Targeted Recovery of Complexed Heavy Metal from Wastewater to Mixed‐Metal MOFs Electrocatalytic Membrane for Antibiotics Degradation: Tunable Radical and Non‐Radical Pathway

Abstract Complex heavy metals in industrial wastewater threaten global water safety, while their sustainable treatment and direct utilization from complex water matrices are still challenging. Herein, a decomplexation‐electroreduction‐targeted conversion coupling electrochemical strategy is developed to recover the complexed heavy metal and then in situ convert into a metal–organic frameworks (MOFs) electrocatalytic membrane (ECM) for enhanced antibiotics degradation. Ethylenediaminetetraacetic acid‐metal (Cu, Pb, Zn) is efficiently decomplexed (92‐97%) with high metal recovery (87‐99%), and metal‐trimesic acid (BTC) MOFs are well grown on the substrate. The multi‐metal active sites in CuPbZn‐BTC endowed ECM with abundant oxygen vacancy, Lewis acid sites, fast electron transfer and suppressed oxygen evolution reaction, which presented much superior antibiotics removal (92‐99%) than monometallic MOFs ECM; moreover, radical (•OH, •O 2 − and SO 4 •− ) and non‐radical ( 1 O 2 ) pathways are precisely adjusted by modulating metal ratios under electricity without the addition of chemicals (H 2 O 2 or persulfate) and the mechanism is due to the activation of reactive oxygen species (ROS) precursors (O 2 , H 2 O and SO 4 2− ) as revealed by in situ Raman spectra and ROS identification. The potential application is demonstrated by the recovery of heavy metals from simulated electroplating wastewater into mixed‐metal MOFs ECM that presented efficient and stable antibiotics degradation for surface water remediation.