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DOI10.1126/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
ISSN0036-8075
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
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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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