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TRANSCRIPT
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Abstract
241
Faculty of Science, Toyama University,
OMITA ATAKE ASAKI AKAGUCHI
NOUE AMAJIMA AMAMOTO
stitute for Radiation Biology and Medicine, Hiroshima University, Kasumi, Minami-ku, Hiroshima
Low Level Radioactivity Laboratory, Institute of Nature and Environmental Technology,
Kanazawa University, Wake, Nomi, Ishikawa , Japan.
Gofuku, Toyama , Japan.
Faculty of Fine Arts and Infor-
matics, Kanazawa Gakuin University, Sue, Kanazawa, Ishikawa , Japan.
Research In-
, Japan.
J. Hot Spring Sci.
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 ( U and U), major chemical components and hydrogen and oxy-
gen isotope ratios. The waters sampled were the mixture of local meteoric water and
seawater, including fossil seawater in origin from the relationship among D, O and Cl
and chemical composition. The Ra concentrations in water samples varied in the wide
range from . mBq/kg, and occurrence of saline waters having high concentra-
tions over mBq/kg was confirmed in some of them. The Ra concentrations showed
a trend increasing with the increase of TDS in the water samples. The Ra/ Ra activity
ratios ( . . ) of water samples were comparable to or slightly higher compared with
Th/ U activity ratios of common rocks in Japan. The U concentrations of water
Junpei T , Hiroshi S , Keiichi S , Aya S ,
Mutsuo I , Yasunori H and Masayoshi Y
Radium Isotope in Na-Cl Type Saline Waters
from Deep Wells around Coastal Area in
Ishikawa Prefecture, Japan
Na-Cl
Ra
+
+
, ,
- -
. .
,,0 ,,2
,-2 ,-.
+2
,,0
,,0
,,2 ,,0
,-, ,-2 ,-2
+ , - .
+ + +
+ , - .
+ + +
3-* 2/// -+3*
,* +, ,, ,+ , +3
3,- +,,.,.
3,- +,,.
3-* 2///3,* +-3, +*
3,* +-3,1-. 2//- + , -
1-. 2//-
/2 ,.+ ,// ,**3
+ 12 ,+.--1*
* 2- . 3
d d
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242
Radium isotope, Na-Cl type saline spring water, Deep well, Coastal area, Ishikawa
Prefecture
samples were extremely low ranging from less than detectable to . mBq/kg. These
findings suggest that the main processes for supplying Ra isotope to water were probably
not by rock dissolution but by both -recoil from Th isotopes and desorption reaction of
Ra isotopes from water-rock interface.
Key words :
Na-Cl
Ra Ra, Ra U U, U
D O D- O-Cl
Na-Cl
Ra . mBq kg Ra
Ra Ra . .
Th U
U . mBq kg
Ra Th
Th Ra
: Na-Cl
U Ra : y Th Ra . y
Ra . d U Ra . d Ra
Ra
Clark and Turekian,
Ra Rn
Nakai, ; Ra
; Kanai, Ra : .
Bq kg ; Ra : . Bq L ; Kanai,
Ra : . Bq L ;
Ra : Bq L ; Behounek
Ra : Bq kg ; Sturchio
Ra : Bq L ; Kraemer and Reid,
Ra : Bq L ; Moise
Ra
Ra Kraemer and Reid, ;
Sturchio
Na-Cl
Ra
et al.,
et al.,
et al.,
et al.,
,,0 ,,2 ,-2 ,-.
+2 +2
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Fig. (a) Geological map of Ishikawa Prefecture, Japan, with sampling sites of Na-Cl type saline waters and
river waters, and (b) geological cross-section at six lines (A-F). These maps were compiled based on
Kaseno ( ) and Ohwada ( ).et al.
