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@SiO2@Fe3O4.Among 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.
出处
《石油学报（石油加工）》
EI
CAS
CSCD
北大核心
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
