Radiation effects of ions and gamma rays in sodium borosilicate glasses Haibo Peng 20190926 School of Nuclear science and technology Lanzhou University Out line Background Difference in alpha beta and gamma decays ID: 935462
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Slide1
Joint ICTP-IAEA International School on Nuclear Waste Vitrification
Radiation effects of ions and gamma rays in sodium borosilicate glasses
Haibo Peng
2019.09.26
School of Nuclear science and technology, Lanzhou University
Slide2Out line
BackgroundDifference in alpha, beta and gamma decaysRadiation effects in sodium borosilicate glasses with impact of ions
Radiation effects in fused silica with impact of ionsRadiation effects
in sodium borosilicate glasses with irradiation of gamma rays
Conclusions
Acknowlagements
2
Slide3Background
3
Fuel-burning power plant
Qinshan
nuclear power plant
Spent nuclear fuel
Middle level radioactive waste
High level radioactive waste
Deep geological disposal for 10,000 years
Slide4Background
Which materials can be solidified the HLW?What radiation effects will happen in vitrification which is in condition of long time radiation.
How to keep HLW isolating from the biosphere?How to
evaluate safety
of vitrification?
Radiation effects in vitrificationRadiation effects in borosilicate glass
4
Slide5Cumulative Decays with time in vitrification
5
Weber, W.J.,
Radiation effect in nuclear waste glasses.
Nucl. Instr. and Meth. B, 1988.
32
: p. 471-479.
Slide6Dose evolution with storage time
6
Weber, Journal of material research, 1997.
12
: p. 1948-1978.
Abosorbed dose: Gy deposited energy J/kg
Radiation dose : dpa displacement per atom
Slide7Characteristics in α, β and γ
decays7
Parent nucleus
Alpha
Daughter nucleus
High energy
about 5MeV
Long range in glass
about 20 micro meter
Less displacement in materials
Helium bubble
Low energy
about 100 keV
Short Range
about 20 nm
More displacement in materials
A serial daughter nuclei
Slide8Characteristics in α, β and γ
decays8
Parent nucleus
Alpha
Daughter nucleus
beta
neutrino
Low energy
from keV to MeV
Long range
from micro meter to mm
Much less displacement in materials
Carries energy
No influence on materials
gamma
Low energy
from
keV
to MeV
Long range
less displacement in materials
Produce electron as well
Along with alpha and beta decays
Slide9Interaction of gamma with materials
9
photon
h
nucleus
photoelectron
Compton effect
Photoelectric effect
Electron-positron pair production
After interactions
of materials with gamma rays, the
electron and nucleus are
collided by gamma rays and p
roductions are gamma rays and electrons
Slide10Interaction of beta with materials
Ionization energy lossRadiation energy lossBremsstrahlung
Productions of interaction of betawith materials are lower energy electrons and photons.
10
Slide11Interaction of ions with target atoms
11
ion
Target nucleus
electron
Alpha
Recoiled nucleus
Slide12Radiation effects by alpha decay
Alpha particle and recoiled ionhigh energy low energyElectrons and nuclei
nuclei helium bubble
no
low displacement high displacement
340
2000
12
Slide13Part I: Radiation effects in borosilicate glasses with impact of ions
13
Slide14Simulation of alpha and gamma decays
How to simulate radiation effects in glass by alpha decay? Radiation effects in glass by irradiation of ionsHow to simulate radiation effects in glass by gamma/beta decay? Radiation effects in glass by irradiation of electron/gamma
TEM? Electron beam? Gamma ?
14
Peuget
, S.
, et al.
(2006).
Nucl
. Instr. and Meth. B
246
(2): 379-386
Wang, T.-S.
, et al.
(2019). Journal of Inorganic Materials
34(7): 741
Slide15Compositions of borosilicate glasses
15
Mol%
NBS1
NBS2
NBS4
NBS5
NBS6
NBS7
NBS8
SiO2
Mol%
ISG
Na
2
O
25
16
20
14.14
15.33
16.67
17.86
0
Na
2
O
12.60
SiO
2
60.04
67.26
64
67.26
64.51
61.4
58.67
100
SiO
2
60.20
B
2
O
3
14.96
16.74
16
18.6
20.16
21.93
23.47
0
B
2
O
3
16.00
Al2O3
3.80
R=Na
2
O/B
2
O
3
1.671
0.956
1.250
0.760
0.760
0.760
0.761
*
CaO
5.70
K=SiO
2
/B
2
O
3
4.013
4.018
4.000
3.616
3.200
2.800
2.500
*
ZrO2
1.70
Density
(g/cm
3
)
2.46
2.497
2.441
2.460
2.454
2.488
2.36
2.501
Slide16Irradiation methods and damaged region distributions
Ions Single-energy ions Multi-energy ionsGamma rays
60Co 1.33,1.17 MeV
16
Ions
Energy
(MeV)
Range
(
μ
m
)
Sample
Kr
4
2.4
NBS1
NBS2
Xe
5
2.0
NBS1
NBS2
SiO
2
-1
Xe
Multi
energy
1.6
0.6
NBS1
3.2
1.3
NBS2
5
2.0
SiO
2
-1
P
0.3
0.4
NBS1
NBS2
SiO
2
-1
Ne
Multi
energy
0.125
0.3
NBS1
0.3
0.7
NBS2
0.6
1.1
Au
7
2.0
NBS1
NBS2
Different Irradiation methods on glass with ions
Damage distribution in glass by impact of single and multi-energy ions
Irradiation of ions
Irradiation of gamma rays
Thickness of damaged region ~micrometers
Thickness
of
damaged region
~
milimeters
Slide17Formation of oxygen in glass by irradiation of ions
17
Oxygen in borosilicate glass irradiated with
Ar
ions
No bubbles in glass were observed.
