Abstract
The in-pile performance of ceramic fuels is significantly affected by the fission products. In this work, we have performed first-principles density functional theoretical calculations to study the interaction between metallic fission products (barium and zirconium) and the uranium dinitride UN2 matrix. The thermodynamic properties and bonding nature of Ba and Zr atoms in different incorporation configurations indicate that Zr is more soluble in UN2 matrix than Ba. With increasing the concentration of the impurity atoms, Zr-doped UN2 exhibits a slight tendency to contract, while Ba-doped UN2 tends to swell. Based on the competition between steric effect and chemical interaction, various incorporation trends for Ba and Zr in UN2 as well as in UN have been understood.
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Thomson RK, Cantat T, Scott BL, Morris DE, Batista ER, Kiplinger JL. Uranium azide photolysis results in C–H bond activation and provides evidence for a terminal uranium nitride. Nat Chem, 2010, 2: 723–729
International Nuclear Societies Council (INSC). A Vision for the Second Fifty Years of Nuclear Energy. USA: American Nuclear Society, 1996
Lan JH, Zhao ZC, Wu Q, Zhao YL, Chai ZF, Shi WQ. Firstprinciples DFT+U modeling of defect behaviors in antiferromagnetic uranium mononitride. J App Phys, 2013, 114: 223516
Lu Y, Wang BT, Li RW, Shi HL, Zhang P. Structural, electronic, mechanical, and thermodynamic properties of UN2: systematic density functional calculations. J Nucl Mater, 2011, 410: 46–51
Obodo KO, Chetty N. GGA+U studies of the early actinide mononitrides and dinitrides. J Nucl Mater, 2013, 442: 235–244
Brillant G, Pasturel A. Study of Ba and Zr stability in U2±XO by density functional calculations. Phys Rev B, 2008, 77: 184110
Zhang YJ, Lan J, Bo T, Wang CZ, Chai ZF, Shi WQ. First-principles study of barium and zirconium stability in uranium mononitride nuclear fuels. J Phys Chem, 2014, 118: 14579–14585
Varshney D, Shriya S. Pressure and temperature dependent elastic, mechanical and thermodynamical properties of nuclear fuel: UO2 and UN2. J Nucl Mater, 2013, 440: 344–365
Moore KT, van der Laan G. Nature of the 5f states in actinide metals. Rev Mod Phys, 2009, 81: 235–298
Curry N. An investigation of the magnetic structure of uranium nitride by neutron diffraction. Proc Phys Soc, 1965, 86: 1193
Gryaznov D, Heifets E, Kotomin E. The first-principles treatment of the electron-correlation and spin-orbital effects in uranium mononitride nuclear fuels. Phys Chem Chem Phys, 2012, 14: 4482–4490
Geng HY, Chen Y, Kaneta Y, Kinoshita M, Wu Q. Interplay of defect cluster and the stability of xenon in uranium dioxide from density functional calculations. Phys Rev B, 2010, 82: 094106
Dorado B, Andersson DA, Stanek CR, Bertolus M, Uberuaga BP, Martin G, Freyss M, Garcia P. First-principles calculations of uranium diffusion in uranium dioxide. Phys Rev B, 2012, 86: 035110
Ducher R, Dubourg R, Barrachin M, Pasturel A. First-principles study of defect behavior in irradiated uranium monocarbide. Phys Rev B, 2011, 83: 104107
Meredig B, Thompson A, Hansen H, Wolverton C, van de Walle A. Method for locating low-energy solutions within DFT+U. Phys Rev B, 2010, 82: 195128
Dorado B, Amadon B, Freyss M, Bertolus M. DFT+U calculations of the ground state and metastable states of uranium dioxide. Phys Rev B, 2009, 79: 235125
Gryaznov D, Heifets E, Kotomin E. Ab initio DFT+U study of He atom incorporation into UO2 crystals. Phys Chem Chem Phys, 2009, 11: 7241–7247
Lan JH, Wang L, Li S, Yuan LY, Feng YX, Sun W, Zhao YL, Chai ZF, Shi WQ. First principles modeling of zirconium solution in bulk UO2. J Appl Phy, 2013, 113: 183514
Blöchl PE. Projector augmented-wave method. Phys Rev B, 1994, 50: 17953–17979
Kresse G, Furthmüller J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys Rev B, 1996, 54: 11169–11186
Kresse G, Joubert D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys Rev B, 1999, 59: 1758
Perdew JP, Burke K, Ernzerhof M. Generalized gradient approximation made simple. Phys Rev Lett, 1996, 77: 3865–3868
Monkhorst HJ, Pack JD. Special points for brillouin-zone integrations. Phys Rev B, 1976, 13: 5188–5192
Bader RF. Atoms in Molecules: A Quantum Theory. Oxford and New York: Clarendon Press, 1990
Freyss M. First-principles study of uranium carbide: accommodation of point defects and of helium, xenon, and oxygen impurities. Phys Rev B, 2010, 81: 014101
Wang SX, Yang Y, Sun B, Li RW, Liu SJ, Zhang P. Activated molecular adsorption of CO on the Be(0001) surface: a densityfunctional theory study. Phys Rev B, 2009, 80: 115434
Grimes R, Catlow C. The stability of fission products in uranium dioxide. Philos Trans R Soc A-Math Phys Eng Sci, 1991, 335: 609–634
Shannon RD. Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Crystallogr A, 1976, 32: 751–767
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Zhang, Y., Lan, J., Wu, Q. et al. Theoretical investigation on the solution behaviors of Ba and Zr in uranium dinitride. Sci. China Chem. 58, 1891–1897 (2015). https://doi.org/10.1007/s11426-015-5441-7
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DOI: https://doi.org/10.1007/s11426-015-5441-7