Kinetics of propane dehydrogenation over Pt-Sn/Al2O3

被引:45
作者
Gomez-Quero, Santiago [1 ]
Tsoufis, Theodoros [2 ]
Rudolf, Petra [2 ]
Makkee, Michiel [3 ]
Kapteijn, Freek [3 ]
Rothenberg, Gadi [1 ]
机构
[1] Univ Amsterdam, Vant Hoff Inst Mol Sci, NL-1090 GD Amsterdam, Netherlands
[2] Univ Groningen, Zernike Inst Adv Mat, NL-9747 AG Groningen, Netherlands
[3] Delft Univ Technol, Dept Chem Engn, NL-2628 BL Delft, Netherlands
关键词
RAY PHOTOELECTRON-SPECTROSCOPY; SUPPORTED PLATINUM CATALYSTS; PT/AL2O3; CATALYSTS; PTSN CATALYST; SN; ALUMINA; HYDROGEN; PROPENE; TIN; PERFORMANCE;
D O I
10.1039/c2cy20488f
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 kinetics of the gas-phase dehydrogenation of propane over Pt-Sn (1 : 1 mol ratio) supported on Al2O3 was investigated for the first time over the high range of reactant/products partial pressures (up to 0.875 atm). The Pt precursor was reduced to metallic form after a temperature-programmed reduction (TPR) at 873 K. X-ray photoelectron spectroscopy (XPS) analysis suggests that a Pt-Sn surface alloy forms, decreasing the H-2 adsorption on the Pt-Sn sites (5.6 nm in average size) relative to monometallic Pt (6.8 nm). We performed kinetic studies in the absence of mass/heat transfer limitations. The incorporation of Sn into Pt in Pt-Sn/Al2O3 enhanced the catalytic activity and stability when compared to Pt/Al2O3. We attribute this response to the surface electronic interaction between Pt and Sn. The initial propane consumption rate increases with the partial pressure of propane and decreases with the partial pressure of propene, while varying that of hydrogen has a negligible effect. Applying the Langmuir-Hinshelwood-Hougen-Watson (LHHW) approach, the most likely kinetic model is non-dissociative adsorption of propane with simultaneous release of H-2, where surface reaction is the rate-limiting step. Our results of the kinetic aspects provide practical insights relevant to propane dehydrogenation.
引用
收藏
页码:962 / 971
页数:10
相关论文
共 86 条
[1]   In situ characterisation of carbon-containing species formed on chromia/alumina during propane dehydrogenation [J].
Airaksinen, SMK ;
Bañares, MA ;
Krause, AOI .
JOURNAL OF CATALYSIS, 2005, 230 (02) :507-513
[2]   A novel, highly efficient catalyst for propane dehydrogenation [J].
Akporiaye, D ;
Jensen, SF ;
Olsbye, U ;
Rohr, F ;
Rytter, E ;
Ronnekleiv, M ;
Spjelkavik, AI .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2001, 40 (22) :4741-4748
[3]  
[Anonymous], 2008, SEARCH PUBMED
[4]   Kinetics for dehydrogenation of propane on Pt-Sn-K/γ-Al2O3 catalyst [J].
Assabumrungrat, S ;
Jhoraleecharnchai, W ;
Praserthdam, P ;
Goto, S .
JOURNAL OF CHEMICAL ENGINEERING OF JAPAN, 2000, 33 (03) :529-532
[5]   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
[6]   n-Butane dehydrogenation on Pt, PtSn and PtGe supported on γ-Al2O3 deposited on spheres of α-Al2O3 by washcoating [J].
Ballarini, Adriana D. ;
Zgolicz, Patricia ;
Vilella, Irene M. J. ;
de Miguel, Sergio R. ;
Castro, Alberto A. ;
Scelza, Osvaldo A. .
APPLIED CATALYSIS A-GENERAL, 2010, 381 (1-2) :83-91
[7]   PROPANE DEHYDROGENATION OVER SUPPORTED PLATINUM CATALYSTS - EFFECT OF TIN AS A PROMOTER [J].
BARIAS, OA ;
HOLMEN, A ;
BLEKKAN, EA .
CATALYSIS TODAY, 1995, 24 (03) :361-364
[8]   Propane dehydrogenation over supported Pt and Pt-Sn catalysts: Catalyst preparation, characterization, and activity measurements [J].
Barias, OA ;
Holmen, A ;
Blekkan, EA .
JOURNAL OF CATALYSIS, 1996, 158 (01) :1-12
[9]  
BARIAS OA, 1994, STUD SURF SCI CATAL, V88, P519
[10]   Genesis of the active-component precursor in the synthesis of Pt/Al2O3 catalysts:: I.: Transformation of the [PtCl6]2- complex in the interaction between chloroplatinic acid and the γ-Al2O3 surface [J].
Bel'skaya, O. B. ;
Karymova, R. Kh. ;
Kochubey, D. I. ;
Duplyakin, V. K. .
KINETICS AND CATALYSIS, 2008, 49 (05) :720-728