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Concept

Hydrogenase

Related publications (23)

Proteome adaptations of the organohalide-respiring Desulfitobacterium hafniense strain DCB-2 to various energy metabolisms

Christof Holliger, Julien Maillard, Romain Hamelin, Florence Armand, Mathilde Stéphanie Willemin

IntroductionDesulfitobacterium hafniense was isolated for its ability to use organohalogens as terminal electron acceptors via organohalide respiration (OHR). In contrast to obligate OHR bacteria, Desulfitobacterium spp. show a highly versatile energy meta ...

Frontiers Media SA2023

The Function of Two Radical-SAM Enzymes, HcgA and HcgG, in the Biosynthesis of the [Fe]-Hydrogenase Cofactor

Xile Hu, Huijie Pan, Yiwei Zheng

In the biosynthesis of the iron-guanylylpyridinol (FeGP) cofactor, 6-carboxymethyl-5-methyl-4-hydroxy-2-pyridinol (1) is 3-methylated to form 2, then 4-guanylylated to form 3, and converted into the full cofactor. HcgA-G proteins catalyze the biosynthetic ...

Wiley-VCH Verlag GmbH2022

High-Valent Nickel Promoted by Atomically Embedded Copper for Efficient Water Oxidation

Jun Li

Efficient and low-cost electrocatalysts for oxygen evolution reaction (OER), particularly in neutral conditions, are of significant importance for renewable energy technologies such as CO2 reduction and seawater splitting electrolysis. High-valent transiti ...

AMER CHEMICAL SOC2020

A catalytically active [Mn]-hydrogenase incorporating a non-native metal cofactor

Xile Hu, Farzaneh Fadaei Tirani, Matthew Wodrich, Huijie Pan

Nature carefully selects specific metal ions for incorporation into the enzymes that catalyse the chemical reactions necessary for life. Hydrogenases, enzymes that activate molecular H-2, exclusively utilize Ni and Fe in [NiFe]-, [FeFe]- and [Fe]-hydrogean ...

2019

The atomic-resolution crystal structure of activated [Fe]-hydrogenase

Xile Hu, Matthew Wodrich

Hydrogenases are promising templates for constructing new H-2-based catalysts. [Fe]-hydrogenase, which features an ironguanylylpyridinol (FeGP) cofactor, catalyses a reversible hydride transfer from H-2 to methenyl-tetrahydromethanopterin (methenyl-H4MPT+, ...

NATURE PUBLISHING GROUP2019

Towards artificial methanogenesis: biosynthesis of the [Fe]-hydrogenase cofactor and characterization of the semisynthetic hydrogenase

Xile Hu, Tao Xu, Lichen Bai

The greenhouse gas and energy carrier methane is produced on Earth mainly by methanogenic archaea. In the hydrogenotrophic methanogenic pathway the reduction of one CO2 to one methane molecule requires four molecules of H-2 containing eight electrons. Four ...

Royal Soc Chemistry2017

Natural inspirations for metal–ligand cooperative catalysis

Xile Hu, Matthew Wodrich

In conventional homogeneous catalysis, supporting ligands act as spectators that do not interact directly with substrates. However, in metal–ligand cooperative catalysis, ligands are involved in facilitating reaction pathways that would be less favourable ...

2017

A Functional Model of [Fe]-Hydrogenase

Rosario Scopelliti, Xile Hu, Matthew Wodrich, Tao Xu, Simona Mazza

[Fe]-Hydrogenase catalyzes the hydrogenation of a biological substrate via the heterolytic splitting of molecular hydrogen. While many synthetic models of [Fe]-hydrogenase have been prepared, none yet are capable of activating H-2 on their own. Here, we re ...

American Chemical Society2016

Identification of HcgC as a SAM-Dependent Pyridinol Methyltransferase in [Fe]-Hydrogenase Cofactor Biosynthesis

Xile Hu, Tao Xu, Lichen Bai

Previous retrosynthetic and isotope-labeling studies have indicated that biosynthesis of the iron guanylylpyridinol (FeGP) cofactor of [Fe]-hydrogenase requires a methyltransferase. This hypothetical enzyme covalently attaches the methyl group at the 3-pos ...

Wiley-Blackwell2016

Reconstitution of [Fe]-hydrogenase using model complexes

Xile Hu, Matthew Wodrich, Dafa Chen, Tao Xu

[Fe]-Hydrogenase catalyses the reversible hydrogenation of a methenyltetrahydromethanopterin substrate, which is an intermediate step during the methanogenesis from CO2 and H-2. The active site contains an iron-guanylylpyridinol cofactor, in which Fe2+ is ...

