Low pressure amide hydrogenation enabled by magnetocatalysis

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Sheng-Hsiang Lin, Sihana Ahmedi, Aaron Kretschmer, Carlotta Campalani, Yves Kayser, Liqun Kang, Serena DeBeer, Walter Leitner, Alexis Bordet
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引用次数: 0

Abstract

The catalytic hydrogenation of amides with molecular hydrogen (H2) is an appealing route for the synthesis of valuable amines entering in the preparation of countless organic compounds. Running effective amide hydrogenation under mild H2 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/Al2O3) 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/Al2O3 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 H2. ICNPs@Pt/Al2O3 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.

Abstract Image

通过磁催化实现低压酰胺加氢
用分子氢(H2)催化酰胺的加氢反应是合成有价值胺的一种有吸引力的途径,进入了无数有机化合物的制备中。在温和的氢气压力下进行有效的酰胺加氢是具有挑战性的,尽管在研究和工业中需要排除专门的高压技术。在这里,我们表明用标准负载催化剂的磁催化可以在温和的条件下实现前所未有的酰胺氢化。用碳化铁纳米颗粒(ICNPs)功能化氧化铝上广泛使用的商用铂(Pt/Al2O3),以实现局部和快速的磁感应加热,从而通过热能传递激活邻近的Pt位点。将ICNPs@Pt/Al2O3催化剂暴露在交流磁场中,可以在反应器温度为150°C、3 bar甚至环境压力为H2的条件下,对一系列酰胺进行高活性和选择性的加氢反应。ICNPs@Pt/Al2O3对电力供应的波动做出适应性反应,模仿间歇性可再生能源的使用。这项工作可能为在实验室和生产规模上大大提高酰胺加氢的实用性铺平道路,并更广泛地展示了合成化学中新兴磁催化领域的广阔潜力。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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