UV J. Hot Spring Sci. /3 ,3/ῌ-+3 ,*+*ῌ῍ 
  !" #

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

Geochemical Features and Genetic Process of Hot-spring
Waters Discharged from Deep Hot-spring Wells in
the Miyazaki Plain, Kyushu Island, Japan :Diagenetic Dehydrated Fluid as a Source
Fluid of Hot-spring Water
Shinji OHSAWA+, Kazuhiro AMITA,, Makoto YAMADA+,
Taketoshi MISHIMA+ and Kohei KAZAHAYA-

Abstract
For identiﬁcation of diagenetic dehydrated ﬂuids as source ﬂuids of hot-spring water,
we conducted chemical and isotopic analyses of waters and accompanied gases collectedfrom hot-spring wells in the Miyazaki plain in the fore-arc region of Kyushu Island,
Japan. Interpretation of systematical relationships appearing among chemical and isotope data, and geochemical estimation of hydrothermal temperatures of hot spring waters revealed two hot-spring water source ﬂuids in existing groundwaters of meteoric
origin : squeezed pore water from marine sediments, and hydrothermal ﬂuid of unidentiﬁed generation stored in sedimentary rocks. Geochemical thermodynamic evaluation of
the unidentiﬁed ﬂuids using representative hot spring waters indicated a dehydrated interlayer water from clay mineral (smectite) at around +-*T. Furthermore, comparison to+ 21.ῌ*3*-  !"#$% + Beppu Geothermal Research Laboratory, Institute for Geothermal Sciences, Graduate School of Science,
Kyoto University, Noguchibaru, Beppu, Oita 21.ῌ*3*-, Japan.
,&'()*+)* *+*ῌ2/*, &'&'",-./ + 0 + 1 , Departmentof Earth Science and Technology, Faculty of Engineering and Resource Science, Akita University, +ῌ+ Tegatagakuen-cho, Akita *+*ῌ2/*,, Japan.
-23456789:;45<=>?@+9ABCD9EF+G@+HIJK?L
-*/ῌ2/01 MNOPQ"R + S + S + - Crustal ﬂuid research group, Institute of Geology andGeoinformation, AIST, Higashi +ῌ+ῌ+, Central-1, Tsukuba, Ibaraki -*/ῌ2/01, Japan.

295    







results of a geochemical analysis of accompanied hydrocarbon gases and a geologicalconsideration of genetic process of the source ﬂuids of the hot spring waters implied their
origin at di#erent stages during the burial diagenesis of marine sediments. An importantresult obtained from comparisons of the chemical and isotopic data on some geochemicalsystematic diagrams is that hydrothermal ﬂuid of hot spring waters in the Oita plain, also
located in the fore-arc region of Kyushu, apparently have a di#erent origin and geneticalprocess from hydrothermal ﬂuids of the Miyazaki plain.
Key words : Miyazaki plain, hot spring well, hot-spring water, geochemical feature, origin,
diagenetic dehydrated ﬂuidῒῑ !"#$%&
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N'S%& ij !"#$$J Ckl'D_TjI-`4 m1gngop[qr'<asE-. %&$JF=/RNIN'J=TU^%d*+
t8u8v : %& ,  4 GH R +ῌ ῏ ῍ ῐ ῎wI xTy4z{J|}=TKz#XT ~T,()C6L.+
~# A^M5+T WANJj WOJ PPF^Q=r RC6#Lc.+SN+X T}U +31- W+.Vj^$A/-= ~9$ T} W +32, }+Py{Akl*+ WU'J Ty49OXi.+M/FYZ$  'S*+^ D_*+R7klj
IT\[]^=-6- STJ [\ῌ']01kl/'*H^j-.^.+T - Hb^=iUV^S6 x=_6Skl`J.=-6- y4^ ¡N~9$klJaT=j DEzH¢£~jb@*+`J=.=-6  ¤PS`4 kl`3r¥.+UNS6^ T} P¦. +31. ; Takamatsu et al., +320 §¨01©ªc>b "=«d^2eT¬+^ ©ªf­&fJg=-6
 WCOkl^S h=-6Ui®J jC^z¦'S Ty4zQ$N zH^kXTKzH¯lTOUN
S6'SVO F=©ªJ jC°g[]±p[²³S±´8h8µvXTN¶CO' ·m~Tkl`^SN--.¸ T} Giggenbach et al., +33- W
kl¹º»8'kl^¼=TTO½n^S jC'¶O~9$C296

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Fig. + Locations of investigated hot spring wells () and sampling sites of river waters () withsurface distribution of concerned geologic bodies in this study : Miyazaki group and Shimanto
complex, and the Quaternary volcanic front (dash-dotted line) and some active volcanoes ().

298

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Table +

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Brief summary of hot spring wells

Well
No.

Depth ofwell (m)Depth of screen
head (m)Discharge
form

Discharge rate
(L/min.)*Discharge
temp. ()SiO,*
(mg/L)

+
,
.
/
0
1
2
3
+*
++
+,
++.
+/
+0
+1
+2

+1**
+,**
-*
.2*
+***
2**
+-**
1/*
+-**
-**
+0**
2**
+,**
+***
+-**
+/**
+,**
1ῌ2

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

pumping
pumping
self

self


self
pumping
self
pumping
pumping


self

,/*
/.3
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+/41+34./4.*.-4.
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1++
2*/
0.*
++/*
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.+*
-**
+*.

