Exploring Cr and molten salt interfacial interactions for molten salt applications

Xiaoyang Liu; Yang Liu; Luke D. Gibson; Mingyuan Ge; Daniel Olds; Denis Leshchev; Jianming Bai; Anna M. Plonka; Phillip Halstenberg; Hui Zhong; Sanjit Ghose; Cheng Hung Lin; Xiaoyin Zheng; Xianghui Xiao; Wah Keat Lee; Sheng Dai; German D. Samolyuk; Vyacheslav S. Bryantsev; Anatoly I. Frenkel; Yu Chen Karen Chen-Wiegart

doi:10.1039/d4cp01122h

Exploring Cr and molten salt interfacial interactions for molten salt applications

Xiaoyang Liu, Yang Liu, Luke D. Gibson, Mingyuan Ge, Daniel Olds, Denis Leshchev, Jianming Bai, Anna M. Plonka, Phillip Halstenberg, Hui Zhong, Sanjit Ghose, Cheng Hung Lin, Xiaoyin Zheng, Xianghui Xiao, Wah Keat Lee, Sheng Dai, German D. Samolyuk, Vyacheslav S. Bryantsev, Anatoly I. Frenkel, Yu Chen Karen Chen-Wiegart

Research output: Contribution to journal › Article › peer-review

Abstract

Molten salts play an important role in various energy-related applications such as high-temperature heat transfer fluids and reaction media. However, the extreme molten salt environment causes the degradation of materials, raising safety and sustainability challenges. A fundamental understanding of material-molten salt interfacial evolution is needed. This work studies the transformation of metallic Cr in molten 50/50 mol% KCl-MgCl₂via multi-modal in situ synchrotron X-ray nano-tomography, diffraction and spectroscopy combined with density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. Notably, in addition to the dissolution of Cr in the molten salt to form porous structures, a δ-A15 Cr phase was found to gradually form as a result of the metal-salt interaction. This phase change of Cr is associated with a change in the coordination environment of Cr at the interface. DFT and AIMD simulations provide a basis for understanding the enhanced stability of δ-A15 Cr vs. bcc Cr, by revealing their competitive phase thermodynamics at elevated temperatures and probing the interfacial behavior of the molten salt at relevant facets. This study provides critical insights into the morphological and chemical evolution of metal-molten salt interfaces. The combination of multimodal synchrotron analysis and atomic simulation also offers an opportunity to explore a broader range of systems critical to energy applications.

Original language	English
Pages (from-to)	21342-21356
Number of pages	15
Journal	Physical Chemistry Chemical Physics
Volume	26
Issue number	32
DOIs	https://doi.org/10.1039/d4cp01122h
State	Published - May 22 2024

Funding

This work was supported as part of the Molten Salts in Extreme Environments (MSEE) Energy Frontier Research Center, funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. BNL and ORNL are operated under DOE contracts DE-SC0012704 and DE-AC05-00OR22725, respectively. Work at Stony Brook University was supported by MSEE through a subcontract from BNL. This research used resources, the 8-ID (ISS), 18-ID (FXI), 28-ID-1 (PDF) and 28-ID-2 (XPD) beamlines of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract DE-SC0012704. This research used resources of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science Facility at Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725, as well as resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract DE-AC02-05CH11231 using NERSC award NP-ERCAP0020487. The authors thank Dr Eli Stavitski, the lead scientist of the ISS beamline. The authors thank Lin-Chieh Yu for conducting the SEM analysis. Current and former Chen-Wiegart group members \u2013 Arthur Ronne, Dean Yen, and Chonghang Zhao are acknowledged for conducting the beamtime experiments together at the FXI beamline.

Funders	Funder number
Basic Energy Sciences
U.S. Department of Energy
Office of Science
MSEE
Brookhaven National Laboratory	28-ID-2, 28-ID-1, DE-SC0012704
Brookhaven National Laboratory
DOE Office of Science Facility at Brookhaven National Laboratory	DE-AC05-00OR22725
Lawrence Berkeley National Laboratory	DE-AC02-05CH11231, NP-ERCAP0020487
Lawrence Berkeley National Laboratory

Access to Document

10.1039/d4cp01122h

Cite this

Liu, X., Liu, Y., Gibson, L. D., Ge, M., Olds, D., Leshchev, D., Bai, J., Plonka, A. M., Halstenberg, P., Zhong, H., Ghose, S., Lin, C. H., Zheng, X., Xiao, X., Lee, W. K., Dai, S., Samolyuk, G. D., Bryantsev, V. S., Frenkel, A. I., & Chen-Wiegart, Y. C. K. (2024). Exploring Cr and molten salt interfacial interactions for molten salt applications. Physical Chemistry Chemical Physics, 26(32), 21342-21356. https://doi.org/10.1039/d4cp01122h

