S1. Preparation of the Mn77Fe23 oxygen carriers. Table S1. Amounts of Mn and Fe raw materials in the particle size of 0.1-0.3 mm mixed in every mill container and particle size of the Mn-Fe mixture after the mixing-grinding step. S2. XRD diffraction patterns of the different MnFe-mixed oxides prepared to be used as oxygen carriers. Figure S1. XRD of the 7 Mn-Fe based oxygen carriers. S3. XRD diffraction patterns of the different MnFe-mixed oxides prepared to be used as oxygen carriers. Figure S2. XRD of the samples after long cycles in TGA at high conversions (ca. 80%): (a) MnSA and (b) MnGBMPB+Fe-ore. S4. TGA tests. Figure S3. Variation of the mass sample in TGA under CLOU conditions for the MnGBHNE+Fe-ESF material (870 ºC). Figure S4. Variation of the mass sample in TGA under CLC conditions for the MnGBHNE+Fe-ESF material (reduction: 5%H2+40% H2O, 950 ºC). S5. MnSA sample after 300 redox cycles with △Xs ≈ 80 %. Figure S5. Image of the MnSA oxygen carrier after 300 redox cycles at high conversions (ca. 80 %).

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