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Wiring of Photosystem I and Hydrogenase on an Electrode for Photoelectrochemical H2 Production by using Redox Polymers for Relatively Positive Onset Potential

Tapia, Cristina; Milton, Ross D.; Pankratova, Galina LU ; Minteer, Shelley D.; Åkerlund, Hans Erik LU ; Leech, Dónal; De Lacey, Antonio L.; Pita, Marcos and Gorton, Lo LU (2017) In ChemElectroChem 4(1). p.90-95
Abstract

Photosystem I (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... (More)

Photosystem I (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 O2 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 H2 produced, reaching a maximum of −30 μA cm−2 for the system incorporating Cc-BPEI and showing a relatively positive onset potential at +0.38 V versus SHE.

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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
biocatalysis, enzymes, hydrogen, photosynthesis, polymers
in
ChemElectroChem
volume
4
issue
1
pages
6 pages
publisher
Wiley-Blackwell
external identifiers
  • scopus:84992452934
ISSN
2196-0216
DOI
10.1002/celc.201600506
language
English
LU publication?
yes
id
fe952c3c-586e-4306-be61-af0953d1dc7c
date added to LUP
2017-03-20 14:55:11
date last changed
2017-04-16 04:45:51
@article{fe952c3c-586e-4306-be61-af0953d1dc7c,
  abstract     = {<p>Photosystem I (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<sub>2</sub> inactivation, but only the use of Cc-BPEI yields significant photocurrents for H<sup>+</sup> reduction, likely due to its lower redox potential. The photocurrents obtained are found to be proportional to the quantity of H<sub>2</sub> produced, reaching a maximum of −30 μA cm<sup>−2</sup> for the system incorporating Cc-BPEI and showing a relatively positive onset potential at +0.38 V versus SHE.</p>},
  author       = {Tapia, Cristina and Milton, Ross D. and Pankratova, Galina and Minteer, Shelley D. and Åkerlund, Hans Erik and Leech, Dónal and De Lacey, Antonio L. and Pita, Marcos and Gorton, Lo},
  issn         = {2196-0216},
  keyword      = {biocatalysis,enzymes,hydrogen,photosynthesis,polymers},
  language     = {eng},
  month        = {01},
  number       = {1},
  pages        = {90--95},
  publisher    = {Wiley-Blackwell},
  series       = {ChemElectroChem},
  title        = {Wiring of Photosystem I and Hydrogenase on an Electrode for Photoelectrochemical H<sub>2</sub> Production by using Redox Polymers for Relatively Positive Onset Potential},
  url          = {http://dx.doi.org/10.1002/celc.201600506},
  volume       = {4},
  year         = {2017},
}