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Enviado por Sebastian Montaño Rodriguez

This paperpresentsthetheoreticaldevelopmentandnumericalimplementationofanewmodeling
approachforrepresentingthegroundwaterpathwayinriskassessmentorperformanceassessment
modelofacontaminanttransportsystem.Themodeldevelopedinthepresentstudy,calledthe
ResidenceTimeDistribution(RTD)MixingModel(RTDMM),allowsforanarbitrarydistributionoffluid
travel timestoberepresented,tocapturetheeffectsonthebreakthroughcurveofflowprocessessuch
as channelizedflowandfastpathwaysandcomplexthree-dimensionaldispersion.Mathematical
methodsforconstructingthemodelforagivenRTDarederiveddirectlyfromthetheoryofresidence
time distributionsinflowingsystems.Asimplemixingmodelispresented,alongwiththebasic
equationsrequiredtoenableanarbitraryRTDtobereproducedusingthemodel.Thepractical
advantagesoftheRTDMMincludeeasyincorporationintoamulti-realizationprobabilisticsimulation;
computationalburdennomoreonerousthanaone-dimensionalmodelwiththesamenumberofgrid
cells; andstraightforwardimplementationintoavailableflowandtransportmodelingcodes,enabling
one tothenutilizeadvancedtransportfeaturesofthatcode.Forexample,inthisstudyweincorporated
diffusionintothestagnantfluidintherockmatrixawayfromtheflowingfractures,usingageneralized
dual porositymodelformulation.Asuiteofexamplecalculationspresentedhereinshowedtheutilityof
the RTDMMforthecaseofaradioactivedecaychain,dualporositytransportandsorption.

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journal homepage: www.elsevier.com/locate/cageo

pathway in performance assessment models

Bruce A. Robinson n, Shaoping Chu

Los Alamos National Laboratory, Mail Stop A127, Los Alamos, NM 87545, USA

a r t i c l e i n f o abstract

Article history: This paper presents the theoretical development and numerical implementation of a new modeling

Received 30 August 2011 approach for representing the groundwater pathway in risk assessment or performance assessment

Received in revised form model of a contaminant transport system. The model developed in the present study, called the

30 August 2012

Residence Time Distribution (RTD) Mixing Model (RTDMM), allows for an arbitrary distribution of ﬂuid

Accepted 3 September 2012

Available online 26 September 2012

travel times to be represented, to capture the effects on the breakthrough curve of ﬂow processes such

as channelized ﬂow and fast pathways and complex three-dimensional dispersion. Mathematical

Keywords: methods for constructing the model for a given RTD are derived directly from the theory of residence

Residence time distribution time distributions in ﬂowing systems. A simple mixing model is presented, along with the basic

Mixing model

equations required to enable an arbitrary RTD to be reproduced using the model. The practical

Performance assessment

advantages of the RTDMM include easy incorporation into a multi-realization probabilistic simulation;

Groundwater pathway

computational burden no more onerous than a one-dimensional model with the same number of grid

cells; and straightforward implementation into available ﬂow and transport modeling codes, enabling

one to then utilize advanced transport features of that code. For example, in this study we incorporated

diffusion into the stagnant ﬂuid in the rock matrix away from the ﬂowing fractures, using a generalized

dual porosity model formulation. A suite of example calculations presented herein showed the utility of

the RTDMM for the case of a radioactive decay chain, dual porosity transport and sorption.

Published by Elsevier Ltd.

a systems model.