Oxygen in borosilicate glass irradiated with electron
Boizot
, B.
, et al.
(1999). Journal of Non-Crystalline Solids
243
: 268-272
Chen, L.
, et al.
(2013). Chinese Physics B
22
(12): 126101Zhang, G. F.
, et al. (2013). Nucl. Instr. and Meth. B 316: 218-221
Mir, A. H., et al. (2017). Journal of Nuclear Materials 489: 91-98
Slide18phase separation GIXRD Elementary distributions
TOF-SIMSRadiation effects on borosilicate glass by impact of ion
18
GIXRD spectra
from borosilicate glass pristine and irradiated with heavy ions.
With
irrdadiation
of multi-energy
Xe
ions, elemental distributions of borosilicate glass were uniformed.
Haibo Peng et al.
Radiation effects on borosilicate glass irradiated with ions
, SCIENTIA SINICA
Physica
,
Mechanica
&
Astronomica
, (2018)
Slide19H
is hardness
P
is the maximum force on indenter,
A
is projected area of impression
E
r
is reduced modulus
E
is Young’s modulus
v
is
Poisson’s ratio
Hardness and modulus of borosilicate glass
19
Hardness and modulus of borosilicate glass irradiated with ions.
W. C. Oliver and G. M. Pharr. Journal of Materials Research, 1992. 7: 1564-1583.
Slide20Comparisons of irradiation of different ions
20
v
sat
/ %
△
v
sat
/ %
t/
dpa
△
t/dpa
Hardness
-35.4
1.1
0.0064
7×10
-4
modulus
-18.7
0.6
0.015
0.0018
Hardness and moduli of borosilicate glass with irradiation of ions changed with dose
For irradiation of single energy ions,
irrespective the species of ions
, hardness and modulus dropped with dose.
Nuclear stopping power
played important role in decrease of hardness and modulus.
v
is variation of hardness and modulus
v
sat
is saturated variation
D
is radiation dose
t
is fitting parameter
Karakurt
G,
Abdelouas
A,
Guin
J P, et al.
J
Nucl
Mater, 2016, 475
：
243-254
Haibo Peng et al.
SCIENTIA SINICA
Physica
,
Mechanica
&
Astronomica
, (2018)
Slide21Comparisons of irradiation single and multi energy ion
21
Hardness V.S. Dose for irradiation of single energy ion
Hardness V.S. Dose for irradiation of multi-energy ion
Modulus V.S. Dose for irradiation of single energy ion
Modulus V.S. Dose for irradiation of multi-energy ion
Irradiation
Measurement
V
sat.
/%
ΔV
sat
/%
t/
dpa
Δt/dpa
Xe
and Kr / Single energy
Hardness
-35.4
1.1
0.0064
7×10
-4
Modulus
-18.7
0.6
0.015
0.0018
Xe
and Ne / Multi energy
Hardness
-34.3
1.2
0.013
0.002
Modulus
-18.2
1.6
0.031
0.008
35
18
Slide22Comparisons of irradiation single and multi energy ion
22
Hardness and modulus V.S. Dose for irradiation of single and multi-energy ion
Modulus V.S. Dose for irradiation of multi energy ion
Irradiation
Measurement
V
sat
.
/%
ΔV
sat
/%
t/
dpa
Δt/dpa
Xe
and Kr / Single energy
Hardness
-35.4
1.1
0.0064
7×10
-4
Modulus
-18.7
0.6
0.015
0.0018
Xe
and Ne / Multi energy
Hardness
-34.3
1.2
0.013
0.002
Modulus
-18.2
1.6
0.031
0.008
There were
no difference
in trends of hardness and modulus on dose for
irradiation of single energy ions and multi energy ion
, except for
calculated irradiation dose
.
