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首页> 外文期刊>Catalysis science & technology >A cobalt-substituted Keggin-type polyoxometalate for catalysis of oxidative aromatic cracking reactions in water
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A cobalt-substituted Keggin-type polyoxometalate for catalysis of oxidative aromatic cracking reactions in water

机译：一个cobalt-substituted Keggin-type polyoxometalate的催化氧化芳开裂反应在水里

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摘要

Efficient detoxification of harmful benzene rings into useful carboxylic acids in water is indispensable for achieving a clean water environment. We report herein that oxidative aromatic cracking (OAC) reactions in water were achieved using a catalytic system with a cobalt-substituted Keggin-type polyoxometalate (Co-POM) as a catalyst, an Oxone (R) monopersulfate compound as a sacrificial oxidant and sodium bicarbonate as an additive under mild conditions. Sodium bicarbonate plays a crucial role in the selective OAC reactions by Co-POM using ethylbenzenesulfonate as a model substrate. The reactive species was characterized to be a cobalt(iii)-oxyl species based on P-31 NMR, UV-vis spectroscopic, kinetic, and theoretical analyses. The electrophilicity of the cobalt(iii)-oxyl species was demonstrated by a linear relationship with a negative slope in the Hammett plots of initial rates obtained from the OAC reactions of m-xylenesulfonate derivatives. Besides, we have verified the degradation pathway of the OAC reactions using benzene as a model substrate in the catalytic system. The degradation was initiated by an electrophilic attack of the cobalt(iii)-oxyl species on benzene to yield phenol followed by producing catechol, muconic acid, maleic/fumaric acid, tartaric acid derivatives and formic acid on the basis of H-1 NMR spectroscopic analysis.
机译：有效的有害苯环解毒水是有用的羧酸不可或缺的实现一个干净的水环境。芳香开裂(OAC)反应在水里通过使用一个催化系统cobalt-substituted Keggin-type polyoxometalate(Co-POM)作为催化剂,硫酸氢钾(右)monopersulfate化合物作为牺牲氧化剂和碳酸氢钠作为添加剂在温和条件。作用选择性OAC Co-POM反应使用ethylbenzenesulfonate作为模型底物。的特点是活性物种钴(3)基于31页NMR -oxyl物种,紫外可见光谱、动态和理论分析。(3)钴-oxyl物种证明了与负斜率的线性关系哈米特情节中获得的初始利率OAC反应m-xylenesulfonate衍生品。此外,我们已经验证了降解途径的OAC反应用苯作为模型底物的催化体系。退化是由一个亲电攻击(iii) -oxyl钴物种的苯屈服苯酚生产儿茶酚,紧随其后粘康酸、顺丁烯二酸/反丁烯二酸、酒石酸衍生品和h -甲酸的基础上核磁共振光谱分析。

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