Abstract

This study explores the efficient preparation of few-layered or monolayered kaolinite (K) nanosheets using supercritical gasification exfoliation technology, aiming to enhance their adsorption capacity for Ga(III). Crystal structure and morphology analysis indicated that the exfoliated K nanosheets maintained an excellent hexagonal lamellar crystal shape, with significantly reduced thickness (∼10 nm) while maintaining an unchanged lateral dimension (400 ∼ 600 nm). The exfoliation mechanism primarily relies on the considerable impact force generated by the rapid expansion of supercritical carbon dioxide (CO2) volume during fast pressure release, which facilitates exfoliation between K layers where the interlayer hydrogen bonds have been disrupted by potassium acetate. Batch adsorption experiments demonstrated a significant improvement in the removal rate of exfoliated K for Ga(III), increasing from 50.66 % to 80.47 % under the conditions of a Ga(III) concentration of 15 mg/L and an adsorbent dosage of 0.4 g/L, attributed to the exposure of numerous active sites. Kinetic and isotherm fitting results indicated a monomolecular adsorption process primarily controlled by chemical adsorption, with a maximum theoretical adsorption capacity of 32.90 mg/g for Ga(III). In multivariate mixed adsorption experiments, exfoliated K exhibited good adsorption selectivity for Ga(III), primarily through chemical adsorption of aluminum hydroxide (Al–OH) functional groups and electrostatic adsorption of silicon oxide (Si–O). Density functional theory (DFT) calculations further demonstrated that the bidentate adsorption coordination of K with Ga(III) exhibits higher stability compared to monodentate adsorption coordination, indicating that the adsorption process is mainly dominated by bidentate adsorption. Consequently, the supercritical gasification exfoliation technology, as a recyclable green process, offers efficient exfoliation of K, holding significance implications for the high-value and high-efficiency utilization of K resources, as well as for establishing a green, low-carbon, and recycling development economic system.