
J. Jpn. Soc. Soil Phys.
JK(LM
No. 3-, p. -++ ,**-

 
*ῌ **ῌ

**ῌ

**

Soil Solution Concentration Prediction of Volcanic Ash Soil upon Additionof Acid Solutions di#er in Anion Composition
Kouji KAMEYAMA*, Susumu MATSUKAWA**, Tomoyasu ISHIDA** and Hidemasa KATO*** The United Graduate School of Agricultural Science, Tokyo University of Agriculture
and Technology, Fuchu, Tokyo +2-ῌ2/*3, Japan** Faculty of Agriculture, Utsunomiya University, Utsunomiya -,+ῌ2/*/, Japan
Abstract
The prediction method of soil solution concentration of volcanic ash soil upon repetitive
addition of acid solutions that di#er in equivalent ratios of nitrate to sulfate was examined in thisstudy.

The method for prediction was composed of chemical equilibrium equation, electricalbalance and conservation of mass in soil solutions. The results were summarized in the following.
+)

There was a tendency of aluminum concentration upon addition of HNO- solutionupon

addition of acid mixed solution including NO- and SO.,upon addition of H, SO. solution withequal soil solution pH.
,)

The model adequately described accumulative release of basic cations. This shows it isability to estimate acid bu#ering capacity of cation exchange and mineral weathering.
-)Concentration of monovalent anions was much higher than that of SO., upon addition ofacid solutions. It was considered that monovalent anions that remain in soil solution greatly
a#ected decreasing process of pH and concentration change of basic cations. Therefore, it
seemed that NO-, which are di$cult to be adsorbed in soil, are a#ected the release of basic
cations and pH decreasing in soil when acid rain including NO- and SO., deposited to volcanic
ash soil.
.)

The simulation results agreed well with the measured values of pH and accumulative

release of basic cations. These represent the most serious e#ects of the acid deposition on thesoil. Therefore, parameters used in this simulation model are useful for predicting the maine#ects of the acid deposition on the Kanto loam subsoil.
Key words : acid deposition, volcanic ash soil, acid bu#ering capacity, chemical equilibrium
equation, anion composition

#$ %&'() pH * ..2..3 +,-$ ./(+    +33-+331  - 

0&123456789:;<(<+,69=4!"56 >./?@A./BC./DEF$ ,**,GH )I* NOPQRSRSTUAPSVWX Y+2-ῌ2/*3 NOZ[\]^ -ῌ/ῌ2** _Z`RSPSa Y-,+ῌ2/*/ _Z`]b^ -/*: cd$ efJK$ ghi$ 0Sjkl$ mnopqrs4       NO-

SO.,    NO-, SO., + AEC % ,- NO-, . ,-/ (HNO-, H, SO.*0 12345 (Huete and Mc Coll,+32.* 6789:;< (James and Riha, +323 ;Xu and Ji, ,**+* =>? @)A ! SO., B

C

@

D!#.

EFGH"#6IJK5%$" LM
NO%P. AEC % (Q&ῌ'( +322* @R 6IJK5%$" LM
NS, T345B!U)*
+A
 SO.,

ῌ+
Table +

 !"#$%&' () +33+*
SO.,

3- ¼ (,**-*

NO-



pH (KCl*
pH (H, O*
¹
(῍**+
CEC (cmolc kg+**,[\345 (cmolc kg+**,
Ca,
Mg,
K
Na
[\T345 (cmolc kg+**Cl
NO-
SO.,
8dt

NO- !OSBVHNO-, SO., W -sῌw

Physical and chemical properties of soil

X Y=

/40/
/40,
+1410
,,41,

*4-+
*4,+
*4+1
*4+3

*421
*4-0
+413

*+ : º»*, : Shollenberger t*- : *.*+ M NaOH - (, g : +/* mL* 0

B.@ ,Z#.(Kamewada, +330 ;-) +332* + -T345., [\12/0#1]^_`&= -345 %2 -T3-  W%X YZ5g[\L78'.#vHh  - Du;

45 @ ab 3)c#. (dew]_ -1 ^) +32**a$  -4]5gf"# NO-, SO.,

$LMN_ `!

