介孔CeNiO催化剂的合成及其丙烷氧化脱氢制丙烯反应性能

引用本文: 汪彩彩, 李建辉, 孙毅飞, 朱晓权, 黄传敬, 翁维正, 万惠霖. 介孔CeNiO催化剂的合成及其丙烷氧化脱氢制丙烯反应性能[J]. 物理化学学报, 2011, 27(10): 2421-2426. doi: 10.3866/PKU.WHXB20110932 shu

Citation: WANG Cai-Cai, LI Jian-Hui, SUN Yi-Fei, ZHU Xiao-Quan, HUANG Chuan-Jing, WENG Wei-Zheng, WAN Hui-Lin. Synthesis and Catalytic Performances of Mesoporous CeNiO Catalysts for the Oxidative Dehydrogenation of Propane to Propene[J]. Acta Physico-Chimica Sinica, 2011, 27(10): 2421-2426. doi: 10.3866/PKU.WHXB20110932 shu

介孔CeNiO催化剂的合成及其丙烷氧化脱氢制丙烯反应性能

基金项目:
国家重点基础研究发展规划项目(973) (2010CB732300) (973) (2010CB732300)

国家自然科学基金(21073148, 21033006, 20803060) (21073148, 21033006, 20803060)

福建省自然科学基金(2009J01038)资助 (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(n_Ce/n_Ni=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:

English

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

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 Date: 02 June 2011
Available Online: 27 September 2011
Fund Project:
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)

福建省自然科学基金(2009J01038)资助

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 (n_Ce/n_Ni=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:

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沈阳化工大学材料科学与工程学院沈阳 110142

介孔CeNiO催化剂的合成及其丙烷氧化脱氢制丙烯反应性能

English

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

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

介孔CeNiO催化剂的合成及其丙烷氧化脱氢制丙烯反应性能

English

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

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

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