Chapter 2 Investigations of Soil as a Source of Indoor R a d o n 1
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R. G. Sextro, B. A. Moed, W. W. Nazaroff, K. L. Revzan, and Α. V. Nero Indoor Environment Program, Lawrence Berkeley Laboratory, University of California, Berkeley, CA 94720 The predominant source of indoor radon in most single-family housing in the U.S. is the soil adjacent to the house substructure. We have examined factors influencing the production and transport of radon in soil and into buildings. A number of important param eters have been identified and their effect on radon production and migration assessed, including radium concentration, moisture content, air permeability, and grain size distribution of soils. The potential regional variations in parameters affecting radon have been evaluated by examining geographic data, including surface radium concentrations and general soil data. We have also investigated factors influencing radon migration into individual dwellings. Coupling between the building shell and the surrounding soil has been demonstrated experimentally, and pressure-field map ping and soil permeability measurements have been car ried out. Soil is now recognized as a significant, i f not predominant, source of radon in the indoor environment. This is especially true in those dwellings with elevated indoor radon concentra222 tions. (In this paper, radon refers to Rn, and radium to 226 220 Ra. Although some of the discussion applies to Rn as well, its presence in indoor air is usually limited by its short halflife of 55 s.) Several recent studies of radon entry into homes have been done, including investigations or discussions of the influence of pressure differentials across the building shell, and the role of soil as a source of indoor radon (Nazaroff, e_t al . , 1985a; Nazaroff and Doyle, 1985; Nero and Nazaroff, 1984; DSMA, 1983) . There are a number of reasons to investigate both 'Current address: Environmental Engineering Science, California Institute of Technology, Pasadena, CA 91125 0097-6156/87/0331-0010$06.00/0 © 1987 American Chemical Society
Hopke; Radon and Its Decay Products ACS Symposium Series; American Chemical Society: Washington, DC, 1987.
11
Soil as a Source of Indoor Radon
2. SEXTRO ET AL.
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t h e c h a r a c t e r i s t i c s o f s o i l s and t h e i n t e r a c t i o n i n g s t r u c t u r e . The i n t r i n s i c p r o p e r t i e s of the w i t h t h e d e t a i l s o f t h e b u i l d i n g s t r u c t u r e and i t important determinants of the radon e n t r y r a t e ture. I n a d d i t i o n , b o t h t h e h o u s e and t h e s o i l changes i n ambient e n v i r o n m e n t a l c o n d i t i o n s .
with the buildsoil, combined s operation, are i n t o the struca r e a f f e c t e d by
T h i s p a p e r s u m m a r i z e s our r e c e n t i n v e s t i g a t i o n s o f s o i l as a source of radon. These i n v e s t i g a t i o n s have a t w o - f o l d purpose, and attack the problem from two distinct but complementary approaches. The f i r s t e f f o r t i s t o a s s e m b l e d a t a a t a g e o g r a p h i c a l s c a l e , a p p r o p r i a t e f o r understanding the general c h a r a c t e r i s tics of soils. This approach provides information on the a p p r o p r i a t e s c a l e s and r a n g e s o f i m p o r t a n t s o i l v a r i a b l e s , and how t h e s e m i g h t v a r y w i t h i n and among r e g i o n s . A n o t h e r important aspect of t h i s approach i s to d e r i v e v a l u e s of parameters that may be u s e d i n a p r e d i c t i v e t e c h n i q u e f o r i d e n t i f y i n g a r e a s where h i g h i n d o o r r a d o n l e v e l s a r e most l i k e l y ( N a z a r o f f a t «1 1986; Sextro, 1985). The s e c o n d a p p r o a c h i s t o i n v e s t i g a t e b o t h e x p e r i m e n t a l l y and t h e o r e t i c a l l y t h e i n f l u e n c e o f s o i l s a t a l o c a l i z e d l e v e l , on t h e s c a l e o f an i n d i v i d u a l h o u s e , f o r e x a m p l e . P r o d u c t i o n and t r a n s p o r t o f r a d o n i n s o i l s and m i g r a t i o n o f r a d o n i n t o h o u s e s d e p e n d upon l o c a l soil conditions, and r e s u l t s o f t h e s e s t u d i e s w i l l improve our basic understanding of the physical processes involved. T h i s i n t u r n w i l l a i d i n the s y s t e m a t i c development o f more e f f e c t i v e e n t r y i d e n t i f i c a t i o n and m i t i g a t i o n t e c h n i q u e s t o p r e v e n t or reduce radon e n t r y i n t o d w e l l i n g s .
