Encapsulation of highly viscous CO2 capture solvents for enhanced capture kinetics: Modeling investigation of mass transfer mechanisms

Abstract The encapsulation of highly viscous liquid-like Nanoparticle Organic Hybrid Materials (NOHMs) inside a gas permeable polymer to form SIPs (Solvent Impregnated Polymers) significantly enhanced the CO2 capture kinetics of NOHMs, leading to a remarkable 50-fold increase in CO2 flux compared to the neat NOHMs. To understand the mechanism for enhanced CO2 mass transfer within these hybrid materials, kinetic modeling of CO2 uptake into SIPs containing polyethylenimine functionalized NOHMs, denoted NPEI-SIP, was conducted. CO2 mass transfer into NPEI-SIP films was found to conform, both qualitatively and quantitatively, with a diffusion-controlled moving front model. The diffusion-controlled model was also used to simulate CO2 uptake within a fixed bed containing polydisperse NPEI-SIP particles, and this model accurately predicted experimentally measured breakthrough curves at 25 °C and 50 °C. The 50-fold increase in gas flux was shown to be a consequence of the very large CO2 permeability within the polymer–solvent composite. The increase in gas flux is also dependent on the diffusion–reaction regime in which the chemical solvent operates, and the largest improvement will occur when immobilizing solvents, such as NOHMs, which operate in the instantaneous-reaction regime. The CO2 capacity (~3 mol CO2/kg) and saturation time (~5 min) of 430 μm SIP particles were comparable to popular CO2 chemisorption materials such as amine grafted silicates, in spite of the slow kinetics of NOHM-I-PEI in liquid form (CO2 saturation time ~24 h for a 1 mm thin film).