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化学学报
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化学学报 ›› 2011, Vol. 69 ›› Issue (13): 1524-1532. 上一篇    下一篇

研究论文

Cu负载Fe柱撑钠化海泡石: 结构特点及其丙烯选择性催化还原NO性质研究

叶青*, 闫立娜, 霍飞飞, 王海平, 程水源, 康天放   

  1. (北京工业大学环境与能源工程学院环境科学系 北京 100124)
  • 投稿日期:2010-11-22 修回日期:2011-01-13 发布日期:2011-03-03
  • 通讯作者: 叶青 E-mail:yeqing@bjut.edu.cn
  • 基金资助:

    新型OMS双功能催化体系低温净化VOCs研究;新型双功能“复合OMS”低温催化净化VOCs;基于低温催化净化VOCs双功能OMS的研究

Copper Impregnated Fe-pillared Sodium-treated Sepiolite (Fe-NaPILCS) for Selective Catalytic Reduction of NO with C3H6

YE Qing, YAN Li-Na, HUO Fei-Fei, WANG Hai-Ping, CHENG Shui-Yuan, KANG Tian-Fang   

  1. (Department of Environmental Science, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124)
  • Received:2010-11-22 Revised:2011-01-13 Published:2011-03-03
  • Contact: Qing Ye E-mail:yeqing@bjut.edu.cn

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1055

被引次数

12

采用羟基铁离子柱撑钠化海泡石改性后, 以浸渍法制备了铜负载铁柱撑钠化海泡石Cu/Fe-NaPILCS催化剂, 作为比较以浸渍法制备了铁负载钠化海泡石(Fe-NaSep), 铜负载钠化海泡石(Cu-NaSep)和铜铁负载钠化海泡石(Cu/Fe-NaSep)催化剂. 并将它们应用于C3H6选择性催化还原NO的反应(C3H6-SCR). 通过X射线衍射仪(XRD)、TGA-DTG分析、N2-等温吸附/脱附、H2-程序升温还原(TPR)和X射线光电子能谱仪(XPS)等技术对样品进行表征. N2-等温吸附/脱附和TGA-DTG分析结果表明, Fe-NaPILCS的比表面积和孔体积较海泡石原矿具有较大的增加, 热稳定性也明显提高|XRD和XPS结果表明, 在Cu/Fe-NaPILCS催化剂上同时存在Fe3＋/Fe2＋和Cu2＋/Cu＋不同氧化态的氧化物种, 在Cu和Fe之间存在电子迁移. H2-TPR结果表明, Cu/Fe-NaPILCS催化剂上存在大量的孤立铜离子物种(isolated Cu2＋-ions, (Cu2＋)i). Fe柱撑钠化海泡石负载的Cu/Fe-NaPILCS催化剂的催化活性明显优于未柱撑海泡石负载的Cu/Fe-NaSep催化剂, 这可能与Cu/Fe-NaPILCS具有较大的比表面积、孔体积和更优的氧化还原性能, 及其具有更多有利于C3H6-SCR反应的(Cu2＋)i物种有关.

关键词: Cu/Fe-NaPILCS, 氮氧化物, 丙烯, 选择性催化还原

Fe pillared sodium-modified sepiolite (Fe-NaPILCS) was prepared by intercalation polymerization of iron hydroxyl ions with sodium-treated sepiolite and then calcined at 450 ℃ for 4 h. Cu/Fe-NaPILCS and Cu/Fe-NaSep were prepared by impregnation of Fe-NaPILCS and Fe-NaSep, respectively, with an aqueous solution of Cu-nitrate. These samples were characterized by means of X-ray diffraction (XRD), TGA-DTG, N2-sorption analysis, H2-temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS) techniques and their catalytic performance for the selective catalytic reduction (SCR) of NO by C3H6 were also studied. The results of N2-desorption/adsorption and TGA-DTG showed that due to pillaring, Fe-NaPILCS revealed much higher surface area, pore volume and thermal stability than that of Sep. According to the result of XRD and XPS, there co-exist Fe3＋/Fe2＋ and Cu2＋/Cu＋ and also the strong interaction among Cu, Fe and support over Cu/Fe-NaPILCS and Cu/Fe-NaSep catalysts. H2-TPR showed that Cu/Fe-NaPILCS possessed high amount of isolated Cu2＋ species. Cu/Fe-NaPILCS display more significant activity for selective reduction of NO with C3H6 than that of Cu/Fe-NaSep. This maybe related to its higher surface area, pore volume, better catalytic reduction performance and high amount of isolated Cu2＋ species.

Key words: Cu/Fe-NaPILCS, nitric oxides, propylene, selective catalytic reduction

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