Study of grain size effect of lanthanum oxide catalyzed methane oxidation coupling reaction
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Graphical Abstract
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Abstract
La2O3 catalysts with different grain sizes were prepared under hydrothermal condition. The structure activity relationship of La2O3 catalysts with different grain sizes were investigated by using in-situ XRD, Raman, FT-IR and H2-TPR, O2-TPD. The results showed that the La−O bond of the La2O3 catalyst showed a significant elongation with increasing temperature, which affected its adsorption and dynamic storage of O2. When increasing the grain size up to 57.4 nm, the oxygen storage capacity of the La2O3 catalyst started to decrease, accompanied by the enrichment of surface oxygen species, especially superoxide species, on the catalyst surface, which led to the over-oxidation of CH4 and products and reduced the C2 + hydrocarbons selectivity. The L-La2O3 catalyst with a grain size of 52.3 nm had a suitable content of surface oxygen species and a high oxygen storage capacity at 750 ℃. It exhibited the best C2 + hydrocarbon selectivity up to a CH4/O2 of 3 and a vacancy rate of 1.6 × 105 mL/(g·h).
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