SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2023, Vol. 62 ›› Issue (10): 225-237.DOI: 10.1016/j.cjche.2023.04.002

• Full Length Article • 上一篇    下一篇

Chemical looping conversion of methane via Fe2O3-LaFeO3 calcined from LaFe-MOF precursor

Jitong Deng1, Yongjun Zhang1,2, Xiaopeng Wang3, Wei Zhang1, Hongjing Han1, Haiying Wang1, Huimin Yuan2, Yanan Zhang1, Yanguang Chen1   

  1. 1. College of Chemistry & Chemical Engineering, Northeast Petroleum University, Daqing 163318, China;
    2. PetroChina Daqing Petrochemical Research Center, Daqing 163714, China;
    3. CNPC Safety and Environmental Technology Research Institute Co. LTD., Beijing 102206, China
  • 收稿日期:2022-12-29 修回日期:2023-04-11 出版日期:2023-10-28 发布日期:2023-12-23
  • 通讯作者: Hongjing Han,E-mail:hongjing_han@163.com;Yanguang Chen,E-mail:ygchen79310@126.com
  • 基金资助:
    This work was financially supported by the National Natural Science Foundation of China (21908021), the China Petroleum Science and Technology Innovation Fund project (2021DQ02-0701), the High-Level Talent Project of Heilongjiang Province of China (2020GSP17), the New Energy and New Direction Project of Northeast Petroleum University (XNYXLY202102), and the Guiding Innovation Fund of Northeast Petroleum University (2021YDL-03).

Chemical looping conversion of methane via Fe2O3-LaFeO3 calcined from LaFe-MOF precursor

Jitong Deng1, Yongjun Zhang1,2, Xiaopeng Wang3, Wei Zhang1, Hongjing Han1, Haiying Wang1, Huimin Yuan2, Yanan Zhang1, Yanguang Chen1   

  1. 1. College of Chemistry & Chemical Engineering, Northeast Petroleum University, Daqing 163318, China;
    2. PetroChina Daqing Petrochemical Research Center, Daqing 163714, China;
    3. CNPC Safety and Environmental Technology Research Institute Co. LTD., Beijing 102206, China
  • Received:2022-12-29 Revised:2023-04-11 Online:2023-10-28 Published:2023-12-23
  • Contact: Hongjing Han,E-mail:hongjing_han@163.com;Yanguang Chen,E-mail:ygchen79310@126.com
  • Supported by:
    This work was financially supported by the National Natural Science Foundation of China (21908021), the China Petroleum Science and Technology Innovation Fund project (2021DQ02-0701), the High-Level Talent Project of Heilongjiang Province of China (2020GSP17), the New Energy and New Direction Project of Northeast Petroleum University (XNYXLY202102), and the Guiding Innovation Fund of Northeast Petroleum University (2021YDL-03).

摘要: The effective utilization of natural gas resources is a promising option for the implementation of the “dual carbon” strategy. However, the capture of carbon dioxide with relatively lower concentration after the combustion of natural gas is the crucial step. Fortunately, the lattice oxygen is used for chemical cycle conversion of methane to overcome the shortcomings mentioned above. A method was proposed to synthesize perovskite for methane cycle conversion using metal organic framework as a precursor. Morphology and pore structure of Fe2O3-LaFeO3 composite oxides were regulated by precursor synthesis conditions and calcination process. Moreover, the chemical looping conversion performance of methane was evaluated. The results showed that the pure phase precursor of La[Fe(CN)6]·5H2O was synthesized with the specific surface area of 23.91 m2·g-1 under the crystallization of 10 h and the pH value of 10.5. Fe2O3-LaFeO3 was obtained by controlled calcination of La[Fe(CN)6]·5H2O and Fe2O3 with variable mass ratio. The selectivity of CO2 can reach more than 99% under the optimal parameters of methane chemical looping conversion: m(Fe2O3):m(LaFeO3) = 2:1, the reaction temperature is 900 ℃, the lattice oxygen conversion is less than 40%. Fe2O3-LaFeO3 still has good phase and structure stability after five redox reaction and regeneration cycles.

关键词: Composite, Chemical looping conversion, Carbon dioxide, Metal organic frameworks, Lattice oxygen, Methane

Abstract: The effective utilization of natural gas resources is a promising option for the implementation of the “dual carbon” strategy. However, the capture of carbon dioxide with relatively lower concentration after the combustion of natural gas is the crucial step. Fortunately, the lattice oxygen is used for chemical cycle conversion of methane to overcome the shortcomings mentioned above. A method was proposed to synthesize perovskite for methane cycle conversion using metal organic framework as a precursor. Morphology and pore structure of Fe2O3-LaFeO3 composite oxides were regulated by precursor synthesis conditions and calcination process. Moreover, the chemical looping conversion performance of methane was evaluated. The results showed that the pure phase precursor of La[Fe(CN)6]·5H2O was synthesized with the specific surface area of 23.91 m2·g-1 under the crystallization of 10 h and the pH value of 10.5. Fe2O3-LaFeO3 was obtained by controlled calcination of La[Fe(CN)6]·5H2O and Fe2O3 with variable mass ratio. The selectivity of CO2 can reach more than 99% under the optimal parameters of methane chemical looping conversion: m(Fe2O3):m(LaFeO3) = 2:1, the reaction temperature is 900 ℃, the lattice oxygen conversion is less than 40%. Fe2O3-LaFeO3 still has good phase and structure stability after five redox reaction and regeneration cycles.

Key words: Composite, Chemical looping conversion, Carbon dioxide, Metal organic frameworks, Lattice oxygen, Methane