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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
刊名FARADAY DISCUSSIONS
2017-04-01
DOI10.1039/c6fd00194g
197页:207-224
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
类目[WOS]Chemistry, Physical
研究领域[WOS]Chemistry
关键词[WOS]DENSITY-FUNCTIONAL THEORY ; PARTICLE-SIZE ; REALISTIC CONDITIONS ; FCC-CO(111) SURFACE ; NANOPARTICLES ; GRAPHENE ; DEACTIVATION ; DEPOSITION ; SYNGAS ; PHASE
英文摘要Various 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.
语种英语
WOS记录号WOS:000400580400009
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文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/151972
专题中国科学院大连化学物理研究所
作者单位1.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
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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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