UO2 microstructural evolutions induced by Ni, Mo, and W dopants for intentional forensics

Lopes, Denise Adorno; Ulrich, Tash; Kercher, Andrew; Bronikowski, Michael; Samperton, Kyle; Scott, Spencer; Wellons, Matthew; Green, Gage; Spano, Tyler; Harp, Jason; Nelson, Andrew; Shields, Ashley

doi:10.1016/j.jnucmat.2025.155885

UO2 microstructural evolutions induced by Ni, Mo, and W dopants for intentional forensics

Journal Article · Fri Aug 01 04:00:00 EDT 2025 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2025.155885· OSTI ID:2998704

Lopes, Denise Adorno ^[1]; ^[1]; Kercher, Andrew ^[1]; ^[2]; ^[2]; ^[2]; Wellons, Matthew ^[2]; ^[2]; ^[1]; ^[1]; ^[1]; ^[1]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Savannah River National Laboratory (SRNL), Aiken, SC (United States)

The concept of tagging nuclear fuel with a chemical barcode to enable forensics analysis across the nuclear fuel cycle is an area of active investigation, particularly to ensure fabrication viability without disrupting current fuel performance. This study explored the feasibility of using Ni, Mo, and W isotopic double-spikes as dopants in UO2 fuel from the perspective of fuel fabrication. Doped UO2 pellets were produced using conventional fuel fabrication processes, including powder mixing, sieving, pressing, and sintering in a reductive atmosphere. Two composition levels, 100 and 1000 ppm, were evaluated for each dopant element with isotopic double-spike configurations. For the Ni system, additional dopant concentrations of 250 and 500 ppm were produced with nonperturbed isotopic ratios. The results demonstrated that successful incorporation of Ni, Mo, and W double-spikes into UO2 pellets occurred with minimal shift in final density or dopant loss during pellet fabrication. Isotopic analysis confirmed the presence of the double-spike signature even when diluted with natural isotopic material in ratio of 1:5 in the fabrication process. Microstructural examinations revealed different impacts on grain size compared with undoped UO2. This study showed that Ni incorporation up to ∼500 ppm promoted moderate grain growth, whereas the Mo and W systems caused grain size reduction at all concentrations. Changes in the UO2 lattice parameter as a function of composition were detected exclusively for Ni up to 500 ppm, indicating that the Ni solid solution was the main factor for the observed grain growth. Insoluble (Mo and W) or supersaturated (Ni > 500 ppm) conditions produced grain size reduction. The Ni-doped pellets in the solution range resulted in a final microstructure within fuel specifications, demonstrating its potential benefits of employing complex dopant systems for potential nuclear forensic applications.

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Savannah River National Laboratory (SRNL), Aiken, SC (United States)

Sponsoring Organization:: U.S. Department of Energy; National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation R&D

DOE Contract Number:: 89303321CEM000080

OSTI ID:: 2998704

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 614; ISSN 0022-3115

Publisher:: Elsevier BV

Country of Publication:: United States

Language:: English

References (32)

