Title:
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Improved Electro- and Photocatalytic Water Reduction by Confined Cobalt Catalysts in Streptavidin
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Author:
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Call, Arnau; Casadevall, Carla; Romero-Rivera, Adrian; Martin-Diaconescu, Vlad; Sommer, Dayn J.; Osuna, Sílvia; Ghirlanda, Giovanna; Lloret-Fillol, Julio
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Abstract:
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Incorporation of biotinylated aminopyridine cobalt complexes
derived from the triazacyclononane scaffold into the streptavidin protein leads to
formation of artificial metalloenzymes for water reduction to hydrogen. The
synthesized artificial metalloenzymes have lower overpotential (at the half-peak
up to 100 mV) and higher photocatalytic hydrogen evolution activity (up to 14-
and 10-fold increase in TOF and TON, respectively, at pH 12.5) than the free
biotinylated cobalt complexes. 1H-NMR, EPR and XAS highlight the presence of
the metal complexes upon supramolecular attachment to the streptavidin. pHdependent
catalytic studies and molecular dynamics (MD) simulations suggest
that the increase in the catalytic activity could be induced by the protein residues
positioned close to the metal centers. These findings illustrate the ability of the
biotin−streptavidin technology to produce artificial metalloproteins for photo- and electrocatalytic hydrogen evolution reaction. |
Publication date:
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2019-05-13 |
Subject(s):
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54 |
Rights:
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L'accés als continguts d'aquest document queda condicionat a l'acceptació de les condicions d'ús establertes per la següent llicència Creative Commons:http://creativecommons.org/licenses/by-nc-nd/4.0/ |
Pages:
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5837 p. |
Document type:
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Article Article - Accepted version |
DOI:
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10.1021/acscatal.8b04981
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