A high performance oxygen storage material for chemical looping processes with CO2 captureElectronic supplementary information (ESI) available: Methods, detailed characterisation of Cu-Al LDH precursors and derived mixed metal oxides, including SEM/TEM, XRD, FTIR, thermal analyses, TPR profiles, detailed profiles of O2 release and storage cycles, detailed profiles of cyclic reduction and oxidation cycles, characterisation of used oxygen carrier materials with various techniques, including XRD, S

Chemical looping combustion (CLC) is a novel combustion technology that involves cyclic reduction and oxidation of oxygen storage materials to provide oxygen for the combustion of fuels to CO 2 and H 2 O, whilst giving a pure stream of CO 2 suitable for sequestration or utilisation. Here, we report a method for preparing of oxygen storage materials from layered double hydroxides (LDHs) precursors and demonstrate their applications in the CLC process. The LDHs precursor enables homogeneous mixing of elements at the molecular level, giving a high degree of dispersion and high-loading of active metal oxide in the support after calcination. Using a Cu-Al LDH precursor as a prototype, we demonstrate that rational design of oxygen storage materials by material chemistry significantly improved the reactivity and stability in the high temperature redox cycles. We discovered that the presence of sodium-containing species were effective in inhibiting the formation of copper aluminates (CuAl 2 O 4 or CuAlO 2 ) and stabilising the copper phase in an amorphous support over multiple redox cycles. A representative nanostructured Cu-based oxygen storage material derived from the LDH precursor showed stable gaseous O 2 release capacity (∼5 wt%), stable oxygen storage capacity (∼12 wt%), and stable reaction rates during reversible phase changes between CuO-Cu 2 O-Cu at high temperatures (800-1000 °C). We anticipate that the strategy can be extended to manufacture a variety of metal oxide composites for applications in novel high temperature looping cycles for clean energy production and CO 2 capture. Metal oxides nanocomposite derived from layered double hydroxides (LDHs) precursor demonstrated high oxygen release and storage capacity and excellent thermal stability in high temperature chemical-looping redox cycles for CO 2 capture applications.