物理化学学报 >> 2017, Vol. 33 >> Issue (7): 1453-1461.doi: 10.3866/PKU.WHXB201704104

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Pd/Co3O4纳米颗粒负载于Al2O3纳米片高效催化甲烷燃烧

刘敬伟,杨娜婷,祝艳*()   

  • 收稿日期:2017-02-06 发布日期:2017-05-31
  • 通讯作者: 祝艳 E-mail:zhuy@sari.ac.cn
  • 基金资助:
    国家自然科学基金(21273151);英国能源化学研究所研究基金资助项目

Pd/Co3O4 Nanoparticles Inlaid in Alkaline Al2O3 Nanosheets as an Efficient Catalyst for Catalytic Oxidation of Methane

Jing-Wei LIU,Na-Ting YANG,Yan ZHU*()   

  • Received:2017-02-06 Published:2017-05-31
  • Contact: Yan ZHU E-mail:zhuy@sari.ac.cn
  • Supported by:
    the National Natural Science Foundation of China(21273151);Energy Technologies Institute LLP, England

摘要:

我们报道了一种Pd/Co3O4纳米颗粒负载于Al2O3纳米片的三元催化剂催化甲烷的高效燃烧。其中,Pd/Co3O4负载于碱性氧化铝的复合材料活化甲烷C-H键的能力比SiO2、ZrO2和CeO2以及酸性和中性Al2O3为载体时更强,这是因为Pd/Co3O4/碱性Al2O3拥有更多的氧空穴和吸附氧,对催化剂催化甲烷燃烧有较好的影响。尽管在5%(体积分数)的水蒸气存在下,其催化性能有一定的失活,但在移除水蒸气时,其催化性能可以快速恢复至最佳状态。在模拟真实汽车尾气的氛围下,Pd/Co3O4/碱性Al2O3依然具有较好的催化甲烷燃烧性能,在400℃时可以催化甲烷完全转化。

关键词: Pd/Co3O4, 碱性, 甲烷氧化, 活性, 稳定性

Abstract:

We report an efficient catalyst composed of ternary components prepared by inlaying Pd/Co3O4 nanoparticles in alkaline Al2O3 nanosheets for catalytic oxidation of methane. Pd/Co3O4 inlaid in alkaline Al2O3 exhibited a higher ability to break the C-H bond of methane than Pd/Co3O4 supported on SiO2, ZrO2, CeO2, and acidic or neutral Al2O3. Our results show more oxygen vacancies and higher amounts of surface adsorbed oxygen on the surface of Pd/Co3O4/alkaline Al2O3 than on other catalysts, which is responsible for methane activation and conversion. Further, the Pd/Co3O4/alkaline Al2O3 catalyst can almost restore to its initial value in the absence of water when 5% (volume fraction) vapor water was cut off, although a decrease in activity occurred when water vapor was introduced to the reaction system. Even under a condition similar to the exhaust of a lean-burn natural gas engine, the catalytic performance of the Pd/Co3O4/alkaline Al2O3 catalyst is excellent, that is, methane could be completely converted when the sample temperature in the reaction atmosphere was ramped to 400℃.

Key words: Pd/Co3O4, Alkaline Al2O3, Methane oxidation, Activity, Stability

MSC2000: 

  • O643