This study presents the environmentally sustainable synthesis of zeolites from solar-calcined kaolin and halloysite, emphasizing their application in CO2 capture due to their distinctive porous structures and chemical attributes. Expanding upon prior research that utilized solar energy for kaolin calcination, we now explore halloysite as an alternative clay mineral for zeolite production and CO2 capture. Employing a solar simulator, halloysite was calcined at temperatures ranging from 700 to 1000 °C, resulting in the synthesis of zeolites 4A and 13X via hydrothermal methods. The synthesized zeolites were characterized using X-ray diffraction (XRD), low angle XRD (LA-XRD), transmission electron microscopy (TEM), and field-emission scanning electron microscopy (FE-SEM), and Brunauer–Emmett–Teller (BET) surface area measurements. Notably, the presence of Al-Si spinel, which crystallizes at elevated solar calcination temperatures, persisted within the zeolite 13X matrix, inducing a secondary mesoporous phase. The observed hysteresis in 13X samples, rather than confirming the mesoporous character of zeolite 13X, indicates a tandem effect of mesoporous Al-Si spinel with microporous zeolite 13X, exemplifying systems known as micro/mesoporous zeolitic composites (MZCs). The correlation obtained between the interplanar distances calculated from LA-XRD and pore size distributions acquired from the BJH desorption branches highlights LA-XRD as an alternative analysis method for assessing mesoporosity. While the microporosity of Al-Si spinel possessing 13X samples positively correlates with CO2 capture performance, mesoporosity appears to have minimal impact. Among the zeolites synthesized using solar energy, zeolite 4A (LTA) demonstrates superior CO2 capture capability, achieving an adsorption capacity of 2.15 mmol/g at 25 °C and 1 bar. This study highlights the potential of solar energy in producing eco-friendly zeolites from kaolin and halloysite for improved CO2 capture, advancing sustainable environmental solutions.
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