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Oxygen tolerance of an in silico-designed bioinspired hydrogen-evolving catalyst in water

Author(s): Sit, Patrick H.- L.; Car, Roberto; Cohen, Morrel H.; Selloni, Annabella

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Abstract: Certain bacterial enzymes, the diiron hydrogenases, have turnover numbers for hydrogen production from water as large as 104/s. Their much smaller common active site, composed of earth-abundant materials, has a structure that is an attractive starting point for the design of a practical catalyst for electrocatalytic or solar photocatalytic hydrogen production from water. In earlier work, our group has reported the computational design of [FeFe]P/FeS2, a hydrogenase-inspired catalyst/electrode complex, which is efficient and stable throughout the production cycle. However, the diiron hydrogenases are highly sensitive to ambient oxygen by a mechanism not yet understood in detail. An issue critical for practical use of [FeFe]P/FeS2 is whether this catalyst/electrode complex is tolerant to the ambient oxygen. We report demonstration by ab initio simulations that the complex is indeed tolerant to dissolved oxygen over timescales long enough for practical application, reducing it efficiently. This promising hydrogen-producing catalyst, composed of earth-abundant materials and with a diffusion-limited rate in acidified water, is efficient as well as oxygen tolerant.
Publication Date: 5-Feb-2013
Electronic Publication Date: 22-Jan-2013
Citation: Sit, P. H.- L., Car, R., Cohen, M.H., Selloni, A. (2013). Oxygen tolerance of an in silico-designed bioinspired hydrogen-evolving catalyst in water. Proceedings of the National Academy of Sciences, 110 (6), 2017 - 2022. doi:10.1073/pnas.1215149110
DOI: doi:10.1073/pnas.1215149110
ISSN: 0027-8424
EISSN: 1091-6490
Pages: 110.6: 2017 - 2022
Type of Material: Journal Article
Journal/Proceeding Title: Proceedings of the National Academy of Sciences
Version: Final published version. Article is made available in OAR by the publisher's permission or policy.

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