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<p>Facing with the problem of low activity at low temperatures of Ru-based ammonia decomposition catalyst, herein, the influence of Ru precursor and alkali metal modification on the hydrogen production activity of Ru/Pr<sub>6</sub>O<sub>11</sub> catalyst were studied. The Cs/Ru<sub>3</sub>(CO)<sub>12</sub>/Pr<sub>6</sub>O<sub>11</sub> catalyst exhibited the optimal activity (NH<sub>3</sub> conversion of 46.1% and H<sub>2</sub> production rate of 1.024 mmol·min<sup>−1</sup>·gcat<sup>−1</sup> at 350&#xa0;°C). Characterizations showed that Ru<sub>3</sub>(CO)<sub>12</sub>/Pr<sub>6</sub>O<sub>11</sub> has the smallest Ru particle size and the most uniform size distribution, and the existence of PrO<sub>2</sub> phase in Ru(NO)(NO<sub>3</sub>)<sub>3</sub>/Pr<sub>6</sub>O<sub>11</sub> and Cl<sup>−</sup> groups in RuCl<sub>3</sub>/Pr<sub>6</sub>O<sub>11</sub> reduce the activity. Additionally, due to hydrogen spillover, SMSI and Ru re-distribution, the more alkaline alkali metal has a stronger promoting effect, which follows the law of volcanic curve. In-situ DRIFTS and DFT calculations showed that the rate determining step on Ru(0001) surface is the first dehydrogenation step of NH<sub>3</sub> with the activation barrier of 2.19&#xa0;eV.</p>

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Study on the Effect and Mechanism of Ru Precursors and Alkali Metal Modification on Ru/Pr6O11 Catalysts for Ammonia Decomposition

  • 期刊论文

  • 发表日期：

    2025年4月4日

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  • Bin Guan,
  • Junyan Chen,
  • Zhongqi Zhuang,
  • Lei Zhu,
  • Zeren Ma,
  • Xuehan Hu,
  • Chenyu Zhu,
  • Sikai Zhao,
  • Kaiyou Shu,
  • Hongtao Dang,
  • Junjie Gao,
  • Luyang Zhang,
  • Tiankui Zhu,
  • Zhen Huang

摘要

Facing with the problem of low activity at low temperatures of Ru-based ammonia decomposition catalyst, herein, the influence of Ru precursor and alkali metal modification on the hydrogen production activity of Ru/Pr6O11 catalyst were studied. The Cs/Ru3(CO)12/Pr6O11 catalyst exhibited the optimal activity (NH3 conversion of 46.1% and H2 production rate of 1.024 mmol·min−1·gcat−1 at 350 °C). Characterizations showed that Ru3(CO)12/Pr6O11 has the smallest Ru particle size and the most uniform size distribution, and the existence of PrO2 phase in Ru(NO)(NO3)3/Pr6O11 and Cl− groups in RuCl3/Pr6O11 reduce the activity. Additionally, due to hydrogen spillover, SMSI and Ru re-distribution, the more alkaline alkali metal has a stronger promoting effect, which follows the law of volcanic curve. In-situ DRIFTS and DFT calculations showed that the rate determining step on Ru(0001) surface is the first dehydrogenation step of NH3 with the activation barrier of 2.19 eV.