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DOI | 10.1126/science.aaz6748 |
Structural evidence for a dynamic metallocofactor during N2 reduction by Mo-nitrogenase | |
Kang W.; Lee C.C.; Jasniewski A.J.; Ribbe M.W.; Hu Y. | |
发表日期 | 2020 |
ISSN | 0036-8075 |
起始页码 | 1381 |
结束页码 | 1385 |
卷号 | 368期号:6497 |
英文摘要 | The enzyme nitrogenase uses a suite of complex metallocofactors to reduce dinitrogen (N2) to ammonia. Mechanistic details of this reaction remain sparse. We report a 1.83-angstrom crystal structure of the nitrogenase molybdenum-iron (MoFe) protein captured under physiological N2 turnover conditions. This structure reveals asymmetric displacements of the cofactor belt sulfurs (S2B or S3A and S5A) with distinct dinitrogen species in the two ab dimers of the protein. The sulfur-displaced sites are distinct in the ability of protein ligands to donate protons to the bound dinitrogen species, as well as the elongation of either the Mo-O5 (carboxyl) or Mo-O7 (hydroxyl) distance that switches the Mo-homocitrate ligation from bidentate to monodentate. These results highlight the dynamic nature of the cofactor during catalysis and provide evidence for participation of all belt-sulfur sites in this process. © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works |
关键词 | ammoniacatalysiscrystal structureenzyme activityligandphysiological responsesulfurligandmolybdenum iron proteinnitrogensulfurAzotobacter vinelandiibiocatalysischemistryenzymologyoxidation reduction reactionprotein multimerizationX ray crystallographyAzotobacter vinelandiiBiocatalysisCrystallography, X-RayLigandsMolybdoferredoxinNitrogenOxidation-ReductionProtein MultimerizationSulfur |
语种 | 英语 |
来源机构 | Science |
文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/133410 |
推荐引用方式 GB/T 7714 | Kang W.,Lee C.C.,Jasniewski A.J.,et al. Structural evidence for a dynamic metallocofactor during N2 reduction by Mo-nitrogenase[J]. Science,2020,368(6497). |
APA | Kang W.,Lee C.C.,Jasniewski A.J.,Ribbe M.W.,&Hu Y..(2020).Structural evidence for a dynamic metallocofactor during N2 reduction by Mo-nitrogenase.,368(6497). |
MLA | Kang W.,et al."Structural evidence for a dynamic metallocofactor during N2 reduction by Mo-nitrogenase".368.6497(2020). |
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