银掺杂调控锰铈催化剂的氧空位结构及碳烟燃烧性能

    Regulation of Oxygen Vacancy Structure and Soot Combustion Performance of Mn-Ce Catalysts by Ag Doping

    • 摘要: 为提升柴油机碳烟颗粒的催化燃烧效率,通过银(Ag)掺杂调控锰铈(Mn-Ce)催化剂的氧空位结构,系统探究其对碳烟燃烧性能的影响。采用共沉淀法制备不同锰铈比例的MnOx-CeO2复合催化剂(MnxCey),并通过浸渍法负载3%质量分数的Ag。通过表征分析催化剂的物化性质,并利用程序升温氧化试验分析了催化剂氧化碳烟的性能。研究发现,Ag负载后的Mn33Ce66Ag催化剂的起燃温度(T10=287 ℃)和完全燃烧温度(T90=332 ℃)进一步降低,且循环稳定性优异,三次循环后T90仅升至386 ℃。通过表征分析发现,Ag掺杂通过电子注入稳定Ce3+,增加表面活性氧物种物质的量的比,优化了氧空位浓度。H2程序升温还原证实Ag显著降低表面氧还原温度(Mn20Ce80Ag主还原峰从354.2 ℃移至282.2 ℃),加速氧活化,提高了还原性能。以上结果表明,Mn4+和Ce3+协同促进NO/O2活化,Ag通过抑制CeO2晶粒长大和增强金属−载体相互作用提升稳定性。

       

      Abstract: To enhance the catalytic combustion efficiency of diesel soot particles, the oxygen vacancy structure of Mn-Ce catalysts was modulated via silver (Ag) doping, and its effect on soot combustion performance was investigated. MnOx-CeO2 composite catalysts with different Mn-to-Ce ratios (MnxCey) were prepared using the co-precipitation method, followed by loading 3% mass percentage of Ag via impregnation. Through characterization of the physicochemical properties of the catalysts and temperature-programmed oxidation experiments, the catalytic performance for soot oxidation was analyzed. The results showed that after Ag loading, the Mn33Ce66Ag catalyst exhibited a lower ignition temperature (T10=287 ℃) and a lower complete combustion temperature (T90=332 ℃), along with excellent cyclic stability, as T90 only increased to 386 ℃ after three cycles. Characterization analysis results show that Ag doping stabilizes Ce3+ through electron injection, increases the molar ratio of surface active oxygen species, and optimizes the oxygen vacancy concentration. Through H2 temperature-programmed reduction, it is verified that Ag significantly reduces the surface oxygen reduction temperature (the main reduction peak of Mn20Ce80Ag shifted from 354.2 ℃ to 282.2 ℃), accelerates oxygen activation, and enhances reducibility. The results demonstrate that the synergy between Mn4+ and Ce3+ promotes the activation of NO/O2, while Ag improves stability by inhibiting CeO2 grain growth and enhancing metal−support interactions.

       

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