LMC

J. Hot Spring Sci. /2 ,.+ῌ,// ,**3ῌ῍ Na-Cl  ! Ra "#$ 
OP+ QR S, QNTUV- WX Y.Z[\]+ ^>_`+ ab+ ,*  +,  ,,   ,+  ,  +3  

Radium Isotope in Na-Cl Type Saline Watersfrom Deep Wells around Coastal Area in
Ishikawa Prefecture, Japan
Junpei TOMITA+, Hiroshi SATAKE,, Keiichi SASAKI-, Aya SAKAGUCHI.,Mutsuo INOUE+, Yasunori HAMAJIMA+ and Masayoshi YAMAMOTO+

Abstract
Radium isotope ( Ra and Ra) in twenty three Na-Cl type saline waters obtained
from deep wells around the coastal area of Ishikawa Prefecture, Japan, were measured
along with U isotope (,-2U and ,-.U), major chemical components and hydrogen and oxygen isotope ratios. The waters sampled were the mixture of local meteoric water andseawater, including fossil seawater in origin from the relationship among dD, d+2O and Cl
and chemical composition. The ,,0Ra concentrations in water samples varied in the wide
range from +.12K,+.- mBq/kg, and occurrence of saline waters having high concentrations over -1* mBq/kg was conﬁrmed in some of them. The ,,0Ra concentrations showeda trend increasing with the increase of TDS in the water samples. The ,,2Ra/,,0Ra activity
ratios (*.2-K..3) of water samples were comparable to or slightly higher compared with,-,
Th/,-2U activity ratios of common rocks in Japan. The ,-2U concentrations of water
,,0

,,2

+


 !"#$%&'()*+,-./0 3,-ῌ+,,. 12 ,34567,. + Low Level Radioactivity Laboratory, Institute of Nature and Environmental Technology,
Kanazawa University, Wake, Nomi, Ishikawa 3,-ῌ+,,., Japan.
,3-*ῌ2///   -+3*  , Faculty of Science, Toyama University,Gofuku, Toyama 3-*ῌ2///, Japan.
- 3,* ῌ +-3, 12 <6 +* - Faculty of Fine Arts and Infor 8
39:;
matics, Kanazawa Gakuin University, Sue, Kanazawa, Ishikawa 3,*ῌ+-3,, Japan.
.=>?@*+ABC!D 1-.ῌ2//- => =>EFG + HI ,  - J . Research Institute for Radiation Biology and Medicine, Hiroshima University, Kasumi, Minami-ku, Hiroshima
1-.ῌ2//-, Japan.

241    



 







samples were extremely low ranging from less than detectable to ,.*. mBq/kg. Theseﬁndings suggest that the main processes for supplying Ra isotope to water were probably
not by rock dissolution but by both a-recoil from Th isotopes and desorption reaction of
Ra isotopes from water-rock interface.
Key words : Radium isotope, Na-Cl type saline spring water, Deep well, Coastal area, Ishikawa
Prefectureῒῑ ! ,- "# Na-Cl $%&'()* +,#%& Ra - ,,0Ra, ,,2Ra './ U - ,-2U, ,-.U 012 &3-dD 45673- d+2O '8*9 dD-d+2O-Cl :;456<=2"# ()>,9 Na-Cl $%&? &@A& <A& BCDEFG@HIJ>,9
%&,,0 Ra ? +.12,+.- mBqῌkg DEK9 ,,0Ra ?LHMNOF@M
NOFPQHRS>,9 %& ,,2Raῌ,,0Ra T? *.2-..3* DEU G,#?!"OV ,-,Thῌ,-2U T@WXY#"#ZZM[ DEK9 %& ,-2U ?$\/% ,.*. mBqῌkg DEK9 ] 8^_"# %&Ra -? V&OF`D?ON 0/V'a Vῌ&bc /1deF Th - a f(/)g a *+456 Th -"#hi,9 Ra -L/j1*9,-*k/5U&lmno>,9@pq*9
rstsu : vwxy- ML Na-Cl $%  !   +ῌ ῏ ῍ ῐ ῎
z/?xv{ ,-2U |. ,,0Ra /}~ : +0** y xy ,-,Th |.,,2 Ra /.1/ y 456 ,,.Ra -.00 d xy ,-/U |. ,,-Ra ++..- d  .

 Ra -H1deF G,#-456T'0[FG@/5U 1&a2 Ra 3yZVῌ&*kO <"/ [YO4RH5#,Y9 6 Clark and Turekian,+33*

