Acetylene hydratase: a non-redox enzyme with tungsten and iron-sulfur centers at the active site

Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry
Peter M H Kroneck

Abstract

In living systems, tungsten is exclusively found in microbial enzymes coordinated by the pyranopterin cofactor, with additional metal coordination provided by oxygen and/or sulfur, and/or selenium atoms in diverse arrangements. Prominent examples are formate dehydrogenase, formylmethanofuran dehydrogenase, and aldehyde oxidoreductase all of which catalyze redox reactions. The bacterial enzyme acetylene hydratase (AH) stands out of its class as it catalyzes the conversion of acetylene to acetaldehyde, clearly a non-redox reaction and a reaction distinct from the reduction of acetylene to ethylene by nitrogenase. AH harbors two pyranopterins bound to W, and a [4Fe-4S] cluster. W is coordinated by four dithiolene sulfur atoms, one cysteine sulfur, and one oxygen ligand. AH activity requires a strong reductant suggesting W(IV) as the active oxidation state. Two different types of reaction pathways have been proposed. The 1.26 Å structure reveals a water molecule coordinated to W which could gain a partially positive net charge by the adjacent protonated Asp-13, enabling a direct attack of C2H2. To access the W-Asp site, a substrate channel was evolved distant from where it is found in other members of the DMSOR family. Computationa...Continue Reading

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Citations

Jul 2, 2017·Applied and Environmental Microbiology·Denise M AkobRonald S Oremland
Nov 29, 2017·Beilstein Journal of Organic Chemistry·Matthias Schreyer, Lukas Hintermann
Jun 23, 2018·FEMS Microbiology Ecology·Denise M AkobRonald S Oremland
Mar 7, 2018·Proceedings of the National Academy of Sciences of the United States of America·Jae-Hun Jeoung, Holger Dobbek
Feb 12, 2021·International Journal of Systematic and Evolutionary Microbiology·Shaun M BaesmanRonald S Oremland
Aug 17, 2021·Organometallics·Madeleine A EhweinerNadia C Mösch-Zanetti
May 30, 2019·Inorganic Chemistry·Madeleine A EhweinerNadia C Mösch-Zanetti

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