“…Driven by the challenge to find sustainable and safe sources of energy, molten salts have re-emerged as potential coolants in nuclear reactors five decades since the concept was successfully demonstrated. − Because of their minimal vapor pressure − when compared to water, such systems present many advantages including their potential operation near ambient pressure. Chloride-containing molten salts are intriguing and potentially advantageous for certain applications, − including the development of new generation fast-spectrum molten salt reactors, where chloride salts are preferentially used over fluorides because of their higher atomic weight and reduced moderating capacity. , Consequently, mixtures of MgCl 2 with KCl and/or NaCl are considered to be promising media for Pu(U)Cl 3 -based fuel salts. , There are engineering models that predict bulk thermodynamic properties of molten salts; , yet, major gaps still exist in our understanding of ionic coordination numbers used as input in these models, intermediate-range order, and molten salt interactions with materials in general. The reason why understanding structure (including intermediate-range order and coordination environments) is important to thermodynamics, has to do with the activity coefficients and chemical/electrochemical potentials of the ions. − Specifically, the expectation is that order on multiple scales will affect Lewis acidities or basicities of the ions due to long-range Coulombic interactions; as an example, whereas MgCl 2 readily dissolves UO 2 , CaCl 2 does not …”