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.
| Original language | English |
|---|---|
| Article number | 201 |
| Journal | Nature Communications |
| Volume | 13 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2022 |
| Externally published | Yes |
Funding
We would like to thank the Department of Energy Office of Science, Basic Energy Sciences, DOE-BES Heavy Elements Chemistry for funding under award DE-FG02-13ER16414 (T.E.A.-S.). A special thank you goes to our radiation safety officers, Ashley Gray and Jason Johnson, as well as Oak Ridge National Laboratory for supplying the isotopes used in this study. We would also like to extend our gratitude to the William J. Evans group at the University of California Irvine for supplying Cp′ used in reaction optimization.