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Activated corrosion products in ITER first wall and shielding blanket heat
transfer system

Conference Paper · January 1995


DOI: 10.1109/FUSION.1995.534235 · Source: IEEE Xplore

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Activated Corrosion Products in ITER First Wall and Shielding Blanket Heat Transfer
System

L. Di Pacea, G. Cambib, D.G. Cepragac, E. Sobrerod, M. Costad


a)ENEA Fusion Sector, CR di Frascati, C.P. 65, 00044 Frascati, Rome, Italy
b)Bologna University, Physics Department, Via Imerio 46, 40126 Bologna, Italy
C)ENEA, Innovation Department, Via Don Fiammelli 2, 40129 Bologna, Italy
d)Bologna University, Impianti Nucleari-D.I.E.M., Bologna, Italy
ABSTRACT fusion devices such as ITER, ACPs could be a problem, not
only in terms of occupational dose, but also in the case of
Corrosion and erosion phenomena play an important role in accidents such as LOCAs, because they are not negligible
mobilising activated materials in fusion machines. This paper compared to the whole mobiliseable inventory (MI). In order
deals with the assessment of the activated corrosion products to assess the ACP inventory inside the ITER PHTS, the
(ACPs) related to the primary heat transfer system (PHTS) of French code PACTOLE, developed by CEA for fission
the first wallhhielding blanket (FWISB) of the ITER plant. reactors and qualified on more than 15 years of measurements
ACPs could be a cause for concern in terms of occupational on PWR circuits, has been used.
radiation exposure (ORE) in maintenance scenarios. They
could also be relevant in the case of severe accidents, such as THE PACTOLE CODE
ex-vessel LOCAs. The assessment mainly refers to the TAC-
4 design developed for ITER. The mobilisation of the
activated material has been estimated with the qualified CEA The PACTOLE code [ 11 models the formation, activation,
code PACTOLE. It considers all the chemical and physical migration and deposition of corrosion products, considering
phenomena responsible for corrosion, activation and transport the most important physical and chemical phenomena. (see
of corrosion products in cooling loops. The XSDNRPM-S Fig. 1).
code is used for neutronic calculations; the ANITA-2 code for
activation calculations. The results obtained show the
improvement gained, in terms of corrosion and radioactive
inventory reduction, by avoiding the use of the boron as
additive. Results obtained point out the impact of the main PURIFICATION
water chemistry parameters (e.g. water temperature and pH) * Ion exchangers
on ACP production, transport and deposition. A parametric Filters
comparison has been carried out considering the coolant
flowing during dwell periods, two different in-vessel FWISB
AIS1 316L compositions and two fluences: 0.3 and 3 I cvcs r i
M W *y/m2.

INTRODUCTION (q= molecular diffusi BASE METAL


CORROSION

The presence in the ITER machine of a significant quantity of Phenomena modelled in PACTOLE:
activated corrosion products (ACPs) - a few kg distributed or
' Element concentration gradient between wall and bulk coolant;
deposited on the cooling circuits of the divertor, blanket, ' Solubility;
vacuum vessel coolant loops, as well as in any coolant loops * Oxidation:
ion release;
related to test modules, auxiliary heating or diagnostics oxide formation;
equipment - and the pulse length (- 1000 seconds) make the Dissolution;
ACP inventory evaluation an important task from the safety Precipitation;
* Particulation (particles growth);
point of view. It should be noted that activated corrosion Convection;
products also exist in fission reactors and do not pose a * Mass Transfer:
significant public hazard in these installations, while they are Brownian diffusion;
inertian projection, turbulence;
a significant hazard to site personnel. In fact, ACPs are gravitational;
responsible for about 90% of occupational radiation exposure thermophoresis (heat transfer surfaces):
* Erosion-sticking probability, lift forces;
(ORE) in nuclear fission power plants. * Activation;
ITER has the advantages of a lower operating temperature and Molecular diffusion.
no need to add boric acid, unlike fission reactors. On the
other hand, ITER must operate in a pulsed mode, the varying Fig. 1 Corrosion-product formation, migration and deposition, modelled in
temperatures being conducive to more movement of corrosion PACTOLE
products from walls to water. For LWRs, in the case of
severe accidents, ACPs are negligible in terms of radioactive PACTOLE takes into account five elements: Fe, Ni, Mn, Cr,
inventory (RI), mobilised inventory (MI) and environmental CO and Zr, and at present a maximum of ten activation
source term (EST), compared to the inventory from the reactions that have been selected on the basis of the
reactor core (gas and fission products). On the contrary for importance of the radioactive inventory and the gamma
emission of their daughters:

0-7803-2969-4/95/$4.0001995IEEE 333
Table I
56Fe (n, 2n) 55Fe; 54Fe (n, p) 54Mn; ITER TAC-4 PHTS quarter loop features
55Mn (n, 2n) 54Mn; 55Mn (n, y) 56Mn;
56Fe (n, p) 56Mn 58Ni (n, p) 58C0; Thermal power removed [MW] 575
Inlet and outlet coolant temperature ["C] 150- 200
59Co (n, y) 60Co; 5 2 ~ (n,
r 2n) 51cr; Coolant mass [kg] 188400 (*)
58Ni (n, 2n) 57Ni; 58Ni (n, np) 57Co Coolant flow rate Ikdsl. I~
2742 (32% in-board:
68% out-board)
Coolant speed i n main pipes [ d s ] 4-5
giving the following isotopes: 55Fe, 54Mn, 56Mn, 58C0, Coolant speed in blanket segment 0.3 - 1.5
channels [ d s ]
60Co, lCr, 57Ni, 57C0, which account for at least 90% of - 13145
Total wet surface: [m2]
the total FW/SB material radioactivity. * Out-of-flux wet surface - 5981
Under flux zone wet surface - 7164
According to the models used in PACTOLE, an important (*) excluding pressurizer
driving force of corrosion release, deposit, dissolution and
Table I1
precipitation is the concentration gradient between the surface Matenal Composition adopted in PACTOLE calculations
and the bulk coolant. The equilibrium concentration is given
by the thermodynamic laws and depends on T and the Fe(%) NI(%) CO(%) Cr(%) Mn(%)
chemistry (pH, hydrogen partial pressure, etc.). The base AISI 3 1 6 ~ ( I ) 65.93 13.16 ].@E-4 17.39 0.187
A I C I _.--
? I A I (2) 65 02 12.30 0.17 17.40 1.80
metal oxidation leads to adherent oxide formation as well as ..I-.

AISI 304L 70.45 9.5 0.15 18.00 1.90


to soluble element release. A deposited element can be Inconel Allov 8.00 75.5 0.08 12.40 0.70
dissolved if the element concentration in the bulk water is ( 1 ) Mid-94 composition
below the equilibrium value; on the other hand, a given (2 ) End-94 composition
element may precipitate, if its concentration exceeds the
equilibrium value, and form particulates (cruds). The The geometric schematisation of the quarter FW/SB cooling
precipitate agglomerates by collision to form particles and loop of ITER was obtained by dividing the primary circuit in
their size increases up to limit due to turbulence forces. The 28 regions as shown in Fig. 2.
particles are carried away by the coolant and transported to the
wall (mass transport). The adhesion force of the particles I, -
between each other and with the wall (deposit or oxide) is
assumed to be of magnetic origin. Deposits formed in this
way are under the influence of shear stresses and in some
cases release by erosion can take place. Activation occurs
when ions and cruds pass through the sections under flux. The
activated nuclides, after transportation by the coolant,
penetrate by molecular diffusion inside the deposit and inner
oxide layer and activate them. According to the PACTOLE
model, deposits are ACP particles subject to transport and
erosion and can be considered as mobiliseable inventory (MI);
oxides, on the contrary, are well fixed to the piping wall and
cannot be mobilised during accident conditions.

