NiFe]-hydrogenases revisited: nickel-carboxamido bond formation in a variant with accrued O2-tolerance and a tentative re-interpretation of Ni-SI states

Metallomics : Integrated Biometal Science
Anne VolbedaJuan C Fontecilla-Camps

Abstract

[NiFe]-hydrogenases are well-studied enzymes capable of oxidizing molecular hydrogen and reducing protons. EPR and FTIR spectroscopic studies have shown that these enzymes can be isolated in several redox states that include paramagnetic oxidized inactive Ni-A and Ni-B species and a reduced Ni-C form. The latter and the diamagnetic respectively more oxidized Ni-SI and more reduced Ni-R forms are generally thought to be involved in the catalytic cycle of [NiFe]-hydrogenases. With the exception of Ni-SI, these different stable states have been well characterized. Here, based on the crystal structure of a partially reduced Desulfovibrio fructosovorans (Df) enzyme and data from the literature we propose that at least one of the Ni-SI sub-states contains an unexpected combination of hydride and sulfenic acid moieties. We have also determined the structure of the less oxygen-sensitive Df [NiFe]-hydrogenase V74C mutant and found that more than half of the active site nickel occupies a novel position, called Ni'. In this new position, the metal ion is coordinated by two cysteine thiolates, a bridging species modeled as SH(-) and a main chain carboxamido N atom. The Ni' coordination is similar to the one found in Ni superoxide dismutase...Continue Reading

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Citations

May 27, 2015·International Journal of Molecular Sciences·Namita Khanna, Peter Lindblad
Oct 6, 2015·Journal of the American Chemical Society·Patrick KwanAnne K Jones
Mar 14, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Hulin TaiShun Hirota
Sep 6, 2018·Physical Chemistry Chemical Physics : PCCP·Siyao QiuChenghua Sun
Feb 11, 2016·Biochemical Society Transactions·Lindsey A Flanagan, Alison Parkin
Sep 17, 2019·Journal of the American Chemical Society·Huaiguang LiNicolas Plumeré
Jul 19, 2018·Journal of the American Chemical Society·Jeffrey W SlaterHannah S Shafaat

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