Insights into SO2 Poisoning Mechanisms of Fresh and Hydrothermally Aged Cu-KFI Catalysts for NH3-SCR Reaction

被引：24
作者：
Liu, Zhongqi [1 ,2 ]
Shan, Yulong [1 ,2 ]
Han, Shichao [3 ]
Fu, Yu [1 ,2 ]
Du, Jinpeng [3 ]
Sun, Yu [1 ,2 ]
Shi, Xiaoyan [1 ,2 ]
Yu, Yunbo [1 ,2 ,3 ]
He, Hong [1 ,2 ,3 ]
机构：
[1] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Cont, Beijing 100085, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Inst Urban Environm, Ctr Excellence Reg Atmospher Environm, Xiamen 361021, Peoples R China
来源：
ENVIRONMENTAL SCIENCE & TECHNOLOGY | 2023年 / 57卷 / 10期
基金：
中国国家自然科学基金;
关键词：
KFI zeolite; Cu-KFI; SO2; poisoning; hydrothermal aging; complex poisoning; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; REDUCTION; CU/SSZ-13; SO2; ZEOLITE; IMPACT; DEACTIVATION; ADSORPTION; CU-SSZ-13;
D O I：
10.1021/acs.est.2c09805
中图分类号：
X [环境科学、安全科学];
学科分类号：
08 ; 0830 ;
摘要：
The complex poisoning of Cu-KFI catalysts by SO2 and hydrothermal aging (HTA) was investigated. The low-temperature activity of Cu-KFI catalysts was restrained by the formation of H2SO4 and then CuSO4 after sulfur poisoning. Hydrothermally aged Cu-KFI exhibited better SO2 resistance than fresh Cu-KFI since HTA significantly reduced the number of Brunsted acid sites, which were considered to be the H2SO4 storage sites. The high-temperature activity of SO2-poisoned Cu-KFI was basically unchanged compared to the fresh catalyst. However, SO2 poisoning promoted the high-temperature activity of hydrothermally aged Cu-KFI since it triggered CuOx into CuSO4 species, which was considered as an important role in the NH3-SCR reaction at high temperatures. In addition, hydro-thermally aged Cu-KFI catalysts were more easily regenerated after SO2 poisoning than fresh Cu-KFI on account of the instability of CuSO4.
引用
收藏
页码：4308 / 4317
页数：10
相关论文
共 44 条
[1]   In-situ studies of oxidation/reduction of copper in Cu-CHA SCR catalysts: Comparison of fresh and SO2-poisoned catalysts [J].
Bergman, Usanna L. ;
Dahlin, Sandra ;
Mesilov, Vitaly V. ;
Xiao, Yang ;
Englund, Johanna ;
Xi, Shibo ;
Tang, Chunhua ;
Skoglundh, Magnus ;
Pettersson, Lars J. ;
Bernasek, Steven L. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 269
[2]   Synthesis and characterization of 18-crown-6 ether-containing KFI-type zeolite [J].
Chatelain, T ;
Patarin, J ;
Farre, R ;
Petigny, O ;
Schulz, P .
ZEOLITES, 1996, 17 (04) :328-333
[3]   The different impacts of SO2 and SO3 on Cu/zeolite SCR catalysts [J].
Cheng, Yisun ;
Lambert, Christine ;
Kim, Do Heui ;
Kwak, Ja Hun ;
Cho, Sung June ;
Peden, Charles H. F. .
CATALYSIS TODAY, 2010, 151 (3-4) :266-270
[4]   Promoting Effect of Mn on In Situ Synthesized Cu-SSZ-13 for NH3-SCR [J].
Du, Jinpeng ;
Wang, Jingyi ;
Shi, Xiaoyan ;
Shan, Yulong ;
Zhang, Yan ;
He, Hong .
CATALYSTS, 2020, 10 (12) :1-14
[5]   Effects of SO2 on Cu-SSZ-39 catalyst for the selective catalytic reduction of NOx with NH3 [J].
Du, Jinpeng ;
Shi, Xiaoyan ;
Shan, Yulong ;
Xu, Guangyan ;
Sun, Yu ;
Wang, Yingjie ;
Yu, Yunbo ;
Shan, Wenpo ;
He, Hong .
CATALYSIS SCIENCE & TECHNOLOGY, 2020, 10 (05) :1256-1263
[6]   Promotion of the selective catalytic reduction of NOx with NH3 over microporous Cu-SSZ-13 by H2O and OH groups at low temperatures: a density functional theory study [J].
Fu, Yu ;
He, Guangzhi ;
Shan, Yulong ;
Du, Jinpeng ;
He, Hong .
CATALYSIS SCIENCE & TECHNOLOGY, 2022, 12 (18) :5524-5532
[7]   On the hydrothermal stability of Cu/SSZ-13 SCR catalysts [J].
Gao, Feng ;
Szanyi, Janos .
APPLIED CATALYSIS A-GENERAL, 2018, 560 :185-194
[8]   Impact of SO2-poisoning over the lifetime of a Cu-CHA catalyst for NH3-SCR [J].
Hammershoi, Peter S. ;
Jensen, Anker D. ;
Janssens, Ton V. W. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 238 :104-110
[9]   Importance of the Cu oxidation state for the SO2-poisoning of a Cu-SAPO-34 catalyst in the NH3-SCR reaction [J].
Hammershoi, Peter S. ;
Vennestrom, Peter N. R. ;
Falsig, Hanne ;
Jensen, Anker D. ;
Janssens, Ton V. W. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 236 :377-383
[10]   Reversible and irreversible deactivation of Cu-CHA NH3-SCRcatalysts by SO2 and SO3 [J].
Hammershoi, Peter S. ;
Jangjou, Yasser ;
Epling, William S. ;
Jensen, Anker D. ;
Janssens, Ton V. W. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 226 :38-45
12345