Direct CO₂ capture from simulated and Ambient Air over aminosilane-modified hierarchical silica

Aminosilane-modified Hierarchical silica, HSA and HST-based adsorbents were synthesized by aminosilanization using Hierarchical silica (HS) with 3-aminopropyltriethoxysilane (APS) and N1-(3-trimethoxysilylpropyl)dieth- ylenetriamine (TMPTA), respectively, and characterized to establish their physicochemical, structural, morphological, and porosity properties. Their CO2 adsorption performance was evaluated under direct air capture (DAC) conditions: 1) simulated air with CO2 concentration of 400 ppm in helium (He) at 30 degrees C and 2) indoor air with CO2 concentration >= 400 ppm at 30 degrees C, where HSA and HST modified with 70 wt% of respective aminosilanes outperformed others. The modified HS adsorbents showed an increase in kinetics, CO2 uptake under dry and humid conditions, stable cyclic adsorption-desorption performance, moderate enthalpy of desorption indicating a dominant chemisorption mechanism. Under dry and humid simulated air conditions (400 ppm CO2 in He), HSA-70 displayed a CO2 uptake of 0.82 mmol/g and 1.70 mmol/g, respectively, while HST-70 exhibited enhanced CO2 uptake of 1.54 mmol/g and 2.08 mmol/g, respectively. Cyclic stability of HSA70 and HST-70 was confirmed through five thermal swing adsorption (TSA) cycles. In addition to this, their use for indoor air CO2 capture was also explored through ten short TSA cycles. Developed HSA-70 and HST-70 adsorbents exhibited more selectivity for CO2 over water, demonstrating their usage in practical direct air CO2 capture application.