Rational Construction of Porous Metal-Organic Frameworks for Uranium(VI) Extraction: The Strong Periodic Tendency with a Metal Node

Zhi-Hui Zhang; Jian-Hui Lan; Li-Yong Yuan; Pan-Pan Sheng; Ming-Yang He; Li-Rong Zheng; Qun Chen; Zhi-Fang Chai; John K Gibson; Wei-Qun Shi

doi:10.1021/acsami.0c02121

Rational Construction of Porous Metal-Organic Frameworks for Uranium(VI) Extraction: The Strong Periodic Tendency with a Metal Node

ACS Appl Mater Interfaces. 2020 Mar 25;12(12):14087-14094. doi: 10.1021/acsami.0c02121. Epub 2020 Mar 10.

Authors

Zhi-Hui Zhang¹, Jian-Hui Lan², Li-Yong Yuan², Pan-Pan Sheng¹, Ming-Yang He¹, Li-Rong Zheng³, Qun Chen¹, Zhi-Fang Chai^{2

4}, John K Gibson⁵, Wei-Qun Shi²

Affiliations

¹ Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, Changzhou University, Changzhou 213164, China.
² Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China.
³ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China.
⁴ Engineering Laboratory of Advanced Energy Materials, Ningbo Institute of Industrial Technology, Chinese Academy of Sciences, Ningbo, Zhejiang 315201, China.
⁵ Chemical Sciences Division, Lawrence Berkeley National Laboratory (LBNL), Berkeley, California 94720, United States.

PMID: 32109047
DOI: 10.1021/acsami.0c02121

Abstract

Although metal-organic frameworks (MOFs) have been reported as important porous materials for the potential utility in metal ion separation, coordinating the functionality, structure, and component of MOFs remains a great challenge. Herein, a series of anionic rare earth MOFs (RE-MOFs) were synthesized via a solvothermal template reaction and for the first time explored for uranium(VI) capture from an acidic medium. The unusually high extraction capacity of UO₂²⁺ (e.g., 538 mg U per g of Y-MOF) was achieved through ion-exchange with the concomitant release of Me₂NH₂⁺, during which the uranium(VI) extraction in the series of isostructural RE-MOFs was found to be highly sensitive to the ionic radii of the metal nodes. That is, the uranium(VI) adsorption capacities continuously increased as the ionic radii decreased. In-depth mechanism insight was obtained from molecular dynamics simulations, suggesting that both the accessible pore volume of the MOFs and hydrogen-bonding interactions contribute to the strong periodic tendency of uranium(VI) extraction.

Keywords: adsorption; ionic radii; periodic tendency; rare earth MOFs; uranium.