化工进展 ›› 2019, Vol. 38 ›› Issue (02): 885-891.DOI: 10.16085/j.issn.1000-6613.2018-1358

• 工业催化 • 上一篇    下一篇

CuO含量对Pd/Al2O3催化剂乙醇氧化性能的影响

张申(),郭玉玉,李星颖,李哲()   

  1. 太原理工大学化学化工学院,山西 太原 030024
  • 收稿日期:2018-07-03 修回日期:2018-09-27 出版日期:2019-02-05 发布日期:2019-02-05
  • 通讯作者: 李哲
  • 作者简介:<named-content content-type="corresp-name">张申</named-content>(1990—),男,博士研究生,研究方向为多相催化。E-mail:<email>zhangshen0472@link.tyut.edu.cn</email>。|李哲,教授,博士生导师,研究方向为多相催化。E-mail:<email>lizhe@tyut.edu.cn</email>。
  • 基金资助:
    国家自然科学基金重点实验室项目(21336006);山西省科技攻关项目(20140313002-2)

Effects of CuO content on the performance of Pd/Al2O3 catalysts in ethanol oxidation

Shen ZHANG(),Yuyu GUO,Xingying LI,Zhe LI()   

  1. College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
  • Received:2018-07-03 Revised:2018-09-27 Online:2019-02-05 Published:2019-02-05
  • Contact: Zhe LI

摘要:

采用浸渍法制备了一系列具有不同CuO含量的Pd-CuO/Al2O3催化剂,并将其用于乙醇氧化反应,其结构与性质通过XRD、H2-TPR和NH3-TPD等手段进行分析。结果发现,催化剂的活性并不是随着CuO含量的增加而增强,Pd-1.0%CuO/Al2O3催化剂表现出最佳的活性,其点火温度和完全转化温度比Pd/Al2O3催化剂至少降低了50℃。与Pd/Al2O3催化剂相比,含CuO催化剂增强的衍射峰强度以及氢化钯分解峰的消失,说明Pd-Cu合金结构的形成有利于Pd、Cu物种之间的协同作用。对于Pd-1.0%CuO/Al2O3催化剂来说,还原峰向低温的移动以及还原峰面积的增大说明该催化剂上氧化性物质更易被还原且数量在增加,这对于氧化反应是十分有利的,新出现的还原峰表示Pd、Cu的相互作用生成了新物种。NH3-TPD结果中更高含量的低温酸有利于高活性,而且新出现的脱附峰说明形成了新的酸性位点。

关键词: CuO含量, Pd-CuO/Al2O3, 醇, 氧化, Pd-Cu合金

Abstract:

A series of Pd/Al2O3-CuO catalysts with different CuO contents were prepared by impregnation method. The catalysts were then used in the ethanol oxidation reaction and their structures and properties were investigated by using XRD, H2-TPR and NH3-TPD techniques. The results showed that the reactivity was not always enhanced with the increase of CuO contents. The Pd-1.0%CuO/Al2O3 catalyst showed the best performance whose T 50 and T 90 decreased more than 50℃ in comparison with Pd/Al2O3. Compared to Pd/Al2O3 catalyst, catalysts with CuO showed an enhancement in diffraction peak intensity but no decomposition of palladium hydride, indicating that the Pd-Cu alloy structure was formed leading to the synergistic effect between Pd and Cu species. For Pd-1.0%CuO/Al2O3, the shift of reduction peak to low temperatures and the increase in area demonstrated the reduction of the oxidizing substances on the catalyst and the amount of them was increased which was beneficial to the oxidation reaction. The new reduction peak illustrated that the interaction between Pd and Cu had produced some new species. NH3-TPD results showed the high content of low temperature acid was conducive to the high reactivity and the new desorption peak indicated that new acidic sites were formed on the Pd-1.0%CuO/Al2O3 catalyst.

Key words: CuO contents, Pd-CuO/Al2O3, alcohol, oxidation, Pd-Cu alloy

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