Journal of

ELSEVIER

Hydrolc
Journal of Hydrology 195 (1997) 45-77

222Rn transport in a fractured crystalline rock aquifer: results

from numerical simulations

Peter F. F o l g e r a'b, E i l e e n P o e t e r b, R i c h a r d B. W a n t y c, W a r r e n D a y c, David Fdshman c
=Offu:eof Senator Pete V. Domenici, United States Senate, Washington, DC 20510, USA bColorado School of Mines, Department of Geology and Geological Engineering, Golden, CO 80401, USA U.S. GeologicalSurvey, M.S. 973, Denver Federal Center, Denver, CO 80225, USA

Received 8 July 1996; revised 31 July 1996; accepted 8 August 1996

Abstract Dissolved "~Rn concentrations in ground water from a small wellfield underlain by fractured Middle Proterozoic Pikes Peak Granite southwest of Denver, Colorado range from 124 to 840 kBq m -3 (3360-22700 pCi L-~). Numerical simulations of flow and transport between two wells show that differences in equivalent hydraulic aperture of transmissive fractures, assuming a simplified two-fracture system and the parallel-plate model, can account for the different ~aRn concentrations in each well under steady-state conditions. Transient flow and transport simulations show that ~ R n concentrations along the fracture profile are influenced by 2"Rn concentrations in the adjoining fracture and depend on boundary conditions, proximity of the pumping well to the fracture intersection, transmissivity of the conductive fractures, and pumping rate. Non-homogeneous distribution (point sources) of 222Rnparent radionuclides, uranium and 2~'Ra, can strongly perturb the dissolved " R n concentrations in a fracture system. Without detailed information on the geometry and hydraulic properties of the connected fracture system, it may be impossible to distinguish the influence of factors controlling 2~'Rn distribution or to determine location of 222Rnpoint sources in the field in areas where ground water exhibits moderate 222Rnconcentrations. Flow and transport simulations of a hypothetical muitifracture system consisting of ten connected fractures, each 10 m in length with fracture apertures ranging from 0.1 to 1.0 mm, show that 2~Rn concentrations at the pumping well can vary significantly over time. Assuming parallel-plate flow, transmissivities of the hypothetical system vary over four orders of magnitude because mmsmissivity varies with the cube of fracture aperture. The extreme hydraulic heterogeneity of the simple hypothetical system leads to widely ranging 2Z2Rn values, even assuming homogeneous distribution of uranium and ~ R a along fracture walls. Consequently, it is concluded that 2~Rn concentrations vary, not only with the geometric and stress factors noted above, but also according to local fracture aperture distribution, local groundwater residence time, and flux of ~ R n from parent radionuclides along fracture walls.

0022-1694/97/$17.00 O 1997 Published by ElsevierScience B.V. All rightsreserved PII S0022-1694(96)03243-X

46

P.F. Folger et alJJournal of Hydrology 195 (1997) 45-77

1. Introduction Recently proposed water quality regulations for 222Rn in ground water (a maximum contaminant level (MCL) of 11.1 kBq m-3; 300 pCi L -1, EPA, 1991) have incited interest in understanding processes occurring in and characteristics of aquifers that control 222Rn concentration. Impacts of the proposed ruling may be economically significant nationwide, potentially affecting 33000 water suppliers (Rancher and Drago, 1992) and costing several billion dollars annually. Rancher and Drago (1992) suggest that smaller suppliers (serving less than 500 people) may suffer the greatest economic impact. Small water suppliers and single homes in the Colorado Front Range typically draw water from wells completed in fractured Precambrian granites and metamorphic rocks that contain above crustal average concentrations of uranium. Studies have demonstrated that these wells supply water that almost invariably exceeds the proposed MCL (Lawrence, 1990; Lawrence et al., 1991, 1992; Wanty et al., 1991; Folger et al., 1993, 1994). This paper presents results of field investigations and numerical modelling studies which further our understanding of the distribution of dissolved 2aRn in a fractured rock aquifer as a function of: 1. 222Rnparent radionuclides (uranium and 226Ra); 2. fracture aperture; and 3. ground water flow velocity (conversely, local ground water residence time). This study is concerned with the distribution of dissolved 222Rnon the scale of a single dwelling supplied by one well, or a small mountain-community with well spacings on the order of tens to hundreds of meters. The numerical model discussed below simulates fractures as either single or connected individual flow conduits. Each fracture is assumed to be smooth-walled with finite dimensions, consequently transmissivity (T) varies in the fracture with the third power of the aperture (the well-known cubic law):
T =,y(b)3 /12l ~

(1)

where ~ is the specific weight of water, b is fracture aperture, and p is dynamic viscosity. Both homogeneous and heterogeneous distribution of 226Ra (the radioactive parent of 222Rn) along fracture walls is considered. Emanating power (the amount of 222Rn that enters the fracture void versus the amount of 222Rngenerated in the rock; Tanner, 1964) is assumed to be constant for each scenario, although a homogeneous distribution of 226Ra along a fracture with a differing emanating power is effectively similar to a heterogeneous 226Ra distribution along the fracture wall. Many analytical and numerical solutions have been developed to describe fluid flow and mmsport in fractures (Warren and Root, 1963; Grisak and Pickens, 1980; Shapiro, 1981; Chen, 1986; Huyakoru et al., 1991; and many others). These models include both discrete fracture solutions and combined or dual porosity solutions that couple fluid processes in a permeable matrix with processes in fractures (Streltsova, 1976). Numerical and analytical models applicable to nuclear waste repositories have emphasized the importance of molecular diffusion of a contaminant from a fracture into a hydraulically impermeable matrix, such as granite (Tang et al., 1981; Sudicky and Frind, 1982; Huyakorn et al.,

P.F. Folger et alJJournai of Hydrology 195 (1997) 45-77

47

1991). In these models, the source of radioactive contamination is introduced into the natural system (e.g. a breached waste container or spill). The problem in these cases involves defining the source term and simulating contaminant migration via advection, hydrodynamic dispersion, molecular diffusion, adsorption, and radioactive decay. Conversely, the source of naturally occurring 2nRn is the rocks themselves. When the immediate parent of ~ R n , decays by alpha emission near the water/rock interface, ~2Rn enters the ground water by alpha recoil (Krishnaswami and Seidemann, 1988). Consequently, the emanating power depends on the distance between the 2~'Ra atom and rock-water boundary relative to the alpha recoil distance (Flttgge and Zimens, 1939), as well as on the geometry of the crystal and fracture surface area (Semkow, 1990; Torgersen et al., 1990). Also, processes of dissolution and sorption tend to redistribute uranium and radium in the aquifer, resulting in heterogeneous accumulations of 2~Rn parent radionuclides along fracture walls (Torgersen et al., 1990; Wanty et al., 1991). Therefore, a representative model for 2~Rn transport must account for a continuous, perhaps heterogeneous, source of ~2Rn from the fracture walls throughout the model domain. Numerical modelling allows us to investigate the sensitivity of 2~Rn concentrations in a simplified fractured rock aquifer to aquifer properties measured or estimated in the field. Dissolved ~ R n concentrations in ground water in the Elk Creek Basin near Denver, CO, (Fig. 1) range from 37 to 930 kBq m -3. Concentrations as high as 110000 kBq m -3 have been reported nearby (Lawrence et al., 1991). Even within a single rock type in an area less than 2.5 km 2, 222Rnconcentrations can range from 124 to 840 kBq m -3 (Folger et al., 1996). Aquifer heterogeneity is responsible for the wide range of 222Rn concentrations observed in nature. However, in the field, it may be impossible to distinguish the separate influences of 222Rn source (distribution and emanating power of 226Ra), fracture aperture (dilution at small scale), and ground water residence time (inverse of ground water velocity). Numerical modelling allows us to investigate the sensitivity of 222Rn concentrations in a simplified fractured rock aquifer to aquifer properties measured in the field.

2. The study area

The study area lies within the Elk Creek drainage basin southwest of Denver, near the communities of Conifer and Pine Junction, Colorado (Fig. 1). Eleven wells are completed in Middle Proterozoic Pikes Peak Granite (Bryant et ai., 1981), which is dominantly a coarse grained, equigranular biotite-hornblende granite. 37 samples collected from outcrops of Pikes Peak Granite in the Elk Creek drainage contain an average of five parts per million (ppm) uranium (Frishman et al., unpublished data, 1993). Detailed mapping of an outcrop in the study area (Frishman et al., 1993) revealed that, as in many other areas in the Pikes Peak batholith, numerous aplite dikes and thin pegmatites cut the dominant coarsegrained lithology (Hutchinson, 1988). Frishman et al. (1993, and unpublished data) also showed that uranium and radium concentrations can vary over nearly two orders of magnitude within one moderately sized outcrop of Pikes Peak Granite despite only minor textural variation. Presence of uranium-bearing minerals, such as thorite, results in discrete local zones of high gamma radioactivity in the outcrop over the scale of meters.

48

P;F. Folger et al./Journal of Hydrology 195 (1997) 45-77

ypp

B*.in

A~F~.~

0
I , ,

J
I l | I ,

o 105030 .

b.

/
0
92co-18

' )

, n

200

400 ft
i

w,,~er i l ~

cont~,t (m)-

50

I00 m

water levelsI

June 1992

topogriph~ coulour(m)
O

well Iogllot ill.physically

wellnot logged

Fig. 1. (a) Regional geologic map of study area showing the outline of the Elk Creek catchment rare8and general location of the well field. Mapping simplified from Bryant, 1974a,b, 1976, and B. Bryant, unpublished data, 1974: and (b) location map of the well field showing topography and water table contours. Ground surface elevation at well 92(20-14 is datum. Absolute elevation is approximately 2560 m (8400 ft) above sea level. Map symbols are as follows: Ypp, Pikes Peak Granite (Middle Proterozoic); Ysp, Silver Plume Quartz Monzonite (Middle Proterozoic); Xm, migmatite (Early Proterozoic).

