SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2022, Vol. 46 ›› Issue (6): 73-83.DOI: 10.1016/j.cjche.2021.07.022

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Ni-Al mixed metal oxide with rich oxygen vacancies: CO methanation performance and density functional theory study

Zhouxin Chang1, Feng Yu1,2, Zhisong Liu1, Zijun Wang1, Jiangbing Li1, Bin Dai1, Jinli Zhang1   

  1. 1 Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832003, China;
    2 Bingtuan Industrial Technology Research Institute, Shihezi University, Shihezi 832003, China
  • Received:2021-03-08 Revised:2021-07-14 Online:2022-07-20 Published:2022-06-28
  • Contact: Feng Yu,E-mail:yufeng05@mail.ipc.ac.cn
  • Supported by:
    This work was supported by National Natural Science Foundation of China (No. 22068034) and Science and Technology Innovation Talents Program of Bingtuan (No. 2019CB025).

Ni-Al mixed metal oxide with rich oxygen vacancies: CO methanation performance and density functional theory study

Zhouxin Chang1, Feng Yu1,2, Zhisong Liu1, Zijun Wang1, Jiangbing Li1, Bin Dai1, Jinli Zhang1   

  1. 1 Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832003, China;
    2 Bingtuan Industrial Technology Research Institute, Shihezi University, Shihezi 832003, China
  • 通讯作者: Feng Yu,E-mail:yufeng05@mail.ipc.ac.cn
  • 基金资助:
    This work was supported by National Natural Science Foundation of China (No. 22068034) and Science and Technology Innovation Talents Program of Bingtuan (No. 2019CB025).

Abstract: Ni-Al mixed metal oxides have been successfully prepared by high shear mixer (HSM) and coprecipitation (CP) methods for low temperature CO methanation. In this work, Ni-Al (HSM-CP) catalyst presented small Ni crystallite size and high surface area, which all contribute to the methanation reaction at low temperature conditions. The obtained Ni-Al (HSM-CP) sample exhibited a mass of defective oxygen, thereby accelerating the dissociation of CO and ultimately increasing the activity of the catalyst. Ni-Al (HSM-CP) catalyst offered the best activity with CO conversion = 100% and CH4 selectivity = 93% at 300 ℃, and the CH4 selectivity can reach 81.8% at 200 ℃. In situ Fourier transform infrared spectroscopy and density functional theory show that CHO and COH intermediates with lower activation energy barriers are produced during the reaction, and hydrogen-assisted carbon–oxygen bond scission is more favorable.

Key words: Natural gas, Carbon monoxide methanation, High shear mixer, Oxygen vacancy, Homogeneous catalysis

摘要: Ni-Al mixed metal oxides have been successfully prepared by high shear mixer (HSM) and coprecipitation (CP) methods for low temperature CO methanation. In this work, Ni-Al (HSM-CP) catalyst presented small Ni crystallite size and high surface area, which all contribute to the methanation reaction at low temperature conditions. The obtained Ni-Al (HSM-CP) sample exhibited a mass of defective oxygen, thereby accelerating the dissociation of CO and ultimately increasing the activity of the catalyst. Ni-Al (HSM-CP) catalyst offered the best activity with CO conversion = 100% and CH4 selectivity = 93% at 300 ℃, and the CH4 selectivity can reach 81.8% at 200 ℃. In situ Fourier transform infrared spectroscopy and density functional theory show that CHO and COH intermediates with lower activation energy barriers are produced during the reaction, and hydrogen-assisted carbon–oxygen bond scission is more favorable.

关键词: Natural gas, Carbon monoxide methanation, High shear mixer, Oxygen vacancy, Homogeneous catalysis