The groundwater pathway is an important component of Contaminant transport assessment requiring predictions of

systems models predicting risk in applications such as contami- arrivals at a location downstream is conveniently formulated in

nated sites and nuclear waste repositories. Often, risk- or terms of the travel time or residence time distribution (RTD).

performance-assessment (RA or PA) models consist of a network The RTD is a compact way to describe the composite behavior of

of subsystem models describing the behavior of physical or ﬂuid moving through a groundwater ﬂow system, even when the

chemical barriers to contaminant migration, transport through underlying processes of heterogeneous ﬂow, fast pathways, and

porous media, and the arrival of contaminants at a receptor such hydrodynamic dispersion are complex and uncertain. Represent-

as a wellbore or a compliance boundary. These arrivals typically ing these complexities with a computationally simple model such

are converted from mass ﬂux or concentration to a dose, or to as the one-dimensional advection-dispersion equation (1D-ADE)

some other measure of human or ecological risk. Groundwater may not provide the needed ﬂexibility to examine, say, prefer-

models can be very computationally demanding, especially when ential channeling in a fractured medium or highly heterogeneous,

used in a probabilistic framework involving stochastic distribu- multi-dimensional ﬂow systems. By adopting an RTD-based

tions for uncertain parameters and Monte Carlo analyses for approach, the essential features of the ﬂow system can be

quantiﬁcation of overall system uncertainty (e.g. Arnold et al., represented, and in the case of linear solute transport processes,

2003; Arnold et al., 2008; Robinson et al., 2003). It is often the the information is sufﬁcient to obtain a unique prediction of

case that even if a large-scale, multi-dimensional groundwater solute breakthrough (Robinson and Viswanathan, 2003). Even for

ﬂow and contaminant transport process model is developed, nonlinear reaction processes, the RTD is still a fundamental

determinant of transport behavior, because it captures the degree

of spreading in time of a mass input. Therefore, modeling

methods based on the RTD provide an attractive approach for

n

Corresponding author. Tel.: þ1 505 667 1910; fax: þ1 505 667 5450. representing results from large-scale, complex process models of

E-mail address: robinson@lanl.gov (B.A. Robinson). the groundwater pathway. Alternatively, in generic studies for

http://dx.doi.org/10.1016/j.cageo.2012.09.001

156 B.A. Robinson, S. Chu / Computers & Geosciences 52 (2013) 155–163

which detailed models are not available, an RTD-based approach pathway. In hydrology, advective transport is governed by velo-

is also appropriate because it provides a more ﬂexible way to city variability caused by subsurface heterogeneities, leading to a

represent ﬂow complexities than a simpliﬁed 1D-ADE. range of transport times within the system. Theoretical dispersion

The theory and numerical procedures for characterizing trans- studies and characterization of complex subsurface structures

port in porous media via an RTD-based approach has been the and hydrologic pathways are methods for creating models

subject of previous studies. For example, Robinson and Tester that capture this variability. Beyond advection effects, solute

(1984) observed the dynamics of a fractured geothermal reservoir interactions with the porous media, colloid-facilitated transport,

through the measured RTD in a series of tracer tests, and and diffusion into dead-end pore space adjacent to the ﬂowing

Robinson and Tester (1986) showed how ﬂow maldistribution porosity are physical–chemical processes impacting the distribu-

in a heterogeneous ﬂow system can be quantiﬁed using the tion of solute travel times. This section provides the theory for

tracer-determined RTD. Similarly, Becker and Charbeneau creating a reduced model through the use of RTD theory to

(2000) and Becker and Shapiro (2003) take a residence-time- capture advective travel time variability, after which the methods

based approach to the interpretation of interwell tracer tests. In for including other transport processes is presented.

addition, Rainwater et al. (1987), Dagan and Cvetkovic (1996), Consider a system in which a steady or quasi-steady state ﬂow

and Ginn (2001) all developed techniques for folding reactive ﬁeld is established for the groundwater pathway. Contaminant is

transport into a residence-time-based model. Finally, Robinson typically input at a source, characterized with a time-dependent

and Viswanathan (2003) showed how an arbitrary distribution of source-release model, and the mass ﬂux crossing the far-ﬁeld

travel times could be incorporated directly into a computationally boundary is the computed result from the groundwater pathway.

efﬁcient model in a manner that also allowed the effects of small- Dispersive and diffusive processes, as well as preferential

scale mixing to be bounded. channeling and percolation through pathways of various perme-

