Conditioning of cladding waste

Directorate-General For Translation European Commission

Description

Press compaction and encapsulation by low melting metal alloys
Nuclear energy and safety

Informations

• Publié par: EUROPEAN-COMMISSION
• Nombre de lectures: 12
• Langue: English
• Poids de l'ouvrage: 3 Mo

Extrait

ISSN : 0379-4229
CODEN : EARRDF 4(2) 305-560 (1982)
REPRINTED FROM
VOLUME 4
N UMBER 2 EUROPEAN I 982
APPLIED RESEARCH
REPORTS
A Journal of European Science
and Technology
NUCLEAR SCIENCE AND TECHNOLOGY SECTION
Published for the Commission of the European Communities,
Directorate-General for Scientific and Technical
Information and Information Management
CONDITIONING OF CLADDING WASTE : PRESS COMPACTION AND ENCAPSULATION
BY LOW-MELTING METAL ALLOYS
By J. Broothaerta et al. (EUR 7876)
Harwood Academic Publishers
ï* ¿13
European Appi. Res. Rept.-Nucl. Sci. Technol.
Vol. 4, No. 2 (1982), pp. 413-534
0379-4229/82/0402-413 $ 18.80
Printed in France
CONDITIONING OF CLADDING WASTE :
PRESS COMPACTION AND ENCAPSULATION BY LOW-MELTING
METAL ALLOYS
(Final Report)
J. BROOTHAERTS, L. DE WILDE, F. CASTEELS, P. DE REGGE,
J. VANDERSTEENE, H. VANBRABANT
Studiecentrum voor Kernenergie I Centre d'Etude
de l'Énergie Nucléaire, S.C.K. /C.E.N., Mol, Belgium
This work was performed as part of the European Atomic Energy Community's Indirect
Action Programme (1975-79) on "Management and Storage of Radioactive Waste" — Action
No. 2 : Decontamination and Conditioning of Cladding Hulls from Irradiated Fuel Elements,
Contract No. 030-76-11 WAS Β
EUR 7876
©ECSC, EEC, EAEC, Brussels and Luxembourg, 1982 ¿u
TABLE OF CONTENTS
PREFACE
1. INTRODUCTION
2. EXAMINATION OF FILLING ALLOYS
2.1. Metallurgical data
2.2. Literature review with respect to corrosion
2.3. Experimental corrosion studies
2.4. Leaching of embedded compacts in Antwerpian ground water
2.5. Interaction of lead alloys with cladding waste components and
canister materials
2.5.1. General
2.'5.2. Experimental studies
2.6. General conclusions and selection of the embedment alloy
3. LEACH TESTING OF ACTIVE HULLS
3.1. Introductory remarks
3.2. Sample preparation
3.2.1. Embedded hulls
3.2.2. Bare hulls
3.3. Experimental set-un
3.4. Analytical techniques
3.5. Results
4. TECHNICAL STUDIES
4.1. Compaction of unirradiated cladding waste components
4.1.1. Experimental
4.1.2. Results
4.1.2.1. Effect of compaction parameters
4.1.2.2.t of hydrogen
4.1.2.3. Effect of other cladding waste components
4.2. Embedment in low-melting alloys
4.2.1. Experimental procedure
4.2.2. Results
4.2.2.1. Effect of the casting technique
4.2.2.2.t of other parameters on rest porosity
4.2.2.3. Hydrided zircaloy
4.2.2.4. Shrinkage of filling alloy during solidification
5. CONCEPTUAL STUDY
5.1. Cladding waste arisings and activity data
5.2. Conditioning 415
5.2.1. Reference process
5.2.1.1. Design basis
5.2.1.2. Process description and facility lay-out
5.2.1.3. Processing capacity
5.2.2. Press design
5.2.2.1. Technical characteristics
5.2.2.2. Press operation and maintenance interventions
5.2.2.3. Lifting carriage and ejection slide
5.2.3. Embedment oven
5.2.3.1. Heating power
5.2.3.2. Oven construction
5.2.3.3. Canister cooling
5.2.4. Canister and loading system
5.2.5. Welding station
5.2.6. Secondary waste
5.2.7. Cost estimate
5.3. Product characteristics
5.3.1. Thermal conductivity of product matrix
5.3.2. Radiation aspects
5.4. General : availability of lead
5.5. Hot-cell test unit
6. CONCLUSION
REFERENCES
ACKNOWLEDGEMENTS ¿16
SUMMARY
Experimental and conceptual studies have been carried out with a view to
develop a conditioning process for cladding waste based on press compaction
and lead matrix formation.
Potential embedment alloys, including Pb,Pb-Sb, Pb-Te, Pb-Sn, Pb-Ag and
Pb-Sn-Ca formulations, and samples cut from compacted zircaloy tubing
embedded in Pb 1.5. Sb-alloy, have been submitted to long term corrosion
tests in demineralized water, in groundwater from the aquifer covering the
Boom-clay formation in the Mol-region and in an atmosphere containing
nebulized clay-water. Whereas strong corrosion was observed in the deminer­
alized water, most of the alloys exhibited excellent resistance to the
groundwater and to the clay-water mist on account of the build-up of
protective surface layers. Pure Pb and the Pb 1.5 Sb-alloy were found to
present the best overall corrosion resistance. Based on the specimen weight
changes measured, then rate zas 0.1 to 1 Um y -1 in the ground­
water, 1.5 to 2 Um y-1 in the humid atmosphere and of the order of 100 Um
