Density Functional Theory Investigation of Possible Structures of Radicals in Coal Undergoing O-2 Chemisorption at Ambient Temperature

doi:10.1021/acs.energyfuels.6b03072

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	Density Functional Theory Investigation of Possible Structures of Radicals in Coal Undergoing O-2 Chemisorption at Ambient Temperature
	Zhang, Zhiqiang 1; Kang, Qiannan 1; Yun, Tao 1; Yan, Kefeng2,3
	2017
发表期刊	ENERGY & FUELS
ISSN	0887-0624
卷号	31 期号:1 页码:953-958
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.
文章类型	Article
WOS标题词	Science & Technology ; Technology
DOI	10.1021/acs.energyfuels.6b03072
研究领域[WOS]	Energy & Fuels ; Engineering
关键词[WOS]	STABLE CARBON RADICALS ; PYROLYSIS ; OXIDATION ; RANK
收录类别	SCI
语种	英语
项目资助者	National Science Foundation of China(51404162) ; Science and Technology Innovation Program of Higher Education Institutions Shanxi Province
WOS类目	Energy & Fuels ; Engineering, Chemical
WOS记录号	WOS:000392553800098
出版者	AMER CHEMICAL SOC
引用统计	被引频次：20[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	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.