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

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.