Determining the TiO2-Photocatalytic Aryl-Ring-Opening Mechanism in Aqueous Solution Using Oxygen-18 Labeled O-2 and H2O
文献类型：期刊论文
| 作者 | Pang, Xibin; Chang, Wei; Chen, Chuncheng; Ji, Hongwei; Ma, Wanhong; Zhao, Jincai |
| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 |
| 出版日期 | 2014-06-18 |
| 卷号 | 136期号:24页码:8714-8721 |
| ISSN号 | 0002-7863 |
| DOI | 10.1021/ja5031936 |
| 英文摘要 | The molecules O-2 and H2O dominate the cleavage of aromatic sp(2) C-C bonds, a crucial step in the degradation of aromatic pollutants in aqueous TiO2 photocatalysis, but their precise roles in this process have remained elusive. This can be attributed to the complex oxidative species involved and to a lack of available models for reactions with a high yield of direct products. Here, we used oxygen-18 isotope labeled O-2 and H2O to observe the aromatic ring-opening reaction of the model compound 3,5-di-tert-butylcatechol (DTBC), which was mediated by TiO2 photocatalysis in an aqueous acetonitrile solution. By analyzing the primary intermediate products (similar to 75% yield), especially the seven-membered ring anhydrides that were formed, we obtained direct evidence for the oxygen atom of dioxygen insertion into a C-C bond of the aromatic ring. This indicates that molecular oxygen is the ultimate ring-opening agent in TiO2 photocatalysis and that it undergoes single O atom incorporation rather than the previously proposed molecular oxygen 1,2-addition processes. The ratio of intradiol to extradiol products depends on the particle size of TiO2 catalysts used, which suggests that the O-2 activation is correlated with the available coordination sites on the TiO2 surface in the photocatalytic cleavage of the aromatic ring. |
| 语种 | 英语 |
| WOS记录号 | WOS:000337720200036 |
| 出版者 | AMER CHEMICAL SOC |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/52303]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | Ma, Wanhong |
| 作者单位 | Chinese Acad Sci, Inst Chem, Key Lab Photochem, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China |
| 推荐引用方式 GB/T 7714 | Pang, Xibin,Chang, Wei,Chen, Chuncheng,et al. Determining the TiO2-Photocatalytic Aryl-Ring-Opening Mechanism in Aqueous Solution Using Oxygen-18 Labeled O-2 and H2O[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2014,136(24):8714-8721. |
| APA | Pang, Xibin,Chang, Wei,Chen, Chuncheng,Ji, Hongwei,Ma, Wanhong,&Zhao, Jincai.(2014).Determining the TiO2-Photocatalytic Aryl-Ring-Opening Mechanism in Aqueous Solution Using Oxygen-18 Labeled O-2 and H2O.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,136(24),8714-8721. |
| MLA | Pang, Xibin,et al."Determining the TiO2-Photocatalytic Aryl-Ring-Opening Mechanism in Aqueous Solution Using Oxygen-18 Labeled O-2 and H2O".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 136.24(2014):8714-8721. |
入库方式： OAI收割
来源：化学研究所
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