QUARTER COOLING LOOP AND ITER OPERATION


MODELLING

In order to assess the ACP for 'a quarter cooling loop, the
mid-94 FW-blanket design information (FW combined with
baffle, limiter and blanket shield) was considered. Reference
documents were ITER Technical Advisory Committee n. 4
(TAC-4) [2] and design data of PHTS. Geometric data and
hydraulic characteristics of the quarter loop in outboard
segment channels were processed to obtain the same for the
inboard channels, as they were not stated, taking into account
the different flow rate; 103.6 kg/s for each outboard sector and Fig. 2 ITER quarter FW/SB cooling loop schematisation
73.1 kg/s for each inboard sector. The main parameters
considered to describe the ITER first wall and shielding To run the code, the data required for each region are wetted
blanket quarter cooling loop are listed in Table I. Three
different materials were considered for the cooling pipes. The surface [m21; ratio of open-pore surface to geometric surface;
composition of AISI 316L stainless steel of the FW/SB distribution of the neutron flux; surface roughness [m];
piping was taken from a JCT document [3]; the others were percentage of the coolant flow rate; weight composition of
based on engineering judgement (See Table 11). the material in the region; fluid speed [m.s-l]; equivalent
hydraulic diameter [m]; average temperature of the fluid ["C];

334
temperature of the wall at the region outlet ["C]; relaxation well as not. The former hypothesis is more adherent to
length, which takes into account disturbance in the fluid reality, because it is envisaged that the coolant will flow
motion (i.e. sharp change in the flow area) [m]; coefficient inside the FW/SB modules for most of the dwell periods in
taking into account gravity effect. For each of the ten order to remove the decay heat and corrosion products
activation reactions considered in PACTOLE to model the precipitated onto the piping inner surface. The simulation
activation processes, the following data are necessary: times examined were 4320 days (1080 days burn + 3240 days
reaction rate [s-l] (product of 0.0 integrating the isotopic dwell) for coolant flowing during dwell periods and 1081 days
abundance); ejection rate [s-l]; capture rate [s-'1; recoil range (1079 days full power + 2 days 50% power) for the other
assumption. Two general comments can be made. Regarding
[g . cmT2]. The reaction rate related to the different materials the water chemistry (dwell-stagnant case), the basic
in the various spatial regions was evaluated using the EAF comparison of the nearly pure water (pH300 oc = 5.7) versus
Activation Library of the ANITA-2 code for the nuclear
Li-addition (pH300 o c = 7.1) is as follows: ACP loop
reactions involved and the neutron flux distribution. The 1-D
discrete ordinates technique was used to perform a neutron potential MI is reduced by about one order of magnitude, but
transport analysis by means of the integrated computational this is counterbalanced by an increase in the stainless steel
approach for radiation transport AMPX-SCALE-ANITA [4]. corrosion rate and, consequently, in activity in filters and
The SSP3 approximation was implemented to solve the resins and i n larger fixed oxides on the piping walls.
Furthermore, due to the higher equilibrium solubility of ions,
Boltzman neutron multigroup transport equation using the the deposition of particles on the piping surfaces is reduced,
171 energy-group structure VITAMIN-C library derived from leading to a lower deposited activity. This can be explained
nuclear data, to produce neutron flux distributions. In order to by the different capabilities of filters and resins in removing
give a unique reaction rate for each activation reaction, the cruds and ions from the coolant, which is enhanced in the case
neutron flux of the different regions of the geometric model of higher ACP mass concentration (pH300 oc = 5.7), thereby
(10 inboard and 10 outboard, in radial sense) was averaged, reducing the decontamination role of deposition on the
using their wet surface as weighting factor. Once the average piping. Thus, the water chemistry preferred depends on what
flux for the inboard inlet and return channels and for the is more important - mobiliseable source term or personnel
outboard inlet and return channels was worked out, starting doses.
from corresponding cross sections and from radionuclides
isotopic abundance, the reaction rates were determined. Considering the operative scenario for coolant flowing during
dwell time, three major differences influence the results:
The ITER operating period was simulated for PACTOLE runs
according to the procedure used for the activation calculations. more time for corrosion to occur;
Given the absence of boron, two different water chemistries more time for isotopes to decay;
with no B were considered for the entire operating period [ 5 ] : more time for water chemistry equipment to operate.
the first with a lithium content equal to 0.43 ppm and a
reference pH at 300 "C equal to 7.1; the second with very low The net impact of these factors depends on the water
content of Li (loF4ppm) and a reference pH at 300 O C equal chemistry condition and whether one refers to mobiliseable
to 5.7, (practically pure water). In both cases the H2 content "deposits" versus "oxides". At pH = 7.1, the deposit activity
was set at 35 c m 3 s ~ p / k g corresponding
, to about 3.1 ppm. for dwell flowing is 76% of dwell stagnant, the oxide activity
The fraction of total flow rate derived to CVCS (chemical and increases by 9010, the total ex-vessel deposit activity is 35%
volumetric control system) was assumed equal to 1%, with a higher. The potential MI is 76% of dwell stagnant, while the
cleaning efficiency of resins and filters = 90%. No total loop inventory (including MI plus resins and filters plus
replacement of cleaning media was considered. oxide activity) is 91% higher. At pH = 5.7, the deposit
activity for dwell flowing is about 2.1 times higher than that
RESULTS AND DISCUSSION for the dwell stagnant case, the oxide activity is 4.4 times
higher, the total ex-vessel (deposit + oxide) activity is 7.8
times higher. The potential MI is about 2.1 times higher,
Some PACTOLE calculations were carried out, varying the
while the total loop inventory (including MI plus resins and
following parameters:
filters plus oxide activity) is 4.9 times higher.
coolant flowing, or not, during dwell periods; B. Different compositions f o r FW/SB AISI 316.5
AISI 316L composition; Mid-94 (Mn = 0.187%, CO =
0.0001%)and End-94 (Mn = 1.8%, CO= 0.17%)); Considering a fluence of 3 MW.y/m2 and the coolant flowing
fluence = 0.3 MW.y/m2 and 3.0 MW.y/m2. during dwell times, the influence of different AISI 3 16L
compositions for FW/SB piping was investigated. T h e
In Table 111all PACTOLE results are summarised. corrosion behaviour is nearly the same, due to the same
operative conditions and practically the same AISI 3 16L
A. Coolant flowing, or not, during dwell periods composition. The main differences are found for coolant,
oxide and deposit activity. The total loop potential
The ACP assessments, for a 3 MW.y/m2 fluence and Mid-94 mobiliseable inventory is about twice for AISI 3 16L enriched
316L composition, were carried out considering the coolant in CO and Mn, for both water chemistries (actually 2.2 for pH
flowing during dwell times (including shutdown periods) as = 5.7 and 1.8 for pH = 7.1). The out-of-flux deposit activity
increases by 3% for pH = 5.7 and by 9% for pH = 7.1.

