Developing a molecularly imprinted channels catalyst based on template effect for targeted removal of organic micropollutants from wastewaters

• 3D-MICs catalyst coupled with specific adsorption and targeted degradation was developed. • 3D-MICs catalyst exhibited excellent selectivity for targeted OMPs in a complex water environment. • 3D-MICs catalyst plays the functions of template effect, size-exclusion effect, and spatial confinement. • The enhanced removal efficiency of SMX by MIC-#/PS system in the actual water environment. • The In-situ method and DFT calculation were used to reveal the mechanism of targeted adsorption and degradation. In this study, a novel catalyst with three-dimensional molecularly imprinted channels (3D-MICs) was proposed to preferentially remove the noxious organic micropollutants (OMPs) from wastewaters. The 3D-MICs catalysts exhibited robust selectivity (the imprinting factor reached above 2.04) and larger adsorption capacity (enhanced over 2.7 times), which was benefited from the synergy of template effect and size-exclusion effect. Compared with the original MOF-#/ persulfate (PS) system (40%), the SMX removal by MIC-#/PS system still retained over 91% in simulated wastewater, tap water, and polluted river water, respectively. With the spatial confinement, the degradation products by the MIC-#/PS system showed less quantity (4.6-fold) and lower toxicity than that by the original MOF-#/PS system. In-situ ATR-FTIR analysis and density functional theory (DFT) calculation revealed that the specific adsorption property for the targeted OMPs was mainly realized by the shape of the imprinted cavity, hydrogen bonds, hydrophobic-hydrophobic interaction, π-π stacking, and electrostatic interactions. Finally, the radical and non-radical pathways are involved in the MIC-#/PS system to ensure the high-efficiency removal of SMX. These insights revealed here could pave the way for wastewater treatment.