First-principles investigation of cerium and neodymium diffusion in BCC chromium and vanadium via vacancy-mediated transport

Shousha, Shehab; Beeler, Benjamin W.; Aagesen, Larry Kenneth; Beausoleil, II, Geoffrey L.; Okuniewski, Maria A.

doi:10.1016/j.jnucmat.2025.156125

First-principles investigation of cerium and neodymium diffusion in BCC chromium and vanadium via vacancy-mediated transport

Journal Article · Wed Sep 03 00:00:00 EDT 2025 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2025.156125· OSTI ID:3016177

^[1]; ^[2]; ^[3]; ^[4]; ^[5]

North Carolina State University, Raleigh, NC (United States)
North Carolina State University, Raleigh, NC (United States); Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States); Univ. of Michigan, Ann Arbor, MI (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Purdue Univ., West Lafayette, IN (United States)

Lanthanide transport plays a crucial role in the performance and longevity of metallic nuclear fuels. This study examines the diffusion behavior of Ce and Nd—two major fission products—in body-centered cubic (BCC) Cr and V, which are potential liner or coating materials for mitigating fuel-cladding chemical interactions (FCCI). Using density functional theory (DFT) calculations and self-consistent mean-field (SCMF) analysis, the vacancy-mediated diffusion coefficients are evaluated. Our findings reveal that Ce and Nd act as oversized solutes and are strongly bound to vacancies in BCC Cr and V, with diffusivities in Cr significantly lower than in V and in hexagonal closed-packed (HCP) Zr, as investigated in our previous work. The activation energies for Ce and Nd diffusion are 3.39 and 3.32 eV, respectively, in BCC Cr, and 2.56 and 2.33 eV, respectively, in BCC V. Analysis of vacancy drag and partial diffusion coefficient ratios indicates a strong tendency for lanthanide enrichment at vacancy sinks in BCC Cr, and to a lesser extent in BCC V, with this effect persisting up to the melting point in Cr and remaining substantial for Nd in V at high temperatures. Under irradiation, the increase in vacancy concentration is expected to enhance lanthanide transport, potentially accelerating interactions at liner-cladding interfaces. Although BCC Cr exhibits relatively low lanthanide diffusivities under equilibrium conditions, the expected segregation tendencies under irradiation suggest that Zr liners may be a more favorable option. Further investigations using rate theory, cluster dynamics, and phase-field modeling are required to quantitatively assess the performance of these materials in reactor environments.

View Accepted Manuscript (DOE)

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC07-05ID14517; NE0009271

OSTI ID:: 3016177

Report Number(s):: INL/JOU--25-84541

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Journal Issue: 1 Vol. 617; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (50)

