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Ferrocene-based 2D metal–organic framework nanosheet for highly efficient photocatalytic seawater uranium recovery

Journal 2024 · IF 13.3 · 发表于 2024 年 8 月 28 日
作者: Shilei Zhao,Tiantian Feng,Meng Cao,Tao Liu,Yihui Yuan,Ning Wang
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摘要

Sustainable uranium supply is critical for the long-term development of nuclear energy. The photocatalytic reduction of soluble hexavalent uranium to insoluble tetravalent uranium using photocatalysts has been recognized as a highly promising method for uranium recovery. However, existing photocatalysts face limitations such as restricted visible-light absorption and poor charge transfer capability, which hinder their photocatalytic uranium recovery performance. In this work, 1,1′-ferrocene dicarboxylic acid (FcDA) was introduced to synthesize the photocatalyst Zr-Fc-MOF 3 . The incorporation of FcDA broadened the visible light absorption range and reduced the band gap of Zr-Fc-MOF 3 , thereby enhancing electron-hole pair separation and carrier transport efficiencies. Moreover, the two-dimensional (2D) nanosheet structure of Zr-Fc-MOF 3 provided a large surface area, allowing full exposure of active sites. Additionally, Fe(II) in FcDA generated photoelectrons upon light excitation to facilitate uranium reduction, and the recyclable redox behavior of Fe(II) conferred high reusability of the photocatalyst. Consequently, Zr-Fc-MOF 3 demonstrated a high photocatalytic uranium recovery capacity of 8.29 mg g −1 over 10 days in natural seawater (NSW), with a uranium recovery rate of 0.829 mg g −1 d −1 , surpassing most other photocatalysts applied in NSW. These findings suggest that designing 2D nanosheet materials with ligands capable of efficient photoelectron generation is a promising approach for developing high-performance uranium recovery photocatalysts.

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