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+.0

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,,4,
n.m.
/*4.
.342
-/4*
.-4**
-14+04+**
,-41*

3/43
+24/

-+43
,34/
+241
--43
114/
0.4,04/

234,

+34-

Remarks) * Data referred from the public data tables (Onsen-bunseki-sho), ** The measuring site
is far from the well. n.m. : not measured$ % 

&'()*+,- Table + ./0$

%1 2 31* m

345 +*** m *67889&:&: ;8< %2 +1** m 34=$ >?.4=@A B,-C<
I9*

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No. /,

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No. +0 JP. yzno.f84[*/g0-< &~No. +

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299

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*., XD'YZ

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+® ¯'( %&B} *% D *% D° $`* [\]`* +±JQZ²³´oµ¶03 lQJ#µ¶#·¸0¹3W ºr]#» "¼*+p½Zºr

Table , Analytical results of collected hot spring waters and estimated underground temperatures ofhot spring waters
Well
Na
K
Mg
Ca
Li
Cl
HCOSO.
B
pH
No.
(mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L)
+
,
.
/
0
1
2
3
+*
++
+,
++.
+/
+0
+1
+2

14.
142
14.
240
143
24+
141
24.
24/
142

.3,*
-,.*
.12*
,+1*
,3/*
,*0*
.-.*
+/+*
+0.*
30/*

.14.
+/43
-24,
34+
,.41
+*42
,343
,42
-43
,.4+

+.42
,+4.
.+4.

n.d.
n.d.
3/41

300
2-41
,+.
*4.
,14,
++4++/40
142
,/.

,4*
*401
-43
.4.
,4/
+4+
,4+
*401
+4+
+4,

n.a.
1414/
143

n.a.
--.*
+2/*
.3*

n.a.
0/4*
,242
140

n.a.
++4/
+4*
-343

n.a.
0341
,34*
1,4*

n.a.
/4*
,42
*4.1

n.a.
14/
1414-

n.a.
-3/*
+*/**
//,*

n.a.
,142+4/
.,4-

n.a.
-4*
+/,
0.4/

n.a.
+40
-/+
,.-

n.a.
04+
+4/
.4,

n.d.
34,4*
-*4*

3./*
.03*
10/*
+1,*
-2/*
,,**
01.*
+//*
+13*
+0.**
,.-*
-/3*
+1+*
1*1
/*2*
,--*
+2/**
2***

.3
..1
...
,11*
++0*
+/3*
.01
+,**
+,**
+/0
n.a.
,3,*
,*,*
.,.
n.a.
0+1*
,,-,-

n.d.
+242
,*4,
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.a.
n.d.
n.d.
n.d.
n.a.
+//
n.d.
n.d.

.24.
.+41
+43
,,4,
+/*
1041
+/*
,*40
.*41
.43
n.a.
+33
2-42
34.
n.a.
,20
++4+
.40

dD
()

d+2O
()

q Na-K-Ca*
()

+,4/
,34*
,+41
-*41
+141
,,4.
+*41
-+40
-+4.4*,/4+.4/
,/4.
-241
342
04,
04+/4.

*4*.4*+
.4**
+43*
*4.1
+41,
,431
.4/*
.4,*43/
,4/+43,
,4.,
/431
-40.
.4*+4.3
-4-1

32
2.
+**
+*/
+*3
3,
31
0*
00
02

+-3
+,1
+*
+,.
+*0
33

Remarks) Sampling date ; Nos. +ῌ. : Feb. ++, ,**., Nos. /ῌ++ : Feb. +,, ,**., Nos. +,ῌ+0 : Feb. +-, ,**., No. +1 : Feb. +/,,**., No. +2 : Nov. +, ,**1, n.d. : not detected, n.a. : not analyzed, * : derived from the Na-K-Ca geochemical thermometer mentioned in Nicholson (+33-)

300

" /3 # ,*+*





Table - Results of isotopic and chemical analyses of
surface waters collected from rivers
No.

Name of river

dD
()

d+2O
()

Cl
(mg/L)abcd

Hitotsuse
Hirowatari
KiyotakeOhyodo

.042
.+4*
.+4+
..41

14-1
04/3
040*
043-

+42
/42
,34,
++40

Remarks) Sampling date ; No. a : Feb. ++, ,**., Nos. b andc : Feb. +-, ,**., No. d : Feb. +., ,**.

Table .

Results of chemical and isotopic analyses of gases accompanied with hot spring waters

Well
No.

CO,
(῍)

N,
(῍)

O,
(῍)

CH.
(῍)

C,H0
(῍)

C-H2
(῍)

d+-C CO,()

d+-C CH.
()

d+-C C,H0
()

/
0

+4*+
+4+0

24,.
.4.-

*423
*4,3

2342.
3.4*3

*4*,
*4*,

n.d.
n.d.

/4+
04-

./4,
.24.

