首页> 中文期刊>辽宁石油化工大学学报 >含氮六元杂环氮氧自由基有机催化剂的结构与活性关系

含氮六元杂环氮氧自由基有机催化剂的结构与活性关系

     

摘要

基于氮氧自由基有机催化剂的催化分子氧氧化技术是近年来催化领域关注的热点之一.采用理论方法研究了吡啶环和吡嗪环取代N-羟基邻苯二甲酰亚胺(NHPI)苯环所得含氮六元杂环催化剂的结构与催化活性,考察了质子酸HCl对这类催化剂催化活性的影响.结果表明,含氮六元杂环催化剂的催化活性均高于NHPI,部分催化剂的活性可与高效催化剂N,N'-二羟基邻苯二甲酰亚胺(NDHPI)相当;吡嗪环比吡啶环更有助于提高催化剂的催化活性;HCl与这类催化剂芳环的氢键相互作用可以提高催化剂的催化活性.本研究有助于加深对该类催化剂本征催化活性的认识,也有助于为该类催化剂的催化机理研究和催化氧化实验提供理论指导.%The catalytic oxidation of molecular oxygen based on nitroxide radical organocatalysts is one of the hot topics in the field of catalysis in recent years.The structures and catalytic activity of the nitrogenous six-membered heterocyclic ring obtained by the pyridine ring and the pyrazine ring substituted for the benzene ring of N-Hydroxyphthallimide (NHPI)were studied by theoretical methods.The effect of protonic acid HCl on the catalytic activity of this kind of catalyst was investigated.The results show that the catalytic activity of nitrogenous six-membered heterocyclic ring catalyst is higher than that of NHPI,even some of the catalyst is comparable to that of N,N'-dihydroxypyromellitimide (NDHPI);pyrazine pyridine ring chain is helpful to improve the catalytic activity of the catalyst;HCl hydrogen bond interaction with the aromatic ring of these catalysts can improve the catalytic activity of the catalyst.This study is helpful to deepen the understanding of the intrinsic activity of this kind of catalyst and also to provide theoretical guidance for the catalytic mechanism and catalytic oxidation experiment of this kind of catalyst.

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