Al- < T345B +b%cw]

S4]5g - T345/_ V,ab8d}c)h!iT345 $R 123450

=j6%PH>?@ @R NO-, SO.,

kl)

,    $L

MNS4]5g>?78m9:; kl)

,+ ῌ   efghi%wjkl5

c EFLMN%<n=
>?78op7>H  H, SO. -4]S?@ (ABῌq& +332 ; rM) ,**,* V HNO- .

H,SO. -4]S?@ (C') +332* %< #h

 stDu EF NO-, SO.,

mn(o .*0* cm CpI;q%
, mm .rj"%@sῌw %cῌ+  h 8dt cῌ+ u¡t!"$ ]1  ¢£vV]_4]5g>?78 G=vHt¤ (¥¦"Utw§¨©ª +331* xu#8d%#..

~" «¬y  ­r IJ! pH K 12
345L  345[\Lw
AxyH M"  zN C {+* ,/ P /* mL z®{¯«°± ,.* g 

b±²%| +.* M-NH. Cl - -* mL %«°®{¯, ,* / P³'®{¯ +.* M-HCl

#O|; (rM) ,**,*- *.., *., mL, +.* M-NH. OH - *.., *.,, * mL %,@R PQR  w A M"

 + ´} µ¶ +~/h -* ®" zN}g%ST# w~"  NO-, SO., 

A<U%

·-%¸# .* E  HCl .

$ pH, / P®{¯ *.+, *.*,, *.*+, *.**+, *.***+..* -%V,ab%~. 

NH. OH %

M-NH. Cl -% -* mL ³', /* -* 6\}

FG : h*+,"i~#bO§¨©M¼>7deM

5-* mL > * +2 uv?" 

*.1/

|}
mL

 H

7 |}V+&'()D pH

* /
 :

% *../ mm @,',23 4 ,-. 
7 *+,7 /*+,

KCa, Mg,

K, Na, Al %04/,J  K24

 h*+,

KCl, NO-, SO. %*+,-./01'234 V

7

7 >7h*+,J%L1=<
Kmol L+ V* : >

7 C* : >h*+, KL CN : N 2> !h*+,

Kmol L+ VN : N 2|}:

 KL

^_MNOElectric charges of soil.

" N 2h*+,J5% KCN+VrN+ῌ+
Fig. +

>3

VrN : N 2 KL "4C*V*CNVN Df<F CF m9D -*  
 . / 0+*  1  pH  Cl, NH. qOh*+, K*.*+ M NaOH 7Oh*+,

!

7X h*+,J Kcmolc kg+ "

" #$ pH %&'() Cl %*+,-./01'234 NH. %56
7 2 89 8:;7 NH. ,Cl  <= 3 +.* M-NaNO--* mL/ 7 ,** mL @(2'(A NH. , Cl 

1 >7h*+,"eJ6 M=<8 Cl $6 HNO-

>7de>7de NO- J%L

16f7  N 2M=<8,** mL @(2'(A B C

"

>

7

SO.,, H, SO.

> -* ?" -*  
N+ 2=<>e7J K6J ph*+,% CNVNCN+VrN+ Df<FCF m9D N+ 2=<>eC"

 +* 

6h*+,68`EF B p

EF7 NH. , Cl =< 2 D

EF7

qOh*+,=<h*+,68 HV7NH. , Cl  GHI NH. J KCEC Cl JOh*+,: h*+,J Kcmolc kg+ "

 KAEC "

7

3 D



L

6

EF7MNOPῌ+ Q#$ h*+,JU '@4¡ ¢

7 #$ PR%  K+32+ 6STU

 SO., 9£V :¤`;¥¦"# SO., %§VW7XDY WU¨©MJxV7f pH ..* bO

CEC, AEC Z

VBF[FQ7 #$ U \C] % !
NH. , Cl 

Kmol L+^_M% M*/+*

pH `abObO cYF7 C7f pH -.*  H, SO.