MAUD Rietveld Refinement Software for Neutron Diffraction Texture Studies of Single- and Dual-Phase Materials Saville, Alec I.; Creuziger, Adam; Mitchell, Emily B. Integrating Materials and Manufacturing Innovation, Vol. 10, Issue 3 https://doi.org/10.1007/s40192-021-00224-5	journal	August 2021
Mechanisms of swelling and gas release in uranium dioxide Hilbert, R. F.; Storhok, V. W.; Chubb, W. Journal of Nuclear Materials, Vol. 38, Issue 1 https://doi.org/10.1016/0022-3115(71)90004-3	journal	January 1971
The effect of grain size on the swelling and gas release properties of uo2 during irradiation Turnbull, J. A. Journal of Nuclear Materials, Vol. 50, Issue 1 https://doi.org/10.1016/0022-3115(74)90061-0	journal	February 1974
Surface, grain boundary and interfacial energies in UO2 and UO2-Ni Nikolopoulos, P.; Nazaré, S.; Thümmler, F. Journal of Nuclear Materials, Vol. 71, Issue 1 https://doi.org/10.1016/0022-3115(77)90191-X	journal	December 1977
The chemical state of the fission products in oxide fuels Kleykamp, H. Journal of Nuclear Materials, Vol. 131, Issue 2-3, p. 221-246 https://doi.org/10.1016/0022-3115(85)90460-X	journal	April 1985
On the solubility of chromium sesquioxide in uranium dioxide fuel Leenaers, A.; de Tollenaere, L.; Delafoy, Ch Journal of Nuclear Materials, Vol. 317, Issue 1 https://doi.org/10.1016/S0022-3115(02)01693-8	journal	April 2003
The behaviour of single atoms of molybdenum in urania Nicoll, S.; Matzke, Hj; Grimes, R. W. Journal of Nuclear Materials, Vol. 240, Issue 3 https://doi.org/10.1016/S0022-3115(96)00716-7	journal	February 1997
The role of dopant charge state on defect chemistry and grain growth of doped UO2 Cooper, M. W. D.; Stanek, C. R.; Andersson, D. A. Acta Materialia, Vol. 150 https://doi.org/10.1016/j.actamat.2018.02.020	journal	May 2018
An approach to fuel development and qualification Crawford, Douglas C.; Porter, Douglas L.; Hayes, Steven L. Journal of Nuclear Materials, Vol. 371, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2007.05.029	journal	September 2007
TiO2 doped UO2 fuels sintered by spark plasma sintering Yao, Tiankai; Scott, Spencer M.; Xin, Guoqing Journal of Nuclear Materials, Vol. 469 https://doi.org/10.1016/j.jnucmat.2015.11.025	journal	February 2016
The defect chemistry of U O 2 ± x from atomistic simulations Cooper, M. W. D.; Murphy, S. T.; Andersson, D. A. Journal of Nuclear Materials, Vol. 504 https://doi.org/10.1016/j.jnucmat.2018.02.034	journal	June 2018
Comparative chemical and structural analyses of two uranium dioxide fuel pellets Spano, Tyler L.; Simonetti, Antonio; Corcoran, Loretta Journal of Nuclear Materials, Vol. 518 https://doi.org/10.1016/j.jnucmat.2019.02.038	journal	May 2019
Theoretical study on the mechanical and thermal properties of uranium dioxide doped with lanthanide fission products Vazhappilly, Tijo; Pathak, Arup Kumar Journal of Nuclear Materials, Vol. 519 https://doi.org/10.1016/j.jnucmat.2019.03.032	journal	June 2019
Oxidation and anion lattice defect signatures of hypostoichiometric lanthanide-doped UO2 Olds, Travis A.; Karcher, Samuel E.; Kriegsman, Kyle W. Journal of Nuclear Materials, Vol. 530 https://doi.org/10.1016/j.jnucmat.2019.151959	journal	March 2020
Microstructural and crystallographic effects of sol-gel synthesized Ti-doped UO2 sintered under reducing conditions Silva, Chinthaka M.; Hunt, Rodney D.; Nelson, Andrew T. Journal of Nuclear Materials, Vol. 552 https://doi.org/10.1016/j.jnucmat.2021.153003	journal	August 2021
Effect of added gadolinium oxide on the thermal air oxidation of uranium dioxide Scheele, Randall D.; Hanson, Brady D.; Casella, Andrew M. Journal of Nuclear Materials, Vol. 552 https://doi.org/10.1016/j.jnucmat.2021.153008	journal	August 2021
An evaluation of tri-valent oxide (Cr2O3) as a grain enlarging dopant for UO2 nuclear fuels fabricated under reducing environment Silva, Chinthaka M.; Hunt, Rodney D.; Holliday, Kiel S. Journal of Nuclear Materials, Vol. 553 https://doi.org/10.1016/j.jnucmat.2021.153053	journal	September 2021
