Scalable, durable, and malleable PVMDMS@PVP aerogel catalyst for CO2 capture and successive gas-phase cycloaddition reaction

Abstract

A structurally robust PVMDMS@PVP aerogel catalyst was developed by incorporating polyethyleneimine (PEI) and an ionic liquid, followed by Zn2+ impregnation, for integrated carbon dioxide (CO2) capture and catalytic conversion. The solvent-resistant framework maintains high CO2 adsorption capacity and structural integrity across 50 thermal cycles over a broad temperature range (0–130 °C). Breakthrough experiments confirm excellent CO2/N2 selectivity (5078) under mixed-gas flow at 100 °C. Zn2+-functionalized aerogels enable gas-phase cycloaddition of CO2 with epoxides, achieving > 99% selectivity for propylene carbonate over 1978 h 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 CO2 adsorption efficiency, and battery-relevant carbonate production for advanced CO2 capture and utilization technologies.