Plutonium Hybrid Materials: A Platform to Explore Assembly and Metal–Ligand Bonding

Surbella III, Robert G.; Ducati, Lucas C.; Schofield, Mark H.; McNamara, Bruce K.; Pellegrini, Kristi L.; Corbey, Jordan F.; Schwantes, Jon M.; Autschbach, Jochen; Cahill, Christopher L.

doi:10.1021/acs.inorgchem.2c02084

Title: Plutonium Hybrid Materials: A Platform to Explore Assembly and Metal–Ligand Bonding

Journal Article · Fri Oct 28 00:00:00 EDT 2022 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.2c02084· OSTI ID:1957814

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Univ. of Sao Paulo (Brazil)
George Washington Univ., Washington, DC (United States)
State Univ. of New York (SUNY), Buffalo, NY (United States)

In this work, we report the synthesis of five new hybrid materials containing the [PuCl₆]^2- anion and charge balancing, non-covalent interaction donating 4-X-pyridinium (X = H, Cl, Br, I) cations. Single crystals of the title compounds were grown and harvested from acidic, chloride-rich, aqueous media and their structures were determined via X-ray diffraction. Compounds 1-4, (4XPyH)₂[PuCl₆] and 5, (4IPyH)₄[PuCl₆] · 2Cl, exhibit two distinct sheet-like structure types. Structurally relevant non-covalent interactions were tabulated from crystallographic data and verified computationally using electrostatic surface potential maps and the quantum theory of atoms in molecules (QTAIM) approach. The strength of the hydrogen and halogen bonds was quantified using Kohn-Sham density functional theory and a hierarchy of acceptor-donor pairings established. In turn, the PuIV-Cl bonds were studied using the QTAIM and natural localized molecular orbital (NLMO) approaches to delineate the underlying bond mechanism and hybrid atomic orbital contributions therein. Energy decomposition (ED) and natural ED analyses were also explored to probe the bond mechanism and, more broadly, explore the efficacy of these techniques in studying these anionic systems. The results of the PuIV-Cl bond analyses were compared across composition via analogous treatments of previously reported [PuO₂Cl₄]^2- and [PuCl₃(H₂O)₅] molecular units. In summary, our study indicates that the Pu-Cl bonds are predominately ionic, yet exhibit small varying degrees of covalent character that increase from [PuCl₃(H₂O)₅], [PuO₂Cl₄]^2-, to [PuCl₆]^2-, while the participation of the Pu based s/d and f orbitals concurrently decrease and increase, respectively.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; São Paulo Research Foundation (FAPESP)

Grant/Contract Number:: AC05-76RL01830; FG02-05ER15736; SC0001136; 2017/17750-3; 2020/10246-0; 306844/2020-6

OSTI ID:: 1957814

Report Number(s):: PNNL-SA-172003

Journal Information:: Inorganic Chemistry, Vol. 61, Issue 45; 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
hybrid materials
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transuranic
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CCDC 2179361: Experimental Crystal Structure Determination G., Surbella, Robert; C., Ducati, Lucas; H., Schofield, Mark https://doi.org/10.5517/ccdc.csd.cc2c4sz9 The current record is supplemented by this dataset	dataset	January 2022
CCDC 2179362: Experimental Crystal Structure Determination G., Surbella, Robert; C., Ducati, Lucas; H., Schofield, Mark https://doi.org/10.5517/ccdc.csd.cc2c4t0c The current record is supplemented by this dataset	dataset	January 2022
CCDC 2179363: Experimental Crystal Structure Determination G., Surbella, Robert; C., Ducati, Lucas; H., Schofield, Mark https://doi.org/10.5517/ccdc.csd.cc2c4t1d The current record is supplemented by this dataset	dataset	January 2022
CCDC 2179364: Experimental Crystal Structure Determination G., Surbella, Robert; C., Ducati, Lucas; H., Schofield, Mark https://doi.org/10.5517/ccdc.csd.cc2c4t2f The current record is supplemented by this dataset	dataset	January 2022
CCDC 2179365: Experimental Crystal Structure Determination G., Surbella, Robert; C., Ducati, Lucas; H., Schofield, Mark https://doi.org/10.5517/ccdc.csd.cc2c4t3g The current record is supplemented by this dataset	dataset	January 2022
CCDC 2179391: Experimental Crystal Structure Determination G., Surbella, Robert; C., Ducati, Lucas; H., Schofield, Mark https://doi.org/10.5517/ccdc.csd.cc2c4ty9 The current record is supplemented by this dataset	dataset	January 2022
CCDC 2179392: Experimental Crystal Structure Determination G., Surbella, Robert; C., Ducati, Lucas; H., Schofield, Mark https://doi.org/10.5517/ccdc.csd.cc2c4tzb The current record is supplemented by this dataset	dataset	January 2022
CCDC 2179393: Experimental Crystal Structure Determination G., Surbella, Robert; C., Ducati, Lucas; H., Schofield, Mark https://doi.org/10.5517/ccdc.csd.cc2c4v0d The current record is supplemented by this dataset	dataset	January 2022
CCDC 2179394: Experimental Crystal Structure Determination G., Surbella, Robert; C., Ducati, Lucas; H., Schofield, Mark https://doi.org/10.5517/ccdc.csd.cc2c4v1f The current record is supplemented by this dataset	dataset	January 2022
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Title: Plutonium Hybrid Materials: A Platform to Explore Assembly and Metal–Ligand Bonding

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