106
KAERI/AH-483/98 KR9800586 Leach Behavior of High-Level Borosilicate Glasses under Deep Geological Environment 1998. 2 29-41
KAERI/AH-483/98 KR9800586
Leach Behavior of High-Level BorosilicateGlasses under Deep Geological Environment
1998. 2
2 9 - 4 1
1998. 2.
O]
* ! £ • • § •
Eh,
— 1 -
ABSTRACT
This report presents an overview of the activities in high-level
radioactive waste glass which is considered as the most practicable form
of waste, and also is intended to be use in the disposal of national
high-level radioactive waste in future.
Leach theory of waste glass and the leach effects of ground water,
metal barrier, buffer materials and rocks on the waste glass were
reviewed.
The leach of waste glass was affected by various factors such as
composition, pH and Eh of ground water, temperature, pressure, radiation
and humic acid. The crystallization, crack, weathering and the formation
of altered phases of waste glass which is expected to occur in real
disposal site were reviewed. The results of leaching in laboratory and
in-situ were compared. The behaviors of radioactive elements leached
from waste glass and the use of basalt glass for the long-term natural
analogue of waste glass were also written in this report.
The appraisal of durability of borosilicate waste glass as a waste
media was performed from the known results of leach test and
international in-situ tests were introduced.
- n -
1
4. ^ X T ^ 0 ! ] ^ - ^ 41 # 46
b. —r^l'::ir T3.^-— "n nf 75
80
T^r ^;1- -r/ J=L -gJ QQ
NEXT PAQE(S)left BLANK
3.
Table 1. Compositions of borosilicate waste glasses. 5
Table 2. Effects of waste glass components on processingand product performance. ; 6
Table 3. Representative cooling rates and temperature rangesused in simulated canister cooling heat treatment. 9
Table 4. Solubility of rare-earth elements in glass, mass
percentage fraction of LnxOy. 9
Table 5. Experimentally determined reaction rates at 90 *C. 22
Table 6. Allowed release rates of Np, Pu and Am isotopes
from canistered DWPF glass. 25
Table 7. Variables affecting nuclear waste glass leaching. 31
Table 8. Factors that affect alteration of commercial and
waste glasses. 44Table 9. Compositions of Ballidon Tests (wt.%). 57
Table 10. Characterization of 1 & 2 year Ballidon samples(pineapple slices), (SEM, XES, WAXD and SIMSanalyses). : 58
Table 11. Comparison of mass losses (in g • m"2) for someof the main glasses in various experimentalconditions. 62
Table 12. Conditions for the Round Robin Test 64
_ v -
Table 13. SRL waste glass compositions buried in Stripa ofSweden. : 68
Table 14. Interactions between the components of the wastepackage and the waste form (borosilicate glass) inthe nuclear waste repository. 71
Table 15. Typical compositions of natural analogue glassesin wt.%. 73
- vi -
• «
Figure 1. Schematic diagram of multibarrier package. 3
Figure 2. The accommodation of various active wasteelements into a borosilicate glass. 7
Figure 3. Effect of glass composition on the interactionof glass and water - MCC-1 tests. 11
Figure 4. Compositional correlations of MET waste forms. 13
Figure 5. Proposed 3-stage corrosion process for wasteglasses. 15
Figure 6. Schematic of the DWPF canistered waste showingnominal physical characteristics and relevant glasscompositions. — 19
Figure 7. Schematic showing qualitative behavior of glasscorrosion vs. time. 21
Figure 8. Logarithm of the retention factors for actinidesreleased from R7T7 glass at 90 °C: (o)U, (n)237Np,( o ) 2 3 ^ , (•)239Pu, and (A)241Am. 23
Figure 9. Schematic diagram of TAV test device. 27
Figure 10. Analytical tools used to investigate METwaste glasses. 29
Figure 11. Schematics of the interrelationship of variouscomponents, reactions and reaction, productsduring glass dissolution. 32
- v j i -
Figure 12. Leachability of SRS waste glass as a functionof pH. 35
Figure 13. Deionized and deaerated leachant trends for Naand Si concentrations in gamma-irradiated (1.75x 106 rad/h) vs. nonirradiated static leach testswith PNL 76-68 glass, (a) 50 °C, (b) 70 V, and(c) 90 r trends. 41
Figure 14. Normalized mass loss from R7T7 glass. 50
Figure 15. Comparative results of moist clay test at 90 t:,soxhlet tests at 100 °C and static tests in purewater. 51
Figure 16. Weight losses of PNC reference glasses leached in
various media at 98 °C. 52
Figure 17. Boron depth profile, SIMS PO500, 364 days, 98 °C. 53
Figure 18. SEM observation of in-situ corroded glasses;
(a) SON68 (5y, 16 °C), (b) SON68 (2y, 90 °C),
(c) SM513 (5y 170 °C). 63
Figure 19. Autoclave (dimensions in mm). 65
Figure 20. In-situ testing of SRS waste glass in granite
(Stripa) and salt (WIPP). • 69Figure 21. Boron concentrations in solution in granite and
clay media. 70
Figure 22. Hydrotalcite crystals formed on the (a) R7T7 and(b) basaltic glasses ; (c) TEM micrograph showingthe plate-like morphology of hydrotalcite (R7T7);(d). electron micro- diffraction pattern obtained in
V U l -
the previous particle (2.64 and 1.53 A). 74
Figure 23. Distribution of uranium redox states. 76
Figure 24. Leach rates of metal ions from high iron glass
in pH 7 buffered. 79
- IX -
I.
1996\1S. -
. 1995\1 12
2,381
J3.^, 2010^
29,000
; International Atomic Energy
Agency)fe 2000^^1 o ] s . ^ <$ 200,000
1- ^ 25-30 %
1950^1^
^, 7fli4tq-oHA-1 A]^-§H ^ 7 | | ^ ^|7fl^^.S. ©}a)
©i
^g-fl-^-n-e) (borosilicate glass),
synroc(synthetic rock)[2, 3], phosphate glass, high silica glass, glass
ceramics, FUETAPCFormed Under Elevated Temperature And Pressures)
- 1 -
>l5l«]:
^ ^ - ^ s ] Marcoule4 La Hague 1978^1 °fl
£Efl, A^JE,
Si). -ir 2:A}
- 2 -
tRock
— Backfill— Overpack- CanisterWaste Glass
Figure 1. Schematic diagram of multibarrier package.
_ o
II.
1. ^ ^
5} 20 %3 ^
1,050-1,150
8].
^ . 1 ^ [4],
(network formers), i r^^] (intermediates), ^^^ll(modifiers)S-
] MOx(M:metal, O:oxygen)
90 Kcal/mole *]>&, 60-90 Kcal/mole, 60 Kcal/mole^l*[$]
«V(metastable) # ^ ^ S . S
4 . uL^-^ll- canister^
500 °C) © l ^ H , w o Up^^o)
514. ^AHf-ejjn.s^ioi ^-^-e)^-^ 700-750
- 4 -
Table 1. Compositions of borosilicate waste glasses
(unit : wt.%)
SiO2
B2O3
Na2O
ZnO
CaO
K2O
T1O2
AI2O3
CuO,Li2O,BaO
P205,Ni0,Cr203
Waste
76-68(U.S.A.)
40.0
9.5
7.5
5.0
2.0
-
3.0
-
-
-
-
33.0
ABS-39(Sweden)
48.5
19.1
12.9
-
-
-
-
3.1
-
-
-
16.4
POS77(Japan)
47.5
13.5
2.0
1.0
1.0
1.0
-
2.5
3.0
-
-
28.5
98-20(Germany)
40.2
10.8
21.9
-
2.2
-
3.3
1.1
-
-
-
20.5
XVQ61)
R7T7
(France)45.5
14.0
9.9
2.5
4.0
-
-
4.9
2.0
5.4
1.2
12.1
UK 209
(U.K.)
51.4
11.2
8.4
-
-
-
-
-
4.0
-
-
25.0
Table 2. Effects of waste glass components on processing and
product performance
Component
SiO2
B2O3
Na2O
Li2O
CaO
MgO
TiO2
ZrO2, La2O3
A12O3
FeaOs
U3O8
NiO
MnO2
Processing
[ncrease viscosity greatly
Reduce waste solubility
Reduce viscosity
[ncrease waste solubility
Reduce viscosity & resistivity
Increase waste solubility
Same as Na2O, but greater
effect
Increase tendency to devitrify
Increase then reduce viscosity
& waste solubility
Same as CaO
Reduce tendency to devitrify
Reduce viscosity slightly
Increase then reduce waste
solubility
Increase tendency to devitrify
Reduce waste solubility
Increase viscosity tendency to
devitrify
Reduce viscosity, hard to
dissolve
Reduce tendency to devitrify
Hard to dissolve
Hard to dissolve
Product
[ncrease durability
Low amounts increase, large
amounts reduce durability
Reduce durability
Reduce durability, but less
than Na2O
Increase then reduce durabi
-lity
Same as CaO
Increase durability
Increase durability greatly
Increase durability
Increase durability
Reduce durability
Reduce durability
Increase durability
- 6 -
• SI. B
o o# Na, LI
ir Fission Products
•>!< Corrosion Products
•»• Actinldes
Figure 2. The accommodation of various active waste elements intoa borosilicate glass.
