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Wiring of photosystem i and hydrogenase on an electrode for photoelectrochemical h2production by using redox polymers for relatively positive onset potential

Tapia, Cristina
; 
Milton, Ross D.
; 
Pankratova, Galina
; 
Minteer, Shelley D.
; 
Åkerlund, Hans-Erik
; 
Leech, Dónal
; 
De Lacey, Antonio L.
; 
Pita, Marcos
; 
Gorton, Lo
Repository DOI
Publication Date
2016-09-28
Keywords
biocatalysis, enzymes, hydrogen, photosynthesis, polymers, artificial photosynthesis, desulfovibrio-gigas, cells, photocurrent, evolution
Type
Article
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Citation
Tapia, Cristina; Milton, Ross D. Pankratova, Galina; Minteer, Shelley D.; Åkerlund, Hans-Erik; Leech, Dónal; De Lacey, Antonio L.; Pita, Marcos; Gorton, Lo (2016). Wiring of photosystem i and hydrogenase on an electrode for photoelectrochemical h2production by using redox polymers for relatively positive onset potential. ChemElectroChem 4 (1), 90-95
Abstract
PhotosystemI (PSI) is combined with Desulfovibrio gigas hydrogenase for the bioelectrocatalytic photosynthesis of hydrogen at an electrode surface. The activity of these two biocatalysts is linked by two redox polymers; a redox polymer with a relatively positive potential (loaded with an Os complex) is able to reduce PSI and thus facilitates the production of photoexcited electrons, whereas redox polymers of relatively low potential are able to transfer electrons to the hydrogenase. Two negative-potential redox polymers are tested, with either a viologen pendant (4-methyl-4-bromopropylviologen functionalized linear polyethylenimine) or a cobaltocene pendant (cobaltocene-functionalized branched polyethylenimine, Cc-BPEI). Both are able to protect hydrogenase from O-2 inactivation, but only the use of Cc-BPEI yields significant photocurrents for H+ reduction, likely due to its lower redox potential. The photocurrents obtained are found to be proportional to the quantity of H-2 produced, reaching a maximum of -30Acm(-2) for the system incorporating Cc-BPEI and showing a relatively positive onset potential at +0.38V versus SHE.
Funder
Publisher
Wiley-Blackwell
Publisher DOI
10.1002/celc.201600506
Rights
Attribution-NonCommercial-NoDerivs 3.0 Ireland
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Externally hosted open access publications with University of Galway authors (2)