Atomic H*-mediated electrochemical removal of low concentration antimonite and recovery of antimony from water

Compounds containing antimony (Sb) are broadly used as starting materials for a wide range of industrial products, leading to serious water pollution associated with Sb rock mining as well as Sb leaching. Herein, we proposed an innovative design of an electrified membrane consisted of bimetallic palladium and iron nanoparticles (Pd-Fe NPs) supported on conductive carbon nanotube (CNT) networks. The nanohybrid filter enabled effective generation and retainment of atomic hydrogen (H*) under an electric field, which further contributed to the complete electroreduction of antimonite (Sb(III)). The highest atomic H* yield and Sb(III) removal kinetics were identified once a potential of −1.0 V vs. Ag/AgCl was exerted. Compared to the pristine CNT, Pd-CNT and Fe-CNT filters, the reaction rate constant of the Pd/Fe-CNT filter was increased 5.15-, 2.39-, and 1.76-fold, respectively for electrochemical removal of Sb(III). The results denoted that the superior performance of the Pd/Fe-CNT nanohybrid filter originated from: (1) the flow-through design, which enhanced mass transport, (2) the bimetallic design, which increased the catalytic activity, and (3) the collective contribution from atomic H*-mediated indirect reduction and direct electron transfer reduction mechanisms. The robust system performance occurred over a broad range of pH values, a variety of water matrices and can withstand several cycles of experiments. Our findings highlight an effective electro-filtration strategy to induce atomic H*-mediated electrochemical removal and recovery of Sb from water.