Enhanced Separation Performance of Radioactive Cesium and Cobalt in Graphene Oxide Membrane via Cationic Control

The great applications of nuclear power for the most promising clean energy sources have been challenged by a large amount of radioactive wastewater generated, specifically the Cs⁺/Co²⁺ separation for nuclear waste storage, retreatment or recycling of radioactive wastewater, because of their wide difference in half-life and high heat release. In this work, graphene oxide membranes (GOMs) with interlayer spacing controlled by cations were used to separate mixed Cs⁺/Co²⁺ ions. The separation factors of Cs⁺/Co²⁺ for K⁺-controlled graphene oxide membranes (K-GOMs) was 2∼3 times higher than that of GOMs without treatment. In addition, the separation factors of Cs⁺/Co²⁺ for K-GOMs can be further enhanced with the increase of membranes thickness and change the initial ratios of the two ions. Typically, the separation factors of K-GOMs with a thickness of ∼300 nm reached up to 73.7 ± 3.9. Moreover, the K-GOM showed outstanding stability of the separation performance under long-term operation within 7 days. First-principles calculation revealed that the enhanced ionic selectivity of controlled GOM is induced by the difference of adsorption energies between the hydrated cations and aromatic rings, resulting in a significant increase in the mobility differences between Cs⁺ and Co²⁺ through a fixed narrow interlayer spacing. This study demonstrated excellent separation performances of GO-based membranes based on their size-exclusion effect rather than electrostatic repulsion effect, and we believe this work can enable potential efficient treatment technologies for radioactive wastewater needed urgently.