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Modelling and assessment of thermal conductivity and melting behaviour of

MOX fuel for fast reactor applications

Article in Journal of Nuclear Materials · July 2020

DOI: 10.1016/j.jnucmat.2020.152410

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 Journal of Nuclear Materials 541 (2020) 152410

Contents lists available at ScienceDirect

Journal of Nuclear Materials

journal homepage: www.elsevier.com/locate/jnucmat

Modelling and assessment of thermal conductivity and melting

behaviour of MOX fuel for fast reactor applications
A. Magni a, T. Barani a, A. Del Nevo b, D. Pizzocri a, D. Staicu c, P. Van Uffelen c,∗, L. Luzzi a
a
Politecnico di Milano, Department of Energy, Nuclear Engineering Division, via La Masa 34, 20156, Milano, Italy
b
ENEA, FSN-ING-SIS, CR Brasimone, 40032, Camugnano (BO), Italy
c
European Commission, Joint Research Centre, Directorate for Nuclear Safety and Security, P.O. Box 2340, 76125, Karlsruhe, Germany

a r t i c l e i n f o a b s t r a c t

Article history: Thermal conductivity and melting temperature of nuclear fuel are essential for analysing its performance
Received 20 April 2020 under irradiation, since they determine the fuel temperature profile and the melting safety margin, re-
Revised 22 June 2020
spectively. A starting literature review of data and correlations revealed that most models implemented in
Accepted 18 July 2020
state-of-the-art fuel performance codes (FPCs) describe the evolution of thermal conductivity and melting
Available online 25 July 2020
temperature of Light Water Reactor (LWR) MOX (uranium-plutonium mixed oxide) fuels, in limited ranges
Keywords: of operation and without considering the complete set of fundamental dependencies (i.e., fuel tempera-
Nuclear fuel ture, burn-up, plutonium content, stoichiometry, and porosity). Since innovative Generation IV nuclear
MOX reactor concepts (e.g., ALFRED, ASTRID, MYRRHA) employ MOX fuel to be irradiated in Fast Reactor (FR)
Thermal conductivity conditions, codes need to be extended and validated for application to design and safety analyses on fast
Melting reactor MOX fuel. The aim of this work is to overcome the current modelling and code limitations, pro-
Fast reactor
viding fuel performance codes with suitable correlations to describe the evolution under irradiation of
fast reactor MOX fuel thermal conductivity and melting temperature. The new correlations have been ob-
tained by a statistically assessed fit of the most recent and reliable experimental data. The resulting laws
are grounded on a physical basis and account for a wider set of effects on MOX thermal properties (fuel
temperature, burn-up, deviation from stoichiometry, plutonium content, porosity), providing clear ranges
of applicability for each parameter considered. As a first test series, the new correlations have been im-
plemented in the TRANSURANUS fuel performance code, compared to state-of-the-art correlations, and
assessed against integral data from the HEDL P-19 fast reactor irradiation experiment. The integral val-
idation provides promising results, pointing out a satisfactory agreement with the experimental data,
meaning that the new models can be efficiently applied in engineering fuel performance codes.
© 2020 The Author(s). Published by Elsevier B.V.
This is an open access article under the CC BY license. (http://creativecommons.org/licenses/by/4.0/)

Acronyms HEDL Hanford Engineering Development Laboratory

ALFRED Advanced Lead-cooled Fast Reactor European HM Heavy Metal
Demonstrator HRP Halden Reactor Project
ASTRID Advanced Sodium Technological Reactor for Indus- IFPE International Fuel Performance Experiments
trial Demonstration INSPYRE Investigations Supporting MOX Fuel Licensing for ES-
EBR Experimental Breeder Reactor NII Prototype Reactors
EPMA Electron Probe MicroAnalysis LHR Linear Heat Rate
ESFR-SMART European Sodium Fast Reactor - Safety Measures As- LWR Light Water Reactor
sessment and Research Tools MIMAS MIcronized - MASter blend
ESNII European Sustainable Nuclear Industrial Initiative MOX Mixed-OXide
FBR Fast Breeder Reactor MYRRHA Multi-purpose hYbrid Research Reactor for High-tech
FPC Fuel Performance Code Applications
FR Fast Reactor O/M Oxygen/Metal ratio
OD Outer Diameter
OECD/NEA Organisation for Economic Co-operation and Devel-
∗
Corresponding author. opment / Nuclear Energy Agency
E-mail address: [email protected] (P. Van Uffelen).

https://doi.org/10.1016/j.jnucmat.2020.152410
0022-3115/© 2020 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license. (http://creativecommons.org/licenses/by/4.0/)
2 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410

