Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 110, Issue 6, Pages 2017-2022Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1215149110
Keywords
energy storage; renewable energy; density functional theory; Car-Parrinello molecular dynamics
Categories
Funding
- Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-FG02-06ER-46344]
- Office of Science of the US Department of Energy [DE-AC02-05CH11231]
- Division Of Mathematical Sciences
- Direct For Mathematical & Physical Scien [1040196] Funding Source: National Science Foundation
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Certain bacterial enzymes, the diiron hydrogenases, have turnover numbers for hydrogen production from water as large as 10(4)/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.
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