Journal
JOURNAL OF COLLOID AND INTERFACE SCIENCE
Volume 584, Issue -, Pages 193-203Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2020.09.091
Keywords
Acetonitrile; Catalytic combustion; CuCeOx-HZSM-5 composite catalysts; Synergism
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Funding
- National Natural Science Foundation of China [22076164]
- National Key Research and Development Program of China [2017YFC0210201]
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For the catalytic oxidation of acetonitrile, the Cu-Ce loading of composite catalysts significantly influences the activity, selectivity, and mineralization rate. Highly dispersed CuOx species and Cu2+-exchanged HZSM-5 zeolite contribute to the enhanced activity and N-2 selectivity of the catalyst. Catalysts with low Cu-Ce loading tend to form carbonaceous products, leading to a decrease in the mineralization rate.
A sequence of CuCeOx-HZSM-5 composite catalysts at different Cu-Ce loading synthesized by the citric acid complex impregnation method were evaluated for the catalytic oxidation of acetonitrile. Among which, the 2CuCeO(x)-HZSM-5 sample exhibited the best degradation efficiency. In the temperature range of 225-350 degrees C, its activity and mineralization rate were approximately 100%, and the N-2 selectivity remained more than 93%. The characterization results revealed that all the samples showed an existence of isolated Cu2+ species. And more Cu-Ce mixed oxides covered on HZSM-5 at an elevated Cu-Ce content, leading to the enhanced reducibility. In situ DRIFTS results showed that both oxidation and hydrolysis reaction routes proceeded during the degradation of acetonitrile over the composite catalysts. Their synergism was crucial to guarantee both high activity and N-2 selectivity. The highly dispersed CuOx species ensured the superior activity of the 2CuCeO(x)-HZSM-5 sample. And Cu2+ exchanged HZSM-5 zeolite would be beneficial to N-2 selectivity owing to the improved internal SCR (Selective Catalytic Reduction) reaction to reduce NOx from oxidation routes. Additionally, the mineralization rate was lowered with the formation of carbonaceous products like CH4 and CO for the catalysts at low Cu-Ce loading due to the lack of redox capacity. (C) 2020 Elsevier Inc. All rights reserved.
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