PIE Post-Irradiation Examination which becomes negligible at high temperatures (i.e., same thermal
rmse root mean square error conductivity value at ∼ 20 0 0 K, independently on the O/M ratio).
SBR Short Binderless Route The aforementioned experimental works have been exploited
TD Theoretical Density to build models of MOX fuel thermal conductivity for fast reac-
XANES X-ray Absorption Near Edge Structure tor applications, developed e.g., by Bonnerot [15] and Philippon-
XRD X-Ray Diffraction neau [9], based on the comprehensive review of thermal proper-
ties of oxide fuels carried out by Martin [16]. They showed that
in the wide temperature range between 800 and 3100 K the MOX
1. Introduction thermal conductivity is always lower with respect to UO2 , with
only slight effects of plutonium concentration (below 12 wt.%) in
The development of Generation IV reactor concepts, employing the entire temperature range, and of O/M ratio at high tempera-
uranium-plutonium mixed oxide (MOX1 ) fuel irradiated under fast tures. Inoue [17] proposed a model that was integrally validated
neutron flux, calls for dedicated and advanced fuel modelling with against data from pin irradiation experiments in the JOYO reactor.
respect to the state of the art (target of the INSPYRE H2020 Project More recent works focused on the experimental characterization
[1]). In particular, accurate models of fuel thermal conductivity and and modelling of thermal conductivity of both fresh and irradiated
melting (solidus) temperature evolution under irradiation are of LWR MOX, featured by a low plutonium content up to 15 wt.%, e.g.,
great importance, to correctly evaluate the fuel temperature pro- [18–22]. Instead, recent and up-to-date measurements on fresh fast
file (impacting on both thermal and mechanical behaviour) and reactor MOX have been performed on fuel samples from PHENIX
the margin to melting – one of the most important safety de- (∼ 24 wt.% Pu, stoichiometric, at temperatures < 1650 K) and TRA-
sign criteria [2–4]. The current modelling of thermal properties of BANT (∼ 40 and 45 wt.% Pu, O/M from 1.96 to 2.00, at temper-
fast reactor MOX in fuel performance codes (FPCs, e.g., GERMINAL atures < 1650 K), in the framework of the ESNII+ H2020 Project
[5], TRANSURANUS [6], BISON [7], FEMAXI [8]) is limited, for vari- [23,24]. In the latter, the temperature effect has been the focus,
ous reasons. First, available experimental data regard fresh MOX or and indeed two correlations were derived specifically for PHENIX
LWR irradiation conditions, while only very few data correspond and TRABANT MOX fuel, accounting only for the temperature ef-
to irradiated fast reactor MOX. Second, the main existing correla- fect. As for irradiated fast reactor MOX, the only accessible ex-
tions, validated and employed by FPCs, consider the temperature, perimental measurements of thermal conductivity have been per-
porosity and burn-up effects on MOX thermal conductivity, with- formed by Yamamoto et al. [25] and by the ESNII+ Project on
out accounting, for instance, for the effect of the initial plutonium NESTOR-3 fuel samples [26] (both fuels with ∼ 20 wt.% Pu, but ir-
content [6,9,10]. The current melting temperature correlations do radiated at moderate and high burn-up, i.e., up to 35 GWd/tHM
not incorporate in an assessed way the effects of plutonium con- and 84 and 130 GWd/tHM, respectively). The conclusions of both
tent, deviation from fuel stoichiometry and burn-up [6]. The minor works shed only partial light on the behaviour of thermal conduc-
actinide content (americium and neptunium especially) and its im- tivity as a function of fuel burn-up. Indeed, the degradation of FR
pact on MOX thermal properties is also of great relevance, in view MOX thermal conductivity as burn-up increases has not been defi-
of MOX application in Generation IV fast breeder reactors [11–13]. nitely proven from experimental observations, since the measured
The analysis of minor actinide-bearing MOX is beyond the scope of effect of low and moderate burn-up is slight [25], while at very
the present work and will be considered in a following step. high burn-up the MOX thermal conductivity seems to be higher
Up to now, MOX fuel has been the object of several researches [26]. The lack of sufficient, concordant, and highly reliable experi-
(albeit limited if compared to those concerning UO2 nuclear fuel), mental data can be indicated as the reason why existing thermal
often showcasing conflicting conclusions amongst the different au- conductivity correlations do not represent all the effects experi-
thors. The effect of the plutonium content on the thermal conduc- mentally observed (temperature, burn-up, plutonium content, de-
tivity of fresh U-Pu mixed oxides was already studied in early ex- viation from stoichiometry, porosity).
perimental works (e.g., Gibby [14] and Schmidt (1969), Serizawa As for the state-of-the-art about the melting temperature, early
et al. (1970), Goldsmith et al. (1972), reviewed by Bonnerot [15]). experimental works have been performed by Lyon and Baily on
While Gibby shows a decrease of the thermal conductivity with fresh stoichiometric MOX with a plutonium content up to 85 mol.%
increasing plutonium content (less pronounced as temperature in- [27], by Aitken, Evans (1968) and Reavis (1972), and reported in
creases towards 1500 K), down to a minimum occurring at around [28]. The latter included both fresh and low burn-up MOX, with
70 wt.% Pu, Goldsmith and co-workers support a linear decrease of oxygen-to-metal ratio between 1.97 and 2.00 and a plutonium con-
the thermal conductivity between 0 and 30 wt.% Pu (at low tem- tent up to 60 mol.%. The melting temperature measured in these
peratures between 700 K and 1300 K). Instead, both Schmidt and early campaigns resulted in values sensibly lower than expected,
Serizawa et al. claim that the plutonium content has no influ- and was therefore re-assessed. As a result, it has been proven
ence on MOX thermal diffusivity and conductivity (at temperatures that a tungsten melting capsule strongly contaminates the melted
above 1300 K and in the entire temperature range, respectively). fuel specimen and heavily lowers the observed melting temper-
Concerning the effect of stoichiometry deviation on the fuel ther- ature [29,30]. Other melting experiments performed in tungsten
mal conductivity, it has been the specific focus of investigations by capsules, employing the thermal arrest technique, have been per-
some early works on fresh MOX reported by Bonnerot [15] (Van formed on irradiated fast reactor MOX fuel [25,30–32], on fresh
Craeynest et al. (1968), Weilbacher (1972), Laskiewicz et al. (1971)), MOX [29,33], and on both fresh and irradiated MOX [34,35].
again showing conflicting results. Weilbacher measurements high- More recent experimental campaigns employed rhenium melt-
light a constant effect of the deviation from fuel stoichiometry ing capsules (at least with an inner rhenium layer), to avoid the
(i.e., from oxygen-to-metal ratio, O/M, equal to 2.00) on the ther- distortion of the measured melting temperature [33,35]. Neverthe-
mal conductivity over the entire temperature range (from 800 to less, the most up-to-date experimental technique uses laser heat-
30 0 0 K), while Van Craeynest et al. and Laskiewicz et al. agree on a ing of the sample (e.g., [36,37]), leading to accurate measurements
substantial effect on hypo-stoichiometric fuel at low temperatures, performed on fresh MOX fuel with high Pu content [23,38–40]
(up to 90 mol.%) and featuring also a small inclusion of americium
1 (up to 3.5 mol.%) [40]. Experimental results on Am-MOX are also
The term MOX is herein used referring both to the (U,Pu)O2 homogeneous fuel
envisaged for fast reactor applications and to the heterogeneous uranium and plu- included in older works by Konno et al. [32,34] and Kato et al.
tonium mixed oxide fuel employed in LWRs. [33] (americium content up to 0.9 and 3.3 mol.%, respectively).
 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410 3

Table 1
List of selected experimental data of fresh and irradiated MOX thermal conductivity, including details about the fuel material and the experimental technique employed.

Fresh MOX fuel

Reference Measured fuel Experimental technique

Bonnerot, 1988 (reported Fresh MOX, 95% TD, [Pu] = 20 wt.%, O/M = 1.98, measured Laser-flash method for thermal diffusivity and drop calorimetry
by Carbajo et al., 2001) at T between 1500 and 2260 K (high temperature data). technique for specific heat capacity; conversion to thermal
[19] conductivity. O/M determined by means of thermogravimetric and
XRD analyses.
Ronchi, 1998 (reported by Fresh MOX, 95% TD, [Pu] = 5 wt.%, O/M = 2.00, measured Laser-flash method for thermal diffusivity and drop calorimetry
Carbajo et al., 2001) [19] at T between 2050 and 2700 K (high temperature data). technique for specific heat capacity; conversion to thermal
conductivity.
Staicu et al., 2013 [22] Fresh SBR, sol-gel and MIMAS heterogeneous LWR MOX, Shielded laser-flash device for thermal diffusivity, specific heat
94.5–96% TD, [Pu] = 4.8 to 11.1 wt.%, O/M ∼ 2.000, capacity assumed equal to fresh fuel values from [18, 44]; conversion
measured at T from 500 to 1550 K. to thermal conductivity. Heat treatment was used to obtain
stoichiometric samples (uncertainty of 0.003).
TRABANT (ESNII+ D7.34, Fresh TRABANT MOX fuel: density from ∼93 to 95% TD, Immersion technique for the density, Differential Scanning
2017) [24] [Pu] 40 and 45 mol.%, O/M from 1.96 to 2.00, measured at Calorimetry for the specific heat capacity, laser-flash method for the
T between 500 and 1600 K. thermal diffusivity; conversion to thermal conductivity. O/M
determined by thermal treatment: deduced from the pellet weight
variation and checked with XRD.
PHENIX (ESNII+ D7.41, Fresh PHENIX MOX fuel: 95% TD, [Pu] = 24 mol.%, Differential Scanning Calorimetry for the specific heat capacity,
2017) [23] O/M = 2.00, measured at T between 500 and 1600 K. laser-flash method for the thermal diffusivity; conversion to thermal
conductivity. O/M ratio measured by means of optimized
thermogravimetric analysis, with uncertainty of 0.002 (at 95%
confidence level).

Irradiated MOX fuel

Reference Measured fuel Experimental technique

Yamamoto et al., 1993 Irradiated (U,Pu)O1.97 (8, 19, and 35 GWd/tHM) at LHR Laser-flash method for thermal diffusivity, thermal conductivity
[25] from 12 to 38 kW/m, with fresh fuel density 93–94% TD, obtained from thermal diffusivity, specific heat capacity and density.
[Pu] ∼18 wt.%.
NESTOR-3 (ESNII+ D7.42, Irradiated NESTOR-3 MOX fuel (84 and 130 GWd/tHM), Laser-flash method for the simultaneous measurement of thermal
2017) [26] 96% TD, [Pu] = 24 mol.%, O/M = 2.00, measured at T diffusivity and specific heat capacity (with calorimeter in sample
between 500 and 1600 K. position); conversion to thermal conductivity.

