㕙࠻࠴࠙ࡓỚᐲಽᏓ
3.5 ᑄ᫈ၮḰߣߩᲧセ
ᣣᧄࠕࠗ࠰࠻ࡊදળߩᑄ᫈ၮḰߢߪޔ࿁ኈེ1ᧄ㧔 50 l 㧕ߚࠅޔ✚㊂ߢ400 MBqߣߥ ߞߡࠆ[5]ޕ࿁ߩ࿁ᠲ߮ടᾲឃ᳇ߦࠃࠆ㒰ᨴߢߪ457 kBq/g߹ߢ㒰ᨴߔࠆߎߣ߇ߢ߈ߚ ߎߣ߆ࠄ㧘࿁⊒↢ߒߚ࠲ࡦ࠲࡞✢ߩᑄ᫈‛ߩ✚㊂㧘1.2335 g ߢߪ564 kBq ߣߥࠅ㧘࿁ኈེߦ ᑄ᫈น⢻ߦߥߞߚߣ⸒߃ࠆޕ
৻ᣇ㧘ࠗࠡࠬߦ߅ߌࠆૐࡌ࡞ᕈᑄ᫈‛㧔β ᩭ⒳㧕ߩၮḰߣᲧセߒߡߺࠆߣ[6]㧘ߘߩၮ Ḱ㧔Low Level Waste : LLW㧕ߪ12 MBq/kgߢࠆޕ࿁ߩ943 Kߢ3.5ᤨ㑆ᜬߣ߁᧦ઙߢߩ㒰
ᨴߢߪޔ457 MBq/kg߹ߢ㒰ᨴߢ߈ߚ߇㧘ߎߩၮḰࠍḩߚߔߦߪᦝߦ1/40⒟ᐲ㒰ߔࠆᔅⷐ߇ࠆޕ
හߜ㧘ᦝߦ㜞᷷㧘㐳ᤨ㑆ߩടᾲឃ᳇㧘ࠆߪઁߩᣇᴺࠍᬌ⸛ߔࠆᔅⷐ߇ࠆߣ⠨߃ࠄࠇࠆޕ
߃߫㧘ᢥ₂[6]ߢ␜ߐࠇߡࠆࠃ߁ߥ㧘᳓⚛ߦࠃࠆห឵ᔕࠍ↪ߚ㒰ᨴ߽ലߢࠆߣ⠨
㪇 㪉 㪋 㪍 㪏 㪈㪇 㪈㪉 㪈㪋 㪈㪍 㪈㪏
㪇 㪈 㪉 㪊 㪋 㪌
㪫㪸㩿㪣α㪀 㪫㪸㩿㪤α㪀
㩷
㩷
㪚㫆㫌㫅㫋㫀㫅㪾㩷㫉㪸㫋㪼㪃㩷㪥㩷㪆㩷㪺㫆㫌㫅㫋㫊㩷㫄㫀㫅㪄㪈㩷㩿∆㪜㪀㪄㪈
㪜㫅㪼㫉㪾㫐㩷㫆㪽㩷㪯㪄㫉㪸㫐㫊㪃㩷㪜㩷㪆㩷㫂㪼㪭
㩷㪦㪹㫊
㪘㫉㩿㪢α㪀
㪙㪸㪺㫂㪾㫉㫆㫌㫅㪻
㪇 㪉 㪋 㪍 㪏 㪈㪇 㪈㪉 㪈㪋 㪈㪍 㪈㪏
㪇㪅㪇 㪇㪅㪌 㪈㪅㪇 㪈㪅㪌 㪉㪅㪇
㪫㪸㩿㪣α㪀 㩷
㩷
㪚㫆㫌㫅㫋㫀㫅㪾㩷㫉㪸㫋㪼㪃㩷㪥㩷㪆㩷㪺㫆㫌㫅㫋㫊㩷㫄㫀㫅㪄㪈㩷㩿∆㪜㪀㪄㪈
㪜㫅㪼㫉㪾㫐㩷㫆㪽㩷㪯㪄㫉㪸㫐㫊㪃㩷㪜㩷㪆㩷㫂㪼㪭
㩷㪦㪹㫊㪅
㪙㪸㪺㫂㪾㫉㫆㫌㫅㪻 㪘㫉㩿㪢α㪀 㪫㪸㩿㪤α㪀
10 ߃ࠄࠇࠆߚ㧘ᓟߩ⺖㗴ߣߒߚޕ
4. ߹ߣ
࿁㧘㜞Ớᐲߩ࠻࠴࠙ࡓߢᳪᨴߐࠇߚ࠲ࡦ࠲࡞✢߆ࠄߩ࠻࠴࠙ࡓߩ࿁߅ࠃ߮㒰ᨴࠍ⹜ߺߚޕ
13.3GBq ߩ࠻࠴࠙ࡓࠍๆ⬿ߒߚ࠲ࡦ࠲࡞✢ࠍടᾲߔࠆߎߣߢ11.7 GBqߩ࠻࠴࠙ࡓࠍ࿁ߒ㧘
ߎࠇߪๆ⬿ߒߚ࠻࠴࠙ࡓ㊂ߩ87.8%ߦ⋧ᒰߔࠆޕ943 Kߢ3.5ᤨ㑆ടᾲឃ᳇ߔࠆߎߣߢޔᱷሽ࠻
࠴࠙ࡓ㊂ࠍ564kBq߹ߢ㒰ᨴߔࠆߎߣ߇ߢ߈ߚޕߎߩᱷሽ࠻࠴࠙ࡓ㊂ߪๆ⬿ߒߚ࠻࠴࠙ࡓ㊂
13.3 GBqߩ0.004 %ߦߚࠅ㧘࿁⚳ੌᓟߩ࠻࠴࠙ࡓ㊂1.6 GBqߩ0.04 %ߢࠆޕ߹ߚ㧘ߘߩ
࠲ࡦ࠲࡞✢ࠍ᳓ᶐẃߔࠆߎߣߢᱷሽ࠻࠴࠙ࡓ㊂ߩ⚂ 37㧑ࠍ㒰ᨴߔࠆߎߣ߇ߢ߈ߚޕBIXS ࠬࡍ
ࠢ࠻࡞ࠃࠅޔടᾲߦࠃࠆ㒰ᨴߢߪౝㇱߩ࠻࠴࠙ࡓࠍ㒰ߔࠆߎߣ߇ߢ߈㧘᳓ᶐẃߢߪ࠲ࡦ࠲࡞
✢㕙ߩ࠻࠴࠙ࡓࠍᦝߦ㒰ߢ߈ߚߎߣ߇⏕ߐࠇߚޕ᳓ᶐẃࠍⴕߞߚ࠲ࡦ࠲࡞✢ࠍ⚂212ᣣ 㑆ⓨ᳇ਛߢ▤ߔࠆߎߣߦࠃߞߡޔ࠻࠴࠙ࡓߩౝㇱಽᏓ߇ടᾲߦࠃࠆ㒰ᨴࠍⴕߞߚ⋥ᓟߣหߓ ࠃ߁ߥ⁁ᘒߦߥࠆߎߣ߇⍮ࠄࠇ㧘▤ߦ㓙ߒߡᵈᗧ߇ᔅⷐߢࠆޕ
ᣣᧄߩᑄ᫈ၮḰߣᲧセߔࠆߣ㧘චಽߦᑄ᫈น⢻ߥࡌ࡞߹ߢ㒰ᨴࠍⴕ߁ߎߣ߇᧪ߚޕߒ߆ߒ㧘 ᣣᧄߩၮḰࠃࠅ߽෩ߒࠗࠡࠬߩૐࡌ࡞ᕈᑄ᫈‛ߩၮḰߣᲧセߔࠆߣ㧘㒰ᨴߪචಽߢߪ ߥ߆ߞߚߚ㧘ߐࠄߥࠆ㒰ᨴᣇᴺߩᬌ⸛߇ᔅⷐߢࠆޕ
࿁ߩ߇ߎߞߚߩߪ㧘ታ㛎߇ᆎ߹ࠆ߹ߢߦ࠲ࡦ࠲࡞߇หᤨߦኽߐࠇߡࠆߎߣࠍࡦ
࠲ߩᜂᒰ⠪߇⍮ࠄߐࠇߡߥ߆ߞߚߚߢ㧘ታ㛎⠪߮ࡦ࠲ᜂᒰ⠪㑆ߩᛂߜวࠊߖߩਇ⿷
߇ේ࿃ߢࠆޕᓟߎߩࠃ߁ߥࠍߎߐߥߚߦ߽㧘ห⎇ⓥࠍⴕ߁㓙ߪታ㛎⠪ߣࡦ࠲
ᜂᒰ⠪㑆ߩᛂߜวࠊߖࠍࠃࠅ߽✕ኒߦⴕߥߞߡߊᔅⷐ߇ࠆޕ
ෳ⠨ᢥ₂
[1] M. Matsuyama and K. Watanabe: Fusion Eng. Des. 18 (1991) 91
[2] M. Matsuyama, T. Murai, K. Yoshida, K. Watanabe, H, Iwakiri and N. Yoshida J. Nucl. Mater.
307-311 (2002) 729
[3] W. M. Mueller, J. P. Blackledge and G. G. Libowitz, (“Metal Hydrides”, Academic Press, 1968) [4] Y. Torikai, D. Murata, R.-D. Penzhorn, K. Akaishi, K. Watanabe, M. Matsuyama J. Nucl. Mater.