243
Na-Cl Ra
Ra
Na-Cl Ra
Na-Cl
Ra
Ra mg kg Ra
mBq kg
Na-Cl Ra Ra
Ra Ra Ra
Fig. a Fig. b
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Fig. a , m
Table
L
pH
L Ra U
pH U Fe
pH Ba Ba :
mg NH SO
Ra U BaSO Fe OH
BaSO Fe OH Fe OH
BaSO U BaSO
Ge
Ra Ra Ra
Ge Hamajima
and Komura, NBL No. . -U No. . -
Th KCl Ra Ra keV Pb
keV Pb keV Bi keV Ac keV Ac
Ra Pb Bi Rn Ra
Saito Ra
keV Ra Rn
Ra BaSO Ba
Ra Yamamoto ; Inoue and Komura,
Ra Ba NO Ra : . . mBq g-Ba, Ra :
Barite, Ra : . . mBq/g-Ba, Ra : . . mBq/g-Ba, Inoue and
Komura, Na CO Ba
U
HF, HNO HClO N HCl
Fe U
U Si
U U
. . . . mBq U U
D O
Micro Mass Prism
model Ohsumi and Fujino, ; Epstein and Mayeda,
V-SMOW D O
.
Li , Na , K , Mg , Ca , Cl , Br , SO
et al.,
et al.,
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Table Chemical and isotopic compositions of Na-Cl type saline waters and river waters
245
n.a. n.d. n.d.
n.d. n.d.
n.a.
n.a. n.d. n.d.
n.d. n.d.
n.d. n.d.
Well Li Na K Mg Ca Cl Br SO Alkalinity D O Balance*Sampling
No. depth pHdate
(m) (mg/kg) (meq/L) ( ) ( )
Na-Cl type saline water
a
b
a
b
n.d.*
n.d.
n.d.
a
b n.a.* n.a.
River water
R
R
R
R
R
Sea water* *
* : Cation/anion balance ( cation anion)/( cation anion) in meq L . Density of water was assumed to be
equal 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”.
Na-Cl Ra
Dionex ICS- . M HCl
Na-Cl pH, D O Table
pH . .
cation anion cation anion in meq L
Na-Cl
+
+2 +.
.
/
, -
+ +
,
- ,- - ,
.
/
+2
+
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+1 . ,**0
,1 1 ,**/
+1 . ,**0
+ 2 ,**/
+ 2 ,**/
,3 1 ,**/
,3 1 ,**/
+ 0 ,**1
+ 0 ,**1
+ 0 ,**1
+ 0 ,**1
2 0 ,**1
2 0 ,**1
0 0 ,**1
0 0 ,**1
0 0 ,**1
0 0 ,**1
0 0 ,**1
0 0 ,**1
1 0 ,**1
1 0 ,**1
1 0 ,**1
1 0 ,**1
1 0 ,**1
-* + ,**2
1 0 ,**1
2 0 ,**1
0 0 ,**1
0 0 ,**1
+2 +* ,**/
+. ++ ,**/
14* *4/- 1,4* ,241 ++3. ,14,
043 *4// 1,4- -+41 ++2* ,14.
14+ *4,* ,34- ,+4/ 12. +24/
14- *4+2 ,34* +242 102 +342
140 *4,2 3/4+ 34++ ,-, ++40
043 +4.- 124* .4,, ,+++ ,24+
14* *4,+ +*. ,*4, ,+/ +-4.
14/ *4+- +-. 04+/ 104+ +/4/
14- *4/* ,*- 242- +,2 ,,42
140 +4+0 +2* +.4. 1.4/ +.4/
14, *4*1 .34/ 1243 ,-+ 04/0
14+ ,4** 1.40 /.41 +-2 ,14,
143 *4*/ 1-4/ 3/4* /241 ++42
141 *412 114/ --4, +*. +-4-
14, ,4+0 +./ +-41 /.4/ +-4.
