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

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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.
Funding Information
  • National Natural Science Foundation of China (W2512003)
  • National Natural Science Foundation of China (22572007)
  • National Natural Science Foundation of China (52203349)
  • National Key Research and Development Program of China (2025YFE0101800)
  • Natural Science Foundation of Hebei Province (B2024105009)

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