The Cu migration of Cu-SAPO-34 catalyst for ammonia selective catalytic reduction of NOx during high temperature hydrothermal aging treatment

被引:30
作者
Li, Xianghui [1 ]
Zhao, Yingnan [2 ]
Zhao, Huawang [1 ]
Liu, Mengke [1 ]
Ma, Yuhan [1 ]
Yong, Xin [1 ]
Chen, Hong [3 ]
Li, Yongdan [1 ,2 ]
机构
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin Key Lab Appl Catalysis Sci & Technol, State Key Lab Chem Engn,Sch Chem Engn, Tianjin 300072, Peoples R China
[2] Aalto Univ, Sch Chem Engn, Dept Chem & Met Engn, Espoo 02150, Finland
[3] Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300072, Peoples R China
关键词
NH3 selective catalytic reduction; Hydrothermal treatment; Cu-SAPO-34; zeolite; One-pot synthesis; Ion-exchange preparation; CU/SAPO-34; CATALYSTS; THERMAL-STABILITY; MOLECULAR-SIEVES; ACTIVE-SITES; NH3-SCR; ZEOLITE; PERFORMANCE; NH3; SCR; CU-SSZ-13;
D O I
10.1016/j.cattod.2018.05.029
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Two kinds of Cu-SAPO-34 catalysts, prepared with a one-pot technique using Cu-tetraethylenepentamine as cotemplate and an ion-exchange method, were hydrothermally treated at 750 degrees C for at least 16 h. The migration of Cu species during hydrothermal treatment and the corresponding effect on the selective catalytic reduction (SCR) of NOx were examined and characterized. A certain amount of CuO exists outside and inner the crystallites in the as prepared ion-exchanged sample, whereas copper is mainly atomically dispersed in the one-pot sample existing as isolated Cu2+. After hydrothermal treatment for 16 h, the amount of the inner nanosized CuO in the ion-exchanged sample reduced and the copper disperses to form more isolated Cu2+. However, surface CuO particles increase at the sacrifice of isolated Cu2+ with extending the hydrothermal treatment to 24 h. Aggregation of Cu2+ species also happens during the aging treatment over the one-pot prepared sample where the initial Cu is atomically dispersed as isolated Cu2+. The increase of the amount of the isolated Cu2+ enhances the low-temperature (< 350 degrees C) performance. However, the increase of the amount of surface CuO particles in the aged samples promotes the nonselective NH3 oxidation reaction in the high temperature range and results in the lowering of the SCR activity by limiting NH3 supply.
引用
收藏
页码:126 / 133
页数:8
相关论文
共 46 条
[1]   Recent advances in automotive catalysis for NOx emission control by small-pore microporous materials [J].
Beale, A. M. ;
Gao, F. ;
Lezcano-Gonzalez, I. ;
Peden, C. H. F. ;
Szanyi, J. .
CHEMICAL SOCIETY REVIEWS, 2015, 44 (20) :7371-7405
[2]   The role of pore size on the thermal stability of zeolite supported Cu SCR catalysts [J].
Blakeman, Philip G. ;
Burkholder, Eric M. ;
Chen, Hai-Ying ;
Collier, Jillian E. ;
Fedeyko, Joseph M. ;
Jobson, Hoi ;
Rajaram, Raj R. .
CATALYSIS TODAY, 2014, 231 :56-63
[3]   FTIR adsorption studies of H2O and CH3OH in the isostructural H-SSZ-13 and H-SAPO-34:: Formation of H-bonded adducts and protonated clusters [J].
Bordiga, S ;
Regli, L ;
Lamberti, C ;
Zecchina, A ;
Bjorgen, M ;
Lillerud, KP .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (16) :7724-7732
[4]   Thermal stability and dehydroxylation of Bronsted acid sites in silicoaluminophosphates H-SAPO-11, H-SAPO-81 H-SAPO-31, and H-SAPO-34 investigated by multi-nuclear solid-state NMR spectroscopy [J].
Buchholz, A ;
Wang, W ;
Xu, M ;
Arnold, A ;
Hunger, M .
MICROPOROUS AND MESOPOROUS MATERIALS, 2002, 56 (03) :267-278
[5]   The promotion effect of CeOx on Cu-SAPO-34 catalyst for selective catalytic reduction of NOx with ammonia [J].
Dong, Xuesong ;
Wang, Jihui ;
Zhao, Huawang ;
Li, Yongdan .
CATALYSIS TODAY, 2015, 258 :28-34
[6]   The local environment of Cu+ in Cu-Y zeolite and its relationship to the synthesis of dimethyl carbonate [J].
Drake, Ian J. ;
Zhang, Yihua ;
Briggs, Daniel ;
Lim, Bomyi ;
Chau, Tanguy ;
Bell, Alexis T. .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (24) :11654-11664
[7]   A novel solvothermal approach to synthesize SAPO molecular sieves using organic amines as the solvent and template [J].
Fan, Dong ;
Tian, Peng ;
Xu, Shutao ;
Xia, Qinghua ;
Su, Xiong ;
Zhang, Lin ;
Zhang, Ying ;
He, Yanli ;
Liu, Zhongmin .
JOURNAL OF MATERIALS CHEMISTRY, 2012, 22 (14) :6568-6574
[8]   The effect of synthesis methods on Cu species and active sites over Cu/SAPO-34 for NH3-SCR reaction [J].
Fan, Shikuan ;
Xue, Junjie ;
Yu, Tie ;
Fan, Dequan ;
Hao, Teng ;
Shen, Meiqing ;
Li, Wei .
CATALYSIS SCIENCE & TECHNOLOGY, 2013, 3 (09) :2357-2364
[9]   The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites [J].
Fickel, Dustin W. ;
D'Addio, Elizabeth ;
Lauterbach, Jochen A. ;
Lobo, Raul F. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2011, 102 (3-4) :441-448
[10]   Understanding ammonia selective catalytic reduction kinetics over Cu/SSZ-13 from motion of the Cu ions [J].
Gao, Feng ;
Walter, Eric D. ;
Kollar, Marton ;
Wang, Yilin ;
Szanyi, Janos ;
Peden, Charles H. F. .
JOURNAL OF CATALYSIS, 2014, 319 :1-14