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Zirconium, Titanium Oxide Matrix Of The Nano-catalyst Preparation And Research

Posted on:2005-06-29Degree:MasterType:Thesis
Country:ChinaCandidate:L XuFull Text:PDF
GTID:2191360125452699Subject:Physical chemistry
Abstract/Summary:PDF Full Text Request
1. Preparation, characterization and observed catalytic activity of nanosolid superacids doped by metal ionsSulfated zirconia (SO42-/ZrO2) and Ni2+, A13+, Sn4+, Sn2+, Ag+, V5+, Cr3+ doping SO4 2-/ZrO2 ultrafine particle solid superacid catalysts were prepared by impregnation of zirconium hydroxide with SO42- and different metal ions. The samples were characterized using IR, BET, XRD, TEM, SEM, DTA and chemical analysis method. The acidity and catalytic activity of the catalysts were observed with the probe reactions, the esterification of acetic acid and n-butanol and the cracking reaction of n-hexane. It is found that SO4 2-/ZrO2 doped by different metal ions showed different properties (particle sizes, specific surface area, catalytic activity) and all catalysts were nanometer scale particles (<50 run). Among them, the coordination of metal ions (Ni2+, A13+, Sn4+,Sn2+, etc) and SO42- increased the transition temperature of ZrO2 from tetragonal crystal to monoclinic crystal, meanwhile, crystallite size decreased and specific surface area increased significantly. The reaction results indicate that the SO42-/ZrO2 catalysts doped by Al3+ showed the highest catalytic activity for esterification of acetic acid and n-butanol, and the SO427ZrO2 catalysts doped by Ni2+ showed the highest catalytic activity for cracking reaction of n-hexane. But the doping of Ag+ decreased the transition temperature of ZrO2 in comparison with that of SO42-/ZrO2, and the catalyst of the SO42-/ZrO2 doped by Ag+ showed lower catalytic activity both for esterification of acetic acid and n-butanol and cracking reaction of n-hexane.2. Synthesis of butyl acetate catalyzed over solid superacidsCatalyzed over A1(NO3)3/SZ solid superacid catalyst, butyl acetate has been synthesized from butanol and acetic acid. Reaction condition for synthesis of n-butyl acetate was investigated and the best reaction condition was determined, the conversion proportion of 90.3% was attained under following conditions: 20mL benzene as water-carrying agent, 0.5g catalyst (the catalyst quantity is 2% of acetic acid mass), the mole ratio of butanol to acetic acid was 1.40:1 (i.e., 43g n-butanol and 25g acetic acid) and the temperature was approximate 383K, with water separation and recycle, the reaction time of esterification was only 2h. Acetic acid could react with butanol completely in 4h and conversion of acetic acid reached 98.5%. The catalysts could be recovered easily and used repeatedly for many times without obvious loss of activity.3. Acetone oligomerization on TiO2/NaX-13 molecular sieve surfacesAcetone oligomerization on TiO2/NaX-13 molecular sieve catalyst to form mesitylene (1,3,5-trimethylbenzene) or isophorone were studied in fixed bed reactor in order to find a new way of developing acetone. The experimental results showed that under the condition of normal pressure and reaction temperature 473-523K, LHSV 2~3h-1, the once-through conversion of acetone was about 45% and selectivity of mesityl oxide and mesitylene and isophorone were about 45% and 43% and 12% respectively.
Keywords/Search Tags:Nano-catalyst
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