deuterium permeation induced transmutation experiments...
TRANSCRIPT
© 2014 MITSUBISHI HEAVY INDUSTRIES, LTD. All Rights Reserved.
Deuterium Permeation Induced
Transmutation Experiments using
Nano-Structured Pd/CaO/Pd Multilayer
Thin Film
Y.Iwamura, S.Tsuruga and T.Itoh
Advanced Technology Research Center,
Mitsubishi Heavy Industries, ltd., Japan
2014 CF/LANR(Cold Fusion/Lattice Assisted Nuclear Reactions) Colloquium at MIT,
March.21-23, 2014, Massachusetts Institute of Technology, Cambridge, MA, USA
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Contents
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1. Introduction
3. Preliminary Results on Consecutive
Transmutation Experiments
2. Results of Batch Process Experiments
4. Replication Experiments by Toyota Central
Research and Development Laboratories
2-1. Transmuted Products Analyzed by
ICP-MS, SIMS and XPS
2-2. Observation of g-ray peaks
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2
1. Introduction
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Features of Our Method
3
D2 gas permeation through nano-structured Pd complex
真空
重陽子透過
CaOCaO 2nm
D Flux
Vacuum
D2 gas
D Permeation
Cs,Ba, etc.
Pd nano-sized multilayer film
Pd 20nm
Surface
CaO 2nm
Pd 40nm
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Reactions observed in the case of Gas Permeation
SmBad
150
62
)3(6138
56
4
SmBad
149
62
)3(6137
56
Pr141
59
)2(4133
55
d
Cs
MoSrd
96
42
)2(488
38
1)Alkali metals; Electron Emitter
2)2d, 4d, 6d; capture reactions
TiCad
48
22
)(244
20
OsWd
188
76
)(2184
74
PtWd
190
78
)2(4182
74
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Progress in Permeation Experiments
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~2010
Gas
Permeation
;Basic
Research
2011~2012
Increase of Products
for Future Application
2013~Consecutive Processing
Batch Processing Addition of fixed
quantity of Cs
Consecutive Processing
Aiming
Consecutive
Transmutation
of Cs
Pump
Cs Solution
D
Reaction cell
Pd/CaO/Pd
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2. Results of Batch Process Experiments
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2-1. Transmuted Products Analyzed by
ICP-MS, SIMS and XPS
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Pr Dependence on D2 gas pressure
0
10
20
30
40
50
0 20 40 60 80 100
230kPa
赤:高圧
青:低圧
0
10
20
30
40
50
0 20 40 60 80 100
50℃低圧
50℃高圧
60℃低圧
60℃高圧
70℃低圧
70℃高圧
80℃低圧
80℃高圧
90℃低圧
90℃高圧
50℃低圧
50℃高圧
60℃低圧
60℃高圧
70℃低圧
70℃高圧
80℃低圧
80℃高圧
90℃低圧
90℃高圧
50℃ LP
50℃ HP
60℃ LP
60℃ HP
70℃ LP
70℃ HP
80℃ LP
80℃ HP
90℃ LP
90℃ HP
120~130kPa180~230 kPa
LP: 120~130kPaHP: 180~
230kPa
Red: High Pressure
Blue:
Low Pressure
Pr141
59
133
55 Cs
Conversion Rate(%)
Am
ou
nt
of
Pr
(ng/c
m2)
Pressure Pr
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Gas vs. Electrochemical Permeation
8
Gas Permeation Electrochemical Permeation
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9
Experimental Apparatus aiming Increase of D Density
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SIMS Analysis; E006 Wide Spectra
Mass Number
E-006 center
E-006 corner
No Implantation
No Implantation: Corner
100 120 140 160 180 20010
2
103
104
105
106
SIM
S C
ou
nts
Increase around mass140
Decrease of 133Cs
Pd multilayer film
Center
Corner
D permeated
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11
SIMS Analysis; E006
139La?
140Ce?
141Pr
142Ce?
130 135 140 145 150
20000
40000
60000
80000
100000 E-006 center
E-006 corner
No Implantation
No Implantation: Corner
SIM
S C
ounts
Mass Number
Pd multilayer film
Center
Corner
D permeated
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ICP-MS Analysis; E006
SIMS (point) and ICP-MS (all surface) gave similar results
130 135 140 145 150
2000
4000
6000
8000
10000
Cs Implantation; E006
No Implantation
Co
un
ts
Mass Number
139La?
140Ce?141Pr
142Ce?
Different Tendency from D2 gas permeation © 2014 MITSUBISHI HEAVY INDUSTRIES, LTD. All Rights Reserved.
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Confirmation of the products by XPS
13
930 940 950 960
18400
18800
19200
19600
20000 E6 permeated
Counts
(E6)
Energy(eV)
Pr 3d5/2
Pr 3d3/2
CuF2 2p3/2
CuF2 2p1/2Pr confirmed by XPS
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2-2. Observation of g-ray peaks
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Introduce a Gamma-ray Detector
Ge Detector for g-
ray measurement
Reactor Cell
Pb Shield
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16
Example of Gamma-Ray Detection; E16
Cs ion implanted
1×1016/cm2 20kV
D Permeation
rate is
proportional to
this pressure
0 2 4 6 8 10 12
3
4
5
Ap
pli
ed
Vo
ltag
e(V
)
Period 1 Period 2 Period 3 Background
10days
Pd/Y2O3/Pd multilayer film
0.5MCsNO3-D2O Solution
Cs
Y2O3
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17
Gamma-ray Measurement (period 1 )
Live time = 233,425sec
Gam
ma-
ray C
ount
Rat
e (c
ps)
Energy (keV)
~609.5keV
-0.005
0.000
0.005
0.010
600 610 620 630 640 650
E16 period1
s
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Gamma-ray Measurement (period 2 )
Live time=574,586sec
Gam
ma-
ray
Count
Rat
e (c
ps)
Energy (keV)
E16 period2
~511.5keV;
Annihilation peak?
500 520 540 560 580
-0.004
-0.002
0.000
0.002
0.004
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Gamma-ray Measurement (period 3 )
Live time=71,826sec
500 520 540 560 580-0.004
-0.002
0.00
0
0.002
0.004
Gam
ma-
ray
Count
Rat
e (c
ps)
Energy (keV)
~511.5keV;
Annihilation peak?
E16 period3
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E16 Gamma-ray Measurement Summary
Time Gamma-ray
Period 1 609.5keV gamma-ray detected
No 511keV detected
Period 2 511.5keV gamma-ray detected
No 609.5keV detected
Period 3 511.5keV gamma-ray detected
No 609.5keV detected
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Pr detected by XPS from the center of E16 sample
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930 940 950 96026000
27000
28000
29000
30000
31000
32000
33000
Energy(eV)
Counts
(E16)
E16 permeated
35000
36000
37000
38000
39000
40000
41000
Counts(N
o p
ermeatio
n)
No permeation
Pr 3d5/2Pr 3d3/2
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© 2012 MITSUBISHI HEAVY INDUSTRIES, LTD. All Rights Reserved. 22
E28
Pd/CaO/Pd multilayer film
0.1MCsNO3-D2O Solution
Period 1 BackgroundPeriod 2 21days
CaO
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1445keV
E28 ;1200-1600keV
1200 1250 1300 1350 1400 1450 1500 1550 1600
1E-3
0.01
0.1
E28
E28A
BFB15
Y A
xis
Tit
le
X Axis TitleEnergy(keV)
Em
issio
n R
ate
(cp
s)
Period 1
Period 2
Background
Clear g–ray peak
at 1445keV40K peak
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1745keV
E28 ;1700-1850keV
1700 1750 1800 1850 1900
1E-4
1E-3
0.01
0.1
E28
E28A
BFB15
Y A
xis
Tit
le
X Axis TitleEnergy(keV)
Em
issio
n R
ate
(cp
s)
Period 1
Period 2
Background
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Discussion on emitted g-ray during E28 period1
Unstable nuclei that emit g-ray ranging from 1444.5 to 1445.5keV
Energy(keV) cps
1445 3.50E-03
1109 1.00E-03
1745 3.00E-04
507.4 5.00E-04
578.9 1.00E-04
605 5.00E-04
Detected g-ray energy
We have not succeed to find a nucleus fit for the observed g-ray energies.
・g-rays from unstable nuclei
・g-rays from excited nuclei
・Thermal neutron capture g-rays
Observed g-rays seems to be attributed to minor short lived nuclei.
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3. Preliminary Results on Consecutive
Transmutation Experiments
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Batch vs. Consecutive Processing
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Batch Consecutive
Pump
Cs Solution
D
Reaction cell
Pd/CaO/Pd
Addition of fixed quantity of Cs Circulation of Electrolyte
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Cooling Pd Surface by Circulation of Electrolyte
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Temperature(C)
Deu
teriu
m D
ensi
ty [
D/P
d]
T D/Pd
Cooling is important!
Circulation of Electrolyte
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Experimental Setups for Consecutive Transmutation
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Pump
Reservoir
Reaction Cell
N2 Flow meter
Evacuation
Electrolyte
N2 for Purge
Pd/CaO/Pd
(Cathode)
Pt
(Anode)
All Contact Surfaces with Electrolyte are made of Teflon to Avoid Contamination.
0.1M CsNO3
200mL
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Reaction rates; Batch vs. Consecutive Processing
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0 0.05 0.10 0.15 0.20 0.25
Current Density(mA/cm2)
Rea
ctio
n R
ate
[μg
/cm
2/w
eek
]
10
1
0.1
0.01
Batch Processing
Consecutive processing
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Products; Batch vs. Consecutive Processing
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Pd/CaO/Pd Thin Film 0.1M CsNO3 Solution
BatchConsecutive
BatchConsecutive
La
CePr
La
[g/cm2] [g/solution]
Ce Pr
0
2.0E-7
1.0E-7
1.5E-7
5.0E-8
0.0E+0
2.0E-7
1.0E-7
1.5E-7
5.0E-8
0.0E+0
Batch : Products
Consecutive : Products
On the Pd Thin Film
In Solution
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4. Replication Experiments by Toyota
Central Research and Development
Laboratories, Inc.
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Toyota Paper
T.Hioki et.al, Jpn. J. Appl. Phys. 52(2013) 107301
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Experimental Setup
T. Hioki et.al, Jpn. J. Appl. Phys. 52(2013) 107301
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Results
T. Hioki et.al, Jpn. J. Appl. Phys. 52(2013) 107301
Pr
2.5X1012/cm2
Cs/Pd/CaO/
Pd with D
permeation
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Concluding Remarks
Deuterium Permeation Induced Transmutation Reaction
have been observed in the Pd complexes, which are
composed of Pd and CaO thin film and Pd substrate.
1.
2. Electrochemical permeation aiming the increase the local
deuteron density near the surface of Pd made increase
transmuted products.
Statistically significant g-rays which have clear energy
spectra were detected. At present, we have limited examples.
Further study is necessary.
3.
Preliminary consecutive transmutation experiments gave us
higher reaction rates than batch processing up to now.
Much products were recovered in the solution.
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4.
Toyota R&D Lab successfully reproduced permeation
induced transmutation of Cs into Pr. 5.