Efficient Calcium Looping-Integrated Methane Dry Reforming by Dual Functional Aerosol Ca–Ni–Ce Nanoparticle Clusters

Calcium looping (CaL) integrated with methane dry reforming (DRM) shows promise for carbon capture and utilization. To enhance the CaL–DRM tandem processes, a raspberry-structured aerosol dual-functional material composed of CaO (CO2 adsorbent), Ni (DRM catalyst), and CeO2 (promoter) was fabricated via gas-phase evaporation-induced self-assembly. The utilization of Ca–Ni–Ce is highly beneficial by the creation of metal–support–promoter interaction for promoting an effective carbon capture followed by interfacial catalysis, providing an alternative pathway with enhanced redox ability and reduction of activation energy. The Ca–Ni–Ce composite materials with clustered particle characteristics showed great improvement in the performance of cyclic CaL–DRM in comparison to the reported values: low required carbonation/decarbonation temperatures (400/600 °C), high CO2 uptake efficiency (12.1 mmolCO2/gCaO), ultrahigh CO2 conversion (97.2%) under relatively low-temperature operation (600 °C), and sufficiently high operational stability. Overall, the proposed Ca–Ni–Ce hybrid material fabricated via the aerosol synthetic method demonstrates significant advances in the low-temperature CaL–DRM processes, showing promise as a sustainable chemical engineering route for industrial applications.