摘要
Partially oxidizing methane into syngas via a two-step chemical looping scheme was a promising option for methane transformation. Ce 2 (SO 4 ) 3 was selected to explore the performance and mechanism of methane chemical looping partial oxidation (CLPOM) to syngas. Thermodynamic and kinetic analysis forecast the Ce 2 (SO 4 ) 3 as a promising candidate for CLPOM. Compared with literature, Ce 2 (SO 4 ) 3 not only had an outstanding syngas selectivity, but also an appropriate CH 4 conversion and molar ratio, and CH 4 conversion could reach 90.5 % of thermodynamic result. As revealed via characterization, Ce 2 (SO 4 ) 3 (1 0 2) surface had the highest peak intensity and the migration of lattice oxygen played an important role in CLPOM. Some of them were tend to agglomeration and these small particles were less than 5 μm. Density functional theory calculations demonstrated that CH 4 series dehydrogenation products tended to adsorb at O site and CH 3 → CH 2 + H was the rate-determining step. The reaction of surface lattice oxygen atoms and migration of the internal lattice oxygen atoms could inhibit carbon deposition, promote CH 4 conversion and syngas generation in experiment. Compared with NiO, Ce 2 (SO 4 ) 3 had a lower energy barrier of lattice oxygen migration, which could increase the reaction rate.
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