"ijkl`!IV"#$EF7

/* mL 8m ,.* g %&'m Kno()F p5o -/ mL

mol L  >D% SO.

,KSO., :

ª :¤

>p

ZVX>±T ²;7

-,, 
*.+.0 kg kg++ "J"«¬<­#®`¯=#"°<

QV

de CEC 6X AEC `)f!Ig h*+,J
`M

.

M

 V7³´ !U!  rs#® "f4ῌ, Q7 #$ µ±bO

qrs"7 5o> ?"tD* +2 uvwx

6Mkl"(¶ >qv·±TDY ?

=?" 

t@n¸#VA V77f -¹@6¹yz{0D* -*mL |}7|}8% pH ..*  HNO-, H, SO.
YV% NO-, SO., &(`~# pH ..* eKNO- : SO., *.1/ : *.,/ *./* : *./* *.,/ :@BbwºC%°D#=;7
pH ..*  HNO-, H, SO., e

>7depH " p KAl-  «¬ Pῌ, Q7 #$ pH -.* 
H, SO.

>7deZVXE».{0¨µ ¶ 3- · ,**-6

ῌῌ,Table ,

KF;)C}

!+,- 56-

Chemical equations, equilibrium constants and conditions used in ion concentration prediction+ gdg Al- +.*-.+*0H ,.-/0
xL : HNO Al- +..+.+*0H ,.-1+
xL : rs Al- +.,/3+*-H +.20xL : H, SO.
 Al-H, OAlOH,H
logKf/.*, Wolt, +33.

 Al-,H, OAlOH 
logKf3.-* Wolt, +33.
, ,H, ~ ,HExBCBC,,ExH
logKBCfH &'-HExAlAl--ExH
logKAlfH &' BC,   Ex u/ ExBCExAlExH+- +,CO,H, OHHCO-f
logKf1.2, Wolt, +33.
. ¡¢£¤¢£ SO.,f cmolcῌkgf+ /,3¥SO.,f¦*.,,/¥H¦*.--/¥NO-fClf¦f*.++/xL¢£ NO-fClf cmolcῌkgf+ .0.1¥NO-fClf¦*.-/,¥H¦*.+./¥SO.,f¦f*.*+xL
Al-SO.,fAlSO.
logK-.,* Wolt, +33.
/ + J§¨© ªF
 © ªF Fwcmolcῌkgf+ *.230¥H¦*..*xL
0 «¬56ῒῌ ῏῍ ῏ῑῒῌ ῐ῍ ῐ
ΐ ῎ ῎
ΐ ῎ ῎

1 ./012,f SO,fmol : ­ SO,fcd SO,f.
. AlSO. ¢£ SO.
.
,f+,® SO. AlSO. ¢£ SO,f.
 NO-fClf mol : ­ NO-fClf ¢£ NO-fClf cd NO-fClf+,® NO-fClf ¢£ NO-fClf, BC mol : ­ BC, ¢£ BC, +,® BC, ¢£ BC,

3456

¯^°±

  p Al-+,®²/mol f+,³²/mol´*.*++,³²/molAl- 7[\ Sato et al. +332 +332  Fumoto et al. ,**+   ` pH  Al- DEF

HNO-aH, SO. bI H, SO. cde  cd  Al!"# Al-, AlOH,, Al

OH ,, AlOH -* , AlSO.  / " $%&'(- )* !+,- ./012 3456789
 $:_, !+,-7;<%=)>?$+,'@

 Wolt +33.

A7BC DEFG@

Debye-

Hückel -HIJ) Al KFL'A7 Al- KFMNAOPAQRS (- )*34567TU<%VIW SO.,f g Al- h AlSO. #i9jk%
\ lm Al- DEF#njo$%pS k
q rscde Al- DEF  H, SO. cdeHItYo HNO- cdeHInjo$%
#*jk $: rscdeKF;  NO-f, SO.,f u/vw$% - "rscdxy z kgF{| (, - 7C}; XQ 34Y Al- KF;A~ Ca,, Mg, /~ K, Na /7(+Debye-Hückel -HIDEFG@Zv<% ~ Ca,, Mg, /# +.. 

