Preliminary understanding of initial reaction process for subbituminous coal pyrolysis with molecular dynamics simulation
文献类型：期刊论文
| 作者 | Zhan, Jin-Hui; Wu, Rongcheng; Liu, Xiaoxing; Gao, Shiqiu; Xu, Guangwen |
| 刊名 | FUEL
 |
| 出版日期 | 2014-10-15 |
| 卷号 | 134期号:OCT.页码:283-292 |
| 关键词 | Subbituminous coal Pyrolysis Reactive molecular dynamics Reaction mechanism |
| ISSN号 | 0016-2361 |
| 其他题名 | Fuel |
| 中文摘要 | A series of molecular dynamics simulations using the ReaxFF reactive force field was carried out to investigate the mechanism of initial thermal decomposition associated with pyrolysis of a kind of subbituminous coal. The calculation results show that the primary decomposition reactions of Hatcher subbituminous model begin with intramolecular changes such as the cleavage of unstable C-C and C-O bonds. The formation mechanisms for typical pyrolysis products were explored. For example, the initial pathway for the formation of CO is by the decarbonylation of carbonyl or carboxyl group, while CO2 is mainly produced by hydrogen transfer and decarboxylation of carboxyl groups. CH4 can be formed mainly by CH3 center dot free radical abstracting a hydrogen atom from the hydroxyl group. H-2 is formed by two hydrogen atoms from one or two groups bonding together, which makes the residue fragments more stable. Hydrogen can also react with oxygen-containing free radicals or unsaturated bonds. Combining ReaxFF molecular dynamics (RMD) simulation and density functional theory (DFT) calculation, we find that the free radical C9H9O center dot is an important fragment during the pyrolysis process of Hatcher subbituminous model. As a precursor for cresol, it can capture hydrogen radical to form intermediate C9H10O and may continue to produce o-cresol and ethylene in the presence of hydrogen resource. These simulation results for the initial pyrolysis process and the reaction mechanisms agree with previous experimental observations. (C) 2014 Elsevier Ltd. All rights reserved. |
| 英文摘要 | A series of molecular dynamics simulations using the ReaxFF reactive force field was carried out to investigate the mechanism of initial thermal decomposition associated with pyrolysis of a kind of subbituminous coal. The calculation results show that the primary decomposition reactions of Hatcher subbituminous model begin with intramolecular changes such as the cleavage of unstable C-C and C-O bonds. The formation mechanisms for typical pyrolysis products were explored. For example, the initial pathway for the formation of CO is by the decarbonylation of carbonyl or carboxyl group, while CO2 is mainly produced by hydrogen transfer and decarboxylation of carboxyl groups. CH4 can be formed mainly by CH3 center dot free radical abstracting a hydrogen atom from the hydroxyl group. H-2 is formed by two hydrogen atoms from one or two groups bonding together, which makes the residue fragments more stable. Hydrogen can also react with oxygen-containing free radicals or unsaturated bonds. Combining ReaxFF molecular dynamics (RMD) simulation and density functional theory (DFT) calculation, we find that the free radical C9H9O center dot is an important fragment during the pyrolysis process of Hatcher subbituminous model. As a precursor for cresol, it can capture hydrogen radical to form intermediate C9H10O and may continue to produce o-cresol and ethylene in the presence of hydrogen resource. These simulation results for the initial pyrolysis process and the reaction mechanisms agree with previous experimental observations. (C) 2014 Elsevier Ltd. All rights reserved. |
| WOS标题词 | Science & Technology ; Technology |
| 类目[WOS] | Energy & Fuels ; Engineering, Chemical |
| 研究领域[WOS] | Energy & Fuels ; Engineering |
| 关键词[WOS] | LOW-RANK COAL ; FORCE-FIELD ; STRUCTURE SPECTROSCOPY ; CARBONACEOUS MATERIALS ; CHEMICAL-STRUCTURE ; BROWN-COAL ; REAXFF ; MODEL ; COMBUSTION ; DEVOLATILIZATION |
| 收录类别 | SCI |
| 原文出处 | |
| 语种 | 英语 |
| WOS记录号 | WOS:000340304100034 |
| 公开日期 | 2014-09-30 |
| 版本 | 出版稿 |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/11600]  |
| 专题 | 过程工程研究所_研究所（批量导入） |
| 作者单位 | Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China |
| 推荐引用方式 GB/T 7714 | Zhan, Jin-Hui,Wu, Rongcheng,Liu, Xiaoxing,et al. Preliminary understanding of initial reaction process for subbituminous coal pyrolysis with molecular dynamics simulation[J]. FUEL,2014,134(OCT.):283-292. |
| APA | Zhan, Jin-Hui,Wu, Rongcheng,Liu, Xiaoxing,Gao, Shiqiu,&Xu, Guangwen.(2014).Preliminary understanding of initial reaction process for subbituminous coal pyrolysis with molecular dynamics simulation.FUEL,134(OCT.),283-292. |
| MLA | Zhan, Jin-Hui,et al."Preliminary understanding of initial reaction process for subbituminous coal pyrolysis with molecular dynamics simulation".FUEL 134.OCT.(2014):283-292. |
入库方式： OAI收割
来源：过程工程研究所
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