Molecular basket sorbents polyethylenimine–SBA-15 for CO2 capture from flue gas: Characterization and sorption properties

A series of molecular basket sorbents consisting of SBA-15 loaded with different amounts of polyethylenimine (PEI) have been systematically studied, focusing on their characterization by small angle X-ray scattering (SAXS), N2 physisorption, scanning electron microscopy (SEM), and thermogravimetric analysis (TGA) and their CO2 sorption properties. The meso-structure of SBA-15 was retained after PEI loading. When the PEI loading was no more than 50 wt.%, PEI was dispersed and filled inside the pore channels of SBA-15. Higher PEI loading resulted in a part of the loaded PEI coating on the external surface of the SBA-15 particles and thus caused the agglomeration. The effects of sorption temperature and PEI loading on the CO2 capacity of the PEI/SBA-15 sorbents were examined over a fixed-bed flow system using a model flue gas. The relationship between the sorption performance and the sorbent structure has been discussed. CO2 diffusion in the PEI bulk may play a crucial role for determining the CO2 sorption capacity and sorption/desorption rate at low temperature. With the increase of the sorption temperature, CO2 diffusion can be accelerated and more amine sites may be exposed and accessible for CO2 sorption. As a result, the sorption capacity increases. However, at further higher temperature, e.g., 100 °C, the sorption capacity decreases due to the dominant desorption. In addition, the sorption behavior of SBA-15 and PEI-50/SBA-15 at high CO2 pressures (up to 50 bars) has been studied. The results showed that CO2 sorption over PEI/SBA-15 occurs mainly via chemisorption even under pressurized conditions.

Graphical abstractA series of polyethylenimine–SBA-15 based solid composite materials have been designed via the novel concept of “molecular basket” and systematically characterized and studied on their sorption properties for CO2 capture.Figure optionsDownload full-size imageDownload as PowerPoint slideHighlights► A series of MBS consisting of SBA-15 with different PEI loadings were characterized and evaluated for CO2 capture. ► The texture properties and CO2 sorption properties of MBS vary greatly with PEI loading. ► Temperature profoundly influences the CO2 sorption performance of MBS. ► Both the thermodynamics and kinetics play a crucial role in CO2 capture over MBS. ► CO2 sorption over MBS occurs mainly via chemisorption at both low and high pressures.