Heterogeneous Structure, Mechanisms of Counterion Exchange, and the Spacer Salt Effect in Complex Molten Salt Mixtures Including LaCl3

Matthew S Emerson; Alexander S Ivanov; Leighanne C Gallington; Dmitry S Maltsev; Phillip Halstenberg; Sheng Dai; Santanu Roy; Vyacheslav S Bryantsev; Claudio J Margulis

doi:10.1021/acs.jpcb.4c01429

Back

Heterogeneous Structure, Mechanisms of Counterion Exchange, and the Spacer Salt Effect in Complex Molten Salt Mixtures Including LaCl3

Journal article

Open access

Peer reviewed

Heterogeneous Structure, Mechanisms of Counterion Exchange, and the Spacer Salt Effect in Complex Molten Salt Mixtures Including LaCl3

Matthew S Emerson, Alexander S Ivanov, Leighanne C Gallington, Dmitry S Maltsev, Phillip Halstenberg, Sheng Dai, Santanu Roy, Vyacheslav S Bryantsev and Claudio J Margulis

The journal of physical chemistry. B, Vol.128(16), pp.3972-3980

04/25/2024

DOI: 10.1021/acs.jpcb.4c01429

PMCID: PMC11056984

PMID: 38624173

Appears in UI Libraries Support Open Access

Files and links (1)

url

https://doi.org/10.1021/acs.jpcb.4c01429View

Published (Version of record) Open Access

Abstract

Complex molten chloride salt mixtures of uranium, magnesium, and sodium are top candidates for promising nuclear energy technologies to produce electricity based on molten salt reactors. From a local structural perspective, LaCl3 is similar to UCl3 and hence a good proxy to study these complex salt mixtures. As fission products, lanthanide salts and their mixtures are also very important in their own right. This article describes from an experimental and theory perspective how very different the structural roles of MgCl2 and NaCl are in mixtures with LaCl3. We find that, whereas MgCl2 becomes an integral part of multivalent ionic networks, NaCl separates them. In a recent article (J. Am. Chem. Soc. 2022, 144, 21751-21762) we have called the disruptive behavior of NaCl "the spacer salt effect". Because of the heterogeneous nature of these salt mixtures, there are multiple structural motifs in the melt, each with its particular free energetics. Our work identifies and quantifies these; it also elucidates the mechanisms through which Cl- ions exchange between Mg2+-rich and La3+-rich environments.

UIOWA OA Agreement

Details

Title: Subtitle: Heterogeneous Structure, Mechanisms of Counterion Exchange, and the Spacer Salt Effect in Complex Molten Salt Mixtures Including LaCl3
Creators: Matthew S Emerson - University of Iowa
Alexander S Ivanov - Oak Ridge National Laboratory
Leighanne C Gallington - Argonne National Laboratory
Dmitry S Maltsev - Oak Ridge National Laboratory
Phillip Halstenberg - Oak Ridge National Laboratory
Sheng Dai - Oak Ridge National Laboratory
Santanu Roy - Oak Ridge National Laboratory
Vyacheslav S Bryantsev - Oak Ridge National Laboratory
Claudio J Margulis - University of Iowa
Resource Type: Journal article
Publication Details: The journal of physical chemistry. B, Vol.128(16), pp.3972-3980
Publisher: American Chemical Society
DOI: 10.1021/acs.jpcb.4c01429
PMID: 38624173
PMCID: PMC11056984
eISSN: 1520-5207
Grant note: DOI: 10.13039/100006151, name: Basic Energy Sciences, award: DE-AC02-05CH11231, DE-AC02-06CH11357, DE-AC05-00OR22725, DE-SC0012704
Language: English
Electronic publication date: 04/16/2024
Date published: 04/25/2024
Academic Unit: Chemistry
Record Identifier: 9984616956202771

Metrics

7 Record Views

5 Times Cited - Web of Science