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Sustainable Synthesis of Silicon Precursors Coupled with Hydrogen Delivery Based on Circular Economy via Molecular Cobalt-Based Catalysts

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Sustainable Synthesis of Silicon Precursors Coupled with Hydrogen Delivery Based on Circular Economy via Molecular Cobalt-Based Catalysts

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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


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