Synthesis and Characterization of Isostructural Th(IV) and U(IV) Pyridine Dipyrrolide Complexes

Valerio, Leyla R.; Hakey, Brett M.; Leary, Dylan C.; Stockdale, Erin; Brennessel, William W.; Milsmann, Carsten; Matson, Ellen M.

doi:10.1021/acs.inorgchem.3c04391

Title: Synthesis and Characterization of Isostructural Th(IV) and U(IV) Pyridine Dipyrrolide Complexes

Journal Article · 20 February 2024 · Inorganic Chemistry

DOI: https://doi.org/10.1021/acs.inorgchem.3c04391 · OSTI ID:2309778

Valerio, Leyla R. ^[1];

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University of Rochester, NY (United States)
West Virginia University, Morgantown, WV (United States)

A series of pyridine dipyrrolide actinide(IV) complexes, (^MesPDP^Ph)AnCl₂(THF) and An(^MesPDP^Ph)₂ (An = U, Th, where (^MesPDP^Ph) is the doubly deprotonated form of 2,6- bis(5-(2,4,6-trimethylphenyl)-3-phenyl-1H-pyrrol-2-yl)pyridine), have been prepared. Characterization of all four complexes has been performed through a combination of solid- and solution-state methods, including elemental analysis, single crystal X-ray diffraction, and electronic absorption and nuclear magnetic resonance spectroscopies. Collectively, these data confirm the formation of the mono- and bis-ligated species. Time-dependent density functional theory has been performed on all four An(IV) complexes, providing insight into the nature of electronic transitions that are observed in the electronic absorption spectra of these compounds. Room temperature, solution-state luminescence of the actinide complexes is presented. Both Th(IV) derivatives exhibit strong photoluminescence; in contrast, the U(IV) species are nonemissive.

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Research Organization:: Univ. of Rochester, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0020436

OSTI ID:: 2309778

Alternate ID(s):: OSTI ID: 2367456

Journal Information:: Inorganic Chemistry, Vol. 63, Issue 21; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Aromatic compounds
Electronic absorption
Hydrocarbons
Ligands
Uranium

CCDC 2287252: Experimental Crystal Structure Determination R., Valerio, Leyla; M., Hakey, Brett; C., Leary, Dylan https://doi.org/10.5517/ccdc.csd.cc2gs2bp The current record is supplemented by this dataset	dataset	January 2024
CCDC 2287253: Experimental Crystal Structure Determination R., Valerio, Leyla; M., Hakey, Brett; C., Leary, Dylan https://doi.org/10.5517/ccdc.csd.cc2gs2cq The current record is supplemented by this dataset	dataset	January 2024
CCDC 2287254: Experimental Crystal Structure Determination R., Valerio, Leyla; M., Hakey, Brett; C., Leary, Dylan https://doi.org/10.5517/ccdc.csd.cc2gs2dr The current record is supplemented by this dataset	dataset	January 2024
CCDC 2287255: Experimental Crystal Structure Determination R., Valerio, Leyla; M., Hakey, Brett; C., Leary, Dylan https://doi.org/10.5517/ccdc.csd.cc2gs2fs The current record is supplemented by this dataset	dataset	January 2024
CCDC 2287256: Experimental Crystal Structure Determination R., Valerio, Leyla; M., Hakey, Brett; C., Leary, Dylan https://doi.org/10.5517/ccdc.csd.cc2gs2gt The current record is supplemented by this dataset	dataset	January 2024
CCDC 2287257: Experimental Crystal Structure Determination R., Valerio, Leyla; M., Hakey, Brett; C., Leary, Dylan https://doi.org/10.5517/ccdc.csd.cc2gs2hv The current record is supplemented by this dataset	dataset	January 2024

Title: Synthesis and Characterization of Isostructural Th(IV) and U(IV) Pyridine Dipyrrolide Complexes

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