Catalyst accessibility to chemical reductants in metal–organic frameworks

Roy, Souvik, Pascanu, Vlad, Pullen, Sonja , González Miera, Greco, Martín-Matute, Belén and Ott, Sascha (2017) Catalyst accessibility to chemical reductants in metal–organic frameworks. Chemical Communications, 53 (22). pp. 3257-3260. ISSN 1359-7345

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A molecular H2-evolving catalyst, [Fe2(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.

Keywords:[FeFe] catalysts, Reduction reactions, MOF channels, Electrochemical hydrogen evolution reaction (HER), Carbon-free energy systems
Subjects:F Physical Sciences > F100 Chemistry
F Physical Sciences > F161 Organometallic Chemistry
Divisions:College of Science > School of Chemistry
ID Code:40671
Deposited On:17 Apr 2020 10:08

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