Advances in Adsorption Materials and Coordination Mechanism of Functional Groups for Uranium Extraction from Seawater

doi:10.6023/A24020041

Acta Chimica Sinica ›› 2024, Vol. 82 ›› Issue (4): 458-470.DOI: 10.6023/A24020041 Previous Articles

Review

海水提铀吸附材料及官能团配位机理研究进展

徐晗^a^,^b, 王聪芝^b^,^*(), 刘峙嵘^a^,^*(), 石伟群^b^,^*()

a 东华理工大学核科学与工程学院南昌 330013
b 中国科学院高能物理研究所核能放射化学实验室北京 100049

投稿日期:2024-02-01 发布日期:2024-03-21

作者简介:

徐晗, 东华理工大学硕士研究生, 目前研究方向: 海水提铀理论计算.

王聪芝, 中国科学院高能物理研究所副研究员, 2012年博士毕业于北京理工大学. 长期专注于锕系元素计算与模拟方面的研究, 主要工作集中在海水提铀材料以及高放废液中新型锕系分离配体的理论设计方面. 目前以第一作者和通讯作者在ACS Cent. Sci.、Chem. Commun.、Inorg. Chem.等国内外知名期刊发表数十篇学术论文, 先后主持多项国家自然科学基金项目.

刘峙嵘, 本科毕业于青岛理工大学, 博士毕业于中国原子能科学研究院. 在国内外学术期刊上发表百余篇学术论文、专利12项; 获省部级奖6项. 先后主持国家自然科学基金面上/地区项目/江西省自然科学基金项目/江西省科技支撑计划项目多项. 国家自然科学基金函评专家、中国博士后科学基金评审专家、中国博士后科学基金特别资助评审专家、教育部留学归国人员科研启动基金评审专家. 中国辐射防护学会环境放射化学分会理事、中国核学会锕系元素物理与化学分会理事、中国核学会核化工分会理事. Journal of Hazardous Materials、Environmental Science & Technology、Applied Surface Science等国际学术刊物审稿专家.

石伟群, 中国科学院高能物理研究所研究员, 国家杰出青年科学基金获得者, 长期致力于核燃料循环化学相关基础研究. 在JACS、Angew. Chem、Chem.、Chem. Sci.、CCS Chem.、Nat. Commun、Adv. Mater.等国际知名期刊发表SCI 论文300余篇, 成果被国内外同行广泛关注和引用, 文章总引15000余次, H因子62 (Google Scholar), 2019~2022年每年均入选Elsevier中国高被引学者榜单(核科学技术). 分别担任期刊《Supramolecular Materials》副主编, 《Chinese Chemical Letters》、《Journal of Nuclear Fuel Cycle and Waste Technology》、《International Journal of Advanced Nuclear Reactor Design and Technology》和《Journal of Nuclear Science and Technology》的编委与国际顾问编委, 中文期刊《核化学与放射化学》编委. 现为中国核学会锕系物理与化学分会副理事长、中国有色金属学会熔盐化学与技术专业委员会副主任委员、中国化学会核化学与放射化学专业委员会委员、中国核学会核化工分会常务理事兼副秘书长.

Advances in Adsorption Materials and Coordination Mechanism of Functional Groups for Uranium Extraction from Seawater

Han Xu^a^,^b, Congzhi Wang^b,*(), Zhirong Liu^a,*(), Weiqun Shi^b,*()

a School of Nuclear Science and Engineering, East China University of Technology, Nanchang 330013, China
b Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

Received:2024-02-01 Published:2024-03-21
Contact: * E-mail: wangcongzhi@ihep.ac.cn; zhrliu@ecut.edu.cn; shiwq@ihep.ac.cn

Uranium is one of the most important elements in the development of nuclear industry. However, terrestrial uranium resources are limited and difficult to meet the development needs. Since seawater is rich in uranium resources (about 4.5×10⁹ t), which is more than one thousand times of the known terrestrial uranium resources, how to extract uranium resources from seawater has attracted much attention. However, uranium exists in seawater in the stable carbonate of [UO₂(CO₃)₃]^4-, which has a very low concentration of 3.3 μg/L, and the competitive ions especially for vanadium ions and biological contamination are serious obstacles to the extraction of uranium. Because of these complicated conditions of seawater and the extremely low concentration of uranium, uranium extraction from seawater faces many challenges. Many researchers have carried out a lot of studies, and various methods have been developed for the extraction of uranium from seawater. Among them, the adsorption method has been widely used in the extraction of uranium from seawater. This review focuses on the adsorption materials developed in recent years for uranium extraction from seawater, including inorganic materials, organic materials, inorganic-organic hybrid materials, and analyzes their advantages and disadvantages of the materials in terms of their adsorption capacity, selectivity, antimicrobial properties, stability, and recyclability. At the same time, the coordination mechanism of the typical functional groups such as amidoxime and carboxyl groups as well as other representative functional groups reported in recent years toward uranyl cations have been summarized, and the results show that in addition to amidoxime, other functional groups such as pentadentate chelating ligands also have good affinities for uranyl cations. Besides, the future development of uranium extraction materials from seawater is also prospected. This review is expected to improve our current understanding of the interaction mechanism of functional groups toward uranyl cations, and provide references for the development of efficient materials for uranium extraction from seawater.

Key words: uranium, seawater, adsorption materials, functional groups, coordination mechanism

Cite this article

Han Xu, Congzhi Wang, Zhirong Liu, Weiqun Shi. Advances in Adsorption Materials and Coordination Mechanism of Functional Groups for Uranium Extraction from Seawater[J]. Acta Chimica Sinica, 2024, 82(4): 458-470.

