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
[21]   Alumina- and alumina-zirconia-supported PtSn bimetallics:: Microstructure and performance for the n-butane ODH reaction [J].
Larese, C ;
Campos-Martin, JM ;
Calvino, JJ ;
Blanco, G ;
Fierro, JLG ;
Kang, ZC .
JOURNAL OF CATALYSIS, 2002, 208 (02) :467-478
[22]   The effect of reaction conditions and time on stream on the coke formed during propane dehydrogenation [J].
Larsson, M ;
Hulten, M ;
Blekkan, EA ;
Andersson, B .
JOURNAL OF CATALYSIS, 1996, 164 (01) :44-53
[23]   Surface and structure modification of carbon nanofibers [J].
Lee, Sungho ;
Kim, Tack-Rae ;
Ogale, Amod A. ;
Kim, Myung-Soo .
SYNTHETIC METALS, 2007, 157 (16-17) :644-650
[24]   Coke Formation on Pt-Sn/Al2O3 Catalyst in Propane Dehydrogenation: Coke Characterization and Kinetic Study [J].
Li, Qing ;
Sui, Zhijun ;
Zhou, Xinggui ;
Zhu, Yian ;
Zhou, Jinghong ;
Chen, De .
TOPICS IN CATALYSIS, 2011, 54 (13-15) :888-896
[25]   Kinetics of propane dehydrogenation over Pt-Sn/Al2O3 catalyst [J].
Li, Qing ;
Sui, Zhijun ;
Zhou, Xinggui ;
Chen, De .
APPLIED CATALYSIS A-GENERAL, 2011, 398 (1-2) :18-26
[26]   Raman spectroscopy in graphene [J].
Malard, L. M. ;
Pimenta, M. A. ;
Dresselhaus, G. ;
Dresselhaus, M. S. .
PHYSICS REPORTS-REVIEW SECTION OF PHYSICS LETTERS, 2009, 473 (5-6) :51-87
[27]   Active coke: Carbonaceous materials as catalysts for alkane dehydrogenation [J].
McGregor, James ;
Huang, Zhenyu ;
Parrott, Edward P. J. ;
Zeitler, J. Axel ;
Nguyen, K. Lien ;
Rawson, Jeremy M. ;
Carley, Albert ;
Hansen, Thomas W. ;
Tessonnier, Jean-Philippe ;
Su, Dang Sheng ;
Teschner, Detre ;
Vass, Elaine M. ;
Knop-Gericke, Axel ;
Schloegl, R. ;
Gladden, Lynn F. .
JOURNAL OF CATALYSIS, 2010, 269 (02) :329-339
[28]   Density Functional Theory Study on Propane and Propene Adsorption on Pt(111) and PtSn Alloy Surfaces [J].
Nykanen, L. ;
Honkala, K. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (19) :9578-9586
[29]   Studying disorder in graphite-based systems by Raman spectroscopy [J].
Pimenta, M. A. ;
Dresselhaus, G. ;
Dresselhaus, M. S. ;
Cancado, L. G. ;
Jorio, A. ;
Saito, R. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2007, 9 (11) :1276-1291
[30]  
Praserthdam P, 1997, STUD SURF SCI CATAL, V111, P153