An extensive review of experimental and modelling works ded- for their integral validation against data from the HEDL P-19 fast
icated to MOX melting temperature has been recently performed reactor irradiation experiment. This work represents an advance-
by Calabrese et al. [41], highlighting the importance of the oxygen- ment with respect to the state of the art in fuel performance codes
to-metal ratio for the melting behaviour of MOX fuel, especially in from the property modelling point of view, towards the extension
the high Pu concentration domain, and the prominent role played of FPCs to fast reactor conditions, validation against irradiated MOX
by the plutonium content in MOX fuel for fast breeder reactor ap- fuel data, and application to safety analyses on Generation IV reac-
plications. The effect of the O/M ratio (in the hypo-stoichiometric tor concepts.
range), resulting from the literature review, is currently deemed The paper is organized as follows. The correlations for fast re-
negligible for burn-up values beyond 50 GWd/tHM, where the fuel actor MOX thermal conductivity and melting temperature are de-
stoichiometry is typically reached. For what concerns the burn-up rived, statistically assessed, validated against separate-effect MOX
effect on the MOX melting temperature, it is believed to saturate experimental data and compared with state-of-the-art models in
at high burn-up, justified by the observed decrease of soluble fis- Section 2 and Section 3. The integral validation against a fast reac-
sion products in the fuel matrix [34]. It is indeed considered that tor irradiation experiment is performed in Section 4, showing the
the MOX solidus temperature decreases by 5, 4, and 3 K per 10 accuracy of the code predictions with respect to measured quanti-
GWd/tHM at 50, 100 and 150 GWd/tHM, respectively, as suggested ties of engineering interest. Conclusions are drawn in Section 5.
by [34], and in agreement with [25, 31]. Based on these consid-
erations, a limited number of correlations have been developed to 2. Correlation for thermal conductivity of fast reactor MOX fuel
describe the evolution of the melting temperature of MOX fuels
[6,28,31,32,42,43]. The most comprehensive correlation was pro- The first step towards the proposal of a novel thermal conduc-
posed by Konno et al., considering the dependence on fuel pluto- tivity correlation for fast reactor MOX is the selection of the best
nium and americium contents, burn-up and oxygen-to-metal ratio set of experimental data, i.e., composed of measurements recently
[32]. obtained from up-to-date techniques and covering wide ranges of
Considering the state of the art just recalled, the present work the considered dependencies, as explained in what follows. For
aims at overcoming the current limitations of thermal properties fresh MOX fuel, the selected thermal conductivity data are those
modelling of U-Pu MOX fuel in fuel performance codes. More pre- from [22] and from PHENIX and TRABANT MOX samples (obtained
cisely, the aim is to develop original and more comprehensive in the frame of the ESNII+ Project [23,24]). These most recent
models of thermal conductivity and melting temperature of MOX datasets correspond to low temperature (up to 1650 K), deviation
fuels, applicable to fast reactor irradiation conditions, inclusive of from stoichiometry up to 0.04 (in the hypo-stoichiometric range
all the fundamental dependencies (i.e., fuel temperature, burn-up, [24]) and Pu content ranging from 5 wt.% [22] to 45 wt.% [24], cov-
plutonium content, stoichiometry, porosity), and valid up to high ering both the low and high-Pu regions. Given the lack of recent
temperatures, plutonium contents and burn-up, as required for high-temperature data, older data from Ronchi et al. (1998) and
several Generation IV reactor concepts. The new correlations have Bonnerot et al. (1988) (reported by [19]), still considered as a ref-
been first statistically assessed based on the regressor p-values erence in the field, are included in the fitting dataset. As for irra-
to include all the effects represented by the fitting dataset, and diated fast reactor MOX fuel, the recent ESNII+ Project measure-
then implemented in the TRANSURANUS fuel performance code ments on NESTOR-3 MOX fuel [26], corresponding to high burn-up
4 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410

(i.e., 84 and 130 GWd/tHM), have been selected, together with data Table 2
Results of the fit of the statistically
by Yamamoto et al. [25]. The latter have been employed to derive
assessed k0 (T, x, [Pu], p) correlation
a correlation holding also at low and moderate burn-up (samples (Eq. 2) on the whole set of fresh MOX
at 8, 19 and 35 GWd/tHM). It is worth specifying that these are the thermal conductivity data (Table 1).
only data currently accessible by the authors on thermal conduc-
Regressor Units Estimate
tivity of irradiated fast reactor MOX fuel. Details about the MOX
thermal conductivity data selected are given in Table 1. A0 m•K/W 0.01926
Ax m•K/W 1.06 10−6
First, a novel correlation for fresh MOX thermal conductiv-
APu m•K/W 2.63 10−8
ity (k0 ) is fitted. For this purpose, a physically grounded model B0 m/W 2.39 10−4
k0 (T, x, [Pu], p) is chosen (Eq. 1). The model encompasses the three BPu m/W 1.37 10−13
fundamental mechanisms of heat transport in a solid. The first cor- D W•K/m 5.27 10+9
E K 17109.5
responds to heat transfer via lattice vibration (phononic) and is
dominant at low temperatures. The second and third term corre-
spond to radiative and electronic heat transfer, and dominate at
high temperatures. This basic model is then corrected with the in-
from the hypothesis test, like all the results of the fitting proce-
clusion of plutonium and stoichiometry-dependent terms in the
dure, inherently depend on the chosen fitting dataset. The regres-
lattice contribution, and of a porosity corrective factor as well.
sor initial values, needed by the non-linear fitting procedure, are
Specifically, the stoichiometry and plutonium content effects are
fixed to the values employed by existing correlations for the same
conventionally introduced in k0 as modifications to the A and B
kind of terms [9,53,54]. The stability and independence of the re-
coefficients of the lattice vibration term (see e.g., [3,4]). Hence, the
sulting fit coefficients (not reported here for sake of brevity) have
functional form of the thermal conductivity correlation for fresh
been tested, proving that they hold true performing further itera-
MOX is:
tions and that the non-linear fitting procedure is slightly affected
 1 D
 by their initial values.
+ C T 3 + 2 e− T (1 − p)2.5
E
k0 (T , x, [P u], p) = (1) The statistical significance of the regressors has been tested
A + BT T
against the entire set of selected experimental data on fresh MOX
with A = A0 + Ax · x + APu · [P u] and B = B0 + Bx x + BPu [P u], where (Table 1), as well as against sub-sets of the selected data, featured
x is the deviation from stoichiometry (x = 2 − O/M, considering by at least one constant dependence amongst the parameters of in-
hypo-stoichiometric fuel), [Pu] is the MOX plutonium content, terest (T, x, [Pu]). The aim of these partial fits is to achieve higher
while (1 − p)2.5 is the modified Loeb porosity corrective factor, confidence on the significance of each correlation regressor, focus-
adopted e.g., in the Van Uffelen-Schubert correlation, the reference ing only on the p-values. The fit of the starting k0 over all the se-
model in the TRANSURANUS fuel performance code [6]. A0 , Ax , APu , lected fresh MOX data shows p-values lower than 5% for the fit
B0 , Bx , BPu , C, D, E are the coefficients to be fitted on the selected coefficients A0 , B0 , BPu , D, E (< 10−8 , < 10−16 , 1.5%, 4%, < 10−14 , re-
set of fresh MOX experimental data. spectively), while higher than 5% for Ax , APu , Bx , C (39%, 10%, 46%,
The linear dependency on the deviation from stoichiometry dif- 25%, respectively, values depending on the experimental ranges
fers from the square root term proposed by a few existing corre- covered by the data composing the fitting dataset). Amongst these,
lations for MOX fuel [9,17], for UO2 [45,46] and emerging from the regressors Ax and APu are kept in the final formulation, since Ax
Molecular Dynamics calculations (e.g., [47]), but is supported by has a p-value on the sub-set of (T, x)-dependent data (14%) much
the majority of state-of-the-art models available in literature and lower than Bx (75%), while APu is well represented by the sub-set
in fuel performance codes [10,15,16,18,19]. As for the inclusion of of (T, [Pu])-dependent data (p-value lower than 5%). Additionally,
the plutonium effect in this work, it is in contrast with previous the results of the partial fits confirmed the exclusion of the regres-
works that excluded it, in the ranges 3–15 [18] and 15–30 [9] wt.% sors Bx and C2 , since they are featured by p-values much higher
PuO2 . Indeed, its inclusion finds confirmation in experimental and than 5%, both on the entire set and on the sub-sets (i.e., on the
modelling works on MOX [15,22], and also in theoretical works sub-sets of data corresponding to low temperature and constant p
about thermal diffusivity and conductivity of various types of ma- and [Pu], and to high temperature, respectively).
terials and nuclear fuels [48–50]. The assessed form of the novel correlation for fresh MOX ther-
mal conductivity reads:
 
