氧化羰基化合成碳酸二苯酯纳米催化剂载体的制备及应用  

Synthesis of catalyst support in preparation of diphenyl carbonate with oxidative carbonylation and their application

作　　者：柳鑫华[1] 孙彩云[1] 王庆辉[1] 庞宁波[1] 

机构地区：[1]河北联合大学轻工学院,河北唐山063000

出　　处：《功能材料》2012年第B11期331-334,共4页Journal of Functional Materials

基　　金：河北省自然科学基金资助项目(10215606D);河北省唐山市科技发展计划资助项目(05110301a)

摘　　要：提高氧化羰基化法合成碳酸二苯酯的收率,主要是催化剂的开发,而催化剂的开发关键又是载体及其助催化剂的开发。以柠檬酸、乙酸铜、乙酸钴、乙酸锰和氯化铁的水溶液为原料,采用溶胶-凝胶法和减压干燥工艺制备了(CuO-CoO-MnO)与Fe2O3纳米复合凝胶。采用场发射扫描电镜、电子散射能谱分析和X射线衍射等对纳米复合凝胶的微观结构和组成进行了表征。采用纳米复合凝胶为载体制备了负载型催化剂,用于催化合成碳酸二苯酯(diphenyl carbonate,DPC),并用气相色谱仪对反应液进行了分析。结果表明,催化剂具有更清晰的粒状结构,结晶度高,孔隙率大,能形成纳米级颗粒;催化剂中形成稳定晶相CoFe2O4、CuFeMnO4,减少了助剂流失;催化剂催化合成DPC的质量收率达23.4%。It was important to develop catalyst for improving yield of diphenyl carbonate with oxidative carbonylation. But it was main that catalysts carriers and promoters were developed. （CuO, CoO, MnO） and Fe203 nanocomposite gelatum were prepared by using citric acid aqueous solution of Cu,Co, Mn acetates and chloride ferric via sol gel process and drying under reduced pressure technique. The microstructure and composition of the （CuO,CoO, MnO） and Fe2 03 nanocomposite gelatum were characterized by field emission scanning electron microscopy,transmission electron microscopy, electron dispersive spectroscopy and XRD. Supported catalysts were prepared by using the （CuO,CoO,MnO） and Fe2 03 nanocomposite gelatum as catalyst carriers,and were used in the synthesis of diphenyl carbonate （DPC）. The products were analyzed by gas chromatography. The results show that the （CuO, CoO, MnO） and Fe2 03 nanocomposite gelatum have a clearer acinose structure; hypsi-crystallinity and macro-porosity. Thus nanoscale particles can be formed. The main crystal phase in cata- lyst was CoFe2 04 and CuFeMnO4 ,and the exist of stable crystal phase CoFe2 04 and CuFeMnO4 may contribute to reduce the leaching of active componentand. The yield of DPC was 23.4%.

关 键 词：氧化羰基化 溶胶-凝胶法 催化剂载体 负载型催化剂 制备与表征 

分 类 号：TM285[一般工业技术—材料科学与工程]