Effect of Cu-ZSM-5 catalysts with different CuO particle size on selective catalytic oxidation of N,N-Dimethylformamide

Highlights

● A series of Cu-ZSM-5 catalysts were tested for DMF selective catalytic oxidation.

● Cu-6 nm samples showed the best catalytic activity and N₂ selectivity.

● Redox properties and chemisorbed oxygen impact on DMF catalytic oxidation.

● Isolated Cu²⁺ species and weak acidity have effects on the generation of N₂.

Abstract

N, N-Dimethylformamide (DMF), a nitrogen-containing volatile organic compound (NVOC) with high emissions from the spray industry, has attracted increasing attention. In this study, Cu-ZSM-5 catalysts with different CuO particle sizes of 3, 6, 9 and 12 nm were synthesized and tested for DMF selective catalytic oxidation. The crystal structure and physicochemical properties of the catalyst were studied by various characterization methods. The catalytic activity increases with increasing CuO particle size, and complete conversion can be achieved at 300–350 °C. The Cu-12 nm catalyst has the highest catalytic activity and can achieve complete conversion at 300 °C. The Cu-6 nm sample has the highest N₂ selectivity at lower temperatures, reaching 95% at 300 °C. The activity of the catalysts is determined by the surface CuO cluster species, the bulk CuO species and the chemisorbed surface oxygen species. The high N₂ selectivity of the catalyst is attributed to the ratio of isolated Cu²⁺ and bulk CuO species, and weak acidity is beneficial to the formation of N₂. The results in this work will provide a new design of NVOC catalytic oxidation catalysts.

Graphical abstract

Keywords

N, N-Dimethylformamide / Selective catalytic oxidation / Cu-ZSM-5 / CuO particle size

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Acknowledgements

This work is financially supported by the R&D Program of Beijing Municipal Education Commission (China) (No. KJZD20191443001), Beijing Municipal Science and Technology Commission (China) (No. Z181100000118003), the Key R&D Program of Shanxi Province (China) (No. 201903D311006), the Doctoral research start up fund project of Taiyuan University of science and technology (China) (Nos. 20202053 and 20192039), Research Support for Outstanding Doctors in Shanxi (China) (Nos. 20192043 and 20212060) and Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi (China) (Nos. 2021L311 and 2019L0030).

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