The effect of sulfate species on the activity of NH3-SCR over Cu/SAPO-34

被引:66
|
作者
Wang, Chen [1 ]
Wang, Jun [1 ]
Wang, Jianqiang [1 ]
Yu, Tie [1 ]
Shen, Meiqing [1 ,2 ,3 ]
Wang, Wulin [1 ]
Li, Wei [4 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, State Educ Minist, Tianjin 300072, Peoples R China
[2] Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
[3] Tianjin Univ, State Key Lab Engines, Tianjin 300072, Peoples R China
[4] Chem Sci & Mat Syst Lab, Gen Motors Global Res & Dev, 30500 Mound Rd, Warren, MI 48090 USA
基金
中国国家自然科学基金;
关键词
Deactivation mechanism; Cu/SAPO-34; Sulfur poisoning; Sulfate species; SELECTIVE CATALYTIC-REDUCTION; EXCHANGED MORDENITE; LOW-TEMPERATURE; SULFUR-DIOXIDE; NH3; NO; SO2; REGENERATION; CU-SAPO-34; STABILITY;
D O I
10.1016/j.apcatb.2016.11.033
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 deactivation mechanism by different types of sulfate was investigated for the selective catalytic reduction of NOx on Cu/SAPO-34 catalyst. A Cu/SAPO-34 catalyst was treated with 50 ppm SO2 alone at 150 and 250 degrees C or in the presence of a SCR feed at 250 and 350 degrees C. Copper sulfate was found on all sulfated catalysts, but ammonia sulfate was found only on the catalyst sulfated in the SCR feed at 250 degrees C. In situ DRIFTs results show that both copper sulfate and ammonia sulfate species are formed on the isolated Cu2+ sites. All sulfated catalysts have lower NOx conversions compared with the Unsulfated catalysts due to reduced number of active sites. However, their apparent activation energies fot the SCR reaction remain the same, and their turnover frequencies are identical. This suggests that the deactivation mechanism is similar regardless of the type of sulfate species. On the other hand, it was found that ammonia sulfate was easier to remove than copper sulfate by a desulfation treatment at 600 degrees C, resulting in a larger extent of activity recovery. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:239 / 249
页数:11
相关论文
共 50 条
  • [21] Effect of Si islands on low-temperature hydrothermal stability of Cu/SAPO-34 catalyst for NH3-SCR
    Lin, Chenlu
    Cao, Yi
    Feng, Xi
    Lin, Qingjin
    Xu, Haidi
    Chen, Yaoqiang
    JOURNAL OF THE TAIWAN INSTITUTE OF CHEMICAL ENGINEERS, 2017, 81 : 288 - 294
  • [22] Grain size effect on the high-temperature hydrothermal stability of Cu/SAPO-34 catalysts for NH3-SCR
    Xu, Haidi
    Lin, Chenlu
    Lin, Qingjin
    Feng, Xi
    Zhang, Zhifeng
    Wang, Yun
    Chen, Yaoqiang
    JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING, 2020, 8 (06):
  • [23] Comprehensive effect of tuning Cu/SAPO-34 crystals using PEG on the enhanced hydrothermal stability for NH3-SCR
    Lin, Qingjin
    Liu, Shuang
    Xu, Shuhao
    Xu, Shi
    Pei, Mingming
    Yao, Pan
    Xu, Haidi
    Dan, Yi
    Chen, Yaoqiang
    CATALYSIS SCIENCE & TECHNOLOGY, 2021, 11 (23) : 7640 - 7651
  • [24] Catalytic deactivation mechanism research over Cu/SAPO-34 catalysts for NH3-SCR (II): The impact of copper loading
    Tang, Jiaojiao
    Xu, Minhong
    Yu, Tie
    Ma, Hongfei
    Shen, Meiqing
    Wang, Jun
    CHEMICAL ENGINEERING SCIENCE, 2017, 168 : 414 - 422
  • [25] Insights into the impact of lanthanum on hydrothermal-induced migration and transformation of copper species in Cu/SAPO-34 catalyst for NH3-SCR
    Wang, Huimin
    Li, Wei
    Xu, Siyuan
    Liu, Mo
    Hao, Jiming
    Ning, Ping
    Zhang, Qiulin
    MOLECULAR CATALYSIS, 2021, 515
  • [26] Promotional effect and mechanism of the modification of Ce on the enhanced NH3-SCR efficiency and the low temperature hydrothermal stability over Cu/SAPO-34 catalysts
    Guan, Bin
    Jiang, Han
    Peng, Xuesong
    Wei, Yanfei
    Liu, Ziqian
    Chen, Ting
    Lin, He
    Huang, Zhen
    APPLIED CATALYSIS A-GENERAL, 2021, 617
  • [27] Synthesis and evaluation of Cu-SAPO-34 catalysts for NH3-SCR
    Gao, Feng
    Walter, Eric D.
    Burton, Sarah D.
    Washton, Nancy M.
    Kwak, Ja Hun
    Szanyi, Janos
    Peden, Charles H. F.
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2013, 245
  • [28] The role of isolated Cu2+ location in structural stability of Cu-modified SAPO-34 in NH3-SCR of NO
    Yan, Chundi
    Cheng, Hao
    Yuan, Zhongshan
    Wang, Shudong
    ENVIRONMENTAL TECHNOLOGY, 2015, 36 (02) : 169 - 177
  • [29] Insights into Migration and Transformation of Cu Species during SO2 Poisoning and Hydrothermal Aging of Cu/SAPO-34 NH3-SCR Catalysts
    Wang, Fumei
    Cai, Qi
    He, Xinhua
    Shen, Boxiong
    Negahdar, Leila
    Feng, Shuo
    Beale, Andrew M.
    JOURNAL OF PHYSICAL CHEMISTRY C, 2024, 128 (24): : 9904 - 9914
  • [30] Neodymium promotion on the low-temperature hydrothermal stability of a Cu/SAPO-34 NH3-SCR monolith catalyst
    Feng, Xi
    Lin, Qingjin
    Cao, Yi
    Zhang, Hailong
    Li, Yuanshan
    Xu, Haidi
    Lin, Chenlu
    Chen, Yaoqiang
    JOURNAL OF THE TAIWAN INSTITUTE OF CHEMICAL ENGINEERS, 2017, 80 : 805 - 812