Improved Electro- and Photocatalytic Water Reduction by Confined Cobalt Catalysts in Streptavidin

Arnau Call, Carla Casadevall, Adrian Romero-Rivera, Vlad Martin-Diaconescu, Dayn J. Sommer, Sílvia Osuna, Giovanna Ghirlanda, Julio Lloret-Fillol

Research output: Contribution to journalArticle

Abstract

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. pH-dependent 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.

Original languageEnglish
Pages (from-to)5837-5846
Number of pages10
JournalACS Catalysis
DOIs
Publication statusPublished - Jan 1 2019

Fingerprint

Streptavidin
Cobalt
Hydrogen
Catalysts
Water
Aminopyridines
Metalloproteins
Proteins
Coordination Complexes
Scaffolds (biology)
Biotin
Metal complexes
Scaffolds
Paramagnetic resonance
Molecular dynamics
Catalyst activity
Metals
Nuclear magnetic resonance
Computer simulation

Keywords

  • cobalt complexes
  • electrocatalysis
  • photocatalysis
  • streptavidin-biotin
  • water reduction to hydrogen

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Cite this

Call, A., Casadevall, C., Romero-Rivera, A., Martin-Diaconescu, V., Sommer, D. J., Osuna, S., ... Lloret-Fillol, J. (2019). Improved Electro- and Photocatalytic Water Reduction by Confined Cobalt Catalysts in Streptavidin. ACS Catalysis, 5837-5846. https://doi.org/10.1021/acscatal.8b04981

Improved Electro- and Photocatalytic Water Reduction by Confined Cobalt Catalysts in Streptavidin. / Call, Arnau; Casadevall, Carla; Romero-Rivera, Adrian; Martin-Diaconescu, Vlad; Sommer, Dayn J.; Osuna, Sílvia; Ghirlanda, Giovanna; Lloret-Fillol, Julio.

In: ACS Catalysis, 01.01.2019, p. 5837-5846.

Research output: Contribution to journalArticle

Call, A, Casadevall, C, Romero-Rivera, A, Martin-Diaconescu, V, Sommer, DJ, Osuna, S, Ghirlanda, G & Lloret-Fillol, J 2019, 'Improved Electro- and Photocatalytic Water Reduction by Confined Cobalt Catalysts in Streptavidin', ACS Catalysis, pp. 5837-5846. https://doi.org/10.1021/acscatal.8b04981
Call A, Casadevall C, Romero-Rivera A, Martin-Diaconescu V, Sommer DJ, Osuna S et al. Improved Electro- and Photocatalytic Water Reduction by Confined Cobalt Catalysts in Streptavidin. ACS Catalysis. 2019 Jan 1;5837-5846. https://doi.org/10.1021/acscatal.8b04981
Call, Arnau ; Casadevall, Carla ; Romero-Rivera, Adrian ; Martin-Diaconescu, Vlad ; Sommer, Dayn J. ; Osuna, Sílvia ; Ghirlanda, Giovanna ; Lloret-Fillol, Julio. / Improved Electro- and Photocatalytic Water Reduction by Confined Cobalt Catalysts in Streptavidin. In: ACS Catalysis. 2019 ; pp. 5837-5846.
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