— 7 —
SUt)-[io]. ZLe] 14 -§--8-^ JL^^ l l - canister^ ^ ^
20 w
700 °C<>1H 1000
soxhlet ^ * 1 S
«lH*>5!|t|-[l2]. ^ ] # ^ ^ Sr, Ba, Mo, B, Cr, Fe, Na, Cs ^ i *
?l Al^-°11^ Sr, Ba, Mo,
(Sr, Ba, RE)MoO4^ (RE)BSiO5
(integrity)^-
(capacity)^ °§^^ ^ 3 .
^ ^ -S-«BS|7l 4=1^ ^"^
-i- ^7H?ife. ^^=01 5^4. RUI
-8-8-ja
, Jantzen ^ ^ ^ i h ^ <&o) z^c.^ Fe2O3, RuO2
^ ^ > ^ ^ ^ [ 1 7 ] , Jain ^ ^ -
1.4 41
CeO2» ^^^J-fe &#, La, Nd, S m ^ NaxCayLnz
(SiO4)6O2 (Ln=La, Nd, Sm)^
l - S.4°\]
- 8 -
Table 3. Representative cooling rates and temperature ranges usedin simulated canister cooling heat treatment
Temperature range, °C
1000 - 720
720 - 690
690 - 500
500 - 400
Cooling rate, °C/h
-70
-7.5
-15.8
-7.7
Table 4. Solubility of rare-earth elements in glass, masspercentage fraction of LnxOy
Nuclide
LaCeNdSm
Composites (wt.%)
Phosphate
1.5 - 1.72.0 - 2.32.5 - 2.63.7 - 3.8
Borosilicate
8 - 1 31.5 - 4.2
9 - 1 410 - 15
- 9 -
10 %
780
^ ] 17 wt.%
70 Wt.%» ^ 4 * M ^o>°> * ^
Aj-«_e)7]- -yo^ul-t ^ s . ^ ZnO > MgO > CaO >
PbO > BaO ^.S-3. ^ ^ ^ 4 .
65 Wt.%^H ^ 7
> f-^o] 12 wt.%
45 wt.%o] ^.5).^7f 25 wt.%?!
, 45 wt.%
apatite ^.^°] ^"^SIAJ 1 ^ . Time-Temperature- Transformation diagram
45 wt.% ^ ^
-i- 45 wt.%
^Sj-^l-froimXKfree energy of
hydration)^- ۥ
t|-[22]. MCC-1
-8-Sj# * ^ , Waste Isolation Pilot Plant(WIPP)^
- 1 0 -
1000.
"el
CO
o
-a
a£o
100.
10
0.1
XX
EA glass
*
^
Projected range forDWPF glasses
O Waste Glasses
• Antique Glasses
X Medieval Glasses
• Natural Glasses
D Commercial Glasses
Jasalu
•Tcktiles
l "tD
Pyrex
Sjodu
LibyanDesert
Silica
-200 -150 -100 -50 0 50Free Energy orHydration (kcul/kg glass)
100
Figure 3. Effect of glass composition on the interaction of glass andwater (MCC-1) tests. All glasses were immersed indeionized water (ratio of surface area of glass to volumeof water, SA/V, equals 10 m"1), for 28 days at 90°C. Plotincludes both radioactive and non-radioactive glasses.
-n-
JLSj-^l ^Ajoj] ^ ^ ^ t } - . Hanford Waste Vitrification Plant (HWVP)^l
Composition Variability Study
41[23], J Z ^ ^ l ^ S ^ ^ 4 ^ - 1 ^ A M, 41 # 1 - ,
database^ ^ 4 [ 2 4 , 25].
Materials Interface Interactions Tests (MET) l *] ^ 307}
71
7}
2.
2.1
1 2 -
[85, 15. 0)
GLASS FORMERS
[60, 40, 0] [60, 15, 25]
GO
I MIIT Wastft' Forms & Svslerns
8 SOL 165/28% TDS9 HWVP-HW39
1 0 CATHOLIC U1 1 PNL 76-6812 MCCARM-113 JAERI-Z-20
AECL AS
AVB/SAN 60
TRUW WG 124
BASALT
SON 68-18
HMI PAMLEA
BNFL WG 1 4 SRL 131/35% TDS15 AECLGC MODIFIERS INTERMEDIA! CS
Figure 4. Compositional correlations of MIIT waste forms.
^ : tt&3\. go]
a)
b)
-Si-OM + H20 — > -Si-OH + M+ + OH"
-Si-O-Si- + OH" — > -Si-OH + -Si-O-
-Si-O- + H20 — > -Si-OH •+ OH"
# <+S|-<+S|-M-§r l : ^ pH 7-10
tt, Fe,
-8-«fl
42}-
Savannah River Laboratory(SRLHH
pH
- 1 4 -
HydratedBulk Glass Gel Layer
soHydrated
Liquid LeachantH*
Na OH
pH increases
Stage 1; interdiffusional Process
HydratedBulk Glass Gel Layer
•H,O
Liquid Leachant
Stage 2; Matrix D isso lu t ion
/Precip i tatedHydrated
Bulk Glass Gel LayerLayer
- H 4 S O 4
;;,H4SiO4 Liquid Leachant
H2O
N3 OH"
HT
OH
Stage 3; Surface Layer Formation
Figure 5. Proposed 3-stage corrosion process for wasteglasses.
- 1 5 -
7\
state)°fl>H
, 30].
dissolution: R = K(CS - Co)
diffusion: R = DA(CO - C)
K :
D :
C, Co, Cs : H4Si04 71
I = qL
q :
L : H ^
R = dL/dt o lHS
KCs(l - C/Cs)dL/dt = (1)
1 +
- 16-
0 = qK/D
C/Cs :
C/Cs =
SA :
V :
c»l t=0
(1 + $
a = SA/V (1/CS)
(In (1-ffD) + PL = -aKCst (2)
= 0
L + (£/2) L2 = KCst (3)
SLX}[31, 32],
n 71 canister^ fl-
- 1 7 -
canister
F =
R : J
W :
SA :
R • SA
W
^ - S (g/m2/yr)
canister^ #
(m2)
(g)
R • SA
(RF)i (RF); W
ll[35],
^: canister*!)
-18-
CDI
Free volume
61 cm
DWPF nominal fill heightequivalent to 85% by volume
about 1700 kg of glass
Dished bottom
-H
DWPF design basis waste glasscomposition (wt.%).
Component
SiO2
3,0,
AI2O3
Fe:,O3
Na2O
K2O
Li2O
u;,o8CaO
MgO
MnOTiO2
NiO
Blend
50.2
8.0
4.010.4
8.7
3.9
4.42.1
1.0
1.4
2.0
0.90.9
SRL 202
49.0
8.0
3.811.4
8.93.7
4.7
1.91.2
1.3
2.0
0.90.82
Figure 6. Schematic of the DWPF canistered waste showing nominalphysical characteristics and relevant glass compositions.
96
. Stage o]
Stage
. Stage 3 ^
S34(feedback effect)^
tfl [37], canister^ alumino-silicates^ ^:^r
^ 90
Scheetz
- 2 0 -
g
SO O3
OCC
Reaction Progress / Time
Figure 7. Schematic showing qualitative behavior of glass corrosionvs. time.
- 2 1
Table 5. Experimentally determined reaction rates at 90°C(g/m2/day)
Glass/Leachant
Static tests
PNL 76-68/DIW
SRL 165/DIW
EMS-11/DIWJSS-A/DIW
PNL 76-68/DIW
SRL 131/DIWSRL 131/J-13
SRL 131/J-13
SRL 131/J-13
SRL 202/J-13
SRL 202/J-13
SRL 202/J-13R7T7/DIW
R7T7/Volvic
R7T7/DIW
R7T7/Volvic
R7T7/Volvic
R7T7/Volvic
R7T7/Volvic
S/V (m"1)
2000
2000
200010
10
1010
2000
20,000
10
2000
20,00050
50
400
400
2000
8000
20,000
Forward rate
1.6
0.80
0.0831.5
1.8
3.00.14
0.24
0.84
0.10
0.025
0.04
Saturation rate
0.08
0.024
0.00160.0025
0.0075
0.03
0.021
0.053
0.0016
0.00250.0083
0.0133
0.0045
0.025
0.0006
0.0006
<0.0001
- 2 2 -
ItoCOI
g
0
A A A
<yo
CD
o
O
i
• i
0
. 1
•oQ
-J 1 1 L^J-
l I • f
o
0
r i i ! _ . ! _
i i i l
• .o -
-i i i i
0 100 200 300
Reaction Time, days
400
Figure 8. Logarithm of the retention factors for actinides released from R7T7• glass at 90"C(data from [reference 22]): (O)U, ( Q ^ N p , (O)238Pu,
(•)239Pu, and (A)241Am.
