Comparison of the different promoting effects of Fe-Mn, Ni and Pt on the n-butane isomerization activity of sulfated zirconia catalysts

被引:29
作者
Alvarez, WE [1 ]
Liu, H [1 ]
Resasco, DE [1 ]
机构
[1] UNIV OKLAHOMA,SCH CHEM ENGN,NORMAN,OK 73019
基金
美国国家科学基金会;
关键词
sulfated zirconia; Fe-; Mn- and Pt-promoted catalysts; strong solid acid; n-butane isomerization; bimolecular mechanism;
D O I
10.1016/S0926-860X(97)00088-4
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
The n-butane isomerization has been studied on a series of transition metal-promoted sulfated zirconia catalysts. In support of the bimolecular mechanism that involves the participation of olefins and oligomeric carbenium ions on the surface, it was found that the activity of the catalysts under continuous flow operation was much higher than that obtained in the pulse mode. However, when small quantities of l-butene were added to the pulses, the activity was greatly enhanced. This enhancement significantly varied with the type of metal promoter present in the SZ catalyst. A strong influence of the purity of the n-butane used on activity and sensitivity to hydrogen was observed. When pure n-butane feed was used, the presence of hydrogen had a strong inhibiting effect on activity at low temperatures, but a promoting effect at high temperatures. This promoting effect was particularly prominent on PtSZ and NiSZ catalysts and is primarily due to a decreased deactivation. When n-butane with olefin impurities was used as a feed, the effect of hydrogen was only evident on the PtSZ catalyst. The NiSZ catalyst did not show the inhibition at low temperatures nor the enhanced stability at high temperatures exhibited when n-butane of high purity was used. It was found that the formation of coke has a direct relationship with the low temperature activity. A comparison of the different catalysts investigated under various conditions reflected a trend: the lower the temperature at which n-butane can be converted, the more rapid deactivation and the higher the amount of coke formed. (C) 1997 Elsevier Science B.V.
引用
收藏
页码:103 / 119
页数:17
相关论文
共 30 条
  • [1] ISOMERIZATION OF C-13 LABELED BUTANE OVER FE,MN PROMOTED SULFATED ZRO2 CATALYST
    ADEEVA, V
    LEI, GD
    SACHTLER, WMH
    [J]. APPLIED CATALYSIS A-GENERAL, 1994, 118 (01) : L11 - L15
  • [2] ACID SITES IN SULFATED AND METAL-PROMOTED ZIRCONIUM DIOXIDE CATALYSTS
    ADEEVA, V
    DEHAAN, JW
    JANCHEN, J
    LEI, GD
    SCHUNEMANN, V
    VANDEVEN, LJM
    SACHTLER, WMH
    VANSANTEN, RA
    [J]. JOURNAL OF CATALYSIS, 1995, 151 (02) : 364 - 372
  • [3] Alvarez WE, 1996, STUD SURF SCI CATAL, V101, P553
  • [4] BROWER DM, 1972, PROGR PHYS ORG CHEM, V9, P179
  • [5] LOW-TEMPERATURE SUPERACID CATALYSIS - REACTIONS OF N-BUTANE CATALYZED BY IRON-PROMOTED AND MANGANESE-PROMOTED SULFATED ZIRCONIA
    CHEUNG, TK
    DITRI, JL
    GATES, BC
    [J]. JOURNAL OF CATALYSIS, 1995, 151 (02) : 464 - 466
  • [6] Propane conversion catalyzed by sulfated zirconia, iron- and manganese-promoted sulfated zirconia, and USY zeolite
    Cheung, TK
    Lange, FC
    Gates, BC
    [J]. JOURNAL OF CATALYSIS, 1996, 159 (01) : 99 - 106
  • [7] Induction of activity and deactivation of Fe, Mn-promoted sulfated zirconia catalysts
    Coelho, MA
    Alvarez, WE
    Sikabwe, EC
    White, RL
    Resasco, DE
    [J]. CATALYSIS TODAY, 1996, 28 (04) : 415 - 429
  • [8] MODIFICATION OF THE CATALYTIC PROPERTIES OF SULFATED ZIRCONIA BY ADDITION OF METAL PROMOTERS
    COELHO, MA
    RESASCO, DE
    SIKABWE, EC
    WHITE, RL
    [J]. CATALYSIS LETTERS, 1995, 32 (3-4) : 253 - 262
  • [9] DYNAMIC MODIFICATION OF SURFACE ACID PROPERTIES WITH HYDROGEN MOLECULE FOR ZIRCONIUM-OXIDE PROMOTED BY PLATINUM AND SULFATE-IONS
    EBITANI, K
    TSUJI, J
    HATTORI, H
    KITA, H
    [J]. JOURNAL OF CATALYSIS, 1992, 135 (02) : 609 - 617
  • [10] SKELETAL ISOMERIZATION OF HYDROCARBONS OVER ZIRCONIUM-OXIDE PROMOTED BY PLATINUM AND SULFATE ION
    EBITANI, K
    KONISHI, J
    HATTORI, H
    [J]. JOURNAL OF CATALYSIS, 1991, 130 (01) : 257 - 267