Theoretical study of the formation mechanism of sulfur-containing gases in the co2 gasification of lignite
文献类型：期刊论文
| 作者 | Chen, Shi-Yun1; Ding, Jun-Xia2; Li, Guang-Yue1; Wang, Jie-Ping1; Tian, Yan1; Liang, Ying-Hua1 |
| 刊名 | Fuel
 |
| 出版日期 | 2019-04-15 |
| 卷号 | 242页码:398-407 |
| ISSN号 | 0016-2361 |
| 关键词 | Gasification Lignite Mechanism Sulfur Reaxff |
| DOI | 10.1016/j.fuel.2019.01.010 |
| 通讯作者 | Li, guang-yue(gyli@ncst.edu.cn) ; Liang, ying-hua(liangyh@ncst.edu.cn) |
| 英文摘要 | In this work, molecular dynamics based on a reactive force field (reaxff) and density functional theory (dft) are used to investigate the formation mechanisms of h2s, cos and so2 in the co2 gasification process of lignite, which is very difficult to be obtained by recent experimental method. the molecular representation of lignite, provided by wolfrum, is selected as the structural unit to construct the lignite model and the lignite-o-2 model. reaxff simulations of the two models are then performed for 1 ns at 3000 k. the evolution of h2s, cos and so2 shows a good agreement with the reported formation tendency in the coal pyrolysis process. by analyzing reaxff simulation trajectories using c + + programs, it is inferred that the thermal decomposition of sulfur containing moieties is initiated mainly by cleavage of their carbon sulfur bonds, leading to the same alkylthio intermediates. reaction energies from dft calculation indicate that co2 molecules, as well as alkoxy and aldehyde radicals produced by the reactions between co2 and the carbon structures in lignite, can weaken the carbon-sulfur bonds by stabilizing the cleavage products. the formation reactions of hs, r-s-co2 and r-s-o radicals are respectively key steps in the formation of h2s, cos and so2, which can both be accelerated by co2. the obtained mechanism can successfully explain the reported experimental phenomena and helps to understand the formation processes of sulfur-containing gas during the co2 gasification of lignite. |
| WOS关键词 | GAUSSIAN-BASIS SETS ; MOLECULAR-DYNAMICS ; COAL PYROLYSIS ; OXIDATION PROCESS ; FORCE-FIELD ; BROWN-COAL ; ATOMS LI ; REAXFF ; DESULFURIZATION ; TRANSFORMATION |
| WOS研究方向 | Energy & Fuels ; Engineering |
| WOS类目 | Energy & Fuels ; Engineering, Chemical |
| 语种 | 英语 |
| 出版者 | ELSEVIER SCI LTD |
| WOS记录号 | WOS:000459430100043 |
| URI标识 | http://www.irgrid.ac.cn/handle/1471x/2372761 |
| 专题 | 大连化学物理研究所 |
| 通讯作者 | Li, Guang-Yue; Liang, Ying-Hua |
| 作者单位 | 1.North China Univ Sci & Technol, Coll Chem Engn, Tangshan 063021, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China |
| 推荐引用方式 GB/T 7714 | Chen, Shi-Yun,Ding, Jun-Xia,Li, Guang-Yue,et al. Theoretical study of the formation mechanism of sulfur-containing gases in the co2 gasification of lignite[J]. Fuel,2019,242:398-407. |
| APA | Chen, Shi-Yun,Ding, Jun-Xia,Li, Guang-Yue,Wang, Jie-Ping,Tian, Yan,&Liang, Ying-Hua.(2019).Theoretical study of the formation mechanism of sulfur-containing gases in the co2 gasification of lignite.Fuel,242,398-407. |
| MLA | Chen, Shi-Yun,et al."Theoretical study of the formation mechanism of sulfur-containing gases in the co2 gasification of lignite".Fuel 242(2019):398-407. |
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来源：大连化学物理研究所
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