强静电吸附法制备PdZnx/Al2O3催化1,4-丁炔二醇选择加氢
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大连市科技创新基金(2019J12GX028, 2018RQ09); 2020年中-法“蔡元培”交流合作项目; 中央高校基本科研业务费(DUT21LK02)


PdZnx/Al2O3 catalysts prepared by strong electrostatic adsorption for selective hydrogenation of 1,4-butynediol
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    摘要:

    针对1,4-丁炔二醇选择加氢反应特性,以强静电吸附法可控地制备了一系列Pd、Zn不同物质的量比的PdZnx/Al2O3双金属催化剂,并探究Zn的引入对催化加氢性能的影响。研究发现,少量Zn的添加能够保持催化剂在较高活性的情况下,大幅度改善其对中间产物1,4-丁烯二醇的选择性。其中,PdZn2/Al2O3催化剂表现出较高的催化活性和顺式-1,4-丁烯二醇的选择性。反应在50 ℃,1 MPa的条件下进行,1,4-丁炔二醇在接触时间为6 gcat.·h/mol时的转化率为89%,顺式-1,4-丁烯二醇的选择性可达到85%。结合程序升温还原与X射线电子衍射光谱分析发现前驱体经400 ℃焙烧和400 ℃还原处理后形成了PdZn双金属催化剂。Zn原子的掺入有效调变Pd活性位点的几何效应和电子效应,抑制中间产物的过渡加氢。

    Abstract:

    A series of PdZnx/Al2O3 bimetallic catalysts with different Pd:Zn molar ratios were prepared in a controlled manner by strong electrostatic adsorption for the selective hydrogenation of 1,4-butynediol (BYD), and the effect of Zn introduction on the catalytic hydrogenation was investigated. It was found that the addition of a small amount of Zn was able to maintain the catalyst at a high activity and substantially improve its selectivity for the intermediate cis-1,4-butenediol (cis-BED). The PdZn2/Al2O3 catalyst exhibited high catalytic activity with 89% conversion and selectivity for cis-BED (85%) at 50 °C, 1 MPa H2 pressure, and the contact time of 6 gcat.·h/mol. Combined with temperature-programmed reduction and X-ray photoelectron spectroscopy, it was found that the precursor was calcined at 400 ℃ and reduced at 400 ℃ to form the PdZn bimetallic catalyst. The doping of Zn atoms effectively modulated the geometrical and electronic effects of the Pd active sites, which effectively inhibited the over-hydrogenation of the intermediate products.

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石闯,蒙龙伟,陈霄,吴洁文,范欣悦,梁长海.强静电吸附法制备PdZnx/Al2O3催化1,4-丁炔二醇选择加氢[J].精细化工,2021,38(10):

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  • 收稿日期:2021-03-25
  • 最后修改日期:2021-05-19
  • 录用日期:2021-05-25
  • 在线发布日期: 2021-09-13
  • 出版日期: