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<p>Chemical looping partial oxidation of methane (CLPOM) is an emerging and efficient technology for syngas production from methane. The development of oxygen carriers with high reactivity and excellent cyclic stability is critical for the practical application of this process. In this study, a series of perovskite-type oxygen carriers, LaFe<sub>1-x</sub>Co<sub>x</sub>O<sub>3</sub>, were synthesized via a co-precipitation method and systematically characterized by XRD, XPS, TGA, and SEM. The results demonstrate that the synthesized oxygen carriers possess well-defined perovskite crystal structures with strong lattice oxygen storage and release capabilities. Reactivity evaluation revealed that LaFe<sub>0.7</sub>Co<sub>0.3</sub>O<sub>3</sub> exhibits the optimal CLPOM performance. During 15 consecutive redox cycles, <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\({X}_{C{H}_{4}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>X</mi> <mrow> <mi>C</mi> <msub> <mi>H</mi> <mn>4</mn> </msub> </mrow> </msub> </math></EquationSource> </InlineEquation>, <InlineEquation ID="IEq2"> <EquationSource Format="TEX">\({S}_{{H}_{2}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>S</mi> <msub> <mi>H</mi> <mn>2</mn> </msub> </msub> </math></EquationSource> </InlineEquation>, and <InlineEquation ID="IEq3"> <EquationSource Format="TEX">\({S}_{CO}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>S</mi> <mrow> <mi mathvariant="italic">CO</mi> </mrow> </msub> </math></EquationSource> </InlineEquation> remained stable at 87.22%, 88.69%, and 71.02%, respectively, indicating excellent cyclic stability. Moreover, no obvious sintering was observed after cycling. TGA analysis shows that only 0.45 wt.% carbon accumulated on the oxygen carrier after multiple cycles, confirming its strong resistance to carbon deposition. Density functional theory (DFT) calculations indicate that the CH<sub>3</sub> → CH<sub>2</sub> + H (TS2) is the rate-determining step of methane activation. In addition, the participation of surface lattice oxygen and the migration of bulk lattice oxygen effectively suppress carbon deposition, thereby enhancing methane conversion and syngas selectivity.</p>

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Performance and Stability of LaFe1-xCoxO3 Perovskite Oxygen Carriers in Chemical Looping Partial Oxidation of Methane

  • 期刊论文

  • 发表日期：

    2026年5月28日

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  • Lang Zhao,
  • Ganming Cao,
  • Yue Lai,
  • Yandong Li,
  • Dengfu Chen,
  • Mujun Long,
  • Huamei Duan

摘要

Chemical looping partial oxidation of methane (CLPOM) is an emerging and efficient technology for syngas production from methane. The development of oxygen carriers with high reactivity and excellent cyclic stability is critical for the practical application of this process. In this study, a series of perovskite-type oxygen carriers, LaFe1-xCoxO3, were synthesized via a co-precipitation method and systematically characterized by XRD, XPS, TGA, and SEM. The results demonstrate that the synthesized oxygen carriers possess well-defined perovskite crystal structures with strong lattice oxygen storage and release capabilities. Reactivity evaluation revealed that LaFe0.7Co0.3O3 exhibits the optimal CLPOM performance. During 15 consecutive redox cycles, \({X}_{C{H}_{4}}\) X C H 4 , \({S}_{{H}_{2}}\) S H 2 , and \({S}_{CO}\) S CO remained stable at 87.22%, 88.69%, and 71.02%, respectively, indicating excellent cyclic stability. Moreover, no obvious sintering was observed after cycling. TGA analysis shows that only 0.45 wt.% carbon accumulated on the oxygen carrier after multiple cycles, confirming its strong resistance to carbon deposition. Density functional theory (DFT) calculations indicate that the CH3 → CH2 + H (TS2) is the rate-determining step of methane activation. In addition, the participation of surface lattice oxygen and the migration of bulk lattice oxygen effectively suppress carbon deposition, thereby enhancing methane conversion and syngas selectivity.