Influencing Bonding Interactions of the Neptunyl (V, VI) Cations with Electron-donating and -withdrawing Groups

Augustine, Logan J.; Kasper, Joseph Michael; Forbes, Tori Z.; Mason, Sara E.; Batista, Enrique Ricardo; Yang, Ping

doi:10.1021/acs.inorgchem.2c04538

Influencing Bonding Interactions of the Neptunyl (V, VI) Cations with Electron-donating and -withdrawing Groups

Journal Article · Fri Mar 31 00:00:00 EDT 2023 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.2c04538· OSTI ID:1969244

Augustine, Logan J. ^[1]; ^[1]; Forbes, Tori Z. ^[2]; Mason, Sara E. ^[2]; ^[1]; ^[1]

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Theoretical Division
University of Iowa, Iowa City, IA (United States)

Neptunium makes up the largest percentage of minor actinides found in spent nuclear fuel, yet separations of this element have proven difficult due to its rich redox chemistry. Developing new reprocessing techniques should rely on understanding how to control the Np oxidation state and its interactions with different ligands. Designing new ligands for separations requires understanding how to properly tune a system toward a desired trait through functionalization. Emerging technologies for minor actinide separations focus on ligands containing carboxylate or pyridine functional groups, which are desirable due to their high degree of functionalization. So we use DFT calculations to study the interactions of carboxylate and polypyridine ligands with the neptunyl cation [Np(V/VI)O2]^+/2+. A systematic study is performed by varying the electronic properties of the carboxylate and polypyridine ligands through the inclusion of different electron-withdrawing and electron-donating R groups. We focus on how these groups can affect geometric properties, electronic structure, and bonding characterization as a function of the metal oxidation state and ligand character and discuss how these factors can play a role in neptunium ligand design principles.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS)

Grant/Contract Number:: 89233218CNA000001; SC0014664

OSTI ID:: 1969244

Report Number(s):: LA-UR-22-31735

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 15 Vol. 62; ISSN 0020-1669; ISSN 1520-510X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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