Journal of East China Normal University(Natural Science) >

2023 , Vol. 2023 >Issue 1: 95 - 103

DOI: https://doi.org/10.3969/j.issn.1000-5641.2023.01.010

Catalytic Reaction Technologies

Study of an Na2WO4/Mn7SiO12-SiO2 oxygen-carrier catalyst for chemical looping-oxidative coupling of methane

  • Ya GAO ,
  • Weidong SUN ,
  • Guofeng ZHAO ,
  • Ye LIU ,
  • Yong LU
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  • 1. Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai　200062, China
    2. Institute of Eco-Chongming, Shanghai　202162, China

Received date: 2022-06-15

  Accepted date: 2022-09-21

  Online published: 2023-01-07

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Abstract

A promising chemical looping-oxidative coupling of methane (CL-OCM) oxygen-carrier catalyst, Na2WO4/Mn7SiO12-SiO2, was obtained by adding extra Mn2O3 to Mn2O3-Na2WO4/SiO2 and in-situ activating in the reaction stream. After experiencing an induction period, the oxygen-carrier phase transformed from Mn2O3 to Mn7SiO12 in association with an improvement in C2-C3 selectivity but decreased CH4 conversion. The Na2WO4/Mn7SiO12-SiO2 oxygen-carrier catalysts could also be obtained by directly calcining the Na2WO4/Mn2O3-SiO2 precursor at 800 ℃ in air. At 750 ℃ and a CH4 residence time of 12 s, the catalyst achieved 12% (or 7%) CH4 conversion and 81.5% (or 90.0%) C2-C3 selectivity using a mCat/mCH4 weight ratio of 27 (or 13.5). Notably, only C3H6 was detected as C3 products, whose selectivity was about 5%. The CL-OCM reaction proceeded selectively through the redox cycle mode of Mn7SiO12 $ \leftrightarrow $ [MnSiO3 + MnWO4]. The lattice-oxygen mobility in Mn7SiO12 was much weaker than that in Mn2O3, which improved C2-C3 selectivity but decreased CH4 conversion. Our findings provide guidance for the exploration of more advanced catalytic oxygen-carrier catalysts toward efficient CL-OCM process.

Key words： oxidative coupling of methane to ethylene; chemical looping; oxygen-carrier catalyst; lattice-oxygen oxidation; manganese

Cite this article

Ya GAO , Weidong SUN , Guofeng ZHAO , Ye LIU , Yong LU . Study of an Na2WO4/Mn7SiO12-SiO2 oxygen-carrier catalyst for chemical looping-oxidative coupling of methane[J]. Journal of East China Normal University(Natural Science), 2023 , 2023(1) : 95 -103 . DOI: 10.3969/j.issn.1000-5641.2023.01.010

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