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<p>Selective catalytic oxidation (SCO) of NH<sub>3</sub> to N<sub>2</sub> is one of the most effective methods used to eliminate NH<sub>3</sub> emissions. However, achieving high conversion over a wide operating temperature range while avoiding over-oxidation to NO<sub>x</sub> remains a significant challenge. Here, we report a bi-metallic surficial catalyst (Pt<sub>S</sub>CuO/Al<sub>2</sub>O<sub>3</sub>) with improved Pt atom efficiency that overcomes the limitations of current catalysts. It achieves full NH<sub>3</sub> conversion at 250 °C with a weight hourly space velocity of 600 ml NH<sub>3</sub>·h<sup>−1</sup>·g<sup>−1</sup>, which is 50 °C lower than commercial Pt/Al<sub>2</sub>O<sub>3</sub>, and maintains high N<sub>2</sub> selectivity through a wide temperature window. <i>Operando</i> XAFS studies reveal that the surface Pt atoms in Pt<sub>S</sub>CuO/Al<sub>2</sub>O<sub>3</sub> enhance the redox properties of the Cu species, thus accelerating the Cu<sup>2+</sup> reduction rate and improving the rate of the NH<sub>3</sub>-SCO reaction. Moreover, a synergistic effect between Pt and Cu sites in Pt<sub>S</sub>CuO/Al<sub>2</sub>O<sub>3</sub> contributes to the high selectivity by facilitating internal selective catalytic reduction.</p>

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Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年1月2日

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  • Lu Chen,
  • Xuze Guan,
  • Zhaofu Fei,
  • Hiroyuki Asakura,
  • Lun Zhang,
  • Zhipeng Wang,
  • Xinlian Su,
  • Zhangyi Yao,
  • Luke L. Keenan,
  • Shusaku Hayama,
  • Matthijs A. van Spronsen,
  • Burcu Karagoz,
  • Georg Held,
  • Christopher S. Allen,
  • David G. Hopkinson,
  • Donato Decarolis,
  • June Callison,
  • Paul J. Dyson,
  • Feng Ryan Wang

摘要

Selective catalytic oxidation (SCO) of NH3 to N2 is one of the most effective methods used to eliminate NH3 emissions. However, achieving high conversion over a wide operating temperature range while avoiding over-oxidation to NOx remains a significant challenge. Here, we report a bi-metallic surficial catalyst (PtSCuO/Al2O3) with improved Pt atom efficiency that overcomes the limitations of current catalysts. It achieves full NH3 conversion at 250 °C with a weight hourly space velocity of 600 ml NH3·h−1·g−1, which is 50 °C lower than commercial Pt/Al2O3, and maintains high N2 selectivity through a wide temperature window. Operando XAFS studies reveal that the surface Pt atoms in PtSCuO/Al2O3 enhance the redox properties of the Cu species, thus accelerating the Cu2+ reduction rate and improving the rate of the NH3-SCO reaction. Moreover, a synergistic effect between Pt and Cu sites in PtSCuO/Al2O3 contributes to the high selectivity by facilitating internal selective catalytic reduction.