酸碱双功能MgO/HMCM-22催化剂上Knoevenagel缩合反应

doi:10.1016/S1872-2067(11)60493-2

催化学报 ›› 2013, Vol. 34 ›› Issue (3): 559-566.DOI: 10.1016/S1872-2067(11)60493-2

酸碱双功能MgO/HMCM-22催化剂上Knoevenagel缩合反应

张文飞^a, 梁金花^b, 刘艳秋^a, 孙守飞^a, 任晓乾^a, 姜岷^b

a 南京工业大学化学化工学院, 江苏南京 210009;
b 南京工业大学生物与制药工程学院, 江苏南京 210009

收稿日期:2012-09-30 修回日期:2012-11-26 出版日期:2013-04-02 发布日期:2013-04-03
通讯作者: 任晓乾
基金资助:
国家重点基础研究发展计划(973计划, 2009CB724701); 国家高技术研究发展计划(863计划, 2011AA02A203); 江苏省博士后科研资助计划(1001016C).

Knoevenagel condensation reaction over acid-base bifunctional MgO/HMCM-22 catalysts

ZHANG Wenfei^a, LIANG Jinhua^b, LIU Yanqiu^a, SUN Shoufei^a, REN Xiaoqian^a, JIANG Min^b

a College of Chemistry and Chemical Engineering, Nanjing University of Technology, Nanjing 210009, Jiangsu, China;
b College of Biotechnology and Pharmaceutical Engineering, Nanjing University of Technology, Nanjing 210009, Jiangsu, China

Received:2012-09-30 Revised:2012-11-26 Online:2013-04-02 Published:2013-04-03
Supported by:
This work was supported by the National Basic Research Program of China (973 Program, 2009CB724701), the National High Technology Research and Development Program of China (863 Program, 2011AA02A203), and the Jiangsu Planned Projects for Postdoctoral Research Funds (1001016C).

摘要/Abstract

摘要：

采用浸渍法制备了一系列MgO改性催化剂MgO/HMCM-22, 利用X射线衍射、N₂物理吸附-脱附、扫描电镜、傅里叶变换红外光谱、NH₃及CO₂程序升温脱附等技术对所制催化剂进行了表征. 结果表明, MgO改性后MCM-22分子筛仍保持原有的结构; 随着MgO负载量的增加, 催化剂的碱强度和碱含量显著增加, 而强酸含量明显减少, 弱酸酸位有所增加. 以Knoevenagel缩合为探针反应, 考察了所制催化剂的性能. 在优化的反应条件下, MgO/HMCM-22上苯甲醛转化率高达92.6%. 催化剂 MgO/HMCM-22和MgO/NaMCM-22的催化性能明显优于HMCM-22和MgO. 酸中心和碱中心均对该缩合反应起着重要的促进作用. MgO/HMCM-22对Knoevenagel缩合反应显示出较高的催化活性, 体现出明显的酸碱协同催化作用.

关键词: MCM-22分子筛, 氧化镁, 浸渍, 酸碱双功能, Knoevenagel缩合反应

Abstract:

MgO/HMCM-22 catalysts were prepared by impregnation and characterized by X-ray diffraction, N₂ physical adsorption-desorption, scanning electron microscopy, Fourier-transform infrared spectroscopy, temperature-programmed desorption of NH₃, and temperature-programmed desorption of CO₂. The results show that there were no significant structural changes in theMCM-22 zeolite after modification. Increasing the MgO loading increased the strength and content of the base, whereas the strength of the strong acid decreased significantly and the amount of weak acidic sites increased slightly. Knoevenagel condensation reactions were carried out as the probe reactions over the catalysts. Both acidic sites and basic sites significantly promoted the reaction. The conversion of benzaldehyde reached 92.6% under the optimal conditions. The catalytic performance of MgO/HMCM-22 and MgO/NaMCM-22 was better than that of HMCM-22 and MgO. The MgO/HMCM-22 catalysts gave good catalytic performance for Knoevenagel condensation reactions and exhibited obvious acid-base synergetic effects.

Key words: MCM-22 zeolite, Magnesium oxide, Impregnation, Acid-base bifunction, Knoevenagel condensation reaction

张文飞, 梁金花, 刘艳秋, 孙守飞, 任晓乾, 姜岷. 酸碱双功能MgO/HMCM-22催化剂上Knoevenagel缩合反应[J]. 催化学报, 2013, 34(3): 559-566.

ZHANG Wenfei, LIANG Jinhua, LIU Yanqiu, SUN Shoufei, REN Xiaoqian, JIANG Min. Knoevenagel condensation reaction over acid-base bifunctional MgO/HMCM-22 catalysts[J]. Chinese Journal of Catalysis, 2013, 34(3): 559-566.

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酸碱双功能MgO/HMCM-22催化剂上Knoevenagel缩合反应

Knoevenagel condensation reaction over acid-base bifunctional MgO/HMCM-22 catalysts

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