Efficient removal of uranium under strong acid based on charge separation and protonation coupled covalent organic frameworks

被引:19
作者
Yi, Shun-Mo [1 ,2 ]
Zhang, Cheng-Rong [2 ]
Liu, Xin [2 ]
Chen, Xiao-Juan [2 ]
Qi, Jia-Xin [2 ]
Niu, Cheng-Peng [2 ]
Liu, Jin-Lan [2 ]
Liang, Ru-Ping [1 ,2 ]
Qiu, Jian-Ding [1 ,2 ]
机构
[1] East China Univ Technol, State Key Lab Nucl Resources & Environm, Nanchang 330013, Peoples R China
[2] Nanchang Univ, Sch Chem & Chem Engn, Nanchang 330031, Peoples R China
基金
中国国家自然科学基金;
关键词
Covalent organic frameworks; Uranium; Naphthalene diimide; Photocatalysis;
D O I
10.1016/j.cej.2023.146264
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Efficient removal of UO22+ from radioactive wastewater under strong acid conditions remains a significant challenge due to the competition of excess H+ for adsorption and reduction sites. Here, covalent organic framework with complete charge separation and protonation properties (DANT-BTT) was synthesized for effi-cient removal of UO22+ under strong acids. The DANT-BTT with strong electron-deficient naphthalimide signif-icantly extended light absorption and enhanced intramolecular charge transfer, which significantly improve the separation efficiency of electrons and holes. Additionally, the auxiliary coordination of hydroxyl groups after protonation provides unparalleled selectivity for UO22+ in strong acids, effectively preventing the competition of H+ for adsorption sites. Protonation of nitrogen atoms and ketones also extends light absorption and store electrons, further enhancing the photocatalytic performance of DANT-BTT. Consequently, DANT-BTT can ach-ieve 71 % photoreduction UO22+ efficiency (pH 1) after 60 min irradiation, where dark adsorption accounts for 43 %. This work provides a strategy for the efficient reduction of U(VI) under strong acids.
引用
收藏
页数:8
相关论文
共 50 条
[31]   Boosting Exciton Dissociation and Charge Transfer in Fluorine-Substituted Covalent Organic Frameworks with Biomimetic Electron Pumps for Remarkable Photocatalytic Extraction of Uranium [J].
Wu, Guihong ;
Yu, Fengtao ;
Liu, Yiping ;
Wang, Bo ;
Liu, Yan ;
Qiu, Jianding .
ACS APPLIED MATERIALS & INTERFACES, 2024, 17 (02) :3503-3513
[32]   Covalent organic frameworks filled Pebax hybrid membrane for efficient toluene/N2 separation [J].
Zhao, Jiashuai ;
Liu, Jiating ;
Wang, Yutong ;
Du, Jin ;
Zhu, Ziting ;
Wang, Yuhan ;
Zhao, Junyi ;
Long, Mengying ;
Pan, Fusheng ;
Jiang, Zhongyi .
JOURNAL OF MEMBRANE SCIENCE, 2024, 700
[33]   Lithium Pyrene Squarate Covalent Organic Frameworks for Efficient Lithium and Magnesium Separation from Salt Water [J].
Altaf, Ataf Ali ;
Khosropour, Ahmadreza ;
Zadehnazari, Amin ;
Abbaspourrad, Alireza .
ACS APPLIED MATERIALS & INTERFACES, 2023, 15 (15) :19672-19681
[34]   Benzotrithiophene-based covalent organic frameworks for sensitive fluorescence detection and efficient removal of Ag+ from drinking water [J].
Chen, Lei ;
Hu, Kexin ;
Wang, Jiaqi ;
Ge, Guangyu ;
Ma, Ran ;
Wu, Yongning ;
He, Qinghua .
TALANTA, 2025, 286
[35]   Effective separation and immobilization of uranium(VI) from wastewater using amino and carboxyl groups functionalized covalent organic frameworks [J].
Zhou, Mengfan ;
Wang, Shuqin ;
Liu, Fenglei ;
Hu, Baowei .
SEPARATION AND PURIFICATION TECHNOLOGY, 2024, 338
[36]   A sensing platform for ascorbic acid based on the spatial confinement of covalent organic frameworks [J].
Yang, Jierui ;
Qiu, Huiting ;
Meng, Shuang ;
Yang, Yunhui .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 2024, 308
[37]   Microenvironment Effect Catalysis with Phosphoric Acid-Based Covalent Organic Frameworks [J].
Qiu, Wenqi ;
Cui, Jialin ;
Zhu, Kejin ;
Gao, Meng ;
Zheng, Xuhan ;
Liu, Hui ;
Guo, Zongxia ;
Zhang, Zhenxiu ;
Zhao, Yingjie .
ACS CATALYSIS, 2024, 14 (19) :14780-14786
[38]   Thiadiazole-Based Covalent Organic Frameworks with a Donor-Acceptor Structure: Modulating Intermolecular Charge Transfer for Efficient Photocatalytic Degradation of Typical Emerging Contaminants [J].
Hou, Yanghui ;
Liu, Fuyang ;
Zhang, Boaiqi ;
Tong, Meiping .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2022, 56 (22) :16303-16314
[39]   Engineering N-donor heterocycles on dioxin-linked covalent organic frameworks to in situ improvement uranium separation and extraction selectivity in wastewater and seawater [J].
Yao, Ruihong ;
Wang, Jun ;
Li, Yanli ;
Qu, Wangbo ;
Yang, Bin ;
Lu, Jiao ;
Wu, Zhou ;
Li, Yong ;
Lu, Zhihao ;
Geng, Zhirong ;
Wang, Zhilin .
CHEMICAL ENGINEERING JOURNAL, 2025, 503
[40]   Simultaneous detection and separation of uranium based on a fluorescent amidoxime-functionalized covalent organic polymer [J].
Xiao, Sai Jin ;
Qiu, An Ting ;
Li, Hui Han ;
Wang, Meng Ping ;
Zhang, Li ;
Guo, Kai Xin ;
Guo, Jing ;
Qiu, Jian-Ding .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 2023, 289