Metal-Catalyzed Formation of Organic Pollutants Intermediated by Organic Free Radicals.
Metal-Catalyzed Formation of Organic Pollutants Intermediated by Organic Free Radicals.
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DOI：
10.1021/acs.est.2c05892
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发表时间：
2022-09
影响因子：
11.4
通讯作者：
Shuting Liu;Guorui Liu;Lili Yang;Xiaoyun Liu;Mingxuan Wang;Linjun Qin;M. Zheng
中科院分区：
文献类型：
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作者：
Shuting Liu;Guorui Liu;Lili Yang;Xiaoyun Liu;Mingxuan Wang;Linjun Qin;M. Zheng
在热相关过程中，金属化合物在有机污染物的形成中起着重要作用。然而，金属催化的主要有机污染物以前没有被表征，也没有任何详细的催化机制澄清。本文通过实验室和理论研究，对有机污染物形成过程中金属催化剂表面存在的多种有机自由基中间体进行了细致的区分。研究了不同金属化合物催化下有机自由基中间体种类、浓度及形成机理的差异。结果与有机污染物产物的不同特性相互印证。CuO主要催化高氯化苯氧基中间体和二恶英的形成。在氧化锌表面发现了高比例的半醌自由基和含氧衍生物。不同的是，甲基取代的苯氧自由基和长链产物在Al2O3表面形成。研究结果对富不同金属化合物热相关过程中重点有机污染物的目标排放控制具有指导意义。
Metal compounds play important roles in the formation of organic pollutants during thermal-related processes. However, the metal-catalyzed predominant organic pollutants have not previously been characterized nor have any detailed catalytic mechanisms been clarified. Here, we preciously distinguished the multiple organic free radical intermediates on metal catalyst surfaces during the organic pollutant formation through laboratory and theoretical studies. Differences between the organic free radical intermediate species, concentrations, and formation mechanisms under the catalysis of different metal compounds were investigated. The results were verified mutually with the differed characteristics of organic pollutant products. CuO predominantly catalyzed the formation of highly chlorinated phenoxy radical intermediates and dioxins. High proportions of semiquinone radicals and oxygen-containing derivatives were found on ZnO surfaces. Differently, methyl-substituted phenoxy radicals and long-chain products formed on Al2O3 surfaces. The results will be instructive for the target emission control of priority organic pollutants during thermal-related processes rich in different metal compounds.