Synergistic coacervation–micelle extraction enables rapid and efficient removal of ultrahigh–concentration organic dyes from wastewater

Industrial dye effluents containing ultrahigh concentrations of organic pollutants pose serious environmental threats due to their strong coloration, toxicity, and persistence. Conventional adsorbents and functional materials often require complex synthesis and exhibit limited removal efficiency at high pollutant loadings. In this work, a facile, rapid, efficient, and regenerable coacervation-based extraction strategy has been developed for removing ultrahigh-concentration organic dyes from wastewater. Liquid–liquid phase separation between silicotungstic acid (SiW, H 4 [Si(W 3 O 10 ) 4 ]) and poly(ethylene glycol)- block -poly(propylene glycol)- block -poly(ethylene glycol) (Pluronic P123) micelles enables instantaneous sequestration of methylene blue (MB) at concentrations up to 19,500 mg L −1 , achieving 99.92% removal within 5 min and rendering the treated water colorless. Mechanistic analyses reveal that hydrogen-bonding-driven coacervation, hydrophobic encapsulation within P123 micelles, and electrostatic attraction between cationic dyes and anionic SiW clusters synergistically govern extraction performance. The process is also effective for organic dyes of different charge types, removing rhodamine B (99.91%), methyl orange (69.92%), and bromothymol blue (56.80%). The dense dye-loaded coacervates can be regenerated through Fenton oxidation, maintaining >99% efficiency after reuse. Notably, the coacervates exhibit strong underwater adhesion, enabling simple collection and offering potential reuse as underwater coatings. This work demonstrates a fast, scalable, and energy-efficient separation method for concentrated dye wastewater and highlights coacervation–micelle coupling as a promising platform for treating ionic pollutants and for high-loading encapsulation of hydrophobic compounds. • Coacervation–micelle synergy enables highly efficient dye removal. • Synergistic extraction effectively removes a broad range of organic dyes. • Dye-loaded coacervates exhibit strong underwater adhesion for easy collection. • Cyclic regeneration achieves >99% reuse efficiency with minimal loss. • Multiple molecular interactions synergize to enhance extraction performance.