H2O and SO2 deactivation mechanism of MnOx/MWCNTs for low-temperature SCR of NOx with NH3

被引:117
|
作者
Pan, Siwei [1 ]
Luo, Hongcheng [2 ]
Li, Li [1 ]
Wei, Zhengle [1 ]
Huang, Bichun [2 ,3 ]
机构
[1] Guangdong Power Grid Corp, Elect Power Res Inst, Guangzhou 510080, Guangdong, Peoples R China
[2] S China Univ Technol, Coll Environm & Energy, Guangzhou 510006, Guangdong, Peoples R China
[3] S China Univ Technol, Guangdong Prov Key Lab Atmospher Environm & Pollu, Guangzhou 510006, Guangdong, Peoples R China
基金
中国国家自然科学基金;
关键词
Multi-walled carbon nanotubes; Low-temperature selective catalytic reduction; Deactivation mechanism; H2O; SO2; SELECTIVE CATALYTIC-REDUCTION; WALLED CARBON NANOTUBES; NITRIC-OXIDE; NITROGEN-OXIDES; AMMONIA; OXIDATION; OXYGEN; TITANIA; AL2O3; WATER;
D O I
10.1016/j.molcata.2013.05.009
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The effect of H2O and SO2 on the catalytic activity of manganese oxides supported on multi-walled carbon nanotubes (MnOx/MWCNTs) for low-temperature selective catalytic reduction (SCR) of NOx with NH3 was studied. Also, N-2 adsorption, transient response experiments, X-ray powder diffraction (XRD), Raman spectroscopy, Fourier transform infrared (FT-IR) spectroscopy and in situ FT-IR spectroscopy were performed to investigate the deactivation mechanism of MnOx/MWCNTs catalyst in the presence of H2O or SO2. Experimental results showed that H2O had a reversible negative effect on the catalytic activity of the catalyst. When the temperature was higher than 270 degrees C, the effect of H2O could be negligible. The competitive adsorption of H2O and NH3 on the Lewis acid sites contributed to the deactivation of the catalyst. The integrity increase of MWCNTs in the presence of H2O might be another reason for the deactivation of the catalyst. However, SO2 led to the irreversible deactivation of the catalyst. The higher the reaction temperature, the more dramatically the catalystic activity decreased. The sulfation of the active center atoms was the main poisoning route. Also, formation of ammonium sulfates on the catalyst surface and the competitive adsorption between SO2 and NO were responsible for the partial deactivation of the catalyst to some extent. (c) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:154 / 161
页数:8
相关论文
共 50 条
  • [1] SO2 Deactivation Mechanism of MnOx/MWCNTs Catalyst for Low-Temperature Selective Catalytic Reduction of NOx by Ammonia
    Luo Hong-Cheng
    Huang Bi-Chun
    Fu Ming-Li
    Wu Jun-Liang
    Ye Dai-Qi
    ACTA PHYSICO-CHIMICA SINICA, 2012, 28 (09) : 2175 - 2182
  • [2] Deactivation of MnOx-CeOx/ACF Catalysts for Low-Temperature NH3-SCR in the Presence of SO2
    Shen Bo-Xiong
    Liu Ting
    ACTA PHYSICO-CHIMICA SINICA, 2010, 26 (11) : 3009 - 3016
  • [3] A study of the mechanism of low-temperature SCR of NO with NH3 on MnOx/CeO2
    Xu, Li
    Li, Xiao-Song
    Crocker, Mark
    Zhang, Zhao-Shun
    Zhu, Ai-Min
    Shi, Chuan
    JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2013, 378 : 82 - 90
  • [4] Effect of Ce/Y Addition on Low-Temperature SCR Activity and SO2 and H2O Resistance of MnOx/ZrO2/MWCNTs Catalysts
    Dong, Lifu
    Fan, Yinming
    Ling, Wei
    Yang, Chao
    Huang, Bichun
    CATALYSTS, 2017, 7 (06):
  • [5] A review of Mn-based catalysts for low-temperature NH3-SCR: NOx removal and H2O/SO2 resistance
    Xu, Guiying
    Guo, Xiaolong
    Cheng, Xingxing
    Yu, Jian
    Fang, Baizeng
    NANOSCALE, 2021, 13 (15) : 7052 - 7080
  • [6] Research of SO2 resistance of MnOx catalyst modified by Ce for low temperature SCR with NH3
    Wang, Yan
    Yang, Liu
    Liao, Weiping
    Wang, Fei
    PROGRESS IN ENVIRONMENTAL SCIENCE AND ENGINEERING (ICEESD2011), PTS 1-5, 2012, 356-360 : 529 - +
  • [7] Effects of H2O and SO2 on Selective Catalytic Reduction of NOx by NH3
    Bai, Shuzhan
    Tao, Jianzhong
    Sun, Qiang
    Tong, Dehui
    Li, Guoxiang
    ASIAN JOURNAL OF CHEMISTRY, 2012, 24 (05) : 2135 - 2138
  • [8] Effects of H2O and SO2 on NOx selective catalytic reduction by NH3
    School of Energy and Power Engineering, Shandong University, Jinan 250061, China
    不详
    Neiranji Gongcheng, 2008, 3 (56-58+63): : 56 - 58
  • [9] The insight into the role of Al2O3 in promoting the SO2 tolerance of MnOx for low-temperature selective catalytic reduction of NOx with NH3
    Fan, Zhaoyang
    Shi, Jian-Wen
    Niu, Cihang
    Wang, Baorui
    He, Chi
    Cheng, Yonghong
    CHEMICAL ENGINEERING JOURNAL, 2020, 398
  • [10] Effect of Promoters on the Catalytic Performance and SO2/H2O Resistance of α-MnO2 Catalysts for Low Temperature NH3 -SCR
    Jiang, Haoxi
    Wang, Jing
    Zhou, Jiali
    Chen, Yifei
    Zhang, Minhua
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2019, 58 (04) : 1760 - 1768