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

被引:149
|
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
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