Characterization of Photochemical Processes for H2 Production by CdS Nanorod-[FeFe] Hydrogenase Complexes

Brown, Katherine A.; Wilker, Molly B.; Boehm, Marko; Dukovic, Gordana; King, Paul W.

doi:10.1021/ja2116348

Characterization of Photochemical Processes for H2 Production by CdS Nanorod-[FeFe] Hydrogenase Complexes

Journal Article · Wed Mar 28 00:00:00 EDT 2012 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/ja2116348· OSTI ID:1043784

Brown, Katherine A.; Wilker, Molly B.; Boehm, Marko; Dukovic, Gordana;

We have developed complexes of CdS nanorods capped with 3-mercaptopropionic acid (MPA) and Clostridium acetobutylicum [FeFe]-hydrogenase I (CaI) that photocatalyze reduction of H{sup +} to H{sub 2} at a CaI turnover frequency of 380-900 s{sup -1} and photon conversion efficiencies of up to 20% under illumination at 405 nm. In this paper, we focus on the compositional and mechanistic aspects of CdS:CaI complexes that control the photochemical conversion of solar energy into H{sub 2}. Self-assembly of CdS with CaI was driven by electrostatics, demonstrated as the inhibition of ferredoxin-mediated H{sub 2} evolution by CaI. Production of H{sub 2} by CdS:CaI was observed only under illumination and only in the presence of a sacrificial donor. We explored the effects of the CdS:CaI molar ratio, sacrificial donor concentration, and light intensity on photocatalytic H{sub 2} production, which were interpreted on the basis of contributions to electron transfer, hole transfer, or rate of photon absorption, respectively. Each parameter was found to have pronounced effects on the CdS:CaI photocatalytic activity. Specifically, we found that under 405 nm light at an intensity equivalent to total AM 1.5 solar flux, H{sub 2} production was limited by the rate of photon absorption ({approx}1 ms{sup -1}) and not by the turnover of CaI. Complexes were capable of H{sub 2} production for up to 4 h with a total turnover number of 106 before photocatalytic activity was lost. This loss correlated with inactivation of CaI, resulting from the photo-oxidation of the CdS capping ligand MPA.

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Division of Chemical Sciences, Geosciences, and Biosciences and Biological and Environmental Research Program

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 1043784

Report Number(s):: NREL/JA-2700-53672; MainId:52138; UUID:2d3ea901-f9d4-e411-b769-d89d67132a6d; MainAdminId:34230

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 12 Vol. 134; ISSN JACSAT; ISSN 0002-7863

Country of Publication:: United States

Language:: English

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