Enhancing Catalytic Removal of Autoexhaust Soot Particles via the Modulation of Interfacial Oxygen Vacancies in Cu/CeO2 Catalysts

The purification efficiency of autoexhaust carbon strongly depends on the heterogeneous interface structure between active metal and oxide, which can modulate the local electronic structure of defect sites to promote the activation of reactant molecules. Herein, the high-dispersion CuO clusters supp...

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Veröffentlicht in:Environmental science & technology 2025-01, Vol.59 (4), p.2327-2338
Hauptverfasser: Li, Yuanfeng, Qin, Tian, Xu, Linsheng, Ma, Yaxiao, Guo, Haoqi, Xiong, Jing, Zhang, Peng, Zhao, Zhen, Liu, Xi, Liu, Yunpeng, Zou, Jianping, Chen, Liwei, Wei, Yuechang
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Sprache:eng
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Zusammenfassung:The purification efficiency of autoexhaust carbon strongly depends on the heterogeneous interface structure between active metal and oxide, which can modulate the local electronic structure of defect sites to promote the activation of reactant molecules. Herein, the high-dispersion CuO clusters supported on the well-defined CeO2 nanorods were prepared using the complex deposition slow method. The formation of heteroatomic Cu+-Ov-Ce3+ interfacial structural units as active sites can capture electrons to achieve activation of the NO and O2 molecules. Among all of the synthesized catalysts, the Cu10/CeO2 catalyst exhibits superior catalytic performance (T 50 = 351 °C) along with remarkable tolerance to H2O and SO2 in the removal of soot particles. Through a combination of comprehensive characterizations and density functional theory calculations, it is proposed that the interfacial Cu+-Ov-Ce3+ site, acting as an electron enrichment center, can capture electrons from the Cu d-band and Ce d/f-band to obtain high delocalized electron density, and then enhance the oxidation of NO to NO2, which plays a crucial role in the NO x -assisted catalytic mechanism for soot oxidation. This study presents a novel strategy for developing highly efficient catalysts that exhibit resistance to H2O and SO2, aimed at enhancing the removal of soot particles.
ISSN:0013-936X
1520-5851
1520-5851
DOI:10.1021/acs.est.4c12325