Cationic covalent organic frameworks based on pyridine and triazine for selective extraction of radioactive 99TcO4- from contaminated water

[Display omitted] •A cationic covalent organic framework with triazine and pyridine (COF-Tys) is designed by directly introducing quaternary ammonium.•COF-Tys demonstrates excellent chemical stability and radiation resistance.•COF-Tys exhibits high efficiency and remarkable selectivity in capturing...

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Published inSeparation and purification technology Vol. 354; p. 128786
Main Authors Tang, Qing, Wu, Qun-Yan, Shi, Wei-Qun, Han, Gang, Pan, Xiao-Han, Jin, Ming-Jie, Zheng, De-Rui, Zhou, Guang-Ze-Guo, Zu, Jian-Hua
Format Journal Article
LanguageEnglish
Published Elsevier B.V 19.02.2025
Subjects
99TcO4-/ReO4
Covalent organic frameworks
Ion exchange
Radioactive wastewater
Selective removal
Covalent organic frameworks
Selective removal
Ion exchange
Radioactive wastewater
99TcO4-/ReO4
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Abstract [Display omitted] •A cationic covalent organic framework with triazine and pyridine (COF-Tys) is designed by directly introducing quaternary ammonium.•COF-Tys demonstrates excellent chemical stability and radiation resistance.•COF-Tys exhibits high efficiency and remarkable selectivity in capturing 99TcO4-/ReO4- from diverse contaminated water.•The predominant adsorption mechanism for 99TcO4-/ReO4- is proved to be anion exchange. Efficient elimination of 99TcO4- is crucial for radioactive waste management and environmental protection, but achieving outstanding stability and high selectivity remains a major challenge for the reported adsorbents. In this study, we report a cationic covalent organic framework based on pyridine and triazine (COF-Tys) for the selective extraction of 99TcO4-/ReO4- (a non-radioactive surrogate of 99TcO4-). COF-Tys exhibits excellent stability under acidic or irradiation conditions. Experimental results reveal that COF-Tys possesses high adsorption capacity (422.61 mg/g for ReO4-), rapid kinetics (removing over 99% of 99TcO4- within 5 min), and promising recyclability (less than a 1.5% decrease in ReO4- removal after five adsorption/desorption cycles). Notably, COF-Tys demonstrates remarkable selectivity, adsorbing more than 90% of 99TcO4- even in simulated radioactive solutions with excess competing ions. Furthermore, COF-Tys achieves 97.5% and 80.4% removal of 99TcO4- from contaminated groundwater and seawater within 10 min, respectively. Energy dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS) analyses confirm that the primary mechanism of 99TcO4-/ReO4- adsorption involves anion exchange between Cl- and 99TcO4-/ReO4-. In conclusion, COF-Tys holds tremendous potential as a high-performance adsorbent for the separationof 99TcO4- from radioactive wastewater.
AbstractList [Display omitted] •A cationic covalent organic framework with triazine and pyridine (COF-Tys) is designed by directly introducing quaternary ammonium.•COF-Tys demonstrates excellent chemical stability and radiation resistance.•COF-Tys exhibits high efficiency and remarkable selectivity in capturing 99TcO4-/ReO4- from diverse contaminated water.•The predominant adsorption mechanism for 99TcO4-/ReO4- is proved to be anion exchange. Efficient elimination of 99TcO4- is crucial for radioactive waste management and environmental protection, but achieving outstanding stability and high selectivity remains a major challenge for the reported adsorbents. In this study, we report a cationic covalent organic framework based on pyridine and triazine (COF-Tys) for the selective extraction of 99TcO4-/ReO4- (a non-radioactive surrogate of 99TcO4-). COF-Tys exhibits excellent stability under acidic or irradiation conditions. Experimental results reveal that COF-Tys possesses high adsorption capacity (422.61 mg/g for ReO4-), rapid kinetics (removing over 99% of 99TcO4- within 5 min), and promising recyclability (less than a 1.5% decrease in ReO4- removal after five adsorption/desorption cycles). Notably, COF-Tys demonstrates remarkable selectivity, adsorbing more than 90% of 99TcO4- even in simulated radioactive solutions with excess competing ions. Furthermore, COF-Tys achieves 97.5% and 80.4% removal of 99TcO4- from contaminated groundwater and seawater within 10 min, respectively. Energy dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS) analyses confirm that the primary mechanism of 99TcO4-/ReO4- adsorption involves anion exchange between Cl- and 99TcO4-/ReO4-. In conclusion, COF-Tys holds tremendous potential as a high-performance adsorbent for the separationof 99TcO4- from radioactive wastewater.
ArticleNumber 128786
Author Tang, Qing
Wu, Qun-Yan
Han, Gang
Zu, Jian-Hua
Zheng, De-Rui
Pan, Xiao-Han
Zhou, Guang-Ze-Guo
Jin, Ming-Jie
Shi, Wei-Qun
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  surname: Wu
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  givenname: Wei-Qun
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  givenname: Ming-Jie
  surname: Jin
  fullname: Jin, Ming-Jie
  email: mingjiejin@sjtu.edu.cn
  organization: School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
– sequence: 7
  givenname: De-Rui
  surname: Zheng
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  surname: Zu
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  email: zujianhua@sjtu.edu.cn
  organization: School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
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Keywords Covalent organic frameworks
Selective removal
Ion exchange
Radioactive wastewater
99TcO4-/ReO4
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Snippet [Display omitted] •A cationic covalent organic framework with triazine and pyridine (COF-Tys) is designed by directly introducing quaternary ammonium.•COF-Tys...
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elsevier
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StartPage 128786
SubjectTerms 99TcO4-/ReO4
Covalent organic frameworks
Ion exchange
Radioactive wastewater
Selective removal
Title Cationic covalent organic frameworks based on pyridine and triazine for selective extraction of radioactive 99TcO4- from contaminated water
URI https://dx.doi.org/10.1016/j.seppur.2024.128786
Volume 354
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