Factors
I n f l u e n c i n g P r o d u c t i o n and
General
Desr.rlpi-M on.
tion
and
trated
migration
Table
and
As ciated
U U
mining
i s a mixture
the
matter. rocks
and
1
and
from
are
nominal
which
the
a
for
are
illusvarious
presented
i s p a r t of
slightly of
much e.gof
larger
Bq
the
kg
range
soil
usually, often
1
an
.
In
of
soil
1980).
water
reflects
and that
d e r i v e d by p h y s i -
ranges
are
(Wollenberg, f o r measured rocks,
asso-
than
(Powers eJi «1•
( d u n i t e ) t o 1 t o 1835 those
not
more
~40
m a t e r i a l s are
for rocks, excluding a l k a l i
t h e means o b s e r v e d
by
observed
(gneiss)
than
produc-
are
these
values,
value
found,
solid
rocks
rocks
broader
varies
content The
of
of radon,
m a t e r i a l s , a i r and,
radium
radon
buildings
ranges
Soils
content of surface s o i l s
milling,
activity.
metamorphic
The
typical
been
for ultrabasic
ranges
mean v a l u e s
a
of s o l i d The
chemical
kg"
igneous these
with
influence
into
In
i n a l l soil materials.
milling
c o n c e n t r a t i o n s has
organic
Bq
i s found
mining
magnitude,
1.
their
I, radium
near
20
and
that
and
immediate p a r e n t
or
areas
of
the
with of
cal
Figure
shown i n T a b l e
order radium
soils
i n some c a s e s
I . Ra-226,
U decay s e r i e s ,
Soil
parameters
through
schematically i n
parameters, in
The
M i g r a t i o n n f Radon
from
~
Bq k g "
0 1
1984). for soils,
i s consistent
soils.
Hopke; Radon and Its Decay Products ACS Symposium Series; American Chemical Society: Washington, DC, 1987.
to for
While the with
12
RADON AND ITS DECAY PRODUCTS
Basement
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Indoor Rn
radioactive
decay:
m i g r a t i o n t o air; trapping
Ra-
in s o i l g r a i n s
Water trap
• R A D O N M I G R A T I O N IN S O I L
-•Rn-
diffusion:
f(H 0,
convection: geochemical
emanating
processes
f(H 0, 2
2
e)
f(k, V P )
fraction
d , ...)
F i g u r e 1. Schematic i l l u s t r a t i o n o f f a c t o r s i n f l u e n c i n g t h e p r o d u c t i o n and m i g r a t i o n o f r a d o n i n s o i l s a n d i n t o b u i l d i n g s . Geochemical p r o c e s s e s a f f e c t t h e radium c o n c e n t r a t i o n i n t h e soil. The e m a n a t i n g fraction i s principally dependent upon soil moisture (Σ^Ο) >1, If
N
Pe
In
first
then
second
N
40 Bq k g " ( F i g u r e 3 b ) . A s c a n be s e e n from t h e f i g u r e , the d i f f e r e n c e s i n t h e area radium concentration distributions are q u i t e l a r g e . L e s s t h a n 0.5% o f t h e r a d i u m c o n c e n t r a t i o n d a t a from t h e C h i c o Q u a d r a n g l e a r e above 40 Bq k g , and l e s s than 0.01% a r e a b o v e 60 Bq k g " . I n c o n t r a s t , a l m o s t 6 5 % o f t h e s u r f a c e r a d i u m c o n c e n t r a t i o n d a t a from t h e San J o s e Q u a d r a n g l e h a v e v a l u e s g r e a t e r t h a n 40 Bq k g " w i t h 0.5% above 200 Bq k g " and 0.05% g r e a t e r t h a n 300 Bq k g " . 1
1
1
1
1
1
