K₂CO₃-Impregnated Al/Si Aerogel Prepared by Ambient Pressure Drying for CO₂ Capture: Synthesis, Characterization and Adsorption Characteristics

Abstract

A new potassium-based adsorbent for CO2 capture with Al aerogel used as support is proposed in this work. The adsorbents with different surface modifiers (tetraethyl orthosilicate (TEOS) and trimethyl chlorosilane (TMCS)) and different K2CO3 loadings (10%, 20%, 30% and 40%) were prepared by sol-gel and iso-volume impregnation processes with ambient pressure drying. The CO2 adsorption performance of the adsorbents were tested by a fixed-bed reactor, and their adsorption mechanisms were studied by scanning electron microscopy (SEM), Brunauer Emmett Teller (BET), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, and X-ray fluorescence spectrometry (XRF). Furthermore, the adsorption kinetics and the cycling performance were investigated. The results show that using TEOS to modify the wet gel can introduce SiO2 to increase the strength of the skeleton. On the basis of TEOS modification, TMCS can further modify –OH, thus effectively avoiding the destruction of aerogel structure during ambient drying and K2CO3 impregnation. In this work, the specific surface area and specific pore volume of Al aerogel modified by TEOS + TMCS are up to 635.32 cm2/g and 2.43 cm3/g, respectively. The aerogels without modification (Al-B), TEOS modification (Al/Si) and TEOS + TMCS modification (Al/Si-TMCS) showed the best CO2 adsorption performance at 20%, 30% and 30% K2CO3 loading, respectively. In particular, the CO2 adsorption capacity and K2CO3 utilization rate of Al/Si-TMCS-30K are as high as 2.36 mmol/g and 93.2% at 70 degrees Celsius (°C). Avrami’s fractional order kinetic model can well fit the CO2 adsorption process of potassium-based adsorbents. Al-B-20K has a higher apparent activation energy and a lower adsorption rate during the adsorption process. After 15 adsorption-regeneration cycles, Al/Si-TMCS-30K maintain a stable CO2 adsorption capacity and framework structure, while the microstructure of Al/Si-30K is destroyed, resulting in a decrease in its adsorption capacity by nearly 30%. This work provides key data for the application of Al aerogel in the field of potassium-based adsorbent for CO2 capture.

Keywords

• Al/Si aerogel
• surface modification
• potassium-based adsorbent
• CO₂ adsorption performance
• adsorption kinetics