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

Author

Listed:
  • Lu Chen

    (University College London)

  • Xuze Guan

    (University College London)

  • Zhaofu Fei

    (École Polytechnique Fedérale de Lausanne (EPFL))

  • Hiroyuki Asakura

    (Higashi-Osaka)

  • Lun Zhang

    (University College London)

  • Zhipeng Wang

    (University College London)

  • Xinlian Su

    (University College London)

  • Zhangyi Yao

    (University College London)

  • Luke L. Keenan

    (Chilton)

  • Shusaku Hayama

    (Chilton)

  • Matthijs A. Spronsen

    (Chilton)

  • Burcu Karagoz

    (Chilton)

  • Georg Held

    (Chilton)

  • Christopher S. Allen

    (Chilton
    University of Oxford)

  • David G. Hopkinson

    (Chilton)

  • Donato Decarolis

    (Chilton
    Rutherford Appleton Laboratory)

  • June Callison

    (Rutherford Appleton Laboratory)

  • Paul J. Dyson

    (École Polytechnique Fedérale de Lausanne (EPFL))

  • Feng Ryan Wang

    (University College London)

Abstract

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.

Suggested Citation

  • Lu Chen & Xuze Guan & Zhaofu Fei & Hiroyuki Asakura & Lun Zhang & Zhipeng Wang & Xinlian Su & Zhangyi Yao & Luke L. Keenan & Shusaku Hayama & Matthijs A. Spronsen & Burcu Karagoz & Georg Held & Christ, 2025. "Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites," Nature Communications, Nature, vol. 16(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-024-54820-y
    DOI: 10.1038/s41467-024-54820-y
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    References listed on IDEAS

    as
    1. Suzanne Z. Andersen & Viktor Čolić & Sungeun Yang & Jay A. Schwalbe & Adam C. Nielander & Joshua M. McEnaney & Kasper Enemark-Rasmussen & Jon G. Baker & Aayush R. Singh & Brian A. Rohr & Michael J. St, 2019. "Author Correction: A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements," Nature, Nature, vol. 574(7777), pages 5-5, October.
    2. Suzanne Z. Andersen & Viktor Čolić & Sungeun Yang & Jay A. Schwalbe & Adam C. Nielander & Joshua M. McEnaney & Kasper Enemark-Rasmussen & Jon G. Baker & Aayush R. Singh & Brian A. Rohr & Michael J. St, 2019. "A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements," Nature, Nature, vol. 570(7762), pages 504-508, June.
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