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Insitu Ozonation

Insitu Ozonation

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JO U R N A L O F
C o n ta m in a n t
H y d ro lo g y
E L S E V IE R
Journal of C ontam inant H ydrology 28 (1997) 327-335
E ffica cy
o f in -situ
o z o n a tio n
fo r th e r e m e d ia tio n
o f
PA H
c o n ta m in a te d
s o ils
S u s a n
J. M asten
*, Sim on
H .R . D a v ie s
D e p a r tm e n t o f C it,il a n d E m , ir o n m e n ta l E n g in e e r in g , M ic h ig a n S ta te U n it,e r s iO ' E a s t L a n s in g ,
M 148823, USA
A bstract
P o ly c y c lic
arom atic
hydrocarbons (PAHs)
a re
of environm ental concern
b e c a u s e
m any
PA H s
a re e ith e r c a rc in o g e n s o r p o te n tia l c a rc in o g e n s . P e tro le u m
p ro d u c ts
a re
a m ajor source
of PA H s.
T he
o c c u r r e n c e
o f
PA H
c o n ta m in a tio n
i s
w idespread
a n d
n o v e l
tre a tm e n t
te c h n o lo g ie s
fo r
th e
re m e d ia tio n
o f c o n ta m in a te d
soils are necessary.
O zone
has been
fo u n d
t o
b e
e x tre m e ly
u s e fu l fo r th e d e g ra d a tio n
of PA H s
i n
soils. For these
com pounds,
th e
re a c tio n
w ith
m o le c u la r
o z o n e
a p p e a r s
t o
b e
th e
m ore
im p o rta n t
d e g ra d a tio n
p a th w a y .
G re a te r th a n 9 5 %
rem oval of phenanthrene was
a c h ie v e d w ith a n o z o n a tio n tim e o f 2 .3
h a t a n o z o n e flu x o f 2 5 0 m g h - 1. A fte r 4 .0 h o f tre a tm e n t a t a n o z o n e flu x o f 6 0 0 m g h
1, 9 1 %
o f
th e
p y r e n e
w as
rem oved.
W e
h a v e
a l s o
fo u n d
th a t th e
m ore
h y d ro p h o b ic
PA H s
(e .g .
c h r y s e n e )
react m ore
slo w ly
th a n
w o u ld
b e e x p e c te d
o n
th e b a s is o f th e ir re a c tiv ity
w ith
ozone, suggesting
th a t
p a rtitio n in g
o f
th e
c o n ta m in a n t
in to
s o il
o rg a n ic
m atter
m ay
r e d u c e
th e
re a c tiv ity
o f
th e
com pound. Even
so, after 4
h of exposure
to o z o n e , th e c h r y s e n e c o n c e n tr a tio n in
a c o n ta m in a te d
M e te a
soil w as reduced
fro m
1 0 0 to
5 0 m g k g -t.
O zone
h a s
b e e n
fo u n d
t o
b e
re a d ily
tra n s p o rte d
th ro u g h
c o lu m n s
p a c k e d
w ith
a
num ber
o f
g e o lo g ic a l m a te ria ls , in c lu d in g
O tta w a
sand, M etea
s o il, B o r d e n
a q u ife r m a te ria l a n d
W u rtsm ith
a q u ife r m a te ria l. A ll o f th e s e g e o lo g ic a l m a te ria ls e x e rte d
a lim ite d (fin ite ) o z o n e d e m a n d , i.e . th e
r a t e
of ozone
d e g ra d a tio n
i n
so il c o lu m n s
is very
s lo w
after the
o z o n e
dem and
is m et. M oisture
content was found
to in c re a s e th e o z o n e d e m a n d , m o s t lik e ly o w in g
to th e d is s o lu tio n o f g a s e o u s
o z o n e
in to th e p o re
water. A s once
th e in itia l o z o n e
dem and
is m et, little degradation
of ozone
i s
o b s e rv e d , it s h o u ld b e p o s s ib le to a c h ie v e o z o n e p e n e tra tio n to a c o n s id e ra b le d is ta n c e a w a y
fro m
th e in je c tio n w e ll, s u g g e s tin g th a t in -s itu o z o n a tio n is a fe a s ib le m e a n s o f tre a tin g u n c o n ta m in a te d
* C orresponding author. Tel.:
+ 1 517 353-8539: fax:
+ 1 5 1 7 3 5 5 -0 2 5 0 ; e -m a il: m a s te n @ c e e .m s u .e d u
0 1 6 9 -7 7 2 2 /9 7 /$ 1 7 .0 0
\u00a9
1 9 9 7 E ls e v ie r S c ie n c e B .V . A ll rig h ts re se rv e d .
P IIS 0 16 9 -7 7 2 2 (9 7 )0 0 0 1
9 -3
3 2 8
S .J . M a s te n , S .H .R . D a c ie s / J o u r n a l o f C o n ta m in a n t H y d r o lo g y 2 8 (1 9 9 7 ) 3 2 7 - 3 3 5
u n s a tu ra te d s o ils . T h is is s u b s ta n tia te d b y tw o fie ld s tu d ie s w h e re in -s itu o z o n a tio n w a s a p p a re n tly
successful at rem ediating the sites. \u00a9
1 9 9 7 E ls e v ie r S c ie n c e B .V .
K eyw ords: O zonation;P A H s;In-situ soil rem ediation;Phenanthrene:Pyrene:C hrysene
I. In tr o d u c tio n
P o ly c y c lic
arom atic
h y d r o c a r b o n s
(P A H s)
a re
o f
e n v iro n m e n ta l
c o n c e r n
b e c a u s e
m any
of these
com pounds
a re
e ith e r c a rc in o g e n s
o r p o te n tia l c a rc in o g e n s . T h e
o c c u r -
r e n c e
of PAH
c o n ta m in a tio n
i n
s o ils
i s
w idespread,
a s
g a s o lin e
o r fu e l o il
s p ills
a re
c o m m o n ; in
fact it is estim ated
th a t 9 0 - 9 5 %
o f a ll le a k in g
u n d e r g r o u n d
s to ra g e ta n k s
c o n ta in
p e tro le u m
p ro d u c ts
(U S
E P A ,
1 9 9 5 ).
M any
th o u s a n d s
o f
s ite s
e x is t;
M iller
(1 9 9 4 )
h a s
e s tim a te d
th a t
th e
A ir
F o r c e
a lo n e
n e e d s
t o
re m e d ia te
m ore
th a n
2 0 0 0
p e tro le u m -c o n ta m in a te d site s. W h e re
a fuel spill has occurred, soils in the vadose zone
w ill be
c o n ta m in a te d . B io v e n tin g
a n d
c o n v e n tio n a l s o il v a p o r e x tra c tio n
(s o il v e n tin g )
te c h n iq u e s
h a v e
b e e n
u s e d
t o
re m e d ia te
p e tro le u m
c o n ta m in a tio n ,
b u t
th e
rem oval
e ffic ie n c ie s fo r P A H s a re ty p ic a lly v e ry lo w

