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Studies on Selective Oxidation of Alcohol Catalyzed by Metal Oxides/TEMPO

Author: ZhaoJunFeng
Tutor: YangGuanYu
School: Zhengzhou University
Course: Organic Chemistry
Keywords: Molecular oxygen Alcohol Catalyst TEMPO Metal oxide
CLC: O643.32
Type: Master's thesis
Year: 2007
Downloads: 302
Quote: 1
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Abstract


The oxidation of alcohols to carbonyl compounds in organic chemistry is a very important reaction occupies its important position in the field of basic research and the production of fine chemicals . Using molecular oxygen as the oxidant , the catalytic selective oxidation of alcohols economic green method . 2,2,6,6 - tetramethyl-piperidine -N-oxide radical (TEMPO) is an excellent small organic molecules of the alcohol oxidation catalyst , under mild conditions , efficient and highly selective catalytic alcohol selective oxidation , and has wide alcohol substrates universality. However , numerous studies have shown that TEMPO catalytic oxidation of alcohols always With both help solve the problem of catalyst . This thesis for the first time to use the metal oxide having a redox properties as multi help solve the problem of catalyst , the combination of molecular oxygen in the selective oxidation TEMPO used in catalytic alcohol , the main results achieved are as follows : 1 . The active of MnO 2 < / sub > TEMPO combination can effectively choose catalytic oxidation of benzyl alcohol to benzaldehyde , 10% of the activity of MnO 2 , 10 mol % of the TEMPO 120 ° C , 0.8MPa , 24h , conversion was 81.9 %, and the selectivity of benzaldehyde is greater than 99% . 2. Coprecipitation obtained Cu-Mn composite oxides exhibit markedly high catalytic activity , the reason may be that the uniform dispersion of the synergistic effect of the center of the Cu, Mn . Oxidation of benzyl alcohol under conditions of 120 ° C , conversion rate and selectivity of a variety of Cu-Mn composite oxide is more than 98%. 3. Manganese-copper ratio in the catalytic activity and selectivity of the Cu-Mn composite oxide showed a greater effect , the copper component is large with higher activity , and the catalytic activity was significantly reduced in the manganese group more . Dispersed CuO is a key component of the catalytic activity of the Cu-Mn composite oxide . 4. Proposed, including two metal oxide redox cycle series / TEMPO system might catalytic mechanism , the key step in the catalytic process , expensive metal oxides first TEMPO oxidation generates the corresponding nitrone cation . 5. Cu 2 Mn / TEMPO system can effectively catalyze the oxidation of other alcohol substrates , a variety of substituted benzyl alcohol, cinnamyl alcohol made ??nearly quantitative conversion rate and selectivity . In short , the paper used for the first time the MnO 2 and MnxCuyOz heterogeneous metal oxide as a co- catalyst , different combinations TEMPO constitute efficient the high selective catalytic system for alcohol molecular oxygen oxidation .

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CLC: > Mathematical sciences and chemical > Chemistry > Physical Chemistry ( theoretical chemistry ),chemical physics > Chemical kinetics,catalysis > Catalytic > Catalytic reaction
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