ArticleThe Journal of biological chemistry2011
O2 reactions at the six-iron active site (H-cluster) in [FeFe]-hydrogenase.
Article in The Journal of biological chemistry, 2011. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 26 papers.
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26 citing papers in PubMed, 87 citations in OpenAlex.
- Anaerobic cryoEM protocols for air-sensitive nitrogenase proteins.Nature protocols · 2024Review
- Binding of exogenous cyanide reveals new active-site states in [FeFe] hydrogenases.Chemical science · 2023Article
- Increasing the OACS catalysis · 2023Article
- Second and Outer Coordination Sphere Effects in Nitrogenase, Hydrogenase, Formate Dehydrogenase, and CO Dehydrogenase.Chemical reviews · 2022Review
- Lewis acid protection turns cyanide containing [FeFe]-hydrogenase mimics into proton reduction catalysts.Dalton transactions (Cambridge, England : 2003) · 2022Article
- HydG, the "dangler" iron, and catalytic production of free CO and CNDalton transactions (Cambridge, England : 2003) · 2021Article
- The roles of chalcogenides in OChemical science · 2020Review
- [FeFe]-hydrogenase maturation: H-cluster assembly intermediates tracked by electron paramagnetic resonance, infrared, and X-ray absorption spectroscopy.Journal of biological inorganic chemistry : JBIC : a publication of the Society of Biological Inorganic Chemistry · 2020Article
- Re-routing photosynthetic energy for continuous hydrogen production in vivo.Biotechnology for biofuels · 2019Article
- Overview of the Maturation Machinery of the H-Cluster of [FeFe]-Hydrogenases with a Focus on HydF.International journal of molecular sciences · 2018Review
- Absolute quantification of selected photosynthetic electron transfer proteins in Chlamydomonas reinhardtii in the presence and absence of oxygen.Photosynthesis research · 2018Article
- Mechanism of ONature chemistry · 2017Article
- Vibrational spectroscopy reveals the initial steps of biological hydrogen evolution.Chemical science · 2016Article
- Stepwise isotope editing of [FeFe]-hydrogenases exposes cofactor dynamics.Proceedings of the National Academy of Sciences of the United States of America · 2016Article
- Secondary coordination sphere accelerates hole transfer for enhanced hydrogen photogeneration from [FeFe]-hydrogenase mimic and CdSe QDs in water.Scientific reports · 2016Article
- Lyophilization protects [FeFe]-hydrogenases against O2-induced H-cluster degradation.Scientific reports · 2015Article
- Implementation of photobiological H2 production: the O 2 sensitivity of hydrogenases.Photosynthesis research · 2015Article
- Sustainable hydrogen photoproduction by phosphorus-deprived marine green microalgae Chlorella sp.International journal of molecular sciences · 2015Article
- [FeFe]-hydrogenase abundance and diversity along a vertical redox gradient in Great Salt Lake, USA.International journal of molecular sciences · 2014Article
- Evolutionary and biotechnological implications of robust hydrogenase activity in halophilic strains of Tetraselmis.PloS one · 2014Article
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8 authors at 2 institutions in 1 country.
Funding
No grant is acknowledged in the PubMed record.
Abstract
Irreversible inhibition by molecular oxygen (O(2)) complicates the use of [FeFe]-hydrogenases (HydA) for biotechnological hydrogen (H(2)) production. Modification by O(2) of the active site six-iron complex denoted as the H-cluster ([4Fe4S]-2Fe(H)) of HydA1 from the green alga Chlamydomonas reinhardtii was characterized by x-ray absorption spectroscopy at the iron K-edge. In a time-resolved approach, HydA1 protein samples were prepared after increasing O(2) exposure periods at 0 °C. A kinetic analysis of changes in their x-ray absorption near edge structure and extended X-ray absorption fine structure spectra revealed three phases of O(2) reactions. The first phase (τ(1) ≤ 4 s) is characterized by the formation of an increased number of Fe-O,C bonds, elongation of the Fe-Fe distance in the binuclear unit (2Fe(H)), and oxidation of one iron ion. The second phase (τ(2) ≈ 15 s) causes a ∼50% decrease of the number of ∼2.7-Å Fe-Fe distances in the [4Fe4S] subcluster and the oxidation of one more iron ion. The final phase (τ(3) ≤ 1000 s) leads to the disappearance of most Fe-Fe and Fe-S interactions and further iron oxidation. These results favor a reaction sequence, which involves 1) oxygenation at 2Fe(H(+)) leading to the formation of a reactive oxygen species-like superoxide (O(2)(-)), followed by 2) H-cluster inactivation and destabilization due to ROS attack on the [4Fe4S] cluster to convert it into an apparent [3Fe4S](+) unit, leading to 3) complete O(2)-induced degradation of the remainders of the H-cluster. This mechanism suggests that blocking of ROS diffusion paths and/or altering the redox potential of the [4Fe4S] cubane by genetic engineering may yield improved O(2) tolerance in [FeFe]-hydrogenase.
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