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<p>The activation and valorization of inert molecules (e.g., dinitrogen (N<sub>2</sub>), alkanes, and alkenes) for the synthesis of nitrogen-containing organic compounds have long been a highly sought-after goal in chemistry. However, it remains a formidable challenge, stemming from the inherent chemical inertness of the robust N ≡ N and C-H bonds, as well as the competitive adsorption and activation of reactants. Consequently, examples of direct C-N bond formation using N<sub>2</sub> and alkanes/alkenes as feedstocks remain exceptionally scarce. Herein, we report that sodium hydride supported on magnesium oxide (NaH/MgO) possesses unique multiple reactive sites, which enable the conversion of N<sub>2</sub> and unactivated arenes and facilitate C-N bond formation. The synergistic interplay between sodium, magnesium, and hydride species at the NaH/MgO interface plays a pivotal role in the reduction of N<sub>2</sub> to NH<sub>x</sub> species. These reactive NH<sub>x</sub> intermediates then deprotonate the aryl C-H bond, attack the alkali-interacted aryl ring, and drive the formation of sodium anilide on the surface. Subsequent protonation of sodium anilide yields aniline with high selectivity (&gt;90%). This work demonstrates the feasibility of transforming N<sub>2</sub> and simple arenes into key nitrogen-containing organic compounds via a solid surface-mediated process, thereby opening ample room for developing heterogeneous catalysts for the transformation of N<sub>2</sub> and organic substrates.</p>

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Synthesis of aniline from dinitrogen and benzene mediated by magnesium oxide supported sodium hydride

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月9日

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  • Shixiong Zhang,
  • Yongli Cai,
  • Hong Wen,
  • Liang Liu,
  • Lei Yu,
  • Peng Zhang,
  • Jianping Guo,
  • Ping Chen

摘要

The activation and valorization of inert molecules (e.g., dinitrogen (N2), alkanes, and alkenes) for the synthesis of nitrogen-containing organic compounds have long been a highly sought-after goal in chemistry. However, it remains a formidable challenge, stemming from the inherent chemical inertness of the robust N ≡ N and C-H bonds, as well as the competitive adsorption and activation of reactants. Consequently, examples of direct C-N bond formation using N2 and alkanes/alkenes as feedstocks remain exceptionally scarce. Herein, we report that sodium hydride supported on magnesium oxide (NaH/MgO) possesses unique multiple reactive sites, which enable the conversion of N2 and unactivated arenes and facilitate C-N bond formation. The synergistic interplay between sodium, magnesium, and hydride species at the NaH/MgO interface plays a pivotal role in the reduction of N2 to NHx species. These reactive NHx intermediates then deprotonate the aryl C-H bond, attack the alkali-interacted aryl ring, and drive the formation of sodium anilide on the surface. Subsequent protonation of sodium anilide yields aniline with high selectivity (>90%). This work demonstrates the feasibility of transforming N2 and simple arenes into key nitrogen-containing organic compounds via a solid surface-mediated process, thereby opening ample room for developing heterogeneous catalysts for the transformation of N2 and organic substrates.