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研究了在温和反应条件下自制的TS-1分子筛催化苯羟基化的反应规律.着重考察了酸介质的影响和溶剂的作用,发现在水相和有机相中苯的羟基化和苯酚的进一步羟基化具有不同的规律,有机相中苯的羟基化是主要反应,水相中的主要反应是中间产物苯酚的进一步羟基化,溶剂的作用则是使苯和双氧水分子在TS-1分子筛表面上充分接触并发生反应.发现以丙酮为溶剂,采用乙酸或乙酸酐作介质,较之硫酸介质能更有效地提高苯的转化率;同中性介质相比,苯转化率提高了32%;同硫酸相比,苯转化率提高了15%,苯酚选择性提高了45%.此外,还考察了反应温度、反应时间等其它因素对苯羟基化反应的影响,并在实验基础上推测了TS-1分子筛催化苯羟基化的反应机理.
The reaction rules of benzene hydroxylation catalyzed by TS-1 zeolite under mild reaction conditions were studied. The effects of acid medium and solvent were emphatically investigated. It was found that the hydroxylation of benzene and the further hydroxylation of phenol in water phase and organic phase have different rules. The hydroxylation of benzene in the organic phase is the main reaction. The main reaction is the intermediate hydroxylation of phenol, the role of the solvent is to benzene and hydrogen peroxide molecules in the TS-1 molecular sieve surface full contact and reaction. It was found that using acetone or acetic anhydride as the medium, the benzene conversion rate was improved more effectively than the sulfuric acid medium. Compared with the neutral medium, benzene conversion rate increased by 32%. Compared with the sulfuric acid, benzene conversion 15% increase in phenol selectivity, 45% increase. In addition, the effects of reaction temperature, reaction time and other factors on the hydroxylation of benzene were also investigated. Based on the experimental results, the reaction mechanism of benzene hydroxylation catalyzed by TS-1 zeolite was presumed.