(R . M ille r, p e rs o n a l c o m m u n ic a tio n , 1 9 9 4 ). S in c e m o s t o f th e P A H s a re s e m i- o r n o n -v o la tile , c o n v e n tio n a l so il v e n tin g is re la tiv e ly in e ffe c tiv e .

T he
h ig h e r
m o le c u la r
w e ig h t
PA H s
a re
r e s i s t a n t
t o
b io re m e d ia tio n
a n d
b io re m e d ia tio n
s tu d ie s
s u g g e s t
th a t
m icroorganism s
c a n
o n ly
d e g r a d e
PA H s
th a t
a re
d is s o lv e d
i n
th e
a q u e o u s - p h a s e
a n d
th a t P A H s
s o r b e d
o n to
o r p a rtitio n e d
in to
a
s o lid
phase are not readily degraded
b y m ic ro o rg a n is m s (L u th y
et al., 1994). Thus, prospects
for the
i n - s i t u
b io re m e d ia tio n
of PA H s
i n
s o ils
a re
p o o r,
u n le s s
m eans
a re
fo u n d
t o
s o lu b iliz e th e s e c o n ta m in a n ts .
T he
u se
o f
s o lv e n ts
o r
s u r f a c ta n ts
t o
e n h a n c e
th e
s o lu b ility
o f
th e
h y d ro p h o b ic
c o m p o n e n ts fo u n d in p e tro le u m

