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通过席夫碱化学合成富电子多孔有机聚合物以实现高效碘捕获。

Synthesis of Electron-Rich Porous Organic Polymers via Schiff-Base Chemistry for Efficient Iodine Capture.

机构信息

Key Laboratory of Ministry of Education for Advanced Materials in Tropical Island Resources, Department of Chemistry and Chemical Engineering, Hainan University, No 58, Renmin Avenue, Haikou 570228, China.

China Institute of Atomic Energy, Beijing 102413, China.

出版信息

Molecules. 2022 Aug 12;27(16):5161. doi: 10.3390/molecules27165161.

Abstract

As one of the main nuclear wastes generated in the process of nuclear fission, radioactive iodine has attracted worldwide attention due to its harm to public safety and environmental pollution. Therefore, it is of crucial importance to develop materials that can rapidly and efficiently capture radioactive iodine. Herein, we report the construction of three electron-rich porous organic polymers (POPs), denoted as POP-E, POP-T and POP-P via Schiff base polycondensations reactions between -symmetric adamantane knot and four-branched "linkage" molecules. We demonstrated that all the three POPs showed high iodine adsorption capability, among which the adsorption capacity of POP-T for iodine vapor reached up to 3.94 g·g and the removal rate of iodine in n-hexane solution was up to 99%. The efficient iodine capture mechanism of the POP-T was investigated through systematic comparison of Fourier transform infrared spectroscopy (FT-IR), Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) before and after iodine adsorption. The unique π-π conjugated system between imine bonds linked aromatic rings with iodine result in charge-transfer complexes, which explains the exceptional iodine capture capacity. Additionally, the introduction of heteroatoms into the framework would also enhance the iodine adsorption capability of POPs. Good retention behavior and recycling capacity were also observed for the POPs.

摘要

作为核裂变过程中产生的主要核废料之一,放射性碘因其对公共安全和环境污染的危害而引起了全球关注。因此,开发能够快速高效捕获放射性碘的材料至关重要。在此,我们通过 - 对称金刚烷结和四叉“连接”分子之间的席夫碱缩合反应,构建了三种富电子多孔有机聚合物(POP),分别表示为 POP-E、POP-T 和 POP-P。我们证明,所有三种 POP 都表现出高碘吸附能力,其中 POP-T 对碘蒸气的吸附容量高达 3.94 g·g,正己烷溶液中碘的去除率高达 99%。通过系统比较吸附前后的傅里叶变换红外光谱(FT-IR)、拉曼光谱和 X 射线光电子能谱(XPS),研究了 POP-T 高效碘捕获的机制。亚胺键连接的芳环之间的独特 π-π 共轭体系与碘形成电荷转移配合物,这解释了其异常高的碘捕获能力。此外,杂原子的引入也会增强 POPs 的碘吸附能力。POPs 还表现出良好的保留行为和可回收能力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c94a/9415008/cd168f0a0e6d/molecules-27-05161-sch001.jpg

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