,04-,41Remarks) Sampling date ; Nov. +, ,**1 for chemical composition and carbon isotopes, n.d. : notdetected

$%&'( )*$+,-./0123-ῌ+ ῏῔ΐῑ῍῎ῐῒ

4567891
1 Fig. , +K:;< =:;<>?@?ABC+DEFGHIJ

No. +  No. +. +LL MNOP?N 4 :;<QRSTUVW Na, K XYZN[\]XY^ =:;<A+_N^YZN  =:;<AC`,aQbc+de. SO. + H-ZXY^ fg?h-JNijk

N>lmn+o-.pqrVstuv+w ?IZ1KH.-N xaQ Cl + yJ dzs HCO- + yJ{X|I +Qi}~h5ZXY^
C=:;<AQ HCO-ῌCl d-+ .JIg?.- ho 4 :;<XYRSTUVW 32 ῍ C1 Na NPXQ Na-Cl  Na-Cl, HCO-

o >~H.bg?
Fig. - Q

 HCO-ῌCl d1 TDS '(.HIBXY B+Q Fig. +    j789  +313 JKH.YN A No. +*  No. +1 Q> jIXY^

6XKg?I Na-Cl c1 )*


Q

XYZ1¡Kg¢ £ dzs HCO- + y Na-Cl, HCO-jsh

+de.

+¤h-XY-¥ZN ZZX¦+ >XJ HCO-  Cl dN + +§-£¨1©xª«¬+Y

v+XY­® ~sh HCO-ῌCl dῌTDS ¯ 1K
No. -, No. 1, No. +2 DEFG°w1 >? jsh±H No. +, No. ,, No. +*  No. +1 %&X¥¥{±X²h- B+HI%&³°w'(1´µ h¶·v)*c+5o >?%&! XQ¸¹º^·1±ZNX²h-Z1K»H.- Z]Q ¼½XK°$A1|Z301

Fig. ,  

Major cation and anion compositions of collected hot spring waters in Fig. + with modern seawater.

Fig. - Relation between TDS (total dissolved substance) and HCO-/Cl ratio of hot spring waters
with brine waters at Sadowara area and modern seawater. For the location of Sadowara area,
black-star () in Fig. +.

302

/3 ! ,*+*





"#$%&'(-ῌ, ῏῍ΐ῎ῒῑῐ)*+, dD vs. d+2O -./012" Fig. . 34"5 66789:;<=>? @AB7CDE( HCO-ῌCl FῌTDS G -56H5I1J
 No. +, No. ,, No. -, No. 1, No. +2 -KLM75NJ O-PQRS TE(7UVW1J

 No. +*  No. +1 X OYZ[\D]O,^_"`ab

01HOYZ[\D] cI1JO7U6-5dN%efg hi(FjE HCO- "kl Na-Cl, HCO- mn
TDS G -5X CDE( HCO-ῌCl Fῌ No. +, No. ,, No. -, No. 1, No. +2 -opN%q%r sRS

-ftfuPvw"xy6Hz&NJ {C"|NJPvX}~"#
Pv7U 66"1JPv X 01 No. ., No. /, No. 0, No. 2, No. 3, No. ++,No. +,, No. +-, No. +., No. +/, No. +0 H sRSO"F% d+2O HdD e&"#$%N%e65dN%b )(

u

X dD

vs. Cl G  {w Fig. . 4 "21%e dD vs. d+2O { Pv"QNo. ,  No. 1 X dD vs. Cl G { Pvw"X( OYZ[\D] c

I1JO-RS No. +*  No. +1 4"1%e6  01&UeXsRS"#$%N%eq6H7M )(AX C
DE( HCO-ῌCl FῌTDS G -5
7Ub 
"F% d+2O H No. +, No. ,, No. -, No. 1, No. +2 "ue%2X sRS OYZ[\D] cI1JO Ou dD e& - -RS"N%eHe 7X 6AH 7U ¡¢ - £¤x89:-e%I"¥¦

Fig. . Relationships of dD vs. d+2O and dD vs. Cl of hot spring waters in Miyazaki with modern seawater,river waters in the study area, ranges of pore waters of marine sediments and andesitic volcanic
steam. For data points shown by open diamond (Nos. +, ,, -, 1 and +2), see text or refer Fig. -.
Ranges circled by dotted lines indicate formation waters shown by Kato and Kajiwara (+320).

303  

-ῌ- ῑ῔ΐῐ῍῎῏ῒ ! B " Li # $%$&'()*+ Cl "",(-./ Soluble groupspecies (01 234+*!567 8ῌ9:;<= ()*+ , >?@D"EFG4 Cl "",(8DHIJKLMNOPDQRS('AB2(C*,

G4+*! Giggenbach

and Goguel, +323 TU B-Cl DVWNXY# 8DZ 9DJK([7!"G4+) $%\]()2!$'^_C

G4!(VW`T4+*! ab c3+333 # Tdef( 8D BῌCl g(h*+ !"(i!
Fig. / # 8D BῌCl gA dD "jk 2+lmUn7! BῌCl g# o(,pqUrs( 8DZ 9At!uv7 Cl wxy +** mgῌL Aza!8(h*+# BῌCl g
{|g y*.+ D}N#~9( *.+*.*+ D}N# 9(Z G4+*U,D *.*+D8#':8Af8AHI"i!,D7!" G4! D dD vs. BῌCl gjkn
(G4U8D# oD8D0V/ dD vs. d+2O )r dD vs. Cl wxD
jknA *U3JKG4U/D8y ~9(Z G4+*U,D7!"Aumm NXY+ 4TD3CG4Urs( ~3G4U
8y$DHI8Dh"m+ ¡i!"y¢K?7!"Am+*! TU
HCO-ῌCl g TDS wx 8D0V/ Cl wxD£+()*+?@¤AmU¥D

