一锅水热-浸渍法制备Pd-Fe/SiO2催化剂及其蒽醌加氢性能增强

doi:10.16085/j.issn.1000-6613.2016.12.026

化工进展 ›› 2016, Vol. 35 ›› Issue (12): 3913-3918.DOI: 10.16085/j.issn.1000-6613.2016.12.026

一锅水热-浸渍法制备Pd-Fe/SiO₂催化剂及其蒽醌加氢性能增强

卓俊琳¹, 蔡卫权^1,2, 罗晓雷¹

1 武汉理工大学化学化工与生命科学学院, 湖北武汉 430070;
2 武汉理工大学硅酸盐建筑材料国家重点实验室, 湖北武汉 430070

收稿日期:2016-03-24 修回日期:2016-05-24 出版日期:2016-12-05 发布日期:2016-12-05
通讯作者: 蔡卫权,教授,博士,博士生导师。E-mail:caiwq@whut.edu.cn。
作者简介:卓俊琳(1991-),女,硕士研究生。

One-pot hydrothermal-impregnation synthesis of Pd-Fe/SiO₂ catalyst with enhanced catalytic performance towards 2-ethylanthraquinone hydrogenation

ZHUO Junlin¹, CAI Weiquan^1,2, LUO Xiaolei¹

1 School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, Hubei, China;
2 State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, Hubei, China

Received:2016-03-24 Revised:2016-05-24 Online:2016-12-05 Published:2016-12-05

摘要/Abstract

摘要： 以正硅酸乙酯为硅源，Pluronic三嵌段共聚物P123或四丙基氢氧化铵（TPAOH）为结构调节剂，采用一锅温和水热法成功地合成了Fe-修饰的SiO₂；并以其为载体，采用等体积浸渍法制备了负载型0.3% Pd-3% Fe/SiO₂催化剂。采用XRD、N₂吸附-脱附、CO脉冲吸附法、微型浆态床反应器和高效液相色谱对产物的物相结构、织构性质和2-乙基蒽醌加氢性能进行了表征和测试。结果表明，该催化剂具有较规整的孔道、较窄的孔径分布和适中的比表面积；在蒽醌加氢反应中，该催化剂的氢化效率可达13.1g/L、选择性可达66.1%，并且反应4h时的氢化效率仍高达11g/L。相比之下，典型的工业Pd-催化剂反应1.5h后便因副反应过多而无法进行，且氢化效率仅有5.4g/L，选择性仅有26.2%。研究还发现，以P123为结构调节剂时，掺杂Fe可以提高催化剂的选择性；而以TPAOH为结构调节剂时，掺杂Fe可以同时显著地改善催化剂的活性和选择性。

关键词: 过氧化氢, 2-乙基蒽醌, 加氢, Pd-Fe/SiO₂催化剂, Fe-助剂, 选择性

Abstract: Fe-modified SiO₂ were successfully synthesized via a moderate one-pot hydrothermal process using tetraethoxysilane(TEOS)as silicon source,and Pluronic triblock copolymer P123 or tetrapropyl ammonium hydroxide(TPAOH)as structure directing agent. Then supported catalysts of 0.3%Pd -3%Fe/SiO₂ were prepared by incipient impregnation method. The phase structures,texture properties were characterized by XRD,N₂ adsorption-desorption,CO pulse adsorption and the catalytic performance towards hydrogenation of 2-ethylanthraquinone was evaluated in a micro slurry bed reactor. The results showed that the prepared catalysts possess preferably mesoporous structure,structured channel,narrow pore size distribution and medium specific surface area. In the 2-ethylanthraquinone hydrogenation reaction,the prepared catalysts exhibited a high hydrogenation efficiency of 13.1g/L and a high selectivity of 66.1%,and all the catalysts still had an hydrogenation efficiency of 11g/L after 4h. In contrast,industrial catalyst was unable to work after 1.5h due to excessive side reactions,and its hydrogenation efficiency and selectivity were only 5.4g/L and 26.2%, respectively. The study also showed that when P123 was used as the structure directing agent,the doped Fe-could increase the selectivity of the catalyst,and when TPAOH was used as structure directing agent,the doped Fe-can significantly improve both the activity and selectivity of the catalyst.

Key words: hydrogen peroxide, 2-ethylanthraquinone, hydrogenation, Pd-Fe/SiO₂ catalyst, Fe-promoter, selectivity

中图分类号:

TQ426.94

卓俊琳, 蔡卫权, 罗晓雷. 一锅水热-浸渍法制备Pd-Fe/SiO₂催化剂及其蒽醌加氢性能增强[J]. 化工进展, 2016, 35(12): 3913-3918.

ZHUO Junlin, CAI Weiquan, LUO Xiaolei. One-pot hydrothermal-impregnation synthesis of Pd-Fe/SiO₂ catalyst with enhanced catalytic performance towards 2-ethylanthraquinone hydrogenation[J]. Chemical Industry and Engineering Progree, 2016, 35(12): 3913-3918.

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一锅水热-浸渍法制备Pd-Fe/SiO₂催化剂及其蒽醌加氢性能增强

One-pot hydrothermal-impregnation synthesis of Pd-Fe/SiO₂ catalyst with enhanced catalytic performance towards 2-ethylanthraquinone hydrogenation

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