Probing a variation of the inverse-trans-influence in americium and lanthanide tribromide tris(tricyclohexylphosphine oxide) complexes
Abstract
The synthesis, characterization, and theoretical analysis of meridional americium tribromide tris(tricyclohexylphosphine oxide), mer-AmBr3(OPcy3)3, has been achieved and is compared with its early lanthanide (La to Nd) analogs. The data show that homo trans ligands display significantly shorter bonds than the cis or hetero trans ligands. This is particularly pronounced in the americium compound. DFT along with multiconfigurational CASSCF calculations show that the contraction of the bonds relates qualitatively with overall covalency, i.e. americium shows the most covalent interactions compared to lanthanides. However, the involvement of the 5p and 6p shells in bonding follows a different order, namely cerium > neodymium ~ americium. This study provides further insight into the mechanisms by which ITI operates in low-valent f-block complexes.
- Authors:
-
- Department of Chemistry and Biochemistry, Florida State University, Tallahassee, USA
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST); Florida State Univ., Tallahassee, FL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1599242
- Alternate Identifier(s):
- OSTI ID: 1767704
- Grant/Contract Number:
- FG02-13ER16414; SC0010677; SC0016568
- Resource Type:
- Published Article
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Name: Chemical Science Journal Volume: 11 Journal Issue: 10; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nuclear; defects; mechanical behavior; corrosion; charge transport; superconductivity; magnetism and spin physics; separations; geophysics/geochemistry; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (predictive); synthesis (scalable processing)
Citation Formats
Windorff, Cory J., Celis-Barros, Cristian, Sperling, Joseph M., McKinnon, Noah C., and Albrecht-Schmitt, Thomas E. Probing a variation of the inverse-trans-influence in americium and lanthanide tribromide tris(tricyclohexylphosphine oxide) complexes. United Kingdom: N. p., 2020.
Web. doi:10.1039/C9SC05268B.
Windorff, Cory J., Celis-Barros, Cristian, Sperling, Joseph M., McKinnon, Noah C., & Albrecht-Schmitt, Thomas E. Probing a variation of the inverse-trans-influence in americium and lanthanide tribromide tris(tricyclohexylphosphine oxide) complexes. United Kingdom. https://doi.org/10.1039/C9SC05268B
Windorff, Cory J., Celis-Barros, Cristian, Sperling, Joseph M., McKinnon, Noah C., and Albrecht-Schmitt, Thomas E. Wed .
"Probing a variation of the inverse-trans-influence in americium and lanthanide tribromide tris(tricyclohexylphosphine oxide) complexes". United Kingdom. https://doi.org/10.1039/C9SC05268B.
@article{osti_1599242,
title = {Probing a variation of the inverse-trans-influence in americium and lanthanide tribromide tris(tricyclohexylphosphine oxide) complexes},
author = {Windorff, Cory J. and Celis-Barros, Cristian and Sperling, Joseph M. and McKinnon, Noah C. and Albrecht-Schmitt, Thomas E.},
abstractNote = {The synthesis, characterization, and theoretical analysis of meridional americium tribromide tris(tricyclohexylphosphine oxide), mer-AmBr3(OPcy3)3, has been achieved and is compared with its early lanthanide (La to Nd) analogs. The data show that homo trans ligands display significantly shorter bonds than the cis or hetero trans ligands. This is particularly pronounced in the americium compound. DFT along with multiconfigurational CASSCF calculations show that the contraction of the bonds relates qualitatively with overall covalency, i.e. americium shows the most covalent interactions compared to lanthanides. However, the involvement of the 5p and 6p shells in bonding follows a different order, namely cerium > neodymium ~ americium. This study provides further insight into the mechanisms by which ITI operates in low-valent f-block complexes.},
doi = {10.1039/C9SC05268B},
journal = {Chemical Science},
number = 10,
volume = 11,
place = {United Kingdom},
year = {Wed Mar 11 00:00:00 EDT 2020},
month = {Wed Mar 11 00:00:00 EDT 2020}
}
https://doi.org/10.1039/C9SC05268B
Web of Science
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