363-365 (2007) 462-466
[5] ᣣᧄࠕࠗ࠰࠻ࡊදળ RIᑄ᫈‛ߩ㓸⩄ߦߟߡ:
http://www.jrias.or.jp/index.cfm/6,1633,c,html/1633/20070529_panfu.pdf
[6] A. N. Prevezentsev , A. C. Bell, J. Williams and P. D. Brennan Fusion Eng. Des. 83 (2008) 1364 [6] A. N. Prevezentsev , A. C. Bell, J. Williams and P. D. Brennan Fusion Eng. Des. 83 (2008) 1364
䊉䊷䊃㩷
㊄ዻ᳓⚛ൻ‛↪ᵹ⏛᧤⸘䈱᭴▽䈫䈠䈱ᕈ⢻⹏ଔ㩷
㩷
⿒ਣᖗ჻ޔጟ㦮ޔේ ᱜᙗޔ᧻ጊᄦ ንጊᄢቇ᳓⚛ห⑼ቇ⎇ⓥࡦ࠲
ޥ930-8555 ንጊᏒ3190
㪚㫆㫅㫊㫋㫉㫌㪺㫋㫀㫆㫅㩷㫆㪽㩷㪘㫃㫋㪼㫉㫅㪸㫋㫀㫅㪾㪄㪚㫌㫉㫉㪼㫅㫋㩷㪤㪸㪾㫅㪼㫋㫆㫄㪼㫋㪼㫉㩷㪽㫆㫉㩷㪤㪼㫋㪸㫃㩷㪟㫐㪻㫉㫀㪻㪼㩷 㩷 㪸㫅㪻㩷㪠㫋㫊㩷㪧㪼㫉㪽㫆㫉㫄㪸㫅㪺㪼㩷㪫㪼㫊㫋㫊㩷
㩷
Satoshi Akamaru, Keisuke Okazaki, Masanori Hara, and Masao Matsuyama Hydrogen Isotope Research Center, University of Toyama, Gofuku 3190, Toyama
930-8555, Japan
(ReceivedNovember 21, 2011; accepted March 9, 2012) Abstract
An alternating-current magnetometer was assembled to measure the magnetic susceptibility of metal hydride in hydrogen atmosphere, and its performance tests were carried out. The magnetometer was designed to be integrated into the conventional pressure-composition-temperature (PCT) measurement system without any reconstruction. Calibration of the magnetometer was performed using a paramagnetic Gd2O3 powder, and it gave a linear relationship between the output signal and the magnetic moment of Gd2O3 powder. The magnetic susceptibility of PdHx (0 ≤ x ≤ 0.7) was measured simultaneously with the PCT curve. The magnetic susceptibility of Pd hydride decreased with increasing hydrogen concentration in Pd and finally reached zero at the hydrogen concentration above 0.65. The behavior of magnetic susceptibility and PCT curves quantitatively agreed with the previously reported values.
