SCI和EI收录∣中国化工学会会刊

›› 2014, Vol. 22 ›› Issue (10): 1098-1104.DOI: 10.1016/j.cjche.2014.08.002

• 催化、动力学与反应工程 • 上一篇    下一篇

MgO-SBA-15 Supported Pd-Pb Catalysts for Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate

Li Jiang1,2, Yanyan Diao1, Junxing Han1, Ruiyi Yan1, Xiangping Zhang1, Suojiang Zhang1   

  1. 1 Key Laboratory of Green Process and Engineering, Beijing Key Laboratory of Ionic Liquids Clean Process, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
    2 University of Chinese Academy of Sciences, Beijing 100049, China
  • 收稿日期:2013-02-26 修回日期:2013-05-07 出版日期:2014-10-28 发布日期:2014-12-01
  • 通讯作者: Xiangping Zhang, Suojiang Zhang
  • 基金资助:
    Supported by the Key Program of the National Natural Science Foundation of China (21036007) and the National High-Tech Project of China (2012AA062903).

MgO-SBA-15 Supported Pd-Pb Catalysts for Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate

Li Jiang1,2, Yanyan Diao1, Junxing Han1, Ruiyi Yan1, Xiangping Zhang1, Suojiang Zhang1   

  1. 1 Key Laboratory of Green Process and Engineering, Beijing Key Laboratory of Ionic Liquids Clean Process, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
    2 University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2013-02-26 Revised:2013-05-07 Online:2014-10-28 Published:2014-12-01
  • Supported by:
    Supported by the Key Program of the National Natural Science Foundation of China (21036007) and the National High-Tech Project of China (2012AA062903).

摘要: Novel MgO-SBA-15 supported catalysts were prepared for oxidative esterification of methacrolein (MAL) with methanol to methyl methacrylate (MMA). The MgO-SBA-15 supports were synthesized with different magnesia loadings fromdifferentmagnesiumprecursors and hydrochloric acidmolar concentrations. The MgO-SBA-15 supports and Pd-Pb/MgO-SBA-15 catalysts were characterized by several analysismethods. The results revealed that the addition ofMgO improved the ordered structure of SBA-15 supports and provided surface alkalinity of SBA-15 supports. The average size of the Pd3Pb particles onmagnesia-modified Pd-Pb/MgO-SBA-15 catalystswas smaller than that on the pure silica-based Pd-Pb/SBA-15 catalysts. The experiments on catalyst performance showed that the magnesia-modified Pd-Pb/MgO-SBA-15 catalysts had higher activity than pure silica-based Pd-Pb/SBA-15 catalysts, showing the strong dependence of catalytic activity on the average size of active particles. The difference of activity between Pd-Pb/SBA-15 catalysts and Pd-Pb/MgO-SBA-15 catalystswas due to the discrepant structural properties and surface alkalinity provided by MgO, which led to the different Pd3Pb particle sizes and then resulted in the different number of active sites. Besides magnesia loadings, other factors, such as hydrochloric acid molar concentration and magnesium precursors, had considerable influences on the catalytic activity.

关键词: Methacrolein, Methyl methacrylate, Oxidative esterification, Pd-Pb bimetal, SBA-15

Abstract: Novel MgO-SBA-15 supported catalysts were prepared for oxidative esterification of methacrolein (MAL) with methanol to methyl methacrylate (MMA). The MgO-SBA-15 supports were synthesized with different magnesia loadings fromdifferentmagnesiumprecursors and hydrochloric acidmolar concentrations. The MgO-SBA-15 supports and Pd-Pb/MgO-SBA-15 catalysts were characterized by several analysismethods. The results revealed that the addition ofMgO improved the ordered structure of SBA-15 supports and provided surface alkalinity of SBA-15 supports. The average size of the Pd3Pb particles onmagnesia-modified Pd-Pb/MgO-SBA-15 catalystswas smaller than that on the pure silica-based Pd-Pb/SBA-15 catalysts. The experiments on catalyst performance showed that the magnesia-modified Pd-Pb/MgO-SBA-15 catalysts had higher activity than pure silica-based Pd-Pb/SBA-15 catalysts, showing the strong dependence of catalytic activity on the average size of active particles. The difference of activity between Pd-Pb/SBA-15 catalysts and Pd-Pb/MgO-SBA-15 catalystswas due to the discrepant structural properties and surface alkalinity provided by MgO, which led to the different Pd3Pb particle sizes and then resulted in the different number of active sites. Besides magnesia loadings, other factors, such as hydrochloric acid molar concentration and magnesium precursors, had considerable influences on the catalytic activity.

Key words: Methacrolein, Methyl methacrylate, Oxidative esterification, Pd-Pb bimetal, SBA-15