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Ru-protein-Co biohybrids designed for solar hydrogen production: understanding electron transfer pathways related to photocatalytic function.


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, gen

SUBMITTER: Soltau SR 

PROVIDER: S-EPMC5355951 | biostudies-literature | 2016 Dec

REPOSITORIES: biostudies-literature