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介孔CeNiO催化剂的合成及其丙烷氧化脱氢制丙烯反应性能
  • 期刊名称:物理化学学报(Acta Phys Chim Sin )
  • 时间:0
  • 页码:2421-2426
  • 语言:中文
  • 分类:O643[理学—物理化学;理学—化学]
  • 作者机构:[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
  • 相关基金: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
  • 相关项目:丙烷选择氧化制丙烯醛反应机理的原位谱学研究
中文摘要:

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℃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℃)催化活性.325℃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.

英文摘要:

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 hydrolysis- controlling 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 adsorption- desorption, transmission electron microscopy (TEM), powder X-ray diffraction (XRD), and H2 temperature- programmed reduction (H2-TPR). The results showed that between 400 and 450 ℃, the NiO and CeNiO catalysts exhibited similar catalytic behavior for the ODP reaction but at low temperatures (〈400 ℃) the catalysts doped with Ce had higher catalytic activity. On NiO only a 3.1% propene yield was obtained at 325℃ while the yield on 5CeNiO (nc/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 mainreason for the higher activities of the catalysts.

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