F = [2.5 x 10"3 g / V • d] [96 m l [365 d/yr] / [1.7 x 10b g]
= 5.2 x 10"5 yr"1
(RF)il- ^-5}T$. U 4 Npfe- 5.2 x 10~6 yr"1, Pu^- Am
1.6 x 10~6, 1.6 x 10"7 y r " 1 ^ ^ ^ 4 . J i* r^^ -
?1 ^ ^ ^ ^ J - s ^ - B l ^ ^ ^ 1 ^(0.04 g/m 2 -d) l -
Np, Pu, Am^l ^ # ^ £ 7 } 4 4 8.3 x 10"5, 2.6 x 10"5, 2.6 x 10~6 yr"1!-
, 61 ^ S -
^(inventory) <41
L, -g-
[LEACH-2]5i-
- 2 4 -
Table 6. Allowed release rates of Np, Pu and Am isotopes from canistered DWPF glass
ito
Isotopea
U-233U-234U-235U-236U-238Np-237Pu-238Pu-239pu-240Pu-241Pu-242Am-241
Am-242mAm-243
1000-yr
postclosure
inventory13 (Ci)
6.9E-55.7E-11.7E-41.4E-31.0E-22.0E-25.5E-11.3E+18.1E06.2E-61.2E-21.4E+11.5E-45.3E-3
10,000-yr
postclosureinventory (Ci)
9.2E-45.5E-12.7E-42.8E-31.0E-22.2E-2
-9.7E03.1E03.0E-61.2E-21.0E-5
-5.3E-3
NRC release
rate limit per
year (Ci)4.2E-75.7E-64.2E-74.2E-74.2E-74.2E-75.5E-61.3E-48.1E-54.2E-44.2E-71.4E-74.2E-74.2E-7
Allowed fractional
release rate (yr"1)at 1000 yr
6.1E-31E-5
2.5E-33.0E-44.2E-52.1E-51E-51E-51E-5
6.8E-23.5E-51E-5
2.8E-37.9E-5
Allowed fractional
release rate (yr"1)
at 10,000 yr4.6E-41.0E-51.6E-31.5E-44.2E-52.0E-5
11.3E-52.6E-51.4E-13.5E-5
11
7.9E-5aRadionuclides with a release that must be controlled at 1 part in 100,000 of their own 1,000-yr postclosure
inventory are underlined.bE indicates exponential notation.
Crank -Nicholson implicit methods.
S H^1 7fllH [PHREEQE],
, 44].
2.2
^ ^ ^ ^ fl^^ Chalk Ri
) , 1971\i IAEAfe a
tfl, ZL#^ ^6] A]~g-^}^ ISOClnternational Standards Organization)
23-100 °C
autoclave* ^}-§-«H ^#°^^1 ^rS.1- ^ ^ # ^ - 7>
. Pacific Northwest Laboratory (PNL)-^ Materials
Characterization Center(MCCHH fe JLs\-%] ^ # s l S ^ ^ - ^ ^ - S . MCC-1
[30], PCT(Product Consistency Test)[31] ^-i- 7fl^§>^cf. MCC-1
momoUtic ^M4r
- 2 6 -
Sampling line
Leachatesamplingvalvoi
Leachantsamplingvalve
LEACHING VESSEL
.Glass specimen
Environmental material
Peripheral heater
PRECONDITIONING VESSEL
Environmental material
Platinum proboAir
Water
Pump
Figure 9. Schematic diagram of TAV testdevice.
- 2 7 -
100-200 mesh^i 3.Q*\} &^ *}-%-*}^}, C02
H2O
Infrared Reflection Spectroscopy(IRRS), Tunneling Electron
Microscopy(TEM), Scanning Electron Microscopy(SEM), Auger Electron
Spectroscopy(AES), Secondary Ion Mass Spectrometry (SIMS), X-ray
Diffractometry(XRD), Rutherford Backscattering Spectroscopy(RBS),
Electron Spectroscopy for Chemical Analysis(ESCA), Electron Probe
Micro-Analysis(EPMA), Ion Scattering Spectroscopy(ISS), Mossbauer
Spectroscopy, Raman Spectroscopy, Analytical Electron Microscopy
(AEM), Extended X-ray Absorption Fine Structure(EXAFS), Ultraviolet-
Visible-Near Infrared wavelength (UV-VIS-NIR) spectroscopy,
- 2 8 -
ItoCD
I
SEM/EDX
SolutionAnalyses
RCP. AA. DCPl
IRRS
RBS
AES/ESCA
tc
o
SIMS(static)
I5 20A
V,
SEM9
'* ' ' 4'y w\* Precipitated Layers *' ^^^^ ^ JL' t T
WAXD
Interaction Zones
Buli. Waste Glass
SIMS(dynamic)
'is.PrecipitatedLayers
InteractionZones
Figure 10. Analytical tools used to investigate MIIT waste glasses.
AA(Atomic Absorption), ICPdnductively Coupled
Plasma) spectroscopy, a~, y —£! ^ l ^ 1 ^ , INAAdnstrumental Neutron
Activation Analysis), IDMS (Isotope Dilution Mass Spectrometry),
sa-
3.
Clark ^ ^ ^ ^ ^ ^
A]^O^ "a^l^ofl « HlS^S*l-5il4[48]. DOE l Environmental
Restoration and Waste Management (EM) S
(^•*1, Yucca Mountain ^ ^ - ^ ^ -g-^H SiS
3.1
]. Canadian Nuclear Waste
Management Program^]*\T= ^ ^ -
^^[51] , Cecillet 3 # ^ fl-^^i7> JL^-s)^ JL^-^1]^ -g-
150, 250 °C°1H
- 3 0 -
Table 7. Variables affecting nuclear waste glass leaching
1. Environmental factors
- Temperature- Pressure- Expose time- Relative humidity- Solution pH- Radiation damage- Solution composition- Presence of inhibitor in the leaching solution
2. Physical factors- Weathering vs. aqueous leaching- Dynamic vs. static leaching- Exposed surface area to solution volume ratio (SA/V)- Bulk vs. powered glass vs. glass fibers
3. Specimen state- Glass composition- Thermal history; Degree of annealing, Phase separation,
% crystallization- Prior leaching exposure history- Surface features; Roughness, Surface composition- Homogeneity of glass- Surface treatments- Stress
- 3 1 -
Solid•llor»t>onproducU
•oMiondate
R«poiiioiyrock
-halilo.conallilo,polyhtliia....
Figure 11. Schematics of the interrelationship of various components,reactions and reaction products during glass dissolution.
- 3 2 -
1/1000
0.02313}- 0.0315* £-TT J-134 GR-4 *)§}^r ^ 6.984
calcite, hydroxyapatite^
Mg~Si
17171
Q = ktff
Q :
k :
a
- 3 3 -
^54
Power Reactor and Nuclear Fuel Development Co.(PNCH*l-c-
A S ^ ^ - ^ , 5[- <y- x)-s}+, ^^°}*L7} ^7}^. ^ ^ - ^ » o
soxhlet ^ ^ ^ ^ ^ ^ ^ - ^ ^ ^ l ^ A]i§]-^4[58]. ZL oif 3.$]
. 5E?h Np-i: i^-§1-fe Nevada Test
Site (NTS)
3.2
3711 iH1^4. pH #
MgCM
^ S pH 5 -
^-^ pH
- 3 4 -
0.03
oUJ
<
V)
0.01
0 0
AClORANGE
0ESIRA81E RANGE OF pH FOR I
GROUNOWATERS DURING STORAGE
6pH
10 11
Figure 12. Leachability of SRS waste glass as a function of pH.
- 3 5 -
41 # 3 1 ^ ^#^4 pH i 44 ^ 1 44\J4. PH i~
• ^
, pH
7> 8~10
110 ^ 190 °C^ 4 ^ 1 - i - °l-g-«H ^ ^ pH< l R7T7
1 mM
^7f l§H CaMoO47>
MO7]- rfcSS]^ ^
i- 1 ^ « H , pH 6.
Pacific Northwest Laboratory(PNL)$\ West Valley Demonstration Project
[11].
^ ^ S - S . Eh^ ^ ^ 4 " 37)1
- Sf-§>JL 9XG.E-3- canister
44
- 3 6 -
U, Np, Pu
34 1-^ - #ol]
Pu^- CraA
3.3
Lurtz
95, 110-125, 200 "C
Ar+5%H2
canister°fl
4-g-fi] Arrhenius
Dissolution rate = A e~Ea/RT
A :
Ea :
R :
T :
80 kj/mole
-§-5fl7]-
# ^ 100
7J
kj/mole^-
- 3 7 -
- 8 S -
(K-t* ft ft
•[69 ' 8 9 ] - t i ^ i ^ ^ TT-fci I&U M ^ toHd -br?r?y to
^^)3;noipdoutp ^ ^ ^ ^ [ 3 [ o ' I t a ^ & t s ^ [a
"5Halo HROT [cl-#fe to^feTT ^kl|p-l*lo T-m 0002
to(SOOZ)lfe-t?TTta^
(9Uin{0A ;UBl{0B9|/SSB^S JO
'[99]-titfS
[99 '
OSS
OSZ 'OST ^-ferl: ft^[Y#^r k l b ^ ^ ^ ^ l o ^ teO. OSZ ^ S OST -[9S]
l o * « a 06
- 6 6 -
82 '
'a
^01x^9-9
9'S
|n -f-
01 -fera 06 '
ZJLAH
tol>-& '[89]
029 '
HTfo
^ 7 } &£4[73, 74].
, PNL 76-68
. 90 1
SRL165
, 77].
, 69].
