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
期刊名称：Angewandte Chemie (International ed. in English)
年：2019
卷：58
期：12
页码：3795-3799
ISSN：1521-3773
关键词：N-N formation,N-O cleavage,NO reduction,flavo-diiron protein,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-N2 O reduction activity of non-heme diiron enzymes, herein we report a strong second-coordination-sphere interaction between a conserved Tyr197 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-N2 O reduction activity of non-heme diiron enzymes, herein we report a strong second-coordination-sphere interaction between a conserved Tyr197 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 57 Fe M?ssbauer modeling in elucidating the structural features of not only first, but also second coordination spheres of the key transient species involved in NO/O2 activation by non-heme diiron enzymes.? 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. ...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
人气指数：2
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