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

•Heat capacity data of U3Si5 were obtained using a Quantum Design Physical Properties Measurement System (PPMS) from 2.4 to 397.4 K.•An upturn characteristic of spin-fluctuations in Cp/T (T) was observed below 10 K.•The Gibbs free energy of formation of U3Si5 from the elements was determined to be –...

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Veröffentlicht in:Journal of nuclear materials 2021-12, Vol.557, p.153282, Article 153282
Hauptverfasser: Baker, Jason L., White, Josh T., Chen, Aiping, Ulrich, Tasheima, Roback, Robert R., Xu, Hongwu
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Sprache:eng
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Zusammenfassung:•Heat capacity data of U3Si5 were obtained using a Quantum Design Physical Properties Measurement System (PPMS) from 2.4 to 397.4 K.•An upturn characteristic of spin-fluctuations in Cp/T (T) was observed below 10 K.•The Gibbs free energy of formation of U3Si5 from the elements was determined to be –45.2 ± 9.0 kJ•mol−1•atom−1. 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 Cp/T (T) below 10 K and have attributed this behavior to potential spin-fluctuations (SF) with an SF temperature (Tsf) of 27 K. An enhancement of LTHC was also observed, as manifested by a large electronic heat capacity coefficient (γel) of 342.9 mJ/mol•K2. From the heat capacity data, the following thermodynamic parameters were determined: the characteristic Debye temperature (θD) over the temperature range 30 – 397 K is 177 ± 2 K, and the standard entropy (Δ0298.15S∘) 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 (ΔfHel∘) of U3Si5, the Gibbs free energy of formation of U3Si5 from the elements (ΔfGel∘) was determined to be –45.2 ± 9.0 kJ•mol−1•atom−1.
ISSN:0022-3115
1873-4820
DOI:10.1016/j.jnucmat.2021.153282