7/4[Y %&vwxy Ra -? vu{ ,,,Rn @8/, Nakai, +3.* ; 92ῌ  +313 diD/ [N " ,,0Ra 'M/%&HR
S>,Y[F   +3// ; Kanai, +322 6:V1"#;SeF<= ,,0Ra : 0.,Bqῌkg ;   +3// 456¡ ,,0Ra : +.. BqῌL ; Kanai, +322 xv{%¢>£"#;S

eF¤? ,,0Ra : *.// BqῌL ;   +3// OH@'"O%DEF A ¥c/¦'Q§F@ 6 ¨©ª«rBL& ,,0Ra : ,1 BqῌL ; Behounek et al., +3-/2CA/DEeFL& ,,0Ra  : +,2 Bqῌkg ; Sturchio et al., ,**+ r¬ªF
G­H"#5#,FL& ,,0Ra  : /2 BqῌL ; Kraemer and Reid, +32. ®A¯IL&,,0Ra  : +, BqῌL ; Moise et al., ,*** O A&'?F"/ °FL' L&/$\/M Ra -HRS>,Y[F i9 2CAZr¬ªF¯I"#5#,
FL& ,,0Ra ?L@J[l:'IeG@K±>,Y[F Kraemer and Reid, +32. ;Sturchio et al., ,**+£L

!²³´M/5UNOZ ! "#A&Z<A&'µ¶@eF

ML Na-Cl $%H5#,F5g/OK9 6 ·¸# ,**1 ¹P 7/4
[Y ,,0Ra 'M/? ºW"»#,9D*"QR>,Y[O"K9H ¼½
242

" /2 # ,**3 Na-Cl  Ra $%&'() ,,0Ra *+)*,-./0123456;<=>?@ABC

783(, 9+$%&.:

(D)* Na-Cl % ,,0Ra 1D*%E

F+GH3(I,JKLMNOP( QIO R JD)* Na-Cl + S.@A
BCO Ra BTUVWXYῌZ[1\]^ Q_` abc@ABC%&.: 8
5de ,,0Ra 1D* fgOh( +!+*2 mgῌkg ij klmn%op3(, ,,0Ra +-1* mBqῌkg ij q r  ,**/ %EF1st^ uvwOJ abc@ABC Na-Cl  Ra *%x.:yz^ Ra 1D*%EF{|1 ,,0Ra *&}~ ,,2Raῌ,,0Ra klm4, 
,+  

^





abcB&}~ 0 BB 1 Q Fig. + a &}~ Fig. + b %2^
abc%J" ?1EF &}~ "&}~  +L ^:.( Fig. + a abcJ

BC,^:¡ :.(+ I J Oh(¢£?¤¥j%¦§L^:&e Qj%"?"&}~+L^:.(

Fig. + b¨©ª«J ,**/ ¬ 1 ­,**2 ¬ + ­% ':@ABC1®% ¯ ,- B%&Fig. + (a) Geological map of Ishikawa Prefecture, Japan, with sampling sites of Na-Cl type saline waters andriver waters, and (b) geological cross-section at six lines (A-F). These maps were compiled based on
Kaseno (+33-) and Ohwada et al. (,**1).

243   











 Fig. + a  ! +,*** m "#$ %&''()*+,Table + -./0! 120 3 0 4056 *+/ 7 89:;./< =) /!>?@"A !9#$B$%/CDE&* ,*-* L @A F(-'G(5)H!*+
IJK&'@A  pH !L *,M>-.A N/0 !OPQRSK1T>23A UV4>WMX,ῌ, ῎῍῏ῐ

UV4>WMX YM 5 ,* L : RaῌU />0  >67Z:[\
pH : + ]^>A ,-,U N89_`aba?cd Fe- efgha:[\ 5 , :i[;Aj

<=>A ?> hJklh:[\ pH :5 , >@AA Ba, efgha Bm> Ba, :.3, mg nCD NH., SO. Eo:[\ , :iFGj p'>hJklh:[\ Eo:H

I>A Ra ?cd U JqK:F(r( BaSO. ?cd Fe OH- sLM>c,t8A Fj u
vJwaxyJ?cdzNO>c, BaSO. n Fe OH- LP:t8A Fe OH- :{7Z>E|A }~>c, BaSO. n U PKxyJ:OA t8A BaSO. ! QR>?;0** A STj gR`JU>VW>XYA  =>j Z Ge $T:0g [QK__ga>c, ,,0 Ra ?cd ,,2 Ra 6Z:.TAH Ra JqK-\6Z)H! ]^ ^-.4\SKPJ Ge $T:0-.A Hamajima
and Komura, ,**. QK_aIa! NBL _`  No. .,ῌ+ ..*.῍-U No. 13 +.*+῍Th ?cd KCla b" >c,BA ,,0Ra ?cd ,,2Ra 6Z! F(r( ,3/ keV ,+.Pb

-/, keV ,+.Pb 0*3 keV ,+.Bi ?cd --2 keV ,,2Ac 3++ keV ,,2Ac c[W>c$A ,,0Ra 6Z:d*-../)H ,+.Pb ?cd ,+.Bi e*+/ Rn ,,0Ra d -.1T&'f-gp(/- Saito et al., ,**,

