Structural transformation of metal oxo species within UiO-66 type metal–organic frameworks
Abstract
Studying the coordination of actinide-based metal oxo clusters can provide valuable insights for nuclear energy technologies and radioactive waste containment. Metal–organic frameworks serve as a platform to directly interrogate the structure and properties of understudied actinide elements, including thorium. Examples of structural evolutions within Th oxo species within MOFs are rare yet relevant for nuclear waste speciation in solution. Herein, we report the serendipitous discovery of the structural evolution of Th-UiO-66 containing a hexanuclear Th node to a mononuclear Th(bdc)2(dmf)2 upon the evaporation of solvent from the reaction. We observe a partial reversal of Th(bdc)2(dmf)2 back to Th-UiO-66 upon hydrothermal treatment, indicating the complex dynamics of Th oxo species in solution. As a result, we report that isolated Ce-UiO-66 similarly transforms to a newly isolated 1D CeIII carboxylate chain MOF named NU-351 under the same conditions as Th-UiO-66, while Zr-UiO-66 and Hf-UiO-66 retain their structures.
- Authors:
-
- Northwestern University, Evanston, IL (United States)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States); University of Notre Dame, IN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1978858
- Alternate Identifier(s):
- OSTI ID: 1874512
- Grant/Contract Number:
- FG02-03ER15457; NA0003763; DGE-1842165
- Resource Type:
- Accepted Manuscript
- Journal Name:
- CrystEngComm
- Additional Journal Information:
- Journal Volume: 24; Journal Issue: 28; Journal ID: ISSN 1466-8033
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Crystallography
Citation Formats
Wasson, Megan C., Xie, Haomiao, Wang, Xingjie, Duncan, Joshua S., and Farha, Omar K. Structural transformation of metal oxo species within UiO-66 type metal–organic frameworks. United States: N. p., 2022.
Web. doi:10.1039/d2ce00650b.
Wasson, Megan C., Xie, Haomiao, Wang, Xingjie, Duncan, Joshua S., & Farha, Omar K. Structural transformation of metal oxo species within UiO-66 type metal–organic frameworks. United States. https://doi.org/10.1039/d2ce00650b
Wasson, Megan C., Xie, Haomiao, Wang, Xingjie, Duncan, Joshua S., and Farha, Omar K. Thu .
"Structural transformation of metal oxo species within UiO-66 type metal–organic frameworks". United States. https://doi.org/10.1039/d2ce00650b. https://www.osti.gov/servlets/purl/1978858.
@article{osti_1978858,
title = {Structural transformation of metal oxo species within UiO-66 type metal–organic frameworks},
author = {Wasson, Megan C. and Xie, Haomiao and Wang, Xingjie and Duncan, Joshua S. and Farha, Omar K.},
abstractNote = {Studying the coordination of actinide-based metal oxo clusters can provide valuable insights for nuclear energy technologies and radioactive waste containment. Metal–organic frameworks serve as a platform to directly interrogate the structure and properties of understudied actinide elements, including thorium. Examples of structural evolutions within Th oxo species within MOFs are rare yet relevant for nuclear waste speciation in solution. Herein, we report the serendipitous discovery of the structural evolution of Th-UiO-66 containing a hexanuclear Th node to a mononuclear Th(bdc)2(dmf)2 upon the evaporation of solvent from the reaction. We observe a partial reversal of Th(bdc)2(dmf)2 back to Th-UiO-66 upon hydrothermal treatment, indicating the complex dynamics of Th oxo species in solution. As a result, we report that isolated Ce-UiO-66 similarly transforms to a newly isolated 1D CeIII carboxylate chain MOF named NU-351 under the same conditions as Th-UiO-66, while Zr-UiO-66 and Hf-UiO-66 retain their structures.},
doi = {10.1039/d2ce00650b},
journal = {CrystEngComm},
number = 28,
volume = 24,
place = {United States},
year = {Thu Jun 30 00:00:00 EDT 2022},
month = {Thu Jun 30 00:00:00 EDT 2022}
}
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