Discovering the remarkable deNOx activity and anti-K poisoning of MnFeOx/H-Beta composite catalyst

SEPARATION AND PURIFICATION TECHNOLOGY(2024)

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摘要
The practical application of MnFeOx catalyst is limited due to its narrow temperature window and poor resistance to alkali metal poisoning, such as K and Na. Alkali metal poisoning has always been a major factor in the deactivation of fixed-source denitration (deNOx) catalysts. Despite high activity at around 200(degrees)C , the catalyst's susceptibility to alkali metal poisoning hinders its effectiveness. In this study, a novel MnFeOx/H-Beta composite catalyst was prepared by the simple wet impregnation method. Beta zeolite, known for its large specific surface area compared to MnFeOx, special twelve-membered ring channel, and abundant acid sites, was introduced to adjust the acid and redox active sites. This resulted in MnFeOx/H-Beta having a wider temperature window and excellent resistance to K poisoning. Notably, the NOx conversion rate exceeded 80% between 180 and 460 C . K poisoning significantly reduces the acidity of the catalyst, as confirmed by various characterizations such as NH3TPD and NH3 adsorption in situ DRIFTs. After K poisoning, the total acid content of MnFeOx/H-Beta decreased from 14.99 to 9.47 mmol g(-1). The low acid content of MnFeOx allows the active sites to be easily covered by K, resulting in a reduction of the SCR performance, which can be attributed to the reduction of active nitrate species. The abundant acid sites of MnFeOx/H-Beta act as sacrificial sites and can coordinate with alkali metal K, thereby alleviating the poisoning of the catalyst to some extent. DFT calculations confirmed K binding to Bronsted acid sites on H-Beta zeolite, mitigating the detrimental impact of K on catalyst activity and lifetime. This research offers a pathway for designing efficient and alkali metal-resistant deNO(x )catalysts for real-world industrial applications.
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关键词
Beta zeolite,MnFeOx,Composite catalyst,NH3-SCR,K resistance,Mechanism
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