y-1 in the demineralized water. The nature and composition of the reaction
products formed have been determined by structural analysis techniques.
Interactions of the proposed embedment alloy, Pb 1.5 Sb, with the cladding
waste components and with candidate canister materials have been examined.
Effective wetting of zircaloy was only obrained after long contact at
higher temperatures. Deleterious effects on the canister material were
found to be due to impurities present in the embedment alloy used in the
preliminary tests and were avoided by using an alloy composition of better
purity.
Samples of compacted, inactive, zircaloy tubing embedded in Pb 1.5 Sb
showed excellent resistance to leaching by Antwerpian groundwater. The
product quality with respect to the immobilization of radio-active contam­
inants could not be demonstrated however, as excessive contraction of the
embedment alloy occurred in test samples prepared with uncompacted hulls
from an irradiated fuel rod.
Appropriate work conditions for the conditioning process have been deter­
mined in technical-scale tests with inactive materials. The volume reduc­
tion achived, and product density obtained, were measured at different
compaction pressures, waste compositions and press loading conditions.
Densification to 70 7, of the density of zircaloy is obtained at 245 MPa, to
60 % TD at about 140 MPa. No special effects were observed in the case of
hydrided zircaloy. The compacts formed were satisfactorily embedded in Pb
1.5 Sb at a temperature of 723 K. Casting of the alloy at atmospheric
pressure resulted in a product with rest porosities corresponding to 15-18
vol. Z, whereas this was only 3-5 vol. 7, after a preliminary degassing of
embedment container to 150 Pa. 417
Examination of product sections indicated that excellent penetration of the
embedment alloy occurs even in highly densified zones, and that adequate
joining with the waste components is obtained, although no soldering
interaction with zircaloy is found at this embedment temperature. The rest
porosity was found to consist of isolated voids, scattered throughout the
matrix.
Conceptual work has been devoted to the industrial applocation of this
conditioning method, and a suitable process lay-out for the waste arisings
from medium to large-capacity reprocessing plants has been developed. With
a press force of 15 MN, waste batches of 20-25 kg would be compacted to 60
% TD in a die of 340 mm diameter. This corresponds to a volume reduction
factor of about 4.4. The briquettes formed would subsequently piled-up in
closely fitting storage canister which, after evacuation to 150 Pa and
heating to 723 K, would be filled-up with the embedment alloy. At a total
height of 1500 mm, these canisters would contain the cladding waste aris­
ings from about 1.4 tU. A basic design of the press, adapted for remote
operation and maintenance, and a functional lay-out of the process cells
and equipment have been worked out.
Cost estimations made for an application in a 300 tU/y -plant indicated
that the cladding waste produced could be conditioned at an expenditure of
80 000 BF per tU processed.
In completion of this programme, preparative work has been devoted to the
definition of the equipment to be installed in a hot cell test facility for
further work with active hull materials. 418
PREFACE
The mana.geme.nt o¿ cladding umte. deienvzi ierioui concern on account o(¡
the voluminoui amounti Involved and the high leveli o(, β/γ- and a-activitieA
aiiociated. The current practiie o(¡ itonage, ¿η water-(¡tiled baiiim οι
iiloi, ¿6only provisionally acceptable ; economic and ia(¡ety requinementi
call {¡on. convention o{¡ thti law-demiXy metallic ¿map into a mote compact
and betten, isolated (¡onm.
With the view o& making iuitable conditioning pnoceA&e& available at the
time o& large-icale {¡uel reprocuiing in the member itateli, R i V-wonk in
thti (¡ield hai been initiated by the European Atomic Energy Community.
Presi compaction followed by embedment o& the demi^ied material in loui-
melttng lead alloy ¿i pnopoied by the SCK/CEN. Tkii procesi would achieve
coniidenable volume reduction and aaure immobilization o(¡ the (¡tiiion
products and TRU-elementi present in a matnÂx o{¡ high integrity and long
tehm itabiliXy.
The development pn.ogh.amme undertaken included :
- examination and ielection o{ appropriate embedment alloyi with regard to
the conAoiion and leach resistance ;
- detenmination o{¡ the open.a