Design, synthesis and catalytic performance of vanadium-incorporated mesoporous silica KIT-6 catalysts for the oxidative dehydrogenation of propane to propylene

被引:62
作者
Liu, Qinglong [1 ]
Li, Jianmei [1 ]
Zhao, Zhen [1 ,2 ]
Gao, Manglai [1 ]
Kong, Lian [1 ]
Liu, Jian [1 ]
Wei, Yuechang [1 ]
机构
[1] China Univ Petr, State Kev Lab Heavy Oil Proc, Beijing 102249, Peoples R China
[2] Shenyang Normal Univ, Inst Catalysis Energy & Environm, Shenyang 110034, Peoples R China
基金
中国国家自然科学基金;
关键词
METAL-OXIDE CATALYSTS; SELECTIVE OXIDATION; RAMAN-SPECTROSCOPY; BETA ZEOLITE; SBA-15; ETHANE; FORMALDEHYDE; METHANE; MCM-41; ETHYLENE;
D O I
10.1039/c6cy00404k
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
A series of vanadium-incorporated mesoporous materials V-KIT-6 with different vanadium contents were synthesized by combining a direct hydrothermal method with a pH adjusting method and applied as catalysts for the oxidative dehydrogenation of propane. The structures of the catalysts were characterized by various techniques including N-2 adsorption-desorption, XRD, TEM, SEM, UV-vis DRS, H-2-TPR and Raman spectroscopy. The results reveal that the pH value plays a key role in the structure of the catalysts and the incorporated content of vanadium in the synthesis process of V-KIT-6 materials. The frameworkincorporation of various contents of vanadium under mild acidic conditions (pH = 5) preserves the welldefined 3D interconnected mesoporous features of KIT-6 and promotes the dispersion of vanadium oxide species. The V-KIT-6 catalysts show much higher catalytic selectivity and productivity to propylene in the oxidative dehydrogenation of propane than the corresponding supported vanadium catalyst. The highest selectivity sum of C2H4 + C3H6 (70.2%) is obtained over the 5V-KIT-6 catalyst; meanwhile, a high space-time yield (STYC3H6) of 3.91 kg(propylene) kg(cat)(-1) h(-1) is obtained. The superior catalytic performance of the V-KIT- 6 catalysts in the oxidative dehydrogenation of propane can be ascribed to the high concentration of highly dispersed active sites as well as the favorable property of mass transfer and accessibility of the active sites to the reactant molecules in the 3D interconnected mesopores.
引用
收藏
页码:5927 / 5941
页数:15
相关论文
共 58 条
  • [1] Effect of Synthesis Conditions on the Structure and Catalytic Performance of V- and Ce-Incorporated SBA-15-like Materials in Propane Selective Oxidation
    Aktas, Ozge
    Yasyerli, Sena
    Dogu, Gulsen
    Dogu, Timur
    [J]. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2010, 49 (15) : 6790 - 6802
  • [2] How Strain Affects the Reactivity of Surface Metal Oxide Catalysts
    Amakawa, Kazuhiko
    Sun, Lili
    Guo, Chunsheng
    Haevecker, Michael
    Kube, Pierre
    Wachs, Israel E.
    Lwin, Soe
    Frenkel, Anatoly I.
    Patlolla, Anitha
    Hermann, Klaus
    Schloegl, Robert
    Trunschke, Annette
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (51) : 13553 - 13557
  • [3] Effect of catalyst structure on oxidative dehydrogenation of ethane and propane on alumina-supported vanadia
    Argyle, MD
    Chen, KD
    Bell, AT
    Iglesia, E
    [J]. JOURNAL OF CATALYSIS, 2002, 208 (01) : 139 - 149
  • [4] BASE CF, 1970, HYDROLYSIS CATION
  • [5] On the partial oxidation of propane and propylene on mixed metal oxide catalysts
    Bettahar, MM
    Costentin, G
    Savary, L
    Lavalley, JC
    [J]. APPLIED CATALYSIS A-GENERAL, 1996, 145 (1-2) : 1 - 48
  • [6] Study of vanadium based mesoporous silicas for oxidative dehydrogenation of propane and n-butane
    Bulanek, Roman
    Kaluzova, Alena
    Setnicka, Michal
    Zukal, Arnost
    Cicmanec, Pavel
    Mayerova, Jana
    [J]. CATALYSIS TODAY, 2012, 179 (01) : 149 - 158
  • [7] Molecular structure and activity of molybdena catalysts supported on zirconia for ethane oxidative dehydrogenation studied by operando Raman spectroscopy
    Christodoulakis, Antonios
    Boghosian, Soghomon
    [J]. JOURNAL OF CATALYSIS, 2008, 260 (01) : 178 - 187
  • [8] Synthesis and characterization of V-SBA-1 cubic mesoporous molecular sieves
    Dai, LX
    Tabata, K
    Suzuki, E
    Tatsumi, T
    [J]. CHEMISTRY OF MATERIALS, 2001, 13 (01) : 208 - 212
  • [9] Catalytic performance of vanadium incorporated MCM-41 catalysts for the partial oxidation of methane to formaldehyde
    Du, GA
    Lim, SY
    Yang, YH
    Wang, C
    Pfefferle, L
    Haller, GL
    [J]. APPLIED CATALYSIS A-GENERAL, 2006, 302 (01) : 48 - 61
  • [10] Synthesis, characterization, and catalytic performance of highly dispersed vanadium grafted SBA-15 catalyst
    Du, Guoan
    Lim, Sangyun
    Pinault, Mathieu
    Wang, Chuan
    Fang, Fang
    Pfefferle, Lisa
    Haller, Gary L.
    [J]. JOURNAL OF CATALYSIS, 2008, 253 (01) : 74 - 90