Synthesis and Characterization of Pyridine Dipyrrolide Uranyl Complexes
Abstract
The first actinide complexes of the pyridine dipyrrolide (PDP) ligand class, (MesPDPPh)UO2(THF) and (Cl2PhPDPPh)UO2(THF), are reported as the UVI uranyl adducts of the bulky aryl substituted pincers (MesPDPPh)2– and (Cl2PhPDPPh)2– (derived from 2,6-bis(5-(2,4,6-trimethylphenyl)-3- phenyl-1H-pyrrol-2-yl)pyridine (H2 MesPDPPh, Mes = 2,4,6-trimethylphenyl), and 2,6-bis(5-(2,6-dichlorophenyl)-3-phenyl-1H-pyrrol- 2-yl)pyridine (H2 Cl2PhPDPPh, Cl2 Ph = 2,6-dichlorophenyl), respectively). Following the in situ deprotonation of the proligand with lithium hexamethyldisilazide to generate the corresponding dilithium salts (e.g., Li2 ArPDPPh, Ar = Mes of Cl2Ph), salt metathesis with [UO2Cl2(THF)2]2 afforded both compounds in moderate yields. The characterization of each species has been undertaken by a combination of solid- and solution-state methods, including combustion analysis, infrared, electronic absorption, and NMR spectroscopies. In both complexes, single-crystal X-ray diffraction has revealed a distorted octahedral geometry in the solid state, enforced by the bite angle of the rigid meridional (ArPDPPh)2– pincer ligand. The electrochemical analysis of both compounds by cyclic voltammetry in tetrahydrofuran (THF) reveals rich redox profiles, including events assigned as UVI/UV redox couples. A time-dependent density functional theory study has been performed on (MesPDPPh)UO2(THF) and provides insight into the nature of the transitions that comprise its electronic absorption spectrum.
- Authors:
-
[1];
[2];
[1];
[2];
[1]
- Department of Chemistry, University of Rochester, Rochester, New York 14627, United States
- C. Eugene Bennett Department of Chemistry, West Virginia University, Morgantown, West Virginia 26506, United States
- Publication Date:
- Research Org.:
- Univ. of Rochester, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1863118
- Alternate Identifier(s):
- OSTI ID: 1864661
- Grant/Contract Number:
- SC0020436
- Resource Type:
- Published Article
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Name: Inorganic Chemistry Journal Volume: 61 Journal Issue: 16; Journal ID: ISSN 0020-1669
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ligands; Redox reactions; Pyridines; Aromatic compounds; Cations
Citation Formats
Hakey, Brett M., Leary, Dylan C., Lopez, Lauren M., Valerio, Leyla R., Brennessel, William W., Milsmann, Carsten, and Matson, Ellen M. Synthesis and Characterization of Pyridine Dipyrrolide Uranyl Complexes. United States: N. p., 2022.
Web. doi:10.1021/acs.inorgchem.2c00348.
Hakey, Brett M., Leary, Dylan C., Lopez, Lauren M., Valerio, Leyla R., Brennessel, William W., Milsmann, Carsten, & Matson, Ellen M. Synthesis and Characterization of Pyridine Dipyrrolide Uranyl Complexes. United States. https://doi.org/10.1021/acs.inorgchem.2c00348
Hakey, Brett M., Leary, Dylan C., Lopez, Lauren M., Valerio, Leyla R., Brennessel, William W., Milsmann, Carsten, and Matson, Ellen M. Thu .
"Synthesis and Characterization of Pyridine Dipyrrolide Uranyl Complexes". United States. https://doi.org/10.1021/acs.inorgchem.2c00348.
@article{osti_1863118,
title = {Synthesis and Characterization of Pyridine Dipyrrolide Uranyl Complexes},
author = {Hakey, Brett M. and Leary, Dylan C. and Lopez, Lauren M. and Valerio, Leyla R. and Brennessel, William W. and Milsmann, Carsten and Matson, Ellen M.},
abstractNote = {The first actinide complexes of the pyridine dipyrrolide (PDP) ligand class, (MesPDPPh)UO2(THF) and (Cl2PhPDPPh)UO2(THF), are reported as the UVI uranyl adducts of the bulky aryl substituted pincers (MesPDPPh)2– and (Cl2PhPDPPh)2– (derived from 2,6-bis(5-(2,4,6-trimethylphenyl)-3- phenyl-1H-pyrrol-2-yl)pyridine (H2 MesPDPPh, Mes = 2,4,6-trimethylphenyl), and 2,6-bis(5-(2,6-dichlorophenyl)-3-phenyl-1H-pyrrol- 2-yl)pyridine (H2 Cl2PhPDPPh, Cl2 Ph = 2,6-dichlorophenyl), respectively). Following the in situ deprotonation of the proligand with lithium hexamethyldisilazide to generate the corresponding dilithium salts (e.g., Li2 ArPDPPh, Ar = Mes of Cl2Ph), salt metathesis with [UO2Cl2(THF)2]2 afforded both compounds in moderate yields. The characterization of each species has been undertaken by a combination of solid- and solution-state methods, including combustion analysis, infrared, electronic absorption, and NMR spectroscopies. In both complexes, single-crystal X-ray diffraction has revealed a distorted octahedral geometry in the solid state, enforced by the bite angle of the rigid meridional (ArPDPPh)2– pincer ligand. The electrochemical analysis of both compounds by cyclic voltammetry in tetrahydrofuran (THF) reveals rich redox profiles, including events assigned as UVI/UV redox couples. A time-dependent density functional theory study has been performed on (MesPDPPh)UO2(THF) and provides insight into the nature of the transitions that comprise its electronic absorption spectrum.},
doi = {10.1021/acs.inorgchem.2c00348},
journal = {Inorganic Chemistry},
number = 16,
volume = 61,
place = {United States},
year = {Thu Apr 14 00:00:00 EDT 2022},
month = {Thu Apr 14 00:00:00 EDT 2022}
}
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