Al- DEF7[\ Al- DEF]^@A7I ptY} \)}Q  ®¯ : delO?+,-56789:;<῍ῌ,
Fig. ,

7

@

῍ῌ-

pH ..* ,-;<;<
bc

Relation between pH and p (Al-ῌ) upon
addition of HNO-, H, SO. and mixed
solutions.

Fig. -

Accumulative anion adsorption after
addition of pH ..* mixed solutions.

HNO-, H, SO.,
pH-p Al-,-;<@89,-23°῎ῌTable -

Al h

23

¡/

h¢£¤* ¥¦¤Chemical equations, equilibrium constants and conditions used in
evaluation of aluminum species concentrations+§ h¢£¤
Al-H, O$AlOH,H
Al-,H, O$AlOH, ,HAl--H, O$AlOH*--H
Al-SO.,'$AlSO.
,§ ¨T©

logK$'/.*,
logK$'3.-*
logK$'+..33
logK$-.,**
ªAl$Al-AlOH,AlOH
, AlOH-AlSO.

-§ «¬¥¦

ῌ Al _'ªAl ῌ῍῍­*.**+Al _ , 
 BC, :Ca , Mg , K , Na   
,,^x] ^_ht?RHyz{W|)>? R * [\]^}~^(Y _*

pH  _t?_  ῌ+  !"# log CEC$*.,13 pH*.-1. +og %C&

NO-', SO.,' 4lO? pH ..* ,-;<'*.,31 ()* pH ..* +,- %C&$+.+*'. mol L'+

 NO-', SO.,' bcῌ- 

/0123,-456789:;<=>?@* pH 0

SO.

,'



NO-' :

4 *./* : *./* f *.,/ : *.1/ ,-;<ABC+D+EFGH CEC :IJHKLMN@* NO-' bc4O H* ;<O/PQ=>  R * CEC  pH STH

NO-' 489bc O/<|* 894

UVGHWX O( YZ* UV[\]^HY _GHO`* U
Vabcdefgh * ijkHgl!89GmnGo? pq* +331

( * r^4sTt?uevwGH* bcde[\] / UV NO-' 4;<=>SO.,' UVf89,-W|)>   * * SO.,' H NO-' f89
bc=>t/* SO.,' 4sTt?89,-GH

NO-' HKLbc=>O/R4=> w±K ² 3- ³ Q,**-R

8 NO-   NO-

-

NO

SO.

,

SO.,



  !" #$%&'()* ! + , -. NO- / SO.,
=> :; 

0123

Cl %," ! Cl-.

456789:;<?012 @" %ABC< DE F
Cl IJ

 ! + GH NO-KLMNOP(F!

QBolt and

Bruggenwert, +32*R+ S( TU NO-, Cl

V + W?012 , XYZ + W?012
QNO-[ClR, W?012 QSO.,R " VA

B(C< 

+*\ ]?012^_ABL ?012

ῌ.

pH ..*  HNO-, H, SO., p 78V-.
 z{K|0127}_ QFwR`
a012bc QH[R 

Fig. .

Relation between elution of basic cations and Hydrogen ion upon additionof pH ..* HNO-, H, SO. and mixed
solutions.

_ `a012bc ?012bc " 012^?012bcde<  Vf< Freundlich gPhi QMesquita and Vieira e Silva, ,**,R Vj
+ S ?012iklmnoL pH ..* 
HNO-, H, SO., p 78

pH -.*  H, SO. 78V-.

 qr=>s!t+, Guvwxy5

z{K|0127}_

L ]z{K|012~:;_ 34Kz{_V6z{K|012^:;_Bloom and Grigal Q+32/R

A

! Q+331R

O Guvwxy5 z{K|0127}_ 78`
a012bcde<  Vf<i QHelgeson et al.,+32.R VjAB+ S Guvwxyi Qfῐ,῏ iR L pH ..*  HNO-, H, SO., p 78V-.
῎

Guvwxy5 z{K|0127}_ 78`a012bcs!t Qῐ.R+.    .+pH, 

NO-, SO., _ *

pH ..* p 78V

Y-. 78 pH qr AB   V  ῐ /    + * \  9  logKBCH,

ῌ/
Fig. /

logKAlH Qfῐ, ῌ ῍ iR L r|01

pH ..* p 78V-.
pH qr AB

78

Measured and predicted pH in soil
solutions upon addition of pH ..* mixed
solutions.

