Bilanin-Artigado, C.; Tiburcio, E.; Ferrando-Soria, J.; Armentano, D.; Leyva Perez, A.; Pardo, E. (2021). Crystallographic Visualization of a Double Water Molecule Addition on a Pt-1-MOF during the Low-temperature Water-Gas Shift Reaction. ChemCatChem. 13(4):1195-1200. https://doi.org/10.1002/cctc.202001492
Por favor, use este identificador para citar o enlazar este ítem: http://hdl.handle.net/10251/183206
Título:
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Crystallographic Visualization of a Double Water Molecule Addition on a Pt-1-MOF during the Low-temperature Water-Gas Shift Reaction
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Autor:
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Bilanin-Artigado, Cristina
Tiburcio, Estefanía
Ferrando-Soria, Jesús
Armentano, Donatella
Leyva Perez, Antonio
Pardo, Emilio
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Entidad UPV:
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Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química
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Fecha difusión:
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Resumen:
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[EN] The low-temperature water-gas shift reaction (WGSR, CO+H2O H-2+CO2) is considered a very promising reaction -candidate for fuel cells- despite an efficient and robust catalyst is still desirable. One of the more ...[+]
[EN] The low-temperature water-gas shift reaction (WGSR, CO+H2O H-2+CO2) is considered a very promising reaction -candidate for fuel cells- despite an efficient and robust catalyst is still desirable. One of the more prominent catalysts for this reaction is based on single Pt atoms (Pt-1) on different supports, which are supposed to manifold the reaction by the accepted mechanism for the general WGSR, i. e. by addition of one H2O molecule to CO, with generation of CO2 and H-2. Here we show, experimentally, that not one but two H2O molecules are added to CO on the Pt-1 catalyst, as assessed by a combination of reactivity experiments with soluble Pt catalysts, kinetic and spectroscopic measurements, and finally by in-operando single crystal X-ray diffraction on a Pt-1-MOF, to visualize the formation of the hemiacetal intermediate on the solid catalytic site. These results confirm our previous DFT predictions and provide a paradigmatic shift in the assumed mechanism of the WGSR, which may open the debate if two H2O molecules are recurrently added during the WGSR, not only for Pt-1 catalysts but also for other metal catalysts.
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Palabras clave:
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Water gas shift reaction
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Single atom catalyst
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Metal-organic framework
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Platinum
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Crystallography
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Derechos de uso:
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Reserva de todos los derechos
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Fuente:
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ChemCatChem. (issn:
1867-3880
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DOI:
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10.1002/cctc.202001492
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Editorial:
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John Wiley & Sons
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Versión del editor:
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https://doi.org/10.1002/cctc.202001492
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Código del Proyecto:
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info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2017-86735-P/ES/CATALISIS CON ATOMOS METALICOS AISLADOS Y CLUSTERES ULTRAPEQUEÑOS BIEN DEFINIDOS, SIN LIGANDOS Y CONFINADOS/
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info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2017-86735-P/ES/CATALISIS CON ATOMOS METALICOS AISLADOS Y CLUSTERES ULTRAPEQUEÑOS BIEN DEFINIDOS, SIN LIGANDOS Y CONFINADOS/
info:eu-repo/grantAgreement/MINECO//CEX2019-000919-M/
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-104778GB-I00/ES/DESARROLLO DE POLIMEROS DE COORDINACION POROSOS FUNCIONALES CON APLICACIONES TECNOLOGICAS Y MEDIOAMBIENTALES/
info:eu-repo/grantAgreement/Fundació Bancària Caixa d'Estalvis i Pensions de Barcelona//LCF%2FBQ%2FPR19%2F11700011/
info:eu-repo/grantAgreement/EC/H2020/814804/EU
info:eu-repo/grantAgreement/Fondazione Cariplo//2019-2090/
info:eu-repo/grantAgreement/Fundació Bancària Caixa d'Estalvis i Pensions de Barcelona//100010434/
info:eu-repo/grantAgreement/MINECO//SEV-2016-0683//Programa Estatal de Fomento de la Investigación Científica y Técnica de Excelencia/
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Descripción:
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This is the peer reviewed version of the following article: C. Bilanin, E. Tiburcio, J. Ferrando-Soria, D. Armentano, A. Leyva-Pérez, E. Pardo, ChemCatChem 2021, 13, 1195, which has been published in final form at https://doi.org/10.1002/cctc.202001492. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving.
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Agradecimientos:
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This work was supported by the Ministero dell'Istruzione, dell'Universita e della Ricerca (Italy) and the Ministerio de Ciencia e Innovacion (Spain) (Projects PID2019-104778GB-I00 and CTQ2017-86735-P and the excellence ...[+]
This work was supported by the Ministero dell'Istruzione, dell'Universita e della Ricerca (Italy) and the Ministerio de Ciencia e Innovacion (Spain) (Projects PID2019-104778GB-I00 and CTQ2017-86735-P and the excellence units "Severo Ochoa" SEV-2016-0683 and "Maria de Maeztu" CEX2019-000919-M). C. B. and E. T. thank ITQ and MINECO for the concession of fellowships. Thanks are extended to the "2019 Post-doctoral Junior Leader-Retaining Fellowship, la Caixa Foundation (ID100010434 and fellowship code LCF/BQ/PR19/11700011" (J. F.-S.). D.A. acknowledges the financial support of the Fondazione CARIPLO / "Economia Circolare: ricerca per un futuro sostenibile" 2019, Grant number: 2019-2090, MOCA. We thank to Dr. R. Adam, Dr. J. Oliver-Meseguer and J. C. Arango for their help. E.P. acknowledges the financial support of the European Research Council under the European Union's Horizon 2020 research and innovation programme / ERC Grant Agreement No 814804, MOF-reactors. We acknowledge Diamond Light Source for awarded beamtime and provision of synchrotron radiation facilities with dosing gas cell and thank Dr Mark Warren for his assistance at I19 beamline (Proposal number MT18768-2).
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Tipo:
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Artículo
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