Mechanism of degradation of a nitrogenous heterocycle induced by a reductive radical: decomposition of a sym-triazine ring
文献类型：期刊论文
| 作者 | Lyu, GX; Shi, GS; Tang, L; Fang, HP; Wu, MH |
| 刊名 | PHYSICAL CHEMISTRY CHEMICAL PHYSICS
 |
| 出版日期 | 2017 |
| 卷号 | 19期号:14页码:9354-9357 |
| ISSN号 | 1463-9076 |
| DOI | 10.1039/c7cp00004a |
| 文献子类 | 期刊论文 |
| 英文摘要 | Cyanuric acid is a major component of many materials and chemicals, and is the most important intermediate in the degradation processes of sym-triazine compounds in the natural environment, as well as being used for water treatment. However, the degradation mechanism of cyanuric acid is still unclear in various advanced oxidation processes (AOPs), where (OH)-O-center dot is usually regarded as the dominant radical. Here, using a combination of density functional theory calculations and experimental observations, we unexpectedly show that the sym-triazine ring structure is broken efficiently by reductive free radicals - hydrogen radicals (H-center dot), rather than traditional (OH)-O-center dot. The energy barrier of cyanuric acid reacting with H-center dot to form the -NH2 group and break the sym-triazine ring is only 4.96 kcal mol(-1), which is clearly lower than that of cyanuric acid reacting with (OH)-O-center dot (13.32 kcal mol(-1)). Our theoretical predictions are further confirmed by gamma photon irradiation experiments, which show that when H-center dot is present in the reaction, the nitrogen in cyanuric acid (or other nitrogenous compounds including primidone and bezafibrate) rapidly degrades into NH4+. In contrast, when H-center dot is scavenged, cyanuric acid stops degrading into NH4+. Our results provide new insight for understanding the decomposition of nitrogenous materials, and we are the first to shed light on the key role of H-center dot in organic transformation processes. |
| 语种 | 英语 |
| WOS记录号 | WOS:000399164400003 |
| 源URL | [http://ir.sinap.ac.cn/handle/331007/27377]  |
| 专题 | 上海应用物理研究所_中科院上海应用物理研究所2011-2017年 |
| 推荐引用方式 GB/T 7714 | Lyu, GX,Shi, GS,Tang, L,et al. Mechanism of degradation of a nitrogenous heterocycle induced by a reductive radical: decomposition of a sym-triazine ring[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2017,19(14):9354-9357. |
| APA | Lyu, GX,Shi, GS,Tang, L,Fang, HP,&Wu, MH.(2017).Mechanism of degradation of a nitrogenous heterocycle induced by a reductive radical: decomposition of a sym-triazine ring.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,19(14),9354-9357. |
| MLA | Lyu, GX,et al."Mechanism of degradation of a nitrogenous heterocycle induced by a reductive radical: decomposition of a sym-triazine ring".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 19.14(2017):9354-9357. |
入库方式： OAI收割
来源：上海应用物理研究所
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