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基于碳烟颗粒催化氧化的三维有序大孔催化剂制备及性能

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闫帅, 李水荣, 李宗沅, 王夺, 叶跃元, 刘运权. 基于碳烟颗粒催化氧化的三维有序大孔催化剂制备及性能[J]. 环境工程学报, 2018, 12(9): 2548-2557. doi: 10.12030/j.cjee.201803224
引用本文: 闫帅, 李水荣, 李宗沅, 王夺, 叶跃元, 刘运权. 基于碳烟颗粒催化氧化的三维有序大孔催化剂制备及性能[J]. 环境工程学报, 2018, 12(9): 2548-2557. doi: 10.12030/j.cjee.201803224
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YAN Shuai, LI Shuirong, LI Zongyuan, WANG Duo, YE Yueyuan, LIU Yunquan. Preparation of three-dimensionally ordered macroporous spinel-type catalysts and their performance for catalytic oxidation of soot[J]. Chinese Journal of Environmental Engineering, 2018, 12(9): 2548-2557. doi: 10.12030/j.cjee.201803224
Citation: YAN Shuai, LI Shuirong, LI Zongyuan, WANG Duo, YE Yueyuan, LIU Yunquan. Preparation of three-dimensionally ordered macroporous spinel-type catalysts and their performance for catalytic oxidation of soot[J]. Chinese Journal of Environmental Engineering, 2018, 12(9): 2548-2557. doi: 10.12030/j.cjee.201803224
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基于碳烟颗粒催化氧化的三维有序大孔催化剂制备及性能

  • 1.

    厦门大学能源学院，厦门 361102

  • 基金项目:

    国家自然科学基金资助项目（21276214）

    福建省科技厅重点项目（2016H6024）

    福建省自然科学基金资助项目（2015J05033）

Preparation of three-dimensionally ordered macroporous spinel-type catalysts and their performance for catalytic oxidation of soot

  • 1.

    College of Energy, Xiamen University, Xiamen 361102, China

  • Fund Project:

  • 摘要: 三维有序大孔钴锰尖晶石催化剂（3DOM CoMn2O4）以及三维有序大孔镧、铈掺杂的钴锰尖晶石催化剂（3DOM RxCo1-xMn2O4（R=Ce, La））由胶晶模板法成功合成。通过对所得的催化剂在NOx协助下的碳烟催化氧化活性评价，优化了Ce/Co和La/Co的配比。此外，还对目标催化剂进行了XRD、N2吸脱附、Raman、H2-TPR、SEM、XPS等表征。结果表明：3DOM结构增强了催化剂与碳烟颗粒之间的接触，对碳烟氧化等“固-固-气”非均相催化反应具有明显的提升作用。此外，铈和镧的掺杂增大了活性氧物种的浓度，从而增强了钴锰尖晶石催化剂的催化氧化能力。在松散接触工况下，3DOM Ce0.9Co0.1Mn2O4的Tig（起燃温度）和Tm（CO2出口浓度最大时的温度）分别为285 oC和377 oC，3DOM La0.3Co0.7Mn2O4的Tig和Tm分别为287 oC和376 oC。
    Abstract: Three-dimensionally ordered macroporous (3DOM) CoMn2O4 and 3DOM RxCo1-xMn2O4(R=Ce, La) spinel were successfully synthesized with the colloidal crystal template method. The catalytic activities of these catalysts for NOx-assisted soot combustion were evaluated, and the optimum ratios of Ce/Co and La/Co were determined. XRD, SEM, N2 adsorption-desorption, XPS, Raman and H2-TPR were employed to characterize the prepared samples. It was found that 3DOM structure provides better contact between soot and catalysts compared to other structures，thus promoting the heterogeneous catalytic soot oxidations in solid-solid-gas interfaces. In addition, the doping of cerium or lanthanum improved the catalytic oxidation capability of spinels by increasing the concentrations of active oxygen species. And under loose contact, Tig = 285 oC and Tm = 377 oC were achieved for 3DOM Ce0.9Co0.1Mn2O4 catalysts, while Tig = 287 oC and Tm = 376 oC were achieved for 3DOM La0.3Co0.7Mn2O4, both of which are the enhanced catalytic activities.
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  • 刊出日期:  2018-09-20

基于碳烟颗粒催化氧化的三维有序大孔催化剂制备及性能

  • 1. 厦门大学能源学院，厦门 361102
基金项目:

国家自然科学基金资助项目（21276214）

福建省科技厅重点项目（2016H6024）

福建省自然科学基金资助项目（2015J05033）

摘要: 三维有序大孔钴锰尖晶石催化剂（3DOM CoMn2O4）以及三维有序大孔镧、铈掺杂的钴锰尖晶石催化剂（3DOM RxCo1-xMn2O4（R=Ce, La））由胶晶模板法成功合成。通过对所得的催化剂在NOx协助下的碳烟催化氧化活性评价，优化了Ce/Co和La/Co的配比。此外，还对目标催化剂进行了XRD、N2吸脱附、Raman、H2-TPR、SEM、XPS等表征。结果表明：3DOM结构增强了催化剂与碳烟颗粒之间的接触，对碳烟氧化等“固-固-气”非均相催化反应具有明显的提升作用。此外，铈和镧的掺杂增大了活性氧物种的浓度，从而增强了钴锰尖晶石催化剂的催化氧化能力。在松散接触工况下，3DOM Ce0.9Co0.1Mn2O4的Tig（起燃温度）和Tm（CO2出口浓度最大时的温度）分别为285 oC和377 oC，3DOM La0.3Co0.7Mn2O4的Tig和Tm分别为287 oC和376 oC。

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