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
[1]   LATTICE-DYNAMICAL MODEL FOR GRAPHITE [J].
ALJISHI, R ;
DRESSELHAUS, G .
PHYSICAL REVIEW B, 1982, 26 (08) :4514-4522
[2]   Influence of Calcium Addition on Catalytic Properties of PtSn/ZSM-5 Catalyst for Propane Dehydrogenation [J].
Bai, Linyang ;
Zhou, Yuming ;
Zhang, Yiwei ;
Liu, Hui ;
Tang, Menghan .
CATALYSIS LETTERS, 2009, 129 (3-4) :449-456
[3]   Real-time control of a catalytic solid in a fixed-bed reactor based on in situ spectroscopy [J].
Bennici, Simona M. ;
Vogelaar, Bas M. ;
Nijhuis, T. Alexander ;
Weckhuysen, Bert M. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (28) :5412-5416
[4]   XANES, Raman and XRD study of anthracene-based cokes and saccharose-based chars submitted to high-temperature pyrolysis [J].
Bernard, S. ;
Beyssac, O. ;
Benzerara, K. ;
Findling, N. ;
Tzvetkov, G. ;
Brown, G. E., Jr. .
CARBON, 2010, 48 (09) :2506-2516
[5]   Highly selective and stable bimetallic catalysts supported on different materials for n-butane dehydrogenation [J].
Bocanegra, S. ;
Ballarini, A. ;
Zgolicz, P. ;
Scelza, O. ;
de Miguel, S. .
CATALYSIS TODAY, 2009, 143 (3-4) :334-340
[6]   Dehydrogenation of propane on chromia/alumina catalysts promoted by tin [J].
Cabrera, Franklin ;
Ardissone, Daniel ;
Gorriz, Osvaldo F. .
CATALYSIS TODAY, 2008, 133 (1-4) :800-804
[7]   Light cracked naphtha processing: Controlling chemistry for maximum propylene production [J].
Corma, A ;
Melo, FV ;
Sauvanaud, L ;
Ortega, F .
CATALYSIS TODAY, 2005, 107-08 :699-706
[8]   Raman spectroscopy on isolated single wall carbon nanotubes [J].
Dresselhaus, MS ;
Dresselhaus, G ;
Jorio, A ;
Souza, AG ;
Saito, R .
CARBON, 2002, 40 (12) :2043-2061
[9]   Effect of Sodium Addition to PtSn/AlSBA-15 on the Catalytic Properties in Propane Dehydrogenation [J].
Duan, Yongzheng ;
Zhou, Yuming ;
Zhang, Yiwei ;
Sheng, Xiaoli ;
Xue, Mengwei .
CATALYSIS LETTERS, 2011, 141 (01) :120-127
[10]   Hydrogen adsorption and diffusion on Pt {111} and PtSn {111} [J].
Fearon, Joanne ;
Watson, Graeme W. .
JOURNAL OF MATERIALS CHEMISTRY, 2006, 16 (20) :1989-1996