Abstract
Pyrite affects the adsorption of tylosin (TYL) due to their coexistence in the lake system. As well as the reactivity groups of S–S-H, S-OH, and Fe-OH, defects also have the possibilities to influence the adsorption of organic contaminants. However, the role of these active sites in antibiotic adsorption on pyrite has not been deeply studied. Besides, pH, N, P, dissolved oxygen, and dissolved organic matter (DOM) fluctuate greatly in lake at different seasons, which may change the surface characteristics of pyrite. Hence, the adsorption of TYL on natural pyrite considered solution chemistry and DOM in lake water was explored in this study. The fitting results of the kinetic and isotherm models showed that the adsorption included physical and chemical interactions. The neutral initial solution pH was conductive to TYL adsorption owing to the combined result of electrostatic and cover of Fe-oxyhydroxide. NO3− and NH4+ had no effect on TYL adsorption, whereas H2PO4− promoted adsorption by forming flocculent Fe(H2PO4)3 precipitates. The dissolved oxygen increased adsorption. This is due to the co-promotion of the pyrite oxidation by oxygen and sulfur defects. The Fe(II)-DOM complex caused by pyrite surface oxidation reduced the concentration of TYL in solution by gathering. Except for the surface charge, reactivity groups on pyrite significantly influenced the adsorption of TYL. The bond fracture of S–S resulted in sulfur defects that contributed to pyrite oxidation. As a result, Fe(III)/Fe(II) on the surface of pyrite or in solution produced a complex Fe(III)/Fe(II) with anions and DOM. In addition, Fe(III)-S on sulfur defects interacted with the O–H of TYL through hydrogen bonding. Furthermore, the Fe–O-C bond is formed by the interaction of C–OH on TYL and Fe(III) (hydr)oxides on the surface of pyrite. The study provides a deep insight into the effect of pyrite surface active sites on amphoteric antibiotic adsorption. It helps to understand antibiotic migration and interactions with widespread pyrite in the real environment.
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The datasets used and analyzed during the current study are available from the corresponding author on reasonable request.
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Funding
This work was supported by the National Natural Science Foundation of China (grant numbers 41967042, 747U21A20179, and 41807392) and the Natural Science Foundation of Guangxi (grant number 2018GXNSFBA281097).
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All authors contributed to the study conception and design. Material preparation, data collection, and analysis were performed by Qian Zhang, Jinwen Zhou, and Xiaohua Shu. The first draft of the manuscript was written by Qian Zhang and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
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Highlights
1. The sulfur defects existed on pyrite accelerate the oxidation of pyrite.
2. Fe(III)-S on sulfur defects interacts with O-H of TYL through hydrogen bonding.
3. Fe-O-C forms between C-OH on TYL and Fe(III) (hydr)oxides on the surface of pyrite.
4. The solution chemistry and DOM affect TYL adsorption ultimately related to oxidation of pyrite.
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Zhang, Q., Zhou, J., Zhang, L. et al. Sulfur defect and Fe(III) (hydr)oxides on pyrite surface mediate tylosin adsorption in lake water: effect of solution chemistry and dissolved organic matter. Environ Sci Pollut Res 29, 90248–90258 (2022). https://doi.org/10.1007/s11356-022-22140-7
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DOI: https://doi.org/10.1007/s11356-022-22140-7