hM*< ,,0Ra

6Z! +20 keV  Ra niA?, Rn f!5n:mjA/ 7,,0 Ra t89! BaSO. t89nkAn 5A t89lB: ¡m Ba

a!A¢A¢ Ra JqK*£np(/< Yamamoto et al., +323 ; Inoue and Komura, ,**1 U
V*! Ra JqK£no57Zg¤ Ba NO-, ,,0Ra : 1.0,.* mBqῌg-Ba, ,,2Ra : $¥¦]^ 7!Wpq Barite, ,,0Ra : *.1*.+ mBq/g-Ba, ,,2Ra : *.,*.+ mBq/g-Ba, Inoue andKomura, ,**1 :efghanA0 Wpq! Na,CO- r|>c,stA Ba,efgha:@AA h }o U PKxyJ! E3xgv:|./< wJ§ava>¨
A HF, HNO- ?cd HClO. uv:A ©w: +* N HCl >E|A ª«O¬­aw­:0
Exy$>c, Fe :z®Aj ¯ª°J±²{³vP¤M>c, U :OῌstA Fj stA U JqK: |QwJ`Q} >Q~A Si K$T:0 a [
QK__ga>c,.TA ´µ ,-2U ?cd ,-.U ¶PJK`·­! F(r(*.+.-*.*.2 ?cd *.+02*.*/+ mBq *+ UV*!

H ,-2U ?cd ,-.U T-¶

PJK`·­ - ]^)H $¥¦]^nA JqKc dD ?cdZ JqKc d+2O ! F(r(¸x:0 ¹
Q  º M ?cd V ZN 

¹Q  º M>c, 3 .J q KcT/  Micro Mass Prism

model>c,-.A Ohsumi and Fujino, +320 ; Epstein and Mayeda, +3/- -.! _` V-SMOW JqKc&'» d  nA9  *A dD ?cd d+2O -.sZ! F(r( , ?cd *.+ *+/E3N Li, Na, K, Mg,, Ca,, Cl, Br, SO., !ª°JK¼_P½a244

% /2 & ,**3 Na-Cl  Ra 

Dionex ICS-+*** '()*+,! -./0 *+1 *.+ M HCl 2345+6789!

- 
-+ Na-Cl 

Na-Cl *+:; pH, <=>?@A" dD B(C d+2O 2 Table + 'DE!  pH 1 0.0#2.+ 7" FGH7I9! <=>?@A*+:;JKLMNOKLMPQRM
S ῌcationῌanionῌῌcationῌanion in meq L+ 1$+*ῌ TU7I9! VWXYZTable +

Chemical and isotopic compositions of Na-Cl type saline waters and river waters

Well
No. Sampling
depth pH
date(m)
Na-Cl type saline water+a ,1ῌ1ῌ,**/+,** 14*+b +1ῌ.ῌ,**0043,a ,1ῌ1ῌ,**/+,** 14+,b +1ῌ.ῌ,**0
14- +ῌ2ῌ,**/2** 140. +ῌ2ῌ,**/+,* 043/ ,3ῌ1ῌ,**/+*** 14*
0 ,3ῌ1ῌ,**/+-** 14/
1 +ῌ0ῌ,**1++0* 142 +ῌ0ῌ,**1+/** 140
3 +ῌ0ῌ,**1
3** 14,+* +ῌ0ῌ,**1+*** 14+++ 2ῌ0ῌ,**1+,** 143+, 2ῌ0ῌ,**1+-** 141+- 0ῌ0ῌ,**1+*** 14,+. 0ῌ0ῌ,**1+/** 140+/ 0ῌ0ῌ,**1+**+ 14++0 0ῌ0ῌ,**1+,./ 24++1 0ῌ0ῌ,**1+001 14/+2 0ῌ0ῌ,**1/** 140+3 1ῌ0ῌ,**1+*** 14+,* 1ῌ0ῌ,**1+/** 040,+ 1ῌ0ῌ,**1+,** 14*,, 1ῌ0ῌ,**1,** 14.
,-a 1ῌ0ῌ,**1+/** 043,-b -*ῌ+ῌ,**2
14*River watern.a.
R+ 1ῌ0ῌ,**1
R, 2ῌ0ῌ,**1
14n.a.
R- 0ῌ0ῌ,**1n.a.
R. 0ῌ0ῌ,**1
R/ +2ῌ+*ῌ,**/14*+.ῌ++ῌ,**/143
Sea water*,

Li

Na

K

Mg

Ca

Cl

Br

SO.

(mg/kg)Alkalinity(meq/L)

dD

d+2O
()

Balance*+(ῌ)

1,4*
1,4,34,34*
3/4+
124*
+*.
+-.
,*+2*
.34/
1.40
1-4/
114/
+./
++*
-04,
+.4.
+*/
+243
-*40
,3/
,,2
+-,
+,2
+,3

,241
-+41
,+4/
+242
34++
.4,,
,*4,
04+/
242+.4.
1243
/.41
3/4*
--4,
+-41
+,*
+.*
*403
,31
,-4,
0*4,
.-2
3*3
+,40
-*4*
-*4.

