Solid acid characteristics and isobutane/butene alkylation

被引:30
作者
Platon, A [1 ]
Thomson, WJ [1 ]
机构
[1] Washington State Univ, Dept Chem Engn, Pullman, WA 99164 USA
关键词
hydride transfer; alkylation of isobutane; butene; cyclohexene; solid acid catalyst; zeolite beta; sulfated zirconia; ZSM-5;
D O I
10.1016/j.apcata.2004.12.005
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
Catalytic behavior during gas-phase, batch alkylation experiments employing isobutane and 1-butene at 80 degrees C was studied for Beta zeolites with SiO2/Al2O3 (SAR) ratios of 25 (25BEA) and 75 (75BEA), ZSM-5 and sulfated zirconia (SZ). The observed alkylation performance was compared to the low-temperature hydride transfer (HT) activity of the studied catalysts and with their acidity, adsorption capacity and surface area measurements. For all materials studied, a correlation was observed between the measured HT activity and the amount of trimethylpentane (TMP) produced per acid site. The 25BEA catalyst produced the highest amount of trimethylpentane (PAP) and also had the most elevated HT activity. ZSM-5 was found to be inactive for both HT and alkylation, and although SZ had moderate alkylation activity, it also had a higher cracking activity than other materials. Modification by water vapor exposure of 25BEA and SZ did not create any noticeable change in Bronsted acidity, but a dramatic decrease in TMP production was detected on the modified catalysts and explained by competitive adsorption between water and isobutane. The apparent butene conversion correlated well with the total catalyst surface area rather than with the total amount of acid sites. In all the catalysts studied a much stronger interaction with butene than with isobutane was observed, suggesting that competitive adsorption between the two reactants limits isobutane access to the active sites, resulting in limited hydride transfer. (c) 2004 Elsevier B.V. All rights ieserved.
引用
收藏
页码:93 / 100
页数:8
相关论文
共 19 条
[1]   Isomerization of n-butane over acid zeolites -: Role of Broensted and Lewis acid sites [J].
Baburek, E ;
Nováková, J .
APPLIED CATALYSIS A-GENERAL, 1999, 185 (01) :123-130
[2]   Supercritical alkylation and butene dimerization over sulfated zirconia and iron-manganese promoted sulfated zirconia catalysts [J].
Chellappa, AS ;
Miller, RC ;
Thomson, WJ .
APPLIED CATALYSIS A-GENERAL, 2001, 209 (1-2) :359-374
[3]   REACTIONS OF ISOBUTANE WITH BUTENE OVER ZEOLITE CATALYSTS [J].
CHU, YF ;
CHESTER, AW .
ZEOLITES, 1986, 6 (03) :195-200
[4]   INFLUENCE OF PROCESS VARIABLES ON THE CONTINUOUS ALKYLATION OF ISOBUTANE WITH 2-BUTENE ON SUPERACID SULFATED ZIRCONIA CATALYSTS [J].
CORMA, A ;
MARTINEZ, A ;
MARTINEZ, C .
JOURNAL OF CATALYSIS, 1994, 149 (01) :52-60
[5]   A COMPARATIVE-STUDY OF O-4(2-)/ZRO2 AND ZEOLITE-BETA AS CATALYSTS FOR THE ISOMERIZATION OF N-BUTANE AND THE ALKYLATION OF ISOBUTANE WITH 2-BUTENE [J].
CORMA, A ;
JUANRAJADELL, MI ;
LOPEZNIETO, JM ;
MARTINEZ, A ;
MARTINEZ, C .
APPLIED CATALYSIS A-GENERAL, 1994, 111 (02) :175-189
[6]   Product selectivity effects during cracking of alkanes at very short and longer times on stream [J].
Corma, A ;
Miguel, PJ ;
Orchilles, AV .
APPLIED CATALYSIS A-GENERAL, 1996, 138 (01) :57-73
[7]   Common mechanistic aspects of liquid and solid acid catalyzed alkylation of isobutane with n-butene [J].
Feller, A ;
Zuazo, I ;
Guzman, A ;
Barth, JO ;
Lercher, JA .
JOURNAL OF CATALYSIS, 2003, 216 (1-2) :313-323
[8]   Pulsed gas-phase alkylation of isobutane/2-butene over sulfated zirconia [J].
Gore, RB ;
Thomson, WJ .
APPLIED CATALYSIS A-GENERAL, 1998, 168 (01) :23-32
[9]   Isobutane alkylation - Recent developments, and future perspectives [J].
Hommeltoft, SI .
APPLIED CATALYSIS A-GENERAL, 2001, 221 (1-2) :421-428
[10]   An in situ DRIFTS study of the deactivation and regeneration of sulfated zirconia [J].
Li, BH ;
Gonzalez, RD .
CATALYSIS TODAY, 1998, 46 (01) :55-67