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Fig. & Tab. 19

吸附剂类型	优点	缺点
无机吸附材料	制备工艺简单、成本低、吸附率高、易于洗脱	选择性差、在海水中容易流失、不易回收、稳定性差
有机吸附材料	比表面积高、表面化学性质易调节、循环性高、选择性高	制备成本高、制备工艺复杂、易被污染
无机-有机杂化吸附材料	负载率高、比表面积大、稳定性高、选择性高	制备成本高、合成条件苛刻、不易回收

Table 1. Advantages and disadvantages of the adsorption materials for uranium extraction from seawater.

Figure 1. Uranium (VI) speciation in seawater, the dashed gray line corresponds to an approximate seawater pH (about 8.2)[40] (1) UO22+; (2) (UO2)(CO3)(aq); (3) UO2OH+; (4) [(UO2)(CO3)2]2-; (5) Ca2[(UO2)(CO3)3](aq); (6) Mg[(UO2)(CO3)3]2-; (7) Ca[(UO2)(CO3)3]2-; (8) [UO2(CO3)3]4-[40]. Copyright 2016, American Chemical Society

Element	Concentration in seawater
Element	mg•kg^-1 (ppm)	mol•L^-1
Cl	19400	0.546
Na	10800	0.468
Mg	1290	53×10^-3
Ca	413	10.3×10^-3
K	400	10.2×10^-3
Li	0.18	26×10^-6
Ni	0.005	8×10^-9
Fe	0.0034	0.5×10^-9
U	0.0033	14×10^-9
V	0.00183	36×10^-9
Cu	0.001	3×10^-9
S	0.0009	28×10^-3
Pb	0.00003	0.01×10^-9
TIC^a	0.00029	24.2×10^-3
DIP^b	0.00071	2.3×10^-6

Figure 6. (a) Demonstration for mass production of blow spun PIDO NFs as uranium adsorbent[57]. Copyright 2018, American Chemical Society. (b) The ionic crosslinking and selective uranium-adsorption mechanism of the Zn2+-PAO[60]. Copyright 2020, American Chemical Society

Figure 10. Schematic diagram for enhanced uranium extraction by BP-PAO fiber. (a) Fabrication of the BP-PAO fiber. (b) Mechanism for enhanced uranium adsorption by the BP-PAO fiber[84]. Copyright 2020, American Chemical Society

Figure 11. (a) Scheme for adsorption of uranyl ions by UiO-66-AO[90]. Copyright 2017, American Chemical Society. (b) Synthetic route for the formation of MIL-101-OA[94]. Copyright 2019, American Chemical Society. (c) Scheme for targeting uranyl capture by nano-pocket in MOF[93]. Copyright 2020, American Chemical Society. (d) Schematic showing the preparation of HNU-50[96]. Copyright 2020, American Chemical Society

Figure 12. (a) Schematic illustration of the preparation of COF-COOH and COF-HBI[102]. Copyright 2015, American Chemical Society. (b) Synthetic scheme of SO3H-decorated COF (COF-SO3H) and the ammoniated material of [NH4]+[COF-SO3-][105]. Copyright 2019, American Chemical Society. (c) Structure diagram of the uranium adsorbents, JUC-505-AO and JUC-505-COOH[107]. Copyright 2022, American Chemical Society

Figure 15. DFT optimized structures of uranyl complexes in a synergistic coordination mode. (a) HA-AO-, (b) HA-Ac-, (c) AO--Ac- (1∶1), (d) AO--Ac- (2∶1) and (e) AO--AA- (1∶2)[136]. Copyright 2022, American Chemical Society

Figure 16. (a) Structure of PDA ligand[147]. Copyright 2006, American Chemical Society. (b) Schematic structure of UO2(saldien)[157]. (c) Crystal structure of UO2(saldian)[156]. Copyright 2022, American Chemical Society

配体名称	配位机理	亲和力和选择性
偕胺肟	η²双齿配位或单齿配位	与铀酰离子的亲和力较强, 但选择性较低
酰亚胺二肟	三齿配位	相比偕胺肟, 与铀酰离子的亲和力更强, 但选择性更差
双(羟基胺)-1,3,5-三嗪	三齿配位	相比酰亚胺二肟, 与铀酰离子的亲和力更强
羧基(与偕胺肟协同配位)	单齿或双齿配位	与偕胺肟协同配位, 有利于络合铀酰离子
磷酸基(与偕胺肟协同配位)	单齿或双齿配位	与偕胺肟协同配位, 有利于络合铀酰离子
1,10-菲罗啉-2,9-二羧酸	四齿螯合	与铀酰离子的结合能力强于钒离子, 对铀酰离子具有良好的选择性
五齿螯合配体H₂saldian	五齿螯合	与其他金属离子共存时, 对铀酰离子具有较高的选择性

Table 3. Comparison of the interactions between some typical ligands and uranyl ions

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海水提铀吸附材料及官能团配位机理研究进展

Advances in Adsorption Materials and Coordination Mechanism of Functional Groups for Uranium Extraction from Seawater

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[7]	Sun Mengjia, Wu Tianyi, Li Tianyu, Guo Fengqiao, Tang Yang, Mo Hengliang, Yang Zhitao, Wan Pingyu. Research on High Performance Ammonium Removal Materials Based on δ-MnO₂ Nanoplate Arrays Decorated Graphite Felt [J]. Acta Chim. Sinica, 2018, 76(6): 467-474.
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