N, P, and S Codoped Graphene‐Like Carbon Nanosheets for Ultrafast Uranium (VI) Capture with High Capacity,Advanced Science

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N, P, and S Codoped Graphene‐Like Carbon Nanosheets for Ultrafast Uranium (VI) Capture with High Capacity
Advanced Science ( IF 14.3 ) Pub Date : 2018-08-27 , DOI: 10.1002/advs.201800235
Zhe Chen ₁ , Wanying Chen ₁ , Dashuang Jia ₁ , Yang Liu ₁ , Anrui Zhang ₁ , Tao Wen ₁ , Jian Liu ₂ , Yuejie Ai ₁ , Weiguo Song ₂ , Xiangke Wang ₁

Affiliation

The development of functional materials for the highly efficient capture of radionuclides, such as uranium from nuclear waste solutions, is an important and challenging topic. Here, few‐layered N, P, and S codoped graphene‐like carbon nanosheets (NPS‐GLCs) that are fabricated in the 2D confined spacing of silicate RUB‐15 and applied as sorbents to remove U(VI)ions from aqueous solutions are presented. The NPS‐GLCs exhibit a large capacity, wide pH suitability, an ultrafast removal rate, stability at high ionic strengths, and excellent selectivity for U(VI) as compared to multiple competing metal ions. The 2D ultrathin structure of NPS‐GLCs with large spacing of 1 nm not only assures the rapid mass diffusion, but also exposes a sufficient active site for the adsorption. Strong covalent bonds such as POU and SOU are generated between the heteroatom (N, P, S) with UO₂ ²⁺ according to X‐ray photoelectron spectroscopy analysis and density functional theory theoretical calculations. This work highlights the interaction mechanism of low oxidation state heteroatoms with UO₂ ²⁺, thereby shedding light on the material design of uranium immobilization in the pollution cleanup of radionuclides.

中文翻译：

N、P、S 共掺杂类石墨烯碳纳米片用于高容量超快铀 (VI) 捕获

开发用于高效捕获放射性核素（例如从核废料溶液中提取铀）的功能材料是一个重要且具有挑战性的课题。在这里，在硅酸盐 RUB-15 的二维受限间距中制造了多层 N、P 和 S 共掺杂石墨烯类碳纳米片 (NPS-GLC)，并用作吸附剂从水溶液中去除 U(VI) 离子提出。与多种竞争金属离子相比，NPS-GLC 表现出大容量、广泛的 pH 适应性、超快的去除速率、高离子强度下的稳定性以及对 U(VI) 的优异选择性。 NPS-GLC 具有 1 nm 大间距的二维超薄结构不仅保证了快速的质量扩散，而且还暴露了足够的吸附活性位点。根据X射线光电子能谱分析和密度泛函理论计算，杂原子（N、P、S）与UO ₂ ²⁺之间生成P  O  U、S  O  U 等强共价键。该工作突出了低氧化态杂原子与UO ₂ ²⁺的相互作用机制，从而为放射性核素污染净化中铀固定化的材料设计提供了线索。

更新日期：2018-08-27

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