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基于乙二胺四乙酸的亚苯基大环及其无环类似物的铜（II）和铁（III）配合物的结构与过氧化物酶样活性的比较研究

Comparative Studies of Structures and Peroxidase-like Activities of Copper(II) and Iron(III) Complexes with an EDTA-Based Phenylene-Macrocycle and Its Acyclic Analogue.

作者信息

Beltran-Torres Melissa, Sugich-Miranda Rocío, Santacruz-Ortega Hisila, Machi Lorena, Inoue Motomichi, Velázquez-Contreras Enrique F, Soberanes Yedith, Höpfl Herbert, Pérez-González Refugio, Navarro Rosa Elena, Salazar-Medina Alex J, Sotelo Mundo Rogerio R

机构信息

Departamento de Investigación en Polímeros y Materiales and Departamento de Ciencias Químico Biológicas, Universidad de Sonora, Blvd. Luis Encinas y Calle Rosales S/N, Hermosillo, Sonora 83000, Mexico.

Centro de Investigación en Alimentación y Desarrollo A.C. (CIAD), Carretera Gustavo Enrique Astiazarán Rosas Num. 46 Col. La Victoria, Hermosillo, Sonora 83304, Mexico.

出版信息

ACS Omega. 2019 Dec 18;4(27):22487-22496. doi: 10.1021/acsomega.9b03164. eCollection 2019 Dec 31.

DOI:10.1021/acsomega.9b03164
PMID:31909331
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6941385/
Abstract

With the objective of studying the conformational and macrocyclic effects of selected metal chelates on their peroxidase activities, Cu and Fe complexes were synthesized with a macrocyclic derivative of ethylenediaminetetraacetic acid and -phenylenediamine (abbreviated as edtaodH) and its new open-chain analogue (edtabzH). The Fe complex of edtaodH has a peroxidase-like activity, whereas the complex of edtabzH does not. The X-ray study of the former shows the formation of a dimeric molecule {[Fe(edtaod)]O} in which each metal with an octahedral coordination is overposed over the macrocyclic cavity, as a result of rigid macrocyclic frame, to form an Fe-O-Fe bridge; the exposure of the central metal to the environment facilitates the capture of oxygen to drive the biomimetic activity. The peroxidase-inactive Fe complex consists of a mononuclear complex ion [Fe(edtabz)(HO)], the metal ion of which is suited in a distorted pentagonal bipyramid to be protected from environmental oxygen. The copper(II) complexes, which have mononuclear structures with high thermodynamic stability compared with the iron(III) complexes, show no peroxidase activity. The steric effects play a fundamental role in the biomimetic activity.

摘要

为了研究所选金属螯合物的构象和大环效应及其过氧化物酶活性，合成了铜和铁与乙二胺四乙酸和对苯二胺的大环衍生物（缩写为edtaodH）及其新的开链类似物（edtabzH）的配合物。edtaodH的铁配合物具有类过氧化物酶活性，而edtabzH的配合物则没有。对前者的X射线研究表明形成了二聚体分子{[Fe(edtaod)]O}，其中每个具有八面体配位的金属由于刚性大环框架而重叠在大环腔内，形成Fe-O-Fe桥；中心金属暴露于环境中有利于捕获氧气以驱动仿生活性。无过氧化物酶活性的铁配合物由单核络合离子[Fe(edtabz)(H₂O)]组成，其金属离子处于扭曲的五角双锥中以防止环境中的氧气。与铁（III）配合物相比，具有单核结构且具有高热力学稳定性的铜（II）配合物没有过氧化物酶活性。空间效应在仿生活性中起基本作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/19ad/6941385/0fae185a066e/ao9b03164_0007.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/19ad/6941385/5b5ddd8b10af/ao9b03164_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/19ad/6941385/c1faf1b2b87a/ao9b03164_0003.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/19ad/6941385/0fae185a066e/ao9b03164_0007.jpg

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