8 No. +, No. ,, No. -, No. 1, No. +2 y ¦ , §DHI8"¨8HI$©8DMN(
rª+«/m+*!"¬+­U",®7!",m+*!
Fig. 0 #8D B-Li-Cl D;¯V/AlmU,D7!y ,4T"@°±²³²´µ@jky¬+4! ¶· ~3G4U8AHI(i!"¸G
4U8 No. +* " No. +1 # ¹4"º»(jki! 8"",( Cl ¼½ »(

Fig. / Relation between dD and B/Cl ratio of hot spring waters with modern seawater. Discrimination for origins of hot spring waters by B/Cl ratio shown on Y-axis is done by means of an
authorized geochemical method described in Inuyama et al. (+333). For data points shown by
open diamond (Nos. +, ,, -, 1 and +2), see text or refer Figs. - and ..

304

# /3 $ ,*+*





Fig. 0 Relative B-Li-Cl compositions of hot spring waters with modern seawater. Theseelements are classiﬁed into “Soluble group species” recognized in Geothermal geochemistry (e.g. Nicholson, +33-). For data points shown by open diamond (Nos. +,,, -, 1 and +2), see text or refer Figs. -, . and /.

% &'()*+,-./0123-.145*67

 No. /, No. 0, No. 2,

No. 3, No. +,, No. +-, No. +., No. +0 8 9: No. . ;<= B >?@?AB*CDE FG

8HIJKL5M*NO-.0PQKR -* STUVW*X0/L Fig. /YZ-.45[\&']^_ `-.1[ST*aEb-.
1 No. +, No. ,, No. 1 8 B >?@?AB*CD45*67

Wcdefg

 Cl >?@?hi PaP*Oj% [\&']^_ `-.1[ST*ak/b
-.1 No. -  No. +2 8 Li >?@?AB*lmnopOj0PMqpr./0s01t*u.Sv;wx/0y3K=s0p zs{L45ST|}*8s0Q;~K=/0 s 9:%/~-.1 No. . *X0/8 Li >?@?
AB*lmnopOj0PQp%x. 45hlmnop *Sk/K=1LpK=-/ J9*ak/5%1;QQK9  aP*DtQ
pK=
o*8mn%/ lmno [\&']^_ `-.

1[ &'()*+,-./0145 - p% u.p!s
TKST%Rk/

pb%/0"uQK K8%/45;rEJ ub 5;¡k/
mn;¢/3-£10¤Pp H¥¦* o*Rk1¨©§ 23-.p *ª.«¬­®­¯d°s|}*X0/±² ³´µp305  




-ῌ. ῐ῎῏῍ῑ!"#$%&'&()*+,-%./0+ 123 Nicholson, +33- 45()*$(6 789+:;*<=*)>?8@/0>0A*+BCDE @F@ G*HEI/JKLMNO8DPQ>+RSLTU./0 !"# Na-K-Ca "#+E V
W X)Y8DP>0AZ[>@\]^$(0+ Q*"#_7I/ `ab
c*" dc" _#e@ Table , dD >*fg_h/i\*+ Fig. 1 DE Fig. 1 *j

Fig. 1 Relation between dD and the Na-K-Ca geochemical temperature of whole the hot springwaters (upper) and systematical relationships between them of selected hot spring waters(Nos. /, 0, 2, 3, +0 and Nos. +,, +-, +.) by previous data analyses in this study (lower).
For the data analyses and the selection, see text.

306

/3  ,*+*  !"#





$ %&'()*+,-.#/0.1234567 dD 8# # 9$:; <=$0>  ?@#:;AB#C+.D  Fig. 1 E#F= GH# $:;>I = GH#$  JK Fig. +, #LMN.0 > OOP# Q>I = RS

+312 ; T +32+ O No. +,, No. +-, No. +. O No. /, No. 0,
No. 2, No. 3, No. +0 #U )=V=&'(WXY4#N.Z[\5:;]^_`N )= ]#MN, aL# dD >bc$ L#>dc$ e0:;>I=  RR  R= AB> ?@#?@E>fgN.h
N.0 0Hijkg567  ?@> +** lm +-*

56 R]MnN.0 .!o5  po5"q>#b$7#F=,?@%  &#]r7 )=]' No. +,  No. +0 s&'(&(i%#G+. t)*u+8vt ,-w$ 56 R]MN .xyz{i%|}~sῌ+/0 )12#/0.

 )N.ZJ#  

> E#3"F= ?@&>M 4#5g

H ] 3

N Z_6 =,/]7$>   E#3"F= ?@&#/0.8$9]H
.+ 

po - o 5]:5b$ +,?@&]k;

GH

#$ 
+ *u#<=F= &56 , <t~t)*u+8vt#0  +2O #>D D #?N0- <t~t)*u+8vt#0. @>Ac B #>_B C t)]D5 = E Mud volcano ~)#:; =.0 wd& Geopressured hydrothermal system  #¡0. ¢ , £F

s]L/>G¤F=.¡7 *u+ῌ*u]¥+§/56 z¨(X4 SmectiteJ#,-¦ $HI

 =.0

K© Dia et al., +333 ; You et al., ,**. ; Xu et al., ,**0 ; L  ,**3 ; ª ,**3 z¨(X40*+/* #¡0.X«X4 Illite ¬MN­N Dählmann and De Lange, ,**- Fig. 2 #N,GH# ¥OAP56 ®8JQ¯#G+.>R F=  R> +2O #>D
D #?N0,I )]?@&~# )GH$S°4>XY1±Y