1. ✜⸒
㊄ዻ᳓⚛ൻ‛ߪ᳓⚛⾂⬿᧚ᢱߣߒߡߩᔕ↪߇ᦼᓙߐࠇߡ߅ࠅޔᄙ⒳ᄙ᭽ߥ᧚ᢱ㐿⊒߮
ߘߩ᳓⚛ๆ․ᕈߦ㑐ߔࠆၮ␆⎇ⓥ߇⋓ࠎߦⴕࠊࠇߡࠆޕ৻ᣇߢ㊄ዻ᳓⚛ൻ‛ߩ‛
ᕈ㧔㔚⏛᳇ޔᾲޔశ‛ᕈߥߤ㧕ࠍ↪ߒߚᔕ↪⎇ⓥ[1,2]߽ⴕࠊࠇߡࠆ߇ޔ᳓⚛⾂⬿᧚ᢱ㑐 ㅪߩ⎇ⓥߣᲧセߔࠆߣዋߥޕߘߩ৻ߟߩⷐ࿃ߣߒߡޔ㊄ዻ᳓⚛ൻ‛ߩ‛ᕈߦ㑐ߔࠆၮ␆
⎇ⓥ߇ዋߥߎߣ߇⠨߃ࠄࠇࠆޕ
㊄ዻߩ⏛᳇․ᕈߪޔฎߊ߆ࠄ᭽ޘߥᎿᬺຠߦᔕ↪ߐࠇߡࠆޕ߹ߚޔߦ߅ߡ߽
⏛ᕈ᧚ᢱߩᕈ⢻ะࠍ⋡ᜰߒߚ㐿⊒⎇ⓥ߇ⴕࠊࠇߡࠆޕ᧚ᢱ㐿⊒ߩⷰὐ߆ࠄࠆߣޔ㊄ ዻ᳓⚛ൻ‛ߪ⚿᥏ߩ᭴ㅧᄌൻࠍᒁ߈ߎߔߎߣ߆ࠄޔ⏛᳇․ᕈߩᓮᚗߪᣂߚߥ․ᕈߩ
⊒ߦ↪ߢ߈ࠆߣ⠨߃ࠄࠇࠆޕߒ߆ߒޔ㊄ዻ᳓⚛ൻ‛ߪ᳓⚛ๆߦࠃࠅᄙߊ߇ᓸ☳ൻߒޔ ᄢ᳇ਛߦขࠅߔ㓙ߦ㕙㉄ൻߩᓇ㗀ࠍฃߌࠆߚޔ㊄ዻ᳓⚛ൻ‛ߦኻߔࠆ⏛᳇․ᕈߩᱜ
⏕ߥ᷹ቯ߇࿎㔍ߢߞߚޕ
ߘߎߢᧄႎ๔ߢߪޔ᳓⚛ๆ․ᕈߩ⹏ଔߦ↪ࠄࠇߡࠆޔജ-⚵ᚑ-᷷ᐲ․ᕈ 㧔PCT㧕᷹ቯⵝ⟎߆ࠄ㊄ዻ᳓⚛ൻ‛ࠍขࠅߔߎߣߥߊޔ᳓⚛ࠟࠬ㔓࿐᳇ਛߦߡޔ᳓⚛ൻ‛
ߩ⏛᳇․ᕈࠍ᷹ቯߔࠆߚޔPCT ᷹ቯⵝ⟎ߦኈᤃߦ⚵ߺㄟࠆᵹ⏛᧤⸘ߩ᭴▽ࠍⴕޔ ߘߩᕈ⢻⹏ଔࠍPd☳ᧃࠍ↪ߡⴕߞߚޕ
2. ᵹ⏛᧤⸘ߩේℂߣⵝ⟎ߩ᭴▽
2.1. ⶄ⚛⏛ൻ₸
ߪߓߦᵹ⏛႐ਅߢߩ⏛ൻ₸ߦߟߡ◲නߦ⺑ߔࠆ[3]ޕ⏛႐ߩᣇะ߇ᦼ⊛ߦᄌൻ ߔࠆᵹ⏛႐ਅߦ⹜ᢱ߇ࠆ႐วޔ⹜ᢱߩ⏛ൻ₸χ(m3/kg)ߪⶄ⚛⏛ൻ₸χˆߣߒߡએਅߩࠃ ߁ߦ⸥ㅀߐࠇࠆޕ
χ χ
χˆ = ′− j ′′ …(1)
ߎߎߢޔj ߪ⯯ᢙනࠍߔޕ৻⥸ߦχ′ߪ⏛᳇ᔕ╵ߩᵄᢙଐሽᕈࠍ␜ߒޔχ′′ߪ⏛ᕈౝ
ߩ㡆✭⽎ߦࠃࠆ⏛᳇ᔕ╵ߩㆃࠇࠍ␜ߒߡࠆޕߥ߅ޔߎߎߢߪSI න♽㧔E-Bኻ ᔕ㧕ࠍ↪ߡోߡߩᑼࠍ⸥ㅀߔࠆޕᵹ⏛႐Hˆ (Am-1)ਅߢߩ⏛ൻ₸χˆޔ⹜ᢱਛߩ⏛᧤ኒᐲ
Bˆ(Wb/m2)ޔ߮⹜ᢱߩ⾰㊂⏛ൻMˆ (Am2/kg)ߣߩ㑐ଥߪ㕒⏛႐ਅߢߩ㑐ଥߣᄌࠊࠄߕޔ
( )
HBˆ 1 ˆ ˆ
0 χ
µ +
= ޔ Mˆ =χˆHˆ …(2, 3)
ߣߥࠆޕߎߎߢޔµ0ߪ⌀ⓨਛߩㅘ⏛₸ࠍ␜ߔޕᵹ⏛႐Hˆ ߩⷺᝄേᢙࠍω(2π/sec)ߣߔࠆ ߣޔHˆ ߮Bˆߪએਅߩࠃ߁ߦ⸥ㅀߐࠇࠆޕ
t H
Hˆ expω
= 0 …(4)
(
ω −δ)
=B t
Bˆ exp
0 …(5)
H0߮B0ߪߘࠇߙࠇߩᝄߩᄢ߈ߐߢࠅޔt(sec)ߪᤨ㑆ߢࠆޕBˆߦߞߡࠆδ ߪޔ
H0߆ࠄߩ⋧ߩㆃࠇࠍ␜ߔޕ⸥ߒߚࠃ߁ߦޔ⋧ߩㆃࠇߪχ′′ߦ㑐ㅪߔࠆ㗄ߢࠅޔω߇ ዊߐߌࠇ߫δ ߪ߶߷0ߣߥࠆޕߟ߹ࠅߎߩ⁁ᴫਅߢߪޔχ′ߪ㕒⏛႐ਅߢߩ⏛ൻ₸χߣ৻⥌
ߔࠆߎߣ߇⍮ࠄࠇߡࠆޕ(2)-(5)ᑼࠍ↪ࠆߣޔχ′߮χ′′ߪએਅߩࠃ߁ߦ⸥ㅀߐࠇࠆޕ
(
χ) (
ωω δ) ( )
δ( ( )
δ( )
δ)
µ + = = − = exp − = cos − + sin − exp