I n a d d i t i o n t o t h e s e f r e q u e n c y d i s t r i b u t i o n s , maps o f v a r i o u s types have been produced to depict the spatial d i s t r i b u t i o n of the s u r f a c e radium c o n c e n t r a t i o n s . One example i s shown i n F i g u r e 4, w h i c h r e p r e s e n t s d a t a from t h e a e r i a l s u r v e y o f t h e Newark Quadrangle, c o v e r i n g p a r t o f e a s t e r n P e n n s y l v a n i a and n o r t h e r n New J e r s e y . T h e d a t a i n t h i s f i g u r e a r e p l o t t e d on an a p p r o x i mately s i x m i l e by s i x m i l e g r i d . Thus e a c h p o i n t r e p r e s e n t s an average o f t h e data c o l l e c t e d along s i x m i l e s o f t h e f l i g h t l i n e . The frequency d i s t r i b u t i o n o f s u r f a c e radium c o n c e n t r a t i o n s f o r t h i s q u a d r a n g l e a r e a h a s a GM o f 35 Bq k g " , a GSD o f 1.45 a n d an a r i t h m e t i c mean o f 37 Bq k g . From t h e s e d i s t r i b u t i o n parameters, one c a n e s t i m a t e that approximately 7% o f t h e s u r f a c e r a d i u m c o n c e n t r a t i o n d a t a a r e g r e a t e r t h a n 60 Bq k g and l e s s t h a n 0.2% o f t h e d a t a a r e above 100 Bq k g . 1
1
1
W h i l e t h e s e d a t a and t h e r e s u l t i n g maps a r e u s e f u l i n i l l u s t r a t i n g b o t h t h e t r e n d s and v a r i a b i l i t y i n s u r f a c e radium concent r a t i o n s , d e t a i l e d f i e l d examination o f s u r f a c e radium concentrat i o n s i n s e l e c t e d areas i s needed t o determine t h e r e l i a b i l i t y o f
Hopke; Radon and Its Decay Products ACS Symposium Series; American Chemical Society: Washington, DC, 1987.
18
RADON AND ITS DECAY PRODUCTS
10.0
1
1
I
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NARR: All Quadrangles GM =24.9 GSD = 1.75 A M =28.5 ASD = 14.7
0.00
-U 40.00
80.00
120.00
160.00
200.00
Radium (Bq/kg soil)
F i g u r e 2. D i s t r i b u t i o n o f t h e s u r f a c e radium concentration d a t a from t h e N a t i o n a l A i r b o r n e R a d i o m e t r i c R e c o n n a i s s a n c e s u r v e y f o r 394 1° b y 2° q u a d r a n g l e s c o v e r i n g most o f t h e c o n t i g u ous 48 s t a t e s . The d i s t r i b u t i o n p a r a m e t e r s a r e c a l c u l a t e d from t h e d a t a and t h e l o g n o r m a l d i s t r i b u t i o n b a s e d on t h e g e o m e t r i c mearij and s t a n d a r d d e v i a t i o n from t h e d a t a i s shown as a s o l i d curve.
Hopke; Radon and Its Decay Products ACS Symposium Series; American Chemical Society: Washington, DC, 1987.
2. SEXTRO ET AL.
19
Soil as a Source of Indoor Radon π • 1 » NARR: Chico Quadrangle AM
= 19.1
ASD = 6.57 GM = 18.2
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GSD = 1.35
40.00
40.00
80.00 120.00 Radium (Bq/kg soil)
160.00
200.00
80.00 120.00 Radium (Bq/kg soil)
160.00
200.00
F i g u r e 3. D i s t r i b u t i o n o f s u r f a c e radium c o n c e n t r a t i o n s f o r a quadrangle (a) w i t h a GM < 20 Bq k g " and f o r a q u a d r a n g l e (b) w i t h a GM > 40 Bq k g . The c u r v e s r e p r e s e n t lognormal distri b u t i o n s b a s e d on t h e d i s t r i b u t i o n p a r a m e t e r s c a l c u l a t e d from the data. 1
1
Hopke; Radon and Its Decay Products ACS Symposium Series; American Chemical Society: Washington, DC, 1987.
