journal article·2021-04-26Open access

Complex Structure of Molten NaCl–CrCl 3 Salt: Cr–Cl Octahedral Network and Intermediate-Range Order

Qing-Jie Li, David Sprouster, Guiqiu Zheng, Jörg C. Neuefeind, Alexander D. Braatz, Joanna Mcfarlane, Daniel Olds, Stephen Lam, Ju Li, Boris Khaykovich

ACS Applied Energy Materials· Volume 4· Issue 4

Abstract

The resurgence of the molten-salt nuclear reactors (MSRs) creates interesting problems in molten-salt chemistry. As MSRs operate, the composition and physical properties of salts change because of fission and corrosion. Since Cr is the principal corrosion product and NaCl is a common constituent, we studied the atomic structure of molten NaCl–CrCl3. We found networks of CrCl63- octahedra and an intermediate-range order with a nonmonotonic temperature behavior with a remarkable agreement between measurements and ab initio simulations. Even though the corrosion results in minute quantities of dissolved Cr, the speciation of Cr could lead to changes in molten-salt properties in nuclear and solar salts. In particular, we found a much lower melting temperature than expected and a broad metastable liquid–solid coexistence phase. The availability of Cr isotopes with very different neutron scattering properties makes Cr an ideal model multivalent ion for experimental validation of new atomistic models such as neural network interatomic potentials.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Zeolite Catalysis and Synthesis · Solid-state spectroscopy and crystallography · Molten salt chemistry and electrochemical processes

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11784, United States

Nuclear Reactor Laboratory, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Neutron Scattering Science Directorate, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37831-6475, United States

Isotopes and Fuel Cycle Technology Division, Oak Ridge National Laboratory, P.O. Box 2008, Oak Ridge, Tennessee 37831-6243, United States

National Synchrotron Light Source II, Brookhaven National Laboratory, P.O. Box 5000, Upton, New York 11973, United States

Department of Chemical Engineering, University of Massachusetts Lowell, 1 University Avenue, Lowell, Massachusetts 01854, United States

Department of Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Funding

U.S. Department of Energy

References (50)

Show source-provided references
1. Williams D. F. · 2017
2. Lantelme F. · 2013
3. 10.1039/c1pc90003j10.1039/c1pc90003j ↗
4. Hansen J.-P. · 2013
5. Egelstaff P. · 2012
6. 10.1080/00268976.2014.89739610.1080/00268976.2014.897396 ↗
7. 10.1016/j.jnucmat.2014.03.01410.1016/j.jnucmat.2014.03.014 ↗
8. 10.1149/2.007408jes10.1149/2.007408jes ↗
9. 10.1103/physrevlett.98.14640110.1103/physrevlett.98.146401 ↗
10. 10.1016/j.xcrp.2021.10035910.1016/j.xcrp.2021.100359 ↗
11. 10.1016/j.jnucmat.2018.07.03610.1016/j.jnucmat.2018.07.036 ↗
12. Korshunov B. G. · Zh. Neorg. Khim. · 1962 · 7 · 1137
13. 10.1016/0022-1902(63)80218-310.1016/0022-1902(63)80218-3 ↗
14. Vasil’kova I. V. · Zh. Neorg. Khim. · 1964 · 9 · 900
15. Oki T. · Denki Kagaku · 1968 · 36 · 11910.5796/kogyobutsurikagaku.36.119 ↗
16. Phase Equilibria Diagrams Online Database (NIST Standard Reference Database 31) , 2021, www.nist.gov/srd/nist31.cfm.
17. Shaffer J. H. · 197110.2172/4074869 ↗
18. Thoma R. E. · 197110.2172/4675946 ↗
19. 10.1016/j.nimb.2012.05.03710.1016/j.nimb.2012.05.037 ↗
20. Egami T. · 2012
21. 10.1107/s002188981300519010.1107/s0021889813005190 ↗
22. 10.1103/physrevb.47.55810.1103/physrevb.47.558 ↗
23. 10.1103/physrevb.49.1425110.1103/physrevb.49.14251 ↗
24. 10.1103/physrevb.54.1116910.1103/physrevb.54.11169 ↗
25. 10.1016/0927-0256(96)00008-010.1016/0927-0256(96)00008-0 ↗
26. 10.1103/physrevlett.77.386510.1103/physrevlett.77.3865 ↗
27. 10.1103/physrevlett.78.139610.1103/physrevlett.78.1396 ↗
28. 10.1103/physrevb.50.1795310.1103/physrevb.50.17953 ↗
29. 10.1103/physrevb.59.175810.1103/physrevb.59.1758 ↗
30. 10.1002/jcc.2049510.1002/jcc.20495 ↗
31. 10.1002/jcc.2122410.1002/jcc.21224 ↗
32. 10.1016/j.commatsci.2013.10.04310.1016/j.commatsci.2013.10.043 ↗
33. 10.1007/bf0140836210.1007/bf01408362 ↗
34. 10.1107/s056773947600155110.1107/s0567739476001551 ↗
35. 10.1021/acsaem.8b0215710.1021/acsaem.8b02157 ↗
36. 10.1088/0022-3719/15/11/00110.1088/0022-3719/15/11/001 ↗
37. 10.1088/0034-4885/69/1/r0510.1088/0034-4885/69/1/r05 ↗
38. 10.1021/jp306601910.1021/jp3066019 ↗
39. 10.1021/acs.jpclett.9b0284510.1021/acs.jpclett.9b02845 ↗
40. 10.1103/physrevb.43.172610.1103/physrevb.43.1726 ↗
41. 10.1021/acs.jpcb.0c0074510.1021/acs.jpcb.0c00745 ↗
42. 10.1103/physrevb.82.10420810.1103/physrevb.82.104208 ↗
43. 10.1016/s0022-4596(73)80003-910.1016/s0022-4596(73)80003-9 ↗
44. Takamoto, S.; Izumi, S.; Li, J. TeaNet: universal neural network interatomic potential inspired by iterative electronic relaxations. 2019, arXiv:1912.01398. arXiv preprint.
45. 10.1039/c5fd00223k10.1039/c5fd00223k ↗
46. Shirai T. · 1960 · 10
47. 10.1007/s10967-006-0454-510.1007/s10967-006-0454-5 ↗
48. 10.1016/j.anucene.2007.06.01510.1016/j.anucene.2007.06.015 ↗
49. 10.1038/414622a10.1038/414622a ↗
50. 10.1038/nature0347510.1038/nature03475 ↗