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Understanding complete oxidation of methane on spinel oxides at a molecular level

Author

Listed:
  • Franklin Feng Tao

    (University of Kansas
    University of Kansas)

  • Jun-jun Shan

    (University of Kansas
    University of Kansas)

  • Luan Nguyen

    (University of Kansas
    University of Kansas)

  • Ziyun Wang

    (School of Chemistry and Chemical Engineering, Queens University)

  • Shiran Zhang

    (University of Kansas
    University of Kansas)

  • Li Zhang

    (Oak Ridge National Laboratory Oak Ridge)

  • Zili Wu

    (Oak Ridge National Laboratory Oak Ridge)

  • Weixin Huang

    (University of Kansas
    University of Kansas)

  • Shibi Zeng

    (University of Kansas
    University of Kansas)

  • P. Hu

    (School of Chemistry and Chemical Engineering, Queens University)

Abstract

It is crucial to develop a catalyst made of earth-abundant elements highly active for a complete oxidation of methane at a relatively low temperature. NiCo2O4 consisting of earth-abundant elements which can completely oxidize methane in the temperature range of 350–550 °C. Being a cost-effective catalyst, NiCo2O4 exhibits activity higher than precious-metal-based catalysts. Here we report that the higher catalytic activity at the relatively low temperature results from the integration of nickel cations, cobalt cations and surface lattice oxygen atoms/oxygen vacancies at the atomic scale. In situ studies of complete oxidation of methane on NiCo2O4 and theoretical simulations show that methane dissociates to methyl on nickel cations and then couple with surface lattice oxygen atoms to form –CH3O with a following dehydrogenation to −CH2O; a following oxidative dehydrogenation forms CHO; CHO is transformed to product molecules through two different sub-pathways including dehydrogenation of OCHO and CO oxidation.

Suggested Citation

  • Franklin Feng Tao & Jun-jun Shan & Luan Nguyen & Ziyun Wang & Shiran Zhang & Li Zhang & Zili Wu & Weixin Huang & Shibi Zeng & P. Hu, 2015. "Understanding complete oxidation of methane on spinel oxides at a molecular level," Nature Communications, Nature, vol. 6(1), pages 1-10, November.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms8798
    DOI: 10.1038/ncomms8798
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    Cited by:

    1. Xiyi Li & Chao Li & Youxun Xu & Qiong Liu & Mounib Bahri & Liquan Zhang & Nigel D. Browning & Alexander J. Cowan & Junwang Tang, 2023. "Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts," Nature Energy, Nature, vol. 8(9), pages 1013-1022, September.
    2. Jun Ma & Can Zhu & Keke Mao & Wenbin Jiang & Jingxiang Low & Delong Duan & Huanxin Ju & Dong Liu & Kun Wang & Yijing Zang & Shuangming Chen & Hui Zhang & Zeming Qi & Ran Long & Zhi Liu & Li Song & Yuj, 2023. "Sustainable methane utilization technology via photocatalytic halogenation with alkali halides," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    3. He, Li & Fan, Yilin & Bellettre, Jérôme & Yue, Jun & Luo, Lingai, 2020. "A review on catalytic methane combustion at low temperatures: Catalysts, mechanisms, reaction conditions and reactor designs," Renewable and Sustainable Energy Reviews, Elsevier, vol. 119(C).
    4. Wenqing Zhang & Dawei Xi & Yihong Chen & Aobo Chen & Yawen Jiang & Hengjie Liu & Zeyu Zhou & Hui Zhang & Zhi Liu & Ran Long & Yujie Xiong, 2023. "Light-driven flow synthesis of acetic acid from methane with chemical looping," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Wenqing Zhang & Cenfeng Fu & Jingxiang Low & Delong Duan & Jun Ma & Wenbin Jiang & Yihong Chen & Hengjie Liu & Zeming Qi & Ran Long & Yingfang Yao & Xiaobao Li & Hui Zhang & Zhi Liu & Jinlong Yang & Z, 2022. "High-performance photocatalytic nonoxidative conversion of methane to ethane and hydrogen by heteroatoms-engineered TiO2," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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