Precise recognition of palladium through interlaminar chelation in a covalent organic framework

被引:94
作者
Bai, Yaoyao [1 ,2 ]
Chen, Long [1 ,2 ]
He, Linwei [1 ,2 ]
Li, Baoyu [1 ,2 ]
Chen, Lixi [1 ,2 ]
Wu, Fuqi [1 ,2 ]
Chen, Lanhua [1 ,2 ]
Zhang, Mingxing [1 ,2 ]
Liu, Zhiyong [1 ,2 ]
Chai, Zhifang [1 ,2 ]
Wang, Shuao [1 ,2 ]
机构
[1] Soochow Univ, State Key Lab Radiat Med & Protect, Sch Radiol & Interdisciplinary Sci RAD X, Suzhou 215123, Peoples R China
[2] Soochow Univ, Collaborat Innovat Ctr Radiat Med Jiangsu Higher, Suzhou 215123, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
LEVEL LIQUID WASTE; PLATINUM-GROUP METALS; SOLVENT-EXTRACTION; SUZUKI-MIYAURA; SEPARATION; ENERGY; ADSORPTION; EFFICIENT; PLATFORM; ACID;
D O I
10.1016/j.chempr.2022.02.016
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Palladium isotopes as fission products in used nuclear fuel represent precious alternative resources besides its natural reserves and therefore have a high extraction value. The practical use of currently proposed solvent extraction is challenging, originating from the limited stability and separation selectivity of the extractants under harsh reprocessing conditions. Herein, we present an interlayer synergistic binding strategy, a metal-recognition manner deviating from chelation within a single ligand molecule in solvent extraction, for selective palladium chelation in a covalent organic framework The experimental, structural, and theoretical analyses corroborate that the enol-to-keto tautomerization leads to selective synergistic chelation of Pd2+ instead of other undesired metal ions, where two oxygen donors from adjacent layers and two free nitrate ions work together in a planar tetracoordination model. Fast adsorption kinetics, high adsorption capacity, and one-round enrichment of Pd2+ from the simulated high-level nuclear waste solution are unprecedentedly achieved in the dynamic breakthrough experiment.
引用
收藏
页码:1442 / 1459
页数:19
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