ˆ exp ˆ ˆ
1
0 0 0
0 0
0 0 j
H B H
B t
H t B
H
B …(6)
1 cos
0 0
0 −
′= δ
χ µ
H
B …(7)
µ δ
χ sin
0 0
0
H
= B
′′ …(8)
ߟ߹ࠅޔχ′߮χ′′ߪ⹜ᢱਛߩ⏛᧤ኒᐲBˆߩᵹ⏛႐Hˆ ߣหߓ⋧ࠍᜬߟᚑಽߣޔ90oߛߌ
⋧ߩㆃࠇߚᚑಽࠍ᷹ቯߔࠆߎߣߢ᳞ࠆߎߣ߇ߢ߈ࠆޕ 2.2 ᵹ⏛᧤⸘ߩේℂ
ᵹ⏛᧤⸘ߢߪޔᵹ⏛႐ਅߢߩ⹜ᢱਛߩ⏛᧤ኒᐲߩᄌൻࠍ࠰ࡁࠗ࠼ࠦࠗ࡞߳ߩ⺃ዉ
㔚ജߣߒߡᬌߔࠆޕߘߩේℂࠍએਅߦ⺑ߔࠆ[4]ޕᵹ⏛႐⊒↢↪ߣߒߡ↪ࠆඨᓘaޔ 㐳ߐlޔ✢Ꮞ߈ᢙN1ߩਛⓨߩ࠰ࡁࠗ࠼ࠦࠗ࡞1㧔ࠕࠢ࠲ࡦࠬL1㧕ߦએਅߩᵹ㔚Vˆ1ࠍ ශടߔࠆޕ
t j V
Vˆ1= 0exp ω …(9)
V0ߪᵹ㔚ߩᝄߢࠆޕߎߩߣ߈࠰ࡁࠗ࠼ࠦࠗ࡞1ߦᵹࠇࠆ㔚ᵹIˆ1ߪޔ
( )
2(
1)
1 2 1
0 1
1 0 1
1 1 exp exp
ˆ
ˆ ˆ ω θ
ω ω
ω −
= +
= +
= j t
L R
V L
j R
t j V Z
I V ޔ …(10)
ૉߒޔ R
L1
1 tan 1ω
θ = − …(11)
ߣߥࠆޕߎߎߢޔZˆ1ߪ࠰ࡁࠗ࠼ࠦࠗ࡞1ߩⶄ⚛ࠗࡦࡇ࠳ࡦࠬޔR1ߪ࠰ࡁࠗ࠼ࠦࠗ࡞
1ߩ㔚᳇ᛶ᛫ߢࠆޕߎߩ㔚ᵹIˆߦࠃࠅޔ࠰ࡁࠗ࠼ࠦࠗ࡞1ߩ┵߆ࠄ〒㔌xߩ႐ᚲߦ⊒↢
ߔࠆ⏛႐Hˆ1ߪޔⓨߩࠦࠗ࡞ਛߩ⏛᧤ኒᐲBˆ1ࠃࠅએਅߩࠃ߁ߦᦠߌࠆޕ
( )
( ) ( )
2(
1)
1 2 1
0 2 2
2 2 1
2 2 2
2 1 0 1 1
2 exp 2
ˆ ˆ ˆ
θ ω ω
µ
+ −
− +
− −
= +
− +
− −
= +
=
t L j
R V x
l a
x l x
a x l
N
x l a
x l x
a x l
I N H B
…(12)
ߎߩᵹ⏛႐ߩਅߢ࠰ࡁࠗ࠼ࠦࠗ࡞1ߩਛᔃㇱ㧔x = l/2㧕ߦⶄ⚛⏛ൻ₸χˆ1ߩ⹜ᢱࠍኒߦߟ
ߚ႐วޔ⹜ᢱਛߩ⏛᧤ኒᐲBˆ1inߪએਅߩࠃ߁ߦᦠ߈ߐࠇࠆޕ
( )
( )
( )
2(
1)
2 1 1
0 2
1 2 0
1 1 0 1
4 exp ˆ 2
1 ˆ ˆ ˆ 1
θ ω ω
χ µ
χ µ
+ − + +
= +
=
t L j
R V l
a N H Bin
…(13)
ߎߩ⏛᧤ኒᐲߩᄌൻߦࠃࠅޔ࠰ࡁࠗ࠼ࠦࠗ࡞1 ߦ㊀ߨߡᏎߚ࠰ࡁࠗ࠼ࠦࠗ࡞ 2 ߦߪ એਅߩ⺃ዉ㔚ജVˆ2in߇⊒↢ߔࠆޕ
Coil 1
Coil 3
Coil 2
Lock-in Amplifier
Pd powder TMP
H2 RP gas
Fig. 1. Schematic view of alternating current susceptometer and conventional PCT measurement system.
