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    LaMn1−xCuxO3钙钛矿催化剂的组成优化、氧迁移特性及CO氧化性能研究

    Composition Optimization, Oxygen Mobility Characteristics, and CO Oxidation Performance of LaMn1−xCuxO3 Perovskite Catalysts

    • 摘要: CO催化氧化是消除低浓度一氧化碳污染物的重要途径,开发高活性非贵金属氧化物催化剂具有重要意义。针对LaMnO3低温CO氧化活性不足的问题,采用溶胶凝胶法制备了LaMn1−xCuxO3系列钙钛矿催化剂,并系统考察了Cu掺杂量对其CO催化氧化性能的影响。结果表明,Cu掺杂显著提升了LaMnO3的CO氧化活性,系列样品活性随Cu含量增加呈火山型变化,其中LaMn0.6Cu0.4O3表现最佳,T50和T90分别为136 ℃和150 ℃。表征结果表明,LaMn0.6Cu0.4O3优异的CO氧化性能主要归因于Cu-Mn协同作用、表面电子结构调控以及表面活性氧与晶格氧参与能力的增强,反应过程遵循以Mars-van Krevelen机制为主的氧化路径。

       

      Abstract: Catalytic oxidation of CO is an important strategy for eliminating low-concentration carbon monoxide pollutants, and the development of highly active non-noble-metal oxide catalysts is therefore of considerable significance. To address the insufficient low-temperature activity of LaMnO3 for CO oxidation, a series of LaMn1−xCuxO3 perovskite catalysts was prepared by the sol-gel method, and the effect of Cu doping level on their catalytic performance for CO oxidation was systematically investigated. The results show that Cu doping markedly enhances the CO oxidation activity of LaMnO3. The catalytic activity of the series exhibits a volcano-type dependence on Cu content, among which LaMn0.6Cu0.4O3 delivers the best performance, with T50 and T90 values of 136 and 150 °C, respectively. Characterization results indicate that the outstanding CO oxidation performance of LaMn0.6Cu0.4O3 mainly originates from the Cu-Mn synergistic effect, regulation of the surface electronic structure, and the enhanced participation of surface-active oxygen and lattice oxygen. The reaction is proposed to proceed predominantly via a Mars-van Krevelen pathway. This study provides a materials basis for the development of low-cost non-noble-metal catalysts and offers experimental support for understanding the synergistic roles of active oxygen, lattice oxygen, and metal centers in CO oxidation.

       

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