4F=  =.0  , z¨(X4®8LH§/4  *u²'±Y³´µ

8v¶T ·¸|} ¹ ,**3

Lº:F= GH# A 5

6 0HR567 ¢ - #5gN t)EE~*u+ CEU +:VAP#¡0.LSW$s>¤F=.0

K© Brown et al., ,**+ ; Dählmann and De

Lange, ,**- ; Haese et al., ,**0 ; You et al., ,**. $¡ Dählmann and De Lange ,**-HI+JQ¯»¼#H {½Q¯ K© Clay membrane ion ﬁltration,
Ash particle alteration, Bigogenic opal recrystallization, Anaerobic methane oxidation $
307 







 



Fig. 2 A modiﬁed schematic cross-section of smectite and illite showing the crystallographic
sites that hold Li, B and H,O originally illustrated by Williams and Hervig (,**/).

!"#$ Cl
4

Cl

%& '()*+,-./*)0 +2O  1 D 23 5)657895:6;<=8>)?$-@2*)

<A5B CDE#F-EG>HIJ5KL6!8 M'N + OPQRST UVWXYZ5[\6]2 KL6!5^
YZῌYaYZbc

+** _` 0UVWX

0*+/* 5dO?$R e/ UVWXYZ5[\65:6;I*!fg&J6EO$h?$8"#$i*j%EO$+/ kBEO
>lm An opHli$ egUVWXYZῌYaYZbc0qr2 UVWXYZ[\Hl:60K?I*)st5uE7vJ!EO?$0&wg& k?E x k&0''$j%HyBH-z{h
UVWXYZ$YaYZ-S|6(}'~ u -w2 6(}#5)-a
VX$hUVWXYZῌYaYZ5*-@hStability diagram -#2* k5

KL6!-+h6 No. +, $ No. +0 56X K Mg, Na H 5
) -Zh?$Ez,h$)BWU>-.-IJ
,.-Na-smectite+..K*./2Mg,+.13OH,.--illite*.,3quartz*.10Na*.20H,O??E UVWXYZῌYaYZ5*6(}#5)-TJT ~5-//010O k&8M'E^2J65-2)?$h0 k53N854N-G3h5E e ^ 54N5-rIJ 5
5-.$2*8 Na-K-Ca  <=5M' E6 - 2 6¡-7¢h$)B£¤IJ
8¥¦§¨¥¦§5©#95ªE«1>R58 UVWXYZῌYaYZ59
5¬ ­®¯90O  A°$$R9±­®¯ W®UZ²aYZ ³´5µ 'h$g&*) :/m Aoyagi and Kazama, +32* ; 6¶ῌ· +321 ; ¸;ῌu +33+
k&l5c 8¹<ºeI*)R5E8>)0 KL6!5^+** _` =E8³´0EO5E ¸;ῌu +33+ ; Kyser and Hiatt, ,**- ³´ -»I*
6 -^2 TJ Na-K-Ca   $7¢2J 7¢8 Fig. 3 @g&B 6 No. +, ()*8 Na-K-Ca  0 +-3 5$?¼ ³´ 8 +,. 6
No. +0 ()*8 Na-K-Ca  0 +,. 5$?¼ ³´ 8 +-+ $ 6¡5½8 +* > E
308

# /3 $ ,*+*





Fig. 3 Comparison between estimated hydrothermal temperatures by various geochemical
thermometers using chemical data of hot spring waters (Nos. +, and +0) closely related
to a source hydrothermal ﬂuid inferred to be derived from dehydrated inter-layer waterfrom clay mineral (smectite).

%& '()*+,-./ 01 234567
ABCDA

8EFG;<=+( 4EFG;<=89:;<=

5T

'&U( V 4RMW0X0Y,-

9ZHI[\4'& ]^_`a4'[b41cde
24ij50-kl2Q>m Zn+-*ft-24+p +-*

8>%?<@

8HIJKLMNO,P+,%Q R)*Q505S
f +** gh84'Y,opqr



sX

41c@u?vDAῌDCDAwrxyfP3 Stability

diagram f Fig. +* 4PQ @u?vDA

DCDAz{|Q}~45M

mixed-layer clay mineral  f,_42f wr 3Z4>

p@u?vDAῌDCDAwrxy5% fL,1(`Q}4+,-/ wr3Z4Ap] f¡
5 +-* No. +,  No. +0 ¢£

>8¤ 5 ¥¦@u?vDAῌDCDAwrxyZ4§¨+,1& RV] Q@u?vDA© ª >%25R«M>50--¬J
K0Yp
2'¬4 RV] Q@u?vDA© ª >%5­®>%Q¯¬>%0 °S±V+,-0-Z² !-" 4% B-Li-Cl ³Z>´µ_4 B 4¶-¬·f¸'¬4±V>m 4-,¹+,º25»¼>% Fig. 2 4N
309

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



Fig. +* An evaluation of hot spring waters (Nos. +, and +0) closely related
to a source hydrothermal ﬂuid inferred to be derived from dehydrated
inter-layer water from clay mineral (smectite) on a stability diagram ofsmectite and illite at the estimated hydrothermal temperature : +-*and stability boundaries of smectite and illite at ,** and -**.

