▎ 摘　　要

This work investigates the performance of amine functionalised 2D/3D sorbents for CO2 capture. The 2D/3D structures were based on a combination of flake-like reduced graphene-silica oxide (G-Si) aerogel and rod-like mesoporous silica SBA-15. The G-Si aerogel formed mainly silica microporous structures which enveloped graphene sheets. The SBA-15 displayed the classical rod-like mesoporous features with high pore volume. The addition of G-Si aerogel to SBA-15 for the amine functionalised samples significantly reduced the combined total surface area and pore volume. Interestingly, the CO2 sorption capacity increased and peaked for samples containing G-Si aerogel/SBA-15 at 1:20 mass ratio (4.7 wt%), though declining thereafter. This counterintuitive effect of increasing CO2 sorption capacity but decreasing surface area and pore volume was attributed to the special morphological features of the 2D/3D sorbent assembly. At these optimal conditions, the flake-like G-Si aerogel was well intercalated with the rod-like SBA-15. As a result, the inter-particle space formed between the flake-like and rod-like assembly accommodated TEPA which facilitate the mass transfer and reaction between the amine groups and CO2. These special 2D/3D morphological features delivered high CO2 sorption capacity of 6.02 mmol g(-1). The 2D/3D sorbents were also very stable under sorption and desorption cycles whilst heat of sorption were up to 22% lower than the analogue 3D SBA-15/TEPA sorbent.