234V + ]78V-.
 pH ABL pH qr*.- ( ¨ῐ0 1 2 (S©+G+  NO- : SO.,

*.1/ : *.,/ *./* : *./*

§z{K|012 QBC,[R bcL ]78V-.

p 78V-.  pH

¡¢(L£¤q  qr ABbcªy«¬L£¤*GVr G+ GH -.¥(Lqr5Y%¡¦, + W?012 QNO-[ClR , SO., bcL ]AB+-u §z{K|012 QBC R + W?012 QNO,[

[Cl R SO.

,

+


-

bcqr ABV NO

: SO.

,

*.1/ : *.,/ *./* : *./* *.,/ : *.1/ p 78V-.

78V-.  qr AB *.+ mmol L+(G+  NO- : SO.,

*.1/ :*.,/ Qῐ0R  (L SO., bcL­®¯¡°A : +,-. 9cZ '(?!"# $% '(34gh

9

ῌ0

WXYZI,-. /BC,12 + *+,-.
/NO-01Cl02 SO.,0 34 hsr br67 /NO-0 : SO.,0*.1/ : *.,/2

ῌ2

WXYZI,-. /BC,12 + *+,-.
/NO-01Cl02 SO.,0 34 hsr br67 /NO-0 : SO.,0*.,/ : *.1/2

Fig. 0Measured and predicted concentrationof basic cations, monovalent anions andSO., in soil solutions. (NO- : SO., *.1/ : *.,/)

Fig. 2

Measured and predicted concentrationof basic cations, monovalent anions andSO., in soil solutions. (NO- : SO., *.,/ : *.1/)

 +,-.J&D 5LMNO 8


PQ '(> + *+,-. pH R

STUVWXYZI,-.34[\;<]^_#5`a 
., 

bGcdefJgh ijZ  C
H, SO., k% l:m#!"# $% W

pH ..*XYZI,-.nopqJ5 SO.,0 no@AJ br
5hsr 67 tῌ3 +* uvw#

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Fig. 1,1

Measured and predicted concentrationof basic cations, monovalent anions andSO., in soil solutions. (NO- : SO., *./* : *./*)

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SO.,$ G&HIJKL"MNO

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&@&XY)Z["\]^#_`EF/    
NO-$, SO.,$ &a=&b#cdefghῌ3Fig. 3

pH ..* & H, SO. '()*+&kD   /BC,y1
&
OPQ
!Q=>
Measured and predicted accumulative
release of basic cations upon additionof pH ..* H,SO. and mixed solutions.

i&XYOj&kl6mnNO-$, SO.,$ &a=b#oD()p *+

&(3 q&O)rs t&uv%
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pH-p /Al-y1 &z{% HNO-, H, SO., '(*+1+|2t}b
3 %pH q(2& Al-y

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 /NO-$yCl$1 3 % SO.,$ =>8?
("^# + :  pH x7 
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dhi

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pH ..* & H,SO. '(*+¬& SO.,$
&OPQ!Q=>

62<# pH xkD   &Fig. +* Measured and predicted SO., accumulative adsorption after addition of pH ..* H,
SO. and mixed solutions.

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IJKL&§¨6©Q)ªP2?
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and Willemsen, +3211 )u NO-$, SO.,$ &a=
!"# SO.