++3. 2/-2 ,14, 3-1++2* 2-., ,14. 3/*
12. /1-+ +24/ +,0.
102 /1++ +342 +,1.
,-, --1, ++40 0*3,+++ 2/.0 ,24+ ,/2,+/ -23. +-4. -41*
104+ .0/, +/4/ ,4.3+,2 0*1+ ,,42 n.d.*.
1.4/ --/0 +.4/ n.d.
,-+ ,-2+ 04/0 ,0.
+-2 /2*1 ,14, ,43+/241 -.-- ++42 .12+*. --2, +-4- ,,43/.4/ ,+./ +-4. n.d.
323 1-/2 ,.4, 0-++3 ,,-2 14/, ,0*+3.3 2./0 ,14- 0,3.1/ 0.3- ,,4* 0.++/4/ -.+ +402 0*4*+,++ +-+/+ .+4/ +++1/.0 +.*12 .-4/ +++1+**. +/.,3 /*4- +0-+
,1*- +*231 -/4, +/.
--33 +-02/ ./41 .+4,--,, +-.3. ..4- .,4,

*403
*403
*401
*401
*432
*4.2
,4..4024-0
+04,
,4**
+-4*
,4,.
+.41
-*4.
-4//
*43/
*4-2
-42,
-423
*42*
+4.1
+4**4-*
*4,1
*4.*

-.42
-.4*
.+43
.*4/+4.
-34/+4.
.34-340
/+4+
.24*
-34.
.14+
.04/,42
-041
.+4+
+040
-14*
/-43
+-42
34/
++4,
,+40
+-4+
n.a.*/

/40
04*
04/
040
14/
04/
143
14/
14*
240
24041414/
24.
04/
14+
/40
0434*
.4.
,40
,40
/4*
.41
n.a.

*4+
+4,
+4*43
,40
+4*
-41
*4+
+4/
+4+
*4,
*4*
+41
,4*
*4+4+
*4+40
,40
-4/
*4.
+4+
+4,
*4/
*4.
*4+

n.d. ++43 +4,1
n.d. +-4. +43*
*4*+ .+40 .4/n.d. +-4, ,4,*n.d. 04-3 *423
n.d. 0433 *43*4+2 ++*-/ -3+

,43+
,4,3
-4//
,4+/
,40.
,42/
+--1

04+- ++4, n.d.
04-- +-42 n.d.
14-+ -+43 *4+0-42* +-4* n.d.
+.42 /4+. n.d.
+04+ 04*/ n.d.
..+ +32/. 0241

*4/.
*4/,
+4,/
*4.0
*40.
*413
,῍,4.*-

./4* 24.
..4. 24+
.042 24*
.24. 240+42 342
0,42 +*4+

24+
04/
*4+
,4.
34,
-4,

*4/*4//
*4,*
*4+2
*4,2
+4.*4,+*4+*4/*
+4+0
*4*1
,4**
*4*/
*412
,4+0
+41,
*4*,
*4+.
*4+,
*4*,
+4*1
*4.0
*4+0
240++40
++4/

./,2
./01
-.31
-.2+
,,33
--+3
,.-1
,3.1
-311
,-22
+,02
-10+
,-*0
,.+1
+3**
-2.1
++22
-1.,
-03*
,3+
10-2
2,33
2*03
.***
.3*3
.131

-401
.4*/
,*4.
/42/
+,4,
+/4/
,120

*+ : Cation/anion balance(ῌcationῌanion)/(ῌcationῌanion) in meq L+. Density of water was assumed to beequal to unity in this calculation.
*, : The data set was referred from Isshiki (,**/).
*- : The concentrations of carbon species (HCO-, CO-,, CO,) were expressed in mM.
*. : “n.d.” denotes “not detected”.
*/ : “n.a.” denotes “not analyzed”.

245 

       !") #Total Dissolved Solid, TDS ; *+,-./0123456789:;<=$ - +ῌ,1 gῌkg,>?=%
Na-Cl @A B8 dD CDE d+2O - FGHG&/.'&+*( &3.*'&,.0( ,>?=% I=

JK<=LMB8 dD CDE d+2O - FGHG&0-'&..( &+*.+'&2.*( ,>?=% Fig. , #a$ 1
dD-d+2O 8NOPQR% ST8UB- V01 dD2d+2O+* #GMWL$ 1WXYZ[G\]#Craig, +30+$ *+,JK<=LMB- GMWL D^_`a1WXYZ[G=% bG-cd

aef8gB8hiPjklm\=n,>^ #opῌq +32- ; Mizota and Kusakabe, +33.$
b8rs8V0tUBu #LMWL : dD2d+2O,*$ ;_vw<tm #Mizota and Kusakabe,+33. ; Bxῌ +331$% yz78A B8 dD CDE d+2O - {|}1F8rs8LMBD^~mPQ< 1UBP ;R\A B,-tm% A B8 PR\=n1
dD-Cl  #Fig. , #b$$ CDE d+2O-Cl  #Fig. , #c$$ 8NOPWXYZ<=% F8 yz

78A B- F8rs8UB;dB8u81WXYZ[G rs8UB;dB8
,>\b;]Q[G=% z8#No. +0 +3 ,, ,-$ - Cl ]~m1_}}| r

s8UBuI=-FGD^_`a1WXYZ[G= #Fig. , #a$$% b8Dt-ῌ
t8ῌ8rB #;  +320 ; | ,***$ cd¡¢£¤¥B #Brumsack
et al., +33,$ 1Cml_¦§[Glm\% Fig. - #a$ CDE Fig. - #b$ 1 Br-Cl CDE SO.-Cl 8

Fig. , The plots of (a) dD-d+2O, (b) dD-Cl and (c) d+2O-Cl for Na-Cl type saline waters obtained from coastal
area in Ishikawa Prefecture, Japan. Gray solid circle ( ) shows SMOW (Standard Mean Ocean Water).
The solid and dashed lines in Fig. , (a) show LMWL (Local Meteoric Water Line, dD2d+2O,*) and
GMWL (Global Meteoric Water Line, dD2d+2O+*), respectively. Dashed lines in Fig. , (b) show mixing
lines of seawater and local meteoric waters.

