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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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.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.rights.uri info:eu-repo/semantics/openAccess
dc.source 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.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 info:eu-repo/semantics/article
dc.date.updated 2019-11-13T14:43:17Z
dc.identifier.doi https://doi.org/10.1021/jacs.9b04915
dc.identifier.idgrec 135125
dc.embargo.terms 1 year

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