From Thorium to Plutonium: Trends in Actinide(IV) Chloride Structural Chemistry

Wacker, Jennifer N.; Han, Sae Young; Murray, Aphra V.; Vanagas, Nicole A.; Bertke, Jeffery A.; Sperling, Joseph M.; Surbella, III, Robert G.; Knope, Karah E.

doi:10.1021/acs.inorgchem.9b01279

Title: From Thorium to Plutonium: Trends in Actinide(IV) Chloride Structural Chemistry

Journal Article · 12 June 2019 · Inorganic Chemistry

DOI: https://doi.org/10.1021/acs.inorgchem.9b01279 · OSTI ID:1572959

Wacker, Jennifer N. ^[1]; Han, Sae Young ^[1]; Murray, Aphra V. ^[1]; Vanagas, Nicole A. ^[1];

^[1]; Sperling, Joseph M. ^[2]; Surbella, III, Robert G. ^[3];

^[1]

Georgetown Univ., Washington, D.C. (United States)
Florida State Univ., Tallahassee, FL (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

A series of eighteen actinide (IV) compounds were synthesized from acidic aqueous media containing thorium, uranium, or plutonium. The metal cation adopts a variety of different structural units with the general formula [An(H₂O)_xCl_y]^4-y (x=4-7, y=2-4) or AnCl₆^2- charge balanced by protonated nitrogen-containing heterocycles. Compound identities were classified by single crystal X-ray diffraction and subsequently characterized by Raman, IR, and optical absorption spectroscopies. Discrepancies across the early actinides were observed in this family of An(IV)-chlorides, with Th adopting exclusively Th-aquo-chloro species, Pu forming only PuCl₆^2-, and U residing somewhere in between, crystallizing both as U-aquo-chloro and UCl₆^2- monomeric units. Reports of An-H₂O-Cl species are largely absent from tetravalent An solid state discussions despite their identification in chloride solutions. Here, the isolation of unique An(IV)-chlorides may be attributed to nonbonding interactions provided by outer coordination sphere counter-ions that could play a role in stabilizing these structural units. Differences in the structural chemistry of Th, U, and Pu also demonstrate a break in the series despite their common oxidation state and nearly identical synthetic procedures.

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

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1572959

Report Number(s):: PNNL-SA--143237

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 16 Vol. 58; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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