Catalytic properties of palladium nanoclusters synthesized within diblock copolymer films: hydrogenation of ethylene and propylene

被引:63
作者
Ciebien, JF [1 ]
Cohen, RE [1 ]
Duran, A [1 ]
机构
[1] MIT, Dept Chem Engn, Cambridge, MA 02139 USA
来源
SUPRAMOLECULAR SCIENCE | 1998年 / 5卷 / 1-2期
基金
美国国家科学基金会;
关键词
D O I
10.1016/S0968-5677(97)00075-8
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Palladium nanoclusters were synthesized within microphase-separated diblock copolymer films of [MTD](113)[Pd(Cp-N)PA](50) (MTD = methyltetracyclododecene, Cp-N = endo-2-(cyclopentadienylmethyl) norborn-5-ene, PA = eta(3)-1-phenylallyl). The organometallic repeat units were reduced by exposing the films to hydrogen at 100 degrees C, leading to the formation of nearly monodisperse palladium nanoclusters. TEM, SAXS, and WAXS were used to characterized the polymer morphology and cluster size. The nanocomposites were active catalysts for hydrogenation of ethylene and propylene. The cluster size and voids within the polymer matrix were important factors in determining the catalyst activity, expressed as the moles of alkene hydrogenated per mole palladium per second. In contrast to permeation results that showed that the permeability of propylene in polyMTD is greater than that of ethylene, the catalyst activity for hydrogenation of ethylene was greater than that for propylene. (C) 1998 Elsevier Science Limited.
引用
收藏
页码:31 / 39
页数:9
相关论文
共 80 条
[1]   Synthesis and characterization of noble metal colloids in block copolymer micelles [J].
Antonietti, M ;
Wenz, E ;
Bronstein, L ;
Seregina, M .
ADVANCED MATERIALS, 1995, 7 (12) :1000-+
[2]   MAXIMUM PER-PASS CONVERSION IN POROUS MEMBRANE DEHYDROGENATION REACTORS [J].
BADRA, C .
SEPARATION SCIENCE AND TECHNOLOGY, 1994, 29 (02) :275-288
[3]  
BAHNEMANN DW, 1993, ISR J CHEM, V33, P115
[4]   MODELING OF ETHYLBENZENE DEHYDROGENATION IN A CATALYTIC MEMBRANE REACTOR [J].
BECKER, YL ;
DIXON, AG ;
MOSER, WR ;
MA, YH .
JOURNAL OF MEMBRANE SCIENCE, 1993, 77 (2-3) :233-244
[5]  
BERNEY CV, 1988, MACROMOLECULES, V17, P2235
[6]   RELATIONSHIPS BETWEEN PHYSICOCHEMICAL PROPERTIES AND CATALYTIC ACTIVITY OF POLYMER-SUPPORTED PALLADIUM CATALYSTS .1. EXPERIMENTAL INVESTIGATIONS [J].
BIFFIS, A ;
CORAIN, B ;
CVENGROSOVA, Z ;
HRONEC, M ;
JERABEK, K ;
KRALIK, M .
APPLIED CATALYSIS A-GENERAL, 1995, 124 (02) :355-365
[7]   THE ORIGINS OF PARTICLE-SIZE EFFECTS IN HETEROGENEOUS CATALYSIS [J].
BOND, GC .
SURFACE SCIENCE, 1985, 156 (JUN) :966-981
[8]   CLUSTERS, COLLOIDS AND CATALYSIS [J].
BRADLEY, JS ;
HILL, E ;
LEONOWICZ, ME ;
WITZKE, H .
JOURNAL OF MOLECULAR CATALYSIS, 1987, 41 (1-2) :59-74
[9]   THE CHEMISTRY OF RUTHENIUM IN CELLULOSE-ACETATE - REACTIONS WITH CO, H-2, O-2 AND H2O [J].
CHU, JW ;
SHIM, IW .
JOURNAL OF MOLECULAR CATALYSIS, 1993, 78 (02) :189-199
[10]  
CIEBIEN JF, 1997, THESIS MIT