P.F. Folger et alYJournal of Hydrology 195 (1997) 45-77

49

Proximity of these "hot spots" to the rock-water interface determines their potential for producing anomalous amounts of 222Rn in ground water. Local accumulations of uranium and 226Ra are probably responsible for extremely high 2~Rn concentrations (5140 kBq m-3; 139000 pCi L -l) reported in Colorado (Lawrence, 1990). Soil cover is thin or nonexistent in the study area; hence, most ground water flows through fractures in the granite. The potentiometric surface is a subdued expression of topography but is displaced to the south (Fig. 1Co)), possibly owing to the influence of steep high topography north of the well field. Although fractures control flow, waterbearing fractures are sufficiently connected so that the shape of the potentiometfic surface suggests that unconfined flow conditions prevail. A relatively steep hydraulic gradient separates well 92CO-11 from well 92CO-15 (Fig. l(b)), suggesting a zone of lower transmissivity between these two wells. Hsieh and Shapiro (1993) showed that widely varying transmissivity (T; estimated from single- and cross-hole aquifer tests using the Theim equation) is common in heterogeneous fractured rock. The fracture geometry is critical to solute transport as indicated by Tsang (1993), who states that fracture heterogeneity has a much stronger influence on solute transport than on heat transport or pressure propagation. Therefore, 222Rn concentration in ground water depends strongly on individual flow paths from well to well. Accordingly, detailed geophysical logs of four wells were collected to characterize the radioactivity, fracture patterns, and flow properties at the scale of a single well. Borehole geophysics, including acoustic televiewer (ATV), heat-pulse flowmeter (HPF), and natural gamma logs were performed on four wells, 92CO-14, 92CO-16, 92CO-15, and 93CO-1 (Fig. l(b)). The ATV and HPF logs indicate that single fractures provide all of the flow to wells 92CO-14, 92CO-15, and 93 CO-1, and that a single fracture provides at least 65% of the flow to well 92CO-16. Other workers have observed that only a small number of fractures contribute flow to wells drilled in crystalline rocks despite the presence of tens to hundreds of fractures intersecting the borehole (Palllet et al., 1989, 1992; Hsieh and Shapiro, 1993; Paillet, 1993). The degree of interconnection between transmissive fractures in crystalline rock is commonly difficult to quantify without extensive aquifer testing using straddle packers to isolate producing fractures or fracture zones (Hsieh and Neomann, 1985a, b; Hsieh and Shapiro, 1993). Nevertheless, openborehole testing of the four wells indicates that wells 92CO-14 and 92CO-16 are hydraulically connected, as are the pair 92CO-15 and 93CO-1. Pumpingdurations of less than 3 h (at pumping rates between 3 and 25 L min -l) failed to produce measurable drawdown (greater than 0.015 m) between the two well pairs. Single-well aquifer tests in the well field indicate that transmissivities range from 0.07 to 160 m 2 per day. Each test was performed without packers, and therefore transmissivities represent the contribution of all flowing fractures intersecting the borehole. Methods used for performing aquifer tests and an analysis of their results are discussed in Folger et al. (1996). Log-log graphs of drawdown data from single-well aquifer tests of wells 92CO-14 and 92CO-16 suggest that the wells exhibit contrasting flow behavior during the test. Drawdown versus time in well 92CO-14 matches the Tbeis solution for radial flow during early time, but latex time data indicate a constant-head boundary or leakage after approximately 8 min of pumping. Interpretation of early time data on a log-log plot suggests a T of

50

P.F. Folser et al./Journal of Hydrology 195 (1997)45-77

2.9 m 2 per day for the single fracture producing in well 92CO-14 (Folger et al., 1996). A log-log graph of drawdown versus time for well 92CO-16 shows straight line behavior indicating linear flow to the well (Gringarten, 1982; Jenkins and Prentice, 1982; Sen, 1986). Interpretation of the straight-line behavior using the single vertical fracture model of Gringarten and Witherspoon (1972) indicates a T of 0.9 m 2 per day for the major producing fracture intersecting well 92CO-16 (Folger et al., 1996). Hydraulic apertures (HA), calculated using Eq. (1), are 0.38 and 0.24 mm for wells 92CO-14 and 92CO-16, respectively. Given that single fractures dominate flow to each of the four wells, Folger et al. (1996) demonstrated that differences in hydraulic apertures of the flowing fractures, calculated using the cubic law, can explain the differences in ~"2Rnconcentration measured between the wells in each pair. These calculations assumed homogeneous distribution of 2~'Ra along all fracture walls, constant emanating power, and long ground water residence time in each fracture relative to the 2~Rn half-llfe (3.82 days). Consequently, 2~Rn concentration in the ground water is at steady-state with respect to ~ R n generated by the rock, and varies inversely with fracture aperture. Calculations also showed that different hydraulic fracture apertures fail to explain differences in 2~Rn concentration between well pairs, indicating that one or more of the above assumptions was invalid when the calculations included all four wells.

3. Methods

This paper explores the relationship between fracture aperture and ~ R n concentration, incorporates transient flow conditions and heterogeneous distribution of 2~'Ra along fracture walls, and tests sensitivity of ~2Rn concentration to ground water velocity by varying the natural hydraulic gradient. To do so, flow and transport between wells 92CO-14 and 92CO-16 is simulated using the numerical model MT3D (Zheng, 1993). MT3D uses the method of characteristics (MOC), modified method of characteristics (MMOC), or a hybrid of the two algorithms to solve the advection-dispersion equation for solute transport. An irreversible first-order rate term accommodates 222Rndecay. MT3D uses output from any finite-difference block-centered flow model. MODFLOW (McDonald and Harbaugh, 1988) was chosen to simulate flow in the fractures. The MODFLOW grid represents flow in the fracture openings only, not flow occurring through the matrix into or out of the fractures which is assumed to be negligible.

4. Results and discussion

4.1. One-fracture system

Domenico (1987) developed an analytical model for one-dimensional ground water flow, longitudinal and transverse dispersion, and radioactive decay. To compare numerical results for ~'~Rn transport in a single fracture using MT3D against the Domenico (1987)

P.F. Folger et al./Journal of Hydrology 195 (1997)45-77 1 0.9 0.8 0.7 o.e Doawnt~o (1 seT) ene~e~ ~t,~on

51

0.1

.....
0 , i

~,.-..~._-.
i --

. . . . . .

50

1 O0

150 distance (m)

200

250

300

Fig. 2. Resultsof a one-di~ional analytical solutionfor 222Rntransport(Domenico, 1987)comparedwith the MT3D numerical model resultsfor the same parameters.Co refers to source concentration.Arrowsindicate that distance downgmdientcorrespondingto one half-life (3.82 days) is 38 m. model, a simple one-fracture system of constant aperture and a 222Rn point source was constructed. The numerical model consists of one layer 0.24 m m thick (corresponding to the calculated hydraulic apemn'e of the main producing fracture intersecting well 92CO- 16), 50 columns each 1 0 m wide, and a single row 1 0 m wide. Constant hydraulic conductivity (K) of 3744 m per day, calculated assuming parallel-plate flow, is assigned to each cell. Transport is assumed to be advection-dominated in the single fracture with a longitudinal (or,) dispersivity of 0.1 m. A total head drop across the model of 1.335 m is prescribed, resulting in a constant hydraulic gradient 03 of 2.67 x 10 -3 m m -] under steady-state flow. Assuming porosity (~b) in the fracture is 1.0, then steady-state average linear ground water velocity (v) in the system is 10 m per day by:

v=Ki/e~.

(2)

A constant 222Rn source is simulated by applying a small recharge (1.44 10 -37 m per day) t o the source cell, and assigning a large 222Rn concentration (1.44 x 10 32 kg m -3) to the recharge water. The net effect is injection of mass at one grid block in the model without disturbing the steady-state flow system. The same values of v and o~ are included in the Domenico (1987) solution. The dimensions of the source term in the analytical model are very large, so that concentrations vary only in the direction of advective transport. For both the analytical and numerical models, the half-life of the solute is 3.82 days, corresponding to 222Rn. Concentrations in the simulations, are evaluated under steady-state flow conditions. The MT3D and analytical model solution to the single fracture problem are identical lending credence to the numerical model (Fig. 2). The ratio of concentration to starting concentration (C/Co) is 0.5 at a location 38 m downgradient of the source for both

52

P.F. Folger et al./Journal of Hydrology 195 (1997) 45-77

solutions, corresponding to a ground water residence time of one half-'life. After seven half-lives (approximately 270 m from the source), most of the original mass of 222Rn has decayed away (Fig. 2). The analytical solution will suffice for simple one-dimensional problems involving steady-state flow and a single point source in an isotropic and homogeneous system. However, fractured crystalline rock aquifers are inherently heterogeneous and simple analytical solutions for flow and transport are generally inadequate. Moreover, 222Rn is naturally occurring and is produced in crystalline rocks wherever its radioactive parents are located. Therefore, a single point source may be adequate only for problems involving a localized accumulation of uranium and Ra. Accordingly, a numerical model is required to evaluate field conditions.
4.2. Two-fracture system

The simplest physical description of the fracture system between 92CO-14 and 92CO-16 is a connected two fracture model (Fig. 3). Although two-well aquifer tests indicate that the wells are hydraulically connected, the flow path between wells is unknown. The minimum flow path length is 34 m, the distance between wells. The MODFLOW flow model for the two-fracture system consists of five rows, each one meter wide in the y dimension, 60 columns of variable width in the x dimension and a single layer with two different thicknesses (Fig. 4). The smallest cell dimension in the x direction is 2 m. The different layer thicknesses correspond to hydraulic apertures of the producing fractures in wells 92CO-14 and 92CO-16. The fracture intersection is located at the center of the model, where layer thickness changes. Constant head boundaries are assigned to all rows in columns one and 60, and higher head is assigned to column one so that flow is from the small fracture to the large fracture under steady-state conditions. All other active cells are variable head. To simulate leakage via a connection with a prolific fracture or fractures suggested by aquifer tests (discussed below), constant head boundaries are assigned to rows 1 and 5, columns 38 through 60 during transient flow simulations (Fig. 4). Starting heads for the transient simulations of pumping represent values calculated under steady-state flow conditions without pumping. Hydraulic conductivities assigned to each layer in the MODFLOW model are derived from single fracture transmissivities determined by aquifer testing. For well 92CO-14, T equals 3.0 m 2 per day, resulting in a K of 7900 m per day by:
g=T/b

