物理化学学报 >> 2011, Vol. 27 >> Issue (10): 2421-2426.doi: 10.3866/PKU.WHXB20110932

催化和表面科学 上一篇    下一篇

介孔CeNiO催化剂的合成及其丙烷氧化脱氢制丙烯反应性能

汪彩彩, 李建辉, 孙毅飞, 朱晓权, 黄传敬, 翁维正, 万惠霖   

  1. 厦门大学化学化工学院化学系, 固体表面物理化学国家重点实验室, 醇醚酯化工清洁生产国家工程实验室, 福建厦门 361005
  • 收稿日期:2011-06-02 修回日期:2011-07-07 发布日期:2011-09-27
  • 通讯作者: 黄传敬, 万惠霖 E-mail:huangcj@xmu.edu.cn; hlwan@xmu.edu.cn
  • 基金资助:

    国家重点基础研究发展规划项目(973) (2010CB732300), 国家自然科学基金(21073148, 21033006, 20803060)和福建省自然科学基金(2009J01038)资助

Synthesis and Catalytic Performances of Mesoporous CeNiO Catalysts for the Oxidative Dehydrogenation of Propane to Propene

WANG Cai-Cai, LI Jian-Hui, SUN Yi-Fei, ZHU Xiao-Quan, HUANG Chuan-Jing, WENG Wei-Zheng, WAN Hui-Lin   

  1. State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China
  • Received:2011-06-02 Revised:2011-07-07 Published:2011-09-27
  • Contact: HUANG Chuan-Jing, WAN Hui-Lin E-mail:huangcj@xmu.edu.cn; hlwan@xmu.edu.cn
  • Supported by:

    The project was supported by the National Key Basic Research Program of China (973) (2010CB732300), National Natural Science Foundation of China (21073148, 21033006, 20803060), and Natural Science Foundation of Fujian Province, China (2009J01038).

摘要: 以十二烷基硫酸钠(SDS)和三嵌段共聚物P123为混合模板剂, 尿素为沉淀剂, 采用均匀沉淀法制备了具有介孔结构的NiO 和CeNiO催化剂. 考察了催化剂的丙烷氧化脱氢反应性能, 并利用N2吸附-脱附、透射电镜(TEM)、X射线粉末衍射(XRD)和H2程序升温还原(H2-TPR)等技术对催化剂进行了表征. 活性测试结果表明,在400-450°C范围内NiO 和CeNiO 催化剂有相似的催化性能, 但后者表现出较高的低温(<400°C)催化活性. 325°C反应时, 纯NiO上丙烯收率仅为3.1%, 而5CeNiO(nCe/nNi=5%)催化剂上丙烯收率高达12.2%. N2吸附-脱附和TEM结果表明, 制备的NiO 和CeNiO催化剂均有较大的比表面积且具有虫孔状介孔结构. H2-TPR结果表明, CeNiO催化剂中由于Ce的存在使得一部分氧物种的可还原性能明显增强, 这可能是该催化剂具有较高催化活性的重要原因.

关键词: 丙烷, 氧化脱氢, 丙烯, 介孔CeNiO催化剂

Abstract: Mesoporous NiO and CeNiO catalysts were prepared by homogeneous precipitation using sodium dodecyl sulfate (SDS) mixed with triblock copolymer P123 as a template and urea as a hydrolysiscontrolling agent. The prepared catalysts were evaluated for the oxidative dehydrogenation of propane (ODP) to propene and the structure and properties of the catalysts were characterized by N2 adsorptiondesorption, transmission electron microscopy (TEM), powder X-ray diffraction (XRD), and H2 temperatureprogrammed reduction (H2-TPR). The results showed that between 400 and 450°C, the NiO and CeNiO catalysts exhibited similar catalytic behavior for the ODP reaction but at low temperatures (<400°C) the catalysts doped with Ce had higher catalytic activity. On NiO only a 3.1% propene yield was obtained at 325°C while the yield on 5CeNiO (nCe/nNi=5%) was as high as 12.2% at the same temperature. The results of N2 adsorption-desorption and TEM indicated that both the prepared NiO and CeNiO catalysts possessed a high surface area and a wormhole-like mesostructure. The H2-TPR results revealed that part of the oxygen species became more reducible because of the presence of Ce in CeNiO, which may be the main reason for the higher activities of the catalysts.

Key words: Propane, Oxidative dehydrogenation, Propene, Mesoporous CeNiO catalyst

MSC2000: 

  • O643