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磁催化实现的低压酰胺加氢反应

Low pressure amide hydrogenation enabled by magnetocatalysis.

作者信息

Lin Sheng-Hsiang, Ahmedi Sihana, Kretschmer Aaron, Campalani Carlotta, Kayser Yves, Kang Liqun, DeBeer Serena, Leitner Walter, Bordet Alexis

机构信息

Max Planck Institute for Chemical Energy Conversion, Mülheim an der Ruhr, Germany.

Institute of Technical and Macromolecular Chemistry, RWTH Aachen University, Aachen, Germany.

出版信息

Nat Commun. 2025 Apr 11;16(1):3464. doi: 10.1038/s41467-025-58713-6.

DOI:10.1038/s41467-025-58713-6
PMID:40216784
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11992221/
Abstract

The catalytic hydrogenation of amides with molecular hydrogen (H) is an appealing route for the synthesis of valuable amines entering in the preparation of countless organic compounds. Running effective amide hydrogenation under mild H pressures is challenging although desirable to preclude the need for specialized high-pressure technologies in research and industry. Here we show that magnetocatalysis with standard supported catalysts enables unprecedented amide hydrogenation at mild conditions. Widely available and commercial platinum on alumina (Pt/AlO) was functionalized with iron carbide nanoparticles (ICNPs) to allow for localized and rapid magnetic induction heating resulting in the activation of neighboring Pt sites by thermal energy transfer. Exposure of the ICNPs@Pt/AlO catalyst to an alternating current magnetic field enables highly active and selective hydrogenation of a range of amides at a reactor temperature of 150 °C under 3 bar or even ambient pressure of H. ICNPs@Pt/AlO reacts adaptively to fluctuations in electricity supply mimicking the use of intermittent renewable energy sources. This work may pave the way toward a greatly enhanced practicability of amide hydrogenation at the laboratory and production scales, and demonstrates more generally the broad potential of the emerging field of magnetocatalysis for synthetic chemistry.

摘要

利用分子氢(H₂)对酰胺进行催化加氢是合成有价值胺类的一条有吸引力的途径,这些胺类可用于制备无数有机化合物。在温和的氢气压力下进行有效的酰胺加氢具有挑战性,尽管在研究和工业中避免使用专门的高压技术是很理想的。在这里,我们表明,使用标准负载型催化剂的磁催化能够在温和条件下实现前所未有的酰胺加氢。用碳化铁纳米颗粒(ICNPs)对广泛可得的商业氧化铝负载铂(Pt/Al₂O₃)进行功能化,以实现局部快速磁感应加热,从而通过热能传递激活相邻的铂位点。将ICNPs@Pt/Al₂O₃催化剂暴露于交变磁场中,能够在3巴甚至氢气的环境压力下,于150℃的反应器温度下对一系列酰胺进行高活性和选择性加氢。ICNPs@Pt/Al₂O₃能自适应地应对电力供应的波动,类似于使用间歇性可再生能源。这项工作可能为酰胺加氢在实验室和生产规模上大大提高实用性铺平道路,并更广泛地展示了磁催化这一新兴领域在合成化学中的广阔潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/36ee6d5bb184/41467_2025_58713_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/cbc036c070ea/41467_2025_58713_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/2e80bf74fe0e/41467_2025_58713_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/d3feeb127833/41467_2025_58713_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/f29f915f73c5/41467_2025_58713_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/36ee6d5bb184/41467_2025_58713_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/cbc036c070ea/41467_2025_58713_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/2e80bf74fe0e/41467_2025_58713_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/d3feeb127833/41467_2025_58713_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/f29f915f73c5/41467_2025_58713_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54be/11992221/36ee6d5bb184/41467_2025_58713_Fig5_HTML.jpg

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