期刊
CHEMICAL ENGINEERING JOURNAL
卷 434, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.134545
关键词
Heterogeneous catalyst; Selective oxidation; Esters; Carboxylic acids; Catalytic mechanism
资金
- National Natural Science Foun-dation of China [22172067, 21872066, U21B2091]
- Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi [2019L0108]
In this study, nitrogen-doped carbon encapsulated Co-based catalysts were successfully prepared and used for the selective oxidation of alcohols. Controlled experiments revealed the protective effect of the N-doped carbon structure and the synergistic effect between the Co core and Co3O4 species, ensuring high reaction conversion and selectivity. The catalyst's heterogeneity and magnetism allowed for easy recycling and long-term stability.
The sustainable catalytic transformation of alcohols to high value-added fine chemicals is a significant and challenging research topic. Herein, a set of nitrogen-doped carbon encapsulated Co-based catalysts (Co-Co3O4@NC-T) were prepared by using low-cost dicyandiamide, glyoxal and cobalt nitrate as precursors. The obtained catalysts were utilized for the selective oxidation of alcohols to high value-added esters and carboxylic acids with air as the oxygen source and displayed wide applicability for the oxidation of both aromatic and aliphatic alcohols. Based on the controlled experiments, the protective effect of N-doped carbon structure and the synergistic effect between Co core and Co3O4 species guaranteed the high reaction conversion and selectivity. Benefitting from heterogeneity and magnetism of the catalyst, it can be easily recycled and reused for long-term stability. Reasonable mechanisms of selective oxidation reaction were proposed through EPR analysis and controlled experiments. The present work provides a facile strategy for potential large-scale preparation of heterogeneous catalyst for sustainable and green catalytic transformations.
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