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DOI | 10.1038/s41467-018-05431-x |
Accumulating the hydride state in the catalytic cycle of [FeFe]-hydrogenases | |
Winkler, Martin1; Senger, Moritz2; Duan, Jifu1; Esselborn, Julian1; Wittkamp, Florian3; Hofmann, Eckhard4; Apfel, Ulf-Peter3; Stripp, Sven Timo2; Happe, Thomas1 | |
2017-07-19 | |
发表期刊 | NATURE COMMUNICATIONS |
ISSN | 2041-1723 |
出版年 | 2017 |
卷号 | 8 |
文章类型 | Article |
语种 | 英语 |
国家 | Germany |
英文摘要 | H-2 turnover at the [FeFe]-hydrogenase cofactor (H-cluster) is assumed to follow a reversible heterolytic mechanism, first yielding a proton and a hydrido-species which again is double-oxidized to release another proton. Three of the four presumed catalytic intermediates (H-ox, H-red/H-red and H-sred) were characterized, using various spectroscopic techniques. However, in catalytically active enzyme, the state containing the hydrido-species, which is eponymous for the proposed heterolytic mechanism, has yet only been speculated about. We use different strategies to trap and spectroscopically characterize this transient hydride state (H-hyd) for three wild-type [FeFe]-hydrogenases. Applying a novel set-up for real-time attenuated total-reflection Fourier-transform infrared spectroscopy, we monitor compositional changes in the state-specific infrared signatures of [FeFe]-hydrogenases, varying buffer pH and gas composition. We selectively enrich the equilibrium concentration of Hhyd, applying Le Chatelier's principle by simultaneously increasing substrate and product concentrations (H-2/H+). Site-directed manipulation, targeting either the proton-transfer pathway or the adt ligand, significantly enhances H-hyd accumulation independent of pH. |
领域 | 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000405816900001 |
WOS关键词 | COUPLED ELECTRON-TRANSFER ; ACTIVE-SITE ; H-CLUSTER ; DESULFOVIBRIO-DESULFURICANS ; FEFE HYDROGENASES ; SYNTHETIC MODELS ; REDUCED-STATE ; PROTEIN ; IDENTIFICATION ; MECHANISM |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/203923 |
专题 | 资源环境科学 |
作者单位 | 1.Ruhr Univ Bochum, Lehrstuhl Biochem Pflanzen, Fak Biol & Biotechnol, AG Photobiotechnol, Univ Str 150, D-44801 Bochum, Germany; 2.Free Univ Berlin, Dept Phys, Expt Mol Biophys, Arnimallee 14, D-14195 Berlin, Germany; 3.Ruhr Univ Bochum, Fak Chem & Biochem, Lehrstuhl Anorgan Chem Bioanorgan Chem 1, Univ Str 150, D-44801 Bochum, Germany; 4.Ruhr Univ Bochum, AG Prot Kristall, Lehrstuhl Biophys, Fak Biol & Biotechnol, Univ Str 150, D-44801 Bochum, Germany |
推荐引用方式 GB/T 7714 | Winkler, Martin,Senger, Moritz,Duan, Jifu,et al. Accumulating the hydride state in the catalytic cycle of [FeFe]-hydrogenases[J]. NATURE COMMUNICATIONS,2017,8. |
APA | Winkler, Martin.,Senger, Moritz.,Duan, Jifu.,Esselborn, Julian.,Wittkamp, Florian.,...&Happe, Thomas.(2017).Accumulating the hydride state in the catalytic cycle of [FeFe]-hydrogenases.NATURE COMMUNICATIONS,8. |
MLA | Winkler, Martin,et al."Accumulating the hydride state in the catalytic cycle of [FeFe]-hydrogenases".NATURE COMMUNICATIONS 8(2017). |
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