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Influence of synthesis method on catalytic properties and hydrothermal stability of Cu/SSZ-13 for NH3-SCR reaction

Journal 2019 · IF 8.355 · 发表于 2019 年 7 月 29 日
作者: Han Jiang,Bin Guan,Xuesong Peng,Reggie Zhan,He Lin,Zhen Huang
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摘要

This study focuses on investigating the influence of ion-exchange method (ION-F and ION-A) and one-pot method (ONE-F and ONE-A) on catalytic properties and hydrothermal stability of Cu/SSZ-13. It was found that ONE-F catalyst showed better SCR activity, especially at low temperature range below 400 °C. After hydrothermal aging, ION-A exhibited higher low temperature efficiency than ONE-A. The effect of synthesis method on the physicochemical structure, acidity intensity, and Cu species migration or transformation of the fresh and aged Cu/SSZ-13 catalysts were comprehensively characterized by NH 3 -TPO, H 2 -TPR, NH 3 -TPD, ICP, XRF, BET, XRD, SEM, and TEM. ONE-F has more isolated Cu 2+ sites, higher ratio of active sites Cu 2+ -2Z/[Cu(OH)] + -Z, more Lewis acid sites, and smaller particle size than ION-F. However, hydrothermal aging had severe effect on Cu/SSZ-13 prepared by one-pot method, leading to particle aggregation and decrease of active copper sites. According to NH 3 -SCR kinetic studies, smaller particle size and more uniformly distributed active sites over ONE-F resulted in less effect of pore diffusion limitation. Furthermore, in situ DRIFTS results indicated that more monodentate nitrates adsorbed sites and Lewis acid sites existed in ONE-F. On the other hand, monodentate nitrates were identified to be the most active nitrate species, and Lewis acid sites were ascertained to be more active than Brønsted acid sites. Therefore, ONE-F showed more excellent SCR performance than ION-F. However, hydrothermal aging resulted in loss of majority of nitrate adsorbed sites and acid sites over catalyst prepared by one-pot method, leading to lower SCR performance. In conclusion, Cu/SSZ-13 prepared by ion-exchange method has higher hydrothermal stability, however, fresh Cu/SSZ-13 prepared by one-pot method has excellent catalytic properties.

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