Atomic and Ionic Radii of Elements 1 -96 Rahm, Martin; Hoffmann, Roald; Ashcroft, N. W. Chemistry - A European Journal, Vol. 22, Issue 41 https://doi.org/10.1002/chem.201602949	journal	August 2016
Ab-initio simulations of materials using VASP: Density-functional theory and beyond Hafner, Jürgen Journal of Computational Chemistry, Vol. 29, Issue 13 https://doi.org/10.1002/jcc.21057	journal	October 2008
Diffusion of uranium in refractory BCC metals Fedorov, G. B.; Smirnov, E. A.; Zhomov, F. I. Soviet Atomic Energy, Vol. 31, Issue 5 https://doi.org/10.1007/BF01165601	journal	November 1971
Experimental studies of U-Pu-Zr fast reactor fuel pins in the experimental breeder reactor-ll Pahl, R. G.; Porter, D. L.; Lahm, C. E. Metallurgical Transactions A, Vol. 21, Issue 7 https://doi.org/10.1007/BF02647233	journal	July 1990
Effect of Zr thin film on Zr foil as a FCCI barrier between lanthanide (La-Ce) and clad material Lee, Kang Soo; Kim, In Yea; Lee, Wooyoung Metals and Materials International, Vol. 21, Issue 3 https://doi.org/10.1007/s12540-015-4433-7	journal	May 2015
Performance of U-Pu-Zr fuel cast into zirconium molds Crawford, D. C.; Lahm, C. E.; Tsai, H. Journal of Nuclear Materials, Vol. 204 https://doi.org/10.1016/0022-3115(93)90212-H	journal	September 1993
Frequency factors and isotope effects in solid state rate processes Vineyard, George H. Journal of Physics and Chemistry of Solids, Vol. 3, Issue 1-2 https://doi.org/10.1016/0022-3697(57)90059-8	journal	January 1957
Metallic fast reactor fuels Hofman, G. L.; Walters, L. C.; Bauer, T. H. Progress in Nuclear Energy, Vol. 31, Issue 1-2 https://doi.org/10.1016/0149-1970(96)00005-4	journal	January 1997
First principles impurity diffusion coefficients Mantina, M.; Wang, Y.; Chen, L. Q. Acta Materialia, Vol. 57, Issue 14 https://doi.org/10.1016/j.actamat.2009.05.006	journal	August 2009
Calculation of impurity diffusivities in α-Fe using first-principles methods Huang, Shenyan; Worthington, Daniel L.; Asta, Mark Acta Materialia, Vol. 58, Issue 6 https://doi.org/10.1016/j.actamat.2009.11.041	journal	April 2010
A comprehensive first-principles study of pure elements: Vacancy formation and migration energies and self-diffusion coefficients Shang, Shun-Li; Zhou, Bi-Cheng; Wang, William Y. Acta Materialia, Vol. 109 https://doi.org/10.1016/j.actamat.2016.02.031	journal	May 2016
Solute diffusion by self-interstitial defects and radiation-induced segregation in ferritic Fe–X (X=Cr, Cu, Mn, Ni, P, Si) dilute alloys Messina, Luca; Schuler, Thomas; Nastar, Maylise Acta Materialia, Vol. 191 https://doi.org/10.1016/j.actamat.2020.03.038	journal	June 2020
Improvement of the zirconium diffusion barrier between lanthanide (La–Ce) and a clad material by hydrothermal crystallization Jee, Seung Hyun; Lee, Kang Soo; Kim, Jun Hwan Current Applied Physics, Vol. 13, Issue 9 https://doi.org/10.1016/j.cap.2013.08.005	journal	November 2013
KineCluE: A kinetic cluster expansion code to compute transport coefficients beyond the dilute limit Schuler, Thomas; Messina, Luca; Nastar, Maylise Computational Materials Science, Vol. 172 https://doi.org/10.1016/j.commatsci.2019.109191	journal	February 2020
Solute–point defect interactions in bcc systems: Focus on first principles modelling in W and RPV steels Becquart, C. S.; Domain, C. Current Opinion in Solid State and Materials Science, Vol. 16, Issue 3 https://doi.org/10.1016/j.cossms.2012.01.001	journal	June 2012
First-principles study of the binding preferences and diffusion behaviors of solutes in vanadium alloys Deng, Lei; Zhang, Xingming; Tang, Jianfeng Journal of Alloys and Compounds, Vol. 660 https://doi.org/10.1016/j.jallcom.2015.11.085	journal	March 2016
Performance of FCCI barrier foils for U–Zr–X metallic fuel Ryu, Ho Jin; Lee, Byoung Oon; Oh, Seok Jin Journal of Nuclear Materials, Vol. 392, Issue 2 https://doi.org/10.1016/j.jnucmat.2009.03.011	journal	July 2009