McVay ^ ^ 7 ^(^Co, 2.4 X106
SA/V
pHt
- 4 0 -
(b)
oX
_J
"o
g62OO
11
1JO -
50
/
/ / ,
TIME (days)
(c)
TIME (days)
iFigure 13. Deionized and deaerated leachanttrends for Na and Si concentrations ingamma-irradiated (1.75 x 106 radAi) vs.nonirradiatcd static leach tests with PNL76-68 glass, (a) 50 TC trends, (b) 70 ttrends, and (c) 90 *C trends. Testratio at 10 m - i
3.6
Am
-fh
critical flocculation concentration(CFC)
fA]d|| ^ ^ § } ^ +2, +3,
+67} € ^ # ^ +47]- ^ i i l i q - -fM^-i-i- ^^*>7l ^rf. 4 ^ 1 Fe, Zn,
La f-5] # ^ ^ ^AVO] ^ ^ . nfliicf #0]] -g-*fl£]7l 4=1 «>£, Zr^
1 ^5.7}- 8 ppm<y
^Ad claywater°ll 3iJ
ul -n-7] -^•^.ol^.-g- ^
Pu(IV)-Sl ^r-ilr^l^rOlT-l-
M * < * * J L s N s L ^
fe ^ ^ - t - ci^l^l SJSJ:C
* *
Eu,
H83]
r €::
Am,
^1°1 #5.'
Pul W
Al, B^l 4]
!, Portland
#•§- ^ 7 M ? m
Cementl- ^^B
aj-Tiq- 7131 q-1
"r An
clay
El-U-^
water°ll
1 3*41i 11 O -5-1- 1—o" * l
1 #5*-$.
3.7 -B-Bial^M
- 4 2 -
r, SA/V
Yucca Mountain *l
canister^ ^ ^ ^ ^ ^ nfl (tfl7fl canister^ 10%^
c a n i s t e r ^
tJ-[87].
[88, 89].
Gong ^ ^ J I J H a ^ ^ 2 ^ ^ ^ 4 > ^ ^->a-i- "71 ^^-c^ SON68-a-
200 °C
- 4 3 -
Table 8. Factors that affect alteration of commercial and waste glasses
Materials8
CompositionHomogeneityPhases and impuritiesWaste Products1*
Manufacturing8
Materials processingMeltingCasting (SS canister)13
Seal/Interim storage15
Thermal history
Physical statea
Amorphous orcrystalline
CompositionHomogeneityPhases, impurities
and theirdistributions
Surface condition(roughness, flaws,charge)
Prior corrosion
history
Use or storage environmentTimeTemperatureAtmosphereMoisture contentEnvironmental cycling(e.g.,wet/dry, freeze/thaw)pH, Ehb
Geology13
Engineered barrier13
Radiation15
SA/VExternal stressesSolution compositionFlow ratePresence of microbesSolution saturation
'These control the glass characteristicsbApplies only to waste glasses
4 22, 91, 241, 908, 1013, 102111 *)J}Q] 3 W f l 4 ^ AA 0.5, 4, 6, 10,
26, <35 jm^\ *rv\)7\ £ $ 3 S l ^ , ^ . ^ l S ^ l ^ analdme, tobermorite,
apatite, weeksite ^ 4 £ £ : ^ 8 ° 1 , =L ifl- eflfe- Ag2Te03, (Ca,Sr)Mo3O9
(OH)2 ^ %%<>)
••gr smectite ^ 3 M ^- ^•^•^ ^ ^ o j j l , B^^^r y ^ S 0 ^ ^ smectite
(montmorillonite) ^
#(Zn, Cr, Fe, Ni, MnH
smectite(iron silicate and potassium iron alumina-
silicate), weeksite (uranium silicate), zeolite(calcium potassium alumino-
siUcate), tobermorite (calcium silicate) ^ 4 ^^rf!- •^e|7'}7r ^
uranium silicates^- smectite?]-^
3711
- 4 5 -
4.
4.1
X14.
7l^-(thermosyphon pore)#
near fields
^ 1 ^ 7ov Alloy 825
304L i ^ i e i i ^ 7j-oi
Fe, Na, Si,
Inagaki
magnetite^
7>«l-sat|-. Z i-o] magnetite
w ] - ^ ,
FeSiO3 1^i4 FeSi3O3(OH)8
- 4 6 -
©I ^-g- Particle Induced X-ray Emission
Spectrometry^ RBS5.
uj-
pH 7.4^1 -8-3#*l3!Hr(J-13), 90 °C, SAA^=100 m"1
SRP -B-elJl^-^^1 ^#^1^0] 316 iEj5fl^
<>1 ^ 3 g/m2oll ^
0.3, 0.01 g/m2
^^^ canisterM- overpack I l ^ i *}•%• 7}^ ^ - ^ # ^ - SRL
YQ65/TDS) jlSr^l^r ^ ^ 1 ^ ^-^f l^o] JL§±*\)<>]
•^ ^A}s|- cf. n t ^ wf^l-i- I f ^ l S *H 90
^ al^-Sl) SiS-a- ^ - ^ - ^ ^ 1 ^ , SEM, EDS, FT-IRRSS. ^^^^fec-fl , SRL
YalS|-Sfl^ -<b]o)l 3Q4L ^Ejefl^ 7^ Ti(TiCode-12), Pb, Cu(A216) ^£ r
€• ^ ^ * ^^1 ^fe 5J*.£ i4^^^[99] . ZLel 14 cf^. l-^oll^fe. Pb, Cu,
Ti-i-
- 4 7 -
pH7} 9.
fe- ^e.s.t °1 pH
l pH 9.5
, 55],
4.2
ilit
^SCsmectite, illite, bentonite, sand)7} ^%}v\ ^^7} ^ S ^ | porous
medium^] ^^ r^Ti i^ ^£51 ^ - # ^ X^ofl £;Sf- | 6_S*1 -g-^^
xl^A]7l7l nfl^-ol^-ji ^^-§1-JL SU4C1O2, 103].
# Np3f Pu-S-S ^Jtl ^fl-^-n-s]*- smectite, illite,
- 4 8 -
K, £efl, $##, Boom clay, French salt4
thfr^r clay water^ ^-f Ca^
r smectite^l
soxhlet ^
«HC/SA)7>
^ ^ C/SA7]- 3 E
«17> 1:200^1 ^ - f 3 1 ^ 1 ^ %t°] 3.7])
. 98
«171- 1:200*1-
3, 0.3 //mS.
-49 -
NL(rn) 10-3 g.cm-2 •ita•
Smectite 4aSmectite NaBcntonitcSmectite 239PuBidistillcd wat
Figure 14. Normalized mass loss from R7T7 glass.
- 5 0 -
Iat
Smectite
Activated bentorute FB2
Time (months)
Figure 15. Comparative results of moist clay test at 90 °C, soxhlet tests at 100 °C andstatic tests in pure water (mass loss results in mg).
10"3
1 - 3 -CNJ
Eo
10
10"
10-
P0500B/W= 1/200
/
__o—o—a A
o
P0500D W.
P0798D.W.
P07988/W =
P05008/W =
11
11
-
10° 10' 102 103
Leach Time (days)
10*
Figure 16. Weight losses of PNC reference glasses leached invarious media at 98 °C.
- 5 2 -
Depth (//m)
ienCOI
200 300 400 500
Sputtering Time (min)
Figure 17. Boron depth profile, SIMS. PO500, 364 days, 98 t .
600
[106]. ZLS]I4 ^ ^ ^ S l R7T7
4i(retention
A]~g- 7>^^<>1 J l ^ s ] ^ Portland ^ ]^m
K a . ^ Np, Am*
Cs, Sr^r ^flSt+olSi,
pHl- ^<^ -fre)s| ^ - i ) ^ 3711 ^7H^ l fe ^ ^ ° 1 5a4[107, 108]
Zl ^-g-
4.3
SRS
o|
[109].
1)^^11^ : S)-7j-o> ^ ^ - 3 t ^ o . s Swedich Nuclear Fuel Safety Devision of
Nuclear Fuel Supply Co.4 Florida^^-^^ ^-^«S^SAi 1982^^l^fl i4fl
Stripa - b l>H A]^5]-ZL SI4.
Studiecentrum Voor Kernenergie/Center
D'Etude de L'Energie Nucleaire(SCK/CEN)4 SRL^^l ^ - ^ ^ ^ S . ^ 1986
^z] Boom c l ay^ i
-8--8-3?
- 5 4 -
^ f l ^ ^|-g- 1986\i
. MIITe}- l-e)fe WIPP/SRL £
^ 5 ) ^ 9007B o ] ^ ^ JIS)-^ A]s.t 5007fl S]
, canister ^ ^ r overpack
3007fl ofl sfl^^l-fe ^ ^ 1 S ^ * 2000711
4.3.1 ^
^^I'ffl Stripa
^ ^ ^£(moist clay) ^ 7 l i A ^ H I ^ A } ^ 3 1 ^ ^ ^ Np, Pu,
AmAS J
t)-.
