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Tung, Chi-Yen; Tseng, Yu-Ting; Lu, Tsai-Te; Liaw, Wen-Feng
Inorganic chemistry, 11/2021, Letnik: 60, Številka: 21Journal Article
The ubiquitous function of nitric oxide (NO) guided the biological discovery of the natural dinitrosyliron unit (DNIU) Fe(NO)2 as an intermediate/end product after Fe nitrosylation of nonheme cofactors. Because of the natural utilization of this cofactor for the biological storage and delivery of NO, a bioinorganic study of synthetic dinitrosyliron complexes (DNICs) has been extensively explored in the last 2 decades. The bioinorganic study of DNICs involved the development of synthetic methodology, spectroscopic discrimination, biological application of NO-delivery reactivity, and translational application to the (catalytic) transformation of small molecules. In this Forum Article, we aim to provide a systematic review of spectroscopic and computational insights into the bonding nature within the DNIU Fe(NO)2 and the electronic structure of different types of DNICs, which highlights the synchronized advance in synthetic methodology and spectroscopic tools. With regard to the noninnocent nature of a NO ligand, spectroscopic and computational tools were utilized to provide qualitative/quantitative assignment of oxidation states of Fe and NO in DNICs with different redox levels and ligation modes as well as to probe the Fe–NO bonding interaction modulated by supporting ligands. Besides the strong antiferromagnetic coupling between high-spin Fe and paramagnetic NO ligands within the covalent DNIU Fe(NO)2, in polynuclear DNICs, the effects of the Fe···Fe distance, nature of the bridging ligands, and type of bridging modes on the regulation of the magnetic coupling among paramagnetic DNIU Fe(NO)2 are further reviewed. In the last part of this Forum Article, the sequential reaction of {Fe(NO)2}10 DNIC (NO)2Fe(AMP) (1-red) with NO(g), HBF4, and KC8 establishes a synthetic cycle, {Fe(NO)2}9-{Fe(NO)2}9 DNIC (NO)2Fe(μ-dAMP)2Fe(NO)2 (1) → {Fe(NO)2}9 DNIC (NO2)Fe(AMP)BF4 (1-H) → {Fe(NO)2}10 DNIC 1-red → DNIC 1, for the transformation of NO into HNO/N2O. Of importance, the NO-induced transformation of {Fe(NO)2}10 DNIC 1-red and (NO)2Fe(DTA) (2-red; DTA = diethylenetriamine) unravels a synthetic strategy for preparation of the {Fe(NO)2}9-{Fe(NO)2}9 DNICs (NO)2Fe(μ-NHR)2Fe(NO)2 containing amido-bridging ligands, which hold the potential to feature distinctive physical properties, chemical reactivities, and biological applications.
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