CO₂ Adsorption by Amino-Functionalized Graphene-Silica Gels

This work evaluates the CO₂-adsorption relevance and cycling stability of graphene oxide-silica (GO-SiO₂) and reduced graphene oxide-silica (rGO-SiO₂) gels after amine functionalization, demonstrating high-capacity retention under repeated adsorption-desorption cycles: rGO-SiO₂-APTMS retains ≈96.3% of its initial uptake after 50 cycles, while GO-SiO₂-APTMS retains ≈90.0%. The use of surfactants to control the organization of inorganic and organic molecules has enabled the development of ordered mesostructures, such as mesoporous silica and organic/inorganic nanocomposites. Owing to the outstanding properties of graphene and its derivatives, synthesizing mesostructures intercalated between graphene sheets offers nanocomposites with novel morphologies and enhanced functionalities. In this study, GO-SiO₂ and rGO-SiO₂ gels were synthesized and characterized by X-ray diffraction (XRD), differential scanning calorimetry (DSC), thermogravimetric analysis (TG), mass spectrometry (MS), N₂ adsorption-desorption isotherms, and transmission electron microscopy (TEM). The resulting materials exhibit a laminar architecture, with mesoporous silica domains grown between graphene-based layers; the silica contents are 83.6% and 87.6%, and the specific surface areas reach 446 and 710 m²·g^-1, respectively. The laminar architecture is retained regardless of the surfactant-removal route; however, in GO-SiO₂ obtained by solvent extraction, a fraction of the surfactant remains partially trapped. Together with their high surface area, hierarchical porosity, and amenability to surface functionalization, these features establish amine-grafted graphene-silica gels, particularly rGO-SiO₂-APTMS, as promising CO₂-capture adsorbents.