徐大为, 张家琳, 高越, 李新刚. 核壳结构Co3O4@MnOx整体式催化剂的碳烟催化燃烧性能[J]. 燃料化学学报(中英文), 2024, 52(2): 184-194. DOI: 10.19906/j.cnki.JFCT.2023057
引用本文: 徐大为, 张家琳, 高越, 李新刚. 核壳结构Co3O4@MnOx整体式催化剂的碳烟催化燃烧性能[J]. 燃料化学学报(中英文), 2024, 52(2): 184-194. DOI: 10.19906/j.cnki.JFCT.2023057
XU Dawei, ZHANG Jialin, GAO Yue, LI Xingang. Catalytic soot combustion performance of core-shell Co3O4@MnOx monolithic catalyst[J]. Journal of Fuel Chemistry and Technology, 2024, 52(2): 184-194. DOI: 10.19906/j.cnki.JFCT.2023057
Citation: XU Dawei, ZHANG Jialin, GAO Yue, LI Xingang. Catalytic soot combustion performance of core-shell Co3O4@MnOx monolithic catalyst[J]. Journal of Fuel Chemistry and Technology, 2024, 52(2): 184-194. DOI: 10.19906/j.cnki.JFCT.2023057

核壳结构Co3O4@MnOx整体式催化剂的碳烟催化燃烧性能

Catalytic soot combustion performance of core-shell Co3O4@MnOx monolithic catalyst

  • 摘要: 采用两步水热法在泡沫镍基底上合成了具有纳米棒形貌的 Co3O4@MnOx 整体式催化剂,通过X射线衍射、X射线能谱分析、氢气-程序升温还原、X射线光电子能谱、拉曼光谱和碳烟-程序升温还原等手段对催化剂进行表征,在微型固定床反应器上评价了其催化碳烟燃烧性能,通过等温动力学实验探究了催化剂的本征活性。结果表明,Co3O4@MnOx 催化剂呈现了以 Co3O4 为核、以 MnOx 为壳的核壳结构。与催化剂 Co-NW 相比,Co3O4@MnOx 催化剂中 Co3O4 与 MnOx 之间的相互作用使其表面产生了更多高价物种 Mn4+ 和 Mn3+ 以及更多的表面氧空位,其氧化还原性能提高,催化剂的活性氧物种数量增加了两倍,催化性能得到改善,在 NO 存在的反应气氛中使碳烟起燃温度降低148 ℃。此外,相比催化剂 Co-NW,Co3O4@MnOx 催化剂使碳烟燃烧反应的活化能从113.6 kJ/mol降低至102.2 kJ/mol,催化剂的本征活性提高了两倍。

     

    Abstract: The Co3O4@MnOx monolithic catalyst with nanorod morphology was synthesized on nickel foam by a two-step hydrothermal process and characterized by XRD, EDS-mapping, H2-TPR, XPS, Raman and Soot-TPR. The catalytic soot combustion activities of the catalysts were investigated in a fixed-bed micro-reactor and the intrinsic activities of the catalysts were investigated by the isothermal kinetic experiments. The results reveal that the Co3O4@MnOx catalyst shows a core-shell structure with Co3O4 as the core and MnOx as the shell. Compared with Co-NW, there exist more high-valent state species of Mn4+ and Mn3+ and oxygen vacancies on the Co3O4@MnOx catalyst surface due to the interaction between Co3O4 and MnOx, which improve the redox performance of Co3O4@MnOx. Compared with Co-NW, the active oxygen species amount of Co3O4@MnOx is increased by two times, and Co3O4@MnOx shows enhanced activity, which lowers the ignition temperature by 148 ℃ in the presence of NO. Also, compared with Co-NW, Co3O4@MnOx decreases the activation energy of soot combustion reaction from 113.6 to 102.2 kJ/mol, and its intrinsic activity is increased by two times.

     

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