In all implementations of an RTD-based approach, the RTD abilities, lead to a distribution of travel times of the ﬂuid at the

characterizes the range of travel times from ﬂow paths of far-ﬁeld boundary. In the RTD mixing model approach, the

different velocities which arise as a result of the heterogeneities residence time distribution (also called the exit age distribution,

within the ﬂow system. A wide variety of methods have been after Danckwerts, 1953) of a conservative solute is deﬁned as

developed to characterize the RTD in real systems, including: the follows:

1D-ADE; nonideal ﬂow and solute interchange between f(t)dt is the fraction of injected mass arriving at the far-ﬁeld

mobile and immobile ﬂuid (e.g. Tang et al., 1981; Maloszewski boundary with residence times between t and t þdt.

and Zuber, 1993; Amin and Campana, 1996); two-region models The integral of this density function, F(t), is given by

Rt

designed to represent preferential ﬂow with different mean FðtÞ ¼ 0 f ðtÞdt.

velocities in each region (e.g. Destouni et al., 1994; Erickson and In the development that follows, it is assumed that the pathways

Destouni, 1997); and numerical solutions of explicitly deﬁned that contaminants take in traveling from inlet to outlet can be

heterogeneous ﬁelds based on characterization information of a approximated as a steady state, closed ﬂow system. Under this

subsurface system. In advocating for the use of more complex steady state assumption, the relationship between the distribu-

models to represent laboratory-scale tracer transport in soil tion of residence times at the far-ﬁeld boundary and the distribu-

monoliths, Gupta et al. (1999) illustrated the general point tion of ages of molecules in the ﬂow system is given by:

adopted in the present study that the decoupling of advective

1FðaÞ

processes via a Lagrangian representation of the system facilitates IðaÞ ¼ ð1Þ

t

the incorporation of additional diffusion and reactive transport

processes while honoring the available information on the ﬂow where a is the age of a parcel of ﬂuid (the elapsed time since it

system. entered the system), t is the mean residence time, and the

In this paper, the previous work of Robinson and Viswanathan internal age distribution I(a) is deﬁned as:

(2003) is used as the basis for a new computational method, I(a)da is the fraction of the molecules in the system with ages

called the RTD mixing model (RTDMM), which provides an between a and a þ da.

efﬁcient and ﬂexible way to capture the essential features of the The mean residence time t, computed as the ﬁrst moment of the

groundwater pathway. Advective travel times are input directly residence time distribution, is related to the ﬂow rate Q and ﬂuid

into the model in the form of an RTD, allowing other transport volume V of the ﬂow system as follows:

processes such as diffusion into stagnant zones and sorption to be Z 1

readily included. Rather than attempting to replace or improve t¼ tf ðtÞdt ¼ Q =V ð2Þ

0

upon the aforementioned methodologies for representing the

ﬂow system, the approach developed in the present study With these basic relationships in place, we now present a

accommodates an advective RTD of arbitrary complexity, such simple physical model capable of reproducing an arbitrary RTD.

that the additional diffusion or reactive processes can be incor- Models of this sort have long been the focus of theoretical

porated readily. As such, this model may provide an attractive developments in the ﬁeld of chemical reaction engineering. For

approach for representing the transport behavior in a system for example, Zwietering (1958) proposed two related mixing models

which advective processes are captured using any one of the that each reproduce a given RTD, and theoretically bound the

models listed above, or some alternative method. In the sections behavior of nonlinear reactions in liquid-phase systems. One of

that follow, we provide a derivation of the computational method, these mixing models, developed for solute transport and

discuss its implementation in a ﬂow and transport computer extended to sorption by Robinson and Viswanathan (2003), is

code, and present a set of illustrative results using the method. shown in Fig. 1. The pathway is a plug ﬂow model in which ﬂuid

enters on the right hand side, and exits at various locations along

its length. Within the plug ﬂow system, ﬂuid mixing is perfect

2. Residence time distribution theory across the cross section, and there is no axial mixing along the

length. The manifolds on the sides of the models are zero-volume

This section summarizes the RTD theory, originally outlined in pathways that provide the means for ﬂuid and solute to be drawn

