The Regular/Persistent Free Radicals and Associated Reaction Mechanism for the Degradation of 1,2,4-Trichlorobenzene over Different MnO2 Polymorphs
文献类型：期刊论文
| 作者 | Huang, Xinchen; Li, Qianqian; Su, Guijin; Zheng, Minghui; Huang, Chunhua; Wang, Mengjing; Ma, Chunyan ; Wei, Da
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| 刊名 | ENVIRONMENTAL SCIENCE & TECHNOLOGY
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| 出版日期 | 2018-11-20 |
| 卷号 | 52期号:22页码:13351-13360 |
| ISSN号 | 0013-936X |
| 文献子类 | Article |
| 英文摘要 | The role of regular/persistent free radicals on the catalytic activity of K+-tuned MnO2 tunnel structures is poorly understood to date. Herein, three MnO2 polymorphs (alpha-, beta-, and delta-MnO2) were synthesized and examined toward the degradation of 1,2,4-trichlorobenzene (1,2,4-TrCBz) at 300 degrees C. delta-MnO2, with a two-dimensional-layered tunnel structure tuned by K+, exhibited the highest activity among the three MnO2 polymorphs. The electron spin resonance spectroscopy results confirmed that delta-MnO2 featured the most abundant reactive oxygen species (ROS: O-2(-center dot), center dot OH, and O-1(2)), followed by alpha-MnO2 (O-2(-center dot) and O-1(2)), and beta-MnO2 (O-2(-center dot)), being supported by the calculated energy barrier. It was, intriguingly, noted that persistent organic free radicals, newly recognized as emerging surface-stabilized compound, were remarkably detected in alpha- and beta-MnO2/1,2,4-TrCBz systems but not in more reactive delta-MnO2/1,2,4-TrCBz system. These might contribute to discrepant oxidative degradation process. During the oxidative process, intermediates, including benzoic acid and glycerol, formed via attack by ROS. Upon further attack, these intermediates fragmented into smaller molecules such as formic, acetic, propionic, and butyric acids. The present findings give deeper insights into the role of free radicals on the catalytic degradation of chlorinated aromatics. |
| 源URL | [http://ir.rcees.ac.cn/handle/311016/41101]  |
| 专题 | 生态环境研究中心_环境纳米材料实验室 |
| 推荐引用方式 GB/T 7714 | Huang, Xinchen,Li, Qianqian,Su, Guijin,et al. The Regular/Persistent Free Radicals and Associated Reaction Mechanism for the Degradation of 1,2,4-Trichlorobenzene over Different MnO2 Polymorphs[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2018,52(22):13351-13360. |
| APA | Huang, Xinchen.,Li, Qianqian.,Su, Guijin.,Zheng, Minghui.,Huang, Chunhua.,...&Wei, Da.(2018).The Regular/Persistent Free Radicals and Associated Reaction Mechanism for the Degradation of 1,2,4-Trichlorobenzene over Different MnO2 Polymorphs.ENVIRONMENTAL SCIENCE & TECHNOLOGY,52(22),13351-13360. |
| MLA | Huang, Xinchen,et al."The Regular/Persistent Free Radicals and Associated Reaction Mechanism for the Degradation of 1,2,4-Trichlorobenzene over Different MnO2 Polymorphs".ENVIRONMENTAL SCIENCE & TECHNOLOGY 52.22(2018):13351-13360. |
入库方式： OAI收割
来源：生态环境研究中心
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