Uranium extraction by a graphene-based asymmetric electrode configuration through combined complexation, electro-adsorption, and photocatalytic reduction

Recently, capacitive deionization has become a promising approach for uranium extraction owing to its energy-efficiency and environmental benign. However, the adsorbed charged uranium (VI) (U(VI)) would repulse the incoming U(VI) ions, and might re-enter into solution, vastly impeding the improvement of electro-adsorption performance. Reducing the adsorbed U(VI) ions into U(IV) precipitation is an ideal way to address above issues. Here, a coupling approach of photocatalytic reduction and electro-adsorption (PEA) was proposed. An asymmetric electrode configuration, composed of phosphate functionalized graphene (GP) cathode and graphene/TiO2 nanocomposite (GT) anode was rationally designed, and originally proved its enhanced U(VI) extraction via the PEA method. The asymmetric electrode device enables the fast transport of photo-electron and the rapidly directed migration of U(VI) ion to the GP cathode. More importantly, it combines three synthetic mechanisms of complexation, electro-adsorption, and photocatalytic reduction to extract U(VI) ions. As a consequence, the as-designed PEA method shows a higher removal rate of 91.3% in comparison with conventional photocatalytic reduction (PA) and electro-adsorption (EA) methods. Meanwhile, its kinetics rate is 225% and 50% faster than PA and EA methods. Furthermore, an enhanced reduction efficiency of U(VI) to U(IV), good selectivity as well as reusability for PEA method were also obtained. The results provide a potential approach to combine multiple mechanisms for efficient U(VI) extraction from aqueous solution by purposeful design of asymmetric electrodes.