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天然竹条表面偕胺肟基和氨基的分子级铀特异性“纳米孔”的共构建用于从海水中特异性捕获铀。

Co-construction of molecular-level uranyl-specific "nano-holes" with amidoxime and amino groups on natural bamboo strips for specifically capturing uranium from seawater.

机构信息

Key Laboratory of Superlight Materials and Surface Technology, Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China.

Key Laboratory of Superlight Materials and Surface Technology, Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China.

出版信息

J Hazard Mater. 2022 Sep 5;437:129407. doi: 10.1016/j.jhazmat.2022.129407. Epub 2022 Jun 17.

Abstract

Efficiently capturing of uranium (VI) [U(VI)] from seawater elicits unparalleled attraction for sustaining the uplifted requirement for nuclear fuel. However, obtaining the abundant U(VI) resource from seawater has always seriously restricted by competitive adsorption from higher concentrations of competitors, especially vanadium (V) [V(V)]. Herein, based on amidoximized natural bamboo strips with hierarchical porous structure, the molecular-level uranyl-specific "nano-holes" was co-constructed by the intramolecular hydrogen bonds for specifically trapping U(VI) from seawater. Manipulating the branched degrees of amino groups enabled the creation of a series of the molecular-level uranyl-specific "nano-holes" that exhibit ultrahigh affinity and selective adsorption of U(VI) with a adsorption capacity 1.8 fold higher compared to that of V(V) after 30 days floating in the Yellow Sea basin, conquering the long-term challenge of the competitive adsorption of V(V) for amidoxime-based adsorbents applied to extract U(VI) from seawater. The diameter of the molecular-level uranyl-specific "nano-holes" is approximately 12.07 Å, significantly larger than (UO)(OH) (10.37 Å) and smaller than HVO, thereby exhibiting specifically trapping of U(VI) in a series of adsorption experiments with different U(VI)-V(V) ratios. Besides, the adsorption model based on the combination of experimental and theoretical results is accompanied by "hydrogen bond breaking and coordination bond formation".

摘要

从海水中高效捕获铀(VI) [U(VI)] 引起了人们的极大关注,因为这对于维持对核燃料的高需求至关重要。然而,从海水中获取丰富的 U(VI)资源一直受到来自高浓度竞争物,特别是钒(V) [V(V)] 的竞争吸附的严重限制。在此,基于具有分级多孔结构的偕胺肟化天然竹条,通过分子内氢键共同构建了用于从海水中特异性捕获 U(VI)的铀酰特异性“纳米孔”。通过操纵支化度的氨基,可以创建一系列铀酰特异性的“纳米孔”,这些“纳米孔”对 U(VI)表现出超高的亲和力和选择性吸附,在黄海盆地漂浮 30 天后,其对 U(VI)的吸附容量比 V(V)高 1.8 倍,克服了长期以来用于从海水中提取 U(VI)的偕胺肟基吸附剂的 V(V)竞争吸附的挑战。分子级铀酰特异性“纳米孔”的直径约为 12.07 Å,明显大于(UO)(OH) (10.37 Å),小于 HVO,因此在一系列不同 U(VI)-V(V)比例的吸附实验中表现出对 U(VI)的特异性捕获。此外,基于实验和理论结果的组合的吸附模型伴随着“氢键断裂和配位键形成”。

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