Mechanism unravelling for ultrafast and selective (TcO4-)-Tc-99 uptake by a radiation-resistant cationic covalent organic framework: a combined radiological experiment and molecular dynamics simulation study

doi:10.1039/c9sc00172g

CORC > 上海应用物理研究所 > 中国科学院上海应用物理研究所 > 中科院上海应用物理研究所2011-2017年

	Mechanism unravelling for ultrafast and selective (TcO4-)-Tc-99 uptake by a radiation-resistant cationic covalent organic framework: a combined radiological experiment and molecular dynamics simulation study
	He, LW ; Liu, ST ; Chen, L ; Dai, X ; Li, J ; Zhang, MX ; Ma, FY ; Zhang, C ; Yang, ZX ; Zhou, RH
刊名	CHEMICAL SCIENCE
	2019
卷号	10 期号:15 页码:4293—4305
关键词	LAYERED DOUBLE HYDROXIDES ANION-EXCHANGE RESINS TECHNETIUM PERTECHNETATE SEPARATION EFFICIENT CHEMISTRY BEHAVIOR DESIGN ADSORPTION
ISSN号	2041-6520
DOI	10.1039/c9sc00172g
文献子类	期刊论文
英文摘要	Tc-99 is one of the most problematic fission products in the nuclear fuel cycle owing to its large inventory in used nuclear fuel, long half-life, potential radiation hazard, high environmental mobility of its major species (TcO4-)-Tc-99, and its redox-active nature. Ideally, (TcO4-)-Tc-99 should be removed at the first stage, when the used fuel rods are dissolved in highly concentrated nitric acid solution, which can substantially reduce its interference with the solvent extraction process through catalytic redox reactions with the key actinides and diminish the chance of discharge into the environment as the volatile species during the waste vitrification process. However, this task cannot be achieved by any of the reported anion-scavenging materials including traditional polymeric anion-exchange resins, inorganic cationic framework materials, and recently developed cationic metal-organic framework materials, because they either are not stable under the extreme conditions of the combined high acidity and strong radiation field or do not possess the required uptake selectivity towards (TcO4-)-Tc-99 in the presence of a huge excess of competing anions such as NO3- and SO42-. Herein, we present the first study of (TcO4-)-Tc-99 removal under extreme conditions by a two-dimensional conjugated cationic covalent organic framework material, SCU-COF-1. This material exhibits ultrahigh acid stability, great resistance towards both large-dose and irradiation and unprecedented (TcO4-)-Tc-99 uptake capabilities including extremely fast sorption kinetics (sorption equilibrium can be reached within 1 min), ultrahigh uptake capacity (702.4 mg g(-1) for the surrogate ReO4- at a slightly elevated temperature), and good anion-exchange selectivity towards (TcO4-)-Tc-99. These excellent features endow SCU-COF-1 with the practical capabilities of separating (TcO4-)-Tc-99 from both simulant highly acidic fuel reprocessing solutions (3 M nitric acid) and low-activity waste streams at the US legacy nuclear site. The anion-exchange mechanism and the (TcO4-)-Tc-99 uptake selectivity are further demonstrated and clearly visualized by the molecular dynamics simulation investigations.
语种	英语
内容类型	期刊论文
源URL	[http://ir.sinap.ac.cn/handle/331007/31707]
专题	上海应用物理研究所_中科院上海应用物理研究所2011-2017年
作者单位	1.Soochow Univ, Sch Radiat Med & Protect, Collaborat Innovat Ctr Radiol Med Jiangsu Higher, State Key Lab Radiat Med & Protect, Suzhou 215123, Peoples R China; 2.Anhui Univ Sci & Technol, Sch Mat Sci & Engn, Huainan 232001, Peoples R China 3.Chinese Acad Sci, Shanghai Inst Appl Phys, 2019 Jialuo Rd, Shanghai 201800, Peoples R China;
推荐引用方式 GB/T 7714	He, LW,Liu, ST,Chen, L,et al. Mechanism unravelling for ultrafast and selective (TcO4-)-Tc-99 uptake by a radiation-resistant cationic covalent organic framework: a combined radiological experiment and molecular dynamics simulation study[J]. CHEMICAL SCIENCE,2019,10(15):4293—4305.
APA	He, LW.,Liu, ST.,Chen, L.,Dai, X.,Li, J.,...&Wang, S.(2019).Mechanism unravelling for ultrafast and selective (TcO4-)-Tc-99 uptake by a radiation-resistant cationic covalent organic framework: a combined radiological experiment and molecular dynamics simulation study.CHEMICAL SCIENCE,10(15),4293—4305.
MLA	He, LW,et al."Mechanism unravelling for ultrafast and selective (TcO4-)-Tc-99 uptake by a radiation-resistant cationic covalent organic framework: a combined radiological experiment and molecular dynamics simulation study".CHEMICAL SCIENCE 10.15(2019):4293—4305.