Lowering the Cu-O bond energy in CuO nanocatalysts enhances the efficiency of NH<sub>3</sub> oxidation.

Chen, Lu; Guan, Xuze; Yao, Zhangyi; Hayama, Shusaku; Spronsen, Matthijs A van; Karagoz, Burcu; Held, Georg; Hopkinson, David G et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

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 1s → 4p<sub>z</sub> 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 Co<sub>B</sub>Cu/Al<sub>2</sub>O<sub>3</sub> 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 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>.