Advancement of Actinide Metal–Organic Framework Chemistry via Synthesis of Pu-UiO-66
Abstract
We report the synthesis and characterization of the first plutonium metal–organic framework (MOF). Pu-UiO-66 expands the established UiO-66 series, which includes transition metal, lanthanide, and early actinide elements in the hexanuclear nodes. The thermal stability and porosity of Pu-UiO-66 were experimentally determined, and multifaceted computational methods were used to corroborate experimental values, examine inherent defects in the framework, decipher spectroscopic signatures, and elucidate the electronic structure. The crystallization of a plutonium chain side product provides direct evidence of the competition that occurs between modulator and linker in MOF syntheses. Ultimately, the synthesis of Pu-UiO-66 demonstrates adept control of Pu(IV) coordination under hydrolysis-prone conditions, provides an opportunity to extend trends across isostructural UiO-66 frameworks, and serves as the foundation for future plutonium MOF chemistry.
- Authors:
-
[2];
[2];
[2];
[3];
[1]
- Univ. of Notre Dame, IN (United States)
- Univ. of Minnesota, Minneapolis, MN (United States)
- Northwestern Univ., Evanston, IL (United States)
- Publication Date:
- Research Org.:
- University of Notre Dame, IN (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1623393
- Grant/Contract Number:
- NA0003763
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 142; Journal Issue: 20; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; actinides; computational chemistry; metal–organic frameworks; microporous materials; plutonium(IV)
Citation Formats
Hastings, Ashley M., Ray, Debmalya, Jeong, WooSeok, Gagliardi, Laura, Farha, Omar K., and Hixon, Amy E. Advancement of Actinide Metal–Organic Framework Chemistry via Synthesis of Pu-UiO-66. United States: N. p., 2020.
Web. doi:10.1021/jacs.0c01895.
Hastings, Ashley M., Ray, Debmalya, Jeong, WooSeok, Gagliardi, Laura, Farha, Omar K., & Hixon, Amy E. Advancement of Actinide Metal–Organic Framework Chemistry via Synthesis of Pu-UiO-66. United States. https://doi.org/10.1021/jacs.0c01895
Hastings, Ashley M., Ray, Debmalya, Jeong, WooSeok, Gagliardi, Laura, Farha, Omar K., and Hixon, Amy E. Sun .
"Advancement of Actinide Metal–Organic Framework Chemistry via Synthesis of Pu-UiO-66". United States. https://doi.org/10.1021/jacs.0c01895. https://www.osti.gov/servlets/purl/1623393.
@article{osti_1623393,
title = {Advancement of Actinide Metal–Organic Framework Chemistry via Synthesis of Pu-UiO-66},
author = {Hastings, Ashley M. and Ray, Debmalya and Jeong, WooSeok and Gagliardi, Laura and Farha, Omar K. and Hixon, Amy E.},
abstractNote = {We report the synthesis and characterization of the first plutonium metal–organic framework (MOF). Pu-UiO-66 expands the established UiO-66 series, which includes transition metal, lanthanide, and early actinide elements in the hexanuclear nodes. The thermal stability and porosity of Pu-UiO-66 were experimentally determined, and multifaceted computational methods were used to corroborate experimental values, examine inherent defects in the framework, decipher spectroscopic signatures, and elucidate the electronic structure. The crystallization of a plutonium chain side product provides direct evidence of the competition that occurs between modulator and linker in MOF syntheses. Ultimately, the synthesis of Pu-UiO-66 demonstrates adept control of Pu(IV) coordination under hydrolysis-prone conditions, provides an opportunity to extend trends across isostructural UiO-66 frameworks, and serves as the foundation for future plutonium MOF chemistry.},
doi = {10.1021/jacs.0c01895},
journal = {Journal of the American Chemical Society},
number = 20,
volume = 142,
place = {United States},
year = {Sun Apr 26 00:00:00 EDT 2020},
month = {Sun Apr 26 00:00:00 EDT 2020}
}
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