Defect-induced in situ electron-metal-support interactions on MOFs accelerating Fe(Ⅲ)reduction for high-efficiency Fenton reactions
The inefficient reduction of Fe3+and activation of H2O2 in the Fenton reaction severely limit its ap-plication in practical water treatment.In this study,we developed defective NH2-UiO-66(d-NU)with coordinated unsaturated metal sites by adjusting the coordination configuration of Zr,creating a solid-liquid interface to facilitate Fe3+reduction and the sustainable generation of·OH from H2O2 activation.The d-NU/Fe3+/H2O2/Vis system demonstrated highly efficient removal of various or-ganic pollutants,with a rapid Fe2+regeneration rate and exceptional stability over ten cycles.The degradation rate constant of d-NU(0.16112 min-1)was 11 times higher than that of NH2-UiO-66(NU)(0.01466 min-1)without defects.Characterization combined with density functional calcula-tions revealed that defects induced coordination unsaturation of the Zr sites,leading to in situ elec-tron-metal-support interactions between Fe3+and the support via Zr-O-Fe bridges.This accumula-tion of electrons from the unsaturated Zr sites enabled the adsorption of Fe3+at the solid-liquid interface,promoting the formation of Fe2+across a wide pH range with a reduced energy barrier.This study introduces a promising strategy for accelerating Fe3+reduction in the solid-liquid inter-facial Fenton process for the degradation of organic pollutants.
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