Robinson and Viswanathan (2003), as applied to the development from the model, mixed, and instantaneously transmitted to the

of a computationally efﬁcient model for the groundwater outlet. Thus, the physical transport, and if applicable, reaction and

B.A. Robinson, S. Chu / Computers & Geosciences 52 (2013) 155–163 157

Fig. 1. Schematic diagram of RTDMM for the transport model of the groundwater pathway. The mixing model consists of ﬂuid and solute entering on the right hand side,

and leaving and mixing instantaneously via the manifolds along the side of the model. The diagram in the upper right illustrates the ﬂuid balance within a control volume

and expression relating the outlet ﬂow rate to the manifold to the RTD function.

diffusion processes, takes place only within the plug ﬂow model. volume V1/V is given by

By contrast, the manifold is an idealized construct enabling a Z a1 Z a1

prescribed RTD to be reproduced, but does not represent a ½1FðaÞ

V 1 =V ¼ IðaÞda ¼ da ð3Þ

physical section of the pathway. This mixing model, which forms 0 0 t

the underlying basis for the RTDMM, enforces the latest possible

With all terms except a1 known, it may be solved for by

mixing of ﬂuid of different residence time; a simple reversal of all

interpolation. Proceeding along the pathway, the range of ages

ﬂows reproduces the same distribution of residence times, but

associated with each cell is recursively determined for a given

yields the earliest possible mixing. Regardless of the ﬂow direc-

control volume grid using an expression similar to Eq. (3) with the

tion, an essential element in the development of the RTDMM is

integral performed between ai 1 and ai. This range of ages is also

the fact that the placement and ﬂow rates of the side exits are not

the range of residence times of ﬂuid leaving the cell, so the outlet

arbitrary: for a given RTD, there is a unique arrangement of these

ﬂow rate associated with each cell i is computed numerically

paths. This fact is used in the development of the model in the

using:

next section.

qi ¼ Q f ðaÞDa ¼ Q ½Fðai ÞFðai1 Þ ð4Þ

volumes in the numerical grid represent a given range of ages,

3.1. Construction of RTD-based mixing models computed from the prescribed RTD using the relationships

deﬁned above. The output from the model at a given time is

Robinson and Viswanathan (2003) showed how to build a determined by mixing all exit ﬂuid and computing its concentra-

numerical grid and assign the locations and ﬂow rates of the side tion or mass ﬂux.

exits for the system in Fig. 1 in such a way that a given RTD can be We note in passing that this model is an end member that

reproduced. In this paper, we modify the process for building the prescribes the latest possible mixing of ﬂuid with different

model so that, for a given one-dimensional, control-volume ﬁnite residence times. Robinson and Viswanathan (2003) showed that

difference grid, the ﬂow rates of the side exits can be uniquely the opposite extreme of early mixing can be represented by

deﬁned so as to produce the prescribed RTD. The derivation uses reversing all ﬂows in the model: the manifold becomes an

the relationship in Eq. (1) for the internal age distribution and the entrance manifold, and all ﬂuid leaves at the right end of the

minimum mixing model of Fig. 1. This distribution is an age model. This result follows from Zwietering’s original theoretical

inventory for the internal contents of the ﬂow system: this development, which demonstrated the fundamental equivalence

relationship therefore enables a direct mapping onto a control- of the internal age and life expectancy distributions in steady

volume ﬁnite-difference numerical grid for the case of plug ﬂow state, continuous ﬂow systems. As explained in Robinson and

within the model. As indicated in Fig. 1, ﬂuid of different ages is Viswanathan (2003), if nonlinear reactions are included, the

segregated along the ﬂow path, with a of zero at the inlet on the impact of uncertain small-scale mixing processes, relevant for

right end of the model and increasing a to the left. Starting at the nonlinear reactive transport systems, can be assessed in a

right end of the model, the ﬂuid in this cell of volume V1 has an bounding way using these two models as end members. Further-

age between 0 and a1, where a1 is the age for which the fractional more, once the minimum-mixing model described here is

