A Biomimetic System for Studying Salicylate Dioxygenase.

A Biomimetic System for Studying Salicylate Dioxygenase.
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用于研究水杨酸双加氧酶的仿生系统。

DOI:
10.1021/bk-2019-1317.ch004
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发表时间:
2019
期刊:
ACS symposium series. American Chemical Society
影响因子:
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通讯作者:
Chavez,FermanA
Chavez,FermanA
中科院分区:
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文献类型:
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作者:
Banerjee,Atanu;Li,Jia;Molenda,MonikaA;Brennessel,WilliamW;Chavez,FermanA

文献摘要

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我们报告了 [Fe(T1Et4iPrIP)(sal)] (2) (T1Et4iPrIP = 三(1-乙基-4-异丙基-咪唑基)膦;sal2–= 水杨酸双阴离子)的表征,它作为底物结合水杨酸双加氧酶 (SDO) 的模型。配合物2结晶于单斜空间群P21/n,a= 10.7853(12) Å,b= 16.5060(19) Å,c= 21.217(2) Å,β= 94.489(2)°,V= 3765.5(7) Å3。该结构由扭曲的方锥几何形状 (τ= 0.32) 的 FeII 键合组成,具有两个水杨酸氧和两个 T1Et4iPrIP 氮作为基础,顶端位置由另一个配体氮占据。 [Fe(T1Et4iPrIP)(OTf)2] (1),2 的前体,在 O2 存在下催化 1,4-二羟基-2-萘甲酸酯的裂解。 Complex1 还能够在 H2O2 存在下裂解水杨酸酯芳环。该反应向产物形成的过程涉及 FeIII-酚盐物质。
We report the characterization of [Fe(T1Et4iPrIP)(sal)] (2) (T1Et4iPrIP = tris(1-ethyl-4-isopropyl-imidazolyl)phosphine; sal2–= salicylate dianion), which serves as a model for substrate-bound salicylate dioxygenase (SDO). Complex2crystallizes in the monoclinic space groupP21/n witha= 10.7853(12) Å,b= 16.5060(19) Å,c= 21.217(2) Å,β= 94.489(2)°,andV= 3765.5(7) Å3. The structure consists of FeIIbonded in distorted square pyramidal geometry (τ= 0.32) with two salicylate oxygens and two T1Et4iPrIP nitrogens serving as the base and the apical position occupied by the other ligand nitrogen. [Fe(T1Et4iPrIP)(OTf)2] (1), the precursor for2, catalyzes the cleavage of 1,4-dihydroxy-2-naphthoate in the presence of O2. Complex1is also capable of cleaving the salicylate aromatic ring in the presence of H2O2. The progression of this reaction toward product formation involves an FeIII–phenoxide species.