Understanding the Hydrothermal Stability of Potential NH3-SCR Catalyst Cu-KFI Zeolite

ACS CATALYSIS(2024)

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摘要
Al-rich Cu-KFI was found to withstand hydrothermal aging (HTA) at 800 degrees C, while Cu-CHA with a similar Si/Al ratio was deactivated since a much higher energy barrier was required to transform Cu2+ ions to CuOx during HTA in KFI. Specifically, the rate-determining step is the hydrolysis of Cu2+ in KFI but the cross-cage migration of Cu(OH)(2) in CHA. Therefore, the inclusion of two Cu2+ ions in one repeat unit of KFI does not significantly promote CuOx production. However, the accumulated CuOx cannot be completely avoided under such severe hydrothermal aging. It may originate from Cu2+ in the same cage or adjacent cages. This shorter diffusion effectively mitigated the structural integrity deterioration of KFI in comparison to CHA. Nevertheless, HTA reduced the number as well as the reactivity of residual Cu2+ ions in Cu-KFI zeolite catalysts. Quantitative results determined that the activity and stability of the catalyst were maximized when the average lta cage contained about 1.4 Cu2+ ions.
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关键词
Cu-KFI,NH3-SCR,hydrothermal deactivationmechanism,hydrolysis of Cu2+ ions,averageCu(2+) per repeat unit,CuOx
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