( )
( )
( )
− − + +
− +
=
−
=
exp 2 4
exp 2 1 ˆ
ˆ ˆ
2 1 2 1
1 0 2
2 1 0
2 1 2
θ π ω ω
ω δ µ
χ j t
L R
V l
a j NS dt
B S d
Vin in
…(14)
ߎߩᑼߪవ㗡ߩᒐਛߩੑߟߩ㗄ߦಽߌࠄࠇޔ೨ߩ㗄ߪᵹ⏛႐߇ߎߔ㧔⹜ᢱ߇ή႐ วߩ㧕⺃ዉ㔚ജޔᓟߩ㗄ߪ⹜ᢱਛߩ⏛᧤ኒᐲߩᄌൻߦ࿃ߒߚ⺃ዉ㔚ജߣߥߞߡࠆޕ ߎࠇࠃࠅޔ⹜ᢱࠍߚ㓙ߩ⺃ዉ㔚ജ߆ࠄޔ⹜ᢱ߇ή႐วߩ⺃ዉ㔚ജࠍᒁߊߎߣߦ ࠃࠅޔ⹜ᢱߩⶄ⚛⏛ൻ₸ߩᄢ߈ߐχˆ1 ߮⋧ߩߕࠇδ 㧔ᚗߪχ′߮χ′′㧕ߦ㑐ߔࠆᖱႎ ࠍᓧࠆߎߣ߇ߢ߈ࠆޕ
2.3 ᵹ⏛᧤⸘ߩⷐ
᷹ቯⵝ⟎ߩ⇛ࠍ࿑ 1 ߦ␜ߔޕ࿑ਛߩ⎕✢ߢ࿐߹ࠇߚㇱಽ߇ޔ࿁᭴▽ߒߚᵹ⏛᧤⸘
ߢࠅޔߘߩઁߩㇱಽߪᣢሽߩPCT ᷹ቯⵝ⟎ߢࠆޕᵹ⏛᧤⸘ࠍᣢሽߩ᳓⚛ๆ᷹
ቯⵝ⟎ߦ⚵ߺㄟ㓙ߪޔ⹜ᢱ▤એᄖߪⵝ⟎ߩᡷㅧࠍᔅⷐߣߒߥޕ߹ߚޔᵹ⏛᧤⸘ߣPCT
᷹ቯⵝ⟎ߪߦ⁛┙ߦ↪น⢻ߢࠆޕ
ᵹ⏛᧤⸘ߪᵹାภ⊒ାᯏ㧔DF1906, NF ࿁〝⸳⸘ࡉࡠ࠶ࠢ㧕߮ࡠ࠶ࠢࠗࡦࠕࡦࡊ 㧔Model 5210, SEIKO Instruments㧕ޔߘߒߡౝᓘ8 mmޔᄖᓘ10 mmߩ⍹⧷▤ߦᏎߚ3ߟ ߩ࠰ࡁࠗ࠼ࠦࠗ࡞ࠃࠅ᭴ᚑߐࠇࠆޕ࿑ 1 ਛߦ⸥タߒߚᵹ⏛᧤⸘ߩ࠰ࡁࠗ࠼ࠦࠗ࡞ߩ ߁ߜޔᏀߩ࠰ࡁࠗ࠼ࠦࠗ࡞ 1 ߇ᵹ⏛႐⊒↢↪ߢࠅޔฝߩ 2 ߟߩ࠰ࡁࠗ࠼ࠦࠗ
࡞2ޔ3߇⹜ᢱߩ⺃ዉ㔚ജ᷹ቯ↪ߢࠆޕ
࠰ࡁࠗ࠼ࠦࠗ࡞2ߣ3ߪޔᵹ⏛႐⊒↢
ᤨߦࠦࠗ࡞ߩਛ߇ⓨߩ⁁ᘒߢ߶߷หߓ
ജ߇ᓧࠄࠇޔਔ⠪ߩജߩᏅಽ߇߶߷0ߦ ߥࠆࠃ߁ߦᏎ߈ᢙࠍ⺞ᢛߒߡࠆޕߟ߹ࠅ
⹜ᢱ᷹ቯᤨߪޔ ᣇߩ࠰ࡁࠗ࠼ࠦࠗ࡞ߦ
⹜ᢱࠍ㈩⟎ߒޔ߽߁ ᣇߩⓨߩ࠰ࡁࠗ࠼
ࠦࠗ࡞߆ࠄ⊒↢ߔࠆജࠍᏅߒᒁߊߎߣ ߢޔ⹜ᢱߩ⏛ൻ₸ߦ࿃ߒߚ⺃ዉ㔚ജߩ ߺࠍขࠅߔޕߒ߆ߒታ㓙ߦߪޔⓨߩ⁁ᘒ ߢߩ࠰ࡁࠗ࠼ࠦࠗ࡞2߮3ߩജߪቢ
ోߦ৻⥌ߖߕޔ⚿ᨐߣߒߡਔ⠪ߩᏅಽߩ
ജࠍࡠ࠶ࠢࠗࡦࠕࡦࡊߢ᷹ቯߔࠆߣޔ৻ቯ ߩ⺃ዉ㔚ജVback߇ᬌߐࠇࠆޕߟ߹ࠅታ 㓙ߦ⹜ᢱࠍ᷹ቯߒߚ႐วޔ࠰ࡁࠗ࠼ࠦࠗ
࡞2ߦ⹜ᢱࠍ⸳⟎ߒ࠰ࡁࠗ࠼ࠦࠗ࡞2ߩ
ജ߆ࠄ࠰ࡁࠗ࠼ࠦࠗ࡞3ߩജࠍᏅߒ
ᒁߚ⺃ዉ㔚ജV2inࠍ᷹ቯߔࠆߣޔ
sample back
in V V
V2 = + …(15)
ߣߥࠆޕߟ߹ࠅޔV2inߪ⹜ᢱߦ࿃ߒߚ⺃ዉ㔚ജVsampleߦVback߇ടࠊߞߚ୯ߣߥࠆޕߎߩ Vbackࠍขࠅ㒰ߊߚޔV2inࠍ᷹ቯߒߚᓟޔ⹜ᢱࠍ࠰ࡁࠗ࠼ࠦࠗ࡞ 3ߦ⒖േߒޔV2inࠍ᷹ቯ ߒߚ႐วߣหߓࠃ߁ߦޔ࠰ࡁࠗ࠼ࠦࠗ࡞ 2 ߩജ߆ࠄ࠰ࡁࠗ࠼ࠦࠗ࡞ 3 ߩജࠍᏅߒ ᒁߚ⺃ዉ㔚ജV3inࠍ᷹ቯߔࠆޕ
