Changxia Li, Justyna Florek, Patrick Guggenberger and Freddy Kleitz
{"title":"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-","authors":"Changxia Li, Justyna Florek, Patrick Guggenberger and Freddy Kleitz","doi":"10.1039/D4TA06442A","DOIUrl":null,"url":null,"abstract":"<p >Covalent organic frameworks (COFs) have developed as efficient and selective adsorbents to mitigate <small><sup>99</sup></small>TcO<small><sub>4</sub></small><small><sup>−</sup></small> contamination. However, the eco-friendly and scalable production of COF-based adsorbents for the removal of <small><sup>99</sup></small>TcO<small><sub>4</sub></small><small><sup>−</sup></small> has not yet been reported. This study explores the potential of a cationic COF (TpDB-COF) synthesized <em>via</em> 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 HNO<small><sub>3</sub></small>), as well as in various organic solvents, making it suitable for harsh nuclear waste environments. Adsorption experiments using ReO<small><sub>4</sub></small><small><sup>−</sup></small> as a surrogate for <small><sup>99</sup></small>TcO<small><sub>4</sub></small><small><sup>−</sup></small> show rapid adsorption kinetics, reaching nearly 100% removal efficiency within 1 min (with initial concentration of 28 ppm at a solid-to-liquid ratio of 1 g L<small><sup>−1</sup></small>), a maximum adsorption capacity of 570 mg g<small><sup>−1</sup></small> and excellent stability. Moreover, the COF maintains high selectivity for ReO<small><sub>4</sub></small><small><sup>−</sup></small> even in the presence of competing anions such as SO<small><sub>4</sub></small><small><sup>2−</sup></small> and NO<small><sub>3</sub></small><small><sup>−</sup></small>. These findings highlight that the hydrothermal synthesis is an effective method to synthesize COF adsorbents for efficient removal of <small><sup>99</sup></small>TcO<small><sub>4</sub></small><small><sup>−</sup></small> and offers a sustainable approach for practical applications.</p>","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":" 1","pages":" 214-219"},"PeriodicalIF":10.7000,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ta/d4ta06442a?page=search","citationCount":"0","resultStr":"{\"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 and Freddy Kleitz\",\"doi\":\"10.1039/D4TA06442A\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Covalent organic frameworks (COFs) have developed as efficient and selective adsorbents to mitigate <small><sup>99</sup></small>TcO<small><sub>4</sub></small><small><sup>−</sup></small> contamination. However, the eco-friendly and scalable production of COF-based adsorbents for the removal of <small><sup>99</sup></small>TcO<small><sub>4</sub></small><small><sup>−</sup></small> has not yet been reported. This study explores the potential of a cationic COF (TpDB-COF) synthesized <em>via</em> 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 HNO<small><sub>3</sub></small>), as well as in various organic solvents, making it suitable for harsh nuclear waste environments. Adsorption experiments using ReO<small><sub>4</sub></small><small><sup>−</sup></small> as a surrogate for <small><sup>99</sup></small>TcO<small><sub>4</sub></small><small><sup>−</sup></small> show rapid adsorption kinetics, reaching nearly 100% removal efficiency within 1 min (with initial concentration of 28 ppm at a solid-to-liquid ratio of 1 g L<small><sup>−1</sup></small>), a maximum adsorption capacity of 570 mg g<small><sup>−1</sup></small> and excellent stability. Moreover, the COF maintains high selectivity for ReO<small><sub>4</sub></small><small><sup>−</sup></small> even in the presence of competing anions such as SO<small><sub>4</sub></small><small><sup>2−</sup></small> and NO<small><sub>3</sub></small><small><sup>−</sup></small>. 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Gram-scale green synthesis of a highly stable cationic covalent organic framework for efficient and selective removal of ReO4−/99TcO4−†
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 ReO4− as a surrogate for 99TcO4− show rapid adsorption kinetics, reaching nearly 100% removal efficiency within 1 min (with initial concentration of 28 ppm at a solid-to-liquid ratio of 1 g L−1), 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 efficient removal of 99TcO4− and offers a sustainable approach for practical applications.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.