Direct conversion of captured CO 2 into syngas via interface‐coupled carbonate activation in dual‐functional materials

Abstract Integrated carbon capture and utilization can reduce the energy penalty of CO 2 valorization, but is often limited by slow transport between capture and catalytic sites. Here, we report a proximity‐engineered dual‐functional material for direct conversion of captured CO 2 into syngas via isothermal calcium‐looping dry reforming of methane at 650°C. Embedding trace Ni into a CaO framework and introducing CeO 2 creates abundant Ni–Ce–Ca interfacial sites with shortened carbonate diffusion pathways, enhanced oxygen mobility, and improved resistance to sintering and coking. The optimized material achieves a CO 2 capture capacity of 12.6 mmol g −1 and a syngas yield of 58 mmol g −1 , representing up to a 2.9‐fold improvement over conventional materials. Operando spectroscopy and density functional theory reveal that captured carbonates are directly converted through a lower‐energy COOH‐mediated interfacial pathway, demonstrating an effective strategy to overcome transport limitations in integrated CO 2 capture and conversion.