35
18
Parameters of fitting lines of trend of hardness and modulus on irradiation dose
Slide23Radiation effects on SiO2 and borosilicate glass
23
Different trends of
Hardness
and modulus
with irradiation
doses for borosilicate glass and SiO
2
Could the
variations of Hardness and modulus in borosilicate glass with irradiation
be attributed to change in
network of silica
?
Haibo
Peng
,
Acta
Physica
Sinica
,
2018. 67(3): 038101
.
Guan, M, Journal of Non-Crystalline Solids, 2019.
518
: p. 118-122.
Hardness V.S. dose
Modulus V.S. dose
Hardness V.S. modulus
Slide24MD simulation of changes in structure of glass
24
Simulation of hardness measurement process
Hardness V.S. dose
Change in boron and silicon coordination with dose
Change in boron relative structure with dose
Broken network by impact of ions
Yuan, W.
, et al.
(2017). The Journal of Chemical Physics
147
(23): 234502
After irradiation of ion, change in hardness of glasses might due to breakage of Si-O-B bond.
Slide25Infrared and Raman spectra of NBS2 glass
25
Formation of BO
3
E. I.
Kamitsos
, et al. J. Phys. Chem. , 1986. 91: 1073-1079.
C.
Gautam
, et al. ISRN Ceramics, 2012. 2012: 1-17.
S. Music, et al. Journal of material science, 1992. 27
: 5269-5275
.
Boron Oxygen
here
I
f
is fluorescence intensity of Raman spectral background,
a
,
b
and
c
are fitting parameters,
ν
R
is
Raman
shift with the unit of cm
-1
Infrared
spectra of NBS2 glass with different doses
Raman
spectra of NBS2 glass with different doses
(a): The hardness and parameter
c
evolved with irradiation of dose. (b):The relation of harness of glass and the parameter of
c
.
P
eak
intensity from infrared spectra
V.S. the
hardness of glass
With irradiation, the
fluorescence on Raman
spectra was function
of Hardness .
Will the disorder in glass have strong influence on fingerprint peaks on Raman spectra?
L. Chen, et al.
Nucl
. Instr. and Meth. B, 2016. 370: 42-48.
L. Chen, et al. Journal of Non-Crystalline Solids, 2016. 448: 6-10.
Si-O-Si
Na
2
O
•
B
2
O
3
•2SiO
2
Q
n
(n=1,2,3,4)
Slide26Volume changes
26
edge
SiO
2
NBS2
Topography of SiO
2
irradiated with
Xe
ions
Topography of NBS2 irradiated with
Xe
ions
The volume changes of glasses irradiated with
Xe
ions
Slide27Volume change in different glasses
27
ISG glass
Volume change in glasses with impact of Heavy ions
Volume change in
vitrifications
doped with HLW
With the accumulation of alpha decays, volume change would be saturated, the saturated values might depend on compositions of glasses.
Weber et al.,
Procedia
Materials Science 7 ( 2014 ) 237 – 246
Slide28Radiation effects in glasses irradiated with ions
For irradiation of ionsTrends of hardness and modulus in borosilicate glass are
similar for irradiation of single and multi energy ions
.
Borosilicate glass
phase separation No
Elementary distributions
No
Hardness and modulus
36% and 18%
structure changes
Boron related Infrared spectra Raman spectra
Volume change IncreaseFormation of oxygen YesFused silicaHardness and modulus Different trendsVolume change
Decrease
28
Slide29Part II: Radiation effects on borosilicate glasses with irradiation of gamma rays
29
Slide30Radiation effects on borosilicate glasses
30
Absorption spectra of NBS1 glasses with different absorbed doses.
Absorption spectra of NBS1 glasses with different absorbed doses.
name
Structure
Energy /
eV
FWHM/
eV
NBOHC
≡
Si-O·
2
4.8
0.18
1.07
POR
≡
Si-O-O·
1.97
5.4
0.17
1.3
POL
≡
Si-O-O-Si
≡
3.8
0.7
E'
≡
Si·
6.2
0.28
Slide31Radiation effects in glasses irradiated with gamma
For borosilicate glass and fused silica with irradiation of gamma
Color center are formed Increased in borosilicate glass
Band gap
Dropped
in borosilicate glass
Urbach
energy
Increased
with absorbed dose
Hardness and modulus
No variation in both glassesDefect density Unknown
31Possible reasons for these effects:
1:Comparing with defects density induced by impact of ions,defect density induced by gamma irradiation was too less.
2:Defects in glass by gamma irradiation, did not come from the network of glass but from the end of network of glass.
Slide32Conclusions
Changes in glasses with impact of ion were confirmed.The possible reason was breakage of boron network
induced by ions.Point defects in sodium borosilicate glasses, which were irradiated with
gamma,
were idenified, so did
changes in band gap and Urbach energy.
No obvious influence on the hardness and modulus of glass were observed.
32
Slide33Acknowlagements
33
Slide34Thank you for your attention.
34