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  X-ray Crystallography and Vibrational Spectroscopy Reveal the Key Determinants of Biocatalytic Dihydrogen Cycling by [NiFe] Hydrogenases

Ilina, Y., Lorent, C., Katz, S., Jeoung, J.-H., Shima, S., Horch, M., et al. (2019). X-ray Crystallography and Vibrational Spectroscopy Reveal the Key Determinants of Biocatalytic Dihydrogen Cycling by [NiFe] Hydrogenases. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 58(51), 18710-18714. doi:10.1002/anie.201908258.

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 Creators:
Ilina, Yulia1, Author
Lorent, Christian1, Author
Katz, Sagie1, Author
Jeoung, Jae-Hun1, Author
Shima, Seigo2, Author              
Horch, Marius1, Author
Zebger, Ingo1, Author
Dobbek, Holger1, Author
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1external, ou_persistent22              
2Department-Independent Research Group Microbial Protein Structure, Max Planck Institute for Terrestrial Microbiology, Max Planck Society, ou_3266277              

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 Abstract: [NiFe] hydrogenases are complex model enzymes for the reversible cleavage of dihydrogen (H-2). However, structural determinants of efficient H-2 binding to their [NiFe] active site are not properly understood. Here, we present crystallographic and vibrational-spectroscopic insights into the unexplored structure of the H-2-binding [NiFe] intermediate. Using an F-420-reducing [NiFe]-hydrogenase from Methanosarcina barkeri as a model enzyme, we show that the protein backbone provides a strained chelating scaffold that tunes the [NiFe] active site for efficient H-2 binding and conversion. The protein matrix also directs H-2 diffusion to the [NiFe] site via two gas channels and allows the distribution of electrons between functional protomers through a subunit-bridging FeS cluster. Our findings emphasize the relevance of an atypical Ni coordination, thereby providing a blueprint for the design of bio-inspired H-2-conversion catalysts.

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 Dates: 2019
 Publication Status: Published in print
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 Identifiers: ISI: 000492435000001
DOI: 10.1002/anie.201908258
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Title: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Source Genre: Journal
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Pages: - Volume / Issue: 58 (51) Sequence Number: - Start / End Page: 18710 - 18714 Identifier: ISSN: 1433-7851