Fe柱撑海泡石负载Cu催化剂:结构特点及其C3H6选择性催化还原NO催化性质
Cu-Supported on Fe-Pillared Sepiolite: Characterization and Selective Catalytic Reduction (SCR) of NO by Propene
作者单位
叶 青 北京工业大学环境与能源工程学院环境科学系北京 100124 
闫立娜 北京工业大学环境与能源工程学院环境科学系北京 100124 
霍飞飞 北京工业大学环境与能源工程学院环境科学系北京 100124 
王海平 北京工业大学环境与能源工程学院环境科学系北京 100124 
程水源 北京工业大学环境与能源工程学院环境科学系北京 100124 
康天放 北京工业大学环境与能源工程学院环境科学系北京 100124 
摘要: 通过羟基铁离子柱撑将海泡石(Sep)改性成Fe柱撑海泡石(Fe-PILSEP),使用浸渍法(IM)将Cu负载在Fe-PILSEP上,制得不同铜含量的xCu/Fe-PILSEP催化剂。通过X射线衍射(XRD)、N2-吸附/脱附、H2-程序升温还原(TPR)和X射线光电子能谱(XPS)等对样品进行表征,并测定其对丙烯选择性催化还原NO的催化活性。N2-吸附/脱附和TGA结果表明,Fe-PILSEP的比表面积和孔体积较海泡石原矿Sep极大地增加,热稳定性也明显优于Sep。XRD和XPS结果表明,在xCu/Fe-PILSEP催化剂上同时存在Fe3+/Fe2+和Cu2+/Cu+不同氧化态的氧化物,而且Fe与海泡石之间存在相互作用,Fe和Cu之间存在电子迁移。H2-TPR结果表明,xCu/Fe-PILSEP催化剂上存在不同聚集状态的氧化铜物种。xCu/Fe-PILSEP催化剂的丙烯选择性催化还原NO的催化活性明显优于Fe-PILSEP催化剂,这可能与Fe和Cu的氧化还原性有关。xCu/Fe-PILSEP的催化活性与Cu负载量相关,其中10Cu/Fe-PILSEP催化剂显示出最高的活性,这与其高的比表面积、孔体积和氧化还原性能,及其具有更多有利于HC-SCR反应的孤立Cu2+((Cu2+)i)物种有关。
关键词: Fe柱撑海泡石  Cu  C3H6选择性催化还原NO
基金项目: 
Abstract: Fe pillared sepiolite (Fe-PILSEP) was prepared by the intercalation of polymerization of iron hydroxyl ions with sepiolite and then calcining at 450 ℃. Cu supported on Fe-PILSEP catalysts (xCu/Fe-PILSEP (x=5, 10, 15, 20wt%)) with different copper loadings were prepared by impregnation method. xCu/Fe-PILSEP were characterized by X-ray diffraction (XRD), X-ray fluorescence spectrometry (XRF), 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 propene were also studied. The results of N2-desorption/adsorption and TGA show that due to pillaring, there is a distinctively increase of Fe-PILSEP in surface area, pore volume and thermal stability. XRD and XPS results verify that Fe2+/Fe3+ and Cu+/Cu2+ are co-existed, respectively, over xCu/Fe-PILSEP catalyst and there is some strong interaction among Cu, Fe and sepiolite support. H2-TPR results show that there are isolated Cu2+ and oxygenated clusters CuO species and the amount of latter increases with copper loading. The xCu/Fe-PILSEP samples display significant activity in the NO reduction with a maximum for a Cu content close to 10wt%. A decay of catalytic activity is observed with the increase of copper loading, due to the increase of oxygenated clusters CuO species.
Keywords: Fe-pillared sepiolite  Cu  selective catalytic reduction of NO by C3H6
 
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叶 青,闫立娜,霍飞飞,王海平,程水源,康天放.Fe柱撑海泡石负载Cu催化剂:结构特点及其C3H6选择性催化还原NO催化性质[J].无机化学学报,2012,28(1):103-112.
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