Zr-SBA-15催化肉桂醛MPV转移加氢性能
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国家自然科学基金项目(面上项目,重点项目,重大项目)


MPV Transfer Hydrogenation Performance of Cinnamaldehyde over Zr-SBA-15 Catalyst
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The National Natural Science Foundation of China (General Program, Key Program, Major Research Plan)

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    摘要:

    以正硅酸乙酯和硝酸氧锆为原料,采用一锅法制备了不同Zr/Si物质的量比的Zr-SBA-15催化剂,借助N2物理吸附、X射线粉末衍射、NH3-程序升温脱附、吡啶-原位红外等考察了Zr/Si物质的量比对Zr-SBA-15结构、织构、表面酸性质及催化肉桂醛Meerwein-Ponndorf-Verley(MPV)转移加氢性能的影响;结合催化剂表征与催化肉桂醛MPV转移加氢性能评价结果,探讨了Zr-SBA-15结构、织构及表面酸性质对其催化肉桂醛MPV转移加氢性能的影响机制。结果表明,所制备的Zr-SBA-15催化剂均呈现规整的六方介孔结构特征,表面酸中心以L酸为主。随Zr/Si物质的量比增加,Zr-SBA-15催化剂的最可几孔径逐渐减小,L酸量持续增加,B酸量变化不大,肉桂醛转化率呈现先增加后趋于稳定的趋势,目标产物肉桂醇选择性增加,副产物1-苯丙烯-2-丙基醚选择性下降。在Zr/Si物质的量比为0.1时,Zr-SBA-15催化剂显示最优的催化性能,肉桂醛转化率为96.2 %,目标产物肉桂醇选择性达到95.2 %,经7次循环后催化剂仍保持90%以上的肉桂醛转化率和95%以上的肉桂醇选择性。

    Abstract:

    The Zr-SBA-15 catalysts with different Zr/Si ratio were prepared by one pot method using te-traethoxysilane and zirconium dinitrate oxide as precursors. The effects of Zr/Si ratio on the structure, tex-ture, surface acidity and catalytic performance of Zr-SBA-15 catalysts for the (Meerwein-Ponndorf-Verley) MPV transfer hydrogenation of cinnamaldehyde were investigated, by means of N2 physical adsorption, X-ray powder diffraction, NH3 temperature-programmed desorption and pyridine in situ infrared. The re-sults show that the prepared Zr-SBA-15 catalysts exhibited regular hexagonal mesoporous structure with L acid as the main surface acid center. With the increase of Zr/Si mole ratio, the most probable pore size of Zr-SBA-15 catalyst decreased gradually, the amount of L acid increased continuously, and the amount of B acid changed lightly. The cinnamaldehyde conversion increased first and then tended to be stable. The selectivity of the target product cinnamol increased, while selectivity of the by-product 1- benzene propyl-ene-2-propyl ether decreased. When the Zr/Si mole ratio was 0.1, the Zr-SBA-15 catalyst showed the op-timal catalytic performance: the conversion of cinnamaldehyde reached 96.2%, and the selectivity of cin-namyl alcohol was 95.2%. The conversion of cinnamaldehyde kept over 90%, and the selectivity of cin-namyl alcohol was above 95% after 8 times cycle application experiment.

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盖媛媛,李建法,孙瑞霞,李海涛. Zr-SBA-15催化肉桂醛MPV转移加氢性能[J].精细化工,2019,36(5):

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  • 收稿日期:2018-08-14
  • 最后修改日期:2018-12-27
  • 录用日期:2018-12-28
  • 在线发布日期: 2019-03-28
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