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 CeO

2

-based solid solution and promotes the dispersion of free Fe

2

O

3

. 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 H

2

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.