1 D
( 1 − p )2 . 5
E
k0 (T , x, [P u], p) = + 2 e− T (2)
A0 + Ax · x + APu · [P u] + (B0 + BPu [P u] )T T

The fit of the statistically assessed k0 (Eq. 2) on the complete

set of selected fresh MOX data leads to the results collected in
In addition to the straightforward fitting, the statistical signifi- Table 2. The final regressor values have been obtained imposing
cance and weight of each term of the correlation have been anal- their positivity as constraint, in order to guarantee a physically
ysed and evaluated. The multi-dimensional fit has been performed grounded significance. All the included effects degrade the ther-
using MATLAB tools [51] and the R code [52], to obtain (besides mal conductivity, as expected from experimental observations (re-
the regressor values) the associated p-values, along with the confi- ported in Table 1 and in other literature works, e.g., [15,20,21]) and
dence intervals and the fit residuals. The significance of each term theoretical considerations about phonon interactions with lattice
of the starting correlation has been evaluated taking the p-value defects. The coefficient values reported in Table 2 hold for T ex-
associated to each regressor as figure of merit (compared to a
threshold p-value of 5%, corresponding to a 95% confidence on the
significance of a regressor). In this way, in the framework of a sta-
2
tistical hypothesis test, a regressor is kept in the final form of the The radiative contribution to the thermal conductivity, CT3 , dominates at very
high temperatures, a region where the available MOX thermal conductivity experi-
correlation if the associated p-value is below 5%, otherwise it is mental data are scarce. Instead, the exclusion of the regressor Bx is physically justi-
rejected as statistically insignificant (i.e., not well represented by fied by the fact that B describes the phonon-phonon collisions, while A depends on
the fitting dataset). It is worth clarifying that the p-values obtained impurities or alloying additions, so it is apt to include the fuel stoichiometry effect.
 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410 5

Table 3
Values of the coefficients of the kirr (T, x,
[Pu], p, bu) correlation (Eq. 3), fitted on
the set of irradiated MOX thermal con-
ductivity data [25,26].

Regressor Units Estimate

kinf W/(m•K) 1.755

ϕ GWd/tHM 128.75

at extended burn-up values, pointing out the thermal conductivity

degradation [61]. This is attributed to the accumulation of point
defects and fission products, which increase the phonon scatter-
ing (represented by the A term in the lattice thermal conductivity
model), although thermal conductivity degradation was indicated
to saturate beyond approximately 50 GWd/tHM in the mid-1990s
Fig. 1. Experimental data on fresh MOX thermal conductivity (considered as fit
dataset, Table 1, blue dots), as a function of temperature, compared to the corre- [62]. The correlation hence reads
sponding predictions provided by the correlation developed in this work (orange   bu

dots, Eq. 2 and Table 2). (For interpretation of the references to colour in this figure kirr (T , x, [P u], p, bu) = kin f + k0 (T , x, [P u], p) − kin f · e− ϕ (3)
legend, the reader is referred to the web version of this article.)
where k0 (T, x, [Pu], p) is the fresh MOX thermal conductivity cal-
culated with Eq. 2 (employing the coefficient values collected in
Table 2), bu is the fuel burn-up in GWd/tHM, kinf is the asymp-
pressed in K, [Pu] in atomic fraction, p in TD fraction. The thermal totic thermal conductivity at high burn-up based on the only two
conductivity k0 is calculated in W/(m•K). available sets of experimental data on irradiated fast reactor MOX
The obtained effect of plutonium content and deviation from thermal conductivity [25,26], ϕ is the correlation coefficient fit-
stoichiometry (in the hypo-stoichiometric range) on the MOX ther- ted on [25,26] (see Table 1). This formulation is still applicable
mal conductivity is minor if compared to the temperature ef- to fresh MOX fuel, since at zero burn-up kirr (T , x, [P u], p, bu) =
fect, as results from the coefficient values reported in Table 2. k0 (T , x, [P u], p), from Eq. 3. The asymptotic lower limit for the ther-
Indeed, the values of Ax , APu and BPu are orders of magnitude mal conductivity degradation with burn-up (kinf ), in principle de-
lower than A0 and B0 , which are the basic coefficients compos- pending on plutonium content, deviation from stoichiometry and
ing a lattice vibration contribution to thermal conductivity only porosity of the fuel of interest, has been fixed based on the avail-
dependent on temperature. A slight effect of the plutonium con- able experimental data. Its value is derived from an extrapolation
tent, in the range between 0 and 45 wt.%, is supported by litera- of the experimental behaviour of thermal conductivity from Ya-
ture works concerning both LWR [18] and FBR MOX [9], and by mamoto and NESTOR-3 data [25,26], at the highest common tem-
the recent measurements on TRABANT fresh MOX fuel performed perature of measurement (i.e., 1480 K, corresponding to the lowest
in the framework of the ESNII+ H2020 Project [24]. Instead, the thermal conductivity data), to a burn-up of 200 GWd/tHM, consid-
effect of deviation from stoichiometry reveals negligible due to the ered as limit fuel burn-up for Generation IV reactor applications
lack of data points, amongst the available ones, associated to a sig- [11,63]. The correlation coefficients are collected in Table 3, includ-
nificant hypo-stoichiometry. Indeed, most of the fresh MOX data ing the value of ϕ resulting from data fitting.
correspond to material stoichiometry, also due to measurement The agreement between the correlation predictions (Eq. 3) and
conditions leading to O/M = 2.00 [22,23]. The availability of addi- the data of irradiated MOX thermal conductivity by Yamamoto
tional experimental data would allow to further assess the hypo- [25], shown in Fig. 2, is satisfactory. Considering also NESTOR-3
stoichiometry impact on the MOX thermal conductivity. data [26] (not reported in Fig. 2 since confidential), the overall av-
The comparison between the thermal conductivity data on erage residual is ∼ 10%, compared to an experimental uncertainty
which the k0 (T, x, [Pu], p) correlation (Eq. 2) has been built and the which is ∼ 8% and ∼ 30% for NESTOR-3 and Yamamoto’s datasets,
fit estimations, as a function of temperature, is shown in Fig. 1. It is respectively.
worth noting that the agreement between data and estimations is From Fig. 2, it is worth noticing that the thermal conductivity
remarkable, both at low and high temperatures. The average resid- values predicted by the new correlation lie inside a 20% error band
ual is 2•10−1 W/(m•K), comparable with the experimental uncer- with respect to Yamamoto’s experimental measurements. More-
tainty, which for these data is between 10% and 20% of the mea- over, the agreement is even better (10% maximum deviation) in the
sured value [19,22–24]. It has been verified that the fit residuals range of thermal conductivity values between 2 and 2.5 W/(m•K)
in T, x, [Pu] are all randomly distributed, with no clear trends. This (circled in Fig. 2), corresponding to the target temperature and
excludes the necessity to correct the fresh MOX thermal conduc- burn-up conditions foreseen for Generation IV fast reactors, i.e.,
tivity correlation herein derived with mixed effects terms (present peak fuel temperature in excess of ∼ 2300 K and discharge fuel
in some existing thermal conductivity correlations [42,55–57]) or burn-up of 150 - 200 GWd/tHM [11,63]. The ranges of applicabil-
additional higher order terms. Such improvements would only be ity of the newly developed correlations for MOX fuel thermal con-
justified in the case of a trend of the associated residuals. Data as- ductivity, corresponding to the ranges covered by the considered
similation techniques such as Bayesian calibration methods (e.g., experimental data, are:
[58]) could then be considered in the future for dealing with po- • Temperature, T: [500, 2700] K.
tential model inadequacies, when more experimental data become • Deviation from stoichiometry, x: [0, 0.04] (hypo-stoichiometry).
available. • Plutonium content, [Pu]: [0, 45] at.%.
In the following step of the model development, an exponential • Porosity, p: [0, 7] %.
degradation with fuel burn-up is chosen as functional form for the • Burn-up, bu: [0, 130] GWd/tHM.
thermal conductivity correlation of irradiated MOX fuel (kirr , Eq. 3).
This is derived from the vast amount of data generated and partly The main limitation of the developed correlation is therefore
provided in the HRP [59] and IFPE [60] databases for LWR fuels the range of discharge burn-up, which may exceed 130 GWd/tHM
6 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410