Performance of a diffusion barrier under a fuel–clad chemical interaction (FCCI) Kim, Jun Hwan; Ryu, Ho Jin; Baek, Jong Hyuk Journal of Nuclear Materials, Vol. 394, Issue 2-3 https://doi.org/10.1016/j.jnucmat.2009.08.018	journal	November 2009
FCCI barrier performance of electroplated Cr for metallic fuel Yang, Seong Woo; Ryu, Ho Jin; Kim, Jun Hwan Journal of Nuclear Materials, Vol. 401, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2010.04.004	journal	June 2010
Vanadium diffusion coating on HT-9 cladding for mitigating the fuel cladding chemical interactions Lo, Wei-Yang; Yang, Yong Journal of Nuclear Materials, Vol. 451, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.03.052	journal	August 2014
Interaction of Ti and Cr atoms with point defects in bcc vanadium: A DFT study Boev, A. O.; Aksyonov, D. A.; Kartamyshev, A. I. Journal of Nuclear Materials, Vol. 492 https://doi.org/10.1016/j.jnucmat.2017.04.046	journal	August 2017
Scanning electron microscopy examination of a Fast Flux Test Facility irradiated U-10Zr fuel cross section clad with HT-9 Harp, Jason M.; Porter, Douglas L.; Miller, Brandon D. Journal of Nuclear Materials, Vol. 494 https://doi.org/10.1016/j.jnucmat.2017.07.040	journal	October 2017
Fuel cladding chemical interaction in metallic sodium fast reactor fuels: A historical perspective Keiser, Dennis D. Journal of Nuclear Materials, Vol. 514 https://doi.org/10.1016/j.jnucmat.2018.09.045	journal	February 2019
First-principles investigation of lanthanides diffusion in HCP zirconium via vacancy-mediated transport Shousha, Shehab; Beeler, Benjamin; Aagesen, Larry K. Journal of Nuclear Materials, Vol. 601 https://doi.org/10.1016/j.jnucmat.2024.155310	journal	December 2024
Comparative study of Cr-coating and Zr-lining method on inner surface of HT9 cladding to mitigate Fuel-Cladding chemical interaction Oh, Jeong Mok; Kim, Dongha; Yoo, Seongsoo Nuclear Engineering and Design, Vol. 421 https://doi.org/10.1016/j.nucengdes.2024.113102	journal	May 2024
Development and preliminary validation of a mechanistic multiscale model for fuel-cladding chemical interaction in metallic nuclear fuels Hirschhorn, J. A.; Aagesen, L. K.; Jiang, C. Nuclear Engineering and Design, Vol. 432 https://doi.org/10.1016/j.nucengdes.2024.113811	journal	February 2025
Significant difference of lanthanide fission products diffusion in Cr and α-Fe: An atomic-level study Yang, Chao; Tian, Jie; Guan, Huaqing Scripta Materialia, Vol. 227 https://doi.org/10.1016/j.scriptamat.2023.115304	journal	April 2023
High-throughput ab-initio dilute solute diffusion database Wu, Henry; Mayeshiba, Tam; Morgan, Dane Scientific Data, Vol. 3, Issue 1 https://doi.org/10.1038/sdata.2016.54	journal	July 2016
A climbing image nudged elastic band method for finding saddle points and minimum energy paths Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904 https://doi.org/10.1063/1.1329672	journal	December 2000
Fuel-Cladding Chemical Interaction in U-Pu-Zr Metallic Fuels: A Critical Review Matthews, Christopher; Unal, Cetin; Galloway, Jack Nuclear Technology, Vol. 198, Issue 3 https://doi.org/10.1080/00295450.2017.1323535	journal	June 2017
Self-consistent formulation of configurational kinetics close to equilibrium: The phenomenological coefficients for diffusion in crystalline solids Nastar, M.; Dobretsov, V. Yu.; Martin, G. Philosophical Magazine A, Vol. 80, Issue 1 https://doi.org/10.1080/01418610008212047	journal	January 2000
Solute and solvent diffusion in V-Zr alloys Pruthi, D. D.; Agarwala, R. P. Philosophical Magazine A, Vol. 49, Issue 2 https://doi.org/10.1080/01418618408234927	journal	August 1984
Vanadium diffusion in V-Co dilute alloys Segel, V.; Pelleg, J. Philosophical Magazine A, Vol. 76, Issue 6 https://doi.org/10.1080/01418619708214223	journal	December 1997
