4.2 Article

Rational Design of a Novel Core-Shell Cu-ZSM-5@Ru/S-1 Tandem Catalyst for the Catalytic Combustion of Dichloromethane

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ACS ES&T ENGINEERING
卷 3, 期 7, 页码 1013-1021

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AMER CHEMICAL SOC
DOI: 10.1021/acsestengg.3c00034

关键词

dichloromethane; catalytic combustion; tandem catalyst; Ru; Cu-ZSM-5

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A novel tandem catalyst, Cu-ZSM-5@Ru/S-1, was developed for the catalytic combustion of dichloromethane (DCM) to achieve a synergistic effect between dissociative adsorption and deep oxidation. The catalyst exhibited high DCM conversion and mineralization rates of over 90% with a low Ru loading of 0.2 wt % under a 5% H2O atmosphere at 290 degrees C. The study also revealed that the Cu-ZSM-5@Ru/S-1 catalyst had significantly higher activity in comparison to Cu-ZSM-5 and Ru/HZSM-5 catalysts. In addition, the catalyst met the national standard for PCDD/F emissions from municipal solid waste incineration.
To achieve a well synergistic effect between dissociative adsorption and deep oxidation during the dichloromethane (DCM) catalytic combustion process, a novel tandem catalyst, Cu-ZSM-5@Ru/S-1, was developed by rationally designing the catalyst structure. Activity experiments revealed that the Cu-ZSM-5@Ru/S-1 catalyst achieved a DCM conversion and mineralization rate of over 90% under a 5% H2O atmosphere at 290 degrees C with a low Ru loading of 0.2 wt %. The mineralization rate of the Cu-ZSM-5@Ru/S-1 was approximately 78% higher than that of the Cu-ZSM-5 catalyst, and the activity was approximately 55% higher than that of the Ru/ HZSM-5 catalyst. Furthermore, the in situ characterizations and simulation results indicated that the DCM catalytic reaction followed a tandem reaction mechanism. The initial dissociative adsorption and conversion of DCM primarily occurred in internal Cu-ZSM-5 active sites, and the deep oxidation of the intermediates was subsequently achieved on the Ru/S-1 shell. The two steps mentioned above acted synergistically to enhance both DCM dechlorination and deep oxidation. In addition, the PCDD/F emission of Cu-ZSM-5@Ru/S-1 catalyst at 350 and 400 degrees C met the national standard for municipal solid waste incineration (0.1 ng I-TEQ Nm-3). Overall, this study provides new strategies for developing highly active and cost-effective catalysts for CVOC catalytic combustion.

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