Escobar-Bedia, FJ.; Martin-Diaconescu, V.; Simonelli, L.; Sabater Picot, MJ.; Concepción Heydorn, P. (2022). Chitosan-Silica as a Cheap Carrier and Green Soft Ligand for Improved Ru-catalyzed Hydroformylation. ChemCatChem. 14(24):1-11. https://doi.org/https://doi.org/10.1002/cctc.202200861
Por favor, use este identificador para citar o enlazar este ítem: http://hdl.handle.net/10251/201246
Title:
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Chitosan-Silica as a Cheap Carrier and Green Soft Ligand for Improved Ru-catalyzed Hydroformylation
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Author:
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Escobar-Bedia, Francisco Javier
Martin-Diaconescu, Vlad
Simonelli, Laura
Sabater Picot, Mª José
Concepción Heydorn, Patricia
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UPV Unit:
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Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química
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Issued date:
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Abstract:
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[EN] Dodecacarbonyltriruthenium Ru-3(CO)(12) has been immobilized onto a biopolymer (chitosan) supported on SiO2 (Ch@SiO2) to give Ru-Ch@SiO2. Ch@SiO2 behaves as a soft, recoverable and bulky ligand allowing the stabilization ...[+]
[EN] Dodecacarbonyltriruthenium Ru-3(CO)(12) has been immobilized onto a biopolymer (chitosan) supported on SiO2 (Ch@SiO2) to give Ru-Ch@SiO2. Ch@SiO2 behaves as a soft, recoverable and bulky ligand allowing the stabilization of released Ru active species and preventing its irreversible reduction to Ru-0. Under these conditions very high activity (TOF= 1086 h(-1); TON=2749) and regioselectivity (n:iso=92 : 8) are obtained, surpassing that of the homogeneous Ru-3(CO)(12) counterpart.Spectroscopic studies have shown that Ru-3(CO)(12) transforms into a mononuclear Run+ (n=2,3) di o try carbonyl species by interacting with the amido/amino groups of the biopolymer, being released into the reaction media whilst stabilized by the chitosan functional groups.The herein 0.5 Ru-Ch@SiO2 catalyst can operate be operated under a semi-continuous mode for at least 14 h without deactivation, representing providing a starting point in the search for a green catalyst with definitive industrial application in hydroformylations. In particular in the search for a heterogeneous catalyst away from the use of phosphines and their known drawbacks (i. e. tedious synthesis, facile oxidation of phosphor center, ..) as well as expensive Rh as active site.
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Copyrigths:
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Reconocimiento (by)
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Source:
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ChemCatChem. (issn:
1867-3880
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DOI:
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https://doi.org/10.1002/cctc.202200861
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Publisher:
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John Wiley & Sons
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Publisher version:
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https://doi.org/10.1002/cctc.202200861
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Project ID:
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info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PGC2018-101247-B-I00/ES/RECONOCIMIENTO MOLECULAR EN CATALIZADORES SOLIDOS/
...[+]
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PGC2018-101247-B-I00/ES/RECONOCIMIENTO MOLECULAR EN CATALIZADORES SOLIDOS/
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-099668-B-C21/ES/VALORIZACION DE CO2: CAPTURA, Y TRANSFORMACION CATALITICA PARA ALMACENAMIENTO DE ENERGIA, COMBUSTIBLES Y PRODUCTOS QUIMICOS/
info:eu-repo/grantAgreement/UPV//PAID//Programa de Ayudas de Investigación y Desarrollo/
info:eu-repo/grantAgreement/GVA//AICO%2F2020%2F205/
info:eu-repo/grantAgreement/ALBA Synchrotron Light Source//2020024106/
info:eu-repo/grantAgreement/ALBA Synchrotron Light Source//2019093692/
info:eu-repo/grantAgreement/ALBA Synchrotron Light Source//BL22-CLAESS/
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Description:
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This is the peer reviewed version of the following article: Escobar¿Bedia, F. J., Martin¿Diaconescu, V., Simonelli, L., Sabater, M. J., & Concepción, P. (2022). Chitosan¿Silica as a Cheap Carrier and Green Soft Ligand for Improved Ru¿catalyzed Hydroformylation. ChemCatChem, 14(24), e202200861, which has been published in final form at https://doi.org/10.1002/cctc.202200861. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving.
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Thanks:
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This research was funded by Ministerio de Ciencia, Innovacion y Universidades, Grants number RTI2018-099668-B-C21 and PGC2018-101247-B-100, and Generalitat Valenciana (GVA), AICO/2020/205. F.J.E.B acknowledges the Polytechnical ...[+]
This research was funded by Ministerio de Ciencia, Innovacion y Universidades, Grants number RTI2018-099668-B-C21 and PGC2018-101247-B-100, and Generalitat Valenciana (GVA), AICO/2020/205. F.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 Investigacion y Desarrollo". XAS experiments were performed at the BL22-CLAESS beamline at the ALBA Synchrotron with the collaboration of ALBA staff as part of projects 2019093692 and 2020024106.
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Type:
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Artículo
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