Ni‐Single‐Atom Mediated 2D Heterostructures for Highly Efficient Uranyl Photoreduction

Abstract Sunlight‐driven photoreduction of the environmentally mobile uranyl (VI) to less soluble tetravalent uranium is of considerable value to environmental sustainability, yet the pursuit for high‐performance semiconductors is plagued by the current disadvantages of inferior charge separation/migration. This study reports that a nickel single atom isolated on a sulfur‐functionalized graphitic carbon nitride/reduced graphene oxide 2D heterostructure enables exceptional uranyl photoreduction. Under only 11 min of visible light irradiation, the single atom anchored semiconductor yields a high removal rate of 99.8% and a record‐high extraction capacity of 4144 mg g⁻¹ in uranyl‐containing wastewater and seawater. Theoretical calculations confirm that the remarkable uranyl photoreduction originates from the synergetic effect of Ni single atoms and intimate heterojunction establishment that can not only promote the separation/migration of photoexcited carriers, but also greatly reduce the energy barrier of uranyl reduction. This study showcases the exciting potential of single atom semiconductors for efficient uranyl removal from uranium‐contaminated aqueous environments.