246

/2 ! ,**3

Fig. -

 Na-Cl  Ra 

The plots of the relation of (a) Br-Cl and (b) SO.-Cl"#$%& '()* Cl + Br ,-*./ 0&123456

789):;<=>?1@A BC89)DEFG4<HI6*JJ Cl + Br HK$L@M4NOP+O?1@ SM  +322 Fig. - a *%>TU*   BrῌCl V,

@+QR
WX

*.**-/ +YZ[\456 Cl + Br ,WHK45@I+<%]/ @ ^ '4, W SO.ῌCl V *.+. T6_`a*b1\$%> Fig. - b I , H
K+O@W<Bc*def [gA?1@I+*T@ hi2jk456 Yamanaka

and Kumagai, ,**0 8lWHK45@+QR@ 7^6

mn4op>q, W 8lW * >?1@
-, Ra  ,,0Ra, ,,2Ra 

U  ,-2U, ,-.URa  ,,0Ra, ,,2Ra U  ,-2U, ,-.U rstjk$ Table , *%& Buvwx<

*71?,ycz{_ Table , *%>  ,,0Ra |T} ,,2Ra r
+.12,+.- mBqῌkg |T} ,.**.,3, mBqῌkg +1\$%> s>TU,X ~* ,,0Ra $r -1* mBqῌkg M * <.> Fig. . a

mn4



\,   Ra : +.2* mBqῌL ; Kanai., +322 0  Ra : //* mBqῌL ; 
,,0

,,0

+3// *> I ^4/ ?1 R "B

 ,,0Ra : 2. mBqῌL ; Nakano-Ohta and Sato, ,**0 0 ,,0Ra : ,2, mBqῌL ; ῌSM +313 T6_1 Fig. . a > > X

/ ?1@q Ra r\+V@+ + ,,0r, ^4*, b1

 ,,2Raῌ,,0Ra V, *.2-..3* 45 I\, "B4 Raῌ Ra V *.1,./ ; Nakano-Ohta and Sato, ,**0 +

001\

,,2

,,0

45 Fig. . b Ra  ¡K,¢£zl45@+QR@< ¤ ¥)O¦

z|T}§z4, ,-,Thῌ,-2U V ¨$©t&@+ ,,2Raῌ,,0Ra V+ª>1
, X ~*..,.3 *.2,., Miyake et al., +31/ 45@ Fig. . b ^ No. ,, *|1?«¬­®¯°±G / +/+** m $ / m ²7o>_  UῌTh$st>+I³ ´z|T}µ¶z l·u¸µ¶z ¸µ¶z µ¶z jµ¶z  ,-,Thῌ,-2U V, X ~*.+3*.-- *.+,+.*. 45 ¹ º»¼½ No.

,,  ,,2Raῌ,,0Ra V, ,.+1 456 Izl ,-,Thῌ,-2U V+V
247






Table ,

No.

,,0
Ra
(mBq/kg)     !"#$

Concentrations of Ra and U isotopes in Na-Cl type saline waters
,,2
,,2
Ra
Ra/,,0Ra(mBq/kg) activity ratio

Na-Cl type saline water+a-/,+,*+ +,1++-3+b-03+*+,33+-3,a,+00
0/.1*,b,*.10*100+412*4,* ,4***4.2.
/,4/+42 ./4*.42//40,*42* ,-4/,43
0040.*403 24.2+40,
1.*4++4+ .243,4320343+40+*+03+*4*+4. +/4+,4.
+*
0,41,4/ 034-.43+++*43+4* +340,4,+,+30/30+/++-341+42 -04--4,+.
,*2,.*.+0.,+0+/,,4++4/ .040-41+034,1*431 ,241,41+1,.4.+40 -+40-4,+2.4,,*4/, -4/**42.
+3--1+.
032.1,*+030-3,,.
,++14,+4, .04--40,,+311.,1,0,-a,+.-.*.,3,+1.
,-b+3+0,+-32/+00
Sea water*- +4*/,4/- *4-214+.

-40+*4.+-4/,*4-3-4*,*4-.
,432*4-.
+4+-*4-**420*4+*.4+2*413+4,2*4,2+4,,*4*2+4./*4*3+4/,*4-,+4++*4*3+42**4,0.43**4,3*43+*4*3,4***4++,4++*4,,-4*3*4.+4,3*4+0*42-*4,,,4*1*4+0,4-+*4+0,403*4,2,4+1*4+/,4***4*3,4*2*4*3*4,+,432,-2
U(mBq/kg),-.
U(mBq/kg)

n.d.*,
n.d.
n.d.
*4*+0*4**.
*4*+.*4**-*4*.1*4**1*4*+/*4**.
*4*.+*4**0*4*.**4**0*4*,.*4**.