Fig. 4. Validation of the thermal conductivity correlation developed in this work

against experimental data on fresh MOX, from Bonnerot [15] and reported by Inoue
[17].
Fig. 2. Comparison between the irradiated MOX thermal conductivity data by Ya-
mamoto [25] and the corresponding predictions given by the novel correlation for
irradiated MOX (Eq. 3). The points circled in orange correspond to the range of ther-
mal conductivity values foreseen during the operation of Generation IV reactors, for
which the correlation predictions are most accurate. (For interpretation of the ref-
erences to colour in this figure legend, the reader is referred to the web version of An independent validation of the new MOX thermal conductiv-
this article.)
ity correlations is provided in Fig. 4. The sets of experimental data
on fast reactor MOX considered for validation, independent from
the ones composing the fitting set, are from Bonnerot [15] and
Inoue [17], reporting older data on fast reactor MOX from Het-
zler (1967), Van Craeynest (1968), Laskiewicz (1971), Fukushima
(1983), Elbel (1985 and 1988). Bonnerot provides measurements
at temperatures between 973 and 2473 K of fresh U-Pu mixed ox-
ides, hypo-stoichiometric with O/M ratio between 1.967 and 1.99,
with Pu contents from 5 wt.% to ∼ 30 wt.% and porosity between
∼ 3% and ∼ 9%. Measurements collected by Inoue (normalized to
100% TD) concern fresh MOX fuel at temperatures between 350
and 2500 K, with Pu content from 20 to 25 wt.%, O/M ratio from
1.96 to 1.99. The cloud of points mostly lays in a 30% deviation
band with respect to the experimental values, with a significant
amount of predictions inside the 10% deviation region (correspond-
ing to the best experimental uncertainty on fresh MOX thermal
conductivity, from recent works [23,24]). Predicted values which
Fig. 3. Temperature behaviour of the MOX thermal conductivity correlation devel- over-estimate the measured ones by more than 30% correspond
oped in this work (blue dots), compared to the main state-of-the-art correlations to the lowest temperatures of the datasets, i.e., closer to 500 K,
for MOX fuel (Philipponneau [9] and Van Uffelen-Schubert [6]). These values refer which is the lower limit of validity of the herein proposed ther-
to stoichiometric MOX, i.e., x = 0, with 20 at.% initial Pu content and 5% porosity, at
10 GWd/tHM burn-up. (For interpretation of the references to colour in this figure
mal conductivity correlation, and below the commercial range of
legend, the reader is referred to the web version of this article.) interest for FBR MOX fuels. Instead, the agreement with data mea-
sured at high temperatures (above 1600 K), included in the op-
erative condition range of fast and Generation IV future reactors,
in Generation IV fuel types. Nevertheless, data assimilation tech- is remarkably good, since the maximum calculated deviation is ∼
niques could be envisaged for a progressive upgrade of the corre- 20% of the experimental value. An independent validation against
lation, as soon as more experimental data on representative irradi- thermal conductivity data on irradiated fast reactor MOX could
ated FBR MOX fuels become available. not be performed, since data other from those used for the fit
In Fig. 3, the behaviour of the new MOX thermal conductiv- [25,26] are not available in the open literature or not accessible
ity correlation as a function of fuel temperature is compared with to the authors. Fig. 5 shows the frequency distribution of the rela-
two main correlations from literature, by Philipponneau [9] and tive differences between the values calculated employing the MOX
Van Uffelen-Schubert ([6], developed for LWR MOX). Results re- thermal conductivity correlation developed in this work and the
fer to stoichiometric MOX, i.e., x = 0, with 20 at.% initial Pu con- experimental data, from Bonnerot [15] and Inoue [17]. For most of
tent and 5% porosity, at 10 GWd/tHM burn-up. The new correla- the correlation predictions (∼ 60% and ∼ 90% of the entire Bon-
tion predicts the highest thermal conductivity values at low tem- nerot and Inoue datasets, respectively), the relative percentage er-
perature, while the three correlations all provide values between 2 ror with respect to the experimental data is below 20%, hence
and 2.5 W/(m•K) at 2500 K. Table 4 reports the root mean square comparable with the state-of-the-art experimental uncertainty on
errors of the three correlations considered, compared to the en- MOX thermal conductivity (reported between 10 and 20% of the
tire set of fitted thermal conductivity experimental data (concern- measured value, as previously mentioned). The largest deviations
ing both fresh and irradiated MOX, Table 1). The error of the cor- are observed for the lower temperature values (between 350 and
relation developed in this work is less than half the error of the 1200 K, hence below the temperature range relevant for FBR MOX
two state-of-the-art correlations herein considered for comparison fuel during irradiation) and correspond to the points outside the
[6,9]. 30% deviation band in Fig. 4.
 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410 7

Table 4
Root mean square error of the MOX thermal conductivity correlation developed in this work, com-
pared to the main state-of-the-art correlations for MOX fuel, over the entire set of data considered in
this work (both fresh and irradiated MOX, Table 1).

Philipponneau [9] Van Uffelen-Schubert [6] This work

Root mean square error (rmse) 0.33 0.34 0.16

Fig. 5. Frequency distribution of the relative differences between calculated values (from the MOX thermal conductivity correlation developed in this work) and experimental
data, from Bonnerot ([15], left) and Inoue ([17], right). The figure also reports the number of data points analysed and the root mean square error (rmse) of the correlation,
compared to the two experimental datasets.

