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

doi:10.1007/s11783-022-1557-0

Front. Environ. Sci. Eng.

2022, Vol. 16

Issue (10) : 125 https://doi.org/10.1007/s11783-022-1557-0

RESEARCH ARTICLE

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

Xin Xing¹, Na Li², Dandan Liu¹, Jie Cheng²(

), Zhengping Hao²

¹. College of Environmental Science and Engineering, Taiyuan University of Science and Technology, Taiyuan 030024, China
². National Engineering Laboratory for VOCs Pollution Control Material & Technology, Research Center for Environmental Material and Pollution Control Technology, University of Chinese Academy of Sciences, Beijing 101408, China

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Abstract

● 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.

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.

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

Corresponding Author(s): Jie Cheng

Online First Date: 02 March 2022 Issue Date: 31 March 2022

Cite this article:

Xin Xing,Na Li,Dandan Liu, et al. Effect of Cu-ZSM-5 catalysts with different CuO particle size on selective catalytic oxidation of N,N-Dimethylformamide[J]. Front. Environ. Sci. Eng., 2022, 16(10): 125.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-022-1557-0
https://academic.hep.com.cn/fese/EN/Y2022/V16/I10/125

Fig.1 TEM images of Cu-ZSM-5 catalysts: (a) Cu-12 nm, (b) Cu-9 nm, (c) Cu-6 nm and (d) Cu-3 nm and the corresponding particle size distributions of Cu-ZSM-5 catalysts: (a’) Cu-12 nm, (b’) Cu-9 nm, (c’) Cu-6 nm and (d’) Cu-3 nm.

Fig.2 XRD patterns (a) and locally amplified XRD patterns (b) of Cu-12 nm, Cu-9 nm, Cu-6 nm and Cu-3 nm.

Tab.1 Characteristic reaction temperatures (T₁₀,T₅₀ andT₉₀), composition of Cu species and O species calculated by XPS results

Fig.3 The conversion of DMF (a), the CO selectivity (b), CO₂ selectivity (c), NO selectivity (d), N₂O selectivity (e) and N₂ selectivity (f) in 150–500 °C.

Fig.4 H₂-TPR results of Cu-12 nm, Cu-9 nm, Cu-6 nm and Cu-3 nm.

Fig.5 XPS spectra of Cu 2p (a) and O 1s (b) over Cu-12 nm, Cu-9 nm, Cu-6 nm and Cu-3 nm.

Fig.6 (a) ²⁷Al MAS NMR spectra of Cu-12 nm, Cu-9 nm, Cu-6 nm and Cu-3 nm, (b) Integrated ²⁷Al peak area of 55 ppm.

Fig.7 NH₃-TPD results of Cu-12 nm, Cu-9 nm, Cu-6 nm and Cu-3 nm.

Fig.8 EPR results of Cu-12 nm, Cu-9 nm, Cu-6 nm and Cu-3 nm.

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