In most countries, arsenic (As) and antimony (Sb) are regulated pollutants, due to their significant impacts on the environment and human health. Iron-based (Fe) coagulants play a fundamental role in the removal of both elements from aqueous media. This study aims to investigate the competitive removal of As and Sb in relation to Fe solubility. Coagulation experiments were conducted in synthetic water under various pH and contaminant loading, using ferric chloride (FC) as a coagulant. In the single system, the pentavalent species significantly reduced the Fe solubility and thereby enhanced the mobility of As and Sb under these environmental conditions. The coexistence of pentavalent and trivalent species in the binary system considerably decreases the Fe solubility at acidic conditions while enhancing the dissolution under alkaline conditions, thus affecting the overall removal of both species. The presence of four redox species in the quaternary system decreases the Fe solubility remarkably over a wide pH range, with better Sb removal, as compared to As under similar conditions. The adsorption study of the single system showed a decrease in As(V) adsorption capacity at higher concentration, while in the binary system, the Sb(III) showed strong adsorption potential, compared to other species. In the quaternary system, the presence of all four redox species has a synergistic effect on total Sb adsorption, in comparison to the total As. Furthermore, the results of Fourier transform infrared (FT-IR) analysis of FC composite contaminant flocs confirm that the combined effect of charge neutralization and inner sphere complexation might be a possible removal mechanism. These findings may facilitate the fate, transport and comparative removal of redox species in the heterogeneous aquatic environment.

Coagulation and precipitation appear to be the most efficient and economical methods for the removal of antimony from aqueous solution. In this study, antimony removal from synthetic water and Fe solubility with ferric chloride (FC) coagulation has been investigated. The effects of pH, FC dosage, initial antimony loading and mixed Sb(III), Sb(V) proportions on Fe solubility and antimony removal were studied. The results showed that the Sb(III) removal efficiency increased with the increase of solution pH particularly due to an increase in Fe precipitation. The Sb(V) removal was influenced by the solution pH due to a change in Fe solubility. However, the Fe solubility was only impaired by the Sb(III) species at optimum pH 7. The removal efficiencies of both Sb species were enhanced with an increase in FC dose. The quantitative analysis of the isotherm study revealed the strong adsorption potential of Sb(III) on Fe precipitates as compared to Sb(V). Furthermore, the removal behavior of antimony was inhibited in mixed proportion with high Sb(V) fraction. In conclusion, this study contributes to better understanding the fate of Sb species, their mobilities, and comparative removal behavior, with implications for Fe solubility using ferric chloride in different aqueous environments.

The presence of natural organic matter (NOM) in drinking water sources can stabilize toxic antimony (Sb) species, thus enhancing their mobility and causing adverse effects on human health. Therefore, the present study aims to quantitatively explore the complexation of hydrophobic/hydrophilic NOM, i.e., humic acid (HA), salicylic acid (SA), and L-cysteine (L-cys), with Sb in water. In addition, the removal of Sb(III, V) species and total organic carbon (TOC) was evaluated with ferric chloride (FC) as a coagulant. The results showed a stronger binding affinity of hydrophobic HA as compared to hydrophilic NOM. The optimum FC dose required for Sb(V) removal was found to be higher than that for Sb(III), due to the higher complexation ability of hydrophobic NOM with antimonate than antimonite. TOC removal was found to be higher in hydrophobic ligands than hydrophilic ligands. The high concentration of hydrophobic molecules significantly suppresses the Sb adsorption onto Fe precipitates. An isotherm study suggested a stronger adsorption capacity for the hydrophobic ligand than the hydrophilic ligand. The binding of Sb to NOM in the presence of active Fe sites was significantly reduced, likely due to the adsorption of contaminants onto precipitated Fe. The results of flocs characteristics revealed that mechanisms such as oxidation, complexation, charge neutralization, and adsorption may be involved in the removal of Sb species from water. This study may provide new insights into the complexation behavior of Sb in NOM-laden water as well as the optimization of the coagulant dose during the water treatment process.

Zinc oxide nanoparticles (ZnO NPs) are among the most widely used engineered nanoparticles (ENPs) in various commercial sectors to achieve both social and economic benefits. The post-use release of these NPs to the environment is inevitable, and may pose threat to the human and eco-system. In the present study, we investigated the influence of single and multiple environmental factors on sedimentation behavior of ZnO NPs. The fractional-factorial method based on Taguchi orthogonal array (OA) L 27 (3 13 ) design matrix was used for systematic investigation on the contribution and significance of multiple factors and their interactions. The result of single-factor showed that the ZnO NPs were unstable at or near pH zpc , with high electrolyte concentration; however, the adsorption of natural organic matter (NOM) i.e., humic acid, salicylic acid, and citric acid reverses the surface charge and enhanced NP stability. The Fourier transform infrared (FT-IR) analysis confirms the organic capping ligands on the NP surface. Moreover, the matrix result of analysis of variance (ANOVA) showed that electrolyte concentration and type, and NOM concentration were the most significant factors (p < 0.001) in promoting and influencing aggregation, while the interaction between the factors was also found insignificant. In addition, the result of aggregation kinetics and environmental water samples indicated that the mobility of ENPs may vary substantially in an environment with complex and heterogeneous matrices. This study may contribute to better understanding and prediction of the sedimentation behavior and fate of ZnO NPs in aqueous environments, to facilitate their sustainable use in products and process.

The large-scale production and usage of zinc oxide nanoparticles (ZnO NPs) may lead to their post-release into the aquatic environment. In this study, the effect of hydrophobic/hydrophilic organic ligands on sorption and sedimentation of ZnO NPs has been systematically investigated. In addition, the coagulation efficiency of ZnO NPs, Zn2+, dissolved organic carbon (DOC), and UV254 with varying ferric chloride (FC) dosages in synthetic waters were also evaluated. The results showed that the higher concentration of organic ligands, i.e., humic acid (HA), salicylic acid (SA), and L-cysteine (L-cys) reduced the ζ-potential and hydrodynamic diameter (HDD) of particles, which enhanced the NPs stability. The adsorption of organic ligands onto ZnO NPs was fitted with the Langmuir model, with maximum adsorption capacities of 143, 40.47, and 66.05 mg/g for HA, SA and L-cys respectively. Removal of up to 95% of ZnO NPs and Zn2+ was achieved in studied waters at the effective coagulation zone (ECR), above which excess charge induced by coagulant restabilized the NPs in suspension. Moreover, the removal rate of DOC and UV254 were found to be higher in hydrophobic waters than hydrophilic waters. The width of ECR strongly depends on the characteristics of source water. The waters with hydrophobic ligand and higher UV254 values require more coagulant than hydrophilic waters to achieve the similar ZnO NPs and Zn2+ removal. The results of Fourier transform infrared (FT-IR) analysis of ZnO NPs composite contaminant flocs indicated that the combined effect of enmeshment and charge neutralization might be a possible removal mechanism. These findings may facilitate the prediction of fate, transport, and removal of ZnO NPs in the natural waters, and might contribute to risk assessment, as well as decision making about engineered nanoparticles (ENPs) in aquatic systems.