Molybdenum and Tungsten isotope compositions of UO2 fuel pellets: Implications for isotopically enriched taggants Shollenberger, Quinn R.; Rolison, John M.; Sharp, Michael A. Journal of Nuclear Materials, Vol. 584 https://doi.org/10.1016/j.jnucmat.2023.154583	journal	October 2023
Characterization of the radial microstructural evolution in LWR UO2 using electron backscatter diffraction McKinney, Casey; Seibert, Rachel; Werden, Jesse Journal of Nuclear Materials, Vol. 585 https://doi.org/10.1016/j.jnucmat.2023.154605	journal	November 2023
Performance and properties evolution of near-term accident tolerant fuel: Cr-doped UO₂ Terricabras, Adrien J.; Drewry, Sean M.; Campbell, Keri Journal of Nuclear Materials, Vol. 594 https://doi.org/10.1016/j.jnucmat.2024.155022 155022	journal	June 2024
Sensitivity of UO2 fuel performance to microstructural evolutions driven by dilute additives Cheniour, Amani; Sweet, Ryan T.; Nelson, Andrew T. Nuclear Engineering and Design, Vol. 410 https://doi.org/10.1016/j.nucengdes.2023.112383	journal	August 2023
Taggant materials in forensic science: A review Gooch, James; Daniel, Barbara; Abbate, Vincenzo TrAC Trends in Analytical Chemistry, Vol. 83 https://doi.org/10.1016/j.trac.2016.08.003	journal	October 2016
Trends and perspectives in Nuclear Forensic Science Varga, Z.; Wallenius, M.; Krachler, M. TrAC Trends in Analytical Chemistry, Vol. 146 https://doi.org/10.1016/j.trac.2021.116503	journal	January 2022
Fabrication, defect chemistry and microstructure of Mn-doped UO2 Smith, H.; Townsend, L. T.; Mohun, R. Scientific Reports, Vol. 14, Issue 1 https://doi.org/10.1038/s41598-023-50676-2	journal	January 2024
Raman spectroscopic studies of defect structures and phase transition in hyper-stoichiometric UO2+x He, Heming; Shoesmith, David Physical Chemistry Chemical Physics, Vol. 12, Issue 28 https://doi.org/10.1039/b925495a	journal	January 2010
Fission Gas Behavior during Postirradiation Annealing of Large Grained UO ₂ Fuels Irradiated to 23 GWd/t Une, Katsumi; Kashibe, Shinji; Ito, Kenichi Journal of Nuclear Science and Technology, Vol. 30, Issue 3 https://doi.org/10.1080/18811248.1993.9734473	journal	March 1993
Advanced Doped UO ₂ Pellets in LWR Applications Arborelius, Jakob; Backman, Karin; Hallstadius, Lars Journal of Nuclear Science and Technology, Vol. 43, Issue 9 https://doi.org/10.1080/18811248.2006.9711184	journal	September 2006
Resonant Raman scattering in UO 2 revisited Livneh, Tsachi Physical Review B, Vol. 105, Issue 4 https://doi.org/10.1103/PhysRevB.105.045115	journal	January 2022
Crystallography Open Database – an open-access collection of crystal structures Gražulis, Saulius; Chateigner, Daniel; Downs, Robert T. Journal of Applied Crystallography, Vol. 42, Issue 4 https://doi.org/10.1107/S0021889809016690	journal	May 2009
Preparation and Characterization of Large Grain UO2 for Accident Tolerant Fuel Zhong, Yi; Gao, Rui; Li, Bingqing Frontiers in Materials, Vol. 8 https://doi.org/10.3389/fmats.2021.651074	journal	April 2021
Nuclear fuel irradiation testbed for nuclear security applications Wilson, Brandon A.; Conant, Andrew; Ulrich, Tashiema L. Frontiers in Nuclear Engineering, Vol. 2 https://doi.org/10.3389/fnuen.2023.1123134	journal	February 2023
BEHAVIORS OF MOLYBDENUM IN UO₂FUEL MATRIX Ha, Yeong-Keong; Kim, Jong-Goo; Park, Yang-Soon Nuclear Engineering and Technology, Vol. 43, Issue 3 https://doi.org/10.5516/NET.2011.43.3.309	journal	June 2011

Similar Records

UO₂ microstructural evolutions induced by Ni, Mo, and W dopants for intentional forensics

Journal Article · Thu May 08 20:00:00 EDT 2025 · Journal of Nuclear Materials · OSTI ID:3002825

Synthesis and characterization of isotopically barcoded nickel, molybdenum, and tungsten taggants for intentional nuclear forensics

Journal Article · Tue Dec 17 19:00:00 EST 2024 · Talanta · OSTI ID:2520061

Related Subjects

36 MATERIALS SCIENCE
characterization
dopants
fabrication
intentional forensic
nuclear fule

UO2 microstructural evolutions induced by Ni, Mo, and W dopants for intentional forensics

Citation Formats

References (32)

Similar Records

Related Subjects