20
RADON AND ITS DECAY PRODUCTS
226
• = < 20 Bq/kg soil • =
20-40
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Pennsylvania
76
W
75 30'W
Ra
· =
40-60
· =
ê 60
New Jersey
75
W
74 30'W
74
W
F i g u r e 4. The s p a t i a l d i s t r i b u t i o n o f i n f e r r e d s u r f a c e radium concentrations f o r t h e Newark Q u a d r a n g l e , covering eastern Pennsylvania and n o r t h e r n New J e r s e y . The s t a t e boundaries a r e shown as s o l i d l i n e s , w h i l e t h e c o u n t y b o u n d a r i e s a r e i n d i c a t e d by broken l i n e s . The s p a c i n g b e t w e e n f l i g h t l i n e s i s 6 m i l e s , and e a c h p o i n t r e p r e s e n t s d a t a a v e r a g e d a l o n g s i x m i l e s of each f l i g h t l i n e .
Hopke; Radon and Its Decay Products ACS Symposium Series; American Chemical Society: Washington, DC, 1987.
2.
SEXTRO ET AL.
21
Soil as a Source of Indoor Radon
the data. Such a f i e l d v a l i d a t i o n study has been conducted f o r c o m p a r i s o n w i t h NARR a e r i a l d a t a o b t a i n e d i n t h e Spokane, WA, a r e a . One m i l e segments o f two d i f f e r e n t f l i g h t l i n e s were i n v e s t i g a t e d ; e a c h t r a v e r s e d g r a n i t i c o u t c r o p s and t h e a e r i a l d a t a f o r t h o s e f l i g h t - l i n e segments showed c o n s i d e r a b l e v a r i a t i o n . I n gene r a l , a correspondence was o b s e r v e d b e t w e e n t h e r a d i u m c o n c e n t r a t i o n s b a s e d on t h e a e r i a l d a t a a n d t h e 1 n-gl-hu m e a s u r e m e n t s o f r a d i u m c o n t e n t a n d r a d o n f l u x from s o i l (Moed eJ: a l - 1984) .
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f
As n o t e d i n T a b l e I , a v e r a g e s u r f a c e r a d i u m c o n c e n t r a t i o n s a p p e a r t o v a r y b y a b o u t a f a c t o r o f 20. T h i s can a l s o be seen f r o m t h e d i s t r i b u t i o n s from t h e NARR d a t a . S o i l p e r m e a b i l i t i e s , on t h e o t h e r hand, h a v e much l a r g e r v a r i a t i o n s , a n d t h u s , i n p r i n c i p l e , may h a v e a g r e a t e r i n f l u e n c e on t h e s p a t i a l v a r i a t i o n s i n average i n d o o r radon c o n c e n t r a t i o n s t h a t have been observed. As w i t h t h e case o f s u r f a c e radium c o n c e n t r a t i o n s , t h e s p a t i a l v a r i a b i l i t y o f a i r p e r m e a b i l i t i e s o f s o i l s i s an i m p o r t a n t e l e m e n t i n developing a predictive capability. I n f o r m a t i o n on s u r f a c e s o i l s i s a v a i l a b l e from a number o f s o u r c e s , i n c l u d i n g s u r f a c e s o i l maps c o m p i l e d b y t h e U.S. G e o l o g i c a l S u r v e y and t h e g e o l o g i c a l s u r v e y s o f v a r i o u s s t a t e s . At the p r e s e n t t i m e , t h e c o v e r a g e o f s u c h maps i s n o t c o m p l e t e , n o r h a s any s y s t e m a t i c d a t a on a i r p e r m e a b i l i t y o f s o i l s b e e n compiled. However r e p o r t s i s s u e d b y t h e S o i l C o n s e r v a t i o n S e r v i c e (SCS) o f t h e U.S. D e p a r t m e n t o f A g r i c u l t u r e c o n t a i n i n f o r m a t i o n on most s o i l s on a c o u n t y - b y - c o u n t y b a s i s . W h i l e no d i r e c t a i r p e r m e a b i l ity information