158 B.A. Robinson, S. Chu / Computers & Geosciences 52 (2013) 155–163

implemented, the changes to a computer code required to containing the parameters ‘‘on the ﬂy’’ at the beginning of each

implement the maximum-mixing model are trivial. realization.

To use the RTDMM as the basis for an abstraction model, f(t) A ﬁnal detail concerns the methods by which the RTD of a

and its integral, F(t), must be provided to establish the mixing conservative, non-diffusing solute is included as input to the

model ﬂow rates. Then, transport of a contaminant is modeled by RTDMM. A provision was added to the FEHM code to allow the

including reaction with the porous medium and matrix diffusion RTD to be speciﬁed either as a tabular representation of the

(described below). This pathway can be constructed using vir- breakthrough curve of travel times, or in the form of a para-

tually any reactive transport code that allows for ﬂuid and solute meterized model describing the RTD. The ﬁrst method provides a

sources/sinks to be speciﬁed arbitrarily at each computational convenient way to generate RTD curves directly from a ground-

grid cell. The validity of this implementation to reproduce a given water process model or any other analytical or numerical scheme,

RTD was demonstrated previously in Robinson and Viswanathan using particle tracking or other methods. The second method,

(2003), and additional model comparisons are provided below. used in the present study, provides the option to use a normal or

Then, if reactive chemistry is included in the model, it is no more lognormal distribution to represent the RTD, enabling travel time

computationally demanding than the usual one-dimensional uncertainty to be examined generically, without reference to an

transport models developed with such codes. However, in this underlying process model.

deceptively simple and computationally efﬁcient model, the RTD In summary, the RTDMM is an RTD-based approach that

of the system is fully preserved, thereby enabling ﬂexibility in the provides an alternative to the construction of a physically-based

representation of the distribution of advective travel times model such as the 1D-ADE, models employing solute interchange

through the groundwater pathway. between mobile and immobile ﬂuid, or two-region models with

In an extension of our previous work, the generalized dual ﬂow in parallel pathways. The distinction is that the pathway is

porosity model (GDPM) presented in Zyvoloski et al. (2008) is constructed directly from the RTD curve itself, enabling an RTD of

applied herein to represent diffusion and sorption from the arbitrary complexity to be represented. As such, the intention is

primary porosity, such as a fracture network, into the rock matrix. not that the RTDMM replace any of these other options, but rather

In applying the GDPM formulation after constructing the RTDMM, that it be used in situations in which it is more convenient to

we are taking the approach that the heterogeneous ﬂow processes specify the RTD directly. Examples may include ﬂow systems in

are captured as a distribution of ﬂuid residence times, and the which the RTD is measured using a conservative tracer, or a

purely solute-driven process of molecular diffusion into stagnant complex RTD curve derived from a multi-dimensional ﬂow and

regions of the porous medium are treated separately. The GDPM transport simulator.

method, described and validated in Zyvoloski et al. (2008),

assumes one-dimensional transport into and out of a matrix

connected to each primary porosity node in the RTD mixing 4. Demonstration calculations

model, and allows multiple, closely spaced matrix nodes to be

used to capture sharp concentration gradients immediately adja- This section provides some basic veriﬁcation calculations to

cent to the primary (fracture) ﬂow medium. The model domain of demonstrate the correct functioning of the code, and then

primary porosity and one-dimensional matrix nodes is repre- demonstrates the use of the RTDMM with matrix diffusion to

sented in integrated ﬁnite difference form. The present study simulate groundwater transport for a speciﬁc application. The

