Heat capacity, entropy, formation energy and spin-fluctuation behavior of U3Si5 from 2.4 to 397.4 K

Baker, Jason Lee; White, Joshua Taylor; Chen, Aiping; Ulrich, Tasheima Lixona; Roback, Robert Clifford; Xu, Hongwu

doi:10.1016/j.jnucmat.2021.153282

Title: Heat capacity, entropy, formation energy and spin-fluctuation behavior of U₃Si₅ from 2.4 to 397.4 K

Journal Article · Sat Sep 04 00:00:00 EDT 2021 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2021.153282· OSTI ID:1866968

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Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

U-Si intermetallic compounds are of considerable interest for their applications as accident-tolerant nuclear fuels. Here we present low-temperature heat capacity (LTHC) measurements of one of the U-Si phases, U₃Si₅, using a Quantum Design Physical Properties Measurement System (PPMS) from 2.4 to 397.4 K. We observed an upturn in C_p/T (T) below 10 K and have attributed this behavior to potential spin-fluctuations (SF) with an SF temperature (T_sf) of 27 K. An enhancement of LTHC was also observed, as manifested by a large electronic heat capacity coefficient (γ_el) of 342.9 mJ/mol•K₂. From the heat capacity data, the following thermodynamic parameters were determined: the characteristic Debye temperature (θ_D) over the temperature range 30 – 397 K is 177 ± 2 K, and the standard entropy ($$Δ^{298.15}_0$$$$S^o$) is 283.3 ± 5.7 J•mol^-1•K^-1 (equivalent to 35.4 ± 0.7 J•mol^-1•atom^-1•K^-1). Combined with our previously measured formation enthalpy ($$Δ_fH^°_{el}$$) of U₃Si₅, the Gibbs free energy of formation of U₃Si₅ from the elements ($$Δ_fG^°_{el}$$) was determined to be –45.2 ± 9.0 kJ•mol^-1•atom^-1.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1866968

Alternate ID(s):: OSTI ID: 1820087

Report Number(s):: LA-UR-21-30172; LA-UR-21-24852; TRN: US2306612

Journal Information:: Journal of Nuclear Materials, Vol. 557; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Heat capacity, entropy, formation energy and spin-fluctuation behavior of U3Si5 from 2.4 to 397.4 K

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