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

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6 Scopus citations


Certain bacterial enzymes, the diiron hydrogenases, have turnover numbers for hydrogen production fromwater 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 fromwater. In earlierwork, our group has reported the computational design of [FeFe]P/FeS2, a hydrogenaseinspired 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.

Original languageEnglish (US)
Pages (from-to)2017-2022
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Issue number6
StatePublished - Feb 5 2013

All Science Journal Classification (ASJC) codes

  • General


  • Car-Parrinello molecular dynamics
  • Density functional theory
  • Energy storage
  • Renewable energy


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