represents, to our knowledge, the ﬁrst attempt to couple a goal of the application is to demonstrate the groundwater trans-

residence-time-based conceptual model for advection to a matrix port model for a series of model runs similar to those that will be

diffusion mass exchange model. performed in a full Monte Carlo analysis. All of the features

developed to integrate FEHM with GoldSim to execute a model

for the groundwater pathway are demonstrated, including: a

3.2. Code implementation details multiple species reactive transport model; the ability to para-

meterize an arbitrary distribution of travel times within the

To implement the RTDMM, provisions were developed within primary pathway; generalized dual porosity formulation to

the computer code FEHM (Zyvoloski et al., 1997) to easily input include diffusion in dead-end pathways. Following a simple

an arbitrary RTD, or a parameterized RTD model such as a normal sensitivity analysis, an uncertainty analysis model run is pre-

or lognormal RTD. This choice enabled the model to take advan- sented by conducting a Monte Carlo simulation with the RTDMM,

tage of FEHM’s reactive transport module (Viswanathan et al., using GoldSim as the simulation driver.

1998; Robinson et al., 2000) and the GDPM model (Zyvoloski

et al., 2008) to solve reactive transport with matrix diffusion. To 4.1. Veriﬁcation

facilitate probabilistic simulations, FEHM was also coupled to the

GoldSim software (GoldSim Technology 2010), thereby opening This section illustrates, through a few examples, the correct

the possibility of easily performing Monte Carlo simulations with functioning of the code in reproducing an RTD and incorporating a

parameters passed from GoldSim to FEHM for each realization. To matrix diffusion formulation for a given advective RTD.

accomplish this, GoldSim invokes FEHM at each time step To verify that the model reproduces an arbitrary RTD, the

through a call to FEHM as a dynamic link library (dll), and cedes general approach is to generate that RTD using a separate model,

control of the calculation to FEHM for calculation of the transport or to simply deﬁne its functional form (e.g. assume a lognormal

process in the RTDMM. If sub-timesteps are required for numer- RTD without reference to a physical ﬂow system), and show that

ical convergence or accuracy, FEHM performs this time step the current method reproduces that RTD when it is provided as

adjustment. At the end of each GoldSim time step, FEHM passes input to a RTDMM simulation of a pulse or step input of tracer.

back to GoldSim any mass reaching the outlet of the model, and For veriﬁcation purposes, we present the following cases: a

retains in memory the current concentration distributions so that 1D-ADE model; a lognormal RTD characterized by its lognormal

the calculation can resume for the next GoldSim time interval. mean and standard deviation; and a two-region model similar to

Finally, the ability to change ﬂow and transport parameters from that suggested by Gupta et al. (1999), consisting of a pair of

one realization to the next is implemented using a separate dll parallel 1D-ADE models that mix at the outlet, yielding a bimodal

called by GoldSim that writes the appropriate FEHM input ﬁle RTD. Fig. 2 presents the 1D-ADE model and the lognormal model

B.A. Robinson, S. Chu / Computers & Geosciences 52 (2013) 155–163 159

model and assigns the ﬂow rates so as to reproduce the RTD for

the pulse input of a passive tracer.

Beyond demonstrating that the RTDMM correctly reproduces

the desired RTD, it is necessary to test the functioning of the code

for the more complex situation of diffusion into dead-end pore

space, as represented by a system consisting of ﬂow through

fractures, with diffusion into the rock matrix. For this situation,

both the FEHM model and the analytical solution of Tang et al.

