Selective Catalytic Reduction of NO by NH 3 over One-Pot Prepared Cu-SSZ-13 Catalysts with Different Si/Al Molar Ratio

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HEMICAL KINETICS AND CATALYSIS

Selective Catalytic Reduction of NO by NH3 over One-Pot Prepared Cu-SSZ-13 Catalysts with Different Si/Al Molar Ratio Jiangjiang Fenga, Dongdong Shia, Zhigang Xua, Junqiang Wanga, Yujie Wangb, and Xiaoliang Lia,* a State Key Laboratory Breeding Base of Coal Science and Technology Co-founded by Shanxi Province and the Ministry of Science and Technology, Taiyuan University of Technology, Taiyuan, Shanxi, 030024 China b School of Material and Chemical Engineering, Chuzhou University, Chuzhou, Anhui, 239000 China * e-mail: [email protected]

Received June 6, 2019; revised October 13, 2019; accepted December 17, 2019

Abstract—A series of Cu-SSZ-13 catalysts with different Si/Al molar ratio (10.6, 13.0, and 16.0) were prepared via one-pot method and investigated for the selective catalytic reduction by NH3. It was found that CuSSZ-13 with Si/Al ratio of 13.0 exhibited the best NH3-SCR performance with more than 94% NO conversion from 200 to 550°C. The influence of Si/Al molar ratio on the physical structure, redox behavior, surface acidity and Cu species distribution on the Cu-SSZ-13, together with the NH3 and nitrate adsorption species on the surface of Cu-SSZ-13 were characterized by N2-BET, XRD, NH3-TPD, H2-TPR, XPS, and in-situ DRIFTS, respectively. The characterization results indicated that the BET surface area, zeolite structure, surface acidity, redox properities, Cu2+ concentration, NH3 and nitrate adsorption species on the catalyst surface were closely related to the Si/Al ratio, all of these factors played important roles in the NH3-SCR performance for the Cu-SSZ-13. Keywords: selective catalytic reduction by NH3, Cu-SSZ-13 catalysts DOI: 10.1134/S003602442009006X

Nitrogen oxides (NOx) in the air can cause serious environmental issues, such as acid rain, ozone depletion, haze and photochemical Smog et al. [1]. Hence, NOx shows great hazards to the environment and people’s health. The majority of NOx is generated from stationary (power plants) and mobile sources (diesel engines). In order to control NOx emissions, most countries have implemented strict emission standards. Selective catalytic reduction with NH3 (NH3-SCR) has been accepted as the most effective and widely applied technology for the abatement of NOx. As the core of the NH3-SCR technology, catalyst played a key role during the denitrification process. For the diesel exhaust, the traditional commercial V2O5–WO3 (MoO3)/TiO2 catalyst cannot meet the requirements due to its own defects, such as the narrow reaction temperature window, the toxicity of V2O5 and the inadequate hydrothermal stability [2, 3]. In order to reduce the NOx emissions from diesel exhaust, great efforts have been made to develop novel catalysts. Up to now, various kinds of catalysts have been reported to be active for the abatement of NOx produced from the diesel engine. Among these catalysts, Cu-SSZ-13 has received more research interests compared to the other catalysts in recent years due to its

excellent NH3-SCR catalytic activity and good