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Journal of Nuclear Science and Technology

ISSN: 0022-3131 (Print) 1881-1248 (Online) Journal homepage: https://www.tandfonline.com/loi/tnst20

Characterization of High Burnup Fuel for Safety


Related Fuel Testing

Guido LEDERGERBER , Sousan ABOLHASSANI , Magnus LIMBÄCK , Roger J.


LUNDMARK & Kurt-Åke MAGNUSSON

To cite this article: Guido LEDERGERBER , Sousan ABOLHASSANI , Magnus LIMBÄCK , Roger
J. LUNDMARK & Kurt-Åke MAGNUSSON (2006) Characterization of High Burnup Fuel for Safety
Related Fuel Testing, Journal of Nuclear Science and Technology, 43:9, 1006-1014

To link to this article: https://doi.org/10.1080/18811248.2006.9711189

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Journal of NUCLEAR SCIENCE and TECHNOLOGY, Vol. 43, No. 9, p. 1006–1014 (2006)

ORIGINAL PAPER

Characterization of High Burnup Fuel for Safety Related Fuel Testing


Guido LEDERGERBER1; , Sousan ABOLHASSANI2 , Magnus LIMBÄCK3 ,
Roger J. LUNDMARK1; y and Kurt-Åke MAGNUSSON3
1
Kernkraftwerk Leibstadt AG, CH-5325 Leibstadt, Switzerland
2
Paul Scherrer Institut, CH-5232 Villigen, Switzerland
3
Westinghouse Electric Sweden AB, SE-721 63Västerås, Sweden
(Received January 25, 2006 and accepted in revised form June 8, 2006)

Fuel Assemblies designed and fabricated by Westinghouse Electric Sweden (WSE) to reach high burnup have been
operated in the Leibstadt nuclear power plant (KKL) for seven cycles attaining an assembly average burnup above
60 MWd/kgU. The irradiation conditions in KKL featured linear heat generation rates ranging from 250 W/cm early
in life down to 100 W/cm in the last cycle and normal water chemistry with zinc injection. Selected rods have been
extracted at both intermediate and final irradiation stages and hot cell examinations have been carried out. The results
show that the fuel is well suited for high burnup applications and rod segments have been provided to the OECD
Halden Reactor Program, the OECD Studsvik Cladding Integrity Program and the Japanese ALPS program for dedi-
cated high burnup tests with regard to fission as release and cladding lift-off as well as behavior under power transient,
RIA and LOCA.
KEYWORDS: nuclear fuel, cladding, irradiation, Zircaloy-2, uranium oxide, lead test assemblies, high burn-
up, RIA, LOCA

I. Introduction
The Leibstadt nuclear power plant (KKL) in Switzerland 10
operates a ‘‘GE BWR/6’’ boiling water reactor with a ther- 9
mal power of 3,600 MW, corresponding to a nominal net 8
electrical output of 1,145 MW. The core consists of 648 as-
7
semblies. Commercial operation started in December 1984.
The plant has operated on a 12-month cycle basis, with refu- 6
eling outage in August. Leibstadt performed two reactor 5
thermal power up-rates, the first one after about one year
4
of commercial operation in December 1985 from 3,012 to
3,138 MW, the second one in several steps between October 3
1998 and August 2002 to 3,600 MW. In 1994 a research pro- 2
gram was initiated by KKL, Westinghouse Electric Sweden 1
(former ABB Atom) and Paul Scherrer Institut (PSI) in order
A B C D E F G H I J
to increase the fuel residence time in the reactor. The objec-
Extracted rods
tive of the program was to irradiate a series of Lead Test As-
semblies (LTA) in KKL and to verify the fuel behavior to an
Fig. 1 Description of the fuel assembly and the designation of
assembly average burnup of 60 MWd/kgU derived from an rods. The control rod is indicated by thick solid lines
enrichment limit of 5% 235 Uranium with poolside as well
as non destructive and destructive hot cell examinations.
channel in the centre. This diamond-shaped water channel
II. Fuel and Fuel Assemblies and the water wings between sub-bundles are an integral part
of the fuel channel.1) The rod positions and its orientation to-
For the reload batch of cycle 11 eight LTAs of SVEA-96 wards the control rod are given in Fig. 1. The rods are held
with full size rods were fabricated by Westinghouse Electric in place by the bottom and the top tie plate and by 7 Inconel
Sweden in Västerås for KKL with the aim of being irradiated spacers for each subassembly. The rods used for the exami-
high burnup. nation program covered here originate from fuel assemblies
The SVEA-96 fuel assembly has a lattice with a total AEB067, AEB071 and AEB072 and are all fabricated in one
of 96 rods [4ð551Þ] in four subassemblies and a water campaign with the same pellet fabrication batches and the
same lot of cladding material.

