Ab-initio investigation of the effect of adsorbed salts on segregation of Cr at the Ni (100) surface

Startt, Jacob; Dingreville, Rémi; Raiman, Stephen S.; Deo, Chaitanya

doi:10.1016/j.apsusc.2021.149836

Ab-initio investigation of the effect of adsorbed salts on segregation of Cr at the Ni (100) surface

Journal Article · Sat May 29 00:00:00 EDT 2021 · Applied Surface Science

DOI:https://doi.org/10.1016/j.apsusc.2021.149836· OSTI ID:1787510

Startt, Jacob ^[1]; Dingreville, Rémi ^[1]; Raiman, Stephen S. ^[2]; Deo, Chaitanya ^[3]

Georgia Institute of Technology, Atlanta, GA (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Texas A & M Univ., College Station, TX (United States)
Georgia Institute of Technology, Atlanta, GA (United States)

The dissolution and depletion of chromium (Cr) in salt facing nickel (Ni) alloy surfaces is one of the predominant degradation mechanisms of structural components in molten salt technology. Here, we use density functional theory to investigate the role of electronic level interactions that may underlie the depletion phenomenon of Cr in a Ni (100) surface exposed to various adsorbed salt species. Our results show that, under vacuum, Ni preferentially segregates to the surface layer. Conversely, in the presence of adsorbed anionic salt species (e.g., chlorine (Cl), fluorine (F) or the impurity oxygen (O)) Cr segregation becomes more favorable. In these cases, Cl has the weakest effect on segregation, while O has the strongest effect. Our analysis reveals the strong correlation between Cr segregation and the amount of valence charge transferred between the Cr atom and surface adsorbate: the greater the charge transfer, the lower the segregation energy. We also show that, when considered, secondary cations screen Cr-anion interactions, which in turn reduce the magnitude of the anions effect on segregation. These results shed light on the role of salt impurities likely play in the overall corrosion phenomena in molten salt environments. This work provides insights into the atomic level interactions fundamental to molten salt corrosion and on the importance of maintaining salt purity.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC04-94AL85000; NA0003525

OSTI ID:: 1787510

Alternate ID(s):: OSTI ID: 1786403

Report Number(s):: SAND--2021-5322J; 695892

Journal Information:: Applied Surface Science, Journal Name: Applied Surface Science Vol. 563; ISSN 0169-4332

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (37)