140 +41, ++* +,* 323 ,.4,
14+ *4*, -04, +.* ++3 14/,
24+ *4+. +.4. *403 +3.3 ,14-
14/ *4+, +*/ ,31 .1/ ,,4*
140 *4*, +243 ,-4, +/4/ +402
14+ +4*1 -*40 0*4, +,++ .+4/
040 *4.0 ,3/ .-2 /.0 .-4/
14* *4+0 ,,2 3*3 +**. /*4-
14. 240- +-, +,40 ,1*- -/4,
043 ++40 +,2 -*4* --33 ./41
14* ++4/ +,3 -*4. --,, ..4-
+4,1 ,43+ 04+-
14- +43* ,4,3 04--
*4*+ .4/- -4// 14-+ *4+0
,4,* ,4+/ -42*
14* *423 ,40. +.42
143 *43- ,42/ +04+
*4+2 -3+ +--1 ..+ 0241
+ +,** ./,2 2/-2 3-1 *403 -.42 /40 *4+
+ ./01 2-., 3/* *403 -.4* 04* +4,
, +,** -.31 /1-+ +,0. *401 .+43 04/ +4-
, -.2+ /1++ +,1. *401 .*4- 040 *43
- 2** ,,33 --1, 0*3 *432 /+4. 14/ ,40
. +,* --+3 2/.0 ,/2 *4.2 -34- 04/ +4*
/ +*** ,.-1 -23. -41* ,4.- /+4. 143 -41
0 +-** ,3.1 .0/, ,4.3 .40- .34- 14/ *4+
1 ++0* -311 0*1+ 24-0 -340 14* +4/
2 +/** ,-22 --/0 +04, /+4+ 240 +4+
3 3** +,02 ,-2+ ,0. ,4** .24* 24- *4,
+* +*** -10+ /2*1 ,43+ +-4* -34. 04- *4*
++ +,** ,-*0 -.-- .12 ,4,. .14+ 14- +41
+, +-** ,.+1 --2, ,,43 +.41 .04- 14/ ,4*
+- +*** +3** ,+./ -*4. /,42 24. *4-
+. +/** -2.1 1-/2 0-- -4// -041 04/ +4+
+/ +**+ ++22 ,,-2 ,0* *43/ .+4+ 14+ *4-
+0 +,./ -1., 2./0 0,3 *4-2 +040 /40 +40
+1 +001 -03* 0.3- 0.+ -42, -14* 04- ,40
+2 /** ,3+ -.+ 0*4* -423 /-43 34* -4/
+3 +*** 10-2 +-+/+ +++1 *42* +-42 .4. *4.
,* +/** 2,33 +.*12 +++1 +4.1 34/ ,40 +4+
,+ +,** 2*03 +/.,3 +0-+ +4*- ++4, ,40 +4,
,, ,** .*** +*231 +/. *4-* ,+40 /4* *4/
,- +/** .3*3 +-02/ .+4, *4,1 +-4+ .41 *4.
,- .131 +-.3. .,4, *4.* *4+
+ ++43 ++4, -401 *4/. ./4* 24. 24+
, +-4. +-42 .4*/ *4/, ..4. 24+ 04/
- .+40 -+43 ,*4. +4,/ .042 24* *4+
. +-4, +-4* /42/ *4.0 .24. 24- ,4.
/ 04-3 /4+. +,4, *40. 0+42 342 34,
0433 04*/ +/4/ *413 0,42 +*4+ -4,
++*-/ +32/. ,120 , ,4.
,**/
/2 ,**3
+*** * +
+
0 0 2 +
+*
- +
-
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d d
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Fig. The plots of (a) D- O, (b) D-Cl and (c) O-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, D O ) and
GMWL (Global Meteoric Water Line, D O ), respectively. Dashed lines in Fig. (b) show mixing
lines of seawater and local meteoric waters.
246
Total Dissolved Solid, TDS ; g kg
Na-Cl D O . .
D O . . Fig. a
D- O D O GMWL
Craig, GMWL
; Mizota and Kusakabe,
LMWL : D O Mizota and Kusakabe,
; D O
D-Cl Fig. b O-Cl Fig. c
No. Cl
Fig. a
; Brumsack
Fig. a Fig. b Br-Cl SO -Clet al.,
+2 +2
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+2
,
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+2
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.
