Abstract

The solar-driven thermochemical CO2 conversion is an effective way to achieve the mission of carbon peaking and carbon neutrality. However, finding a material with excellent thermal stability, oxygen exchange capacity, and CO selectivity is one of the most important challenges in the thermochemical CO2 conversion approach. This study investigated the solar thermochemical CO2-splitting characteristics through the synergistic thermal catalytic activity of CuO and NiFe2O4 and the effect of SiC photothermal properties. The thermochemical redox cycling performance of CO2 conversion through thermally activated catalysts was experimentally investigated via thermogravimetric combined quantum chemical calculations to provide comprehensive insights into the physicochemical principles underlying the thermochemical catalytic CO2-splitting. The X-ray diffraction, scanning electron microscopy, and energy spectrum detector technics were developed to gain detail on the crystal structure, surface morphology, and chemical composition changes in the reacting media. The newly synthesized composite material consisting of 25%CuO and 75%NiFe2O4 (CNF-13) coated SiC porous skeleton resulted in higher CO2-splitting catalytic activity with an instantaneous CO production of 10.98mL ⋅ min‐1gCNF‐13−1 and direct CO2-to-CO conversion rate of 33.9% at 1000–1200 K reaction temperature. The thermochemical CO2-splitting activity and redox stability of CNF-13@SiC was promoted by the photothermal properties of SiC support and the formation of Cu2O and Fe3O4 new active material phases easing CO2 reduction at low energy. This study provided experimental and theoretical findings that can be used as guidance for the fundamental research and application of CO2 catalytic conversion into fuels through a solar thermochemical driven strategy.

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