Corresponding author, E-mail: guido.ledergerber@kkl.ch 1. Pellets
y
Present address: Roger J. LUNDMARK, Swissnuclear, Postfach The pellets are with dishing and chamfer and have been
1663, CH 4600 Olten pressed from Ammonium di-Uranate (ADU) powder, sin-
Atomic Energy Society of Japan
1006
Characterization of High Burnup Fuel for Safety Related Fuel Testing 1007

tered at typical conditions and ground to a diameter of sets with burnup values for each node at the time of each
8.19 mm. Rods in position E4 and J9 had fuel pellet enrich- Traveling In-core Probe (TIP) measurement and linear heat
ment of 4.46 and 3.71% 235 U and density of 10.50 and generation rates (LHGR) for all nodes of all rods in the fuel
10.53 g/cm3 respectively. The average grain size was 10– assemblies of the examination program have been calculat-
11 mm. ed. Typical power histories for nodes of the fuel segments
that have been provided for use in the ALPS program are
2. Cladding Material found in Fig. 2. The LHGR during the first two irradiation
The cladding material used for the studied rods is desig- cycles was between 180 and 250 W/cm and declined grad-
nated LK3/L. This type of material fulfils the ASTM spec- ually to 80–100 W/cm in the seventh cycle.
ification for Zircaloy-2 and the concentrations of the alloying
elements relative to the weight of the bulk material are speci- 2. Burnup
fied as: Sn 1.20–1.70%; Fe 0.15–0.20%; Cr 0.05–0.15%; Ni The core thermal balance for the core simulator is calcu-
0.03–0.08%; O 0.09–0.16%; Si 0.005–0.012%; C 0.008– lated in the core supervision program package HEBAL.
0.020%, while the liner contains Sn 0.1–0.4% and Fe The plant thermal power output for the adjustment of
0.02–0.045%. The cladding outer and inner diameters were HEBAL is determined according the VDI guide line ‘‘VDI
9.62 and 8.36 mm respectively, giving a wall thickness of 2048 Richtline zur Prozessdaten Validierung’’ issued 2002
0.63 mm. The initial radial pellet-cladding gap was 0.085 with a dedicated software VALI3.c For KKL the thermal
mm. power variation for 2004 (cycle 20) was determined to
2¼0:6% (confidence 95%) based on a process flow sheet
without any contradiction over the whole cycle. Over the last
III. Irradiation in KKL
10 years the variation of the thermal power was always bet-
The reactor operation for the time of the irradiation of the ter than 1%.
LTA is compiled in Table 1 which includes the dates of the The local burnup as given in Table 2 was calculated with
beginning (BOC) and the end of each cycle (EOC) as well as the lattice code Helios version 1.6 and the core simulator
the cycle length in effective full power days (EFPD). From Presto-2 version 1.10a on a nodal basis. TIP measurement
1998 to 2002 the reactor thermal power was stepwise in- performed once a month always gave radial deviations of
creased from 3,138 to 3,600 MW: 3,327 MW October 31, Root Mean Square (RMS) 2% and axial deviations of
1998; 3,420 MW September 16, 1999 preceded by some RMS 3%. A power gamma scan performed on 39 fuel as-
tests at this power level in February 1999; 3,440 MW March semblies in 2003 confirmed these values and deviations eval-
17, 2000; 3,515 MW October 11, 2000 with a three week test uated have been radial RMS 1.40% and axial RMS 1.89%.
period in September 2000 and finally 3,600 MW on August The same gamma scan campaign was recalculated by
26, 2002. This thermal power results in power density of Phenix/Polca7,d the core monitoring system of Westing-
32 kW/kgU or 62 kW/dm3 . house Electric Sweden,2) and good agreement was found
with deviations evaluated of radial RMS 1.44% and axial
1. Power Histories RMS 2.35%.
The KKL core supervision system ‘‘Minuteman’’a is based
on the core simulation code ‘‘Presto-2’’ and the lattice code 3. KKL Coolant Chemistry
‘‘Helios’’.b Pin power reconstruction was performed for all The condensate cleaning system of KKL takes about two
bundles in the LTA program on a nodal basis. In order to ob- thirds of the condensate. The remaining part, from the third
tain a day-by-day follow-up of the pin power, the reduced low-pressure pre-heater and the high-pressure pre-heater, is
pin power data set created within the core follow calcula- injected directly into the feed water tank. The reactor water
tions has been extended according to the reactor operation. cleaning system has a capacity of 1.2% of the feed water.
The reactor data used are on an hourly basis. The full data Both systems operate with powder resin filter-demineraliser
units. The condenser tubing is fabricated from titanium tub-
Table 1 Operation of the fuel assemblies AEB067, AEB071 and ing. During the irradiation time of the LTA KKL was oper-
AEB072 the core ating with normal water chemistry with zinc injection.
Cycle Length Zinc injection was started in 1990. After an optimization
KKL cycle BOC EOC of the amount of zinc used in the injection plant zinc deplet-
[EFPD]
ed in 64 Zn was applied from cycle 9 (August 1993) onwards.
11 3.09.1994 4.08.1995 312.9 The isotopic compositions of the applied zinc was decreasing
12 2.09.1995 26.07.1996 311.5
from 1.6% 64 Zn in cycle 11 to 1.0% in cycle 14 and kept con-
13 2.09.1996 28.07.1997 316.7
14 29.08.1997 31.07.1998 324.1
stant at this value onwards. Another important change was a
15 24.08.1998 7.08.1999 344.4 significant reduction of the iron concentration in the feed
16 31.08.1999 31.07.2000 351.2 water after the summer 1994 outage at the beginning of cycle
17 21.08.2000 5.08.2001 334.9 10 (BOC 10). This was the consequence of a modification of
the condensate cleaning plant leading to an increased effi-

