Deuterium Permeation Induced Transmutation Experiments using Nano-Structured Pd/CaO/Pd Multilayer Thin Film

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1 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

2 Contents 1. Introduction 2. Results of Batch Process Experiments 2-1. Transmuted Products Analyzed by ICP-MS, SIMS and XPS 2-2. Observation of g-ray peaks 3. Preliminary Results on Consecutive Transmutation Experiments 4. Replication Experiments by Toyota Central Research and Development Laboratories 1

3 1. Introduction 2

4 Features of Our Method D 2 gas permeation through nano-structured Pd complex Cs,Ba, etc. D 2 gas D Permeation Pd nano-sized multilayer film Surface 真空重陽子透過 D Flux Vacuum Pd 40nm CaO 2nm CaO 2nm Pd 20nm 3

Reactions observed in the case of Gas Permeation 1)Alkali metals; Electron Emitter 2)2d, 4d, 6d; capture reactions 133 55 88 38 138 56 137 56 44 20 184 74

5 Reactions observed in the case of Gas Permeation 1)Alkali metals; Electron Emitter 2)2d, 4d, 6d; capture reactions d Cs Ba d 150 Sm 6 (2 ) (2 ) 42 6 (3 ) (3 ) 62 Ba d 149 Sm 62 Pr Sr d 96 Mo 2 ( ) Ca d 48 Ti 2 ( ) 22 W d 188 Os 4 76 (2 ) W d 190 Pt 78 4

Processing Batch Processing Addition of fixed quantity of Cs Consecutive

6 Progress in Permeation Experiments ~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 Reaction cell Pd/CaO/Pd Cs Solution D Aiming Consecutive Transmutation of Cs Pump 5

7 2. Results of Batch Process Experiments 2-1. Transmuted Products Analyzed by ICP-MS, SIMS and XPS 6

8 Pr Dependence on D2 gas pressure Cs Pr Amount of Pr (ng/cm2) LP ５０低圧 50 HP ５０高圧 60 LP ６０低圧 60 HP 60 高圧 70 LP 70 低圧 70 HP 70 高圧 80 LP 80 低圧 80 HP 80 高圧 90 LP 90 低圧 90 HP 90 高圧 Red: High Pressure 赤高圧 40 Blue: Low Pressure 青低圧 kPa LP kPa HP kpa Conversion Rate(%) Pressure Pr 7

9 Gas vs. Electrochemical Permeation Gas Permeation Electrochemical Permeation 8

10 Experimental Apparatus aiming Increase of D Density 9

11 SIMS Counts SIMS Analysis; E006 Wide Spectra Decrease of 133 Cs 10 6 D permeated Center Corner Pd multilayer film E-006 center E-006 corner No Implantation No Implantation: Corner 10 5 Increase around mass Mass Number 10

12 SIMS Counts SIMS Analysis; E E-006 center 140 Ce? E-006 corner No Implantation No Implantation: Corner La? 141 Pr Center Corner D permeated Ce? Pd multilayer film Mass Number 11

ICP-MS Analysis; E006 10000 8000 Cs Implantation; E006 No Implantation Counts 6000 4000 139 La? 140 Ce? 2000 141 Pr 142 Ce?

13 ICP-MS Analysis; E Cs Implantation; E006 No Implantation Counts La? 140 Ce? Pr 142 Ce? Mass Number SIMS (point) and ICP-MS (all surface) gave similar results Different Tendency from D 2 gas permeation 12

14 Confirmation of the products by XPS Pr 3d5/2 E6 permeated Pr 3d3/2 Counts(E6) CuF 2 2p3/ Pr confirmed by XPS CuF 2 2p1/ Energy(eV) 13

15 2-2. Observation of g-ray peaks 14

16 Introduce a Gamma-ray Detector Ge Detector for g- ray measurement Pb Shield Reactor Cell 15

17 Applied Voltage(V) Example of Gamma-Ray Detection; E16 Pd/Y 2 O 3 /Pd multilayer film Cs ion implanted /cm 2 20kV D Permeation rate is proportional to this pressure Y 2 O 3 Cs Period 1 Period 2 Period 3 Background 10days MCsNO 3 -D 2 O Solution 16

18 Gamma-ray Measurement (period 1 ) Gamma-ray Count Rate (cps) ~609.5keV E16 period s Energy (kev) Live time = 233,425sec

