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

doi:10.1016/j.cjche.2021.07.022

Abstract

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

Zhouxin Chang, Feng Yu, Zhisong Liu, Zijun Wang, Jiangbing Li, Bin Dai, Jinli Zhang. Ni-Al mixed metal oxide with rich oxygen vacancies: CO methanation performance and density functional theory study[J]. Chinese Journal of Chemical Engineering, 2022, 46(6): 73-83.

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