Uranyl Peroxide Capsule Self-assembly in Slow Motion Ana Arteaga,1 Lei Zhang,2 Sarah Hickam,2 Mateusz Dembowski,2,3 Peter C. Burns 2 and May Nyman1*
Abstract
Abstract Uranyl‐peroxide capsules are the newest family of polyoxometalates. Although discovered 13 years previously with over 70 topologies reported, there is a lack in the fundamental understanding of assembly mechanisms, particularly the role of the alkali counterions. Herein, the reaction pathway and assembly of uranyl peroxide capsules is reported by tracking the conversion from K + uranyl triperoxide monomer to the K + uranyl‐peroxide U 28 capsule by means of small‐angle X‐ray scattering and Raman spectroscopy. For the first time, the K + uranyl‐peroxide pentamer face is isolated and structurally characterized, giving credence to the long‐held belief that these geometric faces serve as building blocks to the fully formed capsules. Once isolated and re‐dissolved, the pentamer face undergoes rapid conversion to capsule forms, underlining its high reactivity that challenges its isolation. Calorimetric measurements of the studied species confirms the pentamer lies on the energy landscape between the monomer and capsule.
- Authors:
-
- Oregon State Univ., Corvallis, OR (United States). Dept. of Chemistry
- Univ. of Notre Dame, Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Sciences
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA); University of Notre Dame, IN (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1502931
- Alternate Identifier(s):
- OSTI ID: 1503928
- Grant/Contract Number:
- NA0003763
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry - A European Journal
- Additional Journal Information:
- Journal Volume: 25; Journal Issue: 24; Journal ID: ISSN 0947-6539
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; uranyl; Polyoxometalates; X-ray scattering; Calorimetry; crystal structure
Citation Formats
Arteaga, Ana, Zhang, Lei, Hickam, Sarah, Dembowski, Mateusz, Burns, Peter, and Nyman, May. Uranyl Peroxide Capsule Self-assembly in Slow Motion Ana Arteaga,1 Lei Zhang,2 Sarah Hickam,2 Mateusz Dembowski,2,3 Peter C. Burns 2 and May Nyman1*. United States: N. p., 2019.
Web. doi:10.1002/chem.201806227.
Arteaga, Ana, Zhang, Lei, Hickam, Sarah, Dembowski, Mateusz, Burns, Peter, & Nyman, May. Uranyl Peroxide Capsule Self-assembly in Slow Motion Ana Arteaga,1 Lei Zhang,2 Sarah Hickam,2 Mateusz Dembowski,2,3 Peter C. Burns 2 and May Nyman1*. United States. https://doi.org/10.1002/chem.201806227
Arteaga, Ana, Zhang, Lei, Hickam, Sarah, Dembowski, Mateusz, Burns, Peter, and Nyman, May. Wed .
"Uranyl Peroxide Capsule Self-assembly in Slow Motion Ana Arteaga,1 Lei Zhang,2 Sarah Hickam,2 Mateusz Dembowski,2,3 Peter C. Burns 2 and May Nyman1*". United States. https://doi.org/10.1002/chem.201806227. https://www.osti.gov/servlets/purl/1502931.
@article{osti_1502931,
title = {Uranyl Peroxide Capsule Self-assembly in Slow Motion Ana Arteaga,1 Lei Zhang,2 Sarah Hickam,2 Mateusz Dembowski,2,3 Peter C. Burns 2 and May Nyman1*},
author = {Arteaga, Ana and Zhang, Lei and Hickam, Sarah and Dembowski, Mateusz and Burns, Peter and Nyman, May},
abstractNote = {Abstract Uranyl‐peroxide capsules are the newest family of polyoxometalates. Although discovered 13 years previously with over 70 topologies reported, there is a lack in the fundamental understanding of assembly mechanisms, particularly the role of the alkali counterions. Herein, the reaction pathway and assembly of uranyl peroxide capsules is reported by tracking the conversion from K + uranyl triperoxide monomer to the K + uranyl‐peroxide U 28 capsule by means of small‐angle X‐ray scattering and Raman spectroscopy. For the first time, the K + uranyl‐peroxide pentamer face is isolated and structurally characterized, giving credence to the long‐held belief that these geometric faces serve as building blocks to the fully formed capsules. Once isolated and re‐dissolved, the pentamer face undergoes rapid conversion to capsule forms, underlining its high reactivity that challenges its isolation. Calorimetric measurements of the studied species confirms the pentamer lies on the energy landscape between the monomer and capsule.},
doi = {10.1002/chem.201806227},
journal = {Chemistry - A European Journal},
number = 24,
volume = 25,
place = {United States},
year = {Wed Mar 06 00:00:00 EST 2019},
month = {Wed Mar 06 00:00:00 EST 2019}
}
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