Gram-scale green synthesis of a highly stable cationic covalent organic framework for efficient and selective removal of ReO4-/99TcO4-

IF 12.7 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ACS Central Science Pub Date : 2024-11-05 DOI:10.1039/d4ta06442a

Changxia Li, Justyna Florek, Patrick Guggenberger, Freddy Kleitz

{"title":"Gram-scale green synthesis of a highly stable cationic covalent organic framework for efficient and selective removal of ReO4-/99TcO4-","authors":"Changxia Li, Justyna Florek, Patrick Guggenberger, Freddy Kleitz","doi":"10.1039/d4ta06442a","DOIUrl":null,"url":null,"abstract":"Covalent organic frameworks (COFs) have developed as efficient and selective adsorbents to mitigate 99TcO4- contamination. However, the eco-friendly and scalable production of COF-based adsorbents for the removal of 99TcO4- has not yet been reported. This study explores the potential of a cationic COF (TpDB-COF) synthesized via a green hydrothermal method, achieving gram-scale yields per batch, thereby addressing a significant limitation of existing COF production methods. The TpDB-COF demonstrates an exceptional stability in strongly acidic conditions (2 weeks in 3 M HNO3), as well as in various organic solvents, making it suitable for harsh nuclear waste environments. Adsorption experiments using 99ReO4- as a surrogate for 99TcO4- show rapid adsorption kinetics, reaching near 100% removal efficiency within 1 min, a maximum adsorption capacity of 570 mg g-1 and excellent stability. Moreover, the COF maintains high selectivity for ReO4- even in the presence of competing anions such as SO42- and NO3-. These findings highlight that the hydrothermal synthesis is an effective method to synthesize COF adsorbents for effective removal of 99TcO4- and offers a sustainable approach for practical applications.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":null,"pages":null},"PeriodicalIF":12.7000,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Central Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4ta06442a","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

Covalent organic frameworks (COFs) have developed as efficient and selective adsorbents to mitigate 99TcO4- contamination. However, the eco-friendly and scalable production of COF-based adsorbents for the removal of 99TcO4- has not yet been reported. This study explores the potential of a cationic COF (TpDB-COF) synthesized via a green hydrothermal method, achieving gram-scale yields per batch, thereby addressing a significant limitation of existing COF production methods. The TpDB-COF demonstrates an exceptional stability in strongly acidic conditions (2 weeks in 3 M HNO3), as well as in various organic solvents, making it suitable for harsh nuclear waste environments. Adsorption experiments using 99ReO4- as a surrogate for 99TcO4- show rapid adsorption kinetics, reaching near 100% removal efficiency within 1 min, a maximum adsorption capacity of 570 mg g-1 and excellent stability. Moreover, the COF maintains high selectivity for ReO4- even in the presence of competing anions such as SO42- and NO3-. These findings highlight that the hydrothermal synthesis is an effective method to synthesize COF adsorbents for effective removal of 99TcO4- and offers a sustainable approach for practical applications.

查看原文

微信好友朋友圈 QQ好友复制链接

本刊更多论文

克级绿色合成高稳定性阳离子共价有机框架，用于高效和选择性去除 ReO4-/99TcO4-

共价有机框架（COFs）已发展成为一种高效且具有选择性的吸附剂，可用于减轻 99TcO4- 的污染。然而，以 COF 为基础的用于去除 99TcO4- 的生态友好型可扩展吸附剂的生产尚未见报道。本研究探讨了通过绿色水热法合成阳离子 COF（TpDB-COF）的潜力，每批产量达到克级，从而解决了现有 COF 生产方法的一个重大局限。TpDB-COF 在强酸性条件下（3 M HNO3 中 2 周）和各种有机溶剂中均表现出卓越的稳定性，使其适用于苛刻的核废料环境。使用 99ReO4- 作为 99TcO4- 的替代物进行的吸附实验表明，这种材料具有快速的吸附动力学特性，在 1 分钟内就能达到接近 100% 的去除效率，最大吸附容量为 570 mg g-1，而且具有出色的稳定性。此外，即使存在 SO42- 和 NO3- 等竞争阴离子，COF 对 ReO4- 也能保持较高的选择性。这些发现突出表明，水热合成法是合成 COF 吸附剂以有效去除 99TcO4- 的有效方法，并为实际应用提供了一种可持续的方法。

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分钟内获得全文去求助

来源期刊

ACS Central Science Chemical Engineering-General Chemical Engineering

CiteScore

25.50

自引率

0.50%

发文量

194

审稿时长

10 weeks

期刊介绍： ACS Central Science publishes significant primary reports on research in chemistry and allied fields where chemical approaches are pivotal. As the first fully open-access journal by the American Chemical Society, it covers compelling and important contributions to the broad chemistry and scientific community. "Central science," a term popularized nearly 40 years ago, emphasizes chemistry's central role in connecting physical and life sciences, and fundamental sciences with applied disciplines like medicine and engineering. The journal focuses on exceptional quality articles, addressing advances in fundamental chemistry and interdisciplinary research.