i s contained i n these r e p o r t s , t h e d a t a and d e s c r i p t i v e m a t e r i a l c o n t a i n e d t h e r e may b e u s e f u l i n e s t i m a t i n g air permeabilities. We h a v e u s e d t h e s e i n d i c a t o r s t o e s t i m a t e p e r m e a b i l i t y v a l u e s f o r s u r f a c e s o i l s i n Spokane C o u n t y , WA. A g e n e r a l s o i l map o f t h i s c o u n t y i s shown i n F i g u r e 5. T h e s p a t i a l e x t e n t o f two s o i l associations, the Naff-Larkin-Freeman a s s o c i a t i o n ( a r e a 1) and the Garrison-Marble-Springdale a s s o c i a t i o n ( a r e a 2) , a r e s h a d e d in the figure, and d e t a i l e d e s t i m a t e s o f a i r p e r m e a b i l i t y f o r t h e s e two a s s o c i a t i o n h a v e b e e n made, a s d e s c r i b e d b r i e f l y b e l o w . More i n f o r m a t i o n i s g i v e n i n N a z a r o f f a t a T . (1986). r
The N a f f - L a r k i n - F r e e m a n a s s o c i a t i o n c o n t a i n s f i n e - t o mediumtextured s o i l s , moderately-well t o wel1-drained. The G a r r i s o n Marble-Springdale soils, on t h e o t h e r hand, a r e g r a v e l l y and s a n d y ( c o a r s e - t e x t u r e d ) a n d a r e " s o m e w h a t - e x c e s s i v e l y " t o "excess i v e l y " d r a i n e d (USDA, 1 9 6 8 ) . In a d d i t i o n t o t h e s o i l t e x t u r e s , water p e r m e a b i l i t i e s a r e d e s c r i b e d q u a l i t a t i v e l y f o r these s o i l s , l e a d i n g t o t h e e s t i m a t e d r a n g e o f i n t r i n s i c p e r m e a b i l i t i e s shown i n T a b l e I I I f o r t h e s e two s o i l a s s o c i a t i o n s . T h e r e a r e a number o f u n c e r t a i n t i e s a s s o c i a t e d w i t h e s t i m a t ing a i r permeabilities i n this way. The s o i l associations d e s c r i b e d b y t h e SCS on t h e c o u n t y maps g e n e r a l l y c o n s i s t o f one o r more m a j o r s o i l s e r i e s a n d may a l s o i n c l u d e one o r more m i n o r soil series. T h e f r a c t i o n o f t h e mapped a r e a o c c u p i e d b y t h e s e minor soil series, and t h e d e g r e e o f s i m i l a r i t y of physical
Hopke; Radon and Its Decay Products ACS Symposium Series; American Chemical Society: Washington, DC, 1987.
RADON AND ITS DECAY PRODUCTS
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22
F i g u r e 5. G e n e r a l s o i l map from t h e S o i l C o n s e r v a t i o n Service for Spokane C o u n t y , WA. Two s o i l associations discussed i n the t e x t a r e shaded. The Spokane R i v e r i s i n d i c a t e d b y a dashed line and t h e a p p r o x i m a t e boundary f o r the c i t y of Spokane i s shown b y a h e a v y b o r d e r .
Hopke; Radon and Its Decay Products ACS Symposium Series; American Chemical Society: Washington, DC, 1987.
2.
SEXTRO ET AL.
23
Soil as a Source of Indoor Radon
p r o p e r t i e s b e t w e e n t h e m a j o r and m i n o r s o i l s will c o n t r o l the u n c e r t a i n t i e s a s s o c i a t e d with the d e r i v a t i o n of s o i l c h a r a c t e r i s t i c s for a given geographical area. I n t h e c a s e o f t h e two soil a s s o c i a t i o n s d i s c u s s e d h e r e , 77 t o 80% o f t h e r e s p e c t i v e mapped a r e a s a r e a c t u a l l y o c c u p i e d by t h e m a j o r s o i l s e r i e s .
Table
III.
