Insight into the SO2 poisoning mechanism for NOx removal by NH3-SCR over Cu/LTA and Cu/SSZ-13

被引:67
作者
Wang, Aiyong [1 ]
Olsson, Louise [1 ]
机构
[1] Chalmers Univ Technol, Competence Ctr Catalysis, Chem Engn, SE-41296 Gothenburg, Sweden
基金
瑞典研究理事会;
关键词
Cu; LTA; SSZ-13; Standard SCR; Fast SCR; SO2; SELECTIVE CATALYTIC-REDUCTION; HIGH-SILICA LTA; HYDROTHERMAL STABILITY; DENO(X) PERFORMANCE; ACTIVE-SITES; SCR; CU; NH3; TEMPERATURE; IMPACT;
D O I
10.1016/j.cej.2020.125048
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this study, Cu/LTA and Cu/SSZ-13 catalysts are examined for sulfur poisoning and regeneration. The nature of the Cu species was probed with H-2-TPR and in-situ DRIFTS. These characterizations collectively indicate that primarily Z(2)Cu is present in Cu/LTA, whereas Cu/SSZ-13 contains a higher concentration of ZCuOH. ZCuOH is proved to be more vulnerable to SO2 poisoning than Z(2)Cu sites in both Cu/zeolites. H-2-TPR results suggest that the interaction of ZCuOH with the framework in Cu/LTA is much weaker than in Cu/SSZ-13, thereby leading to more susceptibility to SO2 adsorption. Moreover, Cu/LTA can store more SO2 under NH3-SCR conditions in the presence of SO2, and it also has a slower deactivation rate due to the different location of generated (NH4)(2)SO4. Cu/LTA can be fully restored after regeneration at 750 degrees C. However, Cu/SSZ-13 experiences a loss of activity at high temperature, which is attributed to newly formed CuOx clusters.
引用
收藏
页数:12
相关论文
共 67 条
[1]   The Origin of an Unexpected Increase in NH3-SCR Activity of Aged Cu-LTA Catalysts [J].
Ahn, Nak Ho ;
Ryu, Taekyung ;
Kang, Yonjoo ;
Kim, Hyojun ;
Shin, Jiho ;
Nam, In-Sik ;
Hong, Suk Bong .
ACS CATALYSIS, 2017, 7 (10) :6781-6785
[2]   Facile Synthesis and Catalysis of Pure-Silica and Heteroatom LTA [J].
Boal, Ben W. ;
Schmidt, Joel E. ;
Deimund, Mark A. ;
Deem, Michael W. ;
Henling, Lawrence M. ;
Brand, Stephen K. ;
Zones, Stacey I. ;
Davis, Mark E. .
CHEMISTRY OF MATERIALS, 2015, 27 (22) :7774-7779
[3]   Revisiting the nature of Cu sites in the activated Cu-SSZ-13 catalyst for SCR reaction [J].
Borfecchia, E. ;
Lomachenko, K. A. ;
Giordanino, F. ;
Falsig, H. ;
Beato, P. ;
Soldatov, A. V. ;
Bordiga, S. ;
Lamberti, C. .
CHEMICAL SCIENCE, 2015, 6 (01) :548-563
[4]   Activation of oxygen on (NH3-Cu-NH3)+ in NH3-SCR over Cu-CHA [J].
Chen, Lin ;
Falsig, Hanne ;
Janssens, Ton V. W. ;
Gronbeck, Henrik .
JOURNAL OF CATALYSIS, 2018, 358 :179-186
[5]   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
[6]   Flame-synthesized LaCoO3-supported Pd 2.: Catalytic behavior in the reduction of NO by H2 under lean conditions [J].
Chiarello, Gian Luca ;
Ferri, Davide ;
Grunwaldt, Jan-Dierk ;
Forni, Lucio ;
Baiker, Alfons .
JOURNAL OF CATALYSIS, 2007, 252 (02) :137-147
[7]   Steam and alkali resistant Cu-SSZ-13 catalyst for the selective catalytic reduction of NOx in diesel exhaust [J].
Fan, Chi ;
Chen, Zhen ;
Pang, Lei ;
Ming, Shujun ;
Dong, Caiyue ;
Albert, Kouadio Brou ;
Liu, Peng ;
Wang, Jingyu ;
Zhu, Dajian ;
Chen, Hanping ;
Li, Tao .
CHEMICAL ENGINEERING JOURNAL, 2018, 334 :344-354
[8]   Recent Progress in Atomic-Level Understanding of Cu/SSZ-13 Selective Catalytic Reduction Catalysts [J].
Gao, Feng ;
Peden, Charles H. F. .
CATALYSTS, 2018, 8 (04)
[9]   Selective Catalytic Reduction over Cu/SSZ-13: Linking Homo- and Heterogeneous Catalysis [J].
Gao, Feng ;
Mei, Donghai ;
Wang, Yilin ;
Szanyi, Janos ;
Peden, Charles H. F. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (13) :4935-4942
[10]   Effects of Si/Al ratio on Cu/SSZ-13 NH3-SCR catalysts: Implications for the active Cu species and the roles of Bronsted acidity [J].
Gao, Feng ;
Washton, Nancy M. ;
Wang, Yilin ;
Kollar, Marton ;
Szanyi, Janos ;
Peden, Charles H. F. .
JOURNAL OF CATALYSIS, 2015, 331 :25-38