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[Display omitted] • MOFs act as dual-functional adsorbents and electrocatalysts for the removal of PPCPs. • Real active sites of MOFs are pinpointed using in-situ electrochemical methods. • Fe-MOFs exhibit high efficacy and stability in practical wastewater treatment. Pharmaceuticals and personal care products (PPCPs) pose a significant wastewater pollution concern. While electrochemical oxidation is promising, it struggles with slow mass transfer. To address this, we propose a novel strategy utilizing bifunctional metal–organic frameworks (MOFs) that couple an adsorbent with an electrocatalyst. The real active sites within iron-based MOFs responsible for the adsorption of PPCPs are MIL-101(Fe) molecules, while the in-situ formed active sites, α -FeOOH, accelerate the charge transfer under bias, contributing to the electrooxidation of PPCPs. The rapid destruction of adsorbed organics on the dual-functional electrode surface enables to release adsorption sites. This, in turn, paves the way for fast and efficient re-adsorption of PPCPs molecules, consequently promoting mass transfer. Iron-based MOFs exhibit excellent adsorption capacity (∼60 mg g−1 for sulfosalicylic acid, ∼15 mg g−1 for acetaminophen) and electrooxidation ability (94 % removal in 2 h, 31.2 kWh kg−1 COD) with good stability in realistic pharmaceutical wastewater treatment. This study offers a novel strategy for removing PPCPs using molecular electrocatalysts and provides new insights for designing and constructing MOFs for refractory wastewater treatment. [ABSTRACT FROM AUTHOR]

[Display omitted] • Adjustment of structure and interface of MFOC through soft-template is successful. • SMFO-B can achieve high removal rate and efficacy of Sb(V) and strong stability. • Direct tools with EXAFS and CD-MUSIC model showed specific inner-sphere complex. • E2 complex played the most important role in the Sb(V) adsorption onto SMFO-B. To achieve high removal rate and efficacy of Sb(V) from textile wastewater and simultaneously realize cyclic Sb(V) recovery, the structure and surface property of amorphous Mn-doped Fe oxide composite (MFOC) were regulated via the combination of facile soft-template synthesis and sintering treatment. Characterization and adsorption results indicated MFOC structure was greatly changed from aggregated large sphere to dispersive small sphere after adjusted by the optimal Brij-58 (SMFO-B). Because of the generated fasciculate micelle, long carbon chain feature and the lowest residual amount of Brij-58, abundant mesopores were generated and the aggregation of unit particles was apparently decreased for SMFO-B. Surface area and total pore volume of SMFO-B became 10 and 6 times of MFOC and more functional hydroxyl groups were generated and exposed on the interface between SMFO-B and water solution. Additionally, the surface positive potential of SMFO-B under neutral condition was also greatly increased. Thus, the maximum adsorption capacity and rate of SMFO-B towards Sb(V) reached to 147 mg/g and 0.1067 mg/(g·min), 2 and 5 times of MFOC. SMFO-B also possessed better selective adsorption ability, exhibited stronger static and dynamic adsorption performance in real textile wastewater and realized the cyclic desorption and enrichment of Sb(V) due to its better phase stability. X-ray absorption spectroscopy showed two main specific forms, such as bidentate edge-(E2) and corner-sharing (C2) complexes, for the inner-sphere complexation during Sb(V) adsorption and E2 complex was proved to play the most important role through the analysis of CD-MUSIC model. This study supplied an excellent adsorbent for Sb(V) removal from textile wastewater and a deeper insight about Sb(V) adsorption onto amorphous Fe oxide. [ABSTRACT FROM AUTHOR]