,4/+*412+403*4/*

n.d.
n.d.
*4*+/*4**- *4*-,*4**.
*4*,-*4**/n.d.
*4*+1*4**n.d.
*4*,,*4**- *4*/**4**.
*4+/0*4*+, *4,.2*4*+0*4*+3*4**- *4*,/*4**.
*4*,1*4**. *4*/-*4**/*4*/1*4**/ *4*3+*4**1*4*-,*4**. *4*00*4**/*4*3-*4*+* *4,,**4*+1*4*0-*4**0 *4,*-*4*++n.d.
,4+1*4/3

,4,2*4.++4/3*4+0+4-,*4,3+430*4-++4/3*4+3,4*.*4-+,4-2*4-,-4,**4-0

n.d.
+4/+*4*0,4*.*4+**4+0+*4*+,*4*--*4**.
*4++2*4*+**4*,1*4**.
*4*+1*4***4*.3*4*+0.*41,4/n.d.
,42.*4+1+4+3*4*2
0400*4/3+402*4,0-43-*4-3+4,2*4,+4/,*4-/+4-1*4.1+4+.*4*-n.d.
.4,3*4+1,4.,*4+++4*1*4*/*4*/0*4**/*4.0.*4*,.
*4*-.*4**.
*4*,/*4***4*00*4**1,-.
U/,-2U
Geology*.
activity ratio

Tertiary
Tertiary

Tertiary
Tertiary
Tertiary

GraniteTertiary
Tertiary
Tertiary
Tertiary
Tertiary
Tertiary
Tertiary
Tertiary
Granite*+ : Error shows +s standard deviation from counting statistics.
*, : “n.d.” denotes “not detected”. Detection limit is three times of blank level (see text)*- : The data sets of Ra and U isotopes in sea water were referred from Inoue et al. (,**1) and Ku et al.
(+311), respectively.
*. : The geology was referred from stratigraphic column of each spring.

)*!+",- ,,2Raῌ,,0Ra ./0123345678)%!+",9- ,-2U :;2 <=>?@A&,.*. mBqῌkg *BCDE:;78FG% Fig. / D ,-2U:;* Cl -HIJKL% !+",MN, 'OPN,( *Q,-RST78)U*VW ,-2U M,X
9DYZ[\]5)*L)* N,῎Q,RS^D_`ab[\)U*Mcd[\)% eVefM
W Q,-ghMij5 No. +2 Jkj Ll]-!+",2N,῎Q,RS^mnAD_`ab[\ 'Fig. /( U M,XVWko[\]5)U*MKp[\)% qrD Qs,972 U tuv
2wOxyz72{Z|- UO,, '῍( 3}-~w*e]ZL)M xyz72{|- UO, 'ῌ( *e]ZL)* W\]5)% eG!+",2eGmDwMj)mfxyzD[\]5)U*MKp[\ U tuv2{|- UO, 'ῌ( *e]248

/2 ! ,**3 Na-Cl  Ra 

Fig. . Distributions of (a) ,,0Ra contents and (b) ,,2Ra/,,0Ra activity ratios for Na-Cl type saline waters obtained from coastal area in Ishikawa Prefecture, Japan. Gray shaded area () in Fig. . (a) shows theconcentration higher than -1* mBq/kg in ,,0Ra. Gray solid area () in Fig. . (b) represents the range
of ,-, Th/,-2U activity ratio of common rock (granite, basalt) in Japan reported by Miyake et al. (+31/).

Fig. /The relationship between ,-2U concentration and Cl.

"# $%&'()*+,-.)/0. ,-.Uῌ,-2U 12345 +.+30.00 )67-89:; <=,12>?89:. + @A9:+ B 5 a CDEF&G. ,-.U HIJKLMF9:.)/0. N0O Kigoshi, +31+ ; Yamamoto et al., ,**-

249

     

--  Ra!"#$%& '()%&&*#+,- Na-Cl ./0123! +- Ra 456789:%-0;<=>?$;&%$@A# /0B



C#DE1 dD-d+2O-Cl -FG%& H-I-0$J1KLM&*#N0 OPN0 $-QR1DSTUV*!2S H*&-,BW1N01>?$XY&*? C%C Z=N0- ,,0Ra B +- mBqῌkg $ Table ,, Inoue et al., ,**1 [S N0\]- Ra 
45-^B_"? # `a-N0- ,,0Ra B%B@3; ,,0Ra- bc +0** yBd!@efghijXY?$k1"l KLM&*##e-N0- ,,0Ra Bmn1
o$C!3? +- Ra 4560p1%:#M1B qr]$C! bc-&3stu-<=;'([S ,,0Ra 6qr>?#M1Bstu[? ,-2U ...1+*3 y ,-.U ,../+*/ y ,-*Th
1./+*. y - ,,2Ra 6qr>?#M1B ,-,Th +..++*+* y -<=;'v[? C#;A!
Ra 45BwPῒ0pxy)1DA!zY{0p|qrV*!3?$XY&*?

