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水合氧化锆材料上的阴离子交换:用于选择性去除碘酸盐的应用。

Anion exchange on hydrous zirconium oxide materials: application for selective iodate removal.

作者信息

Suorsa Valtteri, Otaki Miho, Suominen Topi, Virkanen Juhani, Reijola Hanna, Bes René, Koivula Risto

机构信息

Radiochemistry Unit, Department of Chemistry, University of Helsinki A.I. Virtasen aukio 1 00014 Helsinki Finland

Department of Geosciences and Geography, University of Helsinki Gustaf Hällströmin katu 2 00014 Helsinki Finland.

出版信息

RSC Adv. 2023 Jan 4;13(2):948-962. doi: 10.1039/d2ra06489h. eCollection 2023 Jan 3.

Abstract

The radioactive I is a top-priority radionuclide due to its the long half-life (1.57 × 10 years) and high mobility. Because of the planned and accidental releases to the environment, specific separation technologies are required to limit the potential radiation dose to human beings. Zirconium oxides are known for their adsorption capability and selectivity to oxyanions and here the applicability to selective IO removal has been investigated regarding the uptake mechanism, regeneration and competition caused by other anions, like environmentally relevant SO . Granular aggregates of hydrous zirconium oxides with and without Sb doping showed high potential for the selective IO removal in the presence of competing anions, like the forementioned SO (apparent capacity between 0.1-0.4 meq g depending on SO concentration). The main uptake mechanism was found to be outer-sphere complexation (ion-exchange) to the protonated hydroxyl groups of hydrous zirconium oxides, but also minor mechanisms were identified including inner-sphere complexation and reduction to I. The materials were observed to be easily and successively regenerated using dilute acid. Hydrous zirconium oxides showed high potential for IO removal from waste solutions regarding technical (high selectivity and apparent capacity) and ecological/economic (feasible regeneration) aspects.

摘要

放射性碘是一种优先级很高的放射性核素,因为其半衰期长(1.57×10年)且迁移性高。由于计划性和意外性的向环境释放,需要特定的分离技术来限制对人类的潜在辐射剂量。氧化锆以其对含氧阴离子的吸附能力和选择性而闻名,在此,针对其对碘酸根的选择性去除,研究了其摄取机制、再生以及由其他阴离子(如环境相关的硫酸根)引起的竞争。含锑和不含锑掺杂的水合氧化锆颗粒聚集体在存在竞争阴离子(如上述硫酸根)的情况下,对碘酸根的选择性去除显示出高潜力(根据硫酸根浓度,表观容量在0.1 - 0.4 meq/g之间)。发现主要摄取机制是与水合氧化锆的质子化羟基发生外层络合(离子交换),但也确定了次要机制,包括内层络合和将碘酸根还原为碘离子。观察到这些材料使用稀酸可轻松且连续地再生。从技术(高选择性和表观容量)以及生态/经济(可行的再生)方面来看,水合氧化锆从废液中去除碘酸根具有很高潜力。

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