期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202313313
关键词
Ammoxidation; Electric Field; Heterogeneous Catalysis; Nitriles; Supported Clusters
This study reports an electric field enhanced ammoxidation system using a supported Fe clusters catalyst, which enables the synthesis of nitriles from aldehydes efficiently at room temperature and ambient air pressure. The synergistic effect between the external electric field and the catalyst promotes the activation of ammonia and dehydrogenation of imine intermediates, resulting in high efficiency and selectivity.
Heterogeneous catalytic ammoxidation provides an eco-friendly route for the cyanide-free synthesis of nitrile compounds, which are important precursors for synthetic chemistry and pharmaceutical applications. However, in general such a process requires high pressures of molecular oxygen at elevated temperatures to accelerate the oxygen reduction and imine dehydrogenation steps, which is highly risky in practical applications. Here, we report an electric field enhanced ammoxidation system using a supported Fe clusters catalyst (Fe/NC), which enables efficient synthesis of nitriles from the corresponding aldehydes under ambient air pressure at room temperature (RT). A synergistic effect between the external electric field and the Fe/NC catalyst promotes the ammonia activation and the dehydrogenation of the generated imine intermediates and avoids the unwanted backwards reaction to aldehydes. This electric field enhanced ammoxidation system presents high efficiency and selectivity for the conversion of a series of aldehydes under mild conditions with high durability, rendering it an attractive process for the green synthesis of nitriles with fragile functional groups. Ammoxidation of aldehydes under ambient oxygen pressure by external electric field and supported Fe clusters is reported. This ammoxidation system presents high efficiency for the conversion of a series of aldehydes under mild conditions, rendering it an attractive process for the synthesis of nitriles.image
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