(3)

where b is fracture aperture. Similarly, Tfor well 92CO-16 is 0.9 m 2 per day, giving a K o f 3800 m per day for the layer representing the main producing fracture. To simulate continuous production of 222Rn from fracture walls in the system, recharge of 1.44 10 -37 m per day is applied to all active cells with a 222Rnconcentration of 1.44 1032 kg m -3. The amount of mass injected is arbitrarily selected, and is not related to actual 222Rnproduction rates in the aquifer, other than to meet an initial assumption of homogeneous 226Ra distribution. Heterogeneous 222Rn production along fracture walls is simulated by changing the concentration or recharge rate of selected cells. The 222Rn decay constant is 0.1814 per day On(2)/half-lifeR~), and because 222Rn is

P.F. Foiger et alJJournal of Hydrology 195 (1997) 4 5 - 77

53

[Rn]=,760Id3qm? (20,500pCi I") (11,800pOi r,) ~o-1~

m?

meters --5

i _~----10 5 - - -,V,-

~ w a t
20 18.3 m

hodzontaiflructwe
at 13.3 m 34m

+M

~kx~ o( t~0-fmc4um~ t o m Smd-~tum tr~tum hm:dum Fig. 3. Downhole acoustic televiewer logs of the upper sections of wells 92CO-14 and 92CO-16. Triangles indicate water table elevations in both wells. Producing fractures were located using the heat-pulse flowmeter tool. Conceptualmodelsof the two-fractmesystemcoctegm~ing to producingfractures at 18.3 m (well 92CO-16) and 13.3 m (well 92CO-14) are shown below the televiewer logs. chemically inert and not involved in adsorption reactions, the retardation factor is 1.0. Porosity in the fracture is assumed to he 1.0 and longitudinal and transverse dispersivity are 1.0 and 0.03 m, respectively. The hybrid algorithm (HMOC), a combination of M O C and M M O C solutions, is used because it is more suitable for advection-dominated problems (Zheng, 1993). Comparison of the Euler algorithm versus the Runge-Kutta fourth-order algorithm to solve advection results in little difference in final 2~Rn concentrations; thus, the Euler algorithm was used because it required less CPU time. Pumping rates in the transient simulations match field pumping rates for single-well

~,
"

'

54

P.F. Folger et alJJournalof Hydrology 195 (1997) 45-77

plan view 60metezs

I I

80 meteau
I

60 meters
I

I i I I I I I I Illlllllllllllllli/z

I I I I

I I I I

I I I I

I I I I

I 111111111111111111111111111111111111111111111 I I IIIIlllllllkllllllllllllllllllllqlllllllllllll IIIIIIllllllllllllllllllllllll]llllllll[llllllll I I I IIII; n'n'''''nlq'

ii

i i i I I I II I

i I I

i I I

~ y
i i|

ZL_
x

Well

fractureintersection well 92CO-14 - - . No flowboondary ---- Constantheadboondaty Pumping well cross section ~.le layer,twe thickne~ 0.38 mmwide ~ flowout

flowin ~

0,24 mmwide

'

Fig. 4. Plan and cross-sectionview of the MODFLOWgrid representinga connected two-fracturesystem. Both wells are 20 m fromthe fractureintersection,givinga flowpathlength of 40 m betweenwells.The arrowindicates point source location for numerical simulations. The cross section indicates-hydraulic aperture of fractures, corresponding to low (well 92CO-16) and high (well 92CO-14) transmissivityfractures. aquifer tests of wells 92CO-14 and 92CO-16 at 35 and 25 m 3 per day, respectively. Concentration of the pumped water is equal to the model-calculated 222Rn concentration in that cell.

4.2.1. Flow in the two-fracture system under steady-state and transient conditions MODFLOW was used here to simulate single well aquifer tests in the two-fracture model. By adjusting boundary conditions and location of the pumping wells, model simulations matched field drawdown data reasonably well at the pumping wells (Fig. 5). The drawdown versus time plot of field data from well 92CO-16 falls nearly on a straight line (Fig. 5(a)), suggesting linear flow behavior in the near-well fracture system (Gringarten, 1982; Folger et al., 1996). Drawdown data from the 92CO-14 aquifer test indicates radial flow or pseudo-radial flow in very early time (less than 8 rain; Fig. 5(b)). However, at later time drawdown increases slowly suggesting that leakage occurs or a constant-head boundary is encountered after 8 rain of pumping. The model boundary conditions described above produce drawdown versus time graphs that match these diagnostic patterns, and fit the field data reasonably well (Fig. 5). Changing the location of the pumping wells in the large and small fractures has only a minor effect on drawdown results. Locating wells 92CO-16 and 92CO-14 20 m from the fracture intersection (so that the wells are 40 m apart) produces drawdown versus time graphs that match the field data well. The model results are very sensitive to storativity, which could not be estimated from field tests because drawdown data were collected only at the pumping well. Assigning storativity (which represents specific yield of the fractured aquifer) of 0.012 to both fractures produces results most closely matching the aquifer test

P.F. Foiger et alJJournal of Hydrology 195 (1997) 45-77

0.1

55

10

100

100

10
4"

i
q~

0.1

0.01

100

"P

10

.g
"13

0.1

0.01 0.1 1 time (rain) 10

100

Fig. 5. Drawdown versus time from single-well aquifer tests completed 7 August 1992 compared against MODFLOW (model) simulation. (a) For well 92C0-16 with pumping rate (Q) of 25 m 3 per day; and (b) for well 92C014 with pumping rate (Q) of 35 m 3 pet day.

data. This is consistent with total porosities ranging from 0.0107 to 0.0232 as measured by Wood et al. 0993) in 32 granite samples. Calibration of the model to field tests does not imply that there is a unique solution to the problem, however, it provides a reasonable starting point for transport simulations.

4.2.2. Rn transport in the two-fracture system under steady-state conditions Under steady-state flow conditions in the two-fracture system with uniformly distributed 2 ~ a , ~ R n concentrations along the fracture depend on residence time (time required to achieve equilibrium with parent 2Z6Ra),and vary inversely with fracture aperture. The objective of simulating the ~ R n concentration profile under steadystate conditions is to reproduce the observed ~ R n concentrations in wells 92CO-14 and 92CO-16, assuming that pumping has not disturbed steady-state 2~Rn concentrations significantly. Simulations under transient flow conditions, described below, demonstrate that this assumption depends on pumping duration, boundary conditions assumed in the model, and contrast in hydraulic apertures of connected fractures. Prescribing fixed heads in the first and last columns of the model with a linear decline in

56

P.F. Folger et aNJouma1 of Hydrology195 (1997) 45-77

iI

o.so --

0.80 -r 0.20 -0.10 -0.00

fmmfl8alun intrnrcllon _ SEgL m

; * * * '; wall a?com

* . ' 'Ib' a . ii'

* ' .I*

. * t*

' ' '90' .?

'is'

' ' j;,l,

dbtUlWhocnWd22CM2

Fig.6. Results from numericalsimulations showing steady-stateconcentrationsin the smell (0.24 mm hydraulic
apert@ and large (0.38 mm hydraulic apertme) fractures.Flow is from left to right (smell qerture fmcture towardslarge apcmm fracture).C. refers to steady-state %n concentration in the small fracture(hydraulic aperture equals 0.24 mm). Steady-stateconcentrationis achieved when C/C. equals 0.63, which reflects the ratio of thefmxun apemms (0.24mtxO.38 mm).

heads that are fixed along the sides of the model (Fig. 4) results in a one-dimensional advective flow field. Distance between wells (in the field) is 34 m, and the measured head difference between wells is 1.5 m, giving an average gradient of 0.044 if flow is directly between wells. By Eq. (l), this gradient produces velocities that are several hundred meters per day. Under these conditions, the model predicts that 2uRn values decrease by only 2% between wells if the fracture intersection is halfway between wells 92CO-16 and 92CO-14. This calculated 2% change in zzzRn abundance is insignificant compared to the analytical uncertainty in measuring 2uRn by liquid scintillation (lo%), reflects the short transit time between wells, and does not explain the difference in 2uRn concentration observed in the field. Changing the average gradient to 0.0001 reduces average ground water velocities to approximately 1 m per day. With the fracture intersection halfway between the two wells, 2vBn concentrations reach a steady-state value in the larger fracture approximately 13 m from the fracture intersection (Fig. 6). However, assuming that andyticd uncertainty is 10%. the ratio of concentration to initial concentration (C/C,) may range from 0.70 to 0.47 for well pair 92CO-14:92CO-16, and the 2uRn concentration may reach steady-state in the larger fracture as close as 5 m from the fracture intersection (Fig. 6). These results suggest that the hydraulic connection between the two wells is not a simple two-fracture system. Probably a zone of much lower transmissivity (or longer distance) connects the two wells along the flow path. Even if the distribution of U6Ra is not homogeneous, a hot spot affecting 2zzRn concentrations at well 92CO-16 would

