Cysteine as a ligand platform in the biosynthesis of the FeFe hydrogenase H cluster

Proceedings of the National Academy of Sciences of the United States of America
Daniel L M SuessR David Britt

Abstract

Hydrogenases catalyze the redox interconversion of protons and H2, an important reaction for a number of metabolic processes and for solar fuel production. In FeFe hydrogenases, catalysis occurs at the H cluster, a metallocofactor comprising a [4Fe-4S]H subcluster coupled to a [2Fe]H subcluster bound by CO, CN(-), and azadithiolate ligands. The [2Fe]H subcluster is assembled by the maturases HydE, HydF, and HydG. HydG is a member of the radical S-adenosyl-L-methionine family of enzymes that transforms Fe and L-tyrosine into an [Fe(CO)2(CN)] synthon that is incorporated into the H cluster. Although it is thought that the site of synthon formation in HydG is the "dangler" Fe of a [5Fe] cluster, many mechanistic aspects of this chemistry remain unresolved including the full ligand set of the synthon, how the dangler Fe initially binds to HydG, and how the synthon is released at the end of the reaction. To address these questions, we herein show that L-cysteine (Cys) binds the auxiliary [4Fe-4S] cluster of HydG and further chelates the dangler Fe. We also demonstrate that a [4Fe-4S]aux[CN] species is generated during HydG catalysis, a process that entails the loss of Cys and the [Fe(CO)2(CN)] fragment; on this basis, we suggest tha...Continue Reading

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Citations

Dec 25, 2015·Proceedings of the National Academy of Sciences of the United States of America·Adrien PagnierJuan C Fontecilla-Camps
Dec 26, 2015·Inorganic Chemistry·Daniel L M SuessR David Britt
Sep 24, 2015·Journal of the American Chemical Society·Agnieszka Adamska-VenkateshWolfgang Lubitz
May 28, 2016·Biochemistry·Eric M ShepardJoan B Broderick
Jun 28, 2016·Current Opinion in Structural Biology·Pedro DinisPeter L Roach
Mar 16, 2017·Journal of the American Chemical Society·Edward J ReijerseStephen P Cramer
Mar 3, 2017·Chembiochem : a European Journal of Chemical Biology·Bing O'DowdEric Oldfield
May 30, 2017·Nature Chemical Biology·Giorgio CasertaMarc Fontecave
Jul 3, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Anna G ScottJoan B Broderick
Oct 2, 2019·Proceedings of the National Academy of Sciences of the United States of America·Guodong RaoThomas B Rauchfuss
Jul 25, 2019·Proceedings of the National Academy of Sciences of the United States of America·Oliver LampretThomas Happe
Dec 12, 2020·Chemical Society Reviews·Julian T KleinhausUlf-Peter Apfel
May 29, 2021·Journal of the American Chemical Society·Roman RohacYvain Nicolet
Jul 10, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Eric M ShepardJoan B Broderick
Sep 12, 2019·Journal of the American Chemical Society·Hao YangBrian M Hoffman
Oct 23, 2018·Accounts of Chemical Research·William E BroderickJoan B Broderick

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