3. Correlation for melting temperature of fast reactor MOX fuel ted to the selected data:

Tm,0 ([P u], [Am], x ) = Tm,U O2 − γPu [P u] − γAm [Am] − γx x (4)

The procedure employed to derive a novel, more comprehen-
sive correlation for MOX melting temperature for fuel performance where Tm,U O2 is the fresh UO2 melting temperature (i.e., 3147 K,
codes is similar to the one adopted for the thermal conductivity according to recent experimental measurements by Manara et al.
correlation. The most recent melting temperature data, obtained [66], recommended by the ESNII+ Catalogue on MOX properties
through reliable experimental techniques (laser heating and ther- [43]), [Pu] and [Am] are the plutonium and americium contents (in
mal arrest in rhenium-coated tungsten capsule), have been se- at./), respectively, x is the deviation from fuel stoichiometry. γ Pu ,
lected as best (most accurate) fitting dataset. In line with the γ Am , γ x are the regressors associated to each effect, to be fitted
considerations reported in Section 1, measurements performed on on the selected fresh MOX melting temperature data. In view of
samples inside a tungsten capsule have been excluded from the the limited set of experimental data, a linear dependency on each
fitting dataset. Moreover, data concerning MOX fuel for fast re- parameter, known to affect (decrease) the melting temperature, is
actor applications have been considered, while allowing to cover assumed, and each effect is considered as independent (i.e., addi-
wide ranges of plutonium contents and deviations from stoi- tive to each other). An americium effect is initially considered since
chiometry (in the hypo-stoichiometric range). Hence, as for fresh some of the considered works ([33], [40]) include data on Am-
MOX, selected data (including two points from PHENIX fuel, ob- bearing fresh MOX fuel, which is of interest for Generation IV type
tained in the framework of the ESNII+ Project) are taken from of fuels. Nonetheless, the Am effect proves to be badly represented
[23,33,35,39,40,64]. Data from [33,39] corresponding to very high by the chosen fitting dataset (p-value greater than 5%), since too
plutonium contents (> 50 wt.%) or to strong hypo-stoichiometry few data from too low content Am-MOX samples are available4 .
(around 1.90) have been excluded from the fitting dataset, since Instead, the statistical analysis (performed again through the R
out of the range of interest of the present work (i.e., plutonium code [52]) indicates that the plutonium and stoichiometry effects
content up to 50 wt.% and deviation from stoichiometry up to must be included in the fresh MOX melting temperature correla-
0.06). Instead, the only suitable data about irradiated fast reactor tion, since the p-values associated to their regressors are very low
MOX are provided by Konno et al. [32]3 . The experimental points (∼ 10−13 and 1.3%, respectively).
selected for the fit are collected in Table 5. As a result of the statistical analysis, the proposed form of the
Previous experimental studies already indicated that both the fresh MOX melting temperature correlation reads:
plutonium content (at least up to 50 wt.%) and the deviation from
stoichiometry decrease the MOX melting temperature with re- Tm,0 ([P u], x ) = Tm,U O2 − γPu [P u] − γx x (5)
spect to fresh, stoichiometric UO2 [32,34,42,53]. A recent theoret- The fit of Eq. 5 over the complete fitting dataset on fresh MOX
ical analysis based on Molecular Dynamics calculations also con- (Table 5) leads to the coefficient values reported in Table 6, hold-
firms this effect of plutonium content in mixed oxides [65]. There- ing for Tm,U O2 expressed in K and [Pu] expressed in atomic frac-
fore, a correlation with the following starting functional form for tion. The analysis of the residual trends does not suggest the intro-
the melting temperature of fresh MOX fuel (Tm,0 ) has first been fit- duction of higher order or mixed terms (instead present in Konno
et al. correlation, involving, e.g., a squared dependence on the plu-
tonium content [32]), since the fit residuals are always randomly
3
This statement is supported by the fact that it is the only work in the open
4
literature reporting the actual values of fuel stoichiometry and plutonium content at An americium effect is represented in the Konno et al. correlation [32], based
the sample burn-up. For this reason, melting temperature data for irradiated MOX on the ideal solution model and obtained performing experimental regression anal-
reported by [35] have been excluded by the fitting dataset. ysis under the hypothesis of additive effects.
8 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410

Table 5
List of selected experimental data of fresh and irradiated MOX melting temperature, including details about the fuel materials and the experimental technique employed.

Fresh MOX fuel

Reference Measured fuel Experimental technique

Kato et al., 2008 [33] Fresh MOX, O/M = 2.000, Pu content from 29.7 to 46.3 Sample heating in a rhenium capsule, analysis of pyrometer
mol.%, Am content from 0.3 to 3.3 mol.%. thermograms. Stoichiometric samples obtained adjusting to 2.00 by
annealing at 1023 K for 5 h at the oxygen potential of ∼ -400 kJ/mol.
Hirosawa et al., 2011 [35] Fresh FR MOX with O/M = 1.99 and Pu content of 31.8 Sample heating in an inner rhenium capsule and outer tungsten
mol.%. capsule, Thermal Arrest technique. O/M measured with the
oxidation–reduction gravimetric method.
Bohler et al., 2014 [39] Fresh MOX, O/M = 2.00, Pu content from 3.7 to 50 mol.%. Laser Heating and analysis of pyrometer thermograms. Fuel
stoichiometry characterized by means of XRD, XANES and Raman
analyses.
Prieur et al., 2015 [40] Fresh MOX, O/M = 1.98, Pu content = 22 mol.%, Am Laser Heating and analysis of pyrometer thermograms. O/M ratio
content = 3.5 mol.%. determined from XANES analyses, with uncertainty of 0.01.
Strach et al., 2016 [64] Fresh MOX, O/M = 2.00, Pu content from 14 to 54 wt.%. Thermal Arrest technique on samples obtained from UO2 and PuO2
powders. Measurements in Ar atmosphere. Stoichiometry was
achieved by atmosphere control during sintering and verified by
powder XRD measurements.
PHENIX (ESNII+ D7.41, Fresh PHENIX MOX, 95% TD, Pu content = 24 mol.%, Laser Heating and fast multi-channel pyrometer. O/M ratio measured
2017) [23] O/M = 2.00 (stoichiometric) and 1.978 (hypo). by means of optimized thermogravimetric analysis, with uncertainty
of 0.002 (at 95% confidence level).

Irradiated MOX fuel

Reference Measured fuel Experimental technique

Konno et al. 2002 [32] Irradiated MOX with burn-up between 8.2 and 110.9 Thermal Arrest technique on sample in a tungsten capsule. Actual
(reports also data by GWd/tHM, O/M = 1.98, Pu content ∼ 17.5 mol.%, Am values of O/M ratio of irradiated samples calculated from the given
Tachibana et al. 1985 and content between 0.13 and 0.16 mol.%. as-fabricated values, by means of a linear increasing O/M model
Komatsu et al. 1988) dependent on the enrichment in 235 U and on burn-up.

