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<p>Tuning the electronic properties of nanocatalysts via doping with monodispersed hetero-metal atoms is an effective method used to enhance catalytic properties. Doping CuO nanoparticles with monodispersed Co atoms using different reductants affords catalysts (Co<sub>B</sub>Cu/Al<sub>2</sub>O<sub>3</sub> and Co<sub>H</sub>Cu/Al<sub>2</sub>O<sub>3</sub>) with strikingly different electronic structures. Compared to Co<sub>H</sub>Cu/Al<sub>2</sub>O<sub>3</sub>, the CuO nanoparticles in Co<sub>B</sub>Cu/Al<sub>2</sub>O<sub>3</sub> have longer and weaker Cu-O bonds, with a lower 1<i>s</i> → 4<i>p</i><sub>z</sub> antibonding transition and higher 4<i>p</i> →&#xa0;1<i>s</i> bonding transition (as demonstrated from HERFD-XANES and valence-to-core X-ray emission spectroscopy). The weaker Cu-O bonds in Co<sub>B</sub>Cu/Al<sub>2</sub>O<sub>3</sub> lead to superior redox activity of the CuO nanoparticles, evidenced from <i>operando</i> XAFS and in-situ near ambient pressure-near edge X-ray absorption fine structures studies. Such superior redox properties of CuO in Co<sub>B</sub>Cu/Al<sub>2</sub>O<sub>3</sub> result in a much reduced activation energy of Co<sub>B</sub>Cu/Al<sub>2</sub>O<sub>3</sub> compared to Co<sub>H</sub>Cu/Al<sub>2</sub>O<sub>3</sub> (40.0 vs. 63.5 kJ/mol), thus leading to an enhancement in catalytic performance in the selective catalytic oxidation of NH<sub>3</sub> to N<sub>2</sub>.</p>

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Lowering the Cu-O bond energy in CuO nanocatalysts enhances the efficiency of NH3 oxidation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月24日

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  • Lu Chen,
  • Xuze Guan,
  • Zhangyi Yao,
  • Shusaku Hayama,
  • Matthijs A. van Spronsen,
  • Burcu Karagoz,
  • Georg Held,
  • David G. Hopkinson,
  • Christopher S. Allen,
  • June Callison,
  • Paul J. Dyson,
  • Feng Ryan Wang

摘要

Tuning the electronic properties of nanocatalysts via doping with monodispersed hetero-metal atoms is an effective method used to enhance catalytic properties. Doping CuO nanoparticles with monodispersed Co atoms using different reductants affords catalysts (CoBCu/Al2O3 and CoHCu/Al2O3) with strikingly different electronic structures. Compared to CoHCu/Al2O3, the CuO nanoparticles in CoBCu/Al2O3 have longer and weaker Cu-O bonds, with a lower 1s → 4pz antibonding transition and higher 4p → 1s bonding transition (as demonstrated from HERFD-XANES and valence-to-core X-ray emission spectroscopy). The weaker Cu-O bonds in CoBCu/Al2O3 lead to superior redox activity of the CuO nanoparticles, evidenced from operando XAFS and in-situ near ambient pressure-near edge X-ray absorption fine structures studies. Such superior redox properties of CuO in CoBCu/Al2O3 result in a much reduced activation energy of CoBCu/Al2O3 compared to CoHCu/Al2O3 (40.0 vs. 63.5 kJ/mol), thus leading to an enhancement in catalytic performance in the selective catalytic oxidation of NH3 to N2.