To explore the effect of spacer structure on the adsorption capability of organo-vermiculites (organo-Vts), a series of aza-containing gemini surfactants (5N, 7N and 8N) are applied to modify Na-vermiculite (Na-Vt). Large interlayer spacing, strong binding strength and high modifier availability are observed in organo-Vts, which endow them with superiority for the adsorption of 2-naphthol (2-NP) and bromophenol blue (BPB). The maximum adsorption capacities of 5N-Vt, 7N-Vt and 8N-Vt toward 2-NP/BPB are 142.08/364.49, 156.61/372.65 and 146.50/287.90 mg/g, respectively, with the adsorption processes well fit by the PSO model and Freundlich isotherm. The quicker adsorption equilibrium of 2-NP than BPB is due to the easier diffusion of smaller 2-NP molecules into the interlayer space of organo-Vts. Moreover, stable regeneration of 7N-Vt is verified, with feasibility in the binary-component system that is demonstrated. A combination of theoretical simulation and characterization is conducted to reveal the adsorption mechanism; the adsorption processes are mainly through partition processes, electrostatic interaction and functional interactions, in which the spacer structure affects the interlayer environment and adsorptive site distribution, whereas the adsorbate structure plays a role in the diffusion process and secondary intermolecular interactions. The results of this study demonstrate the versatile applicability of aza-based organo-Vts targeted at the removal of phenols and dyes as well as provide theoretical guidance for the structural optimization and mechanistic exploration of organo-Vt adsorbents.
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