Valorization Strategies in CO₂ Capture: A New Life for Exhausted Silica-Polyethylenimine

The search for alternative ways to give a second life to materials paved the way for detailed investigation into three silica-polyethylenimine (Si-PEI) materials for the purpose of CO₂ adsorption in carbon capture and storage. A solvent extraction procedure was investigated to recover degraded PEIs and silica, and concomitantly, pyrolysis was evaluated to obtain valuable chemicals such as alkylated pyrazines. An array of thermal (TGA, Py-GC-MS), mechanical (rheology), and spectroscopical (ATR-FTIR, ¹H-¹³C-NMR) methods were applied to PEIs extracted with methanol to determine the relevant physico-chemical features of these polymers when subjected to degradation after use in CO₂ capture. Proxies of degradation associated with the plausible formation of urea/carbamate moieties were revealed by Py-GC-MS, NMR, and ATR-FTIR. The yield of alkylpyrazines estimated by Py-GC-MS highlighted the potential of exhausted PEIs as possibly valuable materials in other applications.