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The Influence of Si/Al Ratios on Adsorption and Desorption Characterizations of Pd/Beta Served as Cold-Start
Ming Jiang1, Jun Wang2, Jianqiang Wang3
1Key Laboratory for Green Chemical Technology of State Education Ministry, School of Chemical Engineering& Technology, Tianjin University, Tianjin 300072, China. jiangming@tju.edu.cn.
Abstract:
: The majority of NOx is exhausted during the cold-start period for the low temperature of vehicle emissions, which can be solved by using Pd/zeolite catalysts to trap NOx at low temperature and release NOx at a high temperature that must be higher than the operating temperature of selective catalytic reduction catalysts (SCR). In this work, several Pd/Beta catalysts were prepared to identify the influence of Si/Al ratios on NO and C₃H₆ adsorption and desorption characterizations. The physicochemical properties were identified using N₂ physical adsorption, Fourier Transform Infrared Spectroscopy (FT-IR), transmission electron microscopy (TEM), X-ray photo electron spectroscopy (XPS), and Na⁺ titration, while the adsorption and desorption characterizations were investigated by catalyst evaluation. The results indicated that the amount of dispersed Pd ions, the main active sites for NO and C₃H₆ adsorption, decreased with the increase of Si/Al ratios. Besides this, the intensity of Brønsted and Lewis acid decreased with the increase of Si/Al ratios, which also led to the decrease of NO and C₃H6 adsorption amounts. Therefore, Pd dispersion and the acidic properties of Pd/Beta together determined the adsorption ability of NO and C₃H₆. Moreover, lower Si/Al ratios resulted in the formation of an additional dispersed Pd cationic species, Pd(OH)⁺, from which adsorbed NO released at a much lower temperature. Finally, an optimum Si/Al ratio of Pd/Beta was found at around 55 due to the balanced performance between the adsorption amounts and desorption temperature.
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