P.F. Folgeret aL/Journal of Hydrology 195 (1997) 45-77

57

influence the concentration at well 92C0-14 if the flow was directly from well to well with a gradient of 0.044. 4.2.3. Rn transport in the two-fracture system under transient conditions One objective of the simulations run under transient conditions is to examine whether 2~Rn concentrations in each fracture will influence concentrations in the connected fracture under pumping conditions. A second objective is to observe how 2~Rn concenwations at the pumping well change if the distribution of 222Rn parent radionuclides on fracture surfaces is not homogeneous. Assuming the steady-state 2"Rn profile across the fracture intersection described above, single well aquifer tests representing pumping wells 92CO-16 and 92CO-14 are simulated for a 24 h period and changes in 2~Rn across the fracture system are determined using MT3D. The 222Rnconcentration in water entering the two-fracture system from constant bead boundaries in columns 38-60 equals the steady-state concentrations in that fracture. Thus, anomalous 222Rn sources external to the two-fracture system are ignored. Pumping well 92CO-16 for 1 h results in a near-symmetrical drawdown cone in the fracture with a radius of influence of several meters (Fig. 7(a)). 2"Rn concentrations across the fracture intersection are not significantly affected after 1 h (Fig. 7(b)). After one day of pumping, drawdown extends across the fracture intersection (Fig. 7(a)). Not surprisingly, the 222Rn concentration profile along the two-fracture system changessignificantly with pumping time compared to steady-state conditions as water with lower 2"Rn concentration is drawn towards thepumping well (Fig. 7(b)). For the boundary conditions prescribed 222 above, the change in Rn concentration becomes measurable (>10%; Mullin and Wanty, 1991) at the pumping well between 6 and 8 h of pumping. After 48 h of pumping, flow conditions are steady-state as the radius of influence reaches the upgradient fixed head boundary. Consequently, ~ R n concentrations at the pumping well are also at steadystate and reflect the mixing of fresh water entering the system across the upgradient fixed head boundary and water entering the system across fixed head boundaries in columns 38-60 (Fig. 7Co)). Apart from boundary influences, 2nRn concentration of water entering the pumping well depends on ground water transit time in each fracture versus decay rate and the rate of 2~Rn flux from fracture walls. For the parameters and boundary conditions assumed in the simulations, the lower concentration water in the larger fracture does not influence the 2~ZRnconcentration in the pumping well for the duration (approximately 1 h) of pumping before obtaining field water samples. The steep hydraulic gradients generated by pumping 92CO-16 induce high ground water velocities close to the pumping well. It is assumed that flow is laminar and there are no head losses owing to well construction and materials, but these assumptions may not be correct for some field situations (Atkinson et al., 1994). Turbulent flow in the fracture may alter the shape of the ~2Rn concentration profiles in Fig. 7(b). Modelling results are sensitive to dispersivity. 222Rn.transport is assumed to be advection-dominated in the two-fracture system, thus concentration profiles should resemble plug flow except for a small amount of mixing caused by diffusion and dispersion owing to velocity variations across the fracture profile. Small longitudinal dispersivities of 0.1-1.0 m (or+= 0.03-0.3 m) produce C/Co profiles that indicate little mixing of lower concentration water from the large fracture as it is drawn towards the

58

P.F. Folger et aL/Journal of Hydrology 195 (1997) 45-77

I0 0 5

20

30

I day (m) 40

50

60

70

80

"\ \ - - l h r \

II /
r[

/
. .

weli92COfr~ture inm'ie~on

15
20

21~ .........
.......
81~

\ ," /
, "

F ,'

,/ /

14

. /

25 30
b.

24brs

I,

"1

- - l h r
i

0.9 O.8

-\ . . .

.........

6In"

0.7
,4Shr

0.6 well~ 0.5

0
~
.
I I !

14
t

10

20 (m) aloos ~

30 40 SO 60 70 s).smn ~ , w i n s vmildeo i,. dw Rn con~auadoa pt~fik wldle pumpin8 we.B~ 1 6

80

l--

0.9

\I
~'

.....

"

"'"
. . . . .

0.1
I.

0.8

.........

lO

0.7

0.6

0.5

I0

20

30

40

50
~

60
(m)

70

80

90

d i m . , ~ ak,nS ~

P.F. Folgeret aL/Journal of Hydrology 195 (1997) 45-77

59

pumping well across the fracture boundary (Fig. 7(c)). In contrast, ~x of 10.0m (c~t = 3.0 m) results in greater mixing and a higher average C/Co profile across the fracture intersection. However, C/Co at the pumping well is approximately the same for all three dispersivity values (Fig. 7(c)). In Contrast to results from pumping well 92CO-16, pumping well 92CO-14 produces a small drawdown cone that widens only slightly after 1 h of pumping and is asymmetric with more drawdown occurring towards the fracture intersection (Fig. 8(a)). Pumping for 24 h affects heads across the fracture intersection, but because of flow across the constanthead boundary, drawdown at the pumping well remains unchanged after 1 h. 222Rn concentrations increase across the fracture profile (Fig. 8(b)) as ground water velocity increases in response to the increasing gradient drawing higher concentration water from the smaller fracture. However, 222Rn concentration at the pumping well is unaffected by higher concentration water crossing the fracture boundary because 222Rnconcentration is a function of both fracture aperture and residence time. Water crossing the fracture intersection resides in the larger fracture for a long time compared to 222Rnhalf-life, thus 222Rn concentration reaches steady-state with respect to the larger volume fracture (Fig. 8(b)). Although drawdown versus time relationships in the model are relatively insensitive to the location of the pumping wells with respect to the fracture intersection, this is not the case for 222Rntransport. If the pumping well is located adjacent to the fracture intersection, then as the hydraulic gradient steepens under transient conditions, the short residence time of water entering from the adjacent fracture, relative to 222Rn half-life, prevents the water from achieving steady-state 222Rnconcentration with respect to the fracture pierced by the pumping well. These results suggest that pumping will significantly alter the 222Rn concentration profile in the two-fracture system in a 24 h test.
4.2.4. Effect of point sources on 222Rn concentration in the two-fracture system Among the potential disturbances to the two-fracture system described above is ground water with anomalous 222Rn concentration entering the system from connected fractures (modelled as constant head boundaries in these simulations). 222Rn concentrations in the connected fractures may differ as a result of different fracture aperture, or from a greater or lesser flux of 222Rn atoms into the ground water from fracture surfaces (heterogeneous 22eRa distribution or emanating power). Alternatively, connected fractures may be close to recharge sources and have 222Rn concentrations near zero. Evidence exists for fractures with different hydraulic apertures and for bedrock with different 222Rn flux within the field area. Transmissivities range over four orders of magnitude based on single-well aquifer tests of 11 wells (Section 3), suggesting that

Fig. 7. (a) Results fromnumericalsimulationsshowingdistanceversusdrawdownprofileat four differenttimes during pumping of well 92CO-16. Pumping rate (Q) equals 25 m 3 per day; (b) concentrationprofile at six different times during pumping of well 92CO-16. Co refers to steady-state 2"Z2Rn concentrationin the small fracture (hydraulicapertureequals0.24 mm); and (c) concentrationprofilecomparingresultsusing longitudinal dispersivities(ax) of 0.1, 1.0, and 10 m. Pumpingwell is 92CO-16.Co refersto steady-state222Rnconcentration in the small fracture.

60

P.F. Folger et al./Journal of Hydrology 195 (1997) 45-77

a. 0.5

~ weU92(X)-i6
0

10

latet~ e,xteat of memm'abledrawdownafter 24 hom~ 20 30 well 92C0-14 50

60

3.5

well 92C0-16 b. 1.00 ~

,,~.

- ........

0.70

~.

0.60
0 . 5 0 . . . . I , , , , ; . . . . : . . . .

/ well 92C0-|4
V
, . . . . : " , , ' I

10

20 30 40 distan~ ~mn well 92C0-16 (m)

50

60

Fig. 8. Results from numerical simulations showing (a) drawdown profile at two different times during pumping of well 92CO-14. Pumping rate (Q) equals 35 m 3 per day; and Co) concentration profile at three different times during pumping of well 92CO-14. Co refers to steady-state ~ R n concentration in the small fracture (hydraulic aperture equals 0.24 ram).

effective hydraulic apertures may also differ considerably. Total gamma borehole geophysical logs show that gamma radiation differs by a factor of two in wells 92CO-16 and 92CO-14, suggesting that the distribution of gamma-emitters is not homogeneous throughout the granite. Studies of other boreholes in the Pikes Peak Granite indicate that uranium sorption on iron oxides may account for some of the variation of uraniumseries radionuclides on fracture surfaces (Section 2). In addition, detailed mapping and gamma-ray surveying were performed on an outcrop within the wellfield, and chemical and X-ray image analyses were done on samples collected from that outcrop (Frishman et al., 1993). Results show that small (meter sized) areas are enriched in relatively rare urani'um-hearing minerals; portions of these areas produce ten times as much gamma radiation as do areas a few meters away. Selected (centimeter sized) samples from these areas contain up to 70 times more uranium and 75 times more 2X'Ra than "background" samples collected from the same outcrop (204 ppm total uranium in

P.F. Folger et alJJournal of Hydrology 195 (1997) 45-77

61

minexalized samples versus 2.84 ppm uranium in "background" samples, 100 versus 1.3 pCi g-1 226Ra;Frishmann, unpublished data, 1993). Goode et al. (1993) examined changes in 222Rn concentration under transient flow conditions resulting from the interaction of two aquifers at Mirror Lake, NH. One aquifer, a system of well-counected fractures in crystalline rock, is linked to an overlying aquifer of glacial drift via an aquitard of poorly connected fractures. Goode et al. (1993) assumed no variation in 222Rn concentration within each aquifer and successfully simulated field observations of falling 222Rn concentration at the pumping well, as water with low amounts of 222Rn in the overlying glacial drift was drawn into the deeper crystalline rock aquifer through the aquitard. The conceptual model of variations in 222Rn concentration under transient flow conditions presented here is similar to that of Goode et al. (1993), except that individual fractures in the connected fracture system may contain water with different steady-state 222Rnconcentrations. If so, then 222Rnconcentrations along a flow path of many connected fractures may vary considerably in space and time during pumping. It is important to first examine variations in 222Rn concentration in a simple system before attempting to visualize a more complicated network of interconnected fractures that exists in nature. To test the influence on 222Rn concentrations in the simple two-fracture system from a single, connected fracture with high amounts of dissolved 222Rn, simulations are conducted with a point source located at the arrow in Fig. 4. Raising the concentration tenfold in a single grid block at the point source location increases the mass flux into the cell without increasing volume flux into the grid block, and physically represents a local zone of 226Rabuildup, by sorption or co-precipitation, along the fracture surface. Alternatively, the point source could represent a zone of uraninm/radium-hearing minerals located close to the fracture surface. Results from a steady-state simulation with the point source are used as starting conditions for the simulations under transient conditions. Results of pumping well 92CO-16 for 24 h show the combined influence of the point source and the different steady-state 222Rn concentrations in each fracture (Fig. 9). Even at early pumping times, dispersion spreads the influence of the point source into the large fracture. Water with lower 222Rn concentration from the large fracture enters the pumping well between 5 and 9 h of pumping (Fig. 10). After 9 h, higher concentration water from the point source reaches the pumping well (Fig. 10). Contours of concentration at 24 h pumping (Fig. 9) show asymmetry in the 2~Rn distribution across the model width owing to high concentration water entering the system from the point source. In contrast, 222Rnconcentrations at well 92CO-14 remain constant after approximately 1 h of pumping (Fig. 11). As shown by the field tests, the cone of depression reaches the constant-head boundary after only 8-10 rain of pumping (Fig. 5). As a result, high concentration water from the point source at the fracture boundary reaches the pumping well relatively quickly in the simulations. As the radius of inflnence expands across the fracture boundary at later time, higher concentration water from the smaller fracture is drawn across the fracture boundary (Fig. 11). Although 222Rn concentration remains constant at the pumping well after 1 h, the concentration profile along the towpath reflects mixing of high concentration water from the point source and the smaller fracture (Fig. 11). The effect of a single point source on 222Rn concentrations in the relatively simple

62

P.F. Folger et aL/Journal of Hydrology 195 (1997) 45-77 1 hoar

. . . . . . . , I i i , i | , , t , ~ i , ,'I . . 4 b . If, , ~! i , s t ,

i
20

'''

'

'

'

'

'

'

'

o
O.

