DICP OpenIR
Carbon induced selective regulation of cobalt-based Fischer-Tropsch catalysts by ethylene treatment
Zhai, Peng1; Chen, Pei-Pei2,3; Xie, Jinglin1; Liu, Jin-Xun2; Zhao, Huabo1; Lin, Lili1; Zhao, Bo1; Su, Hai-Yan2; Zhu, Qingjun4; Li, Wei-Xue2,3; Ma, Ding1
Source PublicationFARADAY DISCUSSIONS
2017-04-01
DOI10.1039/c6fd00194g
Volume197Pages:207-224
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordDENSITY-FUNCTIONAL THEORY ; PARTICLE-SIZE ; REALISTIC CONDITIONS ; FCC-CO(111) SURFACE ; NANOPARTICLES ; GRAPHENE ; DEACTIVATION ; DEPOSITION ; SYNGAS ; PHASE
AbstractVarious carbonaceous species were controllably deposited on Co/Al2O3 catalysts using ethylene as carbon source during the activation process for Fischer-Tropsch synthesis (FTS). Atomic, polymeric and graphitic carbon were distinguished by Raman spectroscopy, thermoanalysis and temperature programmed hydrogenation. Significant changes occurred in both the catalytic activity and selectivity toward hydrocarbon products after ethylene treatment. The activity decreased along with an increase in CH4 selectivity, at the expense of a remarkable decrease of heavy hydrocarbon production, resulting in enhanced selectivity for the gasoline fraction. In situ XPS experiments show the possible electron transfer from cobalt to carbon and the blockage of metallic cobalt sites, which is responsible for the deactivation of the catalyst. DFT calculations reveal that the activation barrier (Ea) of methane formation decreases by 0.61 eV on the carbon-absorbed Co(111) surface, whereas the Ea of the CH + CH coupling reaction changes unnoticeably. Hydrogenation of CHx to methane becomes the preferable route among the elementary reactions on the Co(111) surface, leading to dramatic changes in the product distribution. Detailed coke-induced deactivation mechanisms of Co-based catalysts during FTS are discussed.
Language英语
WOS IDWOS:000400580400009
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Cited Times:2[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/151972
Collection中国科学院大连化学物理研究所
Affiliation1.Peking Univ, Beijing Natl Lab Mol Sci, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
3.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, IChEM Collaborat Innovat Ctr Chem Energy Mat, Coll Chem & Mat Sci,CAS Ctr Excellence Nanosci, Hefei, Peoples R China
4.Future Sci & Technol City, Natl Inst Clean And Low Carbon Energy, Beijing 102209, Peoples R China
Recommended Citation
GB/T 7714
Zhai, Peng,Chen, Pei-Pei,Xie, Jinglin,et al. Carbon induced selective regulation of cobalt-based Fischer-Tropsch catalysts by ethylene treatment[J]. FARADAY DISCUSSIONS,2017,197:207-224.
APA Zhai, Peng.,Chen, Pei-Pei.,Xie, Jinglin.,Liu, Jin-Xun.,Zhao, Huabo.,...&Ma, Ding.(2017).Carbon induced selective regulation of cobalt-based Fischer-Tropsch catalysts by ethylene treatment.FARADAY DISCUSSIONS,197,207-224.
MLA Zhai, Peng,et al."Carbon induced selective regulation of cobalt-based Fischer-Tropsch catalysts by ethylene treatment".FARADAY DISCUSSIONS 197(2017):207-224.
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