0p|- Ra 45-*}1:3!B W1 ῌ +<stu Th 45 -o$ ῍ wP-+~
῎ wP- Th 45 Ra 45-stu - a o$1,E a -. ῏ wP/J wPῒ0

12? Ra 45-01-;XY&*!3? 2Y Sturchio et al., ,**+
--+  Th

{

,,0

Ra 2D

[?; Th B .

,,2

 

Ra -stu[?+< ,-*Th 2D ,-,Th -o$1D? Ra 45-qr-3+[S 4!1-0B51[? 

6& +33+ C#;A! +<stu Th 45 -o$1D? Ra 45-qrB_"?$XY&*?
--, 

1 Ra 45;wP-+~1DS0p|qrV*?R1:3!7>? 8@9-f0%wP-:Jῌ;6<?=;>0[?% V&1/0- 1D?
0-?@X@> "(;[?; B A$C!N0 OPN0 6\]$>?/0;J1 1KLM&*!3?B@¡ ¢¡ 6£>? # wP+~1DS0p|C¤V*# Ra 45Bn!0p|%<V*?$>?$ H-¡D- Ra 45-ef$OB¥-DE1/V*? 2Y Tricca et al., ,**+
Awrrῌ+nῌwRaῌRaArῌ+elRaῌtῌrwῌnῌlRa+*-Ra¦-§123!

Aw r n wRaRaῐAr lRa B H*¨*0- Ra 45 mBqῌkg ERa© gῌcm- fF wP- Ra 45-+~ª s+ wP- Ra 45 mBqῌgRa 45-o$« s+ 6/C GY¬- w 2D r B0p2DwPp6/> w,,0Raw,,2Ra [?$C!­®6£>?$ 0p- ,,2Raῌ,,0Ra C¯HE ,,2RaAwῌ,,0RaAw

B
Awῌ,,0RaAwl,,0Raῌl,,2Raῌ,,2RaArῌ,,0RaAr

,,2Ra

*.**-0 ,,2RaArῌ,,0RaAr῍*.**-0 ,-,ThArῌ,-2UArῑ$@? ῐ §123! wP- ,,0Ra  ,-2U  fF ,,0Ra +~ª6$OV°?$0p- ,,0Ra B"l$?V°?$;" &*#+- ,,0Ra BwP-+~1
DA!±>?$Bk²H[? C%C Ra 45;W1wP-+~1DA!0p|qrV*!3?$>?$ ῑ §1³>DE1 ,,2Raῌ,,0Ra C¯HEB51l@? 2Y I-´/!@µJw2D¶KwB ,-,Thῌ,-2U C¯HEB H*¨* *..,.3 *.2,., Miyake et al.,+31/ [S Th 7LM;+3·¸¹º»VY¼ ,-,Thῌ,-2U C¯HEB 2.. [? Nagai et al.,,**0 :S wP-+~B 0p- ,,2Raῌ,,0Ra C¯HEB ­® ½¼ *.*- N
250

! /2 " ,**3#$% &'#
4

 Na-Cl  Ra  ,,2Raῌ,,0Ra ( )* +,- . /0*12356  ,,2Raῌ,,0Ra (6/0 ,-,Thῌ,-2U (4 :;< &'#=>46 ?8 @A7BC+,- . :HI9 @A ?87BC*7)89- 4

DEFG*,-:**

JK-6 LMN8

4JK-;<1OP /0Q6RST -C Kraemer and Reid, +32. UV/0Q
8H- Ra W6X9K*YZ
---

-

a 

Ra 6[\]#$- Th  a ^8H%_. -# a 8H- Ra 

`abcNdefg#$-*YZ- h.# a &'6i8j ,-.Uῌ,-2U

(k8lE$Jf1m*no#$p Zq Kigoshi, +31+ ; Yamamoto et al.,,**- [\]#$- Th  a ^8H%`arT  Ra 1sJ`8 t

T -*u!,-* a 8H- Ra "vAw6xyHI8#T - Kraemer,+32+
Aw-rrῌ+nῌLῌThArῌ+elRaῌtῌ.rwῌnῌr+*-ῌRa::# L,Th

Ar, r 6 z {Ra |$ % Th  Ra [\] (" mBqῌg %&} cm E#, ῌ ~8KJ /0 %  ,-*Th " A
' %&}EwT-*` ,,0Ra "6P(,- Zq rr,.0 gῌcm- rw
+.* gῌcm- n*.+ L,+*0 cm ,-*ThAr-* mBqῌg r*.*+ cm )* E ῌ ~8 +,-* !8KJ ,,0Ra "6 +*/ mBqῌkg *T - . # r*.***,cm Zq,-9o .6 ,-*ThAr-** mBqῌg 8,-* !8KJ ,,0Ra "6z {/,0/ mBqῌkg, +*/- mBqῌkg *f- .% a 8H-# Ra "

1P9-C86 %)}E,-%HI8TK .6 a 8H% ,,0Ra 1 2`arT I-/0 .6% #? ,-*Th 1"#$- $-K6z./#$-01$- /# !8KJ ,,2Raῌ,,0Ra ( 6Awῌ,,0RaAw῍,-,ThArῌ ,-*ThAr

῍

,,2Ra

*#- ῍ ~1

9HI8 a 8H-`a Ra #6 !8KJ/0 ,-,Thῌ,-*Th ( *24P9- Zq #394/H5/#6 z {* ..

