MnOx/Al-SBA-15的结构性质及低温NH3选择性催化还原NOx

doi:10.3866/PKU.WHXB201210094

物理化学学报 >> 2013, Vol. 29 >> Issue (01): 176-182.doi: 10.3866/PKU.WHXB201210094

MnO_x/Al-SBA-15的结构性质及低温NH₃选择性催化还原NO_x

黄萍¹, 盘思伟², 黄碧纯^1,3, 程华¹, 叶代启^1,3, 吴军良^1,3, 付名利^1,3, 卢圣良⁴

1 华南理工大学环境科学与工程学院, 广州 510006;
2 广东电网公司电力科学研究院, 广州 510080;
3 广东省大气环境与污染控制重点实验室, 广州 510006;
4 广州环保投资有限公司, 广州 510700

收稿日期:2012-08-13 修回日期:2012-10-08 发布日期:2012-12-14
通讯作者: 黄碧纯 E-mail:cebhuang@scut.edu.cn
基金资助:
广州市重大科技专项计划(X2DLB2080501)资助项目

Structural Properties of MnO_x/Al-SBA-15 in Low-Temperature Selective Catalytic Reduction of NO_x with NH₃

HUANG Ping¹, PAN Si-Wei², HUANG Bi-Chun^1,3, CHENG Hua¹, YE Dai-Qi^1,3, WU Jun-Liang^1,3, FU Ming-Li^1,3, LU Sheng-Liang⁴

1 College of Environmental Science & Engineering, South China University of Technology, Guangzhou 510006, P. R. China;
2 Electric Power Research Institute of Guangdong Power Grid Corporation, P. R. China;
3 Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, Guangzhou 510006, P. R. China;
4 Guangzhou Environment Protection Investment Co. Ltd., Guangzhou 510700, P. R. China

Received:2012-08-13 Revised:2012-10-08 Published:2012-12-14
Supported by:
The project was supported by the Significant Technology Special Plan Project of Guangzhou, China (X2DLB2080501).

摘要/Abstract

摘要：

采用后合成法制备MnO_x/Al-SBA-15催化剂, 考察了催化剂的低温NH₃选择性催化还原(SCR)NO_x的性能. 利用傅里叶透射红外变换(FTIR)光谱、N₂吸附-脱附、X射线衍射(XRD)、扫描电镜(SEM)、拉曼光谱(Raman)、X射线光电子能谱(XPS)及NH₃程序升温脱附(NH₃-TPD)的表征手段, 对催化剂的结构性质和SCR性能进行了系统分析. 结果表明, 适量Al的掺杂能提高MnO_x/SBA-15催化剂的SCR活性, 当硅铝摩尔比为50时, 催化剂活性最佳. 表征结果显示, Al掺杂后, 催化剂仍保持良好的骨架结构, 较大比表面、孔容和孔径, 并且Mn在催化剂表面富集, 由低价态转化为高价态, MnO₂为催化剂的主要活性相. 此外, Al的掺杂使MnO_x在催化剂表面高度分散, 表面酸性增强, 从而提高了催化剂的SCR活性.

关键词: 乙酰丙酮锰, 铝, SBA-15, 高分散性, 表面酸性, 选择性催化还原

Abstract:

A series of MnO_x/Al-SBA-15 catalysts were prepared by post synthesis methods for lowtemperature selective catalytic reduction (SCR) of NO_x with NH₃. Structural properties and catalytic performance were comprehensively characterized by Fourier transform infrared (FTIR) spectroscopy, N₂ adsorption-desorption, X-ray powder diffraction (XRD), scanning electron microscopy (SEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and temperature programmed desorption of NH₃ (NH₃-TPD). The results showed that moderate addition of Al improved the SCR activity of the MnO_x/SBA-15 catalyst, and the MnO_x/Al-SBA-15 catalyst with n_Si/n_Al=50 had the highest activity. Characterization results revealed that the doped material MnO_x/Al-SBA-15 catalysts maintained high specific surface area, large pore volume, and uniform pore size. Al doping improved the concentration and valence state of Mn, where MnO₂ was determined to be the main active phase. Owing to a high dispersion of MnO_x and a stronger surface acidity, the MnO_x/Al(50)-SBA-15 catalyst exhibited higher SCR activity.

Key words: Acetyl acetone manganese, Aluminum, SBA-15, High dispersion, Surface acidity, Selective catalytic reduction

黄萍, 盘思伟, 黄碧纯, 程华, 叶代启, 吴军良, 付名利, 卢圣良. MnO_x/Al-SBA-15的结构性质及低温NH₃选择性催化还原NO_x[J]. 物理化学学报, 2013, 29(01), 176-182. doi: 10.3866/PKU.WHXB201210094

HUANG Ping, PAN Si-Wei, HUANG Bi-Chun, CHENG Hua, YE Dai-Qi, WU Jun-Liang, FU Ming-Li, LU Sheng-Liang. Structural Properties of MnO_x/Al-SBA-15 in Low-Temperature Selective Catalytic Reduction of NO_x with NH₃[J]. Acta Phys. -Chim. Sin. 2013, 29(01), 176-182. doi: 10.3866/PKU.WHXB201210094

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201210094

https://www.whxb.pku.edu.cn/CN/Y2013/V29/I01/176

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MnO_x/Al-SBA-15的结构性质及低温NH₃选择性催化还原NO_x

Structural Properties of MnO_x/Al-SBA-15 in Low-Temperature Selective Catalytic Reduction of NO_x with NH₃

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