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CORALUS
 
EXPERIMENT'S NAME
CORrosion of alpha-Active gLass in Underground Storage conditions
LAST MODIFIED
2004-04-15
EXPERIMENT'S ACRONYM
CORALUS
TYPE OF TEST
EBS (backfill) characterization
Glass matrix compatibility
Overpack corrosion
RN’s migration

PERSON RESPONSIBLE
Name : Elie Valcke
Email : evalcke@sckcen.be

R
COLLABORATIONS
SCK•CEN, CEA-Valrhô, GRSJNC

FINANCING ORGANISM(S)
NIRAS/ONDRAF, EC

GLOBAL BUDGET (k€)
~7000 (1997 – 2014)

Phenomena
Components
Safety (sub) functions concerned (if relevant)

i

Corrosion
Glass matrix
SF
C
D
L
SSF
C1
C2
R2
ii
Corrosion
Overpack
SF
R
D
L
SSF
C2
R1
R2
iii
Corrosion
EBS
SF
D
L
SSF
C1
R1
iv
Migration of RNs
EBS
SF
C
D
L
SSF
C1
C2
R1
v
Chemical
Glass matrix
SF
C
D
L
SSF
C1
C2
R2
vi
Chemical
Overpack
SF
R
D
L
SSF
C2
R1
R2
vii
Chemical
EBS
SF
D
L
SSF
C1
R1
viii
Thermal
Glass matrix
SF
C
D
L
SSF
C1
C2
R2
ix
Thermal
Overpack
SF
R
D
L
SSF
C2
R1
R2
x
Thermal
EBS
SF
D
L
SSF
C1
R1
xi
Hydro-mechanical
EBS
SF
D
L
SSF
C1
R1
xii
Irradiation
Glass matrix
SF
C
D
L
SSF
C1
C2
R2
xiii
Irradiation
Overpack
SF
R
D
L
SSF
C2
R1
R2
xiv
Irradiation
EBS
SF
D
L
SSF
C1
R1
xv
Gas generation and transport
EBS
SF
D
L
SSF
C1
R1
 
Background

Before one can take a decision on the technical feasibility of the geological disposal of vitrified high-level long-lived radioactive waste (HLW), the post-closure performance of the entire repository system must be assessed to be able to demonstrate the safety of the disposal concept. The common approach to obtain information for predicting the long-term performance of HLW glass basically consists of laboratory tests and modelling work. The laboratory tests include the evaluation of the various interactions between the HLW glass and the engineered and natural barriers. The experimental results are used to derive parameter values for the conceptual models that aim to describe the observed glass dissolution processes. Source terms can then be defined that describe the expected performance of the disposed HLW glass.

Surface laboratory tests inherently are performed under conditions that are not always representative for the expected repository conditions, especially when a longer test duration is envisaged. Moreover, most laboratory experiments do not integrate all components and processes that influence the glass corrosion. These drawbacks contribute to the existing uncertainties and unreliability of the modelling results. Especially the general public experiences these long-term predictions on HLW glass performance as non-convincing, relying on the argument that they are based on experiments performed under unrealistic laboratory conditions.

In situ tests in the URF HADES enable to perform glass corrosion tests under very realistic conditions, especially for longer test durations, and to integrate all the relevant processes. Therefore, the results from such in situ tests can put in perspective the results from laboratory tests, and hence contribute to increase the reliability of the glass alteration and source term model estimations for vitrified HLW.

 
Objective of the experiment

The objective of the overall CORALUS project is to confirm that the existing long-term predictions on the performance of the SON68 18 17 L1C2A2Z1 reference glass, which are essentially based on the results and insights from surface laboratory experiments, are reliable. This will be done by confronting these data with the results on glass corrosion and radionuclide leaching and migration that are obtained from an integrated in situ corrosion test, performed under very realistic conditions (radioactive glass samples, backfill materials exerting a high swelling pressure, g?irradiation, controlled temperature,...). The conclusions of this comparison will be reported in a final report that will allow both the waste management agencies, the waste glass producers, and the regulatory bodies to evaluate their actual opinion on the technical feasibility of the geological disposal of this waste form, and on the relevance of laboratory-scale glass corrosion tests for deriving parameters for long-term HLW glass performance.

Together with the SON68 glass samples, also samples of other materials are placed on the different CORALUS test tubes for study of the global dissolution (glass), and global corrosion and local pitting corrosion (container materials):

  • non-radioactive PAMELA glass samples from the former Eurochemic reprocessing plant (SM513, SM527, SM539);
  • candidate materials for the metallic overpack: the austenitic stainless steels AISI 316LhMo and UHB 904L and the carbon steel TStE355.
 
Description of the experiment

Design:

Figure 1: Three-dimensional cut-away view of a large test tube (with 60Co sources).
 
