Synthesis of Uranium Single Atom from Radioactive Wastewater for Enhanced Water Dissociation and Hydrogen Evolution

Abstract

As a common nuclide in radioactive wastewater, uranium (U) is generally treated by landfill, which induces the massive abandonment of uranium resources. In this work, a pulse voltammetry method for the synthesis of U single atoms on MoS₂ (U/MoS₂ ) nanosheets from radioactive wastewater for the electrocatalytic alkaline hydrogen evolution reaction (HER) is reported. The mass loading of U single atoms is facilely controlled with high selectivity for coexisting ions in radioactive wastewater. In the electrolyte of 1 m of KOH, U/MoS₂ nanosheets with 5.2% of U single atoms exhibit relatively low overpotentials of 72 mV at 10 mA cm^-2 . The mechanistic study reveals that the HER on U/MoS₂ includes the water dissociation on U single atoms to form OH* and H transfer from OH* to adjacent S-edge atoms. This procedure exhibits decreased activation energy for transition state in water dissociation and optimized Gibbs free energy for H* adsorption.