过渡金属负载钛交联黏土催化剂的制备及其催化性能

PREPARATION OF TI-PILLARED CLAYS MODIFIED WITH TRANSITION METALS AND THEIR CATALYTIC PERFORMANCES

以钛酸正丁酯为钛源制备了钛交联黏土纳米复合材料(Ti-PILC),然后以该钛交联黏土为载体,制备了用于苯酚羟基化反应的过渡金属负载钛交联黏土催化剂Fe-Ti-PILC、Cu-Ti-PILC和V-Ti-PILC。运用XRD、FT-IR、TG-DSC、SEM和元素分析等手段对钛交联黏土纳米复合材料和催化剂进行了表征,还考察了以Fe-Ti-PILC为催化剂的苯酚羟基化反应中溶剂和催化剂用量、n(Phenol)/n(H2O2)、反应温度和反应时间等对反应的影响。结果表明,与Cu-Ti-PILC、V-Ti-PILC相比,Fe-Ti-PILC对苯酚羟基化反应具有较高的催化活性;在以水为溶剂、Fe-Ti-PILC催化剂用量50mg、n(Phenol)/n(H2O2)=3、反应温度70℃、反应时间3h的条件下,苯酚羟基化反应中苯酚的转化率为25.8%,苯二酚选择性为85.8%。

Ti-pillared clay nano-composite （Ti-PILC） was prepared with Ti（n C4H9O）4 as the titanium resource. Then the transition metal supported Ti-pillared clay catalysts, Fe-Ti-PILC. Cu-Ti-PILC and V-Ti PILC, used for phenol hydroxylation reaction were prepared. Ti-PILC, Fe-Ti-PILC, Cu-Ti-PILC and V-Ti-PILC were characterized by XRD, FT-IR, TG-DSC, SEM and element analysis. The effects of solvent, amount of catalyst, molar ratio of phenol to H2O2, reaction temperature and time on the reaction of phenol hydroxylation with Fe-Ti-PILC as catalyst were also investigated. The results showed that Fe Ti-PILC possessed an excellent catalytic activity, compared with Cu-Ti-PILC and V-Ti-PILC. The phenol conversion was 25.8% and the dihydroxybenzene total selectivity reached to 85. 8% in the reaction of phenol hydroxylation with water as solvent and under the conditions of 50 mg Fe-Ti-PILC, n （Phenol）/n （ H2O2 ） = 3, reaction temperature 70℃ and reaction time 3 h.