Amino-functionalized mesoporous silica-magnetic graphene oxide nanocomposites as water-dispersible adsorbents for the removal of the oxytetracycline antibiotic from aqueous solutions: adsorption performance, effects of coexisting ions, and natural organic matter

摘要

The amino-functionalized mesoporous silica-magnetic graphene oxide nanocomposite (A-mGO-Si) was synthesized and used for oxytetracycline (OTC) removal from water. Various factors like the effects of initial concentration, contact time, and influence of pH were investigated. Selective adsorption experiments in connection with coexisting ions and dissolved organic matter (DOM) were also investigated. In this study, humic acid (HA) and tannic acid (TA) were representative of both hydrophobic and hydrophilic DOM, respectively. Results indicated that A-mGO-Si had an adsorption ability for OTC that was relatively greater than that of virgin magnetic graphene oxide (mGO), graphene oxide (GO), Fe3O4 particles, and SBA-15 mesoporous silica and also showed a better uptake removal capacity for OTC at low initial concentration in comparison with the other adsorbents. The adsorption behavior of OTC onto A-mGO-Si could be described by the pseudo-second-order kinetic model and the Freundlich isotherm model. The electrostatic interaction has no influence on the OTC absorbed when the OTC is in an aqueous medium in its zwitterion form (3.22 < pH < 7.46). At high pH, the weak pi-pi EDA interactions and hydrogen bonding may manifest themselves, hence causing a lower adsorption capacity. The main adsorption mechanisms were plausibly activated by H-bonding, and pi-pi EDA interactions, while the electrostatic interaction (cation-pi interaction) might be the minor adsorption mechanism. Addition of individually exogenous ions (Na+, Mg2+, NO-, and CO32-) resulted in a decrease of OTC adsorption due to the emergence of a competitive effect. Considering the presence ofHAand TA in mixed solute systems, the DOMwas likely to form a stronger interaction system with mGO-Si, thereby resulting in an adsorption level which was more competitive in the process at low aqueous phase concentration of OTC. In contrast to the high aqueous phase, the coexistence of DOM could promote OTC adsorption. The phenomenon may reflect the result that a surface complexation mechanism could achieve in adsorptions.