 ! B " #$%&'()*!+,-./0123 B OH- 4567 '8'(9!)*:;<!=>0?: H,O =@A! < BCD#$%&'()*!
E Li "'FG4EHI '8'(9!JH?> K =BC !)*! KLMN=

OPQ @  Cl "R'FG4EHI ST(SUVT( ;+,;-WX)*!"LYZ!DD )*![X\"]^D0=OP 7H_? #$%&'()*`Q;a:b_ B-Li-Cl cde4fgh! B !ij="h!>k7

j=4E

L l;0m-Pj=_4n=OP., 



o No. / = No. 0 `Qpq7Hrs#;9ῌBtbuT& Table . - vwx9
 4!" Bernard y CH. ; d+-C = CH.ῌC,H0C-H2 #;z{y e!|}~(7H>;- Fig. ++ !N By!"  Igari and Sakata, +323 ;   +330 !
  $%;w4&QHs#;uT&>|}~(7H j; Bernardy" s#!K9:;M;ῌῌd0;'hῌ9h;()Hj=_4nwx9h* y;@¡4Eo No. / = No. 0 ;:" #$%&'()*`Q;a:b-=N@¢;>;!
K_ Q;rs# 9: "v';+£!?¤d7H>;4EL Thermogenic ¥4¤d7H>;_¦§¨©X7nH=£ª B,09ῌBtbh-«".¤';¬"4¤7H>; Microbial _$&G­9-WX>¤C _ Table . ! ! ®5N CO, ; d+-C _ CH. ;=nD¯0j=`Q ;°/±"² $%w4&Qs#;uT&>o No. / = No. 0 ;rs#=BC!m4n $%w;:>KH#$%&'()*`Q;a:b-=N:4E= j==³h4E @  ´µ¶·'*¸´:E";¹º-»DWXH:_0NwMw4&Qs#;9:" Fig. ++ ;|}~(t¼`Q ½=7.¤' Microbial 4Ej=_1Zq310

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Fig. ++ Relation between d+-C of CH. and CH./(C,H0C-H2) ratio of accompanied gasesof hot spring waters expressed on the Bernard plot, which is generally used for discrimination of origin of CH. and interpretation of undergoing physical and chemical
processes of hydrocarbon gases. Data of Sadowara, Shintomi and Nichinan are citedfrom Igari and Sakata (+323) and Igari (+330).

#$%&' () CH. *+,-.

*+/,-'01234 5*+6/789:;<=>?'@ABCDE F' GH'. 6IJ*+ CH. .
KLM*+ CH. %NO ῌODPLF4Q-B RST Claypool and Kven-

volden, +32- ; Judd, ,**. , UV*+/PL',-CWBCXYF4 Z[

\]D^_:;CYF4.- 



`ab'%cQ d'efF4*+/'. ῌ ghijMkl%Nm

F4g squeezed pore water from marine sediments 'no KLM*+ CH. pq&^ ῍ rstM uvwxyz {k|'no dehydrated inter-layer water fromclay mineral : smectite 6IJ*+ CH. pq&^ , UVCf}8]F4~ B89p Q ij'3DJF4 release of water from pores and hydrous minerals ; Kyser and Hiatt, ,**- '01234_&

DWBCF4 _BD BBD. B43Q _4'?-QJp
Fig. +, . , UV
No. +0 d'3*+/p_44
Na-K-Ca¦§ *+¨'~ CH. L*+/p'2

B'
 No. +*  No. +1 % No. +, '%¡7¢ uvwxyz῎y£yz¤¥¦§p 

©ª'q&{kl«¬ ­'%_0123Q~^DW ijMC®¯'?4Q Z!'kl«C°d _4311 







 



Fig. +, Estimated hydrothermal temperatures of hot spring waters of Nos. +, and +0 () and hot springwaters of Nos. +* and +1 () closely related to source ﬂuids inferred to be derived from dehydrated
inter-layer water from clay mineral (smectite) and squeezed pore water of marine sediments, respectively, roughly connected to temperature ranges of smectite-illite transformation and CH. generation,
and average changes with burial depth on porosity and geothermal temperature in the Neogene argillaceous sediments of Japan with present-day geothermal gradients at Miyazaki and Nichinan areas.

