Scalable, Durable, and Malleable PVMDMS@PVP Aerogel Catalyst for CO2 Capture and Successive Gas-Phase Cycloaddition Reaction

A structurally robust PVMDMS@PVP aerogel catalyst was developed by incorporating polyethyleneimine (PEI) and an ionic liquid, followed by Zn ²⁺ impregnation, for integrated carbon dioxide (CO ₂ ) capture and catalytic conversion. The solvent-resistant framework maintains high CO ₂ adsorption capacity and structural integrity across 50 thermal cycles over a broad temperature range (0–130°C). Breakthrough experiments confirm excellent CO ₂ /N ₂ selectivity (5078) under mixed-gas flow at 100°C. Zn ²⁺ -functionalized aerogels enable gas-phase cycloaddition of CO ₂ with epoxides, achieving >99% selectivity for propylene carbonate over 1978 hours of continuous operation. Notably, the carbonate product was directly applied as an electrolyte in lithium-ion batteries, validating its electrochemical utility. The aerogel preserved its pore structure, catalytic activity, and monolithic form even after scale-up, demonstrating superior mechanical and chemical durability. This work presents a scalable, multifunctional aerogel catalyst platform that combines long-term stability, high CO ₂ adsorption efficiency, and battery-relevant carbonate production for advanced CO ₂ capture and utilization technologies.