辽宁石油化工大学学报 ›› 2017, Vol. 37 ›› Issue (1): 8-13.DOI: 10.3969/j.issn.1672??6952.2017.01.002

• 石油化工 • 上一篇    下一篇

UiO-66-NH2 负载Pd催化剂的合成、表征及其催化反应

李 想1,张艳梅2,张 静1,储 刚1,权春善2   

  1. 1.辽宁石油化工大学化学与材料科学学院,辽宁抚顺113001; 2.大连民族大学生命科学学院,辽宁大连116600
  • 收稿日期:2016-04-14 修回日期:2016-05-24 出版日期:2017-02-24 发布日期:2017-03-16
  • 通讯作者: 张静(1980-),女,博士,教授,从事纳米功能材料的表面修饰研究;E-mail:jingzhang_dicp@yahoo.com.cn。
  • 作者简介:李想(1991-),男,硕士研究生,从事纳米材料的合成及应用研究;E-mail:lix1991@126.com。
  • 基金资助:
    国家自然科学基金项目(21203017);国家重点实验室开放基金项目(N-11-03);辽宁省高等学校优秀人才支持计划;中央高校基本研究业务费专项资金资助项目(DC201502020304)。

Synthesis,Characterization and Catalytic Reaction of UiO-66-NH2 Supported Pd Catalyst

  • Received:2016-04-14 Revised:2016-05-24 Published:2017-02-24 Online:2017-03-16

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摘要： 以UiO-66-NH2 纳米粒子为载体,采用浸渍和还原的方法制备了担载Pd纳米粒子的多相双功能催化剂UiO-66-NH2 /Pd。用X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、透射电镜(TEM)、扫描电镜(SEM)等手段对材料进行了表征,并分别以芳香烯烃的催化加氢、苯甲醛和氰基乙酸乙酯的Knoevenagel缩合反应为模型反应,考察了UiO-66-NH2/Pd材料的加氢和碱催化性能。研究结果表明,通过浸渍和还原的方法在UiO-66-NH2  上引入了粒径为1nm 左右的Pd纳米粒子,Pd的质量分数为3.4%,材料的结构未发生明显变化。催化剂UiO-66-NH2/Pd能够高效催化多种烯烃的加氢反应,在苯乙烯的催化加氢反应中,催化剂循环使用6次,转化率大于96%,催化剂结构没有明显变化,催化剂UiO-66-NH2/Pd依然具备很好的碱催化能力,在苯甲醛和氰基乙酸乙酯的Knoevenagel缩合反应中表现出较好的催化活性和循环稳定性。

关键词: UiO-66-NH2, Pd, 催化加氢, Knoevenagel缩合反应, 循环

Abstract:

The heterogeneous bifunctional catalyst UiO-66NH2/Pd with Pd nanoparticles has been prepared on metal-organic framework of UiO-66-NH2 using the impregnation and reduction method. The materials were characterized by X ray diffraction (XRD), Fu Liye transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM) and scanning electron microscopy (SEM). The resulting material of UiO-66-NH2/Pd was further evaluated as a potential bifunctional heterogeneous catalyst for olefine hydrogenations and Knoevenagel condensation between benzaldehyde and ethyl cyanoacetate. The results showed that the weight percent of Pd in UiO-66-NH2/Pd was 3.4% and the average Pd particle size of was about 1 nm. The introduction of Pd nanoparticles did not change the framework integrity of UiO-66-NH2. The resulting bifunctional catalyst of UiO66NH2/Pd was first tested in olefine hydrogenations and the results demonstrated that the material was active and stable as a heterogeneous catalyst. It could be reused for at least 6 times without significant loss of its catalytic performance in styrene hydrogenation. Remarkably, its structure was stable during the reactions. Furthermore, it also showed good activity and recycle stability in Knoevenagel condensation between benzaldehyde and ethyl cyanoacetate.

Key words: UiO-66-NH2, Pd, Hydrogenation, Knoevenagel condensation, Recycle

引用本文

李 想,张艳梅,张 静,储 刚,权春善. UiO-66-NH2 负载Pd催化剂的合成、表征及其催化反应[J]. 辽宁石油化工大学学报, 2017, 37(1): 8-13.

LiXiang,ZhangYanmei,ZhangJing,et al. Synthesis,Characterization and Catalytic Reaction of UiO-66-NH2 Supported Pd Catalyst[J]. Journal of Liaoning Petrochemical University, 2017, 37(1): 8-13.

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