Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 12, Pages 14087-14094Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c02121
Keywords
periodic tendency; rare earth MOFs; adsorption; uranium; ionic radii
Funding
- National Natural Science Foundation of China [11775037, 21777161, 21836001, 21806167]
- Youth Innovation Promotion Association, CAS [2017020]
- Science Challenge Project [TZ2016004]
- Major Basic Research Project of the Natural Science Foundation of the Jiangsu Higher Education Institutions [19KJA150001]
- Center for Actinide Science and Technology, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0016568]
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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.
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