文献详情
Origin of Nitric Oxide Reduction Activity in Flavo-Diiron NO Reductase: Key Roles of the Second Coordination Sphere
文献类型：期刊
通讯作者：Chen, H (reprint author), Chinese Acad Sci, Res Educ Ctr Excellence Mol Sci, Key Lab Photochem, BNLMS,Inst Chem, Beijing 100190, Peoples R China.; Lai, WZ (reprint author), Renmin Univ China, Dept Chem, Beijing 100872, Peoples R China.
期刊名称：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION影响因子和分区
年：2019
卷：58
期：12
页码：3795-3799
ISSN：1433-7851
关键词：flavo-diiron protein; N-N formation; N-O cleavage; NO reduction; second coordination sphere
所属部门：化学系
摘要：The second coordination sphere constitutes a distinguishing factor in the active site to modulate enzymatic reactivity. To unravel the origin of NO-to-N2O reduction activity of non-heme diiron enzymes, herein we report a strong second-coordination-sphere interaction between a conserved Tyr(197) and the key iron-nitrosyl intermediate of Tm FDP (flavo-diiron protein), which leads to decreased reaction barriers towards N-N formation and N-O cleavage in NO reduction. This finding supports the direct ...More
The second coordination sphere constitutes a distinguishing factor in the active site to modulate enzymatic reactivity. To unravel the origin of NO-to-N2O reduction activity of non-heme diiron enzymes, herein we report a strong second-coordination-sphere interaction between a conserved Tyr(197) and the key iron-nitrosyl intermediate of Tm FDP (flavo-diiron protein), which leads to decreased reaction barriers towards N-N formation and N-O cleavage in NO reduction. This finding supports the direct coupling of diiron dinitrosyl as the N-N formation mode in our QM/MM modeling, and reconciles the mechanistic controversy of external reduction between FDPs and synthetic biomimetics of the iron-nitrosyls. This work highlights the application of QM/MM Fe-57 Mossbauer modeling in elucidating the structural features of not only first, but also second coordination spheres of the key transient species involved in NO/O-2 activation by non-hence diiron enzymes. ...Hide

DOI：10.1002/anie.201812343
百度学术：Origin of Nitric Oxide Reduction Activity in Flavo-Diiron NO Reductase: Key Roles of the Second Coordination Sphere
语言：外文
被引频次：5
人气指数：1
浏览次数：1
基金：National Natural Science Foundation of China (NSFC)National Natural Science Foundation of China [21873103, 21833011, 21673286]
作者其他论文



Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin.Liu, Yanju, Han, Yongzhen, Zhang, Zongyao, et al. .CHEMICAL SCIENCE. 2019, 10(9), 2613-2622.
Mechanistic Insights into a Stibene Cleavage Oxygenase NOV1 from Quantum Mechanical/Molecular Mechanical Calculations.Lu, Jiarui, Lai, Wenzhen,.CHEMISTRYOPEN. 2019, 8(2), 228-235.
Mechanistic insights into a non-heme 2-oxoglutarate-dependent ethylene-forming enzyme: selectivity of ethylene-formation versusl-Arg hydroxylation.Xue, Junqin, Lu, Jiarui, Lai, Wenzhen,.PHYSICAL CHEMISTRY CHEMICAL PHYSICS. 2019, 21(19), 9957-9968.
Somatic and cultural knowledge: drivers of a habitus-driven model of tacit knowledge acquisition.Chen, Hui, Nunes, Jose Miguel Baptista, Ragsdell, Gillian, et al. .JOURNAL OF DOCUMENTATION. 2019, 75(5), 927-953.
Supervisor developmental feedback and employee performance: The roles of feedback-seeking and political skill.Su, Weilin, Lyu, Bei, Liu, Yanjun, et al. .JOURNAL OF PSYCHOLOGY IN AFRICA. 2019, 29(5), 435-442.