^ , 90 °C«1]Ai 2\i*«?H -e-#^ Np, Am, Pu^r A A 75,
90, 99 %7> isMIM^S-^-E-i lcm ° 1 ^ 1 fti^sa^
Np, Am, Pu^i ^o^oi^fe. zj-zj- of 2, 8, 45-240^1 ?3t*
- 5 5 -
95%
Ordinary Portland C e m e n t * *}-%-•&
Tc, Np, Pu, AmS] -g-*fl
# A | ^ ^U#£ Pu^
, 0.01% o)*}nVoj
Argonne National Laboratory
irfl
SRL SRL
. SRL
-Ei(a9)
SRL SMSS depth
profiled
calcium carbonate, magnesium manganese iron silicate hydroxide, silicon
oxide, calcium silicate, magnesium iron oxide ^
^ H&*m ^ ^ 4 f ( « o ) ^ 1 r Ca, Mg, Fe, S
^ , or^Aife Ca, Ba, Cs, Sr ^-°] ^ ^ ^ 1 5 3 ^ ^ , o]^. &$<£0.2.^1% -§-
# ^ Ca, Ba3f ul^]5.^-Ei -g-#^ Cs, Sr^-S
•56-
Table 9. Compositions for Ballidon Tests (wt.%)
\\
\\
SiCfeAI2O3
CaOFe^sFeOMgOMnO2
Na2O .Li2O
NiOCr2O3
B2O3
ZrO2
TiO2
K2O
Cs2O
CaNO3
SrOSr(NO2)2
UO2
P2O5
Nd2O3
La2O3
BaOPbOCeO2
MOO3
ZnO
Na2CO4
CoalZiolteSums
Pineapple slices165/TDS
54.104.101.5012.30
0.802.9010.304.700.90
6.801.20
0.10
0.10
99.90
131/35%TDS
39.303.301.2016.30
1.004.3012.003.402.00
9.600.400.80
0.10
0.10
0.20
1 1
1.10.20.33.5
100.1
ARM-1
46.505.592.23
6.675.08
11.301.803.21
1.16
0.45
0.655.96
0.66
1.511.871.46
98.90
Basalt
51.3417.686.0315.81
3.840.334.42
99.50
TNXTNX/PHP
43.003.681.4113.150.001,212.489.333.040.940.249.790.040.07
0.07
0.01
0.16
0.050.010.19
0.12
89.04
cores
TNX/165/TDS
46.643.851.5012.340.000.692.7410.254.410.790.026.380.070.06
0.05
0.11
0.23
0.110.030.19
0.27
91.16
Glass CubesFrit131
52.060.350.030.06
1.690.1613.305.120.100.0314.370.460.950.10
0.50
0.27
95.18
Obsidian
83.55
1.59
5.840.280.121.64
0.040.060.935.76
0.10
0.05
100.0
Pyrex
81.002.00
4.00
13.00
100.0
Silica
93.020.390.650.88
0.140.170.03
0.080.060.77
0.01
0.01
0.03
0.05
96.28
Lmtanumbasalt
46.2112.067.81
14.153.900.312.40
0.130.020.040.022.100.43
0.04
0.45
90.13
SRL-131
44.664.260.848.892.401.443.2113.594.100.98
10.580.362.02
0.06
0.05
0.36
97.80
SRL-165
Black_frit
53.14.501.748.512.300.692.059.975.170.99
7.300.67
0.08
97.13
-57
Table 10. Characterization of 1 & 2 year Ballidon samples (pineapple slices), (SEM, XES, WAXD and SIMSanalyses)
00I
Samples
165/TDS
131/35%TDS
ARM-1
Basalt
1 year
SEM/XESAverage
precipitationlayer( a)
~2M
~2n
~2M
Interactionzone(/?)
<lM
<lu
SIMSInteraction
zone(0)
0.2//
0.6//
0.6//
0.6//
WAXD
Structure/Phases
Glassy
Glassy
Glassy
Glassy
2 years
SEM/XESAverage
precipitationlayer( a)
~2/i
~2//
~2//
~2M
Interactionzone(0)
<lf*
<lM
<lfi
<lf
WAXD
Structure/Phases
Magnesium manganese ironsilicate hydroxide
Silicon oxideCalcium carbonateMagnesium manganese iron
silicate hydroxideSilicon oxideCalcium carbonateMagnesium manganese iron
silicate hydroxideSilicon oxideCalcium carbonateCalcium silicateMagnesium iron oxide
137Cs,
Cs, Mg, Sr
Ba-i-
Yucca Mountain^ -§-3 #01
"Tc, ^Np, 238U,
90, 183^2: ^ #
PNL
304L ^ e f l i 7ov^
o.^, 90 °C*\}*\ 30,
pH
8.78-9.12S
ss., pH
B, Mo, Tc
U, NP,
T c ^ ^ ^ l - ^ l 2.3 g/m2S.A^ 7}^
Tc^ 5-10 %$\ ^ # 1 - 1 :
Mofe Tc^ 85 %, Np
7]*\ -§-#£1^
4.3.2
Boom clay
- 5 9 -
Boom clay7} JL2±x\}°] ^#<^1 nl^fe <g^§- 2z*}tf-7) 4)*H 47flsj
71- Al l-o) x| | fe*l | MlaflSM ^-i^-Sa^-^, 404 90
AM-, 90 r ^ l ^ i ^#^c>] lOwfl c| ^S i :4 . ^ M 150
7} ^#^«^1 #^1)1- ^ - f ^ # ^ ^ 1 ^ 1/50S.
, 134Cs,
[110] t}€- ^ 4
Boom clay&}-
Boom clay, 90
SAN60, SM58^Aife 3LS)-^sl ifl^-^ ^ ^ ^ ^ A M - , SM58, SM
513, SON58, SON68<^|Ai^ ^#a^«HlAi cf^- ^ ^ 5 f ^ o ]
- 6 0 -
Boom clay
16, 90, 170 TC*IM 4 4 5, 2,
# X l H ^Bl-ifl^4[115]. 16
0.02-0.08 / imS 4X1 M ^ t f ^ , ^ £H*IHfe- ^ 100*1] ^ H
Boom clay ^
a a s ] S t ^7}§H clay waters.. 90 "C^l^i
^ ^ ^ 4 Pamela/DWK
^ # ^ ^ SiO2
7}
4.3.3
Round Ribon Project°lH
^r ^ l^-SSfH) ZL A l^ s^ i^ : S12S} H 19«=fl i4El-vfl^cl-[ii8, 119].
Harwell ^ ^ Tc, Np, Pu, Am|- ^ t l -frell- ol-8-t
#o] -g-^jiti. 3H^u | - ^j-oj-ofl ^ ^ ^^-^q-fe #•§-
Tsukamotoi
- 6 1 -
Table 11. Comparison of mass losses (in g • m~2) for some of the main glasses invarious experimental conditions
toI
SON68
SM58
SM513
SAN60
In-situ16 °C, 5y
-3
0.3
3
-16
In-situ90 °C, 2y
370
640
165
102
Laboratory90 °C, 2y
280
500
/
50
In-situ170 °C, 5y
2435
disin-tegrated
175
1065
Laboratory170 °C, 2y
320
1500
/
300
(a)
(b)
(c)
Figure 18. SEM observation of in-situ corroded glasses; (a) SON68(5y, 16 t ) , (b) SON68 (2y, 90 °C), (c) SM513 (5y 170 °C).
- 6 3 -
Table 12. Conditions for the Round Robin Test
1.2.3.
4.5.6.7.
8.
Temperature : 90 °CPressure : 1 bar (or higher)Waste form composition particle size :
SON68 (R7T7) glass. 150-250 m + a coupon* (25x25x3 mm)Duration :Repeated t
3*, 7*, 14, 28, 56, 91, 182, 364 days and longer*.ests : 28, 91 and 364 days
Blank tests (no glass) : 28, 91, 182 and 364 daysSolids
Salt
Clay
Granite
SolutionsSaltClayGranite
Glass 2 g powder + coupon*Backfill 200 cm3 saltRock
Glass 2 g powder + coupon*Backfill 92 g smectite clay, 92 g sandRock 182 g3 Boom clay from Mo I
Glass 2 g powder + coupon*Backfill 5 cm smectite clay
95 cm3 sandRock 100 cm3 granite
NaCl, CaSO4, KC1, MgCl2) H2OSynthetic interstitial clay waterVolvic mineral water
* Optional
-64
enI
Granite
two layers
Clay
one layer
Salt
one layer
Sand + Smectite
(95:5 volume)
Granite Powder( < 1mm)
Volvic mineralwater
Clay +Sand +
Smectite
(50:25:25 wt.%)
Solid salt
Synthetic clay water Brine
1. Vessel 2. Lid 3. Specimen holder4. O-ring 5. Lid retaining bolts
6. Thermocouple well7. Leachant inlet and outlet8. Stainless steel mesh 9. Leachant
Figure 19. Autoclave (dimensions in mm)
Group 1 : Mo, B, Li, Cs, Nd
2 : Si, Na, Al, Sr
3 : Fe, Zr
4 : Ca
Group
- g ^ S . - ^ <*^ & # ^ ulHtb ^ 4 y>^-^^- »«fl B, Li,
20-60 %
* T - W ^ I } . Group
Group 3^r ^ § ^ M
-g-o^o] ^^^ .c l - c-1 3J-711 ^ # 4 . ^ H ^ i 1 ? ] Cs l- Sr^l Normalized
Elemental Mass LOSS(NEML)TT B, Li, Mo, Na°ll «l«fl 1/10 «1 > 1 &•%;
. Si, Li, C s t B,
l^ ^ j i ^ 1 ^ | l i l fl]. si
S.71- ^ 50 ppmA5. a ] ^ ^ ^ ^e|7l-fil ^^-§-^£(150 ppmH
- 6 6 -
SRL 5 L ^ J L 3 H | ! - °l-8-*MGEE13) ^ « Stripa
WIPP^ <y-<g*|<*H 2^91 ^ 1 - ^ : jL^-Sfll- depth-profiled
xr JL^M^} -fi-A]- ^ # ? M * M-H}vfl 4[l21]. <>H ^ ^ ^ 1 stripa
- WIPP^ A]^U). -^^^3: pineapple slice ^Bfl^ SRL S ^
^1«|- 345 m lAi 3 m 3 ° 1 ^ bore holei ^^-s | -^4 . SRL
1 pa *}*} S^l^ ^^r ^ # # - i
Boom clays] ^- f JlSj-^l^ ^#^-ol 3.7)1
^ ^ - ^ ^B^^] 4-i- ^ ^ - i " ^A}§V7l ^ § H TAV^^lS R7T7
90 M 1 } ^ ^
New Mexico
pH» ^ ^ 1 ^ 1 4 , ^ ^ " ^ 4 ^J-^-S^oilAlfe pH
5.
