氮化碳异质结用于光催化还原U(Ⅵ)的研究进展

    Carbonitride Heterojunctions for Photocatalytic Reduction of Uranium(Ⅵ)

    • 摘要: 对核工业产生的含铀废水进行铀污染处理和铀资源回收,有利于维护核能的可持续发展。光催化还原技术友好地协同了吸附-还原能力,克服了单一吸附去除的热力学限制,用于核废水中铀去除与回收具有较大的发展潜力。氮化碳基纳米材料因其优异的光化学性能、出色的理化可调性和良好的化学稳定性而被认为是一类光催化U(Ⅵ)还原的理想光催化剂。近年来围绕氮化碳进行的改性和应用研究为光催化铀还原提供了深入见解。近期的研究揭示了基于C3N4的异质结纳米结构的构筑及其对铀的光催化还原过程和机制。本文旨在阐明这一快速发展的主题,立足于光催化还原U(Ⅵ)的机理,着眼于有效改善C3N4的光催化性能,系统总结了基于C3N4异质结光催化材料的设计开发及其在U(Ⅵ)还原中的应用。最后,展望了当前基于C3N4的光催化材料在含铀废水中对U(Ⅵ)的还原去除面临的困难,为未来的突破提供视角和方向。

       

      Abstract: The development and application of nuclear energy is often considered as a potential solution to meet the increasing energy demand. However, it is important to acknowledge that the utilization of nuclear energy resources and the treatment of nuclear waste pollution pose significant challenges that require careful consideration and management. Therefore, it is crucial to address the challenges of uranium pollution treatment and uranium resource recovery to ensure the sustainable development of nuclear energy. The technology of photocatalytic reduction has been found to have a synergistic adsorption reduction ability, which allows it to overcome the thermodynamic limitations of single adsorption removal. As a result, photocatalytic reduction technology is widely recognized as having great potential in the removal and recycling of uranium in nuclear waste liquid. One of the key factors for the effective application of this technology is the acquisition of a catalyst with high photocatalytic reduction ability. Nitride carbon materials are considered an ideal photocatalyst for photocatalytic reduction of U(Ⅵ) due to their excellent photochemical properties, excellent physicochemical adjustability, and good chemical stability. However, the pure g-C3N4 photocatalyst still suffers from its low separation efficiency of photogenerated charge carriers, which results in unsatisfactory photocatalytic activity. In recent years, research on modifying and applying carbon nitride has provided in-depth insights into the reduction of uranium through photocatalysis. Discussing the strategy of modifying C3N4, constructing heterojunction nanostructures, and utilizing them for the photocatalytic reduction of uranium, along with the mechanisms involved. This review summarizes the recent significant progress on the design of g-C3N4-based heterostructure photocatalysts and their special separation/transfer mechanisms of photogenerated charge carriers. On the one hand, according to the key steps of photocatalytic uranium reduction, modification strategies using g-C3N4 photocatalysts can be classified into the following groups: morphology modification, band-structure regulation, and heterostructure construction. Moreover, according to the different transfer mechanisms of photogenerated charge carriers between g-C3N4 and the coupled components, the g-C3N4-based heterostructure photocatalysts can be divided into the following categories: g-C3N4-based conventional Type-Ⅱ heterojunction, g-C3N4-based Z-scheme heterojunction, g-C3N4-based S-scheme heterojunction, and g-C3N4/metal heterostructure. We also focused on the structure-activity relationship between the modification of photocatalytic materials based on carbon nitride and their photocatalytic reduction performance for U(Ⅵ), as well as the mechanism of their catalytic reduction removal. Finally, this section offers concluding remarks and prospects for exploring the challenges and opportunities faced by advanced carbon nitride-based photocatalytic materials in the removal of uranium pollution and the recovery of uranium resources. It also provides directions for future breakthroughs.

       

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