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Issue 12, 2016
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Ru–protein–Co biohybrids designed for solar hydrogen production: understanding electron transfer pathways related to photocatalytic function

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Abstract

A series of Ru–protein–Co biohybrids have been prepared using the electron transfer proteins ferredoxin (Fd) and flavodoxin (Fld) as scaffolds for photocatalytic hydrogen production. The light-generated charge separation within these hybrids has been monitored by transient optical and electron paramagnetic resonance spectroscopies. Two distinct electron transfer pathways are observed. The Ru–Fd–Co biohybrid produces up to 650 turnovers of H2 utilizing an oxidative quenching mechanism for Ru(II)* and a sequential electron transfer pathway via the native [2Fe–2S] cluster to generate a Ru(III)–Fd–Co(I) charge separated state that lasts for ∼6 ms. In contrast, a direct electron transfer pathway occurs for the Ru–ApoFld–Co biohybrid, which lacks an internal electron relay, generating Ru(I)–ApoFld–Co(I) charge separated state that persists for ∼800 μs and produces 85 turnovers of H2 by a reductive quenching mechanism for Ru(II)*. This work demonstrates the utility of protein architectures for linking donor and catalytic function via direct or sequential electron transfer pathways to enable stabilized charge separation which facilitates photocatalysis for solar fuel production.

Graphical abstract: Ru–protein–Co biohybrids designed for solar hydrogen production: understanding electron transfer pathways related to photocatalytic function

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Publication details

The article was received on 14 Jul 2016, accepted on 05 Aug 2016 and first published on 16 Aug 2016


Article type: Edge Article
DOI: 10.1039/C6SC03121H
Citation: Chem. Sci., 2016,7, 7068-7078
  • Open access: Creative Commons BY-NC license
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    Ru–protein–Co biohybrids designed for solar hydrogen production: understanding electron transfer pathways related to photocatalytic function

    S. R. Soltau, P. D. Dahlberg, J. Niklas, O. G. Poluektov, K. L. Mulfort and L. M. Utschig, Chem. Sci., 2016, 7, 7068
    DOI: 10.1039/C6SC03121H

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