Role of brush-like additives in CO2 adsorbents for the enhancement of amine efficiency

Amine adsorbents have been widely investigated for direct CO2 capture from air. However, the low amine efficiency of the widely-studied amine sorbents is the critical factor to hinder the practical application under dry conditions. Herein, we developed the brush-like cetyltrimethylammonium chloride (CTAC) templating strategy to prepare micro-mesoporous silica nanoparticles (MMSN-X) and TEPA-functionalized adsorbents (MMSN-X/TEPA-Y). The character of samples was investigated by transmission electron microscopy, N2 adsorption-desorption, Fourier transform infrared spectroscopy, thermal gravimetric analyzer and X-ray photoelectron spectroscopy. The adsorbent (MMSN-30/TEPA-50) with appropriate amount of brush-like CTAC exhibited higher CO2 adsorption capacities (3.68 mmol/gadsorbent under simulated dry air conditions) than that of the adsorbents with none or less additives. The kinetic and thermodynamic model were applied to investigate the adsorption rate control factors and adsorption behavior of CO2 adsorbents with brush-like CTAC. Moreover, with the effect of brush-like CTAC, the significant variation of adsorption product (conversion from carbamate (CO2/N = 0.5) to carbamic acid (CO2/N = 1)) was detected by in situ Fourier transform infrared spectroscopy. These results demonstrated that the combination of CO2 and amine was altered in the presence of brush-like CTAC and thereby the amine efficiency was enhanced, which could be expected to be an efficient adsorbent for CO2 from air in practical applications. [Display omitted] Diagram for a subtle strategy on development of high-performance adsorbents under the simulated air. •Different density of brush-like CTAC in solid amine sorbents were prepared for CO2 capture.•The optimal capacity of the adsorbent with CTAC (3.68 mmol/g for 0.0400 vol% CO2) was 50% higher than that without CTAC.•The introduction of brush-like CTAC promoted carbamic acid generation and thus enhanced amine efficiency.•In situ FTIR and kinetics models were used to interpret adsorption behavior.