铁和一氧化氮的生物学相关配位化学：电子结构和反应性,Chemical Reviews

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铁和一氧化氮的生物学相关配位化学：电子结构和反应性
Chemical Reviews ( IF 51.4 ) Pub Date : 2021-12-13 , DOI: 10.1021/acs.chemrev.1c00253
Nicolai Lehnert ₁ , Eunsuk Kim ₂ , Hai T Dong ₁ , Jill B Harland ₁ , Andrew P Hunt ₁ , Elizabeth C Manickas ₁ , Kady M Oakley ₂ , John Pham ₂ , Garrett C Reed ₁ , Victor Sosa Alfaro ₁

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一氧化氮 (NO) 是一种重要的信号分子，在生物学中涉及广泛的生理和病理事件。金属配位化学，尤其是铁配位化学，是许多涉及 NO 的生物转化的核心。一系列血红素蛋白、一氧化氮合酶 (NOS)、可溶性鸟苷酸环化酶 (sGC) 和 nitrophorins 负责 NO 的生物合成、传感和运输。或者，NO 可以通过含血红素和铜的亚硝酸盐还原酶 (NIR) 从亚硝酸盐中产生。含 NO 的小分子如亚硝基硫醇和二亚硝基铁络合物 (DNIC) 可以作为 NO 储存和运输的替代载体。一旦 NO 形成，NO 丰富的化学反应导致多种生物活性，包括通过血红素或非血红素铁的 NO 还原酶还原 NO，以及通过 DNIC 进行蛋白质翻译后修饰。我们对生物学中金属位点与 NO 的反应性以及这些转化机制的大部分理解来自对几何和电子结构以及合成模型系统的化学反应性的阐明，与对相关蛋白质的生化和生物物理研究协同作用他们自己。本综述重点介绍蛋白质和模型复合物研究的最新进展，这些进展不仅提高了我们对 NO 的生物学作用的理解，而且为生物医学研究和能源科学中的仿生催化剂设计奠定了基础。

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The Biologically Relevant Coordination Chemistry of Iron and Nitric Oxide: Electronic Structure and Reactivity

Nitric oxide (NO) is an important signaling molecule that is involved in a wide range of physiological and pathological events in biology. Metal coordination chemistry, especially with iron, is at the heart of many biological transformations involving NO. A series of heme proteins, nitric oxide synthases (NOS), soluble guanylate cyclase (sGC), and nitrophorins, are responsible for the biosynthesis, sensing, and transport of NO. Alternatively, NO can be generated from nitrite by heme- and copper-containing nitrite reductases (NIRs). The NO-bearing small molecules such as nitrosothiols and dinitrosyl iron complexes (DNICs) can serve as an alternative vehicle for NO storage and transport. Once NO is formed, the rich reaction chemistry of NO leads to a wide variety of biological activities including reduction of NO by heme or non-heme iron-containing NO reductases and protein post-translational modifications by DNICs. Much of our understanding of the reactivity of metal sites in biology with NO and the mechanisms of these transformations has come from the elucidation of the geometric and electronic structures and chemical reactivity of synthetic model systems, in synergy with biochemical and biophysical studies on the relevant proteins themselves. This review focuses on recent advancements from studies on proteins and model complexes that not only have improved our understanding of the biological roles of NO but also have provided foundations for biomedical research and for bio-inspired catalyst design in energy science.

更新日期：2021-12-22

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