 !" #$ %$ &'()*+,-".$ /01 23.$ .4"$&56 01 7'-"8 9&/ 4":;<=> CH. ?/@A 01?B@&5-C/!"..DE%.F;7GB.$DH;'IJAKLM$NO"&5PQ R$ST US;Q$& #$ .RST4V>WXY-"
Z[,-"? \X]!" 4V>^_`abcῌbdbcef?gh6ij k2.$l.4".$ /?i'6 01 23m$23.nOVKDH$.&opqrV>stZ[,-" Y,?X]A>uk23?vwxOtO"y k2l.N?z
NO6 8 $:4" CH. $ /<=> B.{tDH$nO" CH. ;7GL
$.N?01u Y-"hO6 h-?. No. +, | No. +0 $g}N
OV>s"Z["h?&p" B01 2346 ~Y-"B.;g}!"N !
"AK. No. +*  No. +1 $! #-- 02 +*0 ? ^_`abcῌbdb
cf|/ g} CH. $/@,"Y-"#46Lt h$$$? %&Os?
L/*0* &&56 01 $2&%A>sOsKj +=Ls?',-KZ["h?&p"  No. +*  No. +1 $R #-- -** m,+1** m ; Table +  &$;($)  +32+ ,!!" #-,/ 0, O6 #QZ["$A>*+&5"[Os$4Q B01 2346 ~Y-"B.;g}!".N$!!p$JY->s"$$ $g}.N$@6, @ ;01-$9&gh"
@&$  o.=>¡/!"h?&p 0¢£&¤¥?/,OVK , ¦1$g}
.N?B@01 $@&$nO"^§¨©&ª@Y-K$&5"«2D?Lsh;¬t­®A>s" ¯°-OVK? Fig. . dD vs. d+2O ± dD vs. Cl 3$²³± ­AK$´$ T4ῌµ¶ +320 ?·¸01-$¹5ῌ6º»^.¼.|½7 $.$g}
312

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῏!"#$%"&'()*+,-"#./ 0 formation water -1"&234
5 67289:;<=>(?3@A7&B῏!CACDEA7FGH4
IJ7
.. 



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῏0BT

UVWX  1YN/ O CZ[ D C\"]^_EB,`" abcd
+2e  d+-C fg B e h Li e  dD C`7fg  6^_EB5ij῏!Ck῍]Ol,mn"& Fig. +- H 6opqrC4stV<34 dD
vs. d+2O fg,῏!,x-A7&

'()2Cu"&234 E

vwB

yz!{ |}+['()~ H 3`"& 0 j῏!,vwB῏!67N/2 D C\"]]O5
4/ PQ ,**/ opl53NO " "  6NO<`CV<2muA7#./ ῌ ,**3 6:  dD ]Hvw],
 CH</ E

2 0 j῏!,vwC`l23<]lH<] 6l3 ll3H 6}C# "¡ῒ,¢£"#[lCFig. +. H E

vwB῏!,x-, dD vs. Cl fg¤¥3¦§"&234 E |}+['()~ H  0 j῏!,vwB῏!,x-C¦M Cl e 5 / ¨©^© ªῑ<]"#$«7 .. + ¬32LM&NOC ^ Cl e
3 E



0H­®3<]

vwB῏!2¯& 0 j῏!Ck῍CH°

῎54 ±² ³Y5 ῐ´ῐCµ#./ 6NO<¶·30j5
vlFG2<©H<]5 6¸¹ yz!{i dD º  d+2O »¼ H½ª3

Fig. +- Comparison between water isotope compositions (dD vs. d+2O) of hot spring waters in Miyazaki(in this study) and Oita plain (by Amita et al., ,**/) with modern seawater and ranges of source ﬂuids
of hot spring waters recognized in this study and metamorphic ﬂuids.

313

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



Fig. +. Comparison between hot spring waters in Miyazaki (in this study) and Oita plain(by Amita et al., ,**/) on the correlation diagram of dD vs. Cl with modern seawaterand ranges of source ﬂuids of hot spring waters recognized in this study.

 Cl  !"#$% Cl &'()&*+ ,- ./!0% Cl "1
234563789+:;

&  <=!>?@6A ()B2

6C;D2E;FG HI <=!>2&?@6JK()23B2K
G L7%M8NO)B2&E;" PQK B-Li-Cl RST?UV+WKX"YZ)23B26[\E ]Z"^_()B2K`abKcdA 6ef)B2K()
Fig. +/ & Fig. 0  B-Li-Cl RST?UVghijklmn HI <=!>6o()!6pE q ,**/ KrstZ)  !ughi6v
wxmEF+L)   !& B-Li yKz3{|2 Cl-B yKz3{|K:8 ,tZ)B2" }) QWK~()! q ,**/  Oita-*- Oita-*. Oita-+,& -" ()  KL)}qtZF+L% ,- ./!2 !>K()ikv;} ,- ./!!}q
!>K $)?+?EFikv;}&}+&;" ?!>K()!L)!+L)B26^_E) ; BB26>T? Fig. +-  dD vs. Cl¡U Fig. +. }q¢"£;}¤F& BZq!"¥!<=¦'!O6§8¨£)}q+L) { B-Li yKz3{|!K&<=!>6o()!"©7Z)" #ª«¬ghijklm LiῌB $K­%"¢qZ) BZ& ®U LiῌB $2 dD  ¡K^tZ)03K ¥!<=¦'!OYZ+L)2¢)B
2"+:   1¯ <=!>&&'?+() !>0% Li K(°B2"±²+L)2³f]3+L) P  %;1´ ?µ¶·)K*¸tZ)>*+K` ] B-Li-Cl T?"¹tZ º»q ,**3 ; Sengen et al., in prep.
B-Li yKz¤F 6E ±K ?1T?"  1¯ <=!>

]ZK,¼()B2" }¤:F 7F q ,**/ +&½ZqZ;" B-Li yKz¤
314

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Fig. +/ Relative B-Li-Cl compositions of hot spring waters in the Oita plain (by Amita et al., ,**/)
compared with modern seawater and ranges of source ﬂuids of hot spring waters in the
Miyazaki plain. The attached ﬁgure shows relation between dD and Li/B ratio for hot springwaters in Oita having relatively high B and Li contents. Grayish thick long allow presumablyshows a compositional change path on generated ﬂuids from diagenesis to metamorphism.

