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

IF 15.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2025-10-24 DOI:10.1038/s41467-025-64415-w

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

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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 (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.

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降低CuO纳米催化剂中Cu-O键能可提高NH3氧化效率。

通过掺杂单分散的杂金属原子来调整纳米催化剂的电子性能是一种提高催化性能的有效方法。用不同的还原剂掺杂单分散Co原子的CuO纳米颗粒，使催化剂（cocu /Al2O3和CoHCu/Al2O3）具有明显不同的电子结构。与CoHCu/Al2O3相比，CoHCu/Al2O3中的CuO纳米粒子具有更长的、更弱的Cu-O键，具有更低的1s→4pz反键转变和更高的4p→1s键转变（从herdf - xanes和价核x射线发射光谱中可以看出）。通过对CoBCu/Al2O3中较弱的Cu-O键导致CuO纳米颗粒具有较好的氧化还原活性，这一点从操作氧化物XAFS和近环境压力近边缘x射线吸收精细结构的研究中得到了证明。与CoHCu/Al2O3相比，CoHCu/Al2O3中CuO优异的氧化还原性能使CoHCu/Al2O3的活化能大大降低（40.0 kJ/mol vs. 63.5 kJ/mol），从而提高了选择性催化氧化NH3生成N2的催化性能。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.