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Reaction pathway for partial hydrogenation of 1,3-butadiene over Pt/SiO2
Hu, Chaoquan1; Sun, Jiahan1; Yang, Yafeng1; Zhu, Qingshan1; Yu, Bin2
2017-12-21
发表期刊CATALYSIS SCIENCE & TECHNOLOGY
ISSN2044-4753
卷号7期号:4页码:5932-5943
摘要

The reaction pathway for partial hydrogenation of 1,3-butadiene over a Pt/SiO2 catalyst was explored with a combination of in situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy, intrinsic kinetics, and density functional theory (DFT) calculations. Under the present experimental conditions, the catalyst displayed a nearly constant product composition with similar to 97% selectivity to butenes. In situ DRIFT characterization revealed that the 1-buten-3-yl radical (1B3R), generated from the addition of one hydrogen atom to a terminal carbon of 1,3-butadiene, was the dominant intermediate in the partial hydrogenation of 1,3-butadiene. Kinetic analysis showed that the hydrogenation of 1B3R was the rate-determining step in the formation of butenes. Based on the above experimental results, DFT calculations were employed to investigate the reaction pathway with 1B3R as the intermediate on a Pt(111) surface. Interestingly, it was found that 1B3R can be easily formed from the hydrogenation of 1,3-butadiene with a di-s configuration rather than the most stable tetra-s structure on the Pt(111) surface. This hydrogenation step occurs between the non-coordinated terminal carbon and a hydrogen atom on a top site with an energy barrier of 23.2 kJ mol(-1). The second hydrogenation step from 1B3R to butenes requires relatively higher activation barriers to proceed, being consistent with the experimental kinetics. Finally, the selectivity order for butenes and the structure sensitivity of Pt-catalyzed partial hydrogenation of 1,3-butadiene were discussed.

文章类型Article
WOS标题词Science & Technology ; Physical Sciences
DOI10.1039/c7cy01882g
收录类别SCI
语种英语
关键词[WOS]Selective Hydrogenation ; Vibrational Spectroscopy ; Infrared-spectroscopy ; Catalysts ; Pt(111) ; Surfaces ; Butadiene ; Dft ; Adsorption ; Chemistry
WOS研究方向Chemistry
WOS类目Chemistry, Physical
项目资助者National Natural Science Foundation of China (NFSC)(21606236) ; Center for Mesoscience, Institute of Process Engineering (IPE), Chinese Academy of Sciences (CAS)(COM2016A001)
WOS记录号WOS:000417712800014
引用统计
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/23477
专题研究所(批量导入)
通讯作者Hu, Chaoquan; Zhu, Qingshan
作者单位1.Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China
2.Shandong CISRI CHALCO Rare Earth Technol Co Ltd, Jining 277600, Shandong, Peoples R China
推荐引用方式
GB/T 7714
Hu, Chaoquan,Sun, Jiahan,Yang, Yafeng,et al. Reaction pathway for partial hydrogenation of 1,3-butadiene over Pt/SiO2[J]. CATALYSIS SCIENCE & TECHNOLOGY,2017,7(4):5932-5943.
APA Hu, Chaoquan,Sun, Jiahan,Yang, Yafeng,Zhu, Qingshan,&Yu, Bin.(2017).Reaction pathway for partial hydrogenation of 1,3-butadiene over Pt/SiO2.CATALYSIS SCIENCE & TECHNOLOGY,7(4),5932-5943.
MLA Hu, Chaoquan,et al."Reaction pathway for partial hydrogenation of 1,3-butadiene over Pt/SiO2".CATALYSIS SCIENCE & TECHNOLOGY 7.4(2017):5932-5943.
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