用于增强转移加氢脱卤的不对称CoN3P1单原子催化位点,Green Chemistry

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用于增强转移加氢脱卤的不对称CoN3P1单原子催化位点
Green Chemistry ( IF 9.3 ) Pub Date : 2024-03-13 , DOI: 10.1039/d3gc04739c
Wendi Guo ₁ , Zehui Sun ₁ , Mengjiao Xu ₁ , Kaizhi Wang ₁ , Mugeng Chen ₁ , Conglin Zhu ₁ , Heyong He ₁ , Yongmei Liu ₁ , Yong Cao ₁

Affiliation

从有机物质中高效、环保地去除卤素取代基对于减少持久性卤代化合物造成的生态和健康危害至关重要。在这方面，我们引入了 CoN ₃ P ₁ @NP-PC，这是一种新型的不对称 CoN ₃ P _{1单原子催化剂，它仅使用两当量的 HCOONH}₄作为良性且有效的还原剂，在转移加氢脱卤（HDH）中表现出出色的效率。代理人。该催化剂利用 ZIF-8 前驱体的高孔隙率和大表面积，通过简单的后注入方法合成。通过一系列光谱和显微技术进行的广泛表征证实了 CoN ₃ P ₁ @NP-PC 优异的原子分散性和不对称结构完整性，这更有利于 HCOONH ₄活化，从而可以在电子转移的同时轻松产生氢自由基。在我们的综合评估中，CoN ₃ P ₁ @NP-PC 在转化各种卤化底物、有效处理具有不同官能团和复杂分子结构的化合物方面表现出出色的多功能性。值得注意的是，CoN ₃ P ₁ @NP-PC 被证明在分解 2,4,6-三溴苯酚和四溴双酚 A 等溴化阻燃剂方面特别有效，增强了其作为生态恢复和污染控制强大工具的潜力。

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Asymmetric CoN3P1 single-atom catalytic sites for enhanced transfer hydrodehalogenation

The efficient and environmentally friendly removal of halogen substituents from organic substances is crucial for reducing the ecological and health hazards posed by persistent halogenated compounds. In this regard, we introduce CoN₃P₁@NP-PC, a novel asymmetric CoN₃P₁ single-atom catalyst, which demonstrates outstanding efficiency in transfer hydrodehalogenation (HDH) using just two equivalents of HCOONH₄ as a benign and effective reducing agent. This catalyst was synthesized through a simple post-implantation method, capitalizing on the high porosity and large surface area of ZIF-8 precursors. Extensive characterization via a range of spectroscopic and microscopic techniques confirmed CoN₃P₁@NP-PC's superior atomic dispersion and asymmetric structural integrity, which was more favourable for HCOONH₄ activation allowing facile generation of hydrogen radicals along with electron transfer. In our comprehensive evaluation, CoN₃P₁@NP-PC displayed outstanding versatility for the transformation of a diverse array of halogenated substrates, efficiently processing compounds with varied functional groups and complex molecular structures. Notably, CoN₃P₁@NP-PC proved particularly effective in breaking down brominated flame retardants such as 2,4,6-tribromophenol and tetrabromobisphenol A, reinforcing its potential as a powerful tool for ecological restoration and pollution control.

更新日期：2024-03-13

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