摘要
CO 2 -splitting and thermochemical energy conversion effectiveness are still challenged by the selectivity of metal/metal oxide-based redox materials and associated chemical reaction constraints. This study proposed an interface/substrate engineering approach for improving CO 2 -splitting and thermochemical energy conversion through CuFe 2 O 4 and Co 3 O 4 two-layer coating SiC. The newly prepared material reactive surface area available for gas–solid reactions is characterized by micro-pores CuFe 2 O 4 alloy easing inter-layer oxygen micro mass exchanges across a highly stable SiC-Co 3 O 4 layer. Through a thermogravimetry analysis, oxidation of the thermally activated oxygen carriers exhibited remarkably CO 2 -splitting capacities with a total CO yield of 1919.33 µmol/g at 1300 °C. The further analysis of the material CO 2 -splitting performance at the reactor scale resulted in 919.04 mL (788.94 µmol/g) of CO yield with an instantaneous CO production rate of 22.52 mL/min and chemical energy density of 223.37 kJ/kg at 1000 °C isothermal redox cycles. The reaction kinetic behavior indicated activation energy of 30.65 kJ/mol, which suggested faster CO 2 activation and oxidation kinetic on SiC-Co 3 O 4 -CuFe 2 O 4 O-deficit surfaces. The underlying mechanism for the remarkable thermochemical performances was analyzed by combining experiment and density functional theory (DFT) calculations. The significance of exploiting the synergy between CuFe 2 O 4 and Co 3 O 4 layers and stoichiometric reaction characteristics provided fundamental insights useful for the theoretical modeling and practical application of the solar thermochemical process.
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