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<p>Ammonia (NH<sub>3</sub>) has gained attention as a carbon-free fuel and hydrogen carrier, making its energy-efficient production increasingly important. Here we demonstrate that Ru and BaO, connected by conductive carbon, can separately store e<sup>−</sup> and H<sup>+</sup>, like a chemical capacitor under NH<sub>3</sub> synthesis conditions. H atoms generated on the Ru surface by H<sub>2</sub> activation polarize into H<sup>+</sup>/e<sup>−</sup> pairs. Subsequently, H<sup>+</sup> migrates over the carbon surfaces to neutralize basic BaO, while e<sup>−</sup> accumulates in conductive Ru/carbon. As the work function of carbon decreases, Ru gradually becomes enriched with e<sup>−</sup>, facilitating N<sub>2</sub> activation via π-backdonation and alleviating H<sub>2</sub> poisoning. Thus, an optimized catalyst synthesized using N-doped MWNT with the lowest work function, exhibited 7.4 times higher activity than a reference Ba–Ru/MgO catalyst. The results show that charge distribution within catalysts can be markedly altered under reaction conditions, and its rational control can enable the design of active NH<sub>3</sub> synthesis catalysts.</p><p></p>

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Electron and proton storage on separate Ru and BaO domains mediated by conductive low-work-function carbon to accelerate ammonia synthesis

  • 期刊论文

  • 发表日期：

    2025年2月24日

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  • Yaejun Baik,
  • Seunghyuck Chi,
  • Kyeongjin Lee,
  • DongHwan Oh,
  • Kyungho Lee,
  • Minkee Choi

摘要

Ammonia (NH3) has gained attention as a carbon-free fuel and hydrogen carrier, making its energy-efficient production increasingly important. Here we demonstrate that Ru and BaO, connected by conductive carbon, can separately store e− and H+, like a chemical capacitor under NH3 synthesis conditions. H atoms generated on the Ru surface by H2 activation polarize into H+/e− pairs. Subsequently, H+ migrates over the carbon surfaces to neutralize basic BaO, while e− accumulates in conductive Ru/carbon. As the work function of carbon decreases, Ru gradually becomes enriched with e−, facilitating N2 activation via π-backdonation and alleviating H2 poisoning. Thus, an optimized catalyst synthesized using N-doped MWNT with the lowest work function, exhibited 7.4 times higher activity than a reference Ba–Ru/MgO catalyst. The results show that charge distribution within catalysts can be markedly altered under reaction conditions, and its rational control can enable the design of active NH3 synthesis catalysts.