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Hydroxamate Titanium-Organic Frameworks and the Effect of Siderophore-Type Linkers over Their Photocatalytic Activity

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Hydroxamate Titanium-Organic Frameworks and the Effect of Siderophore-Type Linkers over Their Photocatalytic Activity

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dc.contributor.author	Padial, Natalia M.
dc.contributor.author	Castells-Gil, Javier
dc.contributor.author	Almora-Barrios, Neyvis
dc.contributor.author	Romero Angel, María
dc.contributor.author	Da Silva, Iván
dc.contributor.author	Barawi, Mariam
dc.contributor.author	García-Sánchez, Alba
dc.contributor.author	De la Peña O'Shea, Víctor A.
dc.contributor.author	Martí Gastaldo, Carlos
dc.date.accessioned	2019-11-13T14:43:16Z
dc.date.available	2020-07-18T04:45:06Z
dc.date.issued	2019
dc.identifier.citation	Padial, Natalia M. Castells-Gil, Javier Almora-Barrios, Neyvis Romero Angel, María Da Silva, Iván Barawi, Mariam García-Sánchez, Alba De la Peña O'Shea, Víctor A. Martí Gastaldo, Carlos 2019 Hydroxamate Titanium-Organic Frameworks and the Effect of Siderophore-Type Linkers over Their Photocatalytic Activity Journal of the American Chemical Society 141 36 13124 13133
dc.identifier.uri	https://hdl.handle.net/10550/72193
dc.description.abstract	The chemistry of Metal-Organic Frameworks (MOFs) relies on the controlled linking of organic molecules and inorganic secondary building units to assemble an unlimited number of reticular frameworks. However, the design of porous solids with chemical stability remains still limited to carboxylate or azolate groups. There is a timely opportunity to develop new synthetic platforms that make use of unexplored metal binding groups to produce metal-linker joints with hydrolytical stability. Living organisms use siderophores (iron carriers in greek) to effectively assimilate iron in soluble form. These compounds make use of hard oxodonors as hydroxamate or catecholate groups to coordinate metal Lewis acids like iron, aluminium or titanium to form metal complexes very stable in water. Inspired by the chemistry of these microorganisms, we report the first hydroxamate MOF prepared by direct synthesis. MUV-11 (MUV = Materials of Universidad de Valencia) is a crystalline, porous material (close to 800 m2·g-1) that combines photoactivity with good chemical stability in acid conditions. By using a high-throughput approach, we also demonstrate that this new chemistry is compatible with the formation of single crystalline phases for multiple titanium salts, thus expanding the scope of precursors accessible. Titanium frameworks are regarded as promising materials for photocatalytic applications. Our photoelectrochemical and catalytic tests suggests important differences for MUV-11. Compared to other Ti-MOFs, changes in the photoelectrochemical and photocatalytic activity have been rationalized with computational modelling revealing how the chemistry of siderophores can introduce changes to the electronic structure of the frontier orbitals, relevant to the photocatalytic activity of these solids.
dc.language.iso	eng
dc.relation.ispartof	Journal of the American Chemical Society, 2019, vol. 141, num. 36, p. 13124-13133
dc.subject	Química organometàl·lica
dc.subject	Titani
dc.title	Hydroxamate Titanium-Organic Frameworks and the Effect of Siderophore-Type Linkers over Their Photocatalytic Activity
dc.type	journal article	es_ES
dc.date.updated	2019-11-13T14:43:17Z
dc.identifier.doi	10.1021/jacs.9b04915
dc.identifier.idgrec	135125
dc.embargo.terms	1 year
dc.rights.accessRights	open access	es_ES