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2 +*
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2 ,*
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, ,
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,
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Fig. The plots of the relation of (a) Br-Cl and (b) SO -Cl
247
Na-Cl Ra
Cl Br
Cl Br
Fig. a Br Cl
. Cl Br
SO Cl . Fig. b
Yamanaka
and Kumagai,
Ra Ra, Ra U U, U Table
Table Ra Ra
. mBq kg . mBq kg
Ra mBq kg Fig. a
Ra : mBq L ; Kanai., Ra : mBq L ;
Ra : mBq L ; Nakano-Ohta and Sato, Ra :
mBq L ; Fig. a
Ra
Ra Ra . .
Ra Ra . . ; Nakano-Ohta and Sato,
Fig. b Ra
Th U Ra Ra
. . . . Miyake Fig. b No.
m m U Th
Th U . . . . No.
Ra Ra . Th U
et al.,
Ra Ra, Ra U U, U
.-
.
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,
,
+ 12 ,+.- , ** .,3,
-1* .
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+3//
2. ,**0
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+ ,
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.
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+/ +** /
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,, , +1
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Table Concentrations of Ra and U isotopes in Na-Cl type saline waters
248
activity ratio activity ratioGeology
n.d.
n.d.
n.d.
n.d. n.d.
n.d.
n.d.
n.d. n.d.
Sea water
Ra Ra Ra/ Ra U U U/ UNo. *
(mBq/kg) (mBq/kg) (mBq/kg) (mBq/kg)
Na-Cl type saline water
a * * Tertiary
b
a Tertiary
b
n.d.
Tertiary
Tertiary
Tertiary
Granite
Tertiary
Tertiary
n.d. Tertiary
Tertiary
Tertiary
Tertiary
Tertiary
Tertiary
a Granite
b
*
* : Error shows 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 ( ) and Ku
( ), respectively.
* : The geology was referred from stratigraphic column of each spring.
Ra Ra
U . mBq kg Fig. U
Cl U
No.
Fig. U U
UO
UO
U UO
et al. et al.
,
,,0 ,,2 ,,2 ,,0 ,-2 ,-. ,-. ,-2.
+ ,
-
+
,
-
.
,,2 ,,0
,-2 ,-2
,-2
,,
,
,
-/, +, +,1+ +-3 *4*.1 *4**1
-03 +* +,33 +-3 *4*+/ *4**.
,+0 0 0/. 1* *4*.+ *4**0
,*. 1 0*1 00 *4*+0 *4**. *4*.* *4**0
+412 *4,* ,4** *4.2 *4*+. *4**- *4*,. *4**.
/,4/ +42 ./4* .42
/40, *42* ,-4/ ,43 *4*+/ *4**- *4*-, *4**.
040. *403 24.2 +40, *4*,- *4**/
.*4+ +4+ .243 ,43 *4*+1 *4**-
0343 +40 +*+ 0 *4*,, *4**- *4*/* *4**.
+*4* +4. +/4+ ,4. *4+/0 *4*+, *4,.2 *4*+0
0,41 ,4/ 034- .43 *4*+3 *4**- *4*,/ *4**.
+*43 +4* +340 ,4, *4*,1 *4**. *4*/- *4**/
+30 / 30+ /+ *4*/1 *4**/ *4*3+ *4**1
-341 +42 -04- -4, *4*-, *4**. *4*00 *4**/
,*2, .* .+0. ,+0 *4*3- *4*+* *4,,* *4*+1
,,4+ +4/ .040 -41 *4*0- *4**0 *4,*- *4*++
34,1 *431 ,241 ,41
,.4. +40 -+40 -4, +4/+ *4*0 .4,3 *4+1
.4,, *4/, -4/* *42. ,4*. *4+* ,4., *4++
--1 +. 032 .1 *4+0+ *4*+, +4*1 *4*/
+03 0 -3, ,. *4*-- *4**. *4*/0 *4**/
+14, +4, .04- -40 *4++2 *4*+* *4.0. *4*,.
+31 1 .,1 ,0 *4*,1 *4**. *4*-. *4**.
