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甲烷催化燃烧反应机理及催化剂研究进展

楚培齐 王赛飞 赵世广 张依 邓积光 刘雨溪 郭萌 段二红

楚培齐, 王赛飞, 赵世广, 张依, 邓积光, 刘雨溪, 郭萌, 段二红. 甲烷催化燃烧反应机理及催化剂研究进展[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2021077
引用本文: 楚培齐, 王赛飞, 赵世广, 张依, 邓积光, 刘雨溪, 郭萌, 段二红. 甲烷催化燃烧反应机理及催化剂研究进展[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2021077
CHU Pei-qi, WANG Sai-fei, ZHAO Shi-guang, ZHANG Yi, DENG Ji-guang, LIU Yu-xi, GUO Meng, DUAN Er-hong. Research progress of reaction mechanism and catalysts on catalytic methane combustion[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2021077
Citation: CHU Pei-qi, WANG Sai-fei, ZHAO Shi-guang, ZHANG Yi, DENG Ji-guang, LIU Yu-xi, GUO Meng, DUAN Er-hong. Research progress of reaction mechanism and catalysts on catalytic methane combustion[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2021077

甲烷催化燃烧反应机理及催化剂研究进展

doi: 10.19906/j.cnki.JFCT.2021077
基金项目: 国家自然科学基金(U20A20130);河北省高等学校科学技术研究项目(QN2021059);河北省重点研发计划-资源与环境专项(20373703D);河北科技大学人才研究基金项目(1181400)
详细信息
    作者简介:

    楚培齐:chupeiqivip@163.com

    通讯作者:

    E-mail:wang_saifei@163.com

    E-mail:duan_eh@163.com

  • 中图分类号: TQ426, X701

Research progress of reaction mechanism and catalysts on catalytic methane combustion

Funds: The project was supported by the National Natural Science Foundation of China (U20A20130), Hebei Education Department (QN2021059), Hebei provincial Department of Science and Technology (20373703D) and Introduction of Talent Research Fund project of Hebei University of Science and Technology (1181400)
  • 摘要: 在煤矿开采及燃气轮机等工业应用或移动源领域存在甲烷大体量排放,且传统高温焚烧法会导致二次污染,因此在低温下实现甲烷高效转化成为亟待解决的问题。从能源利用和环境保护角度,催化燃烧技术是实现甲烷废气高效净化的有效措施。本文综述了近年来催化机理和催化剂的研究进展。首先,在实验和理论基础上,总结概括了甲烷氧化机理,其中重点阐述了“Two-term”模型;其次,系统介绍了各催化剂的性能优缺点和改性技术;最后,对甲烷催化未来研究提出展望,即采用结构优化方法来暴露更多活性位点或产生多组分协同催化效果、利用非贵金属掺杂等强化手段制备高效催化剂、进一步通过多重外场共同激发催化性能。此外,各类催化机理的自身完善和新型机理描述符的开发也是未来研究的重要方向。
  • 图  1  催化氧化反应速率曲线

    Figure  1  Catalytic oxidation reaction rate curve

    图  2  (a) LaFexCo1−xO3中B位阳离子d带中心及Op带中心的相对费米能级值; (b) LaFexCo1−xO3催化氧化CH4活性对比图[22]

    Figure  2  (a) Value of B-site metal cation d-band center and O p-band center to the Fermi lever in LaFexCo1−xO3; (b) Comparison of the activity of LaFexCo1−xO3 for the catalytic oxidation of CH4[22]

    图  3  (a) Pt/CeO2的甲烷转化率随时间变化曲线(SO2存在情况)[48]; (b) La-Co基钙钛矿氧化物催化剂表面E-R机理图和表面内MVK机理图[49]

    Figure  3  (a) CH4 conversion curve with time for Pt/CeO2 (in the presence of SO2)[48]; (b) Surface E-R mechanism diagram and intersurface MVK mechanism diagram of La-Co-based chalcogenide oxide catalyst[49]

    图  4  尖晶石的三种结构类型:(a) 正尖晶石, (b)反尖晶石, (c)混合尖晶石[77]

    Figure  4  Three structural types of spinels: (a) ortho-spinel, (b) anti-spinel, and (c) mixed spinel[77]

    图  5  MnCo2O4、NiCo2O4和CuCo2O4尖晶石催化CH4机制[78]

    Figure  5  Mechanism of CH4 catalysis by MnCo2O4, NiCo2O4 and CuCo2O4 spinels[78]

    图  6  钙钛矿型氧化物结构及CH4催化氧化机理图[82]

    Figure  6  Structure of perovskite oxide and mechanism of CH4 catalytic oxidation[82]

    图  7  钙钛矿催化剂的制备方法及改性工艺

    Figure  7  Preparation method and modification process of perovskite catalyst

    图  8  柠檬酸法-溶胶凝胶法(LaCoO3-SC)、乙二醇/甲醇-溶胶凝胶法(LaCoO3-SE)、模板法(LaCoO3-T)、共沉淀法(LaCoO3-P)制备的LaCoO3氧化活性[83]

    Figure  8  Oxidation activity of LaCoO3 prepared by Citric acid sol-gel method (LaCoO3-SC), Ethylene glycol/methanol-sol-gel method (LaCoO3-SE), template method (LaCoO3-T), and co-precipitation method (LaCoO3-P)[83]

    图  9  胶体晶体模板法制备3DOM材料的工艺流程[85]

    Figure  9  Process flow of 3DOM material preparation by colloidal crystal template method[85]

    图  10  LaNi0.5Co0.5O3和LaNi0.8Co0.2O3的结构变化图[88]

    Figure  10  Structural changes of LaNi0.5Co0.5O3 and LaNi0.8Co0.2O3[88]

    表  1  催化剂催化燃烧CH4性能对比

    Table  1  Comparison of CH4 catalytic combustion performance of catalysts

    TypesCatalystsConcentrationAir speedConversion temperatureReferences
    ppmmL·(h·g)−1T90/℃
    Supported Noble Metal0.3%Pd/AlOOH/Al-foam100007200035226
    Co/Ce0.3Zr0.7O2-δ76923300050027
    0.5Pd/M-Co1Ni4100006000032328
    5.0% PdOx/CeO21000001800040029
    Single transition metalCeO2-MnOx100003000054030
    Pd/CeO2100001500033631
    Pd/Co3O4 @ SiO2 100003000045032
    HexaaluminateLaMg0.7 FeAl10.3O19100004800064033
    1.91AuPd1.80/3DOM LaMnAl11O19250002000040234
    PerovskiteCa2FeNiO6100005000064035
    LaMn0.2Fe0.8O3100005000055036
    BaCe0.6Mn0.4O3-δ100002000042337
    LaNi0.2Co0.8O3100005000061038
    下载: 导出CSV
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