MeAPO-11的合成及其在苯酚羟基化反应中的催化性能  

Synthesis and Catalytic Properties of MeAPO-11 Molecular Sieves for Phenol Hydroxylation

作　　者：韶晖[1] 陈霞[1] 王彬彬[1] 钟璟[1] 杨超[2] 

机构地区：[1]常州大学石油化工学院,江苏常州213164 [2]中国科学院过程工程研究所绿色过程与工程重点实验室,北京100190

出　　处：《石油学报（石油加工）》2012年第6期933-939,共7页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：江苏省重点实验室开放课题(KF0806);常州市科技成果转化及产业化计划(CC20110003);江苏省科技支撑计划(BE2011651);江苏省高校自然科学研究重大项目(11KJA610002)资助

摘　　要：采用气相转移法合成了一系列杂原子磷铝分子筛MeAPO-11(Me为Cu、Fe、Zn、Mn),并利用X射线衍射(XRD)、扫描电子显微镜(SEM)、热重-差热分析(TG-DSC)、漫反射紫外-可见光谱(DR UV-Vis)和等离子发射光谱(ICP)对其进行了表征,同时考察了它们对苯酚羟基化反应的催化性能。结果表明,采用气相转移法合成的MeAPO-11分子筛具有较高的结晶度和稳定性,杂原子可以通过同晶取代Al进入分子筛骨架。CuAPO-11具有较高的苯酚羟基化反应催化活性;MnAPO-11催化苯酚羟基化反应中,邻苯二酚选择性较对苯二酚选择性高许多。Me-substituted aluminophosphate molecular sieves MeAPO-11（Me is Cu, Fe, Zn, Mn） were synthesized by vapor-phase transport method （VPT）. The physicochemical properties of MeAPO-11 were characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM）, thermo gravimeter and differential scanning calorimeter （TG-DSC）, diffuse reflectance （DR） UV- Vis spectroscopy and inductively coupled plasma atomic emission spectrometry （ICP）. The catalytic performance of MeAPO-11 molecular sieves was tested by phenol hydroxylation. The results showed that the MeAPO-11 catalysts with high crystallinity and thermal stability were synthesized by VPT. Transition metal atom could be incorporated into the framework through the substitution of A13＋. CuAPO-11 had better catalytic activity for phenol hydroxylation, while over MnAPO-11 the selectivity for catechol was much more than that for hydroquinone.

关 键 词：杂原子磷铝分子筛 气相转移法 MeAPO-11 苯酚羟基化 

分 类 号：TQ426.6[化学工程]