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Acta Phys. Chim. Sin.  2013, Vol. 29 Issue (07): 1550-1557    DOI: 10.3866/PKU.WHXB201304283
CATALYSIS AND SURFACE SCIENCE     
Properties and Roles of Adsorbed NH3 and NOx over Cu/SAPO-34 Zeolite Catalyst in NH3-SCR Process
SHI Lin1, YU Tie1, WANG Xin-Quan1, WANG Jun1, SHEN Mei-Qing1,2
1 Key Laboratory for Green Chemical Technology of State Education Ministry, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, P. R. China;
2 State Key Laboratory of Engines, Tianjin University, Tianjin 300072, P. R. China
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Abstract  

To investigate the adsorption properties and roles of different feed gases in the selective catalytic reduction by ammonia (NH3-SCR), the adsorption sites, strength, and amount as well as reaction rates of NH3 and NOx (a mixture of NO and NO2) on exchanged Cu/SAPO-34 (chabazite zeolite) catalyst were studied. Transient response, temperature programmed desorption (TPD), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments were performed to characterize the catalyst. Transient response experiments showed that NH3 was adsorbed by the catalyst. TPD and DRIFTS indicated that NH3 can be adsorbed at both Br?nsted and Lewis acid sites to form various NH3 adsorption species that show different SCR activities. The adsorption rate of NH3 by Cu2+ cations was the fastest and the adsorption bond strength of NH3-Cu2+ was the strongest between NH3 and the Cu/SAPO-34 catalyst. NOx can be oxidized and stored as nitrates and nitrites on the Cu catalyst. The intermediate species formed at Cu active sites during the NH3-SCR reaction are discussed, allowing SCR reaction mechanisms to be inferred.



Key wordsAmmonia selective catalytic reduction      NOx (NO and NO2)      Cu/SAPO-34      Diffuse reflectance infrared Fourier transform spectrum      Adsorption species     
Received: 15 February 2013      Published: 28 April 2013
MSC2000:  O643  
Fund:  

The project was supported by the National High-Tech Research and Development Program of China (863) (2011AA03A405).

Corresponding Authors: SHEN Mei-Qing     E-mail: mqshen@tju.edu.cn
Cite this article:

SHI Lin, YU Tie, WANG Xin-Quan, WANG Jun, SHEN Mei-Qing. Properties and Roles of Adsorbed NH3 and NOx over Cu/SAPO-34 Zeolite Catalyst in NH3-SCR Process. Acta Phys. Chim. Sin., 2013, 29(07): 1550-1557.

URL:

http://www.whxb.pku.edu.cn/Jwk_wk/wlhx/10.3866/PKU.WHXB201304283     OR     http://www.whxb.pku.edu.cn/Jwk_wk/wlhx/Y2013/V29/I07/1550

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