Density Functional Theory Investigation of Possible Structures of Radicals in Coal Undergoing O-2 Chemisorption at Ambient Temperature
文献类型：期刊论文
| 作者 | Zhang, Zhiqiang1; Kang, Qiannan1; Yun, Tao1; Yan, Kefeng2,3
|
| 刊名 | ENERGY & FUELS
 |
| 出版日期 | 2017 |
| 卷号 | 31期号:1页码:953-958 |
| ISSN号 | 0887-0624 |
| DOI | 10.1021/acs.energyfuels.6b03072 |
| 文献子类 | Article |
| 英文摘要 | We have performed a theoretical study, using density functional theory at the B3LYP/6-311G(d, p) level, of the possible radical types and their structures in coal and their stabilities once they come into contact with atmospheric O-2 at ambient temperature. Eight possible radical types were proposed and explored through fully optimized electronic structure calculations. It was found that the radicals arising from dangling bonds on both the aromatic ring and the alkyl chain via covalent bond rupture are highly reactive toward oxidation, which resulted in the formation of stable oxygen-containing radicals. However, singlet occupied molecular orbital analysis suggested that the obtained radical via O-2 addition on the alkyl group should be attributed to the carbon-centered radical. The aryloxy C-O bond scission actually forms a carbon-centered radical. This type of radical and the radical that originated from odd-numbered carbon fused aromatic rings show high stabilities toward oxidation on account of the positive adsorption free energy change. In addition, the oxidation susceptibility of the radicals derived, from five and seven-membered rings, and nitrogen heteroatom defects in polyaromatic units of coal are also low at 298 K. Unlike the above radicals that could yield a superoxide group through O-2 addition, hydrogen abstraction from a semiquinone radical should be the preferred pathway, which forms a stable quinone group: Meanwhile, small mobile OOH is formed, which may initiate, the chain radical oxidation reaction in low rank coal. |
| WOS关键词 | STABLE CARBON RADICALS ; PYROLYSIS ; OXIDATION ; RANK |
| 语种 | 英语 |
| WOS记录号 | WOS:000392553800098 |
| 出版者 | AMER CHEMICAL SOC |
| 资助机构 | National Science Foundation of China(51404162) ; Science and Technology Innovation Program of Higher Education Institutions Shanxi Province |
| 源URL | [http://ir.giec.ac.cn/handle/344007/14027]  |
| 专题 | 中国科学院广州能源研究所 |
| 通讯作者 | Zhang, Zhiqiang |
| 作者单位 | 1.Taiyuan Univ Technol, Coll Min Engn, Taiyuan 030024, Peoples R China 2.Chinese Acad Sci, Guangzhou Inst Energy Convers, Key Lab Renewable Energy & Gas Hydrate, Guangzhou 510640, Guangdong, Peoples R China 3.Chinese Acad Sci, Guangzhou Ctr Gas Hydrate Res, Guangzhou 510640, Guangdong, Peoples R China |
| 推荐引用方式 GB/T 7714 | Zhang, Zhiqiang,Kang, Qiannan,Yun, Tao,et al. Density Functional Theory Investigation of Possible Structures of Radicals in Coal Undergoing O-2 Chemisorption at Ambient Temperature[J]. ENERGY & FUELS,2017,31(1):953-958. |
| APA | Zhang, Zhiqiang,Kang, Qiannan,Yun, Tao,&Yan, Kefeng.(2017).Density Functional Theory Investigation of Possible Structures of Radicals in Coal Undergoing O-2 Chemisorption at Ambient Temperature.ENERGY & FUELS,31(1),953-958. |
| MLA | Zhang, Zhiqiang,et al."Density Functional Theory Investigation of Possible Structures of Radicals in Coal Undergoing O-2 Chemisorption at Ambient Temperature".ENERGY & FUELS 31.1(2017):953-958. |
入库方式： OAI收割
来源：广州能源研究所
浏览0
下载0
收藏0
其他版本
除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。