Construction of a Hierarchical Core–Shell Z-Scheme Two-Dimensioanl/Two-Dimensional ZnIn₂S₄@TpBpy Heterostructure for Photocatalytic Reduction of U(VI)

Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 6, 2025

The essential nature of the photocatalytic process is charge transfer. To optimize spatial separation photogenerated electron–hole (e–-h+) pairs for high-performance catalytic efficiency, in this work, we have successfully prepared hierarchical core–shell two-dimensional (2D)/2D ZnIn2S4@TpBpy (ZIS@TpBpy) with well-matched Z-scheme interfacial transfer channels uranium (U(VI)) photoreduction. electron configuration was confirmed by internal electric field (IEF) formation analysis, XPS characterization, and DMPO spin-trapping EPR spectroscopy. With large specific surface area abundant active sites, ZIS@TpBpy composite achieved a U(VI) extraction rate 94.08%. In addition, removal constant (0.0137 min–1) 2.05 4.28 times higher than those TpBpy (0.0067 ZnIn2S4 (0.0032 min–1), respectively. First, combination organic inorganic components expanded range visible light absorption utilization. Afterward, under visible-light irradiation, more e–-h+ dissociated migrated to driven IEF heterostructure. Simultaneously, synergistic effect between polarization potential generated sites (N O atoms) framework further accelerated depletion translocation pairs, which significantly improved efficiency reduction U(VI).

Language: Английский

Selective Crystallization Separation of Uranium(VI) Complexes from Lanthanides

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 64(1), P. 202 - 212

Published: Dec. 30, 2024

The limited availability of uranium (U) resources poses significant challenges to the advancement nuclear energy. Recycling from spent fuel is critical, but coexistence lanthanides (Ln) complicates extraction process significantly. Here, we present an N/O ligand, (E)-N′-(pyridin-2-ylmethylene) picolinohydrazide (PYPH), designed for selective recovery U(VI) over Ln(III/IV) in acidic environments. 3,6-Bis(2-pyridinyl)-1,2,4,5-tetrazine (BPTZ) and N,N-dimethylformamide (DMF), when subjected heat, gradually generate PYPH formic acid aqueous solution; this can be employed recovery. This approach, known as situ reactive technique, enhances capture capacity, selectivity, resistance while effectively mitigating interference Ce(IV). At pH 3 0.1 M HNO3, separation factors binary systems exceeded 103 102, respectively, achieving purities exceeding 99%. Monocrystalline structure analysis revealed two-dimensional planar coordination complexes, demonstrating their exceptional selectivity. study underscores potential proposes new avenues developing innovative strategies actinides (An) using structural theoretical modeling.

Language: Английский

Ultrafast Photoassisted Capture of Uranium over Cu₂O/CuO Heterojunction Enabled by Rapid Interfacial Electron Transfer

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 7(1), P. 295 - 303

Published: Dec. 19, 2024

Photoassisted capture of uranium provides a promising strategy for the sustainable utilization nuclear energy. Herein, we constructed Cu2O/CuO heterojunctions in situ by wet-etching method, showing ultrafast reaction kinetics and photocatalytic activity U(VI) reduction. In 8 ppm uranium-containing wastewater, exhibited remarkable extraction efficiency 94.6% within 10 min under irradiation, which exceeded most recently reported photocatalysts. The rate constant was 5.8-time larger than that pure Cu2O. A mechanism study indicated photogenerated electrons reduced CuO species created oxygen vacancy during photocatalysis process, strengthened binding UO22+. rapid electron transfer over heterojunction interfaces enhanced UO22+ strength formed accounted kinetics.

Language: Английский