2026-04-13T05:42:45Zhttps://recercat.cat/oai/request
oai:recercat.cat:2072/3739402024-12-20T15:53:31Zcom_2072_300912com_2072_4427col_2072_301309
RECERCAT author Call, Arnau author Casadevall, Carla author Romero-Rivera, Adrian author Martin-Diaconescu, Vlad author Sommer, Dayn J. author Osuna, Sílvia author Ghirlanda, Giovanna author Lloret-Fillol, Julio 2020-03-09T13:13:49Z2024-04-23T10:16:20Z 2020-03-09T13:13:49Z2024-04-23T10:16:20Z 2019-05-13 http://hdl.handle.net/2072/373940 https://doi.org/10.1021/acscatal.8b04981 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. eng 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/ Improved Electro- and Photocatalytic Water Reduction by Confined Cobalt Catalysts in Streptavidin info:eu-repo/semantics/article info:eu-repo/semantics/acceptedVersion URL https://recercat.cat/bitstream/2072/373940/5/acscatal.8b04981.pdf File MD5 265567395e0f664901b871189d96696b 3319216 application/pdf acscatal.8b04981.pdf URL https://recercat.cat/bitstream/2072/373940/1/acscatal.8b04981.pdf.txt File MD5 9b07360a3a4f3e00b8f922dd2ea37c85 64144 text/plain acscatal.8b04981.pdf.txt