Gas phase methanol oxidation on V-MCM-41

被引:71
作者
Lim, SY [1 ]
Haller, GL [1 ]
机构
[1] Yale Univ, Dept Chem Engn, New Haven, CT 06520 USA
基金
新加坡国家研究基金会;
关键词
methanol oxidation; vanadium substituted MCM-41; active sites; oxygen titration; pyridine TPD; in situ FTIR;
D O I
10.1016/S0926-860X(99)00213-6
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
dGas phase methanol partial oxidation was carried out on a highly ordered vanadium substituted MCM-41 and an acid site related active site is proposed for this reaction. All synthesized samples showed similar values for the methanol percent conversion and the formaldehyde selectivity independent of the vanadium content. The turnover frequency of methanol and formaldehyde was also similar when it was normalized by the accessible active site concentration measured by the oxygen titration at reaction temperature. The active site concentration was found to be correlated with the acid site concentration of V-MCM-41. The main active site is proposed to be a weak Lewis acid site, which has an isolated tetrahedral coordination of vanadium with surrounding oxygen anions. V-MCM-41 is a stable catalyst against gas phase methanol oxidation at 350 degrees C. The saturation value of vanadium concentration in this catalytic system was estimated to be 0.41 wt.%, and produces a very stable isolated tetrahedral coordination V site. (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:277 / 286
页数:10
相关论文
共 34 条
[2]   ON THE MECHANISM OF METHANOL OXIDATION OVER VANADIA-BASED CATALYSTS - A FT-IR STUDY OF THE ADSORPTION OF METHANOL, FORMALDEHYDE AND FORMIC-ACID ON VANADIA AND VANADIA-SILICA [J].
BUSCA, G .
JOURNAL OF MOLECULAR CATALYSIS, 1989, 50 (02) :241-249
[3]   Infrared studies of the reactive adsorption of organic molecules over metal oxides and of the mechanisms of their heterogeneously-catalyzed oxidation [J].
Busca, G .
CATALYSIS TODAY, 1996, 27 (3-4) :457-496
[4]   FT-IR STUDY OF THE ADSORPTION AND TRANSFORMATION OF FORMALDEHYDE ON OXIDE SURFACES [J].
BUSCA, G ;
LAMOTTE, J ;
LAVALLEY, JC ;
LORENZELLI, V .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1987, 109 (17) :5197-5202
[5]   MECHANISM OF SELECTIVE METHANOL OXIDATION OVER VANADIUM-OXIDE TITANIUM-OXIDE CATALYSTS - A FT-IR AND FLOW REACTOR STUDY [J].
BUSCA, G ;
ELMI, AS ;
FORZATTI, P .
JOURNAL OF PHYSICAL CHEMISTRY, 1987, 91 (20) :5263-5269
[6]   CHARACTERIZATION OF SUPPORTED VANADIUM-OXIDE CATALYSTS BY A LOW-TEMPERATURE OXYGEN-CHEMISORPTION TECHNIQUE .3. THE V2O5/ZRO2 SYSTEM ALPHA [J].
CHARY, KVR ;
RAO, BR ;
SUBRAHMANYAM, VS .
APPLIED CATALYSIS, 1991, 74 (01) :1-13
[7]   MECHANISM OF PARTIAL OXIDATION OF METHANOL OVER MOO3 [J].
CHUNG, JS ;
MIRANDA, R ;
BENNETT, CO .
JOURNAL OF CATALYSIS, 1988, 114 (02) :398-410
[8]   Use of mesoporous MCM-41 aluminosilicates as catalysts in the production of fine chemicals: Preparation of dimethylacetals [J].
Climent, MJ ;
Corma, A ;
Iborra, S ;
Navarro, MC ;
Primo, J .
JOURNAL OF CATALYSIS, 1996, 161 (02) :783-789
[9]   PHYSICAL AND CHEMICAL CHARACTERIZATION OF SURFACE VANADIUM-OXIDE SUPPORTED ON TITANIA - INFLUENCE OF THE TITANIA PHASE (ANATASE, RUTILE, BROOKITE AND B) [J].
DEO, G ;
TUREK, AM ;
WACHS, IE ;
MACHEJ, T ;
HABER, J ;
DAS, N ;
ECKERT, H ;
HIRT, AM .
APPLIED CATALYSIS A-GENERAL, 1992, 91 (01) :27-42
[10]   EFFECT OF ADDITIVES ON THE STRUCTURE AND REACTIVITY OF THE SURFACE VANADIUM-OXIDE PHASE IN V2O5 TIO2 CATALYSTS [J].
DEO, G ;
WACHS, IE .
JOURNAL OF CATALYSIS, 1994, 146 (02) :335-345