Improvement of low-temperature hydrothermal stability of Cu/SAPO-34 catalysts by Cu2+ species

被引:141
|
作者
Wang, Jun [1 ]
Fan, Dequan [1 ]
Yu, Tie [1 ]
Wang, Jianqiang [1 ]
Hao, Teng [1 ]
Hu, Xiaoqian [1 ]
Shen, Meiqing [1 ,2 ,3 ]
Li, Wei [4 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, State Educ Minist, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China
[2] Tianjin Univ, State Key Lab Engines, Tianjin 300072, Peoples R China
[3] Collaborat Innovat Ctr Chem Sci & Engn, Tianjin 300072, Peoples R China
[4] Gen Motors Global Res & Dev, Chem Sci & Mat Syst Lab, Warren, MI 48090 USA
关键词
Cu/SAPO-34; Hydrothermal stability; NH3-SCR; Si-O-Al bonds; Cu2+ protection; ELECTRON-SPIN-RESONANCE; ADSORBATE INTERACTION; MOLECULAR-SIEVES; CU(II) LOCATION; ECHO MODULATION; SAPO-34; REDUCTION; TEMPLATE; NOX; ZEOLITE;
D O I
10.1016/j.jcat.2014.11.010
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 destructive effect of H2O on SAPO-34 framework and Cu2+ species protection mechanism at low temperature were studied in this research. A series of Cu/SAPO-34 samples with varying Cu loadings (0-6.78 wt%) were hydrothermally treated at 70 degrees C with 80% humidity. Textural characterization results showed that this treatment led to the collapse of SAPO-34 framework at zero or low Cu loadings, which was caused by the breakage of Si-O-Al bonds proved by ex-situ DRIFTS and NMR results. The copper content increase enhanced SAPO-34 stabilization. Selective catalytic reduction (SCR) reaction rates were severely reduced after the treatment, while this decrease was gradually suppressed with increasing Cu loading up to 6.78 wt%. NH3-TPD and EPR results revealed that both the number of Bronsted acid sites and Cu2+ species decreased after the treatment, which likely contributed to the reduced SCR reaction rates. Our study indicated that the isolated Cu2+ ions were both SCR active site and structure protective agent. (C) 2014 Elsevier Inc. All rights reserved.
引用
收藏
页码:84 / 90
页数:7
相关论文
共 50 条
  • [1] Advances in low-temperature hydrothermal stability of Cu/SAPO-34 zeolite
    Zhang, Qiang
    Yu, Meng-Yun
    Chen, Yan-Hong
    Li, Jian-Xiang
    Kang, Hao
    Shi, Hui-bing
    CHEMICAL PAPERS, 2024, 78 (03) : 1517 - 1527
  • [2] Advances in low-temperature hydrothermal stability of Cu/SAPO-34 zeolite
    Qiang Zhang
    Meng-Yun Yu
    Yan-Hong Chen
    Jian-Xiang Li
    Hao Kang
    Hui-bing Shi
    Chemical Papers, 2024, 78 : 1399 - 1413
  • [3] Low-Temperature NOx Removal Using Cu-Hierarchical SAPO-34 Catalysts with High Hydrothermal Stability
    De Araujo, Brenda Roberta Silveira
    Onrubia-Calvo, Jon Ander
    Petaud, Guillaume
    Nieto-Marquez, Antonio
    Pereda-Ayo, Benat
    Velasco, Juan Ramon Gonzalez
    Caravaca, Angel
    Gil, Sonia
    CHEMCATCHEM, 2023, 15 (11)
  • [4] Destructive and Protective Effects of NH3 on the Low-Temperature Hydrothermal Stability of SAPO-34 and Cu-SAPO-34
    Ma, Yue
    Gao, Yang
    Wu, Xiaodong
    Jin, Baofang
    Ran, Rui
    Si, Zhichun
    Weng, Duan
    ACS APPLIED MATERIALS & INTERFACES, 2022, 14 (38) : 43442 - 43455
  • [5] New insights into the effects of Nd on low-temperature hydrothermal stability of deNOx Cu/SAPO-34 catalysts: A comparative evaluation of the mechanism
    Zhang P.
    Wang H.
    Yu X.
    Chen J.
    Zhang Q.
    Applied Surface Science, 2024, 669
  • [6] Migration of Cu species in Cu/SAPO-34 during hydrothermal aging
    Wang, Lei
    Gaudet, Jason R.
    Li, Wei
    Weng, Duan
    JOURNAL OF CATALYSIS, 2013, 306 : 68 - 77
  • [7] Nature of cerium on improving low-temperature hydrothermal stability of SAPO-34*
    Wang, Qingyun
    Shen, Meiqing
    Wang, Jianqiang
    Wang, Chen
    Wang, Jun
    JOURNAL OF RARE EARTHS, 2021, 39 (05) : 548 - 557
  • [8] Nature of cerium on improving low-temperature hydrothermal stability of SAPO-34
    Qingyun Wang
    Meiqing Shen
    Jianqiang Wang
    Chen Wang
    Jun Wang
    Journal of Rare Earths, 2021, 39 (05) : 548 - 557
  • [9] Improvement of the hydrothermal stability of SAPO-34
    Mees, FDP
    Martens, LRM
    Janssen, MJG
    Verberckmoes, AA
    Vansant, EF
    CHEMICAL COMMUNICATIONS, 2003, (01) : 44 - 45
  • [10] Boosting low-temperature and high-temperature hydrothermal stability of Cu/SAPO-34 for NOx removal via yttrium decoration
    Gao, Lianyun
    Gao, Wenfeng
    Wang, Huimin
    Xu, Siyuan
    Tian, Xiaoyan
    Cao, Jinyan
    Chen, Jianjun
    Zhang, Qiulin
    Ning, Ping
    Hao, Jiming
    CHEMICAL ENGINEERING JOURNAL, 2023, 455