Journal article
Elucidating Ionic Correlations Beyond Simple Charge Alternation in Molten MgCl2–KCl Mixtures
The journal of physical chemistry letters, Vol.10(24), pp.7603-7610
12/19/2019
DOI: 10.1021/acs.jpclett.9b02845
Abstract
The development of technologies for nuclear reactors based on molten salts has seen a big resurgence. The success of thermodynamic models for these hinges in part on our ability to predict at the atomistic level the behavior of pure salts and their mixtures under a range of conditions. In this letter, we present high-energy X-ray scattering experiments and molecular dynamics simulations that describe the molten structure of mixtures of MgCl2 and KCl. As one would expect, KCl is a prototypical salt in which structure is governed by simple charge alternation. In contrast, MgCl2 and its mixtures with KCl display more complex correlations including intermediate-range order and the formation of Cl–-decorated Mg2+ chains. A thorough computational analysis suggests that intermediate-range order beyond charge alternation may be traced to correlations between these chains. An analysis of the coordination structure for Mg2+ ions paints a more complex picture than previously understood, with multiple accessible states of distinct geometries.
Details
- Title: Subtitle
- Elucidating Ionic Correlations Beyond Simple Charge Alternation in Molten MgCl2–KCl Mixtures
- Creators
- Fei Wu - Department of Chemistry, The University of Iowa, Iowa City, Iowa 52242, United StatesSantanu Roy - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesAlexander S Ivanov - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesSimerjeet K Gill - Nuclear Science and Technology Department, Brookhaven National Lab, Upton, New York 11973, United StatesMehmet Topsakal - Nuclear Science and Technology Department, Brookhaven National Lab, Upton, New York 11973, United StatesEric Dooryhee - National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton, New York 11973, United StatesMilinda Abeykoon - National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton, New York 11973, United StatesGihan Kwon - National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton, New York 11973, United StatesLeighanne C Gallington - X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United StatesPhillip Halstenberg - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States, Deptartment of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, United StatesBobby Layne - Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973-5000, United StatesYoshiki Ishii - Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, JapanShannon M Mahurin - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesSheng Dai - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesVyacheslav S Bryantsev - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesClaudio J Margulis - Department of Chemistry, The University of Iowa, Iowa City, Iowa 52242, United States
- Resource Type
- Journal article
- Publication Details
- The journal of physical chemistry letters, Vol.10(24), pp.7603-7610
- DOI
- 10.1021/acs.jpclett.9b02845
- ISSN
- 1948-7185
- eISSN
- 1948-7185
- Grant note
- DOI: 10.13039/501100001691, name: Japan Society for the Promotion of Science, award: JP17J01006; DOI: 10.13039/100006132, name: Office of Science
- Language
- English
- Date published
- 12/19/2019
- Academic Unit
- Chemistry
- Record Identifier
- 9984216703302771
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