- 6 7 -
Table 13. SRL waste glass compositions buried in Stripa of Sweden
Component 131/29.8% TDS 165/29.8% TDS 131/35% TDS
Glass frit
SiO2Na2O
B2O3
TiO2
Li2OMgOZrO2
La2O3
40.612.410.30.74.01.40.40.4
47.79.17.0-
4.90.7.0.7-
37.611.69.60.73.71.30.30.3
Simulated waste
Fe2O3
MnO2
Zeolite
AI2O3
NiOSiO2
CaONa2OCoal
Na2SO4
Cs2CO3a
SrCO3a
U3O8a
Total
13.43.92.92.71.61.2
1.00.90.70.20.10.11.1
100.0
13.43.92.92.71.61.2
1.00.90.70.20.10.11.1
99.9
15.84.53.43.21.91.41.21.00.80.20.20.2
1.3
100.1
'TDS waste was doped with Cs, Sr and U.
68-
ICDCOI
3 -
2-
1 -
Stripa [131/TDS]
Stripa [131/3S%TDS]
131/TOS131/35%TDSStripa-165^"DS
x W1PP-16S/TDS
Strip* [155/TDS1G/ante
I'O 20
Time [mo.]
30
Figure 20. In-situ testing of SRS waste glass in granite (Stripa) and salt (WIPP).
Granitic simulation
B
600
500
400
300
200
100
0 0-0
o o o o o o o o o ?
20 40 60 80 100Weeks
• Monolithic
o Fractured
Bmg
600
500
400
300
200
100
0 (
(
Boom
0
o
3 10 20
Clay
o o
o
• • • •
30 40Weeks
O
•
50
• Monolithic
^ Fractured
Figure 21. Boron concentrations in solution in granite and claymedia.
-70-
Table 14. Interactions between the components of the waste package andthe waste form (borosilicate glass) in the nuclear wasterepository
Tuff repository rock
Stainless steel
Radiation
No effect on glass durability: sorption of certainradionuclides reduces their concentration.No effect in saturated tuff: possible effect inunsaturated system due to sensitized steel.In saturated system, buffers pH change caused byleaching: when moist air irradiated. HNO3 forms
_that_lowe_rs_pHL
No effect.No effect.Increases leaching of glass when O2 present:forms reducing atmosphere in closed systemwhich decreases solubility of certain radionuclides:forms corrosion products which sorb certainradionuclides.No effect on leaching brines but possible effect toincrease Eh of brine! radiation damage in saltreduces Na+ and oxidizes Of.Evidence suggests the products recombine orreact with brine at doses expected in repository.This lowers ^effect on brin_e_ leaching.
Basalt and graniteRepository rock Causes reducing conditions in closed system
which lowers solubility of redox sensitiveelements; some sorptive properties indicated; littleeffect on durability of glass.No effect.Same interactions as in salt; data exist whichsuggests that iron may not cause increasedleaching in reducing environments.In a closed system, radiolysis appears not toincrease the oxidizing potential of therock-groundwater system.
Salt repository rockStainless steelIron overpack
Radiation
Stainless steelIron overpack
Radiation
- 7 1 -
SRL 165<a-frel (basaltic glass)
5ti
paragoniteej-
Luo SRL 165 70
°C
EDSS.
^r paragonite*
^^4, paragonitefe-
. paragonite*
-¥-f}- 10 nm
fl Na, Mg,
smectite7>
Fe, Ti, Al ^^r^l
» 120-240
paragonite7}- Aq-, SRL 165
R7T7
MgCl27l-
, XRD
* 190
hydrotalcite
53t°l 4 ^ 7.68,
7.62 A OL
rhyolitic
tektites7>
- 7 2 -
Table 15. Typical compositions of natural analogue glasses in wt.%
SiO2
AI2O3
B2O3
Na2O
K2O
CaO
MgO
FeO
Fe2O3
T1O2
MnO
P2O5
Li2O
NiO
ZrO2
PbO
CuO
H2O
Basaltglass
50.7
11.7
-
4.5
0.7
10.6
6.7
-
13.1
1.9
0.4
-
-
-
-
-
-
0.1
Rhyoliticglass
74.9
14.2
-
4.68
4.59
0.53
0.02
0.49
0.29
0.04
0.03
-
-
-
-
-
-
0.3
Tektire
74.4
12.17
-
1.32
2.61
1.52
1.85
-
5.58
0.76
0.11
-
-
-
-
-
-
0.01
Egyptionbead
64.75
0.62
-
19.43
' 1.66
7.23
2.53
-
0.31
-
0.02
-
-
-
-
-
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iv.
T", KAERI/NEMAC/RR-167/96, 1996.
2. J. R. Moody, Nucl. Chem Waste Manage., 3, 29, 1982.
3. A. Barkatt et al., Nucl. Chem. Waste Manage., 2, 3, 1981.
^ ^ l e } - ^ , 82-85, 1993(4€).
5. w^ig^ <^ " JL^^W O I -A>^^71#S] tfl^|aii|-^ ^ " , KAERI/NEMAC
/AR-6/92, 1992.
6. J. C. Cunnane et al., Mat. Res. Soc. Symp. Proa, 294, p. 225, 1993.
7. J. A. C. Marples, W. Lutze, M. kawanishi, Mat. Res. Soc. Symp.
Proa, 176, 257-282, 1990.
8. P. A. Tempest, Nucl Tech, 52, 415-425, 1981.
9. W. D. Kingery, H. K. Bowen, D. R. Uhlmann, "Introduction to
ceramics", John Wiley and Sons, pp. 95-100, 1976.
10. J. E. Mendel, et al., "Thermal and radiation effects on borosilicate
waste glasses", IAEA-SM-207/100, IAEA, 2, 49-60, 1976.
11. M. A. H. Reimus, G. F. Piepel, G. B. Mellinger, " West Valley Glass
product qualification durability studies: Effects of composition, redox
state, heat treatment, and groundwater", PNL-SA-15579, 1988.
12. H. Mitamura, T. Banba, T. Murakami, Nucl. Chem. Waste Manage.,
6(3/4), 223-231, 1986.
13. C. M. Jantzen, D. F. Bickford, Mat. Res. Soc. Symp. Proa, 44,
135-146, 1985.
- 8 3 -
14. A. C. Buechele, X. Feng, H. Gu, I. L. Pegg, Mat. Res. Soc. Symp.
Proa, 176, 393-402, 1990.
15. A. C. Buechele et al., Mat. Res. Soc. Symp. Proc, 212, 141-152,
1991.
16. T. V. Palmiter, I. Joseph, L. D. Pye, Mat. Res. Soc. Symp. Proc,
212, 153-158, 1991.
17. C. M. Jantzen, D. F. Bickford, D. G. Karraker, Adv. Ceram., 8, 30-38,
1984.
18. V. J. Jain, S. M. Barnes, Ceram. Trans. 23, 251-257, 1991.
19. Y. I. Matyunin, A. V. Demin, M. I. Fedorova, Atomic Energy, 81(4),
706-709, 1996.
20. E. Vernaz, A. Loida, G. Malow, J. A. C. Marples, H. J. Matzke,
"Long-term stability of high-level waste forms", CEA-CONF-10429,
1990.
21. Kazuhiro Kawamura, Jin Ohuchi, "Characterization of highly waste
loaded glass for HLW", CONF-941075, 1995.
22. M. J. Plodinec, G. G. Wicks, Mat. Res. Soc. Symp. Proc., 333,
148-158, 1994.
23. G. F. Piepel, "A statistical approach for identifying nuclear waste
glass compositions that will meet quality and processability
requirements", PNL-SA18146, 1990.
24. R. D. Peters, C. C. Chapman, J. E. Mendel, C. G. Williams,
"Database for waste glass composition and properties",
CONF-930906-19, 1993.
25. A. A. Kruger, "Glass science tutorial: Lecture No. 7, Waste glass
-84-
technology for Hanford", Funding Organization: USDOE, Washington,
DC, p. 496, 1995.
26. W. G. Ramsey, G. G. Wicks, "WIPP/SRL in-situ tests: Compositional
correlations of MIIT waste glass", DP-MS-89-78, 1989,
27. J. L. Rasce, T. J. Overcamp, C. A. Cicero, "The effect of
compositional parameters on the TCLP and PCT durability of
environmental glasses.", CONF-9509266-1, 1995.
28. E. Y. Vernaz, J. L Dussossoy, "Current state of knowledge of nuclear
waste glass corrosion mechanisms: the case of R7T7 glass", Applied
Geochemistry (suppl. 1), 13-22, 1992.
