复合氧化物的设计合成及其NH3-SCR催化性能研究

doi:10.15541/jim20150100

摘要/Abstract

摘要：

以两种表面活性剂Brij-35和P123作为介孔结构造孔剂, 通过水热晶化法, 制备多种活性组分V₂O₅、WO₃、CuO和Al₂O₃共负载的ZrO₂-TiO₂(ZT)基介孔复合氧化物催化剂V₂O₅-WO₃-CuO-Al₂O₃/ ZrO₂-TiO₂(简称VWCuAl/ZT)。研究结果表明, 活性组分均匀分散于介孔载体中, 该复合催化材料针对NO的NH₃-SCR催化反应中, 相比于浸渍法制备的非介孔I-VWCuAl/ZT和商用催化剂V₂O₅-WO₃/TiO₂(V-W/Ti)表现出优异的低温催化活性和稳定性, 可以在较宽温度范围(200℃~500℃)内实现NO的高效催化还原。

关键词: 水热晶化, 介孔ZrO2-TiO2, VWCuAl/ZT, NH3-SCR, NO

Abstract:

A novel mesoporous ZrO₂-TiO₂ (ZT) based multi-component composite oxide catalyst V₂O₅-WO₃-CuO- Al₂O₃/ZrO₂-TiO₂ (VWCuAl/ZT) was successfully synthesized by one-pot hydrothermal method using both Brij-35 and P123 as composite template. The results indicated that the active species of V₂O₅, WO₃, CuO and Al₂O₃ could be homogeneously dispersed into mesoporous ZrO₂-TiO₂ catalyst carrier. Compared with the reference samples of non-mesoporous I-VWCuAl/ZT and the traditional commercial catalyst V₂O₅-WO₃/TiO₂(V-W/Ti), the prepared VWCuAl/ZT showed a superior low-temperature catalytic activity and high stability over the reaction of NH₃-SCR of NO, especially high catalytic efficacy for NO reduction within a wide temperature range of between 200℃ to 500℃.

Key words: hydrothermal, mesoporous ZrO2-TiO2, VWCuAl/ZT, NH3-SCR, NO

中图分类号:

TQ174

陈英, 周晓霞, 王进, 谢治国, 陈航榕. 复合氧化物的设计合成及其NH₃-SCR催化性能研究[J]. 无机材料学报, 2015, 30(11): 1155-1160.

CHEN Ying, ZHOU Xiao-Xia, WANG Jin, XIE Zhi-Guo, CHEN Hang-Rong. Synthesis of Mesoporous Composite Oxides for the Catalysis of NH₃-SCR[J]. Journal of Inorganic Materials, 2015, 30(11): 1155-1160.

图/表 8

图1 不同催化剂样品及载体ZT的N2吸附-脱附曲线

Fig. 1 N2 adsorption/desorption isotherms of different catalysts and catalyst support ZT

表1 不同催化剂样品及载体ZT的孔结构参数

Table 1 Texture properties of different catalysts and catalyst support ZT

Sample	ZT	VWCuAl/ZT	I-VWCuAl/ZT
S_BET/(m²•g^-1)	99	102	42
Pore size /nm	35.8	14.9	-
V_total/(cm³•g^-1)	0.71	0.36	-

图2 介孔ZT载体与催化剂VWCuAl/ZT的XRD图谱

Fig. 2 XRD patterns of mesoporous ZT support and VWCuAl/ ZT catalyst

图3 (a)介孔ZT载体典型的TEM照片以及相应的SAED图片(插图); (b)催化剂VWCuAl/ZT典型的TEM照片以及相应的SAED图片(插图); (c)对应图(b)的VWCuAl/ZT的EDS图谱及元素含量

Fig. 3 Typical TEM images and the corresponding selected area electron diffraction (SAED) pattern (inset) of mesoporous ZT support (a) and VWCuAl/ZT catalyst (b), and EDS spectrum (c) corresponding to (b) as well as elements weight percentage of VWCuAl/ZT (inset)

图4 催化剂VWCuAl/ZT典型的(a) SEM照片和(b) STEM照片及其相应的元素分布图(c)

Fig. 4 (a) SEM image, (b) STEM image and (c) corresponding elements mapping of VWCuAl/ZT catalyst

图5 催化剂VWCuAl/ZT和商用催化剂(V-W/Ti)的H2-TPR图谱

Fig. 5 H2-TPR profiles of the prepared VWCuAl/ZT and commercial catalysts

图6 商用催化剂以及催化剂VWCuAl/ZT和I-VWCuAl/ZT的催化活性比较

Fig. 6 Comparison of NO conversion over the VWCuAl/ ZT, references commercial catalyst and I-VWCuAl/ZT catalyst

图7 样品VWCuAl/ZT的重复使用性能

Fig. 7 Reusability of the sample VWCuAl/ZT

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复合氧化物的设计合成及其NH₃-SCR催化性能研究

Synthesis of Mesoporous Composite Oxides for the Catalysis of NH₃-SCR

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