,+.- .* .,3, +1. *4*+1 *4**- *4*,/ *4**-
+3+0 ,+ -32/ +00 *4*.3 *4*+0 *4*00 *4**1
+4*/ ,4/- *4-2 14+. .*41 ,4/
+ -40+ *4.+
+ -4/, *4-3
, -4*, *4-.
, ,432 *4-. ,4/+ *412
- +4+- *4-* +403 *4/*
. *420 *4+*
/ .4+2 *413 ,4+1 *4/3
0 +4,2 *4,2
1 +4,, *4*2
2 +4./ *4*3 ,4,2 *4.+
3 +4/, *4-, +4/3 *4+0
+* +4++ *4*3 +4-, *4,3
++ +42* *4,0 +430 *4-+
+, .43* *4,3 +4/3 *4+3
+- *43+ *4*3 ,4*. *4-+
+. ,4** *4++ ,4-2 *4-,
+/ ,4++ *4,, -4,* *4-0
+0 -4*3 *4.-
+1 +4,3 *4+0 ,42. *4+1
+2 *42- *4,, +4+3 *4*2
+3 ,4*1 *4+0 0400 *4/3
,* ,4-+ *4+0 +402 *4,0
,+ ,403 *4,2 -43- *4-3
,, ,4+1 *4+/ +4,2 *4,-
,- ,4** *4*3 +4/, *4-/
,- ,4*2 *4*3 +4-1 *4.1
*4,+ ,432 +4+. *4*-
+
,**1
+311
, *. /
+2
/
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Fig. Distributions of (a) Ra contents and (b) Ra/ Ra activity ratios for Na-Cl type saline waters ob-
tained from coastal area in Ishikawa Prefecture, Japan. Gray shaded area ( ) in Fig. (a) shows the
concentration higher than mBq/kg in Ra. Gray solid area ( ) in Fig. (b) represents the range
of Th/ U activity ratio of common rock (granite, basalt) in Japan reported by Miyake ( ).
Fig. The relationship between U concentration and Cl.
et al.
249
Na-Cl Ra
U U . .
U
Kigoshi, ; Yamamoto et al.,
,,0 ,,2 ,,0
,,0
,-, ,-2
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250
t
Na-Cl
Ra
D- O-Cl
Ra mBq kg Table , Inoue Ra
Ra Ra y
Ra
Ra
Ra U . y U . y Th
. y Ra Th . y
Ra
Ra Th
Th Ra
Ra Sturchio
Ra Ra Th Th Ra
Th
Th Ra
Ra
Ra Ra
Tricca
A n A e n
A n A Ra mBq kg
g cm Ra s Ra mBq g
Ra s
Ra Ra A A
A A A A
. A A . A A
Ra U Ra
Ra Ra
Ra
Ra Ra
Th U . . . . Miyake
Th Th U . Nagai
Ra Ra .
Ra Ra Raw r Ra r w Ra
Ra Raw Ra r Ra
Ra RaRa Ra w w
Ra Ra Ra Raw w Ra Ra r r
Ra Ra Th Ur r r r
et al.,
et al.,
et al.,
w r
et al.,
et al.,
Ra
Th
+2
,,0
,,0 ,,0
,,0
,,0 ,-2 3 ,-. / ,-*
. ,,2 ,-, +*
,,0 ,,2 ,-* ,-,
-
- +
+
,,2 ,,0
,,0 ,-2 ,,0
,,0 ,,0
,,2 ,,0
,-, ,-2
,-, ,-2
,,2 ,,0
+ - , ,**1
+0**
. .1 +* , ./ +*
1 / +* + .+ +*
,**+
.
+33+
,**+
+ + +*
* **-0 * **-0
* . , 3 * 2 , ,
+31/ 2 .
,**0 * *-
,,2 ,,0,,0 ,,2
,,2 ,,0 ,,2 ,,0,,0 ,,2
,,2 ,,0 ,-, ,-2
- -
- - +
- - ,
l
d d
a a
r w r l
r w l
w w
l l
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252
pH Herczeg
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Granitic and Basaltic Rocks in Japan. Proc. nd. Inter. Symp. Natural Radiat. Environ.,
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