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Mechanistic insights into complete hydrogenation of 1,3-butadiene over Pt/SiO2: effect of Pt dispersion and kinetic analysis
Hu, Chaoquan; Sun, Jiahan; Kang, Dongjuan; Zhu, Qingshan; Yang, Yafeng
2017-07-07
发表期刊CATALYSIS SCIENCE & TECHNOLOGY
ISSN2044-4753
卷号7期号:13页码:2717-2728
摘要Gas-phase hydrogenation of 1,3-butadiene was investigated over Pt/SiO2 catalysts with the aim of understanding the complete hydrogenation of dienes. The measurements focused on the effect of Pt dispersion on the product distribution and the kinetics of n-butane formation. Under the investigated conditions with an excess of hydrogen, the selectivity to n-butane sharply decreased from 41.6% to less than 3% at a 1,3-butadiene conversion of similar to 10% when the average Pt particle size increased from 3.9 to 22 nm. Correspondingly, the apparent activation energy for n-butane formation was measured to increase by about 2.7 times. In situ diffuse reflectance infrared Fourier transform (DRIFT) observations via alternating 1,3-butadiene and hydrogen feeds over the catalysts demonstrated that 1-butene was the major reaction intermediate in the process of 1,3-butadiene hydrogenation. By analysis of the kinetic data using the Horiuti-Polanyi mechanism with 1-butene as the intermediate, different reactivities of hydrogen on the catalysts towards C=C bond hydrogenation were proposed to understand the variation of the selectivity to n-butane with Pt dispersion. This viewpoint was further supported by DFT calculation of 1-butene hydrogenation with hydrogen at different sites on the Pt(111) surface.
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
DOI10.1039/c7cy00534b
收录类别SCI
语种英语
关键词[WOS]SELECTIVE HYDROGENATION ; VIBRATIONAL SPECTROSCOPY ; ATMOSPHERIC-PRESSURE ; CATALYTIC-PROPERTIES ; SINGLE-CRYSTALS ; PT(111) ; BUTADIENE ; PLATINUM ; SURFACES ; PALLADIUM
WOS研究方向Chemistry
WOS类目Chemistry, Physical
项目资助者National Natural Science Foundation of China(21606236) ; Center for Mesoscience ; Institute of Process Engineering (IPE) ; Chinese Academy of Sciences (CAS)(COM2016A001)
WOS记录号WOS:000404887400006
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被引频次:3[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/22807
专题多相复杂系统国家重点实验室
作者单位Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China
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Hu, Chaoquan,Sun, Jiahan,Kang, Dongjuan,et al. Mechanistic insights into complete hydrogenation of 1,3-butadiene over Pt/SiO2: effect of Pt dispersion and kinetic analysis[J]. CATALYSIS SCIENCE & TECHNOLOGY,2017,7(13):2717-2728.
APA Hu, Chaoquan,Sun, Jiahan,Kang, Dongjuan,Zhu, Qingshan,&Yang, Yafeng.(2017).Mechanistic insights into complete hydrogenation of 1,3-butadiene over Pt/SiO2: effect of Pt dispersion and kinetic analysis.CATALYSIS SCIENCE & TECHNOLOGY,7(13),2717-2728.
MLA Hu, Chaoquan,et al."Mechanistic insights into complete hydrogenation of 1,3-butadiene over Pt/SiO2: effect of Pt dispersion and kinetic analysis".CATALYSIS SCIENCE & TECHNOLOGY 7.13(2017):2717-2728.
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