Montmorillonite is a natural clay mineral with a 2:1 layered structure and has good adsorption properties.However,it has a poor adsorption effect on organic pollutant because of its surface hydrophilicity.Organo-montmorillonite can improve the adsorption performance for organic pollutant due to the increasing hydrophobicity and extanded interlayer spacing.The main research contents of this article are as follows:(1)Three gemini surfactants with different chain lengths:propylbis(dodecyldimethyl)ammonium chloride(12-3-12),propylbis(hexadecyldimethyl)ammonium chloride(16-3-16)and propylbis(octadecyldimethyl)ammonium chloride(18-3-18)were used to modify calcium-based montmorillonite(Ca-Mt)to prepare a series of organic montmorillonites(G-Mt).(2)The obtained G-Mt was characterized by XRD and FT-IR.The analysis results showed that the three modifiers has successfully intercalated the interlayer of montmorillonite and increased the interlayer spacing of montmorillonite.G-Mt was applied to adsorb emerging micro-contaminants(ECs)of three benzotriazoles including 1-hydroxybenzotriazole(HOBT),benzotriazole(BTA)and 5-methylbenzotriazole(TTA).The experimental results indicated that under the same conditions,the adsorption sequence of the three G-Mt for ECs was G16-Mt>G12-Mt>G18-Mt.Specifically,when the added amount of 16-3-16 was 1.0 CEC,the modified montmorillonite(G16-Mt)exhibited the best adsorption capacity for three ECs.Thus,G16-Mt(1.0 CEC)was selected for the following adsorption experiments.(3)SEM,EDS,TG/DTG and BET analysis methods were carried out to characterize the structure and element content of Ca-Mt and G16-Mt.The results suggested that 16-3-16 has successfully entered the Ca-Mt interlayer and improved the interlayer basal spacing of Ca-Mt,which was beneficial to its adsorption for benzotriazole pollutants.Thus,the conditions of solution p H,reaction temperature,the initial solution concentration and reaction time for G16-Mt to absorb the three organic pollutants were further explored.It can be concluded that the optimal p H for removing HOBT,BTA and TTA was 4,9 and 9,respectively.The Langmuir isotherm model and the pseudo-second-order model fitted well the adsorption processes of the three pollutants.Thermodynamic results elucidated that the adsorption process was endothermic and spontaneous.(4)Based on the above studies,the adsorption performances of Ca-Mt and G16-Mt for Cu2+and benzotriazole pollutants in the single adsorption system and the co-adsorption system were investigated.In the single adsorption system,G16-Mt had a lower adsorption capacity for Cu2+than that of Ca-Mt,but has a higher adsorption capacity for three ECs.In the co-adsorption system,G16-Mt exhibited more adsorption amount for three organic pollutants and Cu2+than Ca-Mt.The results of FT-IR and XPS implied that Cu2+and ECs were adsorbed onto G16-Mt in the co-adsorption system by forming complexes and hydrophobic interactions.In addition,for co-adsorption systems,molecular dynamics simulation(MD),electrostatic potential distribution(ESP)and average localized ionization energy distribution(ALIE)were combined to decode the microscopic adsorption mechanism,indicating that the synergistic effect of Cu2+and ECs in the co-adsorption system promoted its simultaneous removal from wastewater.This research showed that gemini surfactant modified montmorillonite was an efficient,low-cost,non-toxic adsorption material,which provided detailed experimental data for its wide application in wastewater environment. |