335
Table 111
Overall PACTOLE results

Fluence [MWy/m2 ] 3 3 3 0.3 0.3


Coolant flowing during dwell YES NO YES YES NO
periods
AIS1 316L formulation Mid-94 Mid-94 End-94 Mid-94 Mid-94
Water Chemistry p H 3 0 0 0 ~ 5.7 7.1 5.7 7.1 5.7 7.1 5.7 7.1 5.7 7.1
Coolant activity [GBq/m3] 2.06 0.057 0.854 0.023 2.47 0.095 0.513 0.077 0.702 0.078
ACPs total mass in the coolant [g] 19.74 1.83 14.28 2.87 20.02 1.85 25.62 2.73 30.65 3.04
ACPs total mass deposited on piping 4440 1827 716 6447 4253 1996 3058 3095 9777 4686
walls [g]
Average release rate 5.29 0.51 5.73 0.85 5.33 0.52 6.55 0.73 9.89 1.19
[mg/(dm2.month)]
Total specific activity on in-vessel 2892.3 331.7 652.5 183.0 4936.3 637.7 398.7 96.9 262.5 80.2
surfaces [GBq/m2]
Oxide specific activity on in-vessel 2889.8 321.5 650.8 169.2 4928.7 619.0 395.0 81.2 235.6 61.4
surfaces [GBq/m2]
Deposit specific activity on in vessel 2.5 10.2 1.7 13.8 7.6 18.7 3.7 15.7 26.9 18.8
surfaces [GBq/m2]
Total specific activity on out-of- 1.95 0.88 0.25 0.65 2.00 0.96 0.86 1.38 1.98 1.29
vessel surfaces [GBq/m2]
Total deposit activity [GBq] 29621 78396 14223 102988 66137 139551 31180 120131 203520 146547
Total coolant activity [GBq] 421.0 11.7 174.9 4.8 505.3 19.5 105.1 15.9 143.7 15.9
Total loop potential mobiliseable 30.0 78.4 14.4 103.0 66.6 139.6 31.3 120.1 203.7 146.6
inventory (MI) [TBq]
Total loop inventory (excluding 20739 2381 4680 1316 35331 4571 2862 703 1892 583
resins and filters) [TBq]
Resins + fdters activity [TBq] 2624 144 112 9 3000 172 141 15 52 6
Grand total loop inventory 23363 2525 4792 1325 38331 4743 3003 718 1944 589
(including resins + filters) [TBq]

