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<p>The sustainable synthesis on ammonia at mild thermal conditions is a pivotal goal in catalysis, yet finding efficient alternatives to the energy-intensive Haber-Bosch process remains a great challenge. Here we show that a composite material comprising uranium and few-layer graphdiyne (U/GDY) catalyzes ammonia production with high efficiency at low temperature and pressure. We synthesize few-layer GDY in supercritical CO<sub>2</sub> to create a stable scaffold that hosts uranium in specific valency and cluster states. Both experimental results and theoretical calculations reveal that the unique electronic interplay between the 5 <i>f</i> electrons of uranium and the conjugated structure of GDY optimizes the adsorption and activation of nitrogen. This synergism facilitates a favorable reaction pathway involving specific nitrogen recognition and efficient product release. Our findings demonstrate the potential of uranium-based composites in catalysis and offer a strategy for designing actinide-carbon hybrid materials in challenging chemical transformations.</p>

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Thermal catalytic synthesis of ammonia using uranium/graphdiyne composite at mild conditions

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年2月18日

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  • Shijie Xiong,
  • Weiyi Wang,
  • Fan Wang,
  • Shengxiang Li,
  • Yuying Liu,
  • Zhiwen Zhuo,
  • Yuchen Zhang,
  • Xinghai Shen

摘要

The sustainable synthesis on ammonia at mild thermal conditions is a pivotal goal in catalysis, yet finding efficient alternatives to the energy-intensive Haber-Bosch process remains a great challenge. Here we show that a composite material comprising uranium and few-layer graphdiyne (U/GDY) catalyzes ammonia production with high efficiency at low temperature and pressure. We synthesize few-layer GDY in supercritical CO2 to create a stable scaffold that hosts uranium in specific valency and cluster states. Both experimental results and theoretical calculations reveal that the unique electronic interplay between the 5 f electrons of uranium and the conjugated structure of GDY optimizes the adsorption and activation of nitrogen. This synergism facilitates a favorable reaction pathway involving specific nitrogen recognition and efficient product release. Our findings demonstrate the potential of uranium-based composites in catalysis and offer a strategy for designing actinide-carbon hybrid materials in challenging chemical transformations.