Laser-Induced Thermal Decomposition of Uranium Coordination Compounds with Non-oxidic Ligands to Produce Nitride and Carbide Materials

Ferrier, Maryline G.; Childs, Bradley C.; Silva, Chinthaka M.; Greenough, Michelle M.; Moore, Emily E.; Erickson, Karla A.; Monreal, Marisa J.; Colla, Christopher A.; Marple, Maxwell T.; Winston, Logan D.; Burks, Janae N.; Martin, Aiden A.; Jeffries, Jason R.; Holliday, Kiel S.

doi:10.1021/acs.inorgchem.3c03591

Title: Laser-Induced Thermal Decomposition of Uranium Coordination Compounds with Non-oxidic Ligands to Produce Nitride and Carbide Materials

Journal Article · Wed Jan 17 00:00:00 UTC 2024 · Inorganic Chemistry

DOI: https://doi.org/10.1021/acs.inorgchem.3c03591 · OSTI ID:2520590

^[1]; Childs, Bradley C. ^[1];

^[1]; Greenough, Michelle M. ^[1]; Moore, Emily E. ^[1];

^[2]; Monreal, Marisa J. ^[2];

^[1];

^[1]; Winston, Logan D. ^[1]; Burks, Janae N. ^[3];

^[1]; Jeffries, Jason R. ^[1]; Holliday, Kiel S. ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Spelman College, Atlanta, GA (United States)

The production of ceramics from uranium coordination compounds can be achieved through thermal processing if an excess amount of the desired atoms (i.e., C or N), or reactive gaseous products (e.g., methane or nitrogen oxide) is made available to the reactive uranium metal core via decomposition/fragmentation of the surrounding ligand groups. Here, computational thermodynamic approaches were utilized to identify the temperatures necessary to produce uranium metal from some starting compounds—UI₄(TMEDA)₂, UCl₄(TMEDA)₂, UCl₃(pyridine)_x, and UI₃(pyridine)₄. Experimentally, precursors were irradiated by a laser under various gaseous environments (argon, nitrogen, and methane) creating extreme reaction conditions (i.e., fast heating, high temperature profile >2000 °C, and rapid cooling). Despite the fast dynamics associated with laser irradiation, the central uranium atom reacted with the thermal decomposition products of the ligands yielding uranium ceramics. Residual gas analysis identified vaporized products from the laser irradiation, and the final ceramic products were characterized by powder X-ray diffraction. The composition of the uranium precursor as well as the gaseous environment had a direct impact on the production of the final phases.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2520590

Report Number(s):: LLNL--JRNL-852424; 1079400

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 4 Vol. 63; 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
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uranium

Title: Laser-Induced Thermal Decomposition of Uranium Coordination Compounds with Non-oxidic Ligands to Produce Nitride and Carbide Materials

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