This can be explained by the much higher activity for the ORE) and PACTOLE seems to be a suitable tool for coping
radionuclide 6oCo (an increase of three orders of magnitude with it. The relevance of some parameters concerning the
for oxide activity and two orders of magnitude for deposit design (material composition) and operation (water chemistry,
activity on regions under flux and activity dispersed in the coolant T, filters replacement frequency) have been outlined.
coolant). The increase of activity due to Mn-56 is in the range A PACTOLE version with a new model to handle the
of 1.7 - 3.8. Thus, no significant consequences in terms of Cdwater corrosion is under development by CEA. This new
ORE due to routine inspection and maintenance on ex-vessel version will make it possible to perform the ACP assessment
part of PHTS, but an increase for MI of a factor around 2 for the divertor cooling loops.
could be expected in the case of LOCA.
ACKNOWLEDGMENT
C. DlfSerent jluences 3.0 MWy/m2 vs. 0.3 MWy/m2
The authors wish to thank the CEA-Cadarache Laboratory
DFWDEC/SECA/CLL for providing the PACTOLE code; in
Contrary to what one would expect, the loop activity for particular, Dr. S. Anthoni and Dr. J.C. Robin for their help and
lower fluence is no less than the corresponding activity for a assistance in using of the code.
fluence of 3 MW.y/m2, especially for the deposit activity.
There could be two main reasons: the numerical relevance of REFERENCES
shorter-lived isotopes such as 56Mn, so that an equilibrium
value is reached in a short time; and the greater deposit mass
[I] P. Beslu, "PACTOLE: A Calculation Code for Predicting Corrosion
on the piping wall, due to the shorter available time for Product Behaviour and Activation in PWR Primary Coolant Systems",
cleaning media to operate. Thus, considering the coolant SCOS/L,CU90-096, March 1990
[2] P. Rebut, "Detail of the ITER Outline Design Report", ITER TAC - 4, S.
flowing during dwell periods, the potential MI is higher, Diego Joint Work Site, January 10-12, 1994.
while the total loop inventory (including oxides and cleaning [3] G. Saji and E. Cheng, Initial Activation Products Data for Safety Design
media activity) is lower (less time for corrosion to act). and Analysis (Rev. 2); S. Diego Joint Work Site, April 22th, 1994 - ITER S
71 TD 04 93-09-30 Fu.
[4] G. Cambi, D.G. Cepraga, S. Ciattaglia, L. Di Pace and G. Cavallone,
"Source Terms due to the activated corrosion product in primary cooling
loops of ITER"; Fusion Engineering and Design No29 (1995) 207-213.
CONCLUSION [5] L. Di Pace, "Activated corrosion product source terms assessment for
the ITER Heat Transfer System"; doc. ERG-FUSmCN S+E TR 18/94, Rev.
The activated corrosion product assessment is an important 0, December 1994.
task from the safety point of view (determination of MI in
accident conditions and contribution to the estimation of

336

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