Nature Publishing Group2015

Hydrogen-activating models of hydrogenases

Xile Hu, Dafa Chen, Tao Xu

Hydrogenases are biological catalysts for hydrogen evolution and activation. While many model complexes of hydrogenases can catalyze the hydrogen evolution reaction, few of them can react with hydrogen. Here we review the hydrogen-activating models of hydr ...

Elsevier2015

Iron Complexes for Hydrogen Activation and Catalytic Hydrogenation

Simona Mazza

Inspired by Nature several groups have developed structural and functional iron complexes mimicking the active site of the iron-hydrogenases, which show high reactivity in the H2 cleavage. Usually pendant bases have been incorporated onto families of Fe co ...

EPFL2015

Photoelectrochemical Hydrogen Production in Alkaline Solutions Using Cu2O Coated with Earth-Abundant Hydrogen Evolution Catalysts

Michael Graetzel, Xile Hu, Matthew Thomas Mayer, Stanley David Tilley, Laurent Liardet, Carlos Gilberto Morales Guio

The splitting of water into hydrogen and oxygen molecules using sunlight is an attractive method for solar energy storage. Until now, photoelectrochemical hydrogen evolution is mostly studied in acidic solutions, in which the hydrogen evolution is more fac ...

Wiley-Blackwell2015

Synthesis and Reactivity of Mononuclear Iron Models of [Fe]-Hydrogenase that Contain an Acylmethylpyridinol Ligand

Xile Hu, Dafa Chen

[Fe]-hydrogenase has a single iron-containing active site that features an acylmethylpyridinol ligand. This unique ligand environment had yet to be reproduced in synthetic models; however the synthesis and reactivity of a new class of small molecule mimics ...

Wiley-V C H Verlag Gmbh2014

Characterization of the surfaceome of the metal-reducing bacterium Desulfotomaculum reducens

Rizlan Bernier-Latmani, Elena Suvorova Buffat, Romain Hamelin, Elena Cristina Dalla Vecchia, Diego Chiappe, Paul Pao-Yun Shao

Desulfotomaculum reducens strain MI-1 is a Gram-positive, sulfate-reducing bacterium also capable of reducing Fe(III). Metal reduction in Gram-positive bacteria is poorly understood. Here, we investigated Fe(III) reduction with lactate, a non-fermentable s ...

Frontiers Media SA2014

Electronic Elements Governing the Binding of Small Molecules to a [Fe]-hydrogenase Mimic

Xile Hu, Matthew Wodrich

[Fe]-hydrogenase, one of three types of hydrogenases, activates molecular hydrogen. Here, using DFT computations, we examine the electronic elements governing the binding of small ligands to a recently synthesized [Fe]-hydrogenase biomimic. Computed reacti ...

Wiley-Blackwell2013

Reversible protonation of a thiolate ligand in an [Fe]-hydrogenase model complex

Rosario Scopelliti, Xile Hu, Dafa Chen

The thiolate ligand in the five-coordinate model complex 1 of [Fe]-hydrogenase is preferentially and reversibly protonated, even in the presence of an acyl ligand. The results suggest that the Cys176 thiolate ligand in [Fe]-hydrogenase can serve as the int ...

Wiley-VCH Verlag GmbH2012

A Five-Coordinate Iron Center in the Active Site of [Fe]-Hydrogenase: Hints from a Model Study

Rosario Scopelliti, Xile Hu, Dafa Chen

The synthesis, structure, and reactivity of a five-coordinate model complex of [Fe]-hydrogenase are described. The work suggests that the iron center in [Fe]-hydrogenases could be five-coordinate in the resting state. ...

Wiley-VCH Verlag GmbH2011

Hydrogen evolution at polarised liquid/liquid interfaces catalyzed by molybdenum disulfide

Hubert Girault, Xile Hu, Heron Vrubel, Peiyu Ge, Imren Hatay

Molybdenum disulfide microparticles in suspension in an aqueous acidic solution adsorb at the interface with an organic electrolyte solution containing the reducing agent, decamethylferrocene, to catalyse hydrogen evolution. This catalytic process has been ...

2011

Synthesis and Characterization of a Series of Model Complexes of the Active Site of [Fe]-Hydrogenase (Hmd)

Rosario Scopelliti, Xile Hu, Dafa Chen

A series of Fe complexes were synthesized and characterized as small molecule mimics for the active site of [Fe]-hydrogenase (Hmd). The collection includes both structurally new compounds and analogues of previously reported models. These complexes contain ...

2011