Rubio-Gaspar, A.; Misturini, A.; Millan, R.; Almora-Barrios, N.; Tatay, S.; Bon, V.; Bonneau, M.... (2024). Translocation and Confinement of Tetraamines in Adaptable Microporous Cavities. Angewandte Chemie International Edition. 63(30). https://doi.org/10.1002/anie.202402973
Por favor, use este identificador para citar o enlazar este ítem: http://hdl.handle.net/10251/209235
Título:
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Translocation and Confinement of Tetraamines in Adaptable Microporous Cavities
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Autor:
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Rubio-Gaspar, Ana
Misturini, Alechania
Millan, Reisel
Almora-Barrios, Neyvis
Tatay, S.
Bon, Volodymyr
Bonneau, Mickaele
Guillerm, Vincent
Eddaoudi, Mohamed
Navalón Oltra, Sergio
Kaskel, Stefan
Armentano, Donatella
Marti-Gastaldo, Carlos
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Entidad UPV:
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Universitat Politècnica de València. Escuela Técnica Superior de Ingenieros Industriales - Escola Tècnica Superior d'Enginyers Industrials
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Fecha difusión:
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Resumen:
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[EN] Metal-Organic Frameworks can be grafted with amines by coordination to metal vacancies to create amine-appended solid adsorbents, which are being considered as an alternative to using aqueous amine solutions for CO2 ...[+]
[EN] Metal-Organic Frameworks can be grafted with amines by coordination to metal vacancies to create amine-appended solid adsorbents, which are being considered as an alternative to using aqueous amine solutions for CO2 capture. In this study, we propose an alternative mechanism that does not rely on the use of neutral metal vacancies as binding sites but is enabled by the structural adaptability of heterobimetallic Ti2Ca2 clusters. The combination of hard (Ti4+) and soft (Ca2+) metal centers in the inorganic nodes of the framework enables MUV-10 to adapt its pore windows to the presence of triethylenetetramine molecules. This dynamic cluster response facilitates the translocation and binding of tetraamine inside the microporous cavities to enable the formation of bis-coordinate adducts that are stable in water. The extension of this grafting concept from MUV-10 to larger cavities not restrictive to CO2 diffusion will complement other strategies available for the design of molecular sorbents for decarbonization applications.; We introduce an alternative to the use of open metal vacancies in the design of amine-appended adsorbents based on the use of secondary building units combining of hard and soft metal sites. This endows MUV-10 with a flexible response to the uptake of tetraamines that facilitates their translocation into the microporous cavities of the framework to form stable bis-coordinate adducts that can remain stable in water. image
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Palabras clave:
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Tetraamine
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Translocation
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Confinement
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Cluster chemistry
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Pore reconfiguration
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Nanoporous cavities
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Derechos de uso:
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Reconocimiento - No comercial (by-nc)
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Fuente:
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Angewandte Chemie International Edition. (issn:
1433-7851
)
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DOI:
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10.1002/anie.202402973
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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/anie.202402973
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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 2017-2020/PID2020-118117RB-I00/ES/CONTROL QUIMICO DE ESTABILIDAD Y FUNCION EN REDES TITANIO-ORGANICAS PARA FOTOCATALIZADORES POROSOS/
...[+]
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2020-118117RB-I00/ES/CONTROL QUIMICO DE ESTABILIDAD Y FUNCION EN REDES TITANIO-ORGANICAS PARA FOTOCATALIZADORES POROSOS/
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-123856OB-I00/ES/FOTOCATALIZADORES MULTIFUNCIONALES BASADOS EN MATERIALES HIBRIDOS METAL-ORGANICO PARA LA REDUCCION SELECTIVA DE CO2 IMPULSADA POR LA ENERGIA SOLAR A COMBUSTIBLES Y PRODUCTOS/
info:eu-repo/grantAgreement/EC//ERC-2021-COG-101043428/
info:eu-repo/grantAgreement/GVA//ACIF%2F2020%2F090/
info:eu-repo/grantAgreement/GVA//PROMETEU%2F2021%2F054/
info:eu-repo/grantAgreement/GVA//CIPROM%2F2021%2F075/
info:eu-repo/grantAgreement/GVA//MFA%2F2022%2F026/
info:eu-repo/grantAgreement/MICINN//CEX2019-000919-M/
info:eu-repo/grantAgreement/MICINN//CNS2022-135677/
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Agradecimientos:
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This work was supported by the H2020 program (ERC-2021-COG-101043428), the Generalitat Valenciana (PROMETEU/2021/054, IDIFEDER/2021/075 and MFA/2022/026) and the Spanish government (CEX2019-000919-M, PID2020-118117RB-I00 ...[+]
This work was supported by the H2020 program (ERC-2021-COG-101043428), the Generalitat Valenciana (PROMETEU/2021/054, IDIFEDER/2021/075 and MFA/2022/026) and the Spanish government (CEX2019-000919-M, PID2020-118117RB-I00 and CNS2022-135677). A. R.-G. acknowledges the Generalitat Valenciana for a predoctoral grant (ACIF/2020/090). We also thank the University of Valencia for research facilities (NANBIOSIS). S.N. thanks the support of grant PID2021-123856OBI00 funded by MICIU/AEI/10.13039/501100011033 and by ERDF A way of making Europe. We also thank ALBA (XALOC BL13, 2022086946) and Diamond Light Source (I-19, CY28808-1) for the access to Synchrotron beamtime. BSC-RES is also acknowledged for computational resources (QHS-2023-2-0016 and QHS-2023-3-0022).
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Tipo:
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Artículo
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