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&%SO.,$ 789:#;2<#2<#¯°±)²³6"´^ Mixing Cell µ¶· /Appelo
b#oD(efg¸¹&¯°±O"U\])ºP2<#  Appelo, C.A. J. and Willemsen, A. (+321) : Geochemical calculations and observation on salt water
intrusions, I. A combined geochemical/mixing\] : ¸z/¹5º»(EJ!F^B;CD0@ab¼O!F$%&I

11

EJ!F^_`/a0@abc!F$%1

cell model. J. Hydrol., 3. : -+-ῌ--*.
Bloom, P.R. and Grigal, D.F. (+32/) : Modeling soil
response to acidic deposition in nonsulfate ad-pH. '(J 11 : ++ῌ+2.
Mesquita, M.E. and Vieira e Silva, J.M. (,**,) : Prelim-sorbing soils. J. Environ. Qual., +. : .23ῌ.3/.

inary study of pH e#ect in the application ofBolt, G.H. and Bruggenwert (+32*) :  

Langmuir and Freundlich isotherms to Cu-Zn

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+*/  

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competitive adsorption. Geoderma, +*0 : ,+3ῌ,-..

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nῌ&lopῌq6rsῌ@7tῌ84uvῌ1

Fumoto, T., Shindo, J., Oura, N. and Sverdrup, H.

'%+,(yEz/1 Ez/>?@%&'





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w9:pῌ;;<ῌg(,**+) : Adapting the proﬁle model to calculate
the critical loads for East Asian soils by includ-x +33+ : EJ=({| 9 +33+ : 3,*ῌ3,3.
;

Aῌ2}~#ῌB5CDῌ;2E +332 : -ing volcanic glass weathering and alternativeB;CD Ez/0" JFsolubility system. Water, Air and Soil pollution,

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1H : 0.2ῌ0.3.

+-* : +,.1ῌ+,/,.
Helgeson, H.C., Murphy, W.M. and Aagaard, P. (+32.) :Sato, K., Wakamatsu, T. and Takahashi, A. (+332) :Thermodynamic and kinetic constraints on reac-

Acid deposition and ecosystem sensitivity intion rates among minerals and aqueous solution.

East Asia. pp. +,/ῌ+.,, Bashkin, V.N. and Park, S.ῌ

,. Rate constants,e#ective surface area, and theU. eds., Nova Science Publishers Inc., New York.

hydrolysis of feldfer. Geochimica et cosmo-fῌD +332 : EJ=%H(JFz%H(&I

chimica Acta, .2 : ,.*/ῌ,.-,.
Huete, A.R. and Mc Coll, J.G.(+32.) : Soil Cation leaching by “Acid Rain” with Varying Nitrate- to-89 03 : .11ῌ.21.
L5 ¡ῌ@¢£MῌN

Sulfate Ratios. J. Environ. Qual., +- : -00ῌ-1+.

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234567 89 /+ : 3/ῌ+*+.
James, B. J. and Riha, S.R. (+323) : Aluminum leachingby mineral acids in forest soils : I. Nitric-sulfuric
acid di#erences. Soil Sci. Soc. Am. J., /- : ,/3ῌ,0..

:;<=ῌ>?

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M©ª +32+ : 0«¬ pp. /ῌ/1  Mjp +331 : ­ pp. 1-ῌ3/ ®Vp¯
 W°VX

Wolt, J.D. (+33.) : Soil solution chemistry. pp. +/2ῌ+0+,John Wiley & Sons Inc., New York.

Kamewada, K. (+330) : Application of ‘Four-plane
Kmodel’ to the adsorption of K , NO

L-and SO.

,L

from a mixed solution of KNO- and K, SO. on±Yῌ?Z[f +322 : EJ²%H(;M³´ 89 /3 : .+-ῌ.+/.
Xu, R.K. and Ji, G.L. (,**+) : E#ects of H, SO. andAndisols. Soil Sci. Plant Nutr., ., : 2*+ῌ2*2.

HNO- on soil acidiﬁcation and aluminum specia-

MNOPQRSTU ,**, : )Vtion in variable and constant charge soils. Water,*5 +. +%  pp. +*2ῌ+*3 WXYZ[>?

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] +332 :Air and Soil Pollution, +,3 : --ῌ.-.
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