Investigation of Ni-based alumina-supported catalysts for the oxidative dehydrogenation of ethane to ethylene: structural characterization and reactivity studies

被引:326
作者
Heracleous, E
Lee, AF
Wilson, K
Lemonidou, AA
机构
[1] Aristotle Univ Thessaloniki, Dept Chem Engn, GR-54006 Thessaloniki, Greece
[2] Chem Proc Engn Res Inst, CPERI, CERTH, GR-54006 Thessaloniki, Greece
[3] Univ York, Dept Chem, York YO10 5DD, N Yorkshire, England
基金
英国工程与自然科学研究理事会;
关键词
oxidative dehydrogenation; ethane; nickel catalysts; XPS;
D O I
10.1016/j.jcat.2005.01.015
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
In this study, we report the development of efficient Al2O3-supported Ni and promoted Ni-Me (Me = Mo, V, Nb, Ta, Cc) catalysts for the oxidative dehydrogenation of ethane. The effect of nickel loading and the impact of the promoters on the performance of the materials are discussed in the light of a detailed physico-chemical characterization of the catalysts by N-2 adsorption, XRD, XPS, TGA-H-2, and UV-DRS. Nickel was found to interact strongly with alumina, forming surface nickel aluminate-like species in the submonolayer regime, whereas NiO crystallites formed on top of the nickel/alumina interface for multilayer coverages. XPS revealed a chemical modification of the NiO particles accommodated on the alumina support. In terms of catalytic performance, increasing the Ni loading was beneficial and boosted ethane conversion, which surpassed 40% at 450 degrees C for the highest nickel loading catalyst, whereas ethene selectivity was retained at high levels for all Ni/Al2O3 catalysts. Promotion with V, Mo, Co, Nb, and Ta significantly modified both structural and catalytic properties in ethane oxidative dehydrogenation. The introduction of niobium was the most beneficial for ethane ODH, increasing the reactivity toward ethane by more than 50% at the expense of a relatively small drop (10%) in ethene selectivity. (c) 2005 Elsevier Inc. All rights reserved.
引用
收藏
页码:159 / 171
页数:13
相关论文
共 53 条
[31]   Surface reactivity of NiO: Interaction with methanol [J].
Natile, MM ;
Glisenti, A .
CHEMISTRY OF MATERIALS, 2002, 14 (12) :4895-4903
[32]   Study of surface reactivity of cobalt oxides: Interaction with methanol [J].
Natile, MM ;
Glisenti, A .
CHEMISTRY OF MATERIALS, 2002, 14 (07) :3090-3099
[33]   SURFACE COMPOSITION OF BINARY-SYSTEMS - PREDICTION OF SURFACE PHASE-DIAGRAMS OF SOLID-SOLUTIONS [J].
OVERBURY, SH ;
BERTRAND, PA ;
SOMORJAI, GA .
CHEMICAL REVIEWS, 1975, 75 (05) :547-560
[34]   THE DEFECT STRUCTURE OF NICKEL-OXIDE SURFACES AS REVEALED BY PHOTOELECTRON-SPECTROSCOPY [J].
ROBERTS, MW ;
SMART, RS .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1984, 80 :2957-2968
[35]   Role of support in CO2 reforming of CH4 to syngas over Ni catalysts [J].
Ruckenstein, E ;
Hu, YH .
JOURNAL OF CATALYSIS, 1996, 162 (02) :230-238
[36]   Characterization of nickel species on several gamma-alumina supported nickel samples [J].
Salagre, P ;
Fierro, JLG ;
Medina, F ;
Sueiras, JE .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1996, 106 (1-2) :125-134
[37]   Low temperature oxidative dehydrogenation of ethane over catalysts based on group VIII metals [J].
Schuurman, Y ;
Ducarme, V ;
Chen, T ;
Li, W ;
Mirodatos, C ;
Martin, GA .
APPLIED CATALYSIS A-GENERAL, 1997, 163 (1-2) :227-235
[38]   THE OXIDATIVE COUPLING OF METHANE AND THE OXIDATIVE DEHYDROGENATION OF ETHANE OVER A NIOBIUM PROMOTED LITHIUM DOPED MAGNESIUM-OXIDE CATALYST [J].
SWAAN, HM ;
LI, Y ;
SESHAN, K ;
VANOMMEN, JG ;
ROSS, JRH .
CATALYSIS TODAY, 1993, 16 (3-4) :537-546
[39]   Quasiharmonic free energy and derivatives for slabs: Oxide surfaces at elevated temperatures [J].
Taylor, MB ;
Sims, CE ;
Barrera, GD ;
Allan, NL ;
Mackrodt, WC .
PHYSICAL REVIEW B, 1999, 59 (10) :6742-6751
[40]   OXIDATIVE DEHYDROGENATION OF ETHANE OVER CATALYSTS CONTAINING MIXED OXIDES OF MOLYBDENUM AND VANADIUM [J].
THORSTEINSON, EM ;
WILSON, TP ;
YOUNG, FG ;
KASAI, PH .
JOURNAL OF CATALYSIS, 1978, 52 (01) :116-132