29. J. E. Mandel, "Nuclear waste materials handbook - Waste form test
method", DOE/TIC-11400, 1981.
30. C. M. Jantzen, N. E. Bibler, " Product consistency test (PCT) for
DWPF glass: Part I. Test development and protocol", DPST-87-575,
1987.
31. B. Grambow, Mat. Res. Soc Symp. Proa, 44, 15-21, 1985.
32. Advocat T. " Les mecanismes de corrosion en phase aqueuse du
verre nucleaire R7T7. Approche experimentale: Essai de modelisation
thermodynamique and cinetique", PhD thesis, Universite Louis
Pasteur, Strasbourg, France, 1991.
33. S. Gin, Mat. Res. Soc. Symp. Proc, 412, 189-196, 1996.
34. J. C. Cunnane, J. M. Allison, Mat. Res. Soc. Symp. Proa, 333, 3-14,
1994.
35. R. D. Peters, S. C. Slate, PNL-3948, 1981.
36. W. B. White, "Corrosion of glass, ceramic and ceramic
- 8 5 -
superconductor", Noyes Publ., Park Ridge, New Jersey, 1992.
37. W. L. Ebert, J. K. bates, Nucl. TechnoL, 104, 372-84, 1993.
38. L. Tratingnon, J. C. Petit, G. Delia, J. C. Dvan, / . Nucl. Mater, 190,
228-246, 1992.
39. E. Y. Vernaz, Mat. Soc. Symp. Proc, 257, 37-48, 1992.
40. J. K. Bates, W. L. Ebert, T. J. Gerding, "Proc. of Int. High-Level
Radioactive Waste Management Conf.", Las Vegas, NV, April 8-12,
p. 1095, 1990.
41. William. L. Bourcier, Mat. Res. Soc. Symp. Proc., 333, 69-82, 1994.
42. Tsunetaka Banba, "Leaching model of nuclear waste glass", Journal-
of-Nuclear-Science-and-Technology-Tokyo-Japan, 23(12), 1075-1082,
1986.
43. B. Grambow, D. M. Strachan, Mat Res. Soc. Symp. Proc., 112,
713, 1987.
44. D. I. Parkhurst, "PHREEQE - A computer code for geochemical
calulations", USGS/wri-80-96, Government Printing Office, 1980.
45. "Radioactive waste management and disposal", ed. L. Cecille, Elsevier
Science Publishing Co., 302-315, 1991.
46. K. M. Olson, S. C. Marschman, G. F. Piepel, G. K. Whiting, "Product
consistency testing of West Valley compositional variation glass".,
PNL-10191, 1994.
47. ^Hfl^- S], "JL^$\ wo>A]-^^7]^. :&s1-&£ Qty' KAERI-NEMAC
/Ar-14/93, 1993.
48. D. E. Clark, R. L. Schulz, G. G. Wicks, A. R. Lodding, Mat Res.
Soc. Symp. Proa, 333, 107-122, 1994.
-86
49. J. K. Bates, et al., "Radioactive waste processing of high-level
radioactive wastes. Evaluation of factors anticipated to affect waste
glass reaction during repository disposal", ANL-95/20, 1995.
50. B. Grambow, Mat. Res. Soc. Symp. Proa, 333, 167-181, 1994.
51. K. B. Harvey, C. D. Litke, C.A. Larocque, Phys. Chem. Glasses,
33(2), 43-50, 1992.
52. "Radioactive waste management and disposal", ed. L. Cecille, Elsevier
Science Publishing Co., 275-286, 1991.
53. J. Caurel, E. Vermaz, D. Beaufort, Mat Res.,. Soc. Symp. Proc, 176,
309-317, 1990.
54. G. Ramsey, C. M. Jantzen, "Application of the hydration
thermodynamic model for glass durability under saturated tuff
repository conditions", WSRC-PR-90-26, 1990.
55. R. J. Lemire, F. Garisto, Radiochim Acta, 58/59, 37-44, 1992.
56. W. Lutze, B. Grambow, Radiochim Acta, 58/59, 3-7, 1992.
57. Jing C. Sang, et al., Mat. Res. Soc. Symp. Proc, 333, 519-524, 1994.
58. K. Ishiguro, et al., Nuclear Engineering and Design, 116, 61-70,
1989.
59. D. G. Coles, Nucl. Chem. Waste Manage., 2, 245, 1981.
60. G. G. Wicks, P. E. O'Rourke and P. G. Whitkop, "The chemical
durability of Savannar River Plant waste glass as a function of
groundwater pH", DP-MS-81-104, 1982.
61. B. Grambow, R. Muller, A. Rother, W. Lutze, Radiochim. Acta,
52/53, 501-506, 1991.
62. N. E. Bibler, C. M. Jantzen, Mat. Res. Soc. Symp. Proa, 84, 47-66,
87-
1987.
63. Y. Inagaki et al., Mat. Res. Soc. Symp. Proa, 456, 213-220, 1997.
64. K. G. Knauss, et al., Mat. Res. Soc. Symp. Proa, 176, 371-381, 1990.
65. J. Caurel, E. Vermaz, D. Beaufort, Mat. Res. Soc. Symp. Proa, 176,
309-317, 1990.
66. J. A. Stone, Nucl Chem Waste Manage., 2, 113-118, 1981.
67. C. Pescatore, A. J. Machiels, "Effects of water flow rates on
leaching, in geochemical behavior of disposed radioactive waste", G.
S. Barney, (ed.), Washington, DC (USA), American Chemical Society,
349-358, 1984.
68. X. Feng, et al., "Effects of S/V on secondary phase formation on
waste glasses", D. Bickford, S. Bates, V. Jain, G. Smith, (eds.),
CONF-940416, 235-254, 1994.
69. X. Feng, et al., Nuclear Technology, 104(2), 193-206, 1993.
70. N. Godon, E. Vernaz, J. P.-Mestre, "Testing the alteration of waste
glasses under geological storage conditions task 3 characterization of
radioactive waste forms a series of final reports(1985-89) No 18",
EUR-13606EN, 1991.
71. L. Wang, "Transuranium elements leaching from simulated HLW
glasses in synthetic interstitial claywater", INIS-mfl3759, 1992.
72. T. Banba, et al., "Effects of alpha decay on the properties of actual
nuclear waste glass", CONF-941075, 1397-1404, 1995.
73. N. E. Bibler, J. A. Kelley, "Effect of internal alpha radiation on
borosilicate glass containing Savannah River Plant Waste", DP-1482,
May 1978.
74. G. L. McVay et al., Nucl. Chem Waste Manage., 2, 103, 1981.
75. W. L. Ebert, J. K. Bates, T. A. Jr. Abrajano, T. J. Gerding, "The
influence of penetrating gamma radiation on the reaction of simulated
nuclear waste glass in tuff groundwater", CONF-890488-12, 1989.
76. Hiroshi Kamizono, et al., "Durability of high-level waste glass in
flowing groundwater under gamma-irradiation" CONF-941075, 1995.
77. C. L. Crawford, N. E. Bibler, "Effects of temperature and radiation on
the results of the nuclear waste glass product consistency leach
test", CONF-930438, 303- 312, 1994.
78. D. O. Russo et al., Mat. Res. Soc. Symp. Proa, 456, 205-212, 1997.
79. D. J. Wronkiewicz, Mat Res. Soc. Symp. Proa, 333, 83-98, 1994.
80. Lars Carlsen, Pia Lassen, Waste Management, 12, 1-6, 1992.
81. J. C. Dran et al., Radiochim. Acta, 58/59, 17-20, 1992.
82. S. Gin, N. Giodon, J. P. Mestre, E. Y. Vernaz, D. Beaufort, Mat. Res.
Soc. Symp. Proa, 333, 565-572, 1994.
83. J. Wei, P. Van Iseghem, Mat. Res. Soc. Symp. Proa, 456, 189-196,
1997.
84. X. Feng, "Surface layer effects on waste glass corrosion",
CONF-931108-19, 1993.
85. A. S. Barinov, M. I. Ojovan, N. V. Ojovan, Mat. Res. Soc. Symp.
Proc, 412, 265-270, 1996.
86. J. K. Bates, T. J. Gerding, A. B. Woodland, Mat. Res. Soc. Symp.
Proa, 176, 347-354, 1990.
87. John K. Bates, Edgar C. Buck, Mat. Res. Soc. Symp. Proa, 333,
41-54, 1994.
- 8 9 -
88. A. L. Kielpinski, "The long-term acceleration of waste glass
corrosion: A preliminary review", WSROTR-95-0306, 1995.
89. W. L. Gong, R. C. Ewing, L. M. Wang, E. Vernaz, J. K. Bates, W.
L. Ebert, Mat. Res. Soc. Symp. Proa, 412, 197-204, 1996.
90. E. C. Buck, "Analytical electron microscopy examination of solid
reaction products in long-term test of SRL 200 waste glasses",
ANL/CMT/CP—79802, 1993.
91. S. B. Xing, A. C. Buechele, I. L. Pegg, Mat. Res. Soc. Symp. Proa,
333, 541-548, 1994.
92. H. Asano, H. Wakamatsu, M. Akashi, "High level radioactive
waste management", Proceeding of the Third International
Conference, American Nuclear Society, Inc., 2, 1658-69, 1992.
93. Tsuyoshi Imakita, Kaoru Sasakawa, Fumio Matsuda, Ryutaro Wada,
Mat. Res. Soc. Symp. Proc, 333, 573-578, 1994.
