Citation: SHI Lin, YU Tie, WANG Xin-Quan, WANG Jun, SHEN Mei-Qing. Properties and Roles of Adsorbed NH₃ and NO_x over Cu/SAPO-34 Zeolite Catalyst in NH₃-SCR Process[J]. Acta Physico-Chimica Sinica, ;2013, 29(07): 1550-1557. doi: 10.3866/PKU.WHXB201304283 shu

Properties and Roles of Adsorbed NH₃ and NO_x over Cu/SAPO-34 Zeolite Catalyst in NH₃-SCR Process

SHI Lin ¹ ,
YU Tie ¹ ,
WANG Xin-Quan ¹ ,
WANG Jun ¹ ,
SHEN Mei-Qing ^1,2,

1.
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

Received Date: 15 February 2013
Available Online: 28 April 2013
Fund Project: 国家高技术研究发展计划项目(863) (2011AA03A405)资助 (863) (2011AA03A405)

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 NO_x (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. NO_x 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.
- Ammonia selective catalytic reduction,
- NO_x (NO and NO₂),
- Cu/SAPO-34,
- Diffuse reflectance infrared Fourier transform spectrum,
- Adsorption species
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Properties and Roles of Adsorbed NH₃ and NO_x over Cu/SAPO-34 Zeolite Catalyst in NH₃-SCR Process