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Electric Field Enhanced Ammoxidation of Aldehydes Using Supported Fe Clusters Under Ambient Oxygen Pressure.

Authors
  • Wang, Chao1, 2
  • Li, Jialu1, 2
  • Shao, Tianyu1, 2
  • Zhang, Dongsheng1, 2
  • Mai, Yuanqiang1, 2
  • Li, Yongwang2, 3
  • Besenbacher, Flemming4
  • Niemantsverdriet, Hans2, 5
  • Rosei, Federico6
  • Zhong, Jun7
  • Su, Ren1, 2
  • 1 Soochow Institute for Energy and Materials InnovationS (SIEMIS), Soochow University, Suzhou, 215006, China. , (China)
  • 2 SynCat@Beijing, Synfuels China Technology Co. Ltd., Leyuan South Street II, No.1, Yanqi Economic Development Zone C#, Beijing, 101407, China. , (China)
  • 3 State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, CAS, Taiyuan, 030001, China. , (China)
  • 4 Interdisciplinary Nanoscience Center, Aarhus University, Gustav Wieds Vej 14, 8000, Aarhus, Denmark. , (Denmark)
  • 5 Syngaschem BV, Valeriaanlaan 16, 5672 XD, Nuenen (The, Netherlands. , (Netherlands)
  • 6 Department of Chemical and Pharmaceutical Sciences, University of Trieste, Via Giorgeri 1, 34127, Trieste, Italy. , (Italy)
  • 7 Institute of Functional Nano and Soft Materials Laboratory (FUNSOM), Soochow University, Suzhou, 215123, China. , (China)
Type
Published Article
Journal
Angewandte Chemie International Edition in English
Publisher
Wiley (John Wiley & Sons)
Publication Date
Dec 18, 2023
Volume
62
Issue
51
Identifiers
DOI: 10.1002/anie.202313313
PMID: 37930876
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

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. © 2023 Wiley-VCH GmbH.

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