Layered Mg-Al spinel supported Ce-Fe-Zr-O oxygen carriers for chemical looping reforming

doi:10.1016/j.cjche.2020.06.035

Abstract

Abstract: A series of layered Mg-Al spinel supported Ce-Fe-Zr-O oxygen carriers were prepared for co-production of syngas and pure hydrogen via chemical looping steam reforming (CLSR). The presence of magnesium-aluminum layered double oxides (MgAl-LDO) significantly increases the specific surface area of the mixed oxides, reduces the particle size of CeO₂-based solid solution and promotes the dispersion of free Fe₂O₃. When reacting with methane, MgAl-LDO supported oxygen carrier shows much lower temperature for methane oxidation than the pure CeFe-Zr-O sample, indicating enhanced low-temperature reactivity. Among different Ce-Fe-Zr-O(x)/MgAl-LDO samples, the Ce-Fe-Zr-O(40 wt%)/MgAl-LDO sample shows the best performance for the selective oxidation of methane to syngas and the H₂ production by water splitting. After a long period of high temperature redox experiment, the Ce-Fe-Zr-O(40 wt%)/MgAl-LDO oxygen carrier still shows high activity for syngas generation. The comparison on the morphology of the fresh and cycled oxygen carriers indicates that the Mg-Al spinel support still forms a stable skeleton structure with high dispersion of active components on the surface after the long-term cycling, which contributes to excellent redox stability of the Ce-Fe-Zr-O(40 wt%)/MgAl-LDO oxygen carrier.

Key words: Chemical looping reforming, Syngas, Hydrogen, Ce-Fe-Zr-O(x)/MgAl-LDO, Oxygen carrier

摘要： A series of layered Mg-Al spinel supported Ce-Fe-Zr-O oxygen carriers were prepared for co-production of syngas and pure hydrogen via chemical looping steam reforming (CLSR). The presence of magnesium-aluminum layered double oxides (MgAl-LDO) significantly increases the specific surface area of the mixed oxides, reduces the particle size of CeO₂-based solid solution and promotes the dispersion of free Fe₂O₃. When reacting with methane, MgAl-LDO supported oxygen carrier shows much lower temperature for methane oxidation than the pure CeFe-Zr-O sample, indicating enhanced low-temperature reactivity. Among different Ce-Fe-Zr-O(x)/MgAl-LDO samples, the Ce-Fe-Zr-O(40 wt%)/MgAl-LDO sample shows the best performance for the selective oxidation of methane to syngas and the H₂ production by water splitting. After a long period of high temperature redox experiment, the Ce-Fe-Zr-O(40 wt%)/MgAl-LDO oxygen carrier still shows high activity for syngas generation. The comparison on the morphology of the fresh and cycled oxygen carriers indicates that the Mg-Al spinel support still forms a stable skeleton structure with high dispersion of active components on the surface after the long-term cycling, which contributes to excellent redox stability of the Ce-Fe-Zr-O(40 wt%)/MgAl-LDO oxygen carrier.

关键词: Chemical looping reforming, Syngas, Hydrogen, Ce-Fe-Zr-O(x)/MgAl-LDO, Oxygen carrier

Jiangyong Yuan, Yannan Zhao, Haiwen Xu, Chunqiang Lu, Kun Yang, Xing Zhu, Kongzhai Li. Layered Mg-Al spinel supported Ce-Fe-Zr-O oxygen carriers for chemical looping reforming[J]. Chinese Journal of Chemical Engineering, 2020, 28(10): 2668-2676.

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