P e r m e a b i l i t i e s of s e l e c t e d s o i l s
i n Spokane C o u n t y ,
Permeability
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Soil
Naff-LarkinFreeman
1θ"
Garrison-MarbleSpringdale
10"
1 4
1 2
to
10"
1 2
to
ΙΟ"
1 0
-2
X
(0.3
P e t a l Ίed
S U f t - g p p r i f^r.
StndUs.
)
M e a s u r e d by (Range)
D e r i v e d from SCS Information
Association
(m
Experimental
10
WA
LBL
11
- 60)
X
10
11
measurements
of
p a r a m e t e r s a f f e c t i n g s o i l gas t r a n s p o r t and e n t r y i n t o h o u s e s i s very limited. One r e c e n t s t u d y o f two homes w i t h b a s e m e n t s h a s d e m o n s t r a t e d c o u p l i n g b e t w e e n t h e b u i l d i n g s h e l l and t h e s u r r o u n d i n g s o i l and m e a s u r e d c o n v e c t i v e f l o w t h r o u g h t h e s o i l (Nazaroff s i . a l . , 1985b) . U t i l i z i n g an a r r a y o f s o i l p r o b e s surrounding e a c h h o u s e and by d e p r e s s u r i z i n g t h e basement u s i n g a b l o w e r door, the resulting negative pressure field i n the soil was mapped. The e f f e c t o f t h e e n h a n c e d b a s e m e n t d e p r e s s u r i z a t i o n was s e e n a t d i s t a n c e s up t o 5 m from t h e basement w a l l f o r one h o u s e and up t o 3 m i n t h e o t h e r . S o i l gas f l o w s , m e a s u r e d utilizing SFg as a t r a c e r gas, were a l s o d e t e r m i n e d . I n one c a s e n e t m i g r a t i o n v e l o c i t i e s of g r e a t e r than 1 m h were o b s e r v e d w i t h a base ment d e p r e s s u r i z a t i o n o f 30 Pa a t an i n j e c t i o n p o i n t 1.5 m from t h e basement w a l l . 1
A similar set of experiments were c o n d u c t e d as part of d e t a i l e d r a d o n i n v e s t i g a t i o n s i n one h o u s e i n t h e Spokane (WA) area. The pressure-field i n the surrounding soil was mapped u s i n g t e c h n i q u e s d e s c r i b e d i n N a z a r o f f a t aT.. (1985b). S o i l per m e a b i l i t i e s were m e a s u r e d 1η-s! t u u t i l i z i n g an a i r p e r m e a m e t e r s i m i l a r t o t h a t d i s c u s s e d i n DSMA, (1983) . An a r r a y o f 30 s o i l p r o b e s was p l a c e d i n t h e s o i l s u r r o u n d i n g t h e h o u s e , as c a n be s e e n from F i g u r e 6. The p r o b e d e p t h s r a n g e d from 0.5 to 1 m d e e p ; t h e d e p t h s were u s u a l l y l i m i t e d b y t h e a b i l i t y t o p e n e t r a t e t h e s o i l w h i c h c o n t a i n e d a l a r g e number o f r o c k s o f v a r y i n g s i z e s s c a t t e r e d t h r o u g h o u t the s o i l column. The d e e p e s t p r o b e s , with s o i l d e p t h s b e t w e e n 0.8 and 1.0 m, are i n d i c a t e d i n the figure w i t h s q u a r e s , w h i l e p r o b e s w i t h d e p t h s b e t w e e n 0.5 and 0.7 m a r e
Hopke; Radon and Its Decay Products ACS Symposium Series; American Chemical Society: Washington, DC, 1987.
24
RADON AND ITS DECAY PRODUCTS
6.5i •1.5 •5.3
Downloaded by CORNELL UNIV on June 4, 2017 | http://pubs.acs.org Publication Date: February 5, 1987 | doi: 10.1021/bk-1987-0331.ch002
Porch (slab) I
6.3· 4.2·
7.6 1
7.2·£ ·7·8 •6.3
Basement Perimeter
U#7.0
4.6·
5.2· 4.6
•4.6
|-Jb8.4
5.3 4.4