19 Gamma-ray Measurement (period 2 ) Gamma-ray Count Rate (cps) ~511.5keV; Annihilation peak? E16 period Live time=574,586sec Energy (kev) 18

20 Gamma-ray Count Rate (cps) Gamma-ray Measurement (period 3 ) ~511.5keV; Annihilation peak? E16 period Live time=71,826sec Energy (kev) 19

21 E16 Gamma-ray Measurement Summary Time Gamma-ray Period keV gamma-ray detected No 511keV detected Period keV gamma-ray detected No 609.5keV detected Period keV gamma-ray detected No 609.5keV detected 20

Pr detected by XPS from the center of E16 sample Counts(No permeation) Counts(E16) 33000 32000 31000 30000 29000 28000 27000 26000 E16 permeated No

24 E28 ; keV 0.1 Emission Rate(cps) Period 1 E28 E28A BFB15 Period 2 Background Y Axis Title 0.01 Clear g ray peak at 1445keV 1445keV 40 K peak 1E Energy(keV) X Axis Title

25 E28 ; keV 0.1 Emission Rate(cps) Period 1 E28 E28A BFB15 Period 2 Background Y Axis Title E keV 1E Energy(keV) X Axis Title

Discussion on emitted g-ray during E28 period1 Detected g-ray energy Energy(keV) cps 1445 3.50E-03 1109 1.

00E-04 We have not succeed to find a nucleus fit for the observed g- ray energies.

26 Discussion on emitted g-ray during E28 period1 Detected g-ray energy Energy(keV) cps E E E E E E-04 We have not succeed to find a nucleus fit for the observed g- ray energies. Unstable nuclei that emit g-ray ranging from to keV 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.

27 3. Preliminary Results on Consecutive Transmutation Experiments 26

28 Batch vs. Consecutive Processing Batch Consecutive Reaction cell Pd/CaO/Pd Cs Solution D Pump Addition of fixed quantity of Cs Circulation of Electrolyte 27

29 Cooling Pd Surface by Circulation of Electrolyte Deuterium Density [D/Pd] T D/Pd Cooling is important! Circulation of Electrolyte Temperature(C) 28

30 Experimental Setups for Consecutive Transmutation All Contact Surfaces with Electrolyte are made of Teflon to Avoid Contamination. Pump Reaction Cell N 2 for Purge Pt (Anode) Pd/CaO/Pd (Cathode) Electrolyte 0.1M CsNO 3 200mL Reservoir Evacuation N 2 Flow meter 29

31 Reaction rates; Batch vs. Consecutive Processing Reaction Rate [μg/cm 2 /week] 10 Consecutive processing Batch Processing Current Density(mA/cm 2 ) 30

32 Products; Batch vs. Consecutive Processing Pd/CaO/Pd Thin Film 0.1M CsNO 3 Solution [g/cm 2 ] [g/solution] 2.0E-7 2.0E-7 1.5E-7 1.5E-7 Ce Pr 1.0E-7 1.0E-7 La 5.0E-8 0.0E+0 0 La Batch Ce Pr Consecutive 5.0E-8 0.0E+0 Batch Consecutive Batch : Products On the Pd Thin Film Consecutive : Products In Solution 31

33 4. Replication Experiments by Toyota Central Research and Development Laboratories, Inc. 32

34 Toyota Paper T.Hioki et.al, Jpn. J. Appl. Phys. 52(2013)

35 Experimental Setup T. Hioki et.al, Jpn. J. Appl. Phys. 52(2013)

36 Results 2.5X10 12 /cm 2 Pr Cs/Pd/CaO/ Pd with D permeation T. Hioki et.al, Jpn. J. Appl. Phys. 52(2013)

37 Concluding Remarks 1. Deuterium Permeation Induced Transmutation Reaction have been observed in the Pd complexes, which are composed of Pd and CaO thin film and Pd substrate. 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. Preliminary consecutive transmutation experiments gave us higher reaction rates than batch processing up to now. Much products were recovered in the solution. Toyota R&D Lab successfully reproduced permeation induced transmutation of Cs into Pr. 36

38 37

Transmutation Reaction Induced by Deuterium Permeation Through Nanostructured Multi-layer Thin Film

106 Transmutation Reaction Induced by Deuterium Permeation Through Nanostructured Multi-layer Thin Film SHIGENORI TSURUGA *1 KENJI MUTA *1 YUTAKA TANAKA *2 TADASHI SHIMAZU *3 KOJI FUJIMORI *4 TAKEHIKO