Design of blend-amine solid adsorbents for CO2 capture: Enhances adsorption- equilibrium cycle strategies and mechanism

[Display omitted] •A new method of introducing AEEA to improve the adsorption properties of PEI was developed.•CO2 adsorption capacity of AEEA-PEI was increased by 84.6% over that of pure PEI.•The cycling stability of the AEEA-PEI system was markedly enhanced with the introduction of PMDETA.•The enhanced mechanism of AEEA in blend amine was elucidated.•A plausible promote AEEA regeneration mechanism was proposed. Blend amine-functionalized absorbents show great potential in the field of amine scrubbing for CO2, as they harness the absorption benefits of various monomer amines in combination. However, there is a lack of research on the application of the emerging concept of blend amines to solid amine adsorbents. Building upon this foundation, this study firstly incorporated Aminoethylethanolamine (AEEA) into Polyethyleneimine (PEI) of varying molecular weights to create a range of new binary solid amine adsorbents. The research then compared the adsorption performance differences between these binary adsorbents and pure PEI adsorbents. The enhanced dispersion of PEI by AEEA results in an increase in the effective active sites available. The amine efficiency and CO2 adsorption capacity of the AEEA-PEI blend amine system were maximally increased by 92.0% and 84.6%, respectively, compared to the pure PEI system. Furthermore, through DFT calculations, it is clear that the presence of AEEA lowers the overall activation energy of the reaction due to its superior proton acceptance compared to PEI. However, the AEEA-PEI system exhibits weak cycling stability attributed to the limited regeneration capacity of AEEA. Fortunately, this issue can be successfully addressed by introducing a strong base, N,N,N',N'',N''-pentamethyl diethylenetriamine (PMDETA). The CO2 adsorption cycling stability for AEEA-PEI-PMDETA system maximally improved by up to 17.1% compared to the AEEA-PEI system. The mechanism behind the effectively suppression of cycling losses by PMDETA was further elucidated through DFT calculations. Consequently, the novel ternary amine solid adsorbent introduced in this study, aimed at enhancing the CO2 adsorption performance of monomer amine solid adsorbents, offers a fresh strategy for fundamental theoretical investigations into CO2 adsorption.