Oxidative coupling of methane by Mn-Na2WO4/γ-Al2O3 catalyst: effect of Mn/W ratio

doi:10.1007/s11705-023-2367-z

Front. Chem. Sci. Eng.

2024, Vol. 18

Issue (1) : 1 https://doi.org/10.1007/s11705-023-2367-z

RESEARCH ARTICLE

Oxidative coupling of methane by Mn-Na₂WO₄/γ-Al₂O₃ catalyst: effect of Mn/W ratio

Hasan Oliaei Torshizi, Ali Nakhaei Pour(

), Alireza Salimi, Melika Ghadamyari

Department of Chemistry, Faculty of Science, Ferdowsi University of Mashhad, Mashhad 9177948974, Iran

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Abstract

In this study, Mn-Na₂WO₄/γ-Al₂O₃ catalysts with varying ratios of Mn/W were prepared using the dry impregnation method. These catalysts were then tested for their suitability in the oxidative coupling of methane reaction. The X-ray photoelectron results revealed the presence of the tetrahedral WO₄^2– phase in all prepared catalysts. It is believed that the presence of this phase is associated with high catalyst activity, indicating the potential of the catalysts for the desired reaction. The activity results show that the catalyst with a high Mn/W ratio exhibited higher activity at 800 °C, whereas the catalyst with a low Mn/W ratio showed greater activity at 850 °C. This suggests that the Mn/W ratio influences the reaction temperature at which the catalyst is most active. Furthermore, the X-ray diffraction results of the treated catalysts revealed that the catalyst with a high Mn/W ratio exhibited more MnAl₂O₄ at 800 °C, whereas the catalyst with a low Mn/W ratio contained more MnWO₄ at 850 °C. The results suggest that the presence of MnAl₂O₄ sites may promote a more facile Mn²⁺ ↔ Mn³⁺ cycle at lower temperatures than the MnWO₄ site, potentially contributing to the enhanced catalyst activity in the oxidative coupling of methane reaction at 800 °C.

Keywords oxidative coupling of methane Mn-Na₂WO₄ methane Al₂O₃

Corresponding Author(s): Ali Nakhaei Pour

About author: Peng Lei and Charity Ngina Mwangi contributed equally to this work.

Just Accepted Date: 06 September 2023 Issue Date: 06 November 2023

Cite this article:

Hasan Oliaei Torshizi,Ali Nakhaei Pour,Alireza Salimi, et al. Oxidative coupling of methane by Mn-Na₂WO₄/γ-Al₂O₃ catalyst: effect of Mn/W ratio[J]. Front. Chem. Sci. Eng., 2024, 18(1): 1.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-023-2367-z
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I1/1

Fig.1 Schematic representation of the catalyst activity test in the present work (1: gas cylinders, 2: pressure regulators, 3: needle valves, 4: digital pressure controllers, 5: MFC, 6: non-return valves, 7: ball valves, 8: mixing chamber, 9: TIC, 10: cold trap, 11: BPR (back pressure regulator), 12: cold water circulator, 13: flow meter, 14: gas chromatograph (GC), 15: tubular reactor and catalyst bed, 16: tubular furnace).

Fig.2 FTIR of the prepared catalysts.

Fig.3 The XRD patterns of the fresh calcined catalysts.

Fig.4 The XRD patterns of treated catalysts at 800–850 °C, CH₄/O₂ = 4 molar ratios, with a GHSV of 12000 h^–1 at atmospheric pressure after 1-h activity test. Catalysts were (a) treated at 800 °C, (b) treated at 825 °C, and (c) treated at 850 °C (The peak related to γ-Al₂O₃ (■), MnAl₂O₄ (Δ), Na₂WO₄ (●), Mn₂O₃ (▲), and MnWO₄ (?)).

Fig.5 TPR resuolts f the prepared catalysts.

Fig.6 FESEM of the prepared catalysts.

Fig.7 High resolution of Mn 2p of (a) fresh catalysts, (b) treated at 800 °C, (c) treated at 825 °C and (d) treated at 850 °C, and W 4f spectra of (e) the fresh catalysts, (f) treated at 800 °C, (g) treated at 825 °C and (h) treated at 850 °C.

Fig.8 High resolution of O 1s spectra and deconvolution oxygen results of (a) fresh catalysts, (b) treated at 800 °C, (c) treated at 825 °C and (d) treated at 850 °C.

Tab.1 CH₄ conversion (%) and product selectivity (%) of prepared catalysts (SV = 12000 h^–1)

Tab.2 Comparison of the products selectivity (%) of the OCM catalysts

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