products has been suggested. H ow ever, high concentra- tio n s o f th e s o lv e n t o r s u rfa c ta n t a re g e n e ra lly re q u ire d to a c h ie v e g o o d re s u lts (L u th y e t a l.,

1 9 9 4 ).
A lso,
th e
s lo w
d is s o lu tio n
k in e tic s
n e c e s s ita te
lo n g
c o n ta c t-tim e s
a n d
e ffe c tiv e p ro c e d u re s to tre a t th e e x tra c te d P A H s a re o fte n d iffic u lt to d e v e lo p (L u th y
e t
a l.,
1 9 9 4 ).
I n
th e
fie ld ,
th e
h e te ro g e n e ity
o f th e
d e p o s its
m ay
c a u s e
th e
solvent (or
s u r f a c ta n t
s o lu tio n )
t o
b y p a s s
som e
o f
th e
c o n ta m in a te d
z o n e s .
T h u s ,
i n
th e
fie ld ,
d is s o lu tio n ra te s m a y b e m u c h
s lo w e r th a n th a t o b s e r v e d in la b o ra to ry c o lu m n o r b a tc h
studies (Luthy et al.,
1 9 9 4 ).
2. In-situ
o z o n a tio n
I n - s i t u
c h e m ic a l
o x id a tio n
p r o c e s s e s
m ay
b e
u s e d
t o
overcom e
th e
lim ita tio n s
im p o s e d b y th e lo w
a q u e o u s s o lu b ility o f P A H s o n th e ir ra te s o f b io d e g ra d a tio n a n d / o r
d is s o lu tio n .
C h e m ic a l
o x id a tio n
o f
th e s e
com pounds
i s
lik e ly
t o
e n h a n c e
b o th
th e ir
b io d e g ra d a b ility
a n d
a q u e o u s
s o lu b ility ,
s in c e
th e
o x id a tio n
p ro d u c ts
w o u ld
b e
m ore
p o la r th a n
th e
parent com pounds
(G ilb ert,
1 9 8 7 ).
A n
a d v a n ta g e o f c h e m ic a l o x id a tio n
p r o c e s s e s
i s
th a t
th e y
a re
n o t
s u b je c t
t o
som e
o f
th e
r a t e
lim ita tio n s
im posed
o n
S .J . M a s te n , S .H .R . D a v i e s ~ J o u r n a l o f C o n ta m in a n t H y d r o lo g y 2 8 (1 9 9 7 ) 3 2 7 - 3 3 5
3 2 9
b io d e g ra d a tio n
p r o c e s s e s ,
s in c e
th e
c h e m ic a l
o x id a n ts
m ay
d iffu se
i n
th e
a q u e o u s
a n d /o r
g a s e o u s p h a s e to th e re a c tio n
s ite .
T he
u se
of gaseous
o z o n e
for in-situ
c h e m ic a l o x id a tio n
h a s
s ig n ific a n t a d v a n ta g e s
over aqueous-based
s y s te m s fo r th e tre a tm e n t o f u n s a tu ra te d

soils. A s the diffusivity of ozone gas is m uch greater than that for aqueous species, the m ass of ozone that one can c o n ta c t w ith