Table 6 on fresh MOX melting temperature, which is between 30 and 70 K

Results of the fit of the statisti-
[23,33,35,39].
cally assessed Tm, 0 ([Pu], x) correla-
tion (Eq. 5) on the whole set of the In a second step, the correlation for irradiated MOX melting
selected fresh MOX melting temper- temperature is derived by fitting a burn-up dependant function,
ature data. including Tm, 0 ([Pu], x) (Eq. 5, with regressor values in Table 6), to
Regressor Units Estimate the selected data for irradiated fuel [32]. To account for the burn-
up effect, which also degrades the MOX melting point with respect
γ Pu K / at./ 364.85
to the fresh material [32,34,35], an exponential functional form is
γx K 1014.15
again adopted. This has been chosen because the effect of burn-
up reflects the continuous build-up of defects and fission prod-
ucts, which evolves towards saturation [34], and recent Molecu-
lar Dynamics calculations of the melting temperature in mixed ox-
ides [65] suggest a decrease of the melting temperature when a
few atom percent of foreign atoms are introduced in the lattice.
This has been ascribed to a decreasing Frenkel formation energy
in MOX, in turn caused by a lattice mismatch due to the foreign
atoms up to a few percent. The burn-up range considered in this
work is of the order of few atom percent (up to ∼ 110 GWd/tHM),
hence the functional form chosen for the irradiated MOX melting
temperature correlation is written as:
  bu
Tm,irr (bu, [P u], x ) = Tm,in f + Tm,0 − Tm,in f · e− δ (6)
where bu is the fuel burn-up in GWd/tHM, Tm, 0 is the melting
temperature of the fresh fuel according to Eq. 5, while Tm, inf and δ
are the correlation regressors to be fitted. This formulation is con-
sistent with Tm,irr = Tm,0 when the fuel burn-up is equal to zero.
Fig. 6. Comparison between the fresh MOX melting temperature data and the cor-
responding predictions given by the correlation fitted on these data (Eq. 5). (For in-
Fitting this functional form to the irradiated MOX data [32] leads
terpretation of the references to colour in this figure legend, the reader is referred to the regressor values reported in Table 7. The comparison be-
to the web version of this article.) tween the values predicted by the new correlation (Eq. 6) and the
corresponding experimental values is shown in Fig. 7. The aver-
age deviation from the experimental data is around 15 K, compara-
distributed if plotted against [Pu], [Am] or x. The comparison be- ble with the experimental uncertainty reported for irradiated MOX
tween the experimental data and the corresponding values pre- melting temperature (between 10 and 30 K) [32]. The agreement
dicted by the new fresh MOX melting temperature correlation is between calculated and measured values is even better consider-
shown in Fig. 6. ing the experimental uncertainties, as most of the error bars re-
Fig. 6 shows that the agreement between experimental and fit- ported in Fig. 7 include the perfect agreement, represented by the
ted melting temperature values is acceptable, despite some rele- plot diagonal. The ranges of applicability of the newly developed
vant deviations up to 50 K. Nevertheless, the maximum residual correlations for MOX fuel melting temperature, corresponding to
is absolutely comparable with the high experimental uncertainty the ranges covered by the considered experimental data, are:
 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410 9

Table 7 In Fig. 8, the behaviour of the MOX melting temperature corre-

Results of the fit of the Tm, irr (bu,
lation derived in this work, as a function of (a) plutonium content
[Pu], x) correlation (Eq. 6) over the se-
lected irradiated MOX melting tempera- (considering stoichiometric fuel at 10 GWd/tHM) and (b) fuel burn-
ture data. up (considering stoichiometric fuel with 30 at.% initial Pu content),
is compared with two main state-of-the-art correlations, Konno
Regressor Units Estimate
et al. [32] and MATPRO ([42], valid for UO2 and LWR MOX). The
Tm,inf K 2964.92 behaviour of the two state-of-the-art correlations considered for
δ GWd/tHM 40.43
comparison is sensibly different and predicted values differ by
more than one hundred degrees. The new correlation for Tm, irr
provides values between the two state-of-the-art correlations, es-
pecially in terms of plutonium degradation effect. The effect of
plutonium in the MATPRO correlation is negligible, while Konno
et al. correlation is featured by a stronger degradation (decrease)
of the predicted melting temperature with increasing plutonium
content (at 10 GWd/tHM burn-up, as showcased in Fig. 8a). This
could be due to the fact that the plutonium content effect in the
Konno et al. correlation [32] is based on quite old and low (down
to 2850 K at 50 at.% Pu) experimental data on MOX fuels, provided
by Lyon and Baily [27] and by Aitken and Evans [28]. The burn-up
effect is derived by Konno by fitting Japanese experimental data
from JOYO reactor campaigns, reported in his same work [32]. In-
stead, the novel correlation herein proposed is based on a wider
dataset, composed of recent and up-to-date literature works from
various authors (including Konno’s data for the burn-up effect),
showing experimental data of MOX melting temperature which are
higher in value (never lower than 2950 K, as shown in Figs. 6 and
Fig. 7. Comparison between the irradiated MOX melting temperature data and the 7). The correlation developed in this work is featured by its char-
corresponding predictions given by the correlation fitted on these data (Eq. 6). The
acteristic decreasing exponential trend in burn-up (Eq. 6), which
experimental uncertainties, as provided by the original references [30–32], are in-
cluded as horizontal error bars. (For interpretation of the references to colour in leads to higher predicted values at high burn-up. This could be
this figure legend, the reader is referred to the web version of this article.) justified by the fact that, at such burn-up values, either the high
burn-up structure formation in the low temperature fuel region is
accompanied by a reduction of the fission products in the lattice
(observed by means of EPMA [67–69]), or a large fractional release
• Deviation from stoichiometry, x: [0, 0.06] (hypo-stoichiometry). of fission products occurs in FBR MOX fuels in the high temper-
• Plutonium content, [Pu]: [0, 50] at.%. ature region. Table 8 reports the root mean square errors of the
• Burn-up, bu: [0, 110] GWd/tHM.

Fig. 8. Behaviour of the MOX melting temperature correlation herein presented (blue dots), as a function of (a) plutonium content and (b) burn-up, compared to two main
state-of-the-art correlations for MOX fuel (Konno et al. [32] and MATPRO [42]). The calculated values, in both graphs, refer to stoichiometric MOX, i.e., x = 0, while in (a)
bu = 10 GWd/tHM and in (b) [Pu] = 30 at.%. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)

Table 8
Root mean square error of the MOX melting temperature correlation developed in this
work, compared to the main state-of-the-art correlations for MOX fuel, over the entire
set of herein considered data on fresh and irradiated MOX (Table 5).

Konno et al. [32] MATPRO [42] This work

Root mean square error (rmse) 0.014 0.029 0.0065

10 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410

Table 9
Details about the as-fabricated geometry, materials and boundary conditions of the fuel rods irradiated in the HEDL P-19 experiment (TD = Theoretical
Density, OD = Outer Diameter, LHR = Linear Heat Rate).

Rod ID 3 6 7 8 13 20 24 25 26 27 28 30 33 35

Gap size (μm) 127 49.5 79 122 99 123 127 101.5 76 51 43 89 62.5 91.5
Density (%TD) 92.4 90.75 92.4 90.75 90.75 90.75 92.4 92.4 92.4 92.4 92.4 92.4 90.75 90.75
Clad OD (mm) 6.35 5.84 6.35 5.84 5.84 5.84 6.35 6.35 6.35 6.35 6.35 6.35 5.84 5.84
Fuel 25% PuO2 – 75% UO2
Cladding AISI 316 stainless steel (20% cold-worked)
Filling gas 98% He, 2% Ar at 1 bar
O/M 1.96
Active fuel length 343 mm
Na inlet temperature 640 K
Max LHR (kW/m) 64 56.1 66.6 53.8 54.5 54.1 64.6 66 66.9 66.9 67.9 65.6 55.1 54.1
Melting X X X X X X X X X X X X

three correlations considered, when compared to the entire set of

herein considered experimental data, both on fresh and irradiated
MOX fuel (Table 5). The error of the correlation developed in this
work is much lower than the error of the two main state-of-the-art
correlations [32,42] over the considered data.

