Biomimetic Photocatalytic System Designed by Spatially Separated Cocatalysts on Z‐scheme Heterojunction with Identified Charge‐transfer Processes for Boosting Removal of U(VI)

Abstract Designing highly efficient photocatalysts with rapid migration of photogenerated charges and surface reaction kinetics for the photocatalytic removal of uranium (U(VI)) from uranium mine wastewater remains a significant challenge. Inspired by natural photosynthesis, a biomimetic photocatalytic system is assembled by designing a novel hollow nanosphere MnO x @TiO 2 @CdS@Au (MTCA) with loading MnO x and Au nano particles (Au NPs) cocatalysts on the inner and outer surfaces of the TiO 2 @CdS. The spatially separated cocatalysts efficiently drive the photogenerated charges to migrate in opposite directions, while the Z‐scheme heterogeneous shell further separates the interfacial charges. Theoretical calculation identifies multiple consecutive forward charge transfers without charge recombination within MTCA. Thus, MTCA could efficiently remove 99.61% of U(VI) after 15 min of simulated sunlight irradiation within 3 mmol L −1 NaHCO 3 with 0.231 min −1 of the reduction rate constant, outperforming most previously reported photocatalysts. MTCA further significantly removes 91.83% of U(VI) from the natural uranium mining wastewater under sunlight irradiation. This study provides a novel approach to designing an ideal biomimetic photocatalyst for remediating environmental pollution.