Tailored Synthesis of Catalytically Active Cerium Oxide for N, N-Dimethylformamide Oxidation

定制合成催化活性氧化铈用于N,N-二甲基甲酰胺氧化

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Abstract

Cerium oxide nanopowder (CeO(x)) was prepared using the sol-gel method for the catalytic oxidation of N, N-dimethylformamide (DMF). The phase, specific surface area, morphology, ionic states, and redox properties of the obtained nanocatalyst were systematically characterized using XRD, BET, TEM, EDS, XPS, H(2)-TPR, and O(2)-TPO techniques. The results showed that the catalyst had a good crystal structure and spherelike morphology with the aggregation of uniform small grain size. The catalyst showed the presence of more adsorbed oxygen on the catalyst surface. XPS and H(2)-TPR have confirmed the reduction of Ce(4+) species to Ce(3+) species. O(2)-TPR proved the reoxidability of CeO(x), playing a key role during DMF oxidation. The catalyst had a reaction rate of 1.44 mol g(-1)(cat) s(-1) and apparent activation energy of 33.30 ± 3 kJ mol(-1). The catalytic performance showed ~82 ± 2% DMF oxidation at 400 °C. This work's overall results demonstrated that reducing Ce(4+) to Ce(3+) and increasing the amount of adsorbed oxygen provided more suitable active sites for DMF oxidation. Additionally, the catalyst was thermally stable (~86%) after 100 h time-on-stream DMF conversion, which could be a potential catalyst for industrial applications.

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