4.7 Article

Performance and mechanisms of PropS-SH/Ce(dbp)3 coatings in the inhibition of pyrite oxidationtion for acid mine drainage control

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ENVIRONMENTAL POLLUTION
卷 322, 期 -, 页码 -

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ELSEVIER SCI LTD
DOI: 10.1016/j.envpol.2023.121162

关键词

Pyrite; Acid mine drainage; 3-Mercaptopropyltrimethoxysilane; Cerium dibutyl phosphate; Self-healing

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Inhibition of tailings oxidation effectively controls the generation of acid mine wastewater. A PropS-SH/Ce(dbp)3 passivator with excellent passivation performance and self-healing properties was prepared by using 3-mercaptopropyltrimethoxysilane and dibutyl phosphate as the main passivating agent and repair agent respectively. By adjusting the pH and curing time, the passivation coating achieved room-temperature curing and showed enhanced passivation performance with the addition of 0.2 wt% Ce(dbp)3. The passivation and self-healing mechanisms were investigated, and it was found that a cross-linked mesh structure was formed by Si-O-Si bonding and Ce(dbp)3 played a role in repairing the passivation coating.
Inhibition of tailings oxidation could availably control the generation of acid mine wastewater from its source. Organosilanes serving as a high-efficiency inhibitor of the oxidation of pyrite, bring some problems including safety hazards caused by large amounts of organic solvents, difficult high-temperature curing, poor long-term properties, and so on. In our work, the PropS-SH/Ce (dbp)(3) (PS/Ce (dbp)(3)) passivator with excellent passivation performance and self-healing properties was prepared by choosing 3-mercaptopropyltrimethoxysilane (PropS-SH) and dibutyl phosphate (Ce (dbp)(3)) as the main passivating agent and the repair agent, respectively. We reduced the ratio of ethanol to water by adjusting the pH of the organosilane condensation and also achieved room-temperature curing by extending the curing time. Electrochemical and chemical leaching experiments results showed that the most appropriate addition of Ce (dbp)(3) was 0.2 wt% for enhancing the passivation performance of the passivated coating. In a 6-month chemical leaching experiment, the PS/Ce (dbp)(3)-0.2 passivation coating cured at room temperature showed a better passivation effect and maintained 90.55% and 78.54% of total Fe and SO42- passivation efficiencies. The passivation and self-healing mechanisms were investigated by FT-IR, XPS, Si-29 NMR, and other characterization methods, which were as follows: silane formed a cross-linked mesh structure by Si-O-Si bonding, in which Ce (dbp)(3) was physically filled. And the Si-OH on the surface of the passivation film formed Fe-O-Si bonds with the hydroxyl groups on the surface of the pyrite, thus attaching to the surface of the pyrite and isolating the oxidation medium. When the passivation coating was locally damaged, the oxidation reaction caused a change in pH, which accelerated the dissolution of Ce (dbp)(3) in the passivation layer. Ce3+ underwent a valence change and formed a CeO2 precipitate, while dbp(-) could form a complex with Fe2+ on the pyrite surface, both of which worked together to repair the broken passivation coating and prevent the oxidation reaction.

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