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To be structurally well-defined or not to be, that is not the question for iron(III)–poly(4-Vinylpyridine-co-acrylamide) to exhibit catechol dioxygenase activity!
Catalysis Communications ( IF 3.7 ) Pub Date : 2017-11-13 , DOI: 10.1016/j.catcom.2017.11.006
Christopher J. Corcoran , Christian C. Tang , Vasiliki Lykourinou , Andrew C. Terentis , Alexander Angerhofer , Li-June Ming

Metal complexes of a poly(4-vinylpyridine-co-acrylamide) copolymer (P1) exhibit significant hydrolytic and oxidation/oxygenation activities. These metallopolymers exhibit enzyme-mimicking selectivity, cooperativity, and induced-fit mechanism during catalyses. Fe3+-P1 exhibits a significant catechol dioxygenase activity in aqueous media with k2(CA) = 0.011 M−1 s−1 and k2(O2) = 0.213 M−1 s−1 for aerobic oxidative catechol cleavage, comparable to many structurally characterized complexes. The substrate-bound S–Fe(III)-P1 intermediates are characterized by the use of electronic, resonance Raman, and EPR spectroscopic methods. Copolymers generally lack well-defined structures, which nevertheless should not hinder further development of functional metallopolymers for broad applications.



中文翻译:

要在结构上定义明确或不确定,铁(III)-聚(4-乙烯基吡啶--丙烯酰胺)表现出儿茶酚双加氧酶活性不是问题!

聚(4-乙烯基吡啶--丙烯酰胺)共聚物(P1)的金属络合物表现出显着的水解和氧化/氧化活性。这些金属聚合物在催化过程中表现出模仿酶的选择性,协同作用和诱导拟合机理。的Fe 3+ - P1呈现在水性介质中与显著儿茶酚双加氧酶活ķ 2(CA)  = 0.011中号-1 小号-1ķ 2(O2)  = 0.213中号-1 小号-1需氧氧化儿茶酚裂解,可比许多结构特征复杂的化合物。与底物结合的S –Fe(III)-P1中间体的特征是使用电子,共振拉曼光谱和EPR光谱法。共聚物通常缺乏明确定义的结构,然而,这不应阻碍功能性金属聚合物在广泛应用中的进一步发展。

更新日期:2017-11-13
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