Active and Regioselective Ru Single-Site Heterogeneous Catalysts for Alpha-Olefin Hydroformylation
| Autor: | Francisco Javier Escobar-Bedia, Miguel Lopez-Haro, Jose Juan Calvino, Vlad Martin-Diaconescu, Laura Simonelli, Virginia Perez-Dieste, Maria J. Sabater, Patricia Concepción, Avelino Corma |
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| Přispěvatelé: | Ministerio de Ciencia, Innovación y Universidades (España), Ministerio de Economía y Competitividad (España) |
| Rok vydání: | 2022 |
| Předmět: | |
| Zdroj: | ACS Catalysis. 12:4182-4193 |
| ISSN: | 2155-5435 |
| Popis: | A heterogeneous ruthenium catalyst consisting of isolated single atoms and disordered clusters stabilized in a N-doped carbon matrix has been synthesized with very good activity and remarkable regioselectivity in the hydroformylation of 1-hexene. The role of the nitrogen heteroatoms has been probed essential to increase the catalyst stability and activity, enabling the stabilization of Ru(II)-N sites according to X-ray photoelectron spectroscopy (XPS) and XANES. Intrinsic size-dependent activity of Ru species of different atomicity has been extracted, correlating the observed reaction rate and the particle size distribution determined by means of aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, permitting the identification of single-atom sites as the most active ones. This catalyst appears as a promising alternative with respect to its heterogeneous counterparts, paving the way for designing improved Ru heterogeneous catalysts. The research leading to these results has received funding from the Spanish Ministry of Science, Innovation and Universities, through the “Severo Ochoa” Excellence Programme (SEV-2016-0683) and RTI2018-099668-B-C21 and PGC2018-101247-B-100 “Programa Estatal de Generación de Conocimiento”. P.C acknowledges the financial support from the “Generalitat Valenciana” through the project AICO/2020/205. HR-HAADF-STEM measurements were performed at the DME-UCA node of ELECMI ICTS with financial support from FEDER/MINECO (MAT2017-87579-R and PID2019-110018GA-I00); XAS experiments were performed at the BL22-CLÆSS beamline at the ALBA Synchrotron with the collaboration of ALBA staff as part of projects 2019093692 and 2020024106. XPS experiments were performed at the BL24-CIRCE beamline at the ALBA Synchrotron with the collaboration of ALBA staff. J.E.B acknowledges the Polytechnical University of Valencia for the economic support through the grant of an FPI scholarship associated with the PAID programme “Programa de Ayudas de Investigación y Desarrollo”. |
| Databáze: | OpenAIRE |
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