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

Abstract

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.