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<p>Ammonia is a promising hydrogen storage carrier due to its high hydrogen density (17.8 wt %) and mild liquefaction conditions. Plasma-catalytic ammonia synthesis is an alternative synthesis route regarding green ammonia generation at ambient conditions. In this study, Co-doped Mo<sub>2</sub>N-Co catalysts were developed to enhance plasma-catalytic ammonia synthesis, with a focus on the effects of Co/Mo molar ratios and operating parameters. Among the catalysts tested, Mo<sub>2</sub>N-Co<sub>1</sub> possessed the highest ammonia synthesis rate and energy efficiency. Optimal operating conditions including a feed ratio of N<sub>2</sub>:H<sub>2</sub> = 1:1 and a higher discharge power is favored. An ammonia synthesis rate of 11925 µmol·g<sup>−1</sup>·h<sup>−1</sup> and an energy efficiency of 3.6 g-NH<sub>3</sub>·kWh<sup>−1</sup> were achieved over Mo<sub>2</sub>N-Co<sub>1</sub> at a feed ratio of N<sub>2</sub>:H<sub>2</sub> = 1:1 and a discharge power of 57 W. Comprehensive characterizations, including X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, electron paramagnetic resonance, hydrogen temperature-programmed reduction, and ammonia temperature-programmed desorption, demonstrated that Co doping introduced abundant nitrogen vacancies and weak acidic surface, both of which facilitated ammonia desorption and electron transfer. Key reactive intermediates were identified using optical emission spectroscopy, providing insight into the proposed reaction mechanism for this synergistic plasma-catalytic ammonia synthesis over Mo<sub>2</sub>N-Co catalysts.</p>

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Co-doping facilitated plasma-catalytic ammonia synthesis over Mo2N-Co catalysts

  • 期刊论文

  • 发表日期：

    2025年7月30日

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  • Yutong Feng,
  • Bianbian Gao,
  • Guoqiang Cao,
  • Donghai Hu,
  • Yuting Jiao,
  • Chunyu Li,
  • Jiantao Zhao,
  • Yitian Fang

摘要

Ammonia is a promising hydrogen storage carrier due to its high hydrogen density (17.8 wt %) and mild liquefaction conditions. Plasma-catalytic ammonia synthesis is an alternative synthesis route regarding green ammonia generation at ambient conditions. In this study, Co-doped Mo2N-Co catalysts were developed to enhance plasma-catalytic ammonia synthesis, with a focus on the effects of Co/Mo molar ratios and operating parameters. Among the catalysts tested, Mo2N-Co1 possessed the highest ammonia synthesis rate and energy efficiency. Optimal operating conditions including a feed ratio of N2:H2 = 1:1 and a higher discharge power is favored. An ammonia synthesis rate of 11925 µmol·g−1·h−1 and an energy efficiency of 3.6 g-NH3·kWh−1 were achieved over Mo2N-Co1 at a feed ratio of N2:H2 = 1:1 and a discharge power of 57 W. Comprehensive characterizations, including X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, electron paramagnetic resonance, hydrogen temperature-programmed reduction, and ammonia temperature-programmed desorption, demonstrated that Co doping introduced abundant nitrogen vacancies and weak acidic surface, both of which facilitated ammonia desorption and electron transfer. Key reactive intermediates were identified using optical emission spectroscopy, providing insight into the proposed reaction mechanism for this synergistic plasma-catalytic ammonia synthesis over Mo2N-Co catalysts.