Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, 64# Mianshan Road, Mianyang, 621900, Sichuan Province, P. R. China.
Dalton Trans. 2019 Mar 14;48(10):3284-3290. doi: 10.1039/c9dt00434c. Epub 2019 Feb 18.
Efficient and irreversible capture of radioactive nuclides is an important environmental protection task when disposing of nuclear wastewater. This paper uses an "ion trapping" concept to design an efficient adsorbent based on a metal-organic framework (MOF), for removal of radioactive strontium from nuclear wastewater. Two functionalized MOFs were achieved by the introduction of sulfate or oxalate into the pore structure of MOF-808, giving MOF-808-SO and MOF-808-CO, respectively. These functionalized MOF-808 materials exhibit excellent ability to remove Sr from acidic solution due to their particular trapping action, with the maximum Sr adsorption capacities of 176.56 mg g and 206.34 mg g for MOF-808-SO and MOF-808-CO, respectively, surpassing most other inorganic materials. Additionally, 99% of Sr is removed by MOF-808-SO and MOF-808-CO after reaching the equilibrium. Remarkably, these two functionalized MOF-808 materials exhibited selectivity for the removal of Sr from simulated mixed nuclear wastewater, even when there are 10 times as many co-existing ions as Sr ions, demonstrating that anchoring of the trapping groups is a good way to improve Sr adsorption capacity on MOFs. Moreover, both functionalized MOF-808 materials trap Sr ions irreversibly, suggesting these trapping groups have strong ability to bind with Sr. A mechanism study indicated no proton ion exchange occurred during the adsorption process, so the functionalized groups anchored to MOFs play an important role in Sr adsorption. Our present study provides an efficient way to design new adsorbents for the removal of radioactive strontium and other radionuclides from nuclear wastewater.
高效且不可逆地捕获放射性核素是处理核废水时的一项重要环境保护任务。本文利用“离子捕集”概念,设计了一种基于金属-有机骨架(MOF)的高效吸附剂,用于从核废水中去除放射性锶。通过在 MOF-808 的孔结构中引入硫酸盐或草酸盐,得到了两种功能化的 MOF-808,分别为 MOF-808-SO 和 MOF-808-CO。由于其特殊的捕集作用,这些功能化的 MOF-808 材料表现出了从酸性溶液中去除 Sr 的优异能力,MOF-808-SO 和 MOF-808-CO 的最大 Sr 吸附容量分别为 176.56 mg/g 和 206.34 mg/g,超过了大多数其他无机材料。此外,MOF-808-SO 和 MOF-808-CO 在达到平衡后可去除 99%的 Sr。值得注意的是,即使存在 10 倍于 Sr 离子的共存离子,这两种功能化的 MOF-808 材料仍表现出对模拟混合核废水中 Sr 的选择性去除,这表明捕集基团的锚定是提高 MOF 上 Sr 吸附能力的一种有效方法。此外,两种功能化的 MOF-808 材料对 Sr 离子的捕获都是不可逆的,这表明这些捕集基团与 Sr 具有很强的结合能力。机理研究表明,在吸附过程中没有质子离子交换,因此锚定在 MOFs 上的功能化基团在 Sr 吸附中起着重要作用。本研究为设计从核废水中去除放射性锶和其他放射性核素的新型吸附剂提供了一种有效方法。