94. 3 ^ , " i ^ W ^ l ? ] ! - *!£--£ 3RV S.£\ W ^ M J / S H I ^ ^
# -Aa! 'ST1" PhD thesis, Chungnam University Taejon, Korea, 1997.
95. Y. Inagaki, A. Ogata, H. Furuya, K. Idemitsu, T. Banba, T. Maeda,
Mat Res. Soc. Symp. Proc, 412, 257-264, 1996.
96. Susumu Muraoka, Muneaki Sexoo, Yoshii Kobayashi, "Progress
report on safety research on high-level waste management for the
period April 1989 to march 1990", JAERI-M-91-019, 1991.
97. Kaoru Sasakawa, Tsuyoshi Imakita, Ryutaro Wada, Fumio Matsuda,
Mat. Res. Soc. Symp. Proc., 333, 579-584, 1994.
98. N. E. Biblerl "Leaching fully radioactive SRP nuclear waste glass in
tuff groundwater in stainless steel vessel", DP-MS-85-141, 1986.
- 9 0 -
99. J. A. Covington, M. A. Molecke, G.G. Wicks, "WIPP/SRL in-situ
tests: MIIT program-The effects of metal package components",
WSRC-MS-91-074, 1991.
100. J. E. Mendel, "Final report of the defense high-level waste
leaching mechanisms program", PNL-5157 (DE84-016737), 1984.
101. H. U. Zwicky, T. H. Graber, R. Grauer, R. Restani, Mat. Res.
Soa Symp. Proa, 294, 134-144, 1993.
102. G. G. Wicks, B. M. Robnett, W. D. Rankin, "Scientific Basis for
Nuclear Waste Management, Vol. V", 15-24, North-Holland, New
York, 1982.
103. N. Goden, E. Y. Vernaz, "Enhancement of the glass corrosion in
the presence of clay minerals: Testing experimental results with an
integrated glass dissolution model", CONF-921131130, 1992.
104. N. Godon et. al., "Radioactive SON 68 18 17 L1C2A2Z1 glass
interaction with environmental materials. Investigation of irradiation
damage in glass specimens by thermoluminescence", EUR-13613,
1992.
105. K. Hara, K. Idemitsu, "Glass properties and source term models
relevant to disposal", IAEA-TECD0O582, 1991.
106. I. G. McKinley, "The near-field geochemistry of HLW disposal in
an argilleous host rock", NEGRA-NTB-88-26, 1989.
107. K. A. Boult, et al, " Radionuclide release from solidified high level
waste task 3 characterization of radioactive waste forms a series of
final report (1985-89) No 19", EUR-13604, 1991.
108. R. B. Heimann, "Effect of cement on radioactive waste-form
- 9 1 -
performance in multicomponent systems tests at 200 °C",
INIS-mf-12730, 1986.
109. C. G. Jr. Namboodri, G. G. Wicks, "SRL in-situ tests in the United
Kingdom: Part 2, Surface analyses of SRS waste glass buried for
one and two years in limestone at Ballidon, UK", WSRC-RP-91-288,
1991.
110. "High level radioactive waste management", Vol. 2, Proceeding of
the international topic meeting, Las Vegas, Nevada, April 8-12,
1103-1109, 1990.
111. J. K. Bates, et al., "Yucca Mountain Project - Argonne National
Laboratory annual progress report, FY 1994. Yucca mountain
prooject", ANL-94/42, 1995.
112. Fernando Bazen, J. H. Rego, R. D. Aines, "Leaching of actinide-
doped nuclear waste glass in a tuff-dominated system",
UCRL-94721, 1987.
113. P. Van lseghem, K. Berghman, K. Lemmens, W. Timmermans,
Wang Lian, "Laboratory and in-situ interaction between simulated
waste glasses and clay task 3 characterization of radioactive waste
forms a series of final reports (1985-89) No 21", EUR-13607, 1992.
114. A. Lodding, P. Van Iseghem, Mat. Res. Soc. Symp. Proa, 412,
229-238, 1996.
115. Pierre PH. Van Iseghem, Mat. Res. Soc. Symp. Proa, 333, 133-144,
1994.
116. P. Van-Iseghem, H. Yamamoto, "The integrated interaction between
high-level waste glass and the near field barriers", BLG638, 1992.
- 9 2 -
117. P. Van-Iseghem, K. Lemmens, M. Aertsens, M. Put, "Interaction
between HLW glass and clay: experiments versus model., Nuclear
Energy Agency, 75 - Paris (France). Validation through model
testing", 203-217, Organisation for Economic Co-Operation and
Development. Paris, France, 1995.
118. J. A. C. Marples, "The European Commissions Round Robin of their
repository system simulation test. A compilation and evaluation of
the results for the granite option", AERE-R-13660, 1989.
119. L. A. Mertens, W. Lutze, Mat. Res., Soc. Symp.. Proa, 176, 267-274,
1990.
120. J. A. C. Marples, W. Lutze, M. Kawanishi and P. van Iseghem, "A
comparison of the behavior of vitrified HLW in repogitories in salt,
clay and granite. II : Results", EUR-12544, 1990.
121. J. P. Williams, G. G. Wicks, D. E. Clark, A. R. Lodding, "Analyses
of SRS waste glass buried in granite in Sweden and salt in the
united states(U)", WSRC-MS-90-370, 1991.
122. E. Vernaz, A. Loida, G. Malow, J. A. C. Marples, H. J. Matzke,
"Long-term stability of high-level waste forms", CEA-CONF-10429,
1990.
123. N. E. Bibler, C. M. Jantzen, Mat Res. Soc. Symp. Proa, 84, 47-66,
1987.
124. James J. Mazer, Mat. Res. Soc. Symp. Proa, 333. 159-165, 1994.
125. J. L. crovisier, J. Honnorez, B. Fritz, J. C. Petit, Appl. Geochem.
Suppl. Issue, 1, 55, 1992.
126. J. S. Luo, W. L. Ebert, J. J. Mazer, J. K. Bates, Mat. Res. Soc.
- 9 3 -
Symp. Proa, 456, 157-163, 1997.
127. J. K. Bates et al., Nucl. Chem Waste Manage., 5, 63, 1984.
128. A. Abdelouas, J. L. Crovisier, W. Lutze, R. Muller, W. Bernotat,
Mat. Res. Soc. Symp. Proa, 333, 513-518, 1994.
129. H. D. Schreiber et al., Physics Chem. Glasses, 26(1), 24, 1985.
130. K. Miyahara, T. Ashida, N. Tsunoda, Y. Yusa, N. Sasaki, "Static
leaching actinides and fission products from fully radioactive waste
glass of HLLW generated in Tokai reprocessing plant", PNCT
N8410 89-009.
131. W. L. Ebert, J. K. Baqtes, E. C. Buck, M. Gong, S. F. Wolf,
"Disposition of actinides released from high-level waste glass",
CONF-940416, 231-241, 1994.
132. D. J. Wronkiewicz, "Effects of radionuclide decay on waste glass
behavior: A critical review", ANL-93/45, 1993.
133. J. A. Fortner et al., Mat. Res. Soc. Symp. Proc, 456, 165-172, 1997.
134. K. Miyahara, T. Ashida, N. Tsunoda, Y. Yusa, N. Sasaki, "Leaching
behavior of actinides and fission products from fully radioactive
waste glass of HLLW generated in Tokai reprocessing plant"., E.
Warnecke, R. Odoj, R. Simon (eds.). Requirements for waste
acceptance and quality control. Proceedings, 595-607, 1990.
- 9 4 -
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BIBLIOGRAPHIC INFORMATION SHEET
Performing Org.
Report No.Sponsoring Org.
Report No.Stamdard Report No. INIS Subject Code
KAERI/AR-483/98
Title/
Subtitle
Leach Behavior of High-Level Borosilicate Glasses under Deep Geological
Environment
Project Manager
and DepartmentChun, Kwan Sik ( Engineered Barrier Developement )
Researcher and
DepartmentKim, Seung Soo ; Park, Hyun Soo ( Engineered Barrier Developement)
Publication
PlaceTaejon Publisher KAERI
Publication
Date1998. 2.
Page 103 p. 111. & Tab. Yes( V ), No ( ) Size 26 Cm.
Note
Classified Open( V ), Restricted( ),
Class DocumentReport Type State-of-the-Art Report
Sponsoring Org. Contract No.
Abstract (15-20 Lines)
This report presents an overview of the activities in high-level radioactive waste
glass which is considered as the most practicable form of waste, and also is intended to
be use in the disposal of national high-level radioactive waste in future.
Leach theory of waste glass and the leach effects of ground water, metal barrier,
buffer materials and rocks on the waste glass were reviewed.
The leach of waste glass was affected by various factors such as composition, pH
and Eh of ground water, temperature, pressure, radiation and humic acid. The
crystallization, crack, weathering and the formation of altered phases of waste glass
which is expected to occur in real disposal site were reviewed. The results of leaching
in laboratory and in-situ were compared. The behaviors of radioactive elements leached
from waste glass and the use of basalt glass for the long-term natural analogue of waste
glass were also written hi this report.
The appraisal of durability of borosilicate waste glass as a waste media was
performed from the known results of leach test and international in-situ tests were
introduced.Subject Keywords(About 10 words)
leach, high-level, waste glass, borosilicate, geology,