a c
K-Effective LLC, 19422 Blue Bell-PA USA Belsim, Liege, Belgium
b d
Studsvik Scandpower, Kjeller, Norway Westinghouse Electric Sweden, Västerås, Sweden

VOL. 43, NO. 9, SEPTEMBER 2006


1008 G. LEDERGERBER et al.

250 AEB072 J9, Node 10, 1481mm


AEB072 E4, Node 17, 2548mm
Linear heat rate [W/cm]

200

150

100

50
0 200 400 600 800 1000 1200 1400 1600 1800 2000 2200 2400 2600
Time in core [day] Filename: FPP-LHGR vs TIME

Fig. 2 Power histories for AEB072-J9-E, a segment foreseen for LOCA testing and
Segment AEB072-E4-J foreseen for RIA testing in NSRR

Table 2 Average burnup of segments provided for international and national program

Assembly-rod-segment Calc. Burnup


Program
designation nodes (MWd/kg)
AEB068-E4-B 5–7 66.5 OECD-HRP
AEB068-E4-D 9–11 66.7 OECD-HRP
AEB068-E4-SA 16–18 62.2 OECD-SCIP
AEB069-E4-B 5–7 59.4 OECD-HRP/Lift off
AEB069-E4-D 9–11 59.0 OECD-HRP/Lift off
AEB069-E4-RA 16–18 55.9 OECD-SCIP
AEB070-E4-N 14–16 37.7 OECD-SCIP
AEB070-E4-C 5–7 44.3 OECD-HRP
AEB070-E4-D 9–11 42.2 OECD-HRP
AEB071-E4-E 9–10 67.6 ALPS/HR-FGR
AEB071-E4-H 14–15 66.5 ALPS/HR-FGR
AEB071-E4-B 5–7 66.5 OECD-SCIP
AEB072-E4-J 16–18 68.6 ALPS/RIA
AEB072-E4-L 19–20 65.8 ALPS/LOCA
AEB072-J9-E 9–11 72.9 ALPS/LOCA
AEB072-E4-C 5–7 72.3 OECD-HRP
AEB072-E4-E 9–11 73.1 OECD-HRP

