A series of Rh-promoted La0.75Sr0.25(Fe0.80Co0.20)((1-x))AlxO3-delta (x= 0, 0.10, 0.25, 0.40, 0.60) samples were investigated as oxygen reservoirs for the conversion of CH4 to syngas at 873 K and 1 atm. Neutron powder diffraction studies revealed a decreasing rhombohedral distortion on increasing Al-content. XPS and TEM were employed to investigate surface chemistry and morphology of the Al = 0.25 sample. The influence of Al-substitution on the redox properties was studied by flowing titration whereas catalytic properties were studied by means of transient pulses of CH4 and O-2, as well of (CH4)-C-13 and CO. The products (CO, H-2, CO2 and H2O) of the reaction between CH4 and the studied oxides were successfully tuned by tailoring the redox properties of the reducible oxides through the Al-substitution. (C) 2016 Elsevier B.V. All rights reserved.