Dehydrogenation of n-dodecane over Pt-Sn/Mg-Al-O catalysts: Investigating the catalyst performance while monitoring the products

被引:27
作者
Lai, Yulong [1 ,2 ]
He, Songbo [1 ]
Li, Xianru [1 ,2 ]
Sun, Chenglin [1 ]
Seshan, K. [3 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Liaoning, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Univ Twente, MESA Inst Nanotechnol, NL-7500 AE Enschede, Netherlands
关键词
Dehydrogenation; Long chain paraffin; Pt-Sn; Mg-Al-O oxide; In situ; TOF-MS; MAL2O4; M-MG; ISOBUTANE DEHYDROGENATION; BUTANE DEHYDROGENATION; PT-SN/AL2O3; CATALYSTS; METAL PRECURSORS; REGENERATION; PARAFFINS; SELECTIVITY; SUPPORT; LITHIUM;
D O I
10.1016/j.apcata.2013.09.042
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
n-Dodecane was dehydrogenated over Pt-Sn/Mg-Al-O catalysts. Al2O3 and Mg Al-O supports with different Mg/AI mole ratio were prepared using a chemical co-precipitation method. The supports and supported Pt Sn catalysts were characterized using BET, XRD, CO-chemisorption, NH3-TPD, and TG. The dehydrogenation products were analyzed by GC. A single photon ionization time-of-flight mass spectrometer (SPI-TOF-MS) was developed and used to monitor the dehydrogenation products on-line during continuous reactions. Adding Mg to the supports decreased the specific surface area, increased the pore volume and diameter, moderated the acidity, and changed the strong acidic sites to weak ones. The dehydrogenation activity of the catalysts was inhibited, while the mono-olefin selectivity and yield were enhanced by Mg addition. Using a 1/3 Mg/A1 molar ratio generated the optimal n-dodecene yield over the Pt Sn/Mg Al-O catalysts. The TOF-MS was reliable for detecting the dehydrogenation products of the long-chain paraffins rapidly, continuously, and accurately. Interestingly, TOF-MS can be used to monitor the reactions on-line and in situ, providing analyses of the products during high temperature reactions. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:74 / 80
页数:7
相关论文
共 33 条
[1]   IMPORTANCE OF PRETREATMENT ON REGENERATION OF A PT-SN/AL2O3 CATALYST [J].
AFONSO, JC ;
ARANDA, DAG ;
SCHMAL, M ;
FRETY, R .
FUEL PROCESSING TECHNOLOGY, 1995, 42 (01) :3-17
[2]   Effect of Magnesium Addition to PtSnNa/ZSM-5 on the Catalytic Properties in the Dehydrogenation of Propane [J].
Bai, Linyang ;
Zhou, Yuming ;
Zhang, Yiwei ;
Liu, Hui ;
Sheng, Xiaoli .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2009, 48 (22) :9885-9891
[3]  
Barbier J., 1987, CATALYST DEACTIVATIO, P1
[4]   Dehydrogenation and oxydehydrogenation of paraffins to olefins [J].
Bhasin, MM ;
McCain, JH ;
Vora, BV ;
Imai, T ;
Pujadó, PR .
APPLIED CATALYSIS A-GENERAL, 2001, 221 (1-2) :397-419
[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]   Performance of PtSn catalysts supported on MAl2O4 (M: Mg or Zn) in n-butane dehydrogenation:: characterization of the metallic phase [J].
Bocanegra, SA ;
Guerrero-Ruiz, A ;
de Miguel, SR ;
Scelza, OA .
APPLIED CATALYSIS A-GENERAL, 2004, 277 (1-2) :11-22
[7]   n-butane dehydrogenation on PtSn supported on MAl2O4 (M: Mg or Zn) catalysts [J].
Bocanegra, SA ;
de Miguel, SR ;
Castro, AA ;
Scelza, OA .
CATALYSIS LETTERS, 2004, 96 (3-4) :129-140
[8]   The influence of the synthesis routes of MgAl2O4 on its properties and behavior as support of dehydrogenation catalysts [J].
Bocanegra, Sonia A. ;
Ballarini, Adriana D. ;
Scelza, Osvaldo A. ;
de Miguel, Sergio R. .
MATERIALS CHEMISTRY AND PHYSICS, 2008, 111 (2-3) :534-541
[9]  
Broekhoff J.C.P., 1970, STUDIES PORE SYSTEMS
[10]   Trimetallic naphtha reforming catalysts.: I.: Properties of the metal function and influence of the order of addition of the metal precursors on Pt-Re-Sn/γ-Al2O3-Cl [J].
Carvalho, LS ;
Pieck, CL ;
Rangel, MC ;
Fígoli, NS ;
Grau, JM ;
Reyes, P ;
Parera, JM .
APPLIED CATALYSIS A-GENERAL, 2004, 269 (1-2) :91-103