sample back
in V V
V3 = − …(16 )
(15)ᑼ߮(16)ᑼࠃࠅޔV2in߆ࠄ V3inࠍᒁߚ୯∆VߪVsample ߩߺߩജߣߥࠆߎߣ߇ࠊ߆ࠆޕ ᧄ᷹ቯߢߪએߩᚻᴺࠍ↪ߡ∆Vࠍ᷹ቯߒߚޕߘߩ㓙ޔ⹜ᢱ⟎ߩ⒖േߪ࠰ࡁࠗ࠼ࠦࠗ
࡞ోࠍ⒖േߔࠆߎߣߦࠃࠅⴕߞߚޕ߹ߚޔ࿁⺃ዉ㔚ജߩᬌߦ↪ࠆࡠ࠶ࠢࠗࡦࠕ ࡦࡊߢߪޔᵹ㔚ߩᝄ߮ෳᾖାภ㧔ߎߎߢߪ࠰ࡁࠗ࠼ࠦࠗ࡞ 1 ߦࠃࠅ⊒↢ߔࠆ
ᵹ⏛႐㧕߆ࠄߩ⋧ߩߕࠇࠍหᤨߦ᷹ቯน⢻ߢࠅޔߎߩᯏ⢻ࠍ↪ߡޔχ′ߦᲧߔࠆෳ
ᾖାภߣห⋧ߩജ∆Vxޔ߅ࠃ߮χ′′ߦᲧߔࠆ90Oㆃࠇߚ⋧ߩജ∆Vyࠍ᳞ߚޕ 2.4 ᵹ⏛᧤⸘ߩᩞᱜ
᷹ቯߒߚ⺃ዉ㔚ജ߆ࠄ⏛ൻ₸߳ߩᄌ឵ߪޔ੍⏛ൻ₸߇ᣢ⍮ߢࠆᮡḰ⹜ᢱߦࠃࠅᓧ ࠄࠇࠆ⺃ዉ㔚ജߣ⏛ൻ₸ߩ㑐ଥࠍ↪ߡ߅ߎߥߞߚޕ࿁ߪᮡḰ⹜ᢱߣߒߡ Gd2O3☳ᧃ ࠍ↪ߚޕᚲቯߩ㊀㊂ߩGd2O3☳ᧃࠍߟߚ㐳ߐ10 mm⒟ᐲߩ࠹ࡈࡠࡦߩ╴ࠍޔGd2O3
☳ᧃߩ㊀㊂ࠍᄌ߃ߡ5⒳㘃ᚑߒޔߘࠇߙࠇߩ⺃ዉ㔚ജࠍ᷹ቯߒߚޕ᷹ቯߣߒߡGd2O3
☳ᧃ45.4 mgߩ᷹ቯᤨߩ⺃ዉ㔚ജߩᄌൻࠍ࿑2ߦ␜ߔޕ࿑2ߦ␜ߒߚ⺃ዉ㔚ജߪ࠰ࡁ
ࠗ࠼ࠦࠗ࡞2 ߆ࠄ࠰ࡁࠗ࠼ࠦࠗ࡞ 3ߩജࠍᏅߒᒁߚ୯ߢࠅޔᦝߦࡠ࠶ࠢࠗࡦࠕࡦ ࡊߦࠃࠅᵹ⏛႐ߣห⋧ߩVxޔ߮⋧߇90OㆃࠇߚVyࠍಽ㔌ߒߡ᷹ቯߒߚ⚿ᨐߢࠆޕ
߹ߚޔ࿑2ߩԘߩ㗔ၞ߇࠰ࡁࠗ࠼ࠦࠗ࡞2ߦ⹜ᢱࠍ㈩⟎ߒߚ႐วߩജ㧔(15)ᑼߩV2inߦ
⋧ᒰ㧕ޔԙߩ㗔ၞ߇࠰ࡁࠗ࠼ࠦࠗ࡞3ߦ⹜ᢱࠍ㈩⟎ߒߚ႐วߩജ㧔(16)ᑼߩV3inߦ⋧ᒰ㧕 ߢࠆޕߎࠇࠃࠅޔVbackߣߒߡVxߢ-510µVޔVyߢ280 µV⒟ᐲߩജ߇ࠆߎߣ߇ࠊ߆ࠆޕ ߎࠇ߇࠰ࡁࠗ࠼ࠦࠗ࡞ 2 ߮ 3 ߩࠕࡦࡃࡦࠬಽߩജߣߥࠆޕ⹜ᢱߩ⏛ൻ₸ߦኻᔕߔ ࠆޔԘߣԙߩᏅಽ∆Vߪޔ∆Vxߢ14.1 µVജߐࠇࠆߩߦኻߒߡޔ∆Vyߢߪ߶ߣࠎߤ0ߣߥࠆޕ ߟ߹ࠅޔ࿁↪ߚᵄᢙߢߪޔ⋧ߩߕࠇߪ߶߷0ߣߥࠅޔVxࠃࠅ᳞ࠆχ′ߩ୯ߪ㕒⏛
႐ਅߢߩ⏛ൻ₸χߦ߶߷৻⥌ߔࠆߣ߃ࠆޕߎߩ∆VߣGd2O3ߩ㊀㊂ߩ㑐ଥࠍ᷹ቯߒߚ⚿ᨐ ࠍ࿑3ߦ␜ߔޕ᷹ቯߪฦ㊀㊂ߢ5࿁ⴕߞߚޕߎߩ⚿ᨐࠃࠅޔ∆VxߪGd2O3ߩ㊀㊂ߦኻߒߡ⋥
✢㑐ଥޔ∆Vyߪో㗔ၞߢ߶߷ 0ߢࠆߣࠊ߆ࠆޕ∆Vxߩ⋥✢ࠍᦨዊੑਸ਼ᴺߦࠃࠅㄭૃߔࠆߎ ߣߢޔ࿑3ਛߦ␜ߔᑼ߇ᓧࠄࠇߚޕGd2O3ߩ⏛ൻ₸ߪቶ᷷ߢ1.7410-6 m3/kgߢࠆߎߣ߇
⍮ࠄࠇߡ߅ࠅ[5]ޔߎߩ୯ߣᦨዊੑਸ਼ᴺߦࠃࠅᓧࠄࠇߚ⋥✢ߩᑼ߆ࠄޔਅ⸥ߩ⺃ዉ㔚ജ∆Vx (µV)ߣ⏛ൻ₸χ(m3/kg)ߩ㑐ଥᑼࠍᓧߚޕ
( )
W Vx 1.74 10 1
31292 . 0
10386 .
