Urchin-Like CO2-Responsive Magnetic Microspheres for Highly Efficient Organic Dye Removal

CO2-responsive materials have emerged as promising adsorbents for the remediation of refractory organic dyescontaminated wastewater without the formation of byproducts or causing secondary pollution. However, realizing the simultaneous adsorption-separation or complete removal of both anionic and cationic dyes, as well as achieving deeper insights into their adsorption mechanism, still remains a challenge for most reported CO2responsive materials. Herein, a novel type of urchin-like CO2-responsive Fe3O4 microspheres (U-Fe3O4 @P) has been successfully fabricated to enable ultrafast, selective, and reversible adsorption of anionic dyes by utilizing CO2 as a triggering gas. Meanwhile, the CO2-responsive U-Fe3O4 @P microspheres exhibit the capability to initiate Fenton degradation of non-adsorbable cationic dyes. Our findings reveal exceptionally rapid adsorption equilibrium, achieved within a mere 5 min, and an outstanding maximum adsorption capacity of 561.2 mg g-1 for anionic dye methyl orange upon CO2 stimulation. Moreover, 99.8% of cationic dye methylene blue can be effectively degraded through the Fenton reaction. Furthermore, the long-term unresolved interaction mechanism of organic dyes with CO2-responsive materials is deciphered through a comprehensive experimental and theoretical study by density functional theory. This work provides a novel paradigm and guidance for designing nextgeneration eco-friendly CO2-responsive materials for highly efficient purification of complex dye-contaminated wastewater in environmental engineering.