org/10.1016/j.jcat.2023.07.022}},
  volume       = {{426}},
  year         = {{2023}},
}
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