State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012, People's Republic of China.
Dalton Trans. 2009 Dec 21(47):10527-33. doi: 10.1039/b915232f. Epub 2009 Oct 29.
A series of new magnetically recyclable catalysts (MRCs), Ag-M(1-x)Fe(2+x)O(4) (M = Co, Ni, Mn, Zn) nanocomposites, have been synthesized via a generalized one-pot route, and these materials prove to be efficient MRCs in the catalytic epoxidation of styrene. Characterization by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), infrared (IR) and X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), and magnetic measurement reveal that the nanocomposites are assembled from well crystallized Ag and corresponding ferrite primary particles with the assistance of polyvinylpyrrolidone (PVP). The nanocomposite samples are comparable in Brunauer-Emmett-Teller (BET) specific surface areas and are superparamagnetic at room temperature. The as-prepared MRCs exhibit high activities in the epoxidation of styrene in toluene with tert-butylhydroperoxide (TBHP) as the oxidant and very high yields of styrene oxide can be achieved within 5 h of reaction. All the MRCs can be easily recovered by using a magnet and no decrease in the yield of styrene oxide has been observed after several consecutive rounds of reaction. It has been demonstrated that the ferrite supports affect the structure of Ag and the efficiency in oxygen supply and thus the catalytic performance.
一系列新型的可磁回收催化剂(MRCs),Ag-M(1-x)Fe(2+x)O(4)(M=Co、Ni、Mn、Zn)纳米复合材料,通过一种通用的一锅法合成,这些材料被证明是在苯乙烯环氧化反应中高效的 MRCs。通过 X 射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、红外(IR)和 X 射线光电子能谱(XPS)、热重分析(TGA)和磁性测量进行的表征揭示,纳米复合材料由在聚维酮(PVP)的协助下结晶良好的 Ag 和相应的铁氧体初级粒子组装而成。纳米复合材料样品在比表面积上具有可比性,并且在室温下具有超顺磁性。所制备的 MRCs 在以叔丁基过氧化氢(TBHP)为氧化剂的甲苯中的苯乙烯环氧化反应中表现出高活性,在 5 小时的反应时间内可以实现苯乙烯氧化物的非常高的产率。所有的 MRCs 都可以很容易地通过使用磁铁回收,并且在几个连续的反应循环后,苯乙烯氧化物的产率没有观察到下降。已经证明,铁氧体载体影响 Ag 的结构以及供氧效率,从而影响催化性能。