Protocol/explanation :
  • Five test tubes, placed at a distance of 4 to 5 m away from the underground laboratory. The two test tubes hosting 60Co sources are placed vertically, the three test tubes without 60Co sources are placed in a downward angle of 45 ° (see Figure 2).
  • Each test tube consists of three separate modules.
  • Each module contains eight SON68 reference glass samples: two non-radioactive, and six radioactive samples (two doped with NpO2, two with PuO2, and two with Am2O3), loaded on an inner stainless steel support tube. In addition to the SON68 samples, each module contains also other types of glass samples and container materials (see under “Objectives”)


Figure 2: Implantation of the five CORALUS test tubes in the Test Drift of the URF HADES.

  • Glass samples are in direct contact with one of the three backfill materials:
    • dried Boom Clay (Belgian option);
    • bentonite (60 wt%) with sand (35 wt%) and graphite (5 wt%) (Belgian option);
    • bentonite (95 wt%) with powdered SON68 glass frit (5 wt%) (French option).
  • A partially porous outer support tube allows equilibration with the Boom Clay pore water.
  • Built-in piezometers allow to additionally inject Boom Clay pore water and to sample the interstitial solution in the backfill materials during the test.
  • Heating elements enable a working temperature of 30°C or 90°C.
  • In two of the five tubes, three 60Co sources of 500 Ci each will be placed (one per module). Test tubes with 60Co sources will be heated to 90 °C, and simulate the initial disposal phase. Test tubes without 60Co sources will be heated to 30 °C, and simulate the long-term disposal phase.
  • During the test: monitoring of temperature and pore water pressure; sampling and characterisation of the interstitial solution (ionic composition, dissolved gases); on-line measurement of pH and redox potential.
  • After the test: glass analysis (mass loss; SEM-EDS; EPMA, SIMS); radionuclide migration profile; clay characterisation (SEM, XRD).
 
Instrumentation :
  • Thermocouples on inner and outer support tubes
  • Total pressure sensor on the test tubes without 60Co sources
  • Built-in piezometers in inner and outer support tube, each equipped with a water pressure sensor.
  • On-line measurement of pH and redox potential by means of flow-through cells connected to the piezometers.
 
Status/timing/planning :
  • Emplacement of cold (non-radioactive) tube in April 1998 (tube 1; non-radioactive glass samples; no 60Co sources; 90°C). Recovery and dismantling of cold tube in June 1999.
  • Emplacement of radioactive tubes in April 2000 (tube 2; no 60Co sources; 30°C), April 2001 (tube 3; 60Co sources; 90°C); October 2001 (tube 4; 60Co sources; 90°C), and October 2003 (tube 5; no 60Co sources; 30°C).
  • Operation of radioactive tubes (same order) from February 2001 to April 2004, December 2002 – March 2004, April 2003 – March 2009, and (expectedly) May 2004 – April 2014.
  • Recovery of radioactive tubes (same order) in April 2004, March 2004, February 2009, and October 2013, each time immediately followed by dismantling and analyses.
 
Associated works :
  • ·Previous and ongoing projects on dissolution/corrosion of glass and container materials (experimental and modeling work)
  • CERBERUS, other in situ corrosion tests
 
(Preliminary) Results of the experiment :

At present, the radioactive test tubes are still in operation. Hence, there are only the first results on the composition of the interstitial solution of the different backfill materials and for the different conditions (30 °C, no gamma irradiation, 90 °C with gamma irradiation). All solutions are characterized by fairly high salt contents, which are higher for the test tubes at 90 °C. pH values are in the average about 1 unit lower for the tubes at 90 °C. In analogy with the results of the CERBERUS in situ test, we expect that this will have a beneficial effect on the glass dissolution (i.e. a lower dissolution at lower pH). In contrast, redox potentials seem to be higher (less negative) for the test tubes at 90 °C. The differences in pH and redox potential might affect the solubility and the speciation of the leached radionuclides, and hence their migration rate.

The total alpha activity in the piezometer solutions is always below the detection limit for the modules with the bentonite-based backfill materials. For the module with the dried Boom clay, the total alpha activity fluctuates around the detection limit. Alpha spectrometry showed that an occasional small measurable alpha activity is due to the natural radioactivity of Boom clay (U-isotopes). These results demonstrate also that the (four) pre-compacted backfill blocks have strongly swelled, sealing the remaining voids in the modules. This was already demonstrated during the dismantling of the first “dummy” test tube (see bibliography, EUR 19143).

 
Conclusions :
The operation of the radioactive test tubes is ongoing, and proceeds without important problems. First results on glass corrosion and radionuclide migration are expected by the end of 2004.However, after two years of testing, no alpha activity is detected in the piezometer solutions
 
Bibliography :
  • E. Valcke, P. Van Iseghem, N. Godon, and N. Jockwer, "CORALUS: an integrated in situ corrosion test on a-active HLW glass", Proc. Euradwaste 1999 – Radioactive waste management strategies and issues, C. Davies Ed., EUR 19143, 2000. Also published as SCK•CEN report R-3494, 2000.
  • E. Valcke, P. Van Iseghem, S. Smets, S. Labat, N. Godon, N. Jockwer, and K. Wieczorek, "An integrated in situ corrosion test on a-active HLW glass", EUR 19795, contract n° FI4W-CT96-0035, 2001.