'

'

'

'

'

'"

'

'

'

'

'

'

'

i
60 "

10

10

20

30

40

50

8 hours

20

10

O.

10

20

30

40

50

60

16 bouts
I , , , , I , , , I . , , , I , , , I I t I l I I , ~ , I , , , I I t I t t I

20

10

0.

10

20

30

40

50

60

24 horn

20

10

O.

10

20 30 scale is in meters

40

50

6O

0 well g2C0-16 point source

Radon conventralions in arbitrary units

Fig. 9. Results of numerical simulationsplotted on contour graphs at four time intervals showingchanges in Z~Rn concentration while pumping well 92CO-16 at a rate (Q) of 25 rn3 per day. Point source location shown by diamond. Point source initial concentration equal to 10 times the highest initial steady-state concenWafion. Contour values range from 200 to 340 in arbitrary units; initial values reflect steady state concentration without the point source and range from 200 to 320 in arbitrary units. two-fracture system indicates that a combination o f multiple point sources and a more complicated fracture architecture will produce a complex ~ R n concentration profile. Indeed, " R n concentrations at any point in time under transient conditions will be a function of the location o f point sources with respect to the pumping well, geometry of the fracture system, fracture aperture (and associated transmissivities), duration and magnitude o f pumping. The range of 2nRn values measured in the study area ( 1 2 4 - 8 4 0 k b q m -3, nearly a factor of 7) reflects a combination o f all these factors. Typically, n2Rn samples were collected after 1 - 3 h of pumping at low rates ( 5 3 - 1 6 m 3 per day); thus 222Rn concentrations may reflect heterogeneities close to the wellbore. Moreover, the strength o f a local 222Rn source relative to the " b a c k g r o u n d " 2~Rn flux will also determine the degree to which the point source perturbs the system. Unless the

P.F. Folgeret aL/Journalof Hydrology 195 (1997) 45-77

1

63

0.95

0.9

0.~

0.8
0

10

15

20

24

Fig. 10. Results of numericalsimulationsplotted as ~ZRnconcentration versus time at pumpingwell 92CO-16 showing the influence of lower concentration water from the large fracture (0.38 mm hydraulic aperture) and higher concentrationwaterfromthe point source. C,m is the maximumconcentrationat the pumpingwell (initial concentration equals steady state concentration without the influence of the point source).

geometry of a fracture system is well known, it will he extremely difficult to discern the relative influence of multiple point sources and their locations in space.

4.2.3. Effects of in-situ removal of 226Rafrom fracture walls on 222Rn concentration in the two-fracture system Radon ~ is removed from household water supplies most commonly by aeration. However, commercial water suppliers who tap ground water may encounter concomitant problems of fouling and scaling with aeration, which require disinfection and/or chemical treatment. A possible alternative may he removal of ~ R a , the direct source of ~"~Rn, from the surfaces of fractures that are conducting water to the well. Many workers have demonstrated that uranium, the ultimate precursor of both 2~Ra and ~ R n , sorbs strongly onto iron oxyhyclroxides (Fe-ox) in both experimental and field situations (Davis and Leckie, 1978; Hsi, 1981; Campisano, 1987; Lawrence, 1990; Wanty et al., 1991). Folger et al. (1992) observed a strong correlation between natural gamma counts and Fe-ox staining on cuttings collected from well 92CO-1 drilled in Pikes Peak Granite (Fig. 12). Spectral gamma logs from the high gamma zones suggest that uranium-series radionuclides (versus 23~Th-series radionnclides or 4K) are producing the elevated radiation. Laboratory experiments were conducted on selected samples, representing 5 or 10ft drilling intervals, to determine whether uranium was leachable from the rock chip surfaces. Approximately 5 - 6 g of cuttings from each sample interval were placed in 50.0 ml of 0.1 mol NaHCO3 solution for two days, and the solution was analyzed for total uranium by the standard addition method using a Scintrex laser fluorimeter. Results (Fig. 12) show that significantly more uranium was leached from the Fe-ox stained zones than from the unstained intervals, and that uranium values are highest from the zone of most elevated gamma counts. Moreover, wbole-rock delayed neutron analyses

64

P.F. Folger et aLIJournalof Hydrology 195 (1997) 45-77 1hour

t I ' ' '

2O

IIIII
' ' , ! , . , , I ' ' ' " ' ' ' ' I ' ' ' ' I ' ' ' ' I ' ' ' '

10

O.

10

2O

30

40

50

6O

4houm
l l , , , I , , I , I I t , i I I , i , I , , , i J l , , , i

.....
O. 10

i i i-i
20 30 40

......
50

10

60

8 ~
I , I I I i i I I l * | | i ~ , | . I , J 40~ | I , * , | I J ' ' '

'

'

'

'

'

'

'

'

'

'

'

'

'

'

'

'

"

'

'

'

'

'

'

"

'

'

'

'

!
I

2O

10

O.

10

20

3O

4O

50

60

24~
I , , . , I , . , , I , , , , I , , , I , , 4b , I , , | , I J * , !

2O

10

O.

10

20

30

40

50

60

mis
0 well g~(::~14
.

in metem

polnt source

P,~.~ ~

In a d ~ w y tmlet

Fig. 11. Results of numerical simulations plotted on c o n ~ graphs at four time intervals showing changes in 222Rnconcenmulon while pumping well 92CO-14 at a rate (Q) of 35 m s per day. Point source location shown by diamond. Point source initial concentration equal to 10 times the highest initial steady-state concentration. Contour values range from 210 to 340 in arbitrary units; initial values reflect steady state concentration without the point source and range from 200 to 320 in arbimey units.

of sample splits from a few of the same intervals indicate elevated values of both uranium and 226Ra in the Fe-ox stained zones relative to the fresher samples (Fig. 12). The results suggest that uranium and 226Ra are concentrated in Fe-ox coatings along fracture walls and that uranium is easily removed from rock surfaces by carbonate complexation. Assuming that leach solutions can remove 226Rafrom fracture walls, in-sire removal of the 222Rn sour~ may be a plausible alternative to aeration. The procedure would involve injection and removal of a leach solution, and it is therefore critical to explore how the leaching process affects 222Rn concentrations at the wellhead. For example, even if 226Ra removal is 100% efficient, water outside the depleted area will still contain 222Rn concentrations that reflect fracture aperture width and 226Ra distribution alon~.~the fracture surface. With zero 222Rn flux from fracture walls in the affected area, the " R n concentration in water entering the depleted zone will decrease as 222Rndecays. Travel time from

P.F. Folger et al./Journal of Hydrology 195 (1997) 45-77 m gsmma (cps)

65

0....

urgluum
! ....
i

tltTmm

2, ~ .... n9....~...~...~
i - - - , . . . . i . . . . i . . . . i

9....
| . . . .

~ .... t,o
, . . . . J

o,23,5

. . . .

. . . .

I
$5F
60 65 70

8O ,ffig::.

r
|

90 95 100 10$
11o

Fig. 12. Total naturalgamma,degree of iron-oxidestainingon drill cuttings,unmiumand ~ concentratiomin samples of drill cuttings from well 92CO-1. Samplesrepres~t 1.5 m drill intm~ls (5th sample from the top represents a 3 m interval).Degree of iron-oxidestaining is based on an arbilrarycolor scale and vmies from no visible su~in__g(0) to strongly iron-oxidestained (5) determinedby visual inspectionunder a binocularmicroscope. Anows indicate producingfractures or fracttwe zones detennin~ by heat-puhe flowmeterlogging;open arrows indicate producing fractures under pumping conditions. Note scale change between ppm leachable uranium and total uranium. outside the depleted area to the wellbore will determine whether 222Rn concentrations are effectively lowered at the pumping well. Removal of 226Ra can be modelled in the two-fracture system by assigning zero concentration to water entering the affected cells. Removing 226Ra from fracture walls will

