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Structural control for inhibiting SO2 adsorption in porous MnCe nanowire aerogel catalysts for low-temperature NH3-SCR

Journal 2022 · IF 16.744 · 发表于 2022 年 1 月 19 日
作者: Chengzhi Wang,Fengyu Gao,Songjin Ko,Hengheng Liu,Honghong Yi,Xiaolong Tang
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摘要

The presence of SO 2 in industrial flue gases will cause permanent deactivation of the catalyst active centre. Therefore, an effective method to improve the SO 2 resistance of manganese-based catalysts at low temperatures is urgently needed. In this work, a hierarchical porous nanowire structure catalyst was designed by the in situ self-assembly method to inhibit SO 2 adsorption. This hierarchical porous nanowire aerogel catalyst with great BET surface area and surface acidity exhibited NOx conversion above 90% at 100–400 °C. Notably, the NOx conversion of the MnCe-N catalyst was almost not inhibited by SO 2 (250 ppm) compared to the 33% decrease of the MnCe-P catalyst. On the MnCe-P catalyst, SO 2 has strong competitive adsorption with NH 3 and NO, and the stronger adsorption capacity of SO 2 inhibits the adsorption activation of the reaction gas and hinders the reaction proceeding through the L-H mechanism. Meanwhile, a large quantity of sulfate is formed on the catalyst surface, which prevents the active centre to participate in the redox reaction. The structure of nanowires enhances the number of acid sites, facilitates the adsorption and activation of NH 3 , and effectively inhibits the adsorption of SO 2 on the MnCe-N catalyst. Fewer sulfate species are generated and difficult to deposit and aggregate on the catalyst surface, as a result, the active centre is less affected by sulfate species. The stable adsorption of NH 3 -related species ensures reliable reaction on MnCe-N through the E-R mechanism. This work emphasizes the importance of hierarchically porous structures in improving the NH 3 -SCR performance and SO 2 resistance of monolithic catalysts, and provides new insights into the design of highly efficient and stable catalytic materials.

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