A mean field theory for diffusion in a dilute multi-component alloy: a new model for the effect of solutes on self-diffusion Nastar, M. Philosophical Magazine, Vol. 85, Issue 32 https://doi.org/10.1080/14786430500228390	journal	November 2005
Solvent self-diffusion in dilute b.c.c. solid solutions Le Claire, A. D. Philosophical Magazine, Vol. 21, Issue 172 https://doi.org/10.1080/14786437008238468	journal	April 1970
Magnetic studies of annealed and alloyed chromium by neutron diffraction Bacon, G. E.; Cowlam, N. Journal of Physics C: Solid State Physics, Vol. 2, Issue 2 https://doi.org/10.1088/0022-3719/2/2/306	journal	February 1969
Segregation in irradiated alloys: The inverse Kirkendall effect and the effect of constitution on void swelling Marwick, A. D. Journal of Physics F: Metal Physics, Vol. 8, Issue 9 https://doi.org/10.1088/0305-4608/8/9/008	journal	September 1978
Isotope effect in chromium self-diffusion Mundy, J. N.; Tse, C. W.; McFall, W. D. Physical Review B, Vol. 13, Issue 6 https://doi.org/10.1103/PhysRevB.13.2349	journal	March 1976
Self-diffusion in chromium Mundy, J. N.; Hoff, H. A.; Pelleg, J. Physical Review B, Vol. 24, Issue 2 https://doi.org/10.1103/PhysRevB.24.658	journal	July 1981
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
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Self-interstitial atom defects in bcc transition metals: Group-specific trends Nguyen-Manh, D.; Horsfield, A. P.; Dudarev, S. L. Physical Review B, Vol. 73, Issue 2 https://doi.org/10.1103/PhysRevB.73.020101	journal	January 2006
Point defect modeling in materials: Coupling ab initio and elasticity approaches Varvenne, Céline; Bruneval, Fabien; Marinica, Mihai-Cosmin Physical Review B, Vol. 88, Issue 13 https://doi.org/10.1103/PhysRevB.88.134102	journal	October 2013
Exact ab initio transport coefficients in bcc Fe − X ( X = Cr , Cu , Mn , Ni , P , Si ) dilute alloys Messina, Luca; Nastar, Maylise; Garnier, Thomas Physical Review B, Vol. 90, Issue 10 https://doi.org/10.1103/PhysRevB.90.104203	journal	September 2014
Migration mechanism for oversized solutes in cubic lattices: The case of yttrium in iron Bocquet, Jean-Louis; Barouh, Caroline; Fu, Chu-Chun Physical Review B, Vol. 95, Issue 21 https://doi.org/10.1103/PhysRevB.95.214108	journal	June 2017
Elastic dipoles of point defects from atomistic simulations Varvenne, Céline; Clouet, Emmanuel Physical Review B, Vol. 96, Issue 22 https://doi.org/10.1103/PhysRevB.96.224103	journal	December 2017
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
Solute Diffusion in Metals: Larger Atoms Can Move Faster Janotti, A.; Krčmar, M.; Fu, C. L. Physical Review Letters, Vol. 92, Issue 8 https://doi.org/10.1103/PhysRevLett.92.085901	journal	February 2004
First Principles Calculation of the Interdiffusion Coefficient in Binary Alloys Van der Ven, A.; Ceder, G. Physical Review Letters, Vol. 94, Issue 4 https://doi.org/10.1103/PhysRevLett.94.045901	journal	February 2005

Similar Records

First-principles investigation of lanthanides diffusion in HCP zirconium via vacancy-mediated transport

Journal Article · Thu Aug 01 20:00:00 EDT 2024 · Journal of Nuclear Materials · OSTI ID:2499802

Diffusion Behavior of Oversized Fission Products in bcc Fe Cladding: A First-Principles Study

Technical Report · Thu May 08 00:00:00 EDT 2025 · OSTI ID:2566758

Diffusion behavior of lanthanide fission products in bcc Fe cladding: A first-principles study

Journal Article · Sat Jul 12 20:00:00 EDT 2025 · Computational Materials Science · OSTI ID:3001374

Related Subjects

36 - MATERIALS SCIENCE
36 MATERIALS SCIENCE
cladding liner
computational materials science
fuel cladding chemical interaction
lanthanide diffusion

First-principles investigation of cerium and neodymium diffusion in BCC chromium and vanadium via vacancy-mediated transport

Citation Formats

References (50)

Similar Records

Related Subjects