ciency of removing particular iron. During the same outage, 1996, at the end of cycle 11. From cycle 13 onwards KKL
one of the recirculation lines was decontaminated. In order to applied the empirical recommendation from WSE developed
prevent the clean piping wall from being quickly re-contami- during the ESSC evaluation. The iron concentration in the
nated, the amount of zinc injected into the feed water was in- feed water should be larger than twice the input of divalent
creased during the first part of cycle 10. This drastic change ions. The LTAs of this program were in the core since
in the ratio of iron to divalent transition metals, dominated by BOC 11 and were therefore being exposed to the special con-
zinc in the KKL case, in the feed water led to significant ditions at the beginning of their irradiation. The fuel assem-
changes of the reactor water concentrations and the compo- blies were unloaded in August 2001. In examinations outside
sition of CRUD deposited on fuel rod surfaces. These this program it was shown that the cladding material with the
changes were delayed identified as part of the root cause, designation LK3 used for this test program was not affected
in combination with a cladding material with the designation at all from ESSC.3) Nevertheless the CRUD deposited on the
LK2 susceptible to enhanced corrosion at high burnup, for surface of the fuel shows a strong magnetic moment, which
the KKL Enhanced Spacer Shadow Corrosion (ESSC) event impedes oxide thickness measurements with the normal type
identified in May 1997 on SVEA-96 fuel unloaded in August of eddy current lift-off technique.

JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY


Characterization of High Burnup Fuel for Safety Related Fuel Testing 1009

IV. Characterization of Fuel Rods by Non Destruc-


tive and Destructive Techniques
The fuel rods from the LTA have been part of an exten-
sive poolside inspection program performed by WSE onsite
at Leibstadt. Selected rods have been extracted and trans-
ported to PSI for hot cell examination by non-destructive
testing (NDT) as well as destructive testing (DT). The data
of the examined rods are given in Table 3. Based on the
NDT results segments have been selected, cut and prepared
for transportation. Figure 3 provides an outline of the pool-
side inspections including their date of performance and the
fuel assemblies analyzed and rods transported to PSI.

1. Pool Side Inspections


(1) Visual Inspections
The sub-bundle was extracted from the fuel channel for
the visual inspection and in some cases spacers have been
moved downwards for detailed inspection of contact points
Fig. 4 Typical appearance of the rods in the fuel assembly
of the Inconel spacer. The inspection was performed with
AEB072 before brushing and removal of the spacer (rods J6,
the WSE high resolution underwater video camera with sup- J7, J8, J9, J10)
porting equipment. The position of the rod identification
number was used to define the orientation of the rod in the
bundle. The fuel assembly was covered with a red color stands for divalent transition metal (Zn, Ni). In spacer posi-
CRUD which was analyzed to be a hematite, Fe2 O3 , tions the contact points of the springs and the spacer struc-
(Fig. 4). This loose CRUD could be removed by brushing, ture was clearly visible. No spalling or oxide nodules were
leaving a black surface underneath (Fig. 5). This layer with visible.
the black surface was latter analyzed to be a dense layer of (2) Rod Growth
CRUD with a spinel composition: MeFe2 O4 , where Me Fuel rod lengths were measured by placing a perforated
plate on top of the channel and measuring the distance to
the rod top end plug with an indicator clock that is calibrated
Table 3 Data of rods for destructive examinations against a gauge placed in one sub-channel. The channel
length was measured in a similar manner. The measured val-
Rod av. Rod growth FGR by
Assembly-rod ues given in Table 3 are below the upper band for the typical
burnup pool/hot cell puncturing
designation growth of LK3 material in KKL, which was estimated to
(MWd/kg) (%) (%)
0.1% L=L per 10 MWd/kgU.
AEB070-E4 35.9 0.24/0.25 0.3e (3) Oxide Thickness Measurements
AEB069-E4 51.1 0.31/0.31 0.28 The distortion of the eddy current signal was strong, there-
AEB068-E4 57.3 0.41/0.40 0.86 fore reliable measurements of oxide thickness have not been
AEB071-E4 57.4 0.38/0.37 1.46
possible with equipment based on one frequency at the time
AEB072-E4 62.9 0.42/0.40 1.10
AEB072-J9 63.7 0.39/0.40 3.25
of rod extraction. A new method named ‘‘MAGNACROX’’4)
is under development at Westinghouse Electric Sweden. The
e
estimation based on the neighbouring rod AEB070-D5 method is based on multi-frequency eddy current measure-

