五元水滑石的微波晶化法合成及催化苯酚羟基化反应

Catalytic Hydroxylation of Phenol over Pentatomic Hydrotalcite Prepared by Microwave Irradiation

采用微波晶化法合成了二元CuAl、三元CuAlNi、四元CuAlNiFe、五元CuAlNiFeCo水滑石类化合物 ,并将其用于催化苯酚羟基化制苯二酚 ,结果表明五元配合物的催化性能最好。Cu4NiCoFeAlCO3的XRD和IR表征表明其晶体结构为水滑石结构 ;用TEM观察了五元配合物的晶体形貌。五元水滑石催化苯酚羟基化反应结果表明 ,催化剂活性随其铜含量的增加而增大 ;双氧水的有效利用率随苯酚 双氧水摩尔比的升高而增大。以Cu4NiCoFeAlCO3 为催化剂时 ,在苯酚 催化剂质量比为 1 0、1 0mL水作溶剂、0 5g苯酚、苯酚 双氧水摩尔比为 1∶2条件下 ,苯酚转化率为 62 96% ,苯二酚的选择性达到 97 63 %。

This paper introduced solid complex compounds including duality CuAl, ternary CuAlNi, quaternary CuAlNiFe, pentatomic CuAlNiFeCo were synthesized by microwave irradiation, which catalyzed phenol hydroxylation. It was found pentatomic compound was the best catalyst. The crystalline structure and appearance of Cu 4 NiCoFeAlCO 3 were characterized by XRD, IR and TEM, which proved Cu 4 NiCoFeAlCO 3 catalyst had hydrotalcite structure. When pentatomic hydrotalcite catalyzed phenol hydroxylation, catalytic activity was boosted with copper content increasing. Effective utilization rate of H 2 O 2 was enhanced with phenol/ H 2 O 2 molar ratio increasing. The phenol conversion and selectivity of diphenol reached 62.96%, 97.63%, respectively, when Cu 4 NiCoFeAlCO 3 as catalyst, the amount ratio of phenol/catalyst being 10, with 10mL distilled water as solvent, phenol amount being 0.5g, phenol/ H 2 O 2 molar ratio was 1∶2, reaction temperature 70℃, reaction time 2h.