4. Application to the HEDL P-19 irradiation experiment and

integral validation

The correlations for MOX thermal conductivity and melting

temperature developed in this work have been implemented in the
TRANSURANUS fuel performance code, for their assessment against
available integral data (i.e., at the fuel pin level). The effect of the
new correlations on fuel pin performance simulations has been
tested against experimental data from the HEDL P-19 irradiation
experiment, and the TRANSURANUS results are discussed in what
follows.
HEDL P-19 is a fast reactor irradiation experiment performed in Fig. 9. Integral validation (orange points) of the new thermal conductivity and
1971 in the EBR-II reactor (sodium-cooled, open pool type) [70]. It melting temperature correlations for fast reactor MOX against power-to-melt data
from the HEDL P-19 irradiation experiment [70]. The results obtained employing
is a power-to-melt test with the objective to investigate the melt-
state-of-the-art TRANSURANUS correlations are also reported (grey points), for sake
ing propensity of 25% PuO2 , fresh MOX fuel, representative of FBR of comparison. Where grey points are not visible, they are exactly covered by or-
pin design. The experiment aimed to simulate fast start-up situa- ange points. (For interpretation of the references to colour in this figure legend, the
tions, typical of FBRs. The irradiation history consisted in a start- reader is referred to the web version of this article.)
ing slow power ramp (10 hours long, up to 85% of the reactor total
power, i.e., 62.5 MW), after which this steady power level is kept
for 2 hours. After the conditioning phase, the reactor is rapidly fuel performance codes and for application to MOX fuel in fast re-
ramped up to full power, which is kept for ∼ 10 minutes, followed actor conditions.
by reactor scram. The maximum burn-up reached by the fuel in The integral validation against the HEDL P-19 power-to-melt
this experiment is ∼ 1 GWd/tHM. Experimental data on 14 pins are data is reported in Fig. 9, showing generally consistent diago-
available in the HEDL P-19 database, regarding the power-to-melt nal trends (higher the experimental data, higher the correspond-
(i.e., the linear power leading to incipient fuel melting, measured ing calculated value). Predictions are mostly similar, but for some
at the top and bottom of fuel column), which is the main outcome HEDL pins more accurate (closer to the plot diagonal, i.e., to the
of interest from the experiment; the radial and axial extents of fuel perfect agreement with the data) from the new thermal conduc-
melting, and some PIE data about the central void size, the radial tivity and melting temperature correlations. Despite the predicted
extent of the columnar grain region and the fuel-to-cladding gap values are contained within the 20% error band from the exper-
size [70–72]. Table 9 summarizes the main relevant as-fabricated imental values, the power-to-melt data are systematically under-
details and boundary conditions of the HEDL P-19 fuel rods. estimated by TRANSURANUS, indicating the conservative behaviour
The simulation of the HEDL P-19 irradiation experiment has of the code. Anyway, the experimental uncertainty on the power-
been performed with the v1m1j18 version of the TRANSURANUS to-melt measurements, which is reported equal to 6% [70], must be
fuel performance code. The results obtained employing the new considered in order to evaluate the accuracy of the TRANSURANUS
thermal conductivity and melting temperature correlations for fast calculations, along with the uncertainties pertaining to the gap
reactor MOX are validated against experimental data and compared conductance and relocation modelling at beginning of life, as
with the results from state-of-the-art correlations implemented in pointed out recently in a code benchmark of the OECD/NEA and
TRANSURANUS (i.e., the Van Uffelen-Schubert correlation for MOX in the ESFR-SMART Euratom project [74,75].
thermal conductivity [6]; as for the melting temperature, a fixed, Fig. 10 shows the integral validation against HEDL P-19 post-
experimental value of 3035 K is considered, which was measured irradiation examination data, concerning the maximum radial ex-
during the HEDL P-19 campaign and provided in the experimental tent of fuel melting (measured at the peak power node, left plot)
reports [70,71,73]). The aim of this analysis is to quantify the im- and the fuel-cladding gap size (right plot). As for the fuel radial
provement in the code predictions on integral quantities brought melting extent, a general over-estimation of the experimental data
about by the new correlations, besides validating them for use in can be noticed, which is consistent with the under-estimation of
 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410 11

Fig. 10. Integral validation of the new thermal conductivity and melting temperature correlations for fast reactor MOX against radial melting extent data (left plot) and fuel-
cladding gap size data (right plot), at end-of-life, from the HEDL P-19 irradiation experiment [70]. The results obtained employing state-of-the-art TRANSURANUS correlations
are also reported, for sake of comparison. Where grey points are not visible, they are exactly covered by orange points. (For interpretation of the references to colour in this
figure legend, the reader is referred to the web version of this article.)

the power-to-melt. This is also consistent with the over-estimation lations. The code calculations are generally conservative with re-
(for all the experimentally melted pins) of the axial melting ex- spect to the experimental measurements, since the power-to-melt
tent, employing both sets of correlations. Moreover, the code pre- is under-estimated, and the fuel axial and radial melting extents
dicts melting (both radial, as shown in Fig. 10 - left, and axial) are over-estimated.
also for two rods (number 6 and 33, from Table 9) which exper- This work represents a step towards the extension, improve-
imentally are un-melted after the irradiation. The new correlations ment and validation of fuel performance codes for application to
again provide slightly more accurate predictions with respect to safety analyses on fast reactor MOX fuels, of great interest in the
the state-of-the-art. Instead, regarding the final fuel-cladding gap framework of Generation IV reactor concepts development. Addi-
size, no significant improvement can be noticed from the new cor- tional experimental measurements and uncertainty indications will
relations, since calculated values are very similar. Nevertheless, the help to both further improve and validate the novel models herein
gap size is determined by many different phenomena occurring presented (for what concerns e.g., the effect of hypo-stoichiometry
in a fuel rod (e.g., fuel relocation, fuel and cladding swelling and and burn-up on the thermal conductivity), along with data assimi-
creep), overruling the effect of thermal conductivity and melting lation techniques. As a complement, values calculated from Molec-
temperature models. The less accurate predictions, outside the 50% ular Dynamics simulations could further help in supporting and
error band, correspond to those HEDL P-19 pins with the highest interpreting experimental data. As potential future model improve-
as-fabricated gap size, where the aforementioned model uncertain- ment, the development of a mechanistic approach to thermal con-
ties on fuel relocation and gap conductance dominate. ductivity is of great interest, to increase the physical ground of the
model developed in this work. To this end, one could consider ei-
5. Conclusions ther the fission product concentration remaining in the fuel or an
effective fuel burn-up, to account for the effect of annealing of the
In this work, novel and more comprehensive correlations for irradiation damage and fission product removal at high tempera-
the thermal conductivity and melting temperature of fast reactor tures (typical for fast reactor MOX) in the present model. More-
MOX have been developed, fitting recent and reliable experimen- over, the mechanistic approach would be applicable to different
tal data to obtain models that contain all the fundamental effects nuclear fuel materials (e.g., minor actinide-bearing fuels, relevant
(i.e., fuel temperature, burn-up, plutonium content, deviation from for fast breeder Generation IV applications) and different thermal
stoichiometry, porosity). The functional form of these new corre- properties (e.g., thermal diffusivity, heat capacity). Finally, uncer-
lations has been statistically assessed through a p-value analysis, tainty and sensitivity analyses on the thermal properties herein in-
which confirmed the inclusion of the aforementioned dependen- vestigated, which currently are still at preliminary stages for fuel
cies in both models. The validity ranges have been extended with performance codes, are planned, given their fundamental role in
respect to state-of-the-art correlations, now reaching higher tem- the development of fast reactor Generation IV concepts employing
peratures (up to 2700 K, for the thermal conductivity correlation), MOX nuclear fuel.
higher plutonium contents (up to 50 at.%) and higher burn-up (up
to 130 GWd/tHM). Moreover, the correlations herein proposed have
been validated against experimental measurements, with encour- Declaration of Competing Interest
aging results, affected by deviations from the measured data gen-
erally comparable with the experimental uncertainties. The authors declare that they have no known competing finan-
Additionally, the novel MOX thermal conductivity and melt- cial interests or personal relationships that could have appeared to
ing temperature correlations have been implemented in the influence the work reported in this paper.
TRANSURANUS fuel performance code, for validation against inte-
gral data from the HEDL P-19 irradiation experiment, concerning Acknowledgments
MOX fuel in fast reactor start-up conditions. The new correlations
show a promising predictive capability of both integral and local This work has received funding from the Euratom research and
experimental data from post-irradiation examinations, improving training programme 2014–2018 through the INSPYRE project under
or at least matching the predictions from state-of-the art corre- grant agreement No 754329.
12 A. Magni, T. Barani and A. Del Nevo et al. / Journal of Nuclear Materials 541 (2020) 152410

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