Cyclopentadienyl coordination induces unexpected ionic Am-N bonding in an americium bipyridyl complex
Abstract
Variations in bonding between trivalent lanthanides and actinides is critical for reprocessing spent nuclear fuel. The ability to tune bonding and the coordination environment in these trivalent systems is a key factor in identifying a solution for separating lanthanides and actinides. Coordination of 4,4'-bipyridine (4,4'-bpy) and trimethylsilylcyclopentadienide (Cp') to americium introduces unexpectedly ionic Am-N bonding character and unique spectroscopic properties. Here we report the structural characterization of (Cp'3Am)2(μ -4,4'-bpy) and its lanthanide analogue, (Cp'3Nd)2(μ - 4,4'-bpy), by single-crystal X-ray diffraction. Spectroscopic techniques in both solid and solution phase are performed in conjunction with theoretical calculations to probe the effects the unique coordination environment has on the electronic structure.
- Authors:
-
[1];
[1];
[1];
[1];
[1];
[2];
[3];
[1]
- Florida State University, Tallahassee, FL (United States)
- National High Magnetic Field Laboratory, Tallahassee, FL (United States)
- Florida State University, Tallahassee, FL (United States); New Mexico State University, Las Cruces, NM (United States)
- Publication Date:
- Research Org.:
- Florida State Univ., Tallahassee, FL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1904479
- Grant/Contract Number:
- SC0010677; FG02-13ER16414
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; inorganic chemistry; nuclear chemistry; organometallic chemistry
Citation Formats
Long, Brian N., Beltrán-Leiva, María J., Celis-Barros, Cristian, Sperling, Joseph M., Poe, Todd N., Baumbach, Ryan E., Windorff, Cory J., and Albrecht-Schönzart, Thomas E. Cyclopentadienyl coordination induces unexpected ionic Am-N bonding in an americium bipyridyl complex. United States: N. p., 2022.
Web. doi:10.1038/s41467-021-27821-4.
Long, Brian N., Beltrán-Leiva, María J., Celis-Barros, Cristian, Sperling, Joseph M., Poe, Todd N., Baumbach, Ryan E., Windorff, Cory J., & Albrecht-Schönzart, Thomas E. Cyclopentadienyl coordination induces unexpected ionic Am-N bonding in an americium bipyridyl complex. United States. https://doi.org/10.1038/s41467-021-27821-4
Long, Brian N., Beltrán-Leiva, María J., Celis-Barros, Cristian, Sperling, Joseph M., Poe, Todd N., Baumbach, Ryan E., Windorff, Cory J., and Albrecht-Schönzart, Thomas E. Tue .
"Cyclopentadienyl coordination induces unexpected ionic Am-N bonding in an americium bipyridyl complex". United States. https://doi.org/10.1038/s41467-021-27821-4. https://www.osti.gov/servlets/purl/1904479.
@article{osti_1904479,
title = {Cyclopentadienyl coordination induces unexpected ionic Am-N bonding in an americium bipyridyl complex},
author = {Long, Brian N. and Beltrán-Leiva, María J. and Celis-Barros, Cristian and Sperling, Joseph M. and Poe, Todd N. and Baumbach, Ryan E. and Windorff, Cory J. and Albrecht-Schönzart, Thomas E.},
abstractNote = {Variations in bonding between trivalent lanthanides and actinides is critical for reprocessing spent nuclear fuel. The ability to tune bonding and the coordination environment in these trivalent systems is a key factor in identifying a solution for separating lanthanides and actinides. Coordination of 4,4'-bipyridine (4,4'-bpy) and trimethylsilylcyclopentadienide (Cp') to americium introduces unexpectedly ionic Am-N bonding character and unique spectroscopic properties. Here we report the structural characterization of (Cp'3Am)2(μ -4,4'-bpy) and its lanthanide analogue, (Cp'3Nd)2(μ - 4,4'-bpy), by single-crystal X-ray diffraction. Spectroscopic techniques in both solid and solution phase are performed in conjunction with theoretical calculations to probe the effects the unique coordination environment has on the electronic structure.},
doi = {10.1038/s41467-021-27821-4},
journal = {Nature Communications},
number = 1,
volume = 13,
place = {United States},
year = {Tue Jan 11 00:00:00 EST 2022},
month = {Tue Jan 11 00:00:00 EST 2022}
}
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