Strong acid- and irradiation-resistant nitrogen-rich covalent organic polymers with high iodine adsorption capacity

IF 5.3 2区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Molecular Liquids Pub Date : 2024-10-31 DOI:10.1016/j.molliq.2024.126372

Weiwei Du , Cailing Ni , Chao Liu , Hewei Yan , Jun Zhu , Yumei Luo , Ye Tao , Ao Meng , Yuancheng Qin

{"title":"Strong acid- and irradiation-resistant nitrogen-rich covalent organic polymers with high iodine adsorption capacity","authors":"Weiwei Du , Cailing Ni , Chao Liu , Hewei Yan , Jun Zhu , Yumei Luo , Ye Tao , Ao Meng , Yuancheng Qin","doi":"10.1016/j.molliq.2024.126372","DOIUrl":null,"url":null,"abstract":"<div><div>The removal of radioactive iodine from nuclear waste is very important for the development of nuclear energy. Covalent organic polymers (COPs) have been widely investigated for iodine capture due to their simple operation, diverse structures, and abundant pores. However, the disposal of nuclear waste in a strongly acidic and radioactive environment is still a great challenge. Herein, three nitrogen-rich COPs were successfully designed and synthesized by Schiff-base polycondensation reactions. The high density of N atoms in triazines and imines enhanced the binding capacity of iodine molecules, with an optimal gas-phase iodine adsorption capacity of 4.98 g g<sup>−1</sup> and a liquid-phase iodine adsorption capacity of 1224.6 mg g<sup>−1</sup>. The backbone structure of the hydrazone bond connection and the introduction of thiophene effectively enhanced the stability of the TZ-COPs. The adsorption performance of TZ-2 was maintained after 6 M HNO<sub>3</sub> immersion and 100 kGy radiation irradiation, respectively. In addition, TZ-2 still has 92.32 % adsorption performance in five cycles, with excellent reversible regeneration ability. Therefore, this work is important for the preparation of nitrogen-rich COPs for the efficient and reversible removal of radioiodine from nuclear waste.</div></div>","PeriodicalId":371,"journal":{"name":"Journal of Molecular Liquids","volume":"415 ","pages":"Article 126372"},"PeriodicalIF":5.3000,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Molecular Liquids","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0167732224024310","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

Abstract

The removal of radioactive iodine from nuclear waste is very important for the development of nuclear energy. Covalent organic polymers (COPs) have been widely investigated for iodine capture due to their simple operation, diverse structures, and abundant pores. However, the disposal of nuclear waste in a strongly acidic and radioactive environment is still a great challenge. Herein, three nitrogen-rich COPs were successfully designed and synthesized by Schiff-base polycondensation reactions. The high density of N atoms in triazines and imines enhanced the binding capacity of iodine molecules, with an optimal gas-phase iodine adsorption capacity of 4.98 g g⁻¹ and a liquid-phase iodine adsorption capacity of 1224.6 mg g⁻¹. The backbone structure of the hydrazone bond connection and the introduction of thiophene effectively enhanced the stability of the TZ-COPs. The adsorption performance of TZ-2 was maintained after 6 M HNO₃ immersion and 100 kGy radiation irradiation, respectively. In addition, TZ-2 still has 92.32 % adsorption performance in five cycles, with excellent reversible regeneration ability. Therefore, this work is important for the preparation of nitrogen-rich COPs for the efficient and reversible removal of radioiodine from nuclear waste.

查看原文本刊更多论文

具有高碘吸附能力的强酸和耐辐照富氮共价有机聚合物

清除核废料中的放射性碘对核能发展非常重要。共价有机聚合物（COPs）因其操作简单、结构多样、孔隙丰富等特点，已被广泛用于碘捕获研究。然而，在强酸性和放射性环境中处理核废料仍然是一个巨大的挑战。本文通过席夫碱缩聚反应成功设计并合成了三种富氮 COPs。三嗪和亚胺中高密度的 N 原子增强了碘分子的结合能力，最佳气相碘吸附量为 4.98 g g-1，液相碘吸附量为 1224.6 mg g-1。腙键连接的骨架结构和噻吩的引入有效提高了 TZ-COPs 的稳定性。TZ-2 的吸附性能分别在 6 M HNO3 浸泡和 100 kGy 辐射辐照后得以保持。此外，TZ-2 在五个循环中仍有 92.32 % 的吸附性能，具有极佳的可逆再生能力。因此，这项工作对于制备富氮 COPs 从核废料中高效、可逆地去除放射性碘具有重要意义。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Journal of Molecular Liquids 化学-物理：原子、分子和化学物理

CiteScore

10.30

自引率

16.70%

发文量

2597

审稿时长

78 days

期刊介绍： The journal includes papers in the following areas: – Simple organic liquids and mixtures – Ionic liquids – Surfactant solutions (including micelles and vesicles) and liquid interfaces – Colloidal solutions and nanoparticles – Thermotropic and lyotropic liquid crystals – Ferrofluids – Water, aqueous solutions and other hydrogen-bonded liquids – Lubricants, polymer solutions and melts – Molten metals and salts – Phase transitions and critical phenomena in liquids and confined fluids – Self assembly in complex liquids.– Biomolecules in solution The emphasis is on the molecular (or microscopic) understanding of particular liquids or liquid systems, especially concerning structure, dynamics and intermolecular forces. The experimental techniques used may include: – Conventional spectroscopy (mid-IR and far-IR, Raman, NMR, etc.) – Non-linear optics and time resolved spectroscopy (psec, fsec, asec, ISRS, etc.) – Light scattering (Rayleigh, Brillouin, PCS, etc.) – Dielectric relaxation – X-ray and neutron scattering and diffraction. Experimental studies, computer simulations (MD or MC) and analytical theory will be considered for publication; papers just reporting experimental results that do not contribute to the understanding of the fundamentals of molecular and ionic liquids will not be accepted. Only papers of a non-routine nature and advancing the field will be considered for publication.