@article{94ac7104a6704a2aad90ee2d6dabbd47,

title = "Exploring Cr and molten salt interfacial interactions for molten salt applications",

abstract = "Molten salts play an important role in various energy-related applications such as high-temperature heat transfer fluids and reaction media. However, the extreme molten salt environment causes the degradation of materials, raising safety and sustainability challenges. A fundamental understanding of material-molten salt interfacial evolution is needed. This work studies the transformation of metallic Cr in molten 50/50 mol% KCl-MgCl2via multi-modal in situ synchrotron X-ray nano-tomography, diffraction and spectroscopy combined with density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. Notably, in addition to the dissolution of Cr in the molten salt to form porous structures, a δ-A15 Cr phase was found to gradually form as a result of the metal-salt interaction. This phase change of Cr is associated with a change in the coordination environment of Cr at the interface. DFT and AIMD simulations provide a basis for understanding the enhanced stability of δ-A15 Cr vs. bcc Cr, by revealing their competitive phase thermodynamics at elevated temperatures and probing the interfacial behavior of the molten salt at relevant facets. This study provides critical insights into the morphological and chemical evolution of metal-molten salt interfaces. The combination of multimodal synchrotron analysis and atomic simulation also offers an opportunity to explore a broader range of systems critical to energy applications.",

author = "Xiaoyang Liu and Yang Liu and Gibson, {Luke D.} and Mingyuan Ge and Daniel Olds and Denis Leshchev and Jianming Bai and Plonka, {Anna M.} and Phillip Halstenberg and Hui Zhong and Sanjit Ghose and Lin, {Cheng Hung} and Xiaoyin Zheng and Xianghui Xiao and Lee, {Wah Keat} and Sheng Dai and Samolyuk, {German D.} and Bryantsev, {Vyacheslav S.} and Frenkel, {Anatoly I.} and Chen-Wiegart, {Yu Chen Karen}",

note = "Publisher Copyright: {\textcopyright} 2024 The Royal Society of Chemistry.",

year = "2024",

month = may,

day = "22",

doi = "10.1039/d4cp01122h",

language = "English",

volume = "26",

pages = "21342--21356",

journal = "Physical Chemistry Chemical Physics",

issn = "1463-9076",

publisher = "Royal Society of Chemistry",

number = "32",

}

Liu, X, Liu, Y, Gibson, LD, Ge, M, Olds, D, Leshchev, D, Bai, J, Plonka, AM, Halstenberg, P, Zhong, H, Ghose, S, Lin, CH, Zheng, X, Xiao, X, Lee, WK, Dai, S , Samolyuk, GD , Bryantsev, VS, Frenkel, AI & Chen-Wiegart, YCK 2024, 'Exploring Cr and molten salt interfacial interactions for molten salt applications', Physical Chemistry Chemical Physics, vol. 26, no. 32, pp. 21342-21356. https://doi.org/10.1039/d4cp01122h

TY - JOUR

T1 - Exploring Cr and molten salt interfacial interactions for molten salt applications

AU - Liu, Xiaoyang

AU - Liu, Yang

AU - Gibson, Luke D.

AU - Ge, Mingyuan

AU - Olds, Daniel

AU - Leshchev, Denis

AU - Bai, Jianming

AU - Plonka, Anna M.

AU - Halstenberg, Phillip

AU - Zhong, Hui

AU - Ghose, Sanjit

AU - Lin, Cheng Hung

AU - Zheng, Xiaoyin

AU - Xiao, Xianghui

AU - Lee, Wah Keat

AU - Dai, Sheng

AU - Samolyuk, German D.

AU - Bryantsev, Vyacheslav S.

AU - Frenkel, Anatoly I.

AU - Chen-Wiegart, Yu Chen Karen

PY - 2024/5/22

Y1 - 2024/5/22

N2 - Molten salts play an important role in various energy-related applications such as high-temperature heat transfer fluids and reaction media. However, the extreme molten salt environment causes the degradation of materials, raising safety and sustainability challenges. A fundamental understanding of material-molten salt interfacial evolution is needed. This work studies the transformation of metallic Cr in molten 50/50 mol% KCl-MgCl2via multi-modal in situ synchrotron X-ray nano-tomography, diffraction and spectroscopy combined with density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. Notably, in addition to the dissolution of Cr in the molten salt to form porous structures, a δ-A15 Cr phase was found to gradually form as a result of the metal-salt interaction. This phase change of Cr is associated with a change in the coordination environment of Cr at the interface. DFT and AIMD simulations provide a basis for understanding the enhanced stability of δ-A15 Cr vs. bcc Cr, by revealing their competitive phase thermodynamics at elevated temperatures and probing the interfacial behavior of the molten salt at relevant facets. This study provides critical insights into the morphological and chemical evolution of metal-molten salt interfaces. The combination of multimodal synchrotron analysis and atomic simulation also offers an opportunity to explore a broader range of systems critical to energy applications.

AB - Molten salts play an important role in various energy-related applications such as high-temperature heat transfer fluids and reaction media. However, the extreme molten salt environment causes the degradation of materials, raising safety and sustainability challenges. A fundamental understanding of material-molten salt interfacial evolution is needed. This work studies the transformation of metallic Cr in molten 50/50 mol% KCl-MgCl2via multi-modal in situ synchrotron X-ray nano-tomography, diffraction and spectroscopy combined with density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. Notably, in addition to the dissolution of Cr in the molten salt to form porous structures, a δ-A15 Cr phase was found to gradually form as a result of the metal-salt interaction. This phase change of Cr is associated with a change in the coordination environment of Cr at the interface. DFT and AIMD simulations provide a basis for understanding the enhanced stability of δ-A15 Cr vs. bcc Cr, by revealing their competitive phase thermodynamics at elevated temperatures and probing the interfacial behavior of the molten salt at relevant facets. This study provides critical insights into the morphological and chemical evolution of metal-molten salt interfaces. The combination of multimodal synchrotron analysis and atomic simulation also offers an opportunity to explore a broader range of systems critical to energy applications.

UR - http://www.scopus.com/inward/record.url?scp=85195055333&partnerID=8YFLogxK

U2 - 10.1039/d4cp01122h

DO - 10.1039/d4cp01122h

M3 - Article

AN - SCOPUS:85195055333

SN - 1463-9076

VL - 26

SP - 21342

EP - 21356

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

IS - 32

ER -

Exploring Cr and molten salt interfacial interactions for molten salt applications

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this