磁性Zn-BTC@SiO_2@Fe_3O_4催化剂及其对甲苯与对甲基苯甲酰氯酰基化反应的催化性能  

Synthesis of Magnetic Zn-BTC@SiO_2@Fe_3O_4 Catalysts and Their Catalytic Performance for Toluene Acylation With p-Toluoyl Chloride

作　　者：李庆远[1] MUHAMMAD Ammar 季生福[1] 王景艳[1] 刘想 

机构地区：[1]北京化工大学化工资源有效利用国家重点实验室,北京100029

出　　处：《石油学报（石油加工）》2014年第1期126-133,共8页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金项目(21136001;21173018)资助

摘　　要：以磁性SiO2@Fe3O4颗粒为核,在其表面原位合成了金属-有机骨架材料Zn-BTC,制备了一系列新型的Zn-BTC@SiO2@Fe3O4磁性催化剂。采用SEM、TEM、XRD、IR、NH3-TPD和VSM等技术对磁性催化剂的结构和性质进行了表征,并且评价了Zn-BTC@SiO2@Fe3O4磁性催化剂对甲苯和对甲基苯甲酰氯酰基化反应的催化性能。结果表明,一定Zn-BTC含量范围的磁性Zn-BTC@SiO2@Fe3O4催化剂具有好的超顺磁性和酸性;在甲苯和对甲基苯甲酰氯酰基化反应中表现出良好的催化活性,且随着催化剂中Zn-BTC含量的增加,该反应的甲苯转化率逐渐提高;其中Zn-BTC质量分数为36.7%的Zn-BTC@SiO2@Fe3O4催化剂的催化性能最佳,在120℃下,该反应的甲苯转化率可达52.6%;反应后的催化剂经外磁场回收重复使用5次,甲苯的转化率没有明显下降。新型Zn-BTC@SiO2@Fe3O4磁性催化剂在多相催化酰基化反应中具有很好的应用前景。A series of novel magnetic Zn-BTC@SiO2@Fe3O4 catalysts were synthesized by using magnetic SiO2@Fe3O4 nano-particle as the core and Zn-BTC metal-organic framework material as the coating.The structure and properties of the magnetic catalysts were characterized by SEM,TEM,XRD,IR,NH3-TPD and VSM techniques.The catalytic activities of the magnetic catalysts for toluene acylation with p-toluoyl chloride were evaluated.The results showed that the Zn-BTC@SiO2@Fe3O4 magnetic catalysts containing certain content of Zn-BTC exhibited good superparamagnetic properties and acidity.In toluene acylation with p-toluoyl chloride over Zn-BTC @SiO2@Fe3O4,the toluene conversion increased gradually with the increase of Zn-BTC contents in Zn-BTC@[e-mail] the as-synthesized Zn-BTC@SiO2@Fe3O4 samples,the Zn-BTC@SiO2@Fe3O4 containing 36.7% mass fraction of Zn-BTC had better acylation catalytic activity with the toluene conversion of 52.6% at 120℃.The Zn-BTC@SiO2@Fe3O4 catalysts could be reused through the treatment of external magnetic field after reaction.After Zn-BTC@SiO2@Fe3O4 was reused in toluene acylation with p-toluoyl chloride for five times,the toluene conversion was not apparently decreased.This novel magnetic Zn-BTC@SiO2@Fe3O4 catalyst has a potential application in heterogeneous acylation reaction.

关 键 词：金属-有机骨架 Zn-BTC 磁性 催化剂 酰基化 

分 类 号：O627[理学—有机化学] O621.25[理学—化学]