Catalytic combustion of methane over a highly active and stable NiO/CeO<sub>2</sub> catalyst

doi:10.1007/s11705-019-1821-4

Front. Chem. Sci. Eng.

2020, Vol. 14

Issue (4) : 534-545 https://doi.org/10.1007/s11705-019-1821-4

RESEARCH ARTICLE

Catalytic combustion of methane over a highly active and stable NiO/CeO₂ catalyst

Xiuhui Huang^1,²(

), Junfeng Li³, Jun Wang^1,², Zeqiu Li^1,², Jiayin Xu^1,²(

)

¹. School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China
². Shanghai Key Laboratory of Multiphase Flow and Heat Transfer in Power Engineering, Shanghai 200093, China
³. Shanghai MCC20 Construction Co. Ltd., Shanghai 201999, China

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Abstract

In the last decades, many reports dealing with technology for the catalytic combustion of methane (CH₄) have been published. Recently, attention has increasingly focused on the synthesis and catalytic activity of nickel oxides. In this paper, a NiO/CeO₂ catalyst with high catalytic performance in methane combustion was synthesized via a facile impregnation method, and its catalytic activity, stability, and water-resistance during CH₄ combustion were investigated. X-ray diffraction, low-temperature N₂ adsorption, thermogravimetric analysis, Fourier transform infrared spectroscopy, hydrogen temperature programmed reduction, methane temperature programmed surface reaction, Raman spectroscopy, electron paramagnetic resonance, and transmission electron microscope characterization of the catalyst were conducted to determine the origin of its high catalytic activity and stability in detail. The incorporation of NiO was found to enhance the concentration of oxygen vacancies, as well as the activity and amount of surface oxygen. As a result, the mobility of bulk oxygen in CeO₂ was increased. The presence of CeO₂ prevented the aggregation of NiO, enhanced reduction by NiO, and provided more oxygen species for the combustion of CH₄. The results of a kinetics study indicated that the reaction order was about 1.07 for CH₄ and about 0.10 for O₂ over the NiO/CeO₂ catalyst.

Keywords methane combustion NiO/CeO₂ catalyst interaction oxygen vacancy kinetic study

Corresponding Author(s): Xiuhui Huang,Jiayin Xu

Just Accepted Date: 24 July 2019 Online First Date: 27 September 2019 Issue Date: 22 May 2020

Cite this article:

Xiuhui Huang,Junfeng Li,Jun Wang, et al. Catalytic combustion of methane over a highly active and stable NiO/CeO₂ catalyst[J]. Front. Chem. Sci. Eng., 2020, 14(4): 534-545.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-019-1821-4
https://academic.hep.com.cn/fcse/EN/Y2020/V14/I4/534

Fig.1 Effect of the supports on the activity of the supported NiO catalysts (gas space velocity= 60000 mL·g^?¹·h^?¹).

Fig.2 (a) XRD patterns and (b) H₂-TPR profiles of the different NiO catalysts.

Fig.3 Light-off curves of the catalytic combustion of methane over the NiO/CeO₂ catalysts (gas space velocity= 60000 mL·g^?¹·h^?¹).

Tab.1 CH₄ reaction rate over NiO/CeO₂ catalysts at 360°C

Fig.4 Effect of the addition of water vapor in CH₄ combustion over 10 wt-% NiO/CeO₂: (a) without H₂O and (b) with 3.1% water vapor (25°C; gas space velocity= 60000 mL·g^?¹·h^?¹).

Fig.5 Dependence of the reaction rates on the CH₄ and O₂ concentration over the 10 wt-% NiO/CeO₂ catalyst at 320°C: (a) 0.5?4 vol-% CH₄, 4 vol-% O₂, in Ar; (b) 2?10 vol-% O₂, 1 vol-% CH₄, in Ar. (

P CH 4

and

P O 2

, partial pressures; gas space velocity= 30000 mL·g^?¹·h^?¹).

Fig.6 Arrhenius plots of the reaction rate of CH₄ combustion (activation energy, E_a) over (a) pure CeO₂ and 10 wt-% (b) NiO/CeO₂ (gas space velocity= 30000 mL·g^?¹·h^?¹).

Fig.7 XRD patterns of the NiO/CeO₂ samples with various NiO loadings.

Tab.2 Textural properties and catalytic activities of CeO₂ and NiO/CeO₂ samples for CH₄ combustion

Fig.8 H₂-TPR profiles of the CeO₂, NiO, and NiO/CeO₂ samples.

Fig.9 Raman spectra of NiO/CeO₂ with NiO loadings of (a) 0, (b) 1 wt-%, (c) 3 wt-%, (d) 5 wt-%, (e) 7 wt-%, (f) 10 wt-%, (g) 15 wt-%, and (h) 20 wt-%. Inset: Raman spectrum of 10 wt-% NiO/CeO₂.

Fig.10 Special conversion of CH₄ per unit surface area at 460°C vs. (A₅₇₅+A₆₂₀)/A₄₆₂ in the Raman spectra of CeO₂-supported NiO with NiO loadings of 0, 1, 3, 5, 7, and 10 wt-% (gas space velocity= 60000 mL·g^?¹·h^?¹).

Fig.11 MS signals of CO₂ (m/z = 44) from CH₄-TPSR on NiO/CeO₂ with various NiO loadings.

Fig.12 MS signals from CH₄-TPSR on CeO₂ and 10 wt-% NiO/CeO₂ (H₂ (m/z = 2), CH₄ (m/z = 16), CO (m/z = 28), and CO₂ (m/z = 44)).

Fig.13 EPR signals of (a) CeO₂ and (b) 10 wt-% NiO/CeO₂ (inset: magnification of the EPR spectrum).

Fig.14 TEM images of (a) CeO₂ and (b) 10 wt-% NiO/C.

Fig.15 Methane conversion over 10 wt-% NiO/CeO₂ vs. reaction time at 600°C (gas space velocity= 15000 mL·g^?¹·h^?¹).

Fig.16 (a) XRD patterns of CeO₂, fresh 10 wt-% NiO/CeO₂, and used 10 wt-% NiO/CeO₂; (b) H₂-TPR profiles of fresh and used 10 wt-% NiO/CeO₂ catalyst.

Fig.17 (a) FT-IR spectra of fresh and used 10 wt-% NiO/CeO₂; (b) TG-DTA curves of used NiO/CeO₂ catalyst.

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