Zeolite ZSM-5 synthesized in space: catalysts with reduced external surface activity

被引:16
作者
Coker, EN
Jansen, JC
DiRenzo, F
Fajula, F
Martens, JA
Jacobs, PA
Sacco, A
机构
[1] Delft Univ Technol, Fac Chem Technol & Mat Sci, NL-2628 BL Delft, Netherlands
[2] ENSCM, UMR 5618 CNRS, Lab Mat Catalyt & Catalyse Chim Organ, F-34296 Montpellier, France
[3] Katholieke Univ Leuven, Dept Interfasechem, B-3001 Heverlee, Belgium
[4] Northeastern Univ, Dept Civil Engn, Snell Engn Ctr 147, Boston, MA 02115 USA
基金
美国国家航空航天局;
关键词
ZSM-5; low-gravity synthesis; AFM; external surface; aluminum profile;
D O I
10.1016/S1387-1811(01)00298-0
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Two samples of zeolite ZSM-5 were prepared in the free-fall environment (10(-4)-10(-6) g) of low earth orbit aboard the space shuttle Columbia. Using identical solutions and protocols of in situ mixing and hydrothermal treatment, similar samples were prepared on earth using identical hardware. The solutions processed in space produced three principal crystal morphologies: cubic twins, cubic single and elongated prismatic crystals. The terrestrial solutions produced elongated prismatic crystals and cubic twins which settled under gravity into intergrown sheets; unlike the space-grown samples, no single cubic crystals were found. On average, crystals grown in space were larger than those grown on earth. Ignoring multiple intergrowths, the largest crystals from space were cubic, measuring approximate to 300 x 250 x 150 mum(3), while the largest terrestrial crystals were prismatic and about 300 x 100 x 50 mum(3). Little difference in structure between low-gravity and terrestrial crystals was found using single crystal X-ray diffraction. The unit cells of the space samples were up to 0.05% larger in linear dimension than those of similar terrestrial crystals. These results were consistent with data from electron probe microanalysis, which indicated that the aluminum concentration per unit cell in the space crystals was, on average, 2-2.5 times higher than in the terrestrial crystals. Preliminary catalytic testing revealed that the crystals grown in low gravity have lower activity to non-shape selective reactions than those grown on earth. AFM showed that the external surfaces of the space crystals were substantially smoother than those of the terrestrial crystals, while the concentrations of surface hydroxyl groups were found to be significantly higher for the earth-grown crystals. The reduction in the external surface area of the space crystals and the concomitant reduction in hydroxyl group concentrations across the surface could be of significant commercial importance for shape-selective reactions. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:223 / 236
页数:14
相关论文
共 31 条
[1]  
ANDERSON MW, 1999, P 12 INT ZEOL C, V3, P1487
[2]  
CHEN CSH, 1996, J CATAL, V161, P6871
[3]   ZEOLITE SYNTHESIS IN UNSTIRRED BATCH REACTORS .1. NUCLEAR-MAGNETIC-RESONANCE IMAGING OF NONUNIFORM PRE-MIXING [J].
COKER, EN ;
HEES, PS ;
SOTAK, CH ;
DIXON, AG ;
THOMPSON, RW ;
SACCO, A .
MICROPOROUS MATERIALS, 1995, 3 (06) :623-636
[4]   The synthesis of zeolites under micro-gravity conditions: A review [J].
Coker, EN ;
Jansen, JC ;
Martens, JA ;
Jacobs, PA ;
DiRenzo, F ;
Fajula, F ;
Sacco, A .
MICROPOROUS AND MESOPOROUS MATERIALS, 1998, 23 (1-2) :119-136
[5]   Methylamines synthesis: A review [J].
Corbin, DR ;
Schwarz, S ;
Sonnichsen, GC .
CATALYSIS TODAY, 1997, 37 (02) :71-102
[6]   QUINOLINE AS A PROBE MOLECULE FOR DETERMINATION OF EXTERNAL BRONSTED AND LEWIS ACIDITY IN ZEOLITES [J].
CORMA, A ;
FORNES, V ;
REY, F .
ZEOLITES, 1993, 13 (01) :56-59
[7]  
FISKE MR, 1991, SOC PHOTO OPT INSTRU, V1557, P78
[8]   ON THE EXTERNAL AND INTRACRYSTALLINE SURFACE CATALYTIC ACTIVITY OF PENTASIL ZEOLITES [J].
GILSON, JP ;
DEROUANE, EG .
JOURNAL OF CATALYSIS, 1984, 88 (02) :538-541
[9]  
HONGCHEN G, 1999, P 12 INT ZEOL C, V1, P141
[10]   INVESTIGATION OF INTERNAL SILANOL GROUPS AS STRUCTURAL DEFECTS IN ZSM-5-TYPE ZEOLITES [J].
HUNGER, M ;
KARGER, J ;
PFEIFER, H ;
CARO, J ;
ZIBROWIUS, B ;
BULOW, M ;
MOSTOWICZ, R .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1987, 83 :3459-&