Year 1992 1993 1994 1995 1996 1997 1998 1999 2000 2001 2002 2003 2004

KKL Cycle 9 10 11 12 13 14 15 16 17 18 19 20

Transport PSI - Studsvik:


Pool-side visual inspection March 2003
S96+/L, LK2, Demo LK2+, LK3 Segments of rods:
Full pool-side inspection
(visual, oxide, length) AEB070-E4, AEB069-E4,
AEB068-E4, AEB071-E4
AEB070 34,8
and AEB072-E4
AEB069 49
Transports to PSI, full rods:
AEB070-E4, AEB069-E4
AEB068 54.5 AEB068-E4, AEB071-E4,
AEB072-E4 AEB072-J7
AEB067, AEB071, AEB072 AEB072 60 and AEB072-J9

Fig. 3 Outline of the poolside inspection program with transports to PSI and Studsvik

VOL. 43, NO. 9, SEPTEMBER 2006


1010 G. LEDERGERBER et al.

2. Hot Cell Non Destructive Test (NDT)


Upon arrival in the hot-cells the rods have been gently
brushed in order to remove the loose CRUD, leaving the te-
nacious CRUD layer.
(1) Profilometry
Diameter measurements were performed with two linear
variable displacement transducers calibrated with diameter
gauges to an accuracy of 5 mm. Axial profiles were taken
at 0 , 45 and 90 azimuthal position in steps of 0.5 mm.
Nearly no creep down was found in all high burnup rods (as-
semblies AEB068, AEB069, AEB071 AEB072) and the di-
ameter was found to be very close to the as fabricated value.
At spacer positions the contact points were generally noticed
to provide higher values reflecting thick oxide at these very
distinct locations (Fig. 6). Detailed maps of selected spacer
positions measured in steps of 15 azimuthally and 0.5 mm
axially confirmed the finding (Fig. 7). Profilometry measure-
Fig. 5 Typical appearance of the rods after brushing with spacer 3 ments are in agreement with destructive oxide and CRUD
removed in the fuel assembly AEB072 (rods J6, J7, J8, J9, J10) thickness measurements.
(2) Gamma Scanning
Integral scans of full length of the rods in steps of 0.5 mm
ments and a mathematical inversion model, which permits with the Gamma spectrometry were performed. Peak areas
an estimation of the oxide and CRUD thickness on fuel clad- of 95 Zr/Nb, 106 Ru, 125 Sb, 137 Cs and 144 Ce were measured
dings that have CRUD deposits with a magnetic moment. with 10% (Fig. 6 and Fig. 8). Close the highest concen-
Detailed measurements have been performed in the PSI tration of 137 Cs detailed high resolution measurements with
hot-cells and are reported in the following sections. step width of 0.5 mm were performed. No fission product

0 500 1000 1500 2000 2500 3000 3500 4000


9.80
AEB072-E4
Profilometry, diameter [mm]

9.75
Diameter 90-270 degree

9.70

9.65

9.60

oxide measurement average


Layer Thickness [µm]

50 crud measurement average

40

30

20

10

0
Cs-137 activity [cps]

160

140
Cs-137 [cps], 20 sec
Cs-137 [cps], 900 sec
120

0 500 1000 1500 2000 2500 3000 3500 4000


Filename: AEB072-E4 272-25154-KKL
Source: A154PRO02, A154PRO03
Position from tip of bottom end plug [mm] A154GSU01, A154GSN02

Fig. 6 Rod AEB072-E4, non-destructive measurements

JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY


Characterization of High Burnup Fuel for Safety Related Fuel Testing 1011

Fig. 7 Map of spacer position, areas of high values reflect the contact points of spacer and spring

0 500 1000 1500 2000 2500 3000 3500 4000


40
Deviation from 9.62 mm [µm]

30 AEB072-J9 Profilometry Scan 90 - 270 degree


20
10
0
-10
-20
-30
-40
oxid
-50 average
100
Cs-137 activity [cps] Layer Thickness [µm]

std. div.
80 crud
average
60 std. div.