"#$%&'()*+

1 2"3 4 5 6 7

,**3 ,- Oita-*+  Oita-*, ./689:'; <=ῌ>? +302 @A8*BC 6 DEFGHI2;
 MNOP* 68Q

0

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8oU:';FU" ef.FHI2" MNPBo7
OF i7T8}E;7 (ef79:;F.Z 
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Mazzini et al., ,**1

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4Qg=>0  @noKd 'b'c : K*.0/ Al,.* Al*.0/ Si-.-/ O+* OH , ;< : Mg, Fe, Al 0
Si, Al . O+* OH 2  B"7H@pS4 C5!"@Dq !"# A!i;< +** km rE/B7qB#QS" A!i F, ,*** ; Schmidt andPoli, +332  G7!"&ps!"S%dH2I GtJ0KL

u<> B 7 Li vK0wqLxFG&My"#Q& (Marchall et al., ,**0 ; Bebout etal., ,**1  <=>,FGz@N{0OdP#S0=\Q G7!"@psqQ|}R'@SqT ! <4Q ,ps!"&G7
!"%S@TU[#i 9tJ"GtJ0V~W`:XYq7!"0Z; ['G;&\_#QS A!i B-Li-Cl ]^_ Fig. +/ 0`45=>
M;]G; evolutional change  ^_ab0 Cl 0c!"" B 0c!"@

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pῌlpu2"  The stable isotope Laboratory, GNS Science Limitede-eb()  89; ῌ2" <vwsX  xFGy_# 89
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²³b´ : µ:¶GKH( @LQMy5 w·¸0¹4_ºῌῑῐ῍   ¨© ,**/ : ,/0#B#} Yps  // 0.ῌ11.
Aoyagi, K. and Kazama, T. (+32*) : Transformation changes of clay minerals, zeolites and silica
minerals during diagenesis. Sedimentology, ,1, +13ῌ+22.

¡¢~ » ¼ +33+ : £¤N6K=½£u0KL9tJ 45  -+ ,-ῌ-+.
Bebout, G.E. (+33/) : The impact of subduction-zone metamorphism on mantle-ocean chemical
cycling. Chem. Geol., +,0, +3+ῌ,+2.
Bebout, G.E., Bebout, A.E. and Graham, C.M. (,**1) : Cycling of B, Li, and LILE (K, Cs, Rb, Ba,Sr) into subduction zones : SIMS evidence from micas in high-P/T metasedimentary rocks.
316

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Chem. Geol., ,-3, ,2.ῌ-*..
Brown, K.M., Sa#er, D.M. and Bekins, B.A. (,**+) : Smectite diagenesis pore-water freshing andﬂuid ﬂow at the toe of the Nankai wedge. Earth Planet. Sci. Let., +3., 31ῌ+*3.
Claypool, G.E. and Kvenvolden, K.A. (+32-) : Methane and other hydrocarbon gases in marine
sediment. Annu. Rev. Earth Planet. Sci., ++, ,33ῌ-,1.
Dählmann, A. and De Lange, G. J. (,**-) : Fluid-sediment interactions at Eastern Mediterranean
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from the northern Coast ranges, Rumsey Hills, California, USA. Geochim. Cosmochim.
Acta, /2, +021ῌ+033.
Dia, A.N., Castrec-Rouelle, M., Boulegue,
J. and Comeau, P. (+333) : Trinidad mud volcanoes :ŸWhere do the expelled ﬂuids come from? Geochim. Cosmochim. Acta, 0-, +*,-ῌ+*-2.
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#$ % &$'( +312 : )*++,-./01 R+ 2 34 56789 ,3* +ῌ,,.
#$ % +313 : :;9<=> < + 56789 ,3. +ῌ+/.
Giggenbach, W.F. and Goguel, R.L. (+323) : Collection and analysis of geothermal and volcanic
water and gas discharges. Fourth Edition. Report CD,.*+, Chemistry Division, DSIR, 2+
p., New Zealand.
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and geothermal techniques to geothermal exploration in the Middle east, Asia, the Paciﬁcand Africa, ,*3ῌ,-+.
Haese, R.R., Hensen, C. and De Lange, G. J. (,**0) : Pore water geochemistry of Mediterranean
mud volcanoes, Implication for ﬂuid transport and ﬂuid origin. Mar. Geol., ,,/, +3+ῌ,*2.

?$@A $BCD $EFG ,**3 : HIJKL5MN OP ++2 .*2ῌ.,-.
Hurai, V., Simon, K. and Bezak, V. (+331) : Contrasting chemistry and H, O, C isotope composition of greenschist-facies, Hercynian and Alpine metamorphic ﬂuids (Western Carpathians).
Chem. Geol., +-0, ,2+ῌ,3-.

FQRS TUVW XYZE +31. : [\ ]^_ ,/ +2ῌ--.

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Marschall, H.R., Altherr, R., Ludwing, T., Kalt, A., Gmeling,
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mochim. Acta, /-, ,3ῌ.+.
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Schmidt, M.W. and Poli, S. (+332) : Experimentally based water budgets for dehydrationg slabs
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