66

P.F. Folger et aL/Journal of Hydrology 195 (1997) 45-77

involve an injection and subsequent withdrawal of fluid that will leach 226Rafrom fracture walls, but it is difficult to predict the efficiency of the process and extent of leached area. Initial conditions close to what are expected in a fractured-rock aquifer pumped by domestic water supply wells must be established in the model before simulating injection-withdrawal of leach solution and the subsequent effects on 222Rn concentration. Single-family wells are pumped intermittently. Average domestic water usage has been estimated at 0.385 m 3 per day per person (Brown and Caldwell, 1984); however, well owners in mountain communities without lawns tend to be more frugal and a more accurate estimate may be half of the average daily consumption, or 0.192 m 3 per day per person. Usually the pump will run for a few minutes to fill the pressure tank, switching on and off during periods of high water use. The minute-by-minute cycling is ignored here and the periods of high water use and no water use are represented with the following cycle: 6 am-8 am 8 am-12 pm 12 pm-I pm 1 pro-6 pm 6 pro-8 pm 8 pm-6 am pump on pump off pump on pump off pump on pump off

with a pumping rate of 3.2 m 3 per day (assuming a family of four) for the hours when the pump is on. With the same boundary conditions as above, one 24 h cycle of pumping well 92CO-16 produces a drawdown-recovery cycle characterized by a steep drawdown cone during pumping cycles and a flatter, wider drawdown cone during each recovery cycle (Fig. 13). All water is released from or goes into storage during the first 24 h o n - o f f pumping cycle (i.e. flowrate at the boundaries of the model does not change). If the cycle is repeated, so as to represent a typical daily use cycle, then residual drawdown increases by smaller increments during each cycle as the radius of influence expands and eventually encounters constant head boundaries. Changes in residual drawdown are less than 0.02 m after 25 days of this pumping pattern as the system approaches steady-state conditions. The contrasting hydraulic conduodvities of each fracture, and the location of the pumping well with respect to the fracture intersection and the constant head boundaries produce an asymmetric steady-state head profile (Fig. 14(a)). To examine the effects of removing 226Ra from fracture walls, we simulated the injec= tion of 3.79 m 3 (1000 US gallons) of leach solution into well 92CO-16 at a rate of 0.0076 m 3 rain -i (2 US gallons min -i) for 500 rain, and then an equal volume of fluid was removed at the same rate. This represents a volume and flow rate easily supplied by most water well service companies. After the injection/withdrawal sequence, the daily pattern of o n - o f f pumping resumed to simulate the typical daily use cycle described above. Fig. 14(a) shows that the injection/withdrawal head profiles are nearly mirror images, and that one day of cyclic pumping reproduces the steady-state head distribution. The injection solution maintains at least 1% of its original concentration for a distance of 20 m towards the fracture intersection, and 25 m in the opposite direction. Assuming that 226Ra is completely removed for that portion of the fracture system, 222Rn concentrations

P.F. Folger et aL/Journal of Hydrology 195 (1997) 45-77

lal~tl eottmltof ~ 20 ~ 30 40 flea lU]lplq wtdl ~ 1 6 (m) 50 60

67

0
0

I0

70

80

il
I 2 ......... ....... ....... 2.5 7hrm 12hrt 14hrs I!
..

~,

~ 2 4 & s

Fig. 13. Results from numerical simulations showing drawdown profiles at six different times for pumping well 92CO-16. Pumping rate (Q) varies throughout a 24h period to match the average daily-use cycle at a typical mountain home. Well 92CO-16 located at 40 m point on horizontal scale. See text for details.

in the leached zone are set to zero prior to the beginning of the daily use cycle of pumping; 2~Rn concentrations in the unleached portion of the fracture are equal to steady-state concentration prior to leaching (Fig. 14(b)). Fig. 14(b) shows that 2"Rn concentrations in the leached zone increase steadily with time as ~ R n enters the zone in response to the hydraulic gradient induced by pumping. Because the gradient is steep, residence time in the leached portion of the fracture system is short. After 24 h, water reaches the pumping well from outside the leached zone without any measurable decrease in 2~Rn concentration owing to radioactive decay. Under these pumping and boundary conditions, removing the ~aRn source for a distance of 45 m along the fracture makes negligible difference in the 222Rnconcentration at the pumping well. For the simple two-fracture model, the injected fluid must remove all the 22~'Raout past the fixed head boundaries from well 92CO- 16 to effectivelyreduce 2"Rn concentrations at the wellhead. Therefore, in a field application, the leached zone must extend far enough so that ground water travel time from the unleached portion of fractures exceeds seven 2~Rn halflives to reduce concentrations to less than 1% of original concentration. For well 92CO-16, it would be necessary to conduct long-term aquifer tests to evaluate boundary conditions and better estimate the volume of fluid needed to provide an effective 2~Rn mitigation. As described here, the proposed in-situ 2~Ra removal technique would not reduce 2~Rn concentrations at pumping well 92CO-16. Pumping well 92CO-14 using the same pattern shows that 2~Rn concentrations after leaching also depend on the nature of the boundary conditions for the two-fracture model. Drawdown extends to the constant-head boundary shortly after pumping begins (Fig. 5), and residual drawdown equals zero at the pumping well after one 24 h daily-use pumping

68

P.F. Folger et alJJournal of Hydrology 195 (1997) 45-77

- - s s
8

. . . . .

inj

......... wtb~r

24hrs

It It II

l
, -4 , frucuu'e iamnecsiou -8
o
" " " : " " " * " " " : " " " ! . . . . . . : " " " : " " " : " " " : " " " I

so

4o

~o

1oo

12o

14o

i~o

Iso

2oo

e~n ~ I ~ ~ head b~ndm~ ~o~vnSmcUent e ~ u n m h e ~ b o m d ~ (m)

. . . . .

2~

.........

6~

.......

7~

....
b.

"'-

14~ kaeh

! L

w~H 92C0-16

5-a~u~ Inur,~9,a

%
", '%
~0~

"

',

"\

"%
~

I'
;/

.,~
/

l
/

\
I

"
\ \
'

"'- .':,
',

well 92I:X~14

",.
: ~ J

;/ ;I
: :

0 0

I0

~0 30 40 SO 60 ~stance aloq 51etu~ syaSem that indudes kached m l (m)

Olr . . . . . ~lw

70 pe~k, acu

80

.........

well 9 " ~ ! 6 1

0.9
O.8
0.7

" ~ ",,4---m

~ tead~m-----~

0.6
0~

0.4
O.3 02 0.1

fm:tu~

L 10

'

20

30

40

50

60

8o

d~anee a l ~

fnu:Ue ~

that ~ l u d u leached ume (m)

P.F. Folgeret al./Journal of Hydrology 195 (1997) 45-77

69

cycle. Injecting and withdrawing the same volume of leach solution at the same rate as for well 92CO-16 shows that the concentration of the injected solution malntain.~ 1% of original concentration for 20 m towards the fracture intersection, and 15 m in the opposite direction. Most of the solution exits the system along the constant-head boundary adjacent to the pumping well. Therefore, even assuming that 222Rn is not produced along the leached portion of the fracture system as before, 222Rn concentration at the pumping well depends entirely on the water inflowing at the constant-head boundary after one 24 h pumping cycle (Fig. 14(c)). As concluded above, the in-situ 226Ra removal process would not reduce 222Rn concentrations at well 92CO-14 under these conditions unless water flowing across the constant-head boundary contained no 222Rn. These examples illustrate that in the simple two-fracture model under long-term pumping conditions expected for typical single-family water wells, properties of connected, transmissive fractmes (represented as constant-head and constant concentrations boundaries) dominate 222Rn concentrations at the pumping wells. After leaching, the twofracture system is geochemically and hydraulically heterogeneous. Removing adsorbed 226Ra results in heterogeneous distribution of the 222Rn parent radionuclides, and transmissivities of each fracture differ by more than a factor of three because of the cubic law relationship assumed in the model. Yet, given the assumptions of the model, and hydraulic gradients imposed by daffy, cyclic pumping, 222Rnconcentrations at pumping wells 92CO- 16 and 92CO-14 will depend on concentrations at the constant-head boundaries. This occurs because, with long-term pumping, ground water residence time in each fracture is short compared to 222Rn halflife; therefore variations in fracture apemue and 222Rn flux from fracture walls have negligible impact on 222Rn concentrations arriving at the pumping well. It is expected that, in a mature wellfield where long-term pumping has estabfished near steady-state flow conditions, much of the inherent geochemical and hydraulic heterogeneity within a radius of influence (where residence time is short compared to half-life) will not impact 222Rn concentration at the wellhead.
4.2.6. Rn concentrations along a multi.fracture flowpath under steady-state and transient conditions

The travel path for a contaminant in a fractured-ruck aquifer probably follows many interconnected fractures even at the scale of tens to hundreds of meters. Moreover, the flow path may follow only interconnected parts of each fracture plane (Paillet et al., 1987). Much research in recent years has been devoted to describing and understanding flow through variable apertmre channels along a single fracture plane (Tsang and Tsang, 1987; Tsang, 1993) or through channels in multiple connected fractures. Given the inverse relationship between 222Rn concentration and fracture aperture, 222Rn concentrations Fig. 14. Resultsof numericalsimulationsshowing(a) hydraulicheadprofilealongthe fracturesystemfor steadystate (ss)(following25 daysof pumpingfromwell92CO-16),after500 min of injectingleachfluidat a rate (Q) of 0.0076 m3per day (inj),afterwithdrawingthe samevolumeat the sameratefor 500 min (wthdr),and after24 h of cyclic immpingfollowingthe withdrawal (24 in,s); (b) concentrationat six differenttimes while pumping well 92CO-16 for one day following the 1000min injection/withdrawalsequence.The leachedzoneextendsfrom 5-60 m. Co is the steady-state222Rnconcentrationin the small fracture(0.24mm);and (c) concenUationwhile pumping well 92CO-14 followingthe same sequence of injection/withdrawal.The leach zone extends from 20--55 m.

