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
[11]   Surface characterization of Li-modified platinum/tin catalysts for isobutane dehydrogenation [J].
Casella, ML ;
Siri, GJ ;
Santori, GF ;
Ferretti, OA ;
Ramírez-Corredores, MM .
LANGMUIR, 2000, 16 (13) :5639-5643
[12]   Effect of lanthanum on the catalytic properties of PtSn/γ-Al2O3 bimetallic catalysts prepared by successive impregnation and controlled surface reaction [J].
Del Angel, G ;
Bonilla, A ;
Peña, Y ;
Navarrete, J ;
Fierro, JLG ;
Acosta, DR .
JOURNAL OF CATALYSIS, 2003, 219 (01) :63-73
[13]   Study of the citral/acetone reaction on MgyAlOx oxides:: Effect of the chemical composition on catalyst activity, selectivity and stability [J].
Diez, V. K. ;
Di Cosimo, J. I. ;
Apesteguia, C. R. .
APPLIED CATALYSIS A-GENERAL, 2008, 345 (02) :143-151
[14]  
Dunn R.O., 1992, P NPRA ANN M NEW ORL, P22
[15]   Lithium promoted Pt-Sn/Al2O3 catalysts for dehydrogenation of n-decane: Influence of lithium metal precursors [J].
Gokak, DT ;
Basrur, AG ;
Rajeswar, D ;
Rao, GS ;
Krishnamurthy, KR .
REACTION KINETICS AND CATALYSIS LETTERS, 1996, 59 (02) :315-323
[16]   Catalytic dehydrogenation (DH) of light paraffins combined with selective hydrogen combustion (SHC) -: I.: DH → SHC → DH catalysts in series (co-fed process mode) [J].
Grasselli, RK ;
Stern, DL ;
Tsikoyiannis, JG .
APPLIED CATALYSIS A-GENERAL, 1999, 189 (01) :1-8
[17]   Effect of carbon addition on the Pt-Sn/γ-Al2O3 catalyst for long chain paraffin dehydrogenation to olefin [J].
He, Songbo ;
Sun, Chenglin ;
Du, Hongzhang ;
Dai, Xihai ;
Wang, Bin .
CHEMICAL ENGINEERING JOURNAL, 2008, 141 (1-3) :284-289
[18]   Dehydrogenation of long chain paraffins over supported Pt-Sn-K/Al2O3 catalysts: A study of the alumina support effect [J].
He, Songbo ;
Sun, Chenglin ;
Bai, Ziwu ;
Dai, Xihai ;
Wang, Bin .
APPLIED CATALYSIS A-GENERAL, 2009, 356 (01) :88-98
[19]   Single Photon Ionization and Chemical Ionization Combined Ion Source Based on a Vacuum Ultraviolet Lamp for Orthogonal Acceleration Time-of-Flight Mass Spectrometry [J].
Hua, Lei ;
Wu, Qinghao ;
Hou, Keyong ;
Cui, Huapeng ;
Chen, Ping ;
Wang, Weiguo ;
Li, Jinghua ;
Li, Haiyang .
ANALYTICAL CHEMISTRY, 2011, 83 (13) :5309-5316
[20]   Propane dehydrogenation over the PtSn catalyst supported on alumina-modified SBA-15 [J].
Huang, Lihua ;
Xu, Bolian ;
Yang, Lili ;
Fan, Yining .
CATALYSIS COMMUNICATIONS, 2008, 9 (15) :2593-2597