(1981) are used. Fig. 2 compares the analytical solution to the

RTDMM model for the cases of advection and longitudinal

dispersion in the fractures, and diffusion into the surrounding

rock matrix, with and without sorption on the matrix material. In

the GDPM model formulation, the matrix consists of a local one-

dimensional grid of 29 computational grid cells spaced to capture

the concentration gradients due to diffusion near the primary

porosity, as well as deep into the matrix blocks. Sorption in the

matrix is modeled using an equilibrium, linear sorption (Kd)

model. Sorption is assumed to be negligible on the fracture walls

of the primary porosity. The RTDMM model takes the 1D-ADE

RTD (with no matrix diffusion or sorption) as input, and simulates

the output concentration at the end of the ﬂow path in the

presence of matrix diffusion. By contrast, the curve labeled

Fig. 2. Comparison of RTDMM results to expected breakthrough curves for a

constant concentration input. 1D-ADE: RTDMM compared to a numerical solution

‘‘Original model’’ is a simple 1D-ADE model (as opposed to the

for a 1D-ADE solution; Lognormal RTD: RTDMM compared to a lognormal RTD RTDMM approach) with matrix diffusion included. Both of these

breakthrough curve; 1D-ADE, matrix diffusion: RTDMM compared to Tang et al. are compared to the Tang et al. (1981) analytical solution. The fact

(1981) analytical solution and a numerical 1D-ADE solution with matrix diffusion that the RTDMM matches both the 1D-ADE based model and the

included; 1D-ADE, matrix diffusion and sorption: RTDMM compared to Tang et al.

analytical solution demonstrates the correct implementation of

(1981) analytical solution and a numerical 1D-ADE solution with matrix diffusion

and linear equilibrium sorption on the rock matrix included. the FEHM GDPM formulation as an integral component of the

RTDMM model implementation.

nuclide decay chain:

243

Am-239 Pu-235 U-231 Pa

with radionuclide half lives of 7.37 103 y, 2.41 104 y,

7.04 108 y, and 3.25 104 y, respectively. The transport path-

way is taken to be a fractured rock, represented using the GDPM

formulation with a primary porosity consisting of transport

through fractures, and diffusion and sorption within the rock

matrix. Within the fractures, the RTDMM is employed with a

lognormal distribution of travel times within the fracture domain.

This choice demonstrates a signiﬁcant beneﬁt of the RTDMM:

the ability to capture a wide distribution of travel times to study

the inﬂuence of fast pathways through the groundwater pathway,

while retaining the simplicity and convenience of a parameter-

ized model.

Because this demonstration is illustrative, a simpliﬁed source

term consisting of a constant unit source of 243Am at the inlet of

the pathway is employed, with no source of 239Pu, 235U, or 231Pa

(these species are present due to in-growth, however). In an

Fig. 3. Comparison of the RTDMM results to the input RTD (labeled ‘‘Original actual RA or PA analysis, a source term release model would also

model’’) developed from a two-region model consisting of parallel ﬂow through be developed, perhaps with uncertainty represented, and each

two 1D-ADE pathways. Response is for a pulse input of tracer, and concentrations

species would likely have a source.

are normalized such that the mass output is equivalent for the two models.

Parameters in these example calculations are provided in

Table 1. For each uncertain parameter, the ‘‘base case’’ simulation

results (along with the matrix diffusion results, which are is deﬁned as the model with mean or median values selected for

described subsequently); Fig. 3 shows the results of the two- each parameter. Then, a series of individual model runs were

region model for a pulse input of solute. The 1D-ADE and performed to examine model sensitivities when each parameter is

lognormal models are compared for a constant concentration individually varied plus or minus two standard deviations from

step input of tracer, which requires that the RTDMM be compared the mean value. Fig. 4 shows the sensitivity to uncertainties in the

to F(t), the integral of the input RTD. The curves labeled ‘‘Original hydrologic parameters (mean residence time and lognormal

model’’ represent the desired result to which the RTDMM results standard deviation of residence time), and Fig. 5 is a similar set

are compared. The close agreement veriﬁes that when the RTD is of ﬁgures for uncertainty in diffusion and sorption parameters.

160 B.A. Robinson, S. Chu / Computers & Geosciences 52 (2013) 155–163

Table 1

Input hydrologic and transport parameters used in the