40
20
0
180

160

140

120 activity Cs-137 [cps], 20 sec meas. time

0 500 1000 1500 2000 2500 3000 3500 4000


Position from tip of bottom end plug [mm] Filename: AEB072-J9 272-25154-KKL
Source: A154PRO1, A154PRO2
BET02-111 ms, A106GSU01

Fig. 8 Rod AEB072-J9, non-destructive measurements

migration has been found (Fig. 9), as the pellet-pellet inter- different thickness were performed in air. Detailed measure-
faces are still visible. ments in spacer area and at positions foreseen for destructive
(3) Oxide Thickness Measurements examination have been performed. Data for two rods are giv-
The MAGNACROX method, as applied in the spent fuel en in Figs. 6 and 8. The values for oxide thicknesses shown
pool at KKL, was applied also for the hot cell examinations. below 1,500 mm from the bottom end plug are conservative-
The measurements as well as the calibration, using foils of ly overestimated and could not be confirmed by metallo-

VOL. 43, NO. 9, SEPTEMBER 2006


1012 G. LEDERGERBER et al.

Collimator slit width: 0.15 mm Count rate: 900 sec/step Measurement date: 22.-24.3.2002
Table 4 Qualification of Hydrogen measurements
Activity Cs-137 [cps]

170 42
Sample designation Studsvik PSI
Studsvik/PSI H2 -content H2 -content
160 40

Ru-106 Activity [cps]


AEB068-E4-M/-N 202 ppm 208 ppm
150 38 AEB068-E4-E/-G 180 ppm 207 ppm
Activity Nb-95 [cps]

110 36

100 34
shielded cell. The LECO RH-402 analyzer makes use of
1900 1920 1940 1960 1980 2000 the difference in thermal conductivity of the carrier gas.
Position from bottom end plug tip [mm] Within this examination campaign an interlaboratory com-
parison between PSI and Studsvik Nuclear was performed.
Fig. 9 Rod AEB072-E4, detailed gamma scan in the highest burnt
Excellent agreement has been found for samples originating
region
from positions 5 mm apart each other on a rod irradiated for
six cycles in KKL (Table 4).
The method for hydrogen measurements developed at
PSI5) allows a fractionated determination of hydrogen re-
leased from different parts of the cladding material e.g. from
the bulk metal or the outer corrosion layer. Important for the
mechanical properties is the hydrogen in the remaining clad-
ding wall. The measurement series resulted in a value of
88% of hydrogen in the metal and 12% hydrogen being re-
leased at lower temperature from the outer corrosion layer.
The calculated average for total hydrogen content of
AEB072-E4 is 305 ppm (N¼8) and for AEB072-J9 it is
204 ppm (N¼16). The standard deviation was always below
10%. Only small variations in azimuthal and axial direction
could be identified.
(2) Hydrogen Distribution
The precipitated hydrides in the cladding material were
evaluated on pictures taken from the polished and etched
Fig. 10 Cladding of AEB072-E4 at mid height, hydride near the cladding ring specimen (Fig. 11). With image analysis the
surface, oxide layer with the typical crack (arrow) and the curd orientation of the hydrides with a length of >15 mm was
layer on top evaluated. In the mid height specimen of AEB072-E4 7%
radial hydrides were counted, whereas the fraction of radial
hydrides in AEB072-J9 was about 9%. This is well within
graphic examinations. The examination of the oxide thick- the standard deviation of the measurements, which was typ-
ness in the polished specimen has shown that the oxide ically in the order of 4%. The typical fine structure of the hy-
thickness outside the spacers is always below 30 microme- drides near the water side oxide is shown in Fig. 10.
ters. In the region with high burnup at mid height the nodal
average oxide thickness for AEB072-E4 was 18 with a max- 2. CRUD and Water Side Oxide Examinations
imum of 23 mm (Fig. 10) and for AEB072-J9 18 with a max- The morphology of the CRUD and the oxide was exam-
imum of 24 mm. ined with Electron Probe Micro Analysis (EPMA) technique.
(4) Fission Gas Release Mapping of the element distribution gave clear evidence of a
Rod puncturing revealed rod total gas pressure, the free CRUD with two phases (Fig. 12). An Iron-Oxygen phase on
volume and the gas composition. Fission gas release as given top of a denser phase with less Iron, but with zinc, nickel and
in Table 3 was calculated based on the average rod burnup manganese in varying concentrations and oxygen was ob-
and the fission gas yield of 31.07 ml/MWd. A calibration served. The strong distortion of the eddy current signal could
sample with a synthetic fission gas mixture was used to be caused by the granular structure of the surface iron–oxy-
check equipment and procedure prior to puncturing the first gen grains like maghemite [-Fe2 O3 ] or the continuous layer
rod of a batch. of spinel [(Znþ2 ,Niþ2 )(Feþ3 ,Mnþ3 )2 O4 ]. In the case of spinel
layer being responsible for the distortion the surface grain
would be hematite, which has no magnetic moment. There
V. Destructive Examinations
is some evidence that the ferrimagnetisms of the spinel is
1. Cladding Material causing the distortion of the NDT oxide measurements. On
(1) Hydrogen Content a ceramography at mid height of AEB072-J9 the CRUD
Hydrogen is analyzed in PSI by fusion of cladding ring thickness was estimated to be 72 mm.
segments in a graphite crucible under inert gas in a lead No spalling of oxide was seen in any of the examined

JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY


Characterization of High Burnup Fuel for Safety Related Fuel Testing 1013

Fig. 13 Typical rim area of fuel at mid height of AEB072-E4.


The cladding is bound to the fuel. No gap is visible. The line in-
dicates the position of the concentration profiles given in Fig. 14

Fig. 11 Cladding of AEB072-J9 at mid height, typical hydride


tions bound to the cladding with no visual gap (see Fig. 13).
distribution for 220 ppm Hydrogen (cladding outer side left)
The inner zirconia layer formed though pellet-cladding con-
tact is relatively modest. On the higher burned side the typi-
specimens. The water side oxide is strongly bound to the cal rugged structure extends into the fuel.
cladding and also to the CRUD, whereas in most picture a The EPMA shows over the major part of the radius a
small crack within the oxide but on the side towards the rather flat profile for fission products like caesium, rutheni-
CRUD was seen. A typical example is given in Fig. 10. um and neodymium. Strong increase of plutonium and the
The oxide thickness was found to be azimuthally uniform fission products is seen over a width of 300 mm on the high-
and measured values have been averaged (see Sec. IV-1 er burned side (Fig. 14) and only 60 mm on the lower
(3) Oxide thickness measurements). burned side. Concentrations and size of intermetallic fission
products continuously decreased from rim to the centre and
3. Fuel Ceramic Examinations only reach in the rim region the maximum size of 1 mm.
(1) Fuel Structure-EPMA Examinations The xenon profile which is linked to the porosity suggests
The fuel structure of rod AEB072-E4 is with a few excep- three distinct radial zones: rim, dense fuel with small fis-

Fig. 12 CRUD appearance (picture left) and composition at mid height of AEB072-E4, distribution of iron (middle) and
zinc (right). Concentrations are shown with the colors: blue - zero, red - high concentration. Grains of maghemite
[-Fe2 O3 ] or haematite are embedded in a continuous layer of spinel [(Znþ2 ,Niþ2 ) (Feþ3 ,Mnþ3 )2 O4 ]

VOL. 43, NO. 9, SEPTEMBER 2006


1014 G. LEDERGERBER et al.

4.0 3.00 50
Pu-239 Pu240 Pu-241 Pu-242
Pu Cs Xe 2.75 45
3.5 Nd Zr 2.50
40
3.0 2.25