Improved grid-based algorithm for Bader charge allocation Sanville, Edward; Kenny, Steven D.; Smith, Roger Journal of Computational Chemistry, Vol. 28, Issue 5 https://doi.org/10.1002/jcc.20575	journal	January 2007
Magnetic properties of NiCr alloys Besnus, M. J.; Gottehrer, Y.; Munschy, G. Physica Status Solidi (b), Vol. 49, Issue 2 https://doi.org/10.1002/pssb.2220490222	journal	February 1972
Thermodynamic Assessment to Chromium Oxidation in the Production of Stainless Steel Ma, Zhongting; Janke, Dieter steel research international, Vol. 74, Issue 2 https://doi.org/10.1002/srin.200300167	journal	February 2003
Thermodynamic properties of solid alloys of chromium with nickel and iron Mazandarany, F. N.; Pehlke, R. D. Metallurgical Transactions, Vol. 4, Issue 9 https://doi.org/10.1007/BF02643269	journal	September 1973
Curie temperature of nickel Legendre, B.; Sghaier, M. Journal of Thermal Analysis and Calorimetry, Vol. 105, Issue 1 https://doi.org/10.1007/s10973-011-1448-2	journal	March 2011
Ab initio molecular dynamics for liquid metals Kresse, G. Journal of Non-Crystalline Solids, Vol. 192-193 https://doi.org/10.1016/0022-3093(95)00355-X	journal	December 1995
Influence of nickel concentration on point defect migration in high-nickel Fe-Cr-Ni alloys Dimitrov, C.; Dimitrov, O. Journal of Nuclear Materials, Vol. 152, Issue 1 https://doi.org/10.1016/0022-3115(88)90136-5	journal	March 1988
Equilibrium surface segregation for Ni15%Cr(110) Jeng, S. -P.; Holloway, P. H.; Batich, C. D. Surface Science, Vol. 193, Issue 3 https://doi.org/10.1016/0039-6028(88)90437-2	journal	January 1988
Surface energy and magnetism of the 3d metals Aldén, M.; Skriver, H. L.; Mirbt, S. Surface Science, Vol. 315, Issue 1-2 https://doi.org/10.1016/0039-6028(94)90551-7	journal	August 1994
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Incorporation of divalent cations in Cr2O3 during the oxidation of Fe-18%Cr-Ni alloys at 1123° Sharp, W. B. A. Corrosion Science, Vol. 10, Issue 5 https://doi.org/10.1016/S0010-938X(70)80021-X	journal	January 1970
Ni–Cr textured substrates with reduced ferromagnetism for coated conductor applications Thompson, J. R.; Goyal, A.; Christen, D. K. Physica C: Superconductivity, Vol. 370, Issue 3 https://doi.org/10.1016/S0921-4534(01)00937-6	journal	May 2002
Calculated surface segregation in transition metal alloys Ruban, A. V.; Skriver, H. L. Computational Materials Science, Vol. 15, Issue 2 https://doi.org/10.1016/S0927-0256(99)00003-8	journal	June 1999
A fast and robust algorithm for Bader decomposition of charge density Henkelman, Graeme; Arnaldsson, Andri; Jónsson, Hannes Computational Materials Science, Vol. 36, Issue 3 https://doi.org/10.1016/j.commatsci.2005.04.010	journal	June 2006
Corrosion behaviour of stainless steels and a single crystal superalloy in a ternary LiCl–KCl–CsCl molten salt Hofmeister, M.; Klein, L.; Miran, H. Corrosion Science, Vol. 90 https://doi.org/10.1016/j.corsci.2014.09.009	journal	January 2015
Molten salts and nuclear energy production Le Brun, Christian Journal of Nuclear Materials, Vol. 360, Issue 1 https://doi.org/10.1016/j.jnucmat.2006.08.017	journal	January 2007
Effect of moisture on corrosion of Ni-based alloys in molten alkali fluoride FLiNaK salt environments Ouyang, Fan-Yi; Chang, Chi-Hung; You, Bo-Chien Journal of Nuclear Materials, Vol. 437, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.02.021	journal	June 2013
Long-term corrosion behaviors of Hastelloy-N and Hastelloy-B3 in moisture-containing molten FLiNaK salt environments Ouyang, Fan-Yi; Chang, Chi-Hung; Kai, Ji-Jung Journal of Nuclear Materials, Vol. 446, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.11.045	journal	March 2014
Corrosion of 316 stainless steel in high temperature molten Li₂BeF₄ (FLiBe) salt Zheng, Guiqiu; Kelleher, Brian; Cao, Guoping Journal of Nuclear Materials, Vol. 461, p. 143-150 https://doi.org/10.1016/j.jnucmat.2015.03.004	journal	June 2015
Adsorption and diffusion of fluorine on Cr-doped Ni(111) surface: Fluorine-induced initial corrosion of non-passivated Ni-based alloy Ren, Cui-Lan; Han, Han; Gong, Wen-Bin Journal of Nuclear Materials, Vol. 478 https://doi.org/10.1016/j.jnucmat.2016.06.027	journal	September 2016
Aggregation and data analysis of corrosion studies in molten chloride and fluoride salts Raiman, Stephen S.; Lee, Sangkeun Journal of Nuclear Materials, Vol. 511 https://doi.org/10.1016/j.jnucmat.2018.07.036	journal	December 2018
Corrosion behavior of 316SS and Ni-based alloys in a ternary NaCl-KCl-MgCl2 molten salt Sun, Hua; Wang, Jianqiang; Li, Zhijun Solar Energy, Vol. 171 https://doi.org/10.1016/j.solener.2018.06.094	journal	September 2018
Hot corrosion behavior of commercial alloys in thermal energy storage material of molten MgCl2/KCl/NaCl under inert atmosphere Ding, Wenjin; Shi, Hao; Xiu, Yanlei Solar Energy Materials and Solar Cells, Vol. 184 https://doi.org/10.1016/j.solmat.2018.04.025	journal	September 2018
Understanding the surface segregation behavior of transition metals on Ni(111): a first-principles study Yu, Yanlin; Xiao, Wei; Wang, Jianwei Physical Chemistry Chemical Physics, Vol. 18, Issue 38 https://doi.org/10.1039/C6CP02983C	journal	January 2016
First-principle atomistic thermodynamic study on the early-stage corrosion of NiCr alloy under fluoride salt environment Yin, Ya-Ru; Ren, Cui-Lan; Han, Han Physical Chemistry Chemical Physics, Vol. 20, Issue 45 https://doi.org/10.1039/C8CP05045G	journal	January 2018
Accurate and efficient algorithm for Bader charge integration Yu, Min; Trinkle, Dallas R. The Journal of Chemical Physics, Vol. 134, Issue 6 https://doi.org/10.1063/1.3553716	journal	February 2011
Theoretical study of fluorine-induced surface segregation of Cr in non-passivated Ni-based alloys Yin, Ya-Ru; Ren, Cui-Lan; Han, Han Journal of Applied Physics, Vol. 124, Issue 13 https://doi.org/10.1063/1.5047225	journal	October 2018
A grid-based Bader analysis algorithm without lattice bias Tang, W.; Sanville, E.; Henkelman, G. Journal of Physics: Condensed Matter, Vol. 21, Issue 8 https://doi.org/10.1088/0953-8984/21/8/084204	journal	January 2009
High-precision sampling for Brillouin-zone integration in metals Methfessel, M.; Paxton, A. T. Physical Review B, Vol. 40, Issue 6 https://doi.org/10.1103/PhysRevB.40.3616	journal	August 1989
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
First-principles study of point defects in an fcc Fe-10Ni-20Cr model alloy Piochaud, J. B.; Klaver, T. P. C.; Adjanor, G. Physical Review B, Vol. 89, Issue 2 https://doi.org/10.1103/PhysRevB.89.024101	journal	January 2014
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
High Performance Corrosion Resistance of Nickel-Based Alloys in Molten Salt Flibe Kondo, Masatoshi; Nagasaka, Takuya; Muroga, Takeo Fusion Science and Technology, Vol. 56, Issue 1 https://doi.org/10.13182/FST09-A8900	journal	July 2009
Role of nickel in the oxidation of Fe–Cr–Ni alloys in air–water vapour atmospheres Pettersson, R. F. A.; Enecker, J.; Liu, L. Materials at High Temperatures, Vol. 22, Issue 3 https://doi.org/10.3184/096034005782744236	journal	August 2005

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Ab-initio investigation of the effect of adsorbed salts on segregation of Cr at the Ni (100) surface

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