【摘要】 Fe取代系列磷酸铝分子筛 (FeAlPO4 5 ,FeAlPO4 11和FeVPI 5 )在催化氧化芳香族化合物反应 (如苯酚和苯的羟化、苯乙烯的环氧化以及萘酚的氧化 )中具有很高的活性 .系统研究的数据显示 ,在苯酚和苯的羟化及苯乙烯的环氧化反应中 ,FeAlPO4 5及FeAlPO4 11的活性与TS 1催化剂相近 ;在大分子萘酚的氧化反应中 ,FeVPI 5具有较高的活性 ,而小孔的TS 1则没有活性 .比较不同催化剂的活性结果表明 ,骨架中的Fe(Ⅲ )是催化剂的活性中心 .更多还原

【Abstract】 Many metal-containing microporous zeolites have been used in heterogeneous catalytic reactions since TS-1 zeolite used as a catalyst in oxidation reactions. However, some disadvantages of these microporous titanosilicates may limit their application as popular catalysts for oxidation reactions in organic chemistry. In order to obtain new catalysts with relatively simple procedures of preparation, iron-substituted aluminophosphate molecular sieves (FeAlPO 4-5, FeAlPO 4-11 and FeVPI-5, denoted as Fe(Ⅲ)APO) have been hydrothermally synthesized. And these samples are catalytically active in oxidation of aromatic compounds, such as hydroxylation of phenol and benzene, and epoxidation of styrene as well as oxidation of naphthol. The catalytic activity of FeAlPO 4-5 and FeAlPO 4-11 is comparable with that of TS-1 in some reactions. In hydroxylation of phenol and benzene, FeAlPO 4-11 can give conversion of 22.1% and 13.1%, respectively. In styrene epoxidation, FeAlPO 4-11 achieves conversion of 24.7% and selectivity of 55.2%, while TS-1 gives selectivity of 6.2% only, suggesting that the reaction routes in styrene epoxidation are different over these two catalysts. Over FeAlPO 4-11, the isomerization of epoxide hardly occurs in styrene epoxidation. On the contrary, the isomerization of epoxide easily takes place over TS-1. FeVPI-5 shows high activity in naphthol oxidation by H 2O 2 giving conversion of 14.5%, while TS-1 is completely inactive owing to its small pore size. These results suggested that FeVPI-5 is a good candidate for the catalytic oxidation of large organic compounds. The results of Mssbauer spectroscopy of FeAlPO 4-11 and FeAlPO 4-5 suggested that Fe(Ⅲ) in the framework is proposed as the major active sites in the catalytic oxidation.更多还原