Recyclable poly(vinylmethyldimethoxysilane)-poly(vinylpyrrolidone) hybrid aerogel as a robust scaffold for integrated CO2 adsorption and cycloaddition catalysis

초록

Integrating carbon dioxide (CO2) capture and conversion within a single system enables efficient and sustainable catalytic processes. Here, we report a chemically reinforced silica-based aerogel, synthesized by covalent coupling of poly(vinylmethyldimethoxysilane) (PVMDMS) and polyvinylpyrrolidone (PVP), forming a robust poly(vinylmethyldimethoxysilane)@poly(vinylpyrrolidone) (PVMDMS@PVP) scaffold. This aerogel accommodates tetraethylenepentamine (TEPA) and 1-ethyl-3-methylimidazolium bromide ([EMIm]Br) within its hierarchically porous matrix, functioning as a Supported Liquid Phase (SLP) system that immobilizes active liquid components for CO2 adsorption and cycloaddition. The system demonstrated high static CO2 adsorption capacity (5.0 mmol center dot g-1 at 40 degrees C) and superior dynamic performance under CO2/N2 (15:85) flow (5.3 mmol center dot g-1, selectivity 450). Cycloaddition with styrene oxide yielded 86.4 % with 95.1 % selectivity. Following washing and re-impregnation, the aerogel maintained structural integrity and catalytic activity, achieving up to 93.3 % yield and 99.7 % selectivity upon recycling. Pore structure analysis revealed that, although minor changes were observed due to etching during the cycling process, the overall framework and hierarchical pore architecture of the PVMDMS@PVP aerogel remained intact, supporting its structural robustness and recyclability.

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