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dc.contributor.author | Gutiérrez-Tarriño, Silvia | es_ES |
dc.contributor.author | Rojas-Buzo, Sergio | es_ES |
dc.contributor.author | Ortuño, Manuel A. | es_ES |
dc.contributor.author | Oña-Burgos, Pascual | es_ES |
dc.date.accessioned | 2023-05-23T18:01:59Z | |
dc.date.available | 2023-05-23T18:01:59Z | |
dc.date.issued | 2022-12-19 | es_ES |
dc.identifier.issn | 2168-0485 | es_ES |
dc.identifier.uri | http://hdl.handle.net/10251/193544 | |
dc.description.abstract | [EN] The development of a circular economy is a key target to reduce our dependence on fossil fuels and create more sustainable processes. Concerning hydrogen as an energy vector, the use of liquid organic hydrogen carriers is a promising strategy, but most of them present limitations for hydrogen release, such as harsh reaction conditions, poor recyclability, and low-value byproducts. Herein, we present a novel sustainable methodology to produce value-added silicon precursors and concomitant hydrogen via dehydrogenative coupling by using an air- and water-stable cobalt-based catalyst synthesized from dieap and commercially available starting materials. This methodology is applied to the one-pot synthesis of a wide range of alkoxy- substituted silanes using different hydrosilanes and terminal alkenes as reactants in alcohols as green solvents under mild reaction conditions (room temperature and 0.1 mol % cobalt loading). We also demonstrate that the selectivity toward hydrosilylation/hydroalkoxysilylation can be fully controlled by varying the alcohol/water ratio. This implies the development of a circular approach for hydrosilylation/hydroalkoxysilylation reactions, which is unprecedented in this research field up to date. Kinetic and in situ spectroscopic studies (electron paramagnetic resonance, nuclear magnetic resonance, and electrospray ionization mass spectrometry), together with density functional theory simulations, further provide a detailed mechanistic picture of the dehydrogenative coupling and subsequent hydrosilylation. Finally, we illustrate the application of our catalytic system in the synthesis of an industrially relevant polymer precursor coupled with the production of green hydrogen on demand. | es_ES |
dc.description.sponsorship | This work has received financial support from Spanish Government (RTI2018-096399-A-I00 and PID2020-119116RA-I00), Junta de Andalucia (P20_01027 and PYC 20 RE 060 UAL), Xunta Distinguished Researcher program (ED431H 2020/21), the Xunta de Galicia (Centro singular de investigacion de Galicia accreditation 2019-2022, ED431G 2019/03), and the European Union (European Regional Development Fund, ERDF). S.R.-B. acknowledges the Margarita Salas grant financed by Ministerio de Universidades, Spain, and funded by the European Union-Next Generation EU. M.A.O. acknowledges CESGA ("Centro de Super-computacion de Galicia") for providing generous computa-tional resources. | es_ES |
dc.language | Inglés | es_ES |
dc.publisher | American Chemical Society | es_ES |
dc.relation.ispartof | ACS Sustainable Chemistry & Engineering | es_ES |
dc.rights | Reconocimiento (by) | es_ES |
dc.subject | Hydrogen delivery | es_ES |
dc.subject | Green hydrogen | es_ES |
dc.subject | Alkene hydrosilylation | es_ES |
dc.subject | Dehydrogenative coupling | es_ES |
dc.subject | Cobalt complex | es_ES |
dc.subject | Homogeneous catalysis | es_ES |
dc.title | Sustainable Synthesis of Silicon Precursors Coupled with Hydrogen Delivery Based on Circular Economy via Molecular Cobalt-Based Catalysts | es_ES |
dc.type | Artículo | es_ES |
dc.identifier.doi | 10.1021/acssuschemeng.2c04444 | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2020-119116RA-I00/ES/REDES METAL ORGANICAS PARA LA VALORIZACION DE BIOMASA A TRAVES DE SIMULACIONES DE SISTEMAS CATALITICOS/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/Junta de Andalucía//P20_01027/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/Junta de Andalucía//PYC 20 RE 060 UAL/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/Xunta de Galicia//ED431H 2020%2F21//Distinguished Researchers Program/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/Xunta de Galicia//ED431G 2019%2F03/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/AEI//RTI2018-096399-A-I00//CLUSTERES MULTIMETALICOS Y SUBNANOMETRICOS SOPORTADOS: SINTESIS, ESTRUCTURA Y DINAMISMO ATOMICO, Y EMPLEO COMO CATALIZADORES EN LA VALORIZACION DE METANO Y ALCANOS LIGEROS/ | es_ES |
dc.rights.accessRights | Abierto | es_ES |
dc.description.bibliographicCitation | Gutiérrez-Tarriño, S.; Rojas-Buzo, S.; Ortuño, MA.; Oña-Burgos, P. (2022). Sustainable Synthesis of Silicon Precursors Coupled with Hydrogen Delivery Based on Circular Economy via Molecular Cobalt-Based Catalysts. ACS Sustainable Chemistry & Engineering. 10(50):16624-16633. https://doi.org/10.1021/acssuschemeng.2c04444 | es_ES |
dc.description.accrualMethod | S | es_ES |
dc.relation.publisherversion | https://doi.org/10.1021/acssuschemeng.2c04444 | es_ES |
dc.description.upvformatpinicio | 16624 | es_ES |
dc.description.upvformatpfin | 16633 | es_ES |
dc.type.version | info:eu-repo/semantics/publishedVersion | es_ES |
dc.description.volume | 10 | es_ES |
dc.description.issue | 50 | es_ES |
dc.identifier.pmid | 36825066 | es_ES |
dc.identifier.pmcid | PMC9940298 | es_ES |
dc.relation.pasarela | S\484176 | es_ES |
dc.contributor.funder | Xunta de Galicia | es_ES |
dc.contributor.funder | Junta de Andalucía | es_ES |
dc.contributor.funder | Agencia Estatal de Investigación | es_ES |
dc.contributor.funder | European Regional Development Fund | es_ES |
dc.contributor.funder | Universitat Politècnica de València |