TY - JOUR
T1 - Correlational Approach to Predict the Enthalpy of Mixing for Chloride Melt Systems
AU - Schorne-Pinto, Juliano
AU - Yingling, Jacob A.
AU - Christian, Matthew S.
AU - Mofrad, Amir M.
AU - Aslani, Mahmoud A.A.
AU - Besmann, Theodore M.
N1 - Funding Information:
The authors acknowledge support from the MSTDB-TC development effort under the Nuclear Energy Advanced Modeling and Simulation Program administered by Los Alamos National Laboratory, which is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under contract number 89233218NCA000001.
Publisher Copyright:
© 2021 The Authors. Published by American Chemical Society
PY - 2022/1/11
Y1 - 2022/1/11
N2 - A methodology to estimate the heat of mixing (ΔmixH) for salt liquids in unexplored AkCl–AnClx/LnClx (Ak = alkali, An = actinide, Ln = lanthanide) systems is developed. It improves upon previous empirical approaches by eliminating the need for arbitrarily choosing the required composition at maximum short-range ordering, the minimum ΔmixH prior to performing the estimation, which avoids the intrinsic ambiguity of that approach. This semiempirical method has computationally reproduced the behavior of NaCl–UCl3 and KCl–UCl3 systems, providing ΔmixH values that agree well with the reported measurements within a propagated two standard deviations (2σ). The capability of the approach is demonstrated in its application to the entirety of the AkCl–UCl3 and AkCl–PuCl3 systems, the results from which have facilitated the accurate thermodynamic modeling of these and other AkCl–AnCl3/LnCl3 systems. The resultant assessed Gibbs energy functions and models have been incorporated in the Molten Salt Thermal Properties Database–Thermochemical (MSTDB-TC).
AB - A methodology to estimate the heat of mixing (ΔmixH) for salt liquids in unexplored AkCl–AnClx/LnClx (Ak = alkali, An = actinide, Ln = lanthanide) systems is developed. It improves upon previous empirical approaches by eliminating the need for arbitrarily choosing the required composition at maximum short-range ordering, the minimum ΔmixH prior to performing the estimation, which avoids the intrinsic ambiguity of that approach. This semiempirical method has computationally reproduced the behavior of NaCl–UCl3 and KCl–UCl3 systems, providing ΔmixH values that agree well with the reported measurements within a propagated two standard deviations (2σ). The capability of the approach is demonstrated in its application to the entirety of the AkCl–UCl3 and AkCl–PuCl3 systems, the results from which have facilitated the accurate thermodynamic modeling of these and other AkCl–AnCl3/LnCl3 systems. The resultant assessed Gibbs energy functions and models have been incorporated in the Molten Salt Thermal Properties Database–Thermochemical (MSTDB-TC).
UR - https://www.scopus.com/pages/publications/85122321377
U2 - 10.1021/acsomega.1c04755
DO - 10.1021/acsomega.1c04755
M3 - Article
AN - SCOPUS:85122321377
SN - 2470-1343
VL - 7
SP - 362
EP - 371
JO - ACS Omega
JF - ACS Omega
IS - 1
ER -