Catalyst accessibility to chemical reductants in metal–organic frameworks

A molecular H(2)-evolving catalyst, [Fe(2)(cbdt)(CO)(6)] ([FeFe], cbdt = 3-carboxybenzene-1,2-dithiolate), has been attached covalently to an amino-functionalized MIL-101(Cr) through an amide bond. Chemical reduction experiments reveal that the MOF channels can be clogged by ion pairs that are forme...

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Autores principales: Roy, Souvik, Pascanu, Vlad, Pullen, Sonja, González Miera, Greco, Martín-Matute, Belén, Ott, Sascha
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2017
Materias:
Chemistry
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5836565/
https://www.ncbi.nlm.nih.gov/pubmed/28261731
http://dx.doi.org/10.1039/c7cc00022g
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author Roy, Souvik
Pascanu, Vlad
Pullen, Sonja
González Miera, Greco
Martín-Matute, Belén
Ott, Sascha
author_facet Roy, Souvik
Pascanu, Vlad
Pullen, Sonja
González Miera, Greco
Martín-Matute, Belén
Ott, Sascha
author_sort Roy, Souvik
collection PubMed
description A molecular H(2)-evolving catalyst, [Fe(2)(cbdt)(CO)(6)] ([FeFe], cbdt = 3-carboxybenzene-1,2-dithiolate), has been attached covalently to an amino-functionalized MIL-101(Cr) through an amide bond. Chemical reduction experiments reveal that the MOF channels can be clogged by ion pairs that are formed between the oxidized reductant and the reduced catalyst. This effect is lessened in MIL-101-NH-[FeFe] with lower [FeFe] loadings. On longer timescales, it is shown that large proportions of the [FeFe] catalysts within the MOF engage in photochemical hydrogen production and the amount of produced hydrogen is proportional to the catalyst loading.
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spelling pubmed-58365652018-03-12 Catalyst accessibility to chemical reductants in metal–organic frameworks Roy, Souvik Pascanu, Vlad Pullen, Sonja González Miera, Greco Martín-Matute, Belén Ott, Sascha Chem Commun (Camb) Chemistry A molecular H(2)-evolving catalyst, [Fe(2)(cbdt)(CO)(6)] ([FeFe], cbdt = 3-carboxybenzene-1,2-dithiolate), has been attached covalently to an amino-functionalized MIL-101(Cr) through an amide bond. Chemical reduction experiments reveal that the MOF channels can be clogged by ion pairs that are formed between the oxidized reductant and the reduced catalyst. This effect is lessened in MIL-101-NH-[FeFe] with lower [FeFe] loadings. On longer timescales, it is shown that large proportions of the [FeFe] catalysts within the MOF engage in photochemical hydrogen production and the amount of produced hydrogen is proportional to the catalyst loading. Royal Society of Chemistry 2017-03-18 2017-02-23 /pmc/articles/PMC5836565/ /pubmed/28261731 http://dx.doi.org/10.1039/c7cc00022g Text en This journal is © The Royal Society of Chemistry 2017 http://creativecommons.org/licenses/by/3.0/ This article is freely available. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (CC BY 3.0)
spellingShingle Chemistry
Roy, Souvik
Pascanu, Vlad
Pullen, Sonja
González Miera, Greco
Martín-Matute, Belén
Ott, Sascha
Catalyst accessibility to chemical reductants in metal–organic frameworks
title Catalyst accessibility to chemical reductants in metal–organic frameworks
title_full Catalyst accessibility to chemical reductants in metal–organic frameworks
title_fullStr Catalyst accessibility to chemical reductants in metal–organic frameworks
title_full_unstemmed Catalyst accessibility to chemical reductants in metal–organic frameworks
title_short Catalyst accessibility to chemical reductants in metal–organic frameworks
title_sort catalyst accessibility to chemical reductants in metal–organic frameworks
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5836565/
https://www.ncbi.nlm.nih.gov/pubmed/28261731
http://dx.doi.org/10.1039/c7cc00022g
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AT gonzalezmieragreco catalystaccessibilitytochemicalreductantsinmetalorganicframeworks
AT martinmatutebelen catalystaccessibilitytochemicalreductantsinmetalorganicframeworks
AT ottsascha catalystaccessibilitytochemicalreductantsinmetalorganicframeworks

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