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Low temperature catalytic oxidation of propane over cobalt-cerium spinel oxides catalysts

机译:钴铈尖晶石氧化物催化剂上丙烷的低温催化氧化

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摘要

In this study, the cobalt-cerium spinel oxides catalysts were prepared via a citric acid complex method. The catalytic performance and physicochemical properties of the samples for deep propane oxidation were evaluated. Co2Ce1Ox catalysts exhibit the superior low temperature activity with a T-50 value of 220 degrees C, which is much lower than both individual cobalt and cerium oxides. The results show that cerium ions could enter into the spinel-type lattice of the cobalt oxides and lead to the severe lattice distortion. The activated Co-O bonds favor the propane activation and enhance the reducibility of active Co3+ species. Meanwhile, high proportion of Co3+ content and better oxygen mobility are also observed in the cobalt-cerium spinel oxides catalysts. The kinetic and the transient experiments reveal that the reduction step of the catalysts plays a crucial role in the deep catalytic propane oxidation. The reaction rate of Co2Ce1Ox catalyst reaches 0.22 mu mol g(-1) s(-1) at 200 degrees C and its activation energy is the lowest (57.9 kJ mol(-1)). All the results indicate that the combination of redox behaviors of Co3O4 and oxygen vacancies of CeO2 offer useful support for catalysts design toward propane oxidation at low temperature.
机译:在这项研究中,钴-柠檬酸尖晶石氧化物催化剂是通过柠檬酸络合物法制备的。评价了样品对丙烷深度氧化的催化性能和理化性质。 Co2Ce10Ox催化剂具有出色的低温活性,T-50值为220摄氏度,远低于单独的钴氧化物和铈氧化物。结果表明,铈离子可能进入钴氧化物的尖晶石型晶格,并导致严重的晶格畸变。活化的Co-O键有利于丙烷活化并增强活性Co3 +物种的还原性。同时,在钴-铈尖晶石氧化物催化剂中还观察到高比例的Co 3+含量和更好的氧迁移率。动力学和瞬态实验表明,催化剂的还原步骤在丙烷深度催化氧化中起着至关重要的作用。 Co2Ce1Ox催化剂在200摄氏度下的反应速率达到0.22μmol g(-1)s(-1),其活化能最低(57.9 kJ mol(-1))。所有结果表明,Co3O4的氧化还原行为和CeO2的氧空位的结合为催化剂在低温下丙烷的氧化设计提供了有用的支持。

著录项

  • 来源
    《Applied Surface Science》 |2019年第15期|1132-1140|共9页
  • 作者单位

    Zhejiang Univ, State Environm Protect Ctr Coal Fired Air Pollut, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China;

    Zhejiang Univ, State Environm Protect Ctr Coal Fired Air Pollut, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China|Jiangsu Univ Sci & Technol, Sch Energy & Power, Zhenjiang 212003, Jiangsu, Peoples R China;

    Zhejiang Univ, State Environm Protect Ctr Coal Fired Air Pollut, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China;

    Zhejiang Univ, State Environm Protect Ctr Coal Fired Air Pollut, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China;

    Zhejiang Univ, State Environm Protect Ctr Coal Fired Air Pollut, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China;

    Zhejiang Univ, State Environm Protect Ctr Coal Fired Air Pollut, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China;

    Zhejiang Univ, State Environm Protect Ctr Coal Fired Air Pollut, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China;

    Zhejiang Univ, State Environm Protect Ctr Coal Fired Air Pollut, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China;

    Zhejiang Univ, State Environm Protect Ctr Coal Fired Air Pollut, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Propane oxidation; Low temperature; Spinel; Cobalt; Cerium;

    机译:丙烷氧化低温尖晶石钴铈;

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