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The development of a dual Z-scheme photocatalytic system with stable and strong redox capability is essential for uranium recovery from nuclear wastewater and oceanic environments. Guided by density functional theory (DFT) calculations, an aerogel-like dual Z-scheme TiO2/graphitic carbon nitride (g-C3N4)/SnS2 (TCS) heterojunction photocatalyst is rationally designed for visible-light-driven uranium extraction. The TCS system achieves an exceptional uranium extraction efficiency of 99.1% within 120 min without the use of any sacrificial agents, which can be attributed to its aerogel architecture that offers a large specific surface area (211.7 m2/g) and abundant accessible active sites. Moreover, the presence of two synergistic Z-scheme electron transfer pathways significantly promotes the separation and migration of photogenerated charge carriers. Notably, the valence bands of both TiO2 and SnS2 enable hydroxyl radical (·OH) generation, constructing a double-oxidized dual Z-scheme heterojunction that facilitates enhanced H2O2 production and thereby accelerates uranium extraction. Based on these findings, a comprehensive photocatalytic uranium extraction pathway and reaction mechanism are proposed, elucidating the roles of active species and the nature of the final extraction products.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).
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