Efficient Strategy for U(VI) Photoreduction: Simultaneous Construction of U(VI) Confinement Sites and Water Oxidation Sites

ACS Appl Mater Interfaces. 2023 Jan 11;15(1):1063-1072. doi: 10.1021/acsami.2c17849. Epub 2022 Dec 21.

Abstract

Reduction of hexavalent uranium [U(VI)] by the photocatalytic method opens up a novel way to promote the selectivity, kinetics, and capacity during uranium removal, where organic molecules act as the sacrificial agents. However, the addition of sacrificial agents can cause a secondary environmental pollution and increase the cost. Here, a UiO-66-based photocatalyst (denoted as MnOx/NH2-UiO-66) simultaneously with efficient U(VI) confinement sites and water oxidation sites was successfully developed, achieving excellent U(VI) removal without sacrificial agents. In MnOx/NH2-UiO-66, the amino groups served as efficient U(VI) confinement sites and further decreased the U(VI) reduction potential. Besides, MnOx nanoparticles separated the photogenerated electron-hole pairs and provided water oxidation sites. The U(VI) confinement sites and water oxidation sites jointly promoted the U(VI) photoreduction performance of MnOx/NH2-UiO-66, resulting in the removal ratio of MnOx/NH2-UiO-66 for U(VI) achieving 97.8% in 2 h without hole sacrifice agents. This work not only provides an effective UiO-66-based photocatalyst but also offers a strategy for effective U(VI) photoreduction.

Keywords: U(VI) confinement sites; U(VI) photoreduction; UiO-66; carrier separation efficiency; water oxidation cocatalysts.