Isotopic content [at%]


fission products [wt%]
35
2.00
weight percent Pu

2.5
1.75 30

2.0 1.50 25
1.25 20
1.5
1.00
15
1.0 0.75
10
0.50
0.5 Rod side oriented
0.25 5
towards water channel
0.0 0.00 0
0 10 20 30 40 50 60 70 80 90 100 110 120 130 140 150 160 -4 -3 -2 -1 0 1 2 3 4

micrometers Radial position from centre [mm]

Fig. 14 Typical profiles of metals in the closed gap Fig. 15 Profile of Plutonium isotopes of sample from AEB072-E4
of AEB072-E4

ding lift-off, behavior under power transient, RIA and LOCA


sion gas bubbles and porous fuel in the centre with larger of such high burnup fuel as listed in Table 2.
open pores.
(2) Isotope Measurements
Acknowledgment
Five samples with different burnup have been selected for
the measurement of isotopic composition and the concentra- In addition to the direct involved organizations WSE,
tion of uranium, plutonium and neodymium by isotope dilu- KKL and PSI the work was sponsored by E.ON Kernkraft,
tion analysis with a high performance liquid chromatography Germany. The authors also like to thank all co-workers for
system connected to a multicollector inductively coupled their engagement and enduring effort on their contribution
plasma mass spectrometer (HPLC-MC-ICP-MS).6) For qual- to the overall project.
ity assurance a specimen of the ARIANE program7) was re-
analyzed. Recalculation of the isotopic concentrations with
Helios by NOK/KKL resulted in good agreement for 235 U References
(þ1%) and for 238 U (þ0:6%), whereas 239 Pu was under-pre-
dicted by 3 to 7% at similar axial location and 241 Pu was sys- 1) S. Helmersson, H. Nerman, L. Paulsson, ‘‘SVEA-96: BWR Fuel
tematically over-predicted by 6 to 35%. Additional measure- for the 1990s,’’ Nucl. Eur., 1–2, 37–38 (1989).
ments of radial profiles by Secondary Ion Mass Spectrome- 2) J. J. Casal, J. Krouthén, M. Albendea, ‘‘Accurate tools to model
advanced SVEA fuel designs,’’ Nucl. Technol., 151, 51–59
try (SIMS) have been performed (see Fig. 15) and will be
(2005).
further analyzed and compared with calculations.
3) R. J. Lundmark, Enhanced Spacer Shadow Corrosion (ESSC) of
BWR Fuel at Kernkraftwerk Leibstadt (KKL), EPRI, Palo Alto,
VI. Conclusion CA and KKL 1009736, (2004).
4) K.-Å. Magnusson, P. Hellberg, L. P. Pedersen, M. Bastani,
Selected rods and samples have been characterized in ‘‘Description of advanced method for measurement of oxide
great detail at intermediate and final irradiation stages utiliz- layer thickness in the presence of magnetic CRUD,’’ Proc.
ing non destructive techniques (NDT) in the spent fuel pool Jahrestagung Kerntechnik 2001, May 15–17, 2001, Dresden,
and in hot cells. Destructive examinations in the hot cells of Germany, p. 383–387 (2001).
high burnup samples (73 MWd/kg U) have produced accu- 5) A. Hermann, et al., ‘‘Hydrogen distribution between fuel clad-
rate data for the qualification of calculation tools and the ding metal and overlying corrosion layers,’’ Proc. Int. Topical
Meeting on LWR fuel performance, Park City, USA, 372–384
confirmation of measurements with non destructive tech-
(2000).
niques. The results, furthermore, show that the fuel is well 6) I. Günther-Leopold, et al., ‘‘Measurement of isotope ratios on
suited for high burnup applications and typical, well charac- transient signals by MC-ICP,’’ Anal. Bioanal. Chem., 378,
terized high burnup segments have been provided to the 241–249 (2004).
OECD Halden Reactor Program, the OECD Studsvik Clad- 7) M. Lippens, et al., ‘‘Source term assessment: The ARIANE pro-
ding Integrity Program and the Japanese ALPS program gramme,’’ Proc. ICEM’01, Brugge, Belgium, Sept. 30.–Oct. 4,
for dedicated tests with regard to fission gas release and clad- 2001, (2001).

JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY

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