,.3 H *.2,., .% &'# ,,2Raῌ,,0Ra (*.2-..3* 11

#$-
--. ῌRa 6NM-6  Ra ῌ

8 4 738D9o¡"K¢£#6t*

9T JK-1 Zq Moore, +330 8¤¢£¡"9K¢£ ¥¦ῌ§9o #6 Ra
69"#$% surface reactive element *YZ

JK- Zq Tricca et al., ,**+ ,,0Ra"* TDS ¨©E Fig. 0 8ª, Fig. 0 8ª,HI8 ,,0Ra "* TDS A86 q 
6Kf ¡"1P9-* ,,0Ra "fP9-«¬1rT  :014/ ­;/ *YZ- No. +,, ,-, Table , 6 ,,0Ra "* TDS ¨©8KJ/8®

¯°±T - Fig. 0 738 ¡"19K¢£#6O²<³´µ1/0#?¶=·³±
8¶=,-1 ¡"K¢£#6²<³´µ1¶=·³±8¶=4O²<³´µ1`arT -*YZ

JK- Ra 6 `#1 Ra, *4JtV4JK-*YZ

J% Sturchio et al., ,**+ , ²#tV,- Ra 6 ¸<³´µ*¹<º8H% ¡"9K#6/0#?¶=·³±8>»38¶=4 ¡"K#6`8rT -*YZ- Kraemer and Reid, +32. /0 .6%  UῌTh ¼?@½
251    

Fig. 0    The relationship between ,,0Ra concentration and TDS.

 pH  !"#$% Herczeg et al., +322 &'()*+,-./)011

2

345+67 ,,0Ra 89 TDS 1:1;<. => ? =>ῌ@AB (C) Ra DEF1G
HῌI JK1L8MNOPQR-QS L8TUV@4/)W' Ra DEF.@;( XY6)Z9[\]^) Z1_` @;a1 ,,2Raῌ,,0Ra bcd.=> ?1DEFd[
Je^)9fg+6)
--/Ra 

hijQ-7Z9k+ ,,2Raῌ,,0Ra bcd1lmk+ Na-Cl nV@a1 Ra DEF.
o(=> p7.V?1 Th DEF1 a q(rs a Jt(SuvY6 p7 ,,0Ra-TDS

1<wk+ Ra DEF8.o(L8MNO1GHῌI JK => ?1 Th DEF1 a q(Sxp67 Ra DEF1I JK0yz ({|Y6Q)Z9T}~Y6) i7s(Ra DEFT a Jt(SuvY6)_` V@a1 Ra DEFTU84/)7(. Th

DEF[yzVT1s&TY&V4/)k p7.=> p7.V?1 Th

DEFTU84/) /). 11T/) . V@T^)?ῌ
(.=>ῌ@JK(SxY67VTyp6Q)Z990& (,Q.
&T&Y6Q) g* Tricca et al. ,**+ . @a1 Ra  Rn 8[^)(. 1=>1(S@;Y67 Th T=> ?(Q)O[ p7 Sturchio et al. ,**+ . L@a1U81 Ra DEF[^)7( =>1
(S @;a(Y67O1 Th DEFT=> ?(ῌ87? Th isotopeenriched surface layer 1O[Q) Z1 Th 8?.&¥¡p4(¢£1l¤.

1¦§¨©Tª1«¬4/)T => ?(1s&1YVTN¡

1=>1(S@;Y67 Th DEFT 6+(U8(yp6)9fg)9
2345+67V@a1U Ra 80­c4/)9fg+6)

. 



®¯°± k+5+6)UL81 Na-Cl nV. Ra DEF[U8(yz14.&k91²14 >³´µ¶·(m¡^)®¯°± [yz¸ ,- m1 Na-Cl nV@
1 Ra DEF[¤¹7 º»7V@. dD-d+2O-Cl 1<wk+¼@p7.!>¼@[R½
252

! /2 " ,**3#$%&#' Na-Cl  Ra #() ,,0Ra *+,- ,,2Raῌ,,0Ra ./0 1 2+.12,+.- mBqῌkg+,- *.2-..3* 345 6 7895 Ra :;*<=>'?@A  ,,2Raῌ,,0Ra ./'BC ,-,Thῌ,-2U ./#D

EE;FG34%&#  ,-2U 'H<I*34%&# J KL0LFM ,,0Ra *# TDS
N<OP'Q&# O Ra 0 BC RS,T(UVWF X<?@$% ,-,Th +,- ,-*Th  a Y < T a^?_`

a<,5BCZ +,-BCX3[\A Ra ]*Ob cW dF%&#'efW gh0 <,5iW  Ra *:eAjk3(l mn<+k%._opqrstu#(%gh34% ovw Pu (x0 \yN?z
.Y <,5 Ra <(%{ gh3

|}0 ~@#()dF%;

._mX <>gh#AdM34%#
῏

%

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