70

P.F. Folger et al./Journal of Hydrology 195 (1997) 45-77

may vary widely along a given flowpath whether it includes multiple connected fractures of different apertures or variable aperture channels, even when 226Ra is homogeneously distributed along the fracture or channel surfaces. A hypothetical system of 10 connected planar fractures, each with different apertures, was constructed to illustrate this relationship (Fig. 15). Each fracture segment in the model is 10 m long, 1 m wide, and has an aperture ranging from 0.1 to 1 mm. The model grid has 1 row and 100 columns, each 1 m in dimension. Constant head boundaries are imposed on the first and last columns; all other boundaries are no flow. At first glance, the range of fracture apertures may seem small; however, Barton (1993) measured fractures in an outcrop near Mirror Lake, NH and showed that almost 90% of the apertures were less than I mm. Assuming that each fracture is represented by a smooth-walled parallel plate model, transmissivity of each fracture (Tf~) is proportional to the cube of the aperture and ranges over four orders of magnitude (Fig. 15). As expected, steady-state (i = 0.0001 across the fracture system) simulation results using a constant flux of ~ R n from fracture walls shows that the 2nRn concentration in each fracture segment is inversely related to fracture aperture (Fig. 15(b), (d), and (f)). Residence time in segments with apertures of 0.1 and 0.2 mm is too short for U2Rn concentration to achieve steady-state; in all other segments, 2~Rn concentrations reach a steady-state plateau. The sharp decline in ~ R n concentration at 0 and 100 m reflects the assigned zero concentration at the constant head boundaries. The ~aRn concentration profile changes dramatically with pumping and is extremely sensitive to well location (Fig. 15Co), (d), and (f)). As drawdown expands with time, 222Rn concentration in each segment reflects ground water residence time and the influence of the concentrations in the adjoining upgradient fractures. After 24 h of pumping from a well at 50 m, the concentration profile reflects only the influence of the smallest fracture (segment 2) and the zero concentration downgradient constant-head boundary (Fig. 15(b)). Placing the pumping well at different locations in the multifracture system (35 m and 65 m) produces different 222Rnconcentration profiles over the same time period because of the wide range of Tfr~ and the position of each fracture relative to the pumping well (Fig. 15(d) and (f)). The extreme heterogeneity of most fractured rock aquifers is, therefore, reflected in the wide range of 2~Rn concentrations that may occur even assuming that 2~Rn flux from fracture walls is homogeneous. It is important to re-emphasize the relationship between residence time and heterogeneity in this hypothetical model. Under steady-state flow conditions with a small natural hydraulic gradient, the heterogeneous distribution of fracture apertures is reflected by ~ R n concentration along the flowpath. Under pumping conditions, however, ground water residence time in each fracture within the radius of influence decreases in response to the changing hydraufic gradient. Consequently, fractures close to the wellbore cease to influence Z~Rn concentration as the radius of influence expands outwards. Regardless of pumping well location, after 24 h, ~ R n concentrations along the fracture system reflect the influence of only two or three fractures (and/or a constant-head boundary). Numerical simulations (herein) and field data (Goode et al., 1993) suggest that 2~Rn concentrations at the wellhead are time-dependent under pumping conditions in relatively undisturbed aquifers. This suggests that one-time samples collected in the 1l-well study area may not be ~ o d u c i b l e if recollected at times different from the original sampling effort.

P.F. Folgeret olJJournol of Hydrology 195 (1997)45-77

71

distancealongfracturesystem(m)
o

10
5 --

20~

40 !ii.i.!!! i.i.!i..

7~

10--

i lS "0
20--

mgment
TIr~

1
0.115

2
0.0054

3
18.7

4
54.3

5
1.46

6
11.7

7
0.433

8
6.78

9
39.7

10 27.6

epeftum

OA

0.1

0.7

1.0

0.3

0.8

0.2

0.5

0.0

0.8

b.

0.60- ~
1.0-

pump~o wd

0.71 --

"........................ ,
.

"
. . . .

0 hr
lhr

o.4o_
0.29 -0.14 0 0 i 10 I 20 I 30 ! 40

~
,

~
; ........

...........8 hm
2 4 hm - ....~. I 60 I 70 i 80 I 90 I 100

6050

Fig. 15. Results from numerical simulations showing (a) drawdown profile at four different times for a well pumping at a rate (Q) of 5.45 mS per day located at 50 m in a connected mulfifracture system. The middle diagram indicates the location and aperture of each fracture segment ranging from 0.1 to 1.0 mm. Crux is the maximum concentration in the ffactuge system, Tfmeis fracture transmissivity in m 2 per day, aperture is in nun; (b) graph showing concentrations versus distance at five different times in the connected mulfifmctme system. How is from left to fight under steady-state conditions (i = 0.0001); (c) drawdown profile for the same conditions as (a) except the pumping well is located at 35 m; (d) concentration versus distance for same conditions as (b) except the pumping well is located at 35 m; (e) same as (a) and (c) except the pumping well is located at 65 m; (f) same as (b) and (d) except the pumping well is located at 65 m.

72

P,F. Folger et alJJournal of l~drology 195 (1997) 45-77

G.

C 3-

dietanoe along fracture system(m)

lO ~ so 4o 5o 60 70

90

, if illill! iiii!iiill, .............

69la15-

segment Tim(: qxxture

s

1 0.115 0.4

2 0.1

3 0.7

4 54.3 1.0

5 1.46 0.3

6 11.7 0.6

7 0.433 0.2

8 6.78 0.5

9 38.7 0.9

10 27.6 0.8

0.0064 18.7

~1~0
d. 1.o -

__,

:~

- - Z

- - Z

Z z

0.86-- / ~
0.71
- -

p.mp~

w~l

Ohr.
~ : ~ "" ..................... ......

~0.57

().48 -

o.+_y
0.14 lb 2b 3~)

--,'809~3 1(~0

..... lhr ~ 4 his ' .......... 8 hm

4b

5b' I~ 70

Fig. 15. Continued.

2~Rn concentrations in samples collected from wells in estabfished communities throughout the Elk Creek basin, however, probably do not depend on when they are collected during pumping. In either case, variations in 222Rn concentrations reflect the heterogeneous distribution of fracture properties in the aquifer regardless of time of sampling.

S. Summary and conclusions Dissolved 222Rn concentrations in a fractured crystalline rock aquifer depend on fracture aperture, distribution and concentration of parent radionuclides uranium and

P.F. Folger et aL/Journal of Hydrology 195 (1997) 45-77

73

distanoe along
10 I

fracture system

(m)

mgmnt

1 0.115 0.4

2 0.1

3 0.7

4 54.3 1.0

5 1,.46 0.3

6 11.7 0.6

7 0.433 0.2

8 6.78 0.5

9 38.7 0.9

10 27.6 0.8

Tfm:
m

0.0054 18.7

"0

f.

1.0--

pumping we,

0.860.71

Ohr

0.57~i 0.430.29-0.14-0
. . . . . . . . . . . . . . . . . . . . . . . . . . . . .

..... I hr ..... . 4 ~
." . . . . . . . . . . . . . 8~

10

20

30

40

5~)

60

70

80

90

100

Fig. 15. Continued.

226Ra, and groundwater residence time. 222Rnconcentrations in a small wellfield underlain by Pikes Peak Granite range from 130 to 850 kbq m -3 (3400-23 000 pCi L-l). Different fracture apertures can explain the variation in 222Rn concentration between two wells within the small wellfieid assuming a simple connected two-fracture system and homogeneous distribution of 22SRa along the fracture walls. Field evidence suggests that in many cases the distribution of 226Rais not uniform on fracture surfaces, and that anomalous accumulations of 222Rnparent radionuclides may produce the extremely high dissolved 222Rnconcentrations measured in Colorado and elsewhere in the US. The distribution of dissolved 222Rn concentrations along a flowpath in a fractur~

74

P.F. Folger et alJJournal of Hydrology 195 (1997) 45-77

crystalline rock aquifer may be complex under transient flow conditions even for a simple connected two-fracture system. 222Rnconcentrations may vary considerably in a simplified system depending on the differences in steady-state 222Rnconcentrations in adjoining fractures, distance from the pumping well to fracture intersections, duration and magnitude of pumping, and presence of point sources within the radius of influence. Because the flow path in a real system may involve a large number of connected fractures of different apertures, and flow may actually occur only along portions of each fracture plane, 222Rn concentrations can be expectedto vary dramatically over the local scale. It should be noted that for the portion of a fracture system where ground-water residence time is short compared to 222Rnhalf-life, variations in fracture aperture and distribution of 226Ra will not influence dissolved 222Rn concentration. Given the extreme heterogeneity of most fractured crystalline rock aquifers, it may be impossible to distinguish the relative importance of different factors contributing to variable 222Rn concentrations in ground water. Careful and detailed geological observations, geophysical logging, and hydrological testing may reveal a dominating characteristic for an individual well such as a uranium or radium "hot spot" or proximity to a recharge source. However, much of the variability at the tens to hundreds of meters scale may be attributed to characteristics of the rocks and fractures that are impossible to accurately measure in-situ, such as actual fracture aperture, parent radionuclide distribution, emanating power, and surface area of the fracture plane in contact with flowing ground water. Moreover, 222Rn concentration at a water supply well may be timedependent during pumping because of aquifer heterogeneity. Consequently, it is not unreasonable to expect wide variations in dissolved 222Rn concentrations from well to well even within a single rock-type such as the Pikes Peak Granite.

Acknowledgements
This research was partially supported by the Department of Energy under the USGSDOE Interagency Agreement DE-A 105-91ER61143. We appreciate comments by Journal of Hydrology reviewers which greatly improved the paper.

References
Atkinson, L.C., Gale, J.E. and Dudgeonq, C.IL, 1994. New insight into the step-drawdown test in fractured-rock aquifers. Appi. Hydrogeol., 1: 9-18. Barton, C.C., 1993. Characterizing bedrock fractures in outcrop for studies of ground-water hydrology: and example from Mirror Lake,, Grafton County, New Hampshire. U.S. Geol. Surv. Open-File Report, 93454: 31. Brown and Caldwell, 1984. Residential Water Conservation Project: Summary Report. Prepared for the U.S. Deparunent of Housing end Urban Development, Office of Policy Development and Research, Building Technology Division, June, 1984. Bryant, B.H., 1974a. Recotmaissance geologic map of the Conifer quadrangle, Jefferson County, Colorado. U.S. Geol. Surv. Misc. Field Studies Map IVlF-597,scale 1:24,000.