th e
ta rg e t c o n ta m in a n ts
is m u c h
g r e a te r th a n
th a t w h ic h
is possible
w ith
d is s o lv e d
o x id a n ts .
A d d itio n a lly ,
a s
v o la tiliz a tio n
o f
th e
ta rg e t
c h e m ic a l
i s
a l s o
n o t
re q u ire d , it c a n
o v e r c o m e m a s s tra n s fe r lim ita tio n s a s s o c ia te d w ith
soil venting. In-situ
o z o n a tio n
m ay
also be used
to treat the region
n e a r th e
w a te r ta b le b y
u s in g
s p a r g in g .
I n - s i t u
o z o n a tio n
w o u ld
lik e ly
b e
m ore
ra p id
th a n
b io d e g ra d a tio n
o r
s o il
v e n tin g
processes, thereby reducing the rem ediation tim e and, possibly, treatm ent costs.
C o n c e p tu a lly ,
i n - s i t u
o z o n a tio n
i s
sim ilar
t o
s o il
v e n tin g .
V ertical
o r
h o riz o n ta l
in je c tio n
w e lls c a n
be used
to in je c t o z o n e in to th e
subsurface. Fig.
1 illustrates how
a
v e rtic a l in je c tio n w e ll c o u ld b e u s e d to in tro d u c e o z o n e in to u n s a tu ra te d s o ils . E x tra c tio n
w e lls m a y , if n e c e s s a ry , b e u s e d to c o n tro l th e d ire c tio n o f o z o n e flo w
in the subsurface.
H o riz o n ta l
w e lls
c o u ld
a l s o
b e
u s e d
t o
in je c t o z o n e . N e ls o n
a n d
B ro w n
(1 9 9 4 )
h a v e
c la im e d
th a t
th is
te c h n iq u e
i s
m ore
e ffe c tiv e
fo r
th e
in tro d u c tio n
o f
o z o n e
in to
u n s a tu r a te d
s o ils th a n is th e u s e o f v e rtic a l w e lls . H o riz o n ta l w e lls a re a ls o a d v a n ta g e o u s
w hen
u s in g o z o n e in c o m b in a tio n
w ith s p a rg in g
te c h n o lo g ie s . H o w e v e r , w h ile h o riz o n -
tal w ells
m ay
h a v e
som e
a d v a n ta g e s , it is n o t c le a r th a t th e s e
a d v a n ta g e s
w a rra n t th e
a d d itio n a l c o s t n e c e s s a r y to in s ta ll s u c h
w e lls.
In -s itu o z o n a tio n h a s n o t b e e n
w id e ly
u s e d in th e fie ld . H o w e v e r , to o u r k n o w le d g e ,
tw o g ro u p s h a v e u s e d in -s itu o z o n a tio n fo r so il re m e d ia tio n . O n e g ro u p
is a c o n s o rtiu m
of tw o W est C oast com panies (Steffen R obertson
a n d K irs te n C o n s u ltin g E n g in e e rs a n d
S c ie n tis ts
a n d
M c C u llo c h
E n v iro n m e n ta l E q u ip m e n t S a le s). T h is
g ro u p
h a s
c o n d u c te d
th re e
fie ld -s c a le
so il re m e d ia tio n
efforts using
ozone. In
a ll c a s e s , th e c o n ta m in a n ts
o f
in te re s t h a v e b e e n c h lo rin a te d

solvents. The largest of these rem ediation efforts w as at a s ite in C a rs o n C ity , N V . T h is s ite h a d b e e n c o n ta m in a te d w ith te tra c h lo re th y le n e (P C E ). It w as

e s tim a te d
th a t
it w o u ld
ta k e
5
y e a r s
t o
c le a n
u p
th is
s i t e
u s in g
c o n v e n tio n a l
p u m p -a n d -tre a t
m ethods.
T he
ow ner,
a
p ro p e rty
d e v e lo p e r ,
w a n te d
t o
a c c e le ra te
th is
O zone
G e n e ra to r
~ '~
" 1
I
j , i
In je c tio n w e ll
II
. . J
E x h a u s t
b lo w e r
E x tra c tio n w e ll
A ir o r o x y g e n c o n ta in in g
o z o n e
is d ra w nth ro u g h th e
c o n ta m in a te d
z o n e
F ig . 1. S c h e m a tic o f in -s itu o z o n e tre a tm e n t s y s te m .

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