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
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