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Nanotrap grafted anionic MOF for superior uranium extraction from seawater

Abstract:
On-demand uranium extraction from seawater (UES) can mitigate growing sustainable energy needs, while high salinity and low concentration hinder its recovery. A novel anionic metal-organic framework (iMOF-1A) is demonstrated adorned with rare Lewis basic pyrazinic sites as uranyl-specific nanotrap serving as robust ion exchange material for selective uranium extraction, rendering its intrinsic ionic characteristics to minimize leaching. Ionic adsorbents sequestrate 99.8% of the uranium in 120 mins (from 20,000 ppb to 24 ppb) and adsorb large amounts of 1336.8 mg g−1 and 625.6 mg g−1 from uranium-spiked deionized water and artificial seawater, respectively, with high distribution coefficient, KdU ≥ 0.97 × 106 mL g−1. The material offers a very high enrichment index of ≈5754 and it achieves the UES standard of 6.0 mg g−1 in 16 days, and harvests 9.42 mg g−1 in 30 days from natural seawater. Isothermal titration calorimetry (ITC) studies quantify thermodynamic parameters, previously uncharted in uranium sorption experiments. Infrared nearfield nanospectroscopy (nano-FTIR) and tip-force microscopy (TFM) enable chemical and mechanical elucidation of host-guest interaction at atomic level in sub-micron crystals revealing extant capture events throughout the crystal rather than surface solely. Comprehensive experimentally guided computational studies reveal ultrahigh-selectivity for uranium from seawater, marking mechanistic insight.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1002/smll.202302014

Authors

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Role:
Author
ORCID:
0000-0002-0968-0220
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Institution:
University of Oxford
Division:
MPLS
Department:
Engineering Science
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Engineering Science
Role:
Author
ORCID:
0000-0003-2178-3158


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Funder identifier:
https://ror.org/0439y7842
Grant:
EP/R511742/1


Publisher:
Wiley
Journal:
Small More from this journal
Volume:
20
Issue:
3
Article number:
2302014
Place of publication:
Germany
Publication date:
2023-09-12
Acceptance date:
2023-08-08
DOI:
EISSN:
1613-6829
ISSN:
1613-6810
Pmid:
37698252


Language:
English
Keywords:
Pubs id:
1525736
Local pid:
pubs:1525736
Deposit date:
2023-09-21
ARK identifier:

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