DICP OpenIR
Theoretical study of the formation mechanism of sulfur-containing gases in the CO2 gasification of lignite
Chen, Shi-Yun1; Ding, Jun-Xia2; Li, Guang-Yue1; Wang, Jie-Ping1; Tian, Yan1; Liang, Ying-Hua1
Corresponding AuthorLi, Guang-Yue(gyli@ncst.edu.cn) ; Liang, Ying-Hua(liangyh@ncst.edu.cn)
KeywordGasification Lignite Mechanism Sulfur ReaxFF
Source PublicationFUEL
2019-04-15
ISSN0016-2361
DOI10.1016/j.fuel.2019.01.010
Volume242Pages:398-407
Funding ProjectNational Natural Science Foundation of China[21506047] ; Key Fund Project of Hebei Province Department of Education[ZD2016068] ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS[SKLMRD-K201801]
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Fund Project of Hebei Province Department of Education ; Key Fund Project of Hebei Province Department of Education ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Fund Project of Hebei Province Department of Education ; Key Fund Project of Hebei Province Department of Education ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Fund Project of Hebei Province Department of Education ; Key Fund Project of Hebei Province Department of Education ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Fund Project of Hebei Province Department of Education ; Key Fund Project of Hebei Province Department of Education ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS
WOS SubjectEnergy & Fuels ; Engineering, Chemical
WOS Research AreaEnergy & Fuels ; Engineering
WOS KeywordGAUSSIAN-BASIS SETS ; MOLECULAR-DYNAMICS ; COAL PYROLYSIS ; OXIDATION PROCESS ; FORCE-FIELD ; BROWN-COAL ; ATOMS LI ; REAXFF ; DESULFURIZATION ; TRANSFORMATION
AbstractIn 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.
Language英语
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Fund Project of Hebei Province Department of Education ; Key Fund Project of Hebei Province Department of Education ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Fund Project of Hebei Province Department of Education ; Key Fund Project of Hebei Province Department of Education ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Fund Project of Hebei Province Department of Education ; Key Fund Project of Hebei Province Department of Education ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Fund Project of Hebei Province Department of Education ; Key Fund Project of Hebei Province Department of Education ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS ; Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP, CAS
WOS IDWOS:000459430100043
PublisherELSEVIER SCI LTD
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/165985
Collection中国科学院大连化学物理研究所
Corresponding AuthorLi, Guang-Yue; Liang, Ying-Hua
Affiliation1.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
Recommended Citation
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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