AROMATIZATION OF NORMAL-HEXANE BY PLATINUM-CONTAINING MOLECULAR-SIEVES .2. NORMAL-HEXANE REACTIVITY

被引:90
作者
MIELCZARSKI, E
HONG, SB
DAVIS, RJ
DAVIS, ME
机构
[1] VIRGINIA POLYTECH INST & STATE UNIV,DEPT CHEM ENGN,BLACKSBURG,VA 24061
[2] UNIV VIRGINIA,DEPT CHEM ENGN,CHARLOTTESVILLE,VA 22903
基金
美国国家科学基金会;
关键词
D O I
10.1016/0021-9517(92)90235-A
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
Pt/KL, Pt/BaKL, Pt/KBaKL, Pt/NaY, Pt/CsNaY, Pt/NaFAU(C), Pt/hex, Pt/SSZ-24, Pt/silica, and Pt/carbon were tested as catalysts for the aromatization of n-hexane at 460-510°C and atmospheric total pressure in order to study the influence of Pt cluster size and support acidity/basicity, microstructure, and chemical composition on activity and selectivity. Analysis of the catalytic and NH3 temperature-programmed desorption results from Pt/KL, Pt/BaKL, and Pt/KBaKL reveals that the presence of any acidity increases hydrogenolysis at the expense of benzene production. In addition, no increase in aromatization selectivity is observed by the addition of base sites to a Pt/zeolite catalyst, confirming that aromatization of n-hexane over Pt clusters on nonacidic carriers is monofunctional. High selectivity to benzene over most of the zeolite samples demonstrates that support microstructure does not contribute directly to the aromatization selectivity over Pt catalysts. High selectivity to benzene is observed for a Pt/carbon catalyst suggesting that a zeolitic support is not necessary for good performance. In fact, similar reactivity is obtained from microporous (Pt/SSZ-24) and nonmicroporous (Pt/silica) silica supported platinum catalysts with similar H/Pt values. A clear trend of increasing benzene selectivity with decreasing Pt cluster size is found. These observations suggest that the exceptional reactivity of Pt/KL for the aromatization of n-hexane results from the lack of any acidity in the support and the ability of zeolite L to stabilize the formation of extremely small Pt clusters. © 1992.
引用
收藏
页码:359 / 369
页数:11
相关论文
共 22 条
[1]  
BERNARD JR, 1980, 5TH P INT C ZEOL NAP, P686
[2]   PLATINUM-ZEOLITE INTERACTIONS IN ALKALINE L-ZEOLITES - CORRELATIONS BETWEEN CATALYTIC ACTIVITY AND PLATINUM STATE [J].
BESOUKHANOVA, C ;
GUIDOT, J ;
BARTHOMEUF, D ;
BREYSSE, M ;
BERNARD, JR .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1981, 77 :1595-1604
[3]  
Boudart M., 2014, KINETICS HETEROGENEO
[4]   ISOMERIZATION AND DEHYDROCYCLIZATION OF HEXANES OVER MONOFUNCTIONAL SUPPORTED PLATINUM CATALYSTS [J].
DAUTZENBERG, FM ;
PLATTEEUW, JC .
JOURNAL OF CATALYSIS, 1970, 19 (01) :41-+
[5]   A NONPOROUS SUPPORTED-PLATINUM CATALYST FOR AROMATIZATION OF N-HEXANE [J].
DAVIS, RJ ;
DEROUANE, EG .
NATURE, 1991, 349 (6307) :313-315
[6]   SURFACE-STRUCTURE AND TEMPERATURE-DEPENDENCE OF N-HEXANE SKELETAL REARRANGEMENT REACTIONS CATALYZED OVER PLATINUM SINGLE-CRYSTAL SURFACES - MARKED STRUCTURE SENSITIVITY OF AROMATIZATION [J].
DAVIS, SM ;
ZAERA, F ;
SOMORJAI, GA .
JOURNAL OF CATALYSIS, 1984, 85 (01) :206-223
[7]   STRUCTURAL RECOGNITION AND PREORGANIZATION IN ZEOLITE CATALYSIS - DIRECT AROMATIZATION OF NORMAL-HEXANE ON ZEOLITE L-BASED CATALYSTS [J].
DEROUANE, EG ;
VANDERVEKEN, DJ .
APPLIED CATALYSIS, 1988, 45 (01) :L15-L22
[8]   BASE CATALYSIS BY ALKALI-MODIFIED ZEOLITES .1. CATALYTIC ACTIVITY [J].
HATHAWAY, PE ;
DAVIS, ME .
JOURNAL OF CATALYSIS, 1989, 116 (01) :263-278
[9]   HIGH-RESOLUTION, QUASI-EQUILIBRIUM SORPTION STUDIES OF MOLECULAR-SIEVES [J].
HATHAWAY, PE ;
DAVIS, ME .
CATALYSIS LETTERS, 1990, 5 (4-6) :333-348
[10]   AROMATIZATION OF NORMAL-HEXANE BY PLATINUM-CONTAINING MOLECULAR-SIEVES .1. CATALYST PREPARATION BY THE VAPOR-PHASE IMPREGNATION METHOD [J].
HONG, SB ;
MIELCZARSKI, E ;
DAVIS, ME .
JOURNAL OF CATALYSIS, 1992, 134 (01) :349-358