Operando Raman spectroscopy study on the deactivation of Pt/Al2O3 and Pt-Sn/Al2O3 propane dehydrogenation catalysts

被引:110
作者
Sattler, Jesper J. H. B. [1 ]
Beale, Andrew M. [1 ]
Weckhuysen, Bert M. [1 ]
机构
[1] Univ Utrecht, Debye Inst Nanomat Sci, Dept Chem, NL-3584 CG Utrecht, Netherlands
关键词
ETHANE DEHYDROGENATION; CARBONACEOUS MATERIALS; TIME; SN; ADSORPTION; PT-SBA-15; CHEMISTRY; GRAPHITE; DISORDER; SPECTRA;
D O I
10.1039/c3cp50646k
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The deactivation of 0.5 wt% Pt/Al2O3 and 0.5 wt% Pt-1.5 wt% Sn/Al2O3 catalysts has been studied by operando Raman spectroscopy during the dehydrogenation of propane and subsequent regeneration in air for 10 successive dehydrogenation-regeneration cycles. Furthermore, the reaction feed was altered by using different propane/propene/hydrogen ratios. It was found that the addition of hydrogen to the feed increases the catalyst performance and decreases the formation of coke deposits, as was revealed by thermogravimetrical analysis. The positive effect of hydrogen on the catalyst performance is comparable to the addition of Sn, a promoter element which increases both the propane conversion and propene selectivity. Operando Raman spectroscopy showed that hydrogen altered the nature of the coke deposits formed during propane dehydrogenation. Due to this approach it was possible to perform a systematic deconvolution procedure on the Raman spectra. By analysing the related intensity, band position and bandwidth of the different Raman features, it was determined that smaller graphite crystallites, which have less defects, are formed when the partial pressure of hydrogen in the feed was increased.
引用
收藏
页码:12095 / 12103
页数:9
相关论文
共 50 条
[41]   RAMAN SPECTRUM OF GRAPHITE [J].
TUINSTRA, F ;
KOENIG, JL .
JOURNAL OF CHEMICAL PHYSICS, 1970, 53 (03) :1126-&
[42]   The chemistry of ethane dehydrogenation over a supported platinum catalyst [J].
Vincent, R. S. ;
Lindstedt, R. P. ;
Malik, N. A. ;
Reid, I. A. B. ;
Messenger, B. E. .
JOURNAL OF CATALYSIS, 2008, 260 (01) :37-64
[43]   Kinetic and isotopic study of ethane dehydrogenation over a semicommercial Pt,Sn/Mg(Al)O catalyst [J].
Virnovskaia, Anastasia ;
Rytter, Erling ;
Olsbye, Unni .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2008, 47 (19) :7167-7177
[44]   Pt-Sn alloy phases and coke mobility over Pt-Sn/Al2O3 and Pt-Sn/ZnAl2O4 catalysts for propane dehydrogenation [J].
Vu, Bao Khanh ;
Song, Myoung Bok ;
Ahn, In Young ;
Suh, Young-Woong ;
Suh, Dong Jin ;
Kim, Won-Il ;
Koh, Hyoung-Lim ;
Choi, Young Gyo ;
Shin, Eun Woo .
APPLIED CATALYSIS A-GENERAL, 2011, 400 (1-2) :25-33
[45]   Influence of Oxygen Mobility over Supported Pt Catalysts on Combustion Temperature of Coke Generated in Propane Dehydrogenation [J].
Vu, Bao Khanh ;
Shin, Eun Woo .
CATALYSIS LETTERS, 2011, 141 (05) :699-704
[46]   RAMAN-SPECTROSCOPY OF CARBON MATERIALS - STRUCTURAL BASIS OF OBSERVED SPECTRA [J].
WANG, Y ;
ALSMEYER, DC ;
MCCREERY, RL .
CHEMISTRY OF MATERIALS, 1990, 2 (05) :557-563
[47]   Alkane dehydrogenation over supported chromium oxide catalysts [J].
Weckhuysen, BM ;
Schoonheydt, RA .
CATALYSIS TODAY, 1999, 51 (02) :223-232
[48]   Repetitive control and online optimization of Catofin propane process [J].
Won, Wangyun ;
Lee, Kwang Soon ;
Lee, Seokho ;
Jung, Chansul .
COMPUTERS & CHEMICAL ENGINEERING, 2010, 34 (04) :508-517
[49]   DFT study of propane dehydrogenation on Pt catalyst: effects of step sites [J].
Yang, Ming-Lei ;
Zhu, Yi-An ;
Fan, Chen ;
Sui, Zhi-Jun ;
Chen, De ;
Zhou, Xing-Gui .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (08) :3257-3267
[50]   Density functional study of the chemisorption of C1, C2 and C3 intermediates in propane dissociation on Pt(111) [J].
Yang, Ming-Lei ;
Zhu, Yi-An ;
Fan, Chen ;
Sui, Zhi-Jun ;
Chen, De ;
Zhou, Xing-Gui .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2010, 321 (1-2) :42-49