P.F. Foiger et alJJournal of Hydrology 195 (1997) 45-77

75

Bryant, B.H., 1974b. Reconnaissance geologic map of the Pine quadrangle, Jefferson County, Colorado. U.S. Geol. Surv. Misc. Field Studies Map MF-598, scale 1:24,000. Bryant, B.H., 1976. Reconnaissance geologic map of the Bailey quadrangle, Jefferson and Park Counties, Colorado. U.S. Geol. Surv. Misc. Field Studies Map MF-816, scale 1:24,000. Bryant, B.H., McGrew, L.W. and Wobns, R.A., 1981. Geologic map of the Denver 10 2 quadrangle, northcentral Colorado. U.S. Geol. Surv. Misc. Invest. Series Map I-1163. Campisano, C.D., 1987. Geochemical, hydrologic, and geologic factors affecting radon-222 and radium-226 concentrations in ground waters at Deerlieid, New Hampshire. M.S. Thesis, University of New Hampshire, 132 pp. Chert, C.S., 1986. Solutions for radionuclide transport from an injection well into a single fracture in a porous formation. Water Resonr. Res., 22(4): 508-518. Davis, J.A. and Leckie, J.O., 1978. Surface ionization and complexation at the oxide/water interface. 11. Surface properties of amorphous iron oxyhydroxide and adsorption of metal ions. J, Col. Inter. SCi., 67: 90-107. Domenico, P.A., 1987. An analytical model for multidimensional transport of a decaying contaminant species. J. Hydrol., 91: 49-58. EPA, 1991. Nation primary drinking water regulations; radionuclides: proposed rule. Fed. RegisL, 56: 3305033127. Flttgge, S. and Zimens, ICE., 1939. Die bestimmung yon korngrossen und run diffuaionskonstanten ans dean emaniervermogun. (Die theorie der emaniermethode). Z. Phys. Chem., 1542: 179-220. Foiger, P.F., Nyberg, P., Wanty, R.B. and Poeter, E., 1994. Relationships between 222Rn dissolved in ground water suppfies and indoor " R n concentrations in some Colorado Front Range houses. Health. Phys., 67(3): 244-252. Folger, P.F., Poeter, E., Wanty, R.B., Frishman, D. and Day, W., 1996. Controls on 222Rnvariations in a fracuaed crystalline rock aquifer evaluated using aquifer tests and geophysical logging. Ground Water, 34(2): 250261. Foiger, P.F., Wanty, R.B., Day, W.C., Frishman, D., Taylor, T. and Poeter, E., 1992. Radon in a fractured bedrock aquifer, relationships with rock type and distribution of parent radionuclides. Geol. Sne. Am. Absu-. Prog., 24(7): A78. Folger, P.F., Wanty, R.B., Nyberg, P. and Poeter, E., 1993. Measuring the contribution of " R n in well water to indoor air by long-term and continuous monitoring. In: Proceedings from the 35th Rocky Mountain Conference on Analytical Chemistry, Abstr. Pro8., 25th-29th July, Denver, CO. Frishman, D., Day, W.C., Fuiger, F.F., Wanty, R.B., Briggs, P.H. and Poeter, E., 1993. Bedrock geologic controls on radon abundance in well water, Conifer, Colorado. Proceedings of the 1993 International Radon Conference, Denver, 20th-22nd September, pp. IV20-IV30. Cmode, DJ., Hsieh, F.A., Shapiro, A.M., Wood, W.W. and Kraemer, T.F., 1993. Concentration history during pumping from a leaky aquifer with stratified initial concentration. Hydraulic Engineering '93, San Francisco, 25th-30th June, pp. 29-35. Gringarten, A.C., 1982. Flow-test evaluation of fractured reservoirs. Geol. Sec. Am. Spec. Pap., 189: 237-264. Gringarten, A.C. and Witherspoon, P.A., 1972. A method of analysing pumping test data from fractmed aquifers. Proceedings of the Symposium on Percolation in Fissured Rock, 3, Stuttgart, pp. B l-B9. Grisak, G.E. and Pickens, I.R., 1980. Solute transport through fractured media 1. The effect of malrix diffusion. Water Resour. Res., 16(4): 719-730. Hsi, D.C., 1981. Soq3fion of uranium (VI) by iron oxides. PhD Thesis, Colorado School of Mines, Golden, CO, 154 pp. Hsieh, P.A. and Neumann, S.P., 1985a. Field determination of the three-dimensional hydraulic conductivity tensor of anisotropic media 1. Theory. Water Resour. Res., 21 (11): 1655-1665. Hsieh, P.A. and Neumann, S.P., 1985b. Field determination of the threc-dimensional hydraulic conductivity tensor of anisotropic media 2. Methodology and application to fractured rocks. Water. Reanor. Res., 21(11): 1667-1676. Hsieh, P.A. and Shapiro, A.M., 1993. Flow and transport properties of a 120m by 80m by 60m block of fractured crystalline rock at the Mirror Lake site, New Hampshire. Geol. Soc. Am. Abs. with Ping., 25(6): A-487. Hutchinson, R.M., 1988. Granite-tectonics of the Pikes peak composite batholith, Colorado. Geological Society

76

P.F. Folger et al./Journal of Hydrology 195 (1997) 45-77

of America Field Trip Cmidebook, Colorado School of Mines Professional Contribution no. 12, Colorado School of Mines, Golden, CO, pp. 47-54. Huyakorn, P.S., White, H,O. Jr. and Wadsworth, T.D., 1991. TRAFRAP-WT: A two-dimensional finite element code for simulating fluid flow and transport of radionuclides in fractured porous media with water table boundary conditions. International Groundwater Modelling Center, software manual. Jenkins, D.N. and Prentice, J.K., 1982. Theory for aquifer test analysis in fractured rocks under linear (nonradial) flow conditions. Ground Water, 20(1): 12-21. Krishnaswami, S. and Scidemann, D.E., 1988. Comparative study of ~Rn, 4Ax,and 3TArleakage from rocks and minerals: implications for the role of nanopores in gas transport through natural silicates. Geochim. Cosmochim. Act& 52(3): 655-658. Lawrence, E.P., 1990. Hydrogeologic and geochemical processes affecting the distribution of 2~'Rn and its parent radionuclides in ground water, Conifer, Colorado. M.S. Thesis T-3923, Colorado School of Mines, Golden, CO, 181 pp. Lawrence, E.P., Poeter, E. and Wanty, R., 1991. Geohydrologic, geochemical, and geologic controls on the occurrence of radon in ground water near Conifer, Colorado, USA. J. Hydrol., 127: 367-386. Lawrence, E.P., Wanty, R.B. and Nyherg, P., 1992. Contribution of ~Z2Rnin domestic water supplies to 222Rnin indoor air in Colorado homes. Health. Phys., 62(2): 171-177. Mcdonald, M.G. and Harbangh, A.W., 1988. A modular three-dimensional finite-difference ground-water flow model. U.S. Geological Survey Techniques for Water Resource Investigation, 0t-A1,576 pp. Mullin, A. and W anty, R.B., 1991. A comparison of two techniques for radon-222 measurement in water samples. Field studies of redon in rocks, soils, and water. US Geol. Surv. Bull., 1971: 231-235. Paiilet, F.L., 1993. Using borehole geophysics and cross-borehole flow testing ~o define hydraulic connections between fracture zones in bedrock aquifers. J. Appl. Goophys., 30: 261-279. Palllet, F.L., Hess, A.H., Cheng, C.H. and Hardin, E., 1987. Characterization of fracture permeability with highresolution vertical flow measurements during borehole pumping. Ground Water, 25(1): 28-40. Palllet, F.L., Novakowski, K. and Lapcevic, P., 1992. Analysis of transient flows in boreholes during pumping in fractured formations. Transactions of the Society of Professional Well Log Analysts 33rd Annual Logging Symposium, Oklahoma City, OK, paper S. Palllet, F.L., Waltz, J. and Boyle, R.E., 1989. Geophysical log investigation of formation changes produced by hydraulic fracture stimulation in a crystalliue-hedrock aquifer. Proceedings of the Third International Symposium on Borehole Geophysics for Minerals, Geotechnical, and Groundwater Applications, Las Vegas, 2nd-5th October 1989, pp. 571-594. Rancher, R.S. and Drago, J.A., 1992. Estimating the cost of compliance with the drinking water standard for radon. J. Am. Water Works Assoc., 84(3): 51-65. Semkow, T.M., 1990. Recoil-emanation theory applied to radon release from mineral grains. Geochim. Cosmochim. Act& 54: 425--440. Sen, Z., 1986. Aquifer test analysis in fractured rocks with linear flow pattern. Ground Water, 24(1): 72-78. Shapiro, A.M., 1981. Fractured porous media: equations development and parameter identification. Ph.D. dissertation, Princeton Uniyersity, Princeton, NJ, 373 pp. Streltsova, T.D., 1976. Hydrodynamics of groundwater flow in fractured formation. Water Resour. Res., 12: 405414. Sudicky, E.A. and Frind, E.O., 1982. Contaminant transport in fractured porous media: analytical solutions for a system of parallel fractures. Water Resonr. Res., 18(6); 1654-1642. Tang, D.H., Frind, E.O. and Sudicky, E.A., 1981. Contaminant transport in fractured porous media: analytical solution for a single fracture. Water Resonr. Res., 17(3): 555-564. Tanner, A.B., 1964. Radon migration in the ground: a review. The Natural Radiation Environment. University of Chicago Press, Chicago, IL, pp. 161-190. Torgersen, T., Benoit, J. and Mackie, D., 1990. Controls on groundwater Rn-222 concentrations in fractured rock. Geophys. Res. Leu., 17(6): 845-848. Tsang, C.F., 1993. Tracer transport in fracture systems. In: J. Bear, C.F. Tsang and G. de Marsily (Editors), Flow and Transport in Fractured Rock. Academic Press, San Diego, pp. 237-266. Tsang, Y.W., and C.F. Tsan8. 1987. Channel model of flow through fractured media. Water Resour. Res., 23(3): 467--479.

P.F. Folgcr et alJJouma1 of H+dogy Wanty, R.B., I-wmcc.

195 (1997) 45-77

71

E.P. and Gundersen. L.C.S., 1991. A theoretical model for the flux of radon-222 from rock to ground water. Geol. Sot. Am. Spec. Pap., 271: 73-78. Wnren, J.E. and Root, P.J., 1963. The behavior of naturally fractured reservoirs. J. Sot. Pet. Eng., September: 245-255. Wood W.W.. Shapiro, A.M. and Hsieh. P.A.. 1993. Gbservational, experimental. and inferred evidence for solute diffusion in fractured granite aquifers: examples from the Mirror Lake Watershed, Grafton County, New Hampshire. US Geol. Surv. Open-File Rep., 93-454: 13. zheng, C., 1993. Extension of the method of charactektics for simulation of solute hamport in three dimensions. Grouod Water, 31(3): 456-465.