0 × × 6×
−
= ∆ −
χ …(17)
ߎߎߢޔW (mg)ߪ᷹ቯ⹜ᢱߩ㊀㊂ࠍ␜ߔޕPd ᳓⚛ൻ‛ߩ᷹ቯߦࠃࠅᓧࠄࠇߚ∆Vxߪߎߩᑼ
ࠍ↪ߡ⏛ൻ₸ߦᄌ឵ߒߚޕ߹ߚޔฦ㊀㊂ߢ᷹ቯߒߚ 5 ὐߩᮡḰᏅࠍ᳞ࠆߣޔᦨᄢߢ
0.208µVߢߞߚޕᮡḰᏅߩ2ࠍಽ⸃⢻ߣߔࠆߣޔPd᷹ቯᤨߢߩⵝ⟎ߩಽ⸃⢻ߪᑼ
ࠃࠅ2.1710-9 m3/kgߣⓍ߽ࠄࠇߚޕ 㧔㧡㧕Pd᳓⚛ൻ‛ߩ᷹ቯ
᷹ቯ⹜ᢱߢࠆ Pd㧔99.9㧑ޔ࠾ࠦ㧕ߪޔ᧼⁁ߩ߽ߩࠍࡒ࠶ࠢ߿ߔࠅߢ☳ᧃ⁁ߦട Ꮏߒߚ߽ߩࠍ↪ߚޕߘߩᓟޔPCT᷹ቯⵝ⟎ߦขࠅઃߌߚ⍹⧷࡞ਛߦޔ⚂1 gߩ☳ᧃPd ࠍࠇޔ࡞ਛࠍ510-5 Paએਅ߹ߢឃ᳇ߒߚޕߘߩᓟޔᵴᕈൻಣℂߣߒߡ523 Kߢ2 hߩ ടᾲឃ᳇ࠍⴕޔ಄ළᓟߩ⁁ᘒࠍ᳓⚛Ớᐲ[H]/[Pd] = 0ߣߒߚޕߎߎ߆ࠄPdߦ৻ቯ㊂ߩH2
ࠟࠬࠍዉߒޔPd᳓⚛ൻ‛ߣ᳇⋧ߩH2ࠟࠬ߇ᐔⴧߦ㆐ߒߚߩߜߦޔ⸥ⵝ⟎ߦࠃࠅPd᳓
⚛ൻ‛ߩ⺃ዉ㔚ജࠍ᷹ቯߒߚޕߎࠇࠍޔᐔⴧ߇0.1 MPa⒟ᐲߦߥࠆ߹ߢ➅ࠅߒⴕߞߚޕ
⺃ዉ㔚ജߩ᷹ቯߪޔ295 ~ 300 Kߩቶ᷷ߦߡޔ࠰ࡁࠗ࠼ࠦࠗ࡞1ߦᵄᢙ487 Hzޔᵹ ᝄVp-p㧔ᦨᄢ୯ߣᦨዊ୯ߩᏅ㧕10 Vߩᵹ㔚ࠍශടߔࠆߎߣߢⴕߞߚޕ
3. ታ㛎⚿ᨐ
࿑4ߦᵹ⏛᧤⸘ࠍ↪ߡ᷹ቯߒߚPd᳓⚛ൻ‛ߩ∆Vx߮∆Vyߩ᳓⚛Ớᐲଐሽᕈޔ߮ᐔ ⴧߩ᳓⚛Ớᐲଐሽᕈࠍ␜ߔޕPdߩᐔⴧߪ[H]/[Pd] = 0.05એ0.6ᧂḩߢ߶߷৻ቯߩ୯ࠍ
␜ߒޔ[H]/[Pd] > 0.6ߢᕆỗߦჇടߒߚޕߎߩะߪㆊߦ᷹ቯߐࠇߚ⚿ᨐ[6]ߣࠃߊ৻⥌ߒ
ߚޕ
ᐔⴧߣหᤨߦ᷹ቯߒߚ∆Vx߅ࠃ߮∆Vyߦߟߡߪޔ∆Vxߪ᳓⚛Ớᐲ߇㜞ߊߥࠆߦᓥන
⺞ߦᷫዋߒޔ[H]/[Pd] = 0.65ߢߪ߶߷0ߦ㆐ߒߚޕ߹ߚޔߘࠇએߩ᳓⚛Ớᐲߢߪ∆Vxߪ Fig. 2. Typical measurement result of
in-phase and out-of-phase output voltage for 45.4 mg Gd2O3 powder.
Fig. 3. Gd2O3 weight dependence of output signal,∆Vx and ∆Vy. The dashed line shows the result by least squared fit to ∆Vx.
-520 -515 -510 -505 -500
270 275 280 285 290
0 100 200 300 400 500 600
Gd2O
3 powder (45.4 mg)
output voltage, V x / µV output voltage, V y / µV
time, t / sec
f = 487 Hz, Vp-p = 10 V, 295 K
∆Vx
㽲 㽳
0 2 4 6 8 10 12 14 16
0 2 4 6 8 10 12 14 16
0 10 20 30 40 50
Gd2O3 powder
y = 0.10386 + 0.31292x , R= 0.99913
output signal, ∆V x_Gd2O3 / µV
Gd2O
3 weight, w
Gd2O3 / mg
output signal, ∆V Y_Gd2O3 / µV
ᄌൻߒߥ߆ߞߚޕ৻ᣇޔ∆Vyߪ[H]/[Pd] = 0.2⒟ᐲ߹ߢ߶߷৻ቯߢࠅޔ0ߢߪߥ㒢ߩ୯ ࠍ␜ߒߚޕ[H]/[Pd] > 0.2ߢߪޔ∆Vyߪ[H]/[Pd]ߩჇടߦᓥන⺞ᷫዋߒޔ∆Vx߇߶߷0ߣߥࠆ
[H]/[Pd] = 0.65એߦ߅ߡ߽න⺞ᷫዋߒ0ߦߪߥࠄߥ߆ߞߚޕ೨ㅀߒߚࠃ߁ߦޔ࿁ታ㛎
ߢ↪ߚᵹ⏛႐ߩᝄേᢙߪචಽዊߐߣ⠨߃ࠄࠇޔ߹ߚ PdߪPauli Ᏹ⏛ᕈߢࠅᄢ߈ߥ
⏛᳇ࡕࡔࡦ࠻ࠍᜬߚߥߎߣ߆ࠄޔ∆Vy= 0ࠍ␜ߔߪߕߢࠆޕߎߩ∆Vy߇㒢ߩ୯ࠍ␜ߔ
ේ࿃ߣߒߡޔᵹ⏛႐ਛߦ߅ߡ⹜ᢱਛߦ⊒↢ߔࠆ⺃ዉ㔚ᵹߦࠃࠆᓇ㗀߇⠨߃ࠄࠇࠆޕߟ
߹ࠅޔPd᳓⚛ൻ‛ߩ᳓⚛Ớᐲ߇ჇടߔࠆߎߣߢPd☳ᧃ߇⤘ᒛߒ☳ᧃห჻ߩ⚿ว߇ᡷༀߐࠇ ࠆߚޔ⺃ዉ㔚ᵹߩࡄࠬ߇㐳ߊ᭴▽ߢ߈ࠆࠃ߁ߦߥࠅޔ⚿ᨐߣߒߡ⺃ዉ㔚ᵹߦࠃࠅ⊒↢ߔ ࠆ⏛᧤߇ᄢ߈ߊߥࠆߚߢߪߥ߆ߣផኤߢ߈ࠆޕૉߒޔߎࠇࠄߩ⸃ᨆߪᦝߥࠆ⚦ߥ᷹
ቯ߮⸃ᨆ߇ᔅⷐߣߥࠆߚޔᤨὐߢߪߎࠇએߩᬌ⸛ߪⴕࠊߥޕ
࿑ 5ߦ(17)ᑼࠍ↪ߡ∆Vxߩ୯ࠍ⏛ൻ₸χߦᄌ឵ߒߚ⚿ᨐࠍ␜ߔޕࠊߖߡ SQUID⏛᧤
⸘ࠍ↪ߡ᷹ቯߐࠇߚㆊߩ᷹ቯ⚿ᨐ[7]ࠍ␜ߒߚޕ࿁᷹ቯߐࠇߚ⚿ᨐߣޔㆊߦ᷹ቯߐ ࠇߚ⚿ᨐߪޔቯ㊂⊛ߦࠃߊ৻⥌ߒߚޕએࠃࠅޔ࿁᭴▽ߒߚᵹ⏛᧤⸘ߦࠃࠅ᳓⚛ൻ‛
ߩ⏛ൻ₸߇᷹ቯน⢻ߢࠆߎߣ߇␜ߐࠇߚޕ
4. ߹ߣ
㊄ዻ᳓⚛ൻ‛᷹ቯ↪ᵹ⏛᧤⸘ࠍߒޔߘߩᕈ⢻⹏ଔࠍⴕߞߚޕߒߚᵹ⏛᧤⸘
ߪޔ⹜ᢱࠍ᳓⚛㔓࿐᳇ࠃࠅขࠅߔߎߣήߊ᷹ቯ߇ߢ߈ࠆࠃ߁ޔᣢሽߩ PCT᷹ቯⵝ⟎ࠍᡷ ㅧߖߕߦขࠅઃߌࠄࠇࠆࠃ߁⸳⸘ߒߚޕGd2O3☳ᧃࠍ↪ߡ⏛᧤⸘ߩᩞᱜࠍⴕߞߚߣߎࠈޔ
᷹ቯ㔚ߣ Gd2O3 ㊀㊂ߩ㑆ߢࠃ⋥✢㑐ଥ߇ᓧࠄࠇޔߎࠇࠃࠅޔ᷹ቯ㔚߆ࠄ⏛ൻ₸߳ߩ ᄌ឵ᑼ߮⏛᧤⸘ߩಽ⸃⢻2.1710-9 m3/kg߇ᓧࠄࠇߚޕᧄⵝ⟎ࠍ↪ߡPd᳓⚛ൻ‛ߩ⏛
ൻ₸᷹ቯࠍⴕߞߚ⚿ᨐޔㆊߦႎ๔ߐࠇߚ୯ߣቯ㊂⊛ߦࠃߊ৻⥌ߒߚޕએࠃࠅޔᵹ⏛
᧤⸘ࠍ↪ߚ㊄ዻ᳓⚛ൻ‛ߩ⏛ൻ₸᷹ቯ߇චಽน⢻ߢࠆߎߣ߇␜ߐࠇߚޕ Fig. 4. Hydrogen concentration dependence
of output signal and equilibrium pressure for Pd hydride. The dashed line for equilibrium pressure is guide to the eye.
Fig. 5. Hydrogen concentration dependence of magnetic susceptibility of Pd hydride. The figure includes the data reported by Hara et al.[5]
0 10 20 30 40 50 60 70
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 our work Hara et al.
magnetic susceptibility,χ' / 10-9 m3 /kg
[H]/[Pd]
-10 -5 0 5 10 15
0.1 1 10 100
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7
output voltage, ∆Vx,∆Vy / µV equilibrium pressure, P / kPa
[H]/[Pd]
∆Vx
∆Vy P
Reference
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Application-oriented Properties, (Springer-Verlag, Berlin, 1978).
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