Synergistic promotions between CO₂ capture and in-situ conversion on Ni-CaO composite catalyst

The integrated CO₂ capture and conversion (iCCC) technology has been booming as a promising cost-effective approach for Carbon Neutrality. However, the lack of the long-sought molecular consensus about the synergistic effect between the adsorption and in-situ catalytic reaction hinders its development. Herein, we illustrate the synergistic promotions between CO₂ capture and in-situ conversion through constructing the consecutive high-temperature Calcium-looping and dry reforming of methane processes. With systematic experimental measurements and density functional theory calculations, we reveal that the pathways of the reduction of carbonate and the dehydrogenation of CH₄ can be interactively facilitated by the participation of the intermediates produced in each process on the supported Ni-CaO composite catalyst. Specifically, the adsorptive/catalytic interface, which is controlled by balancing the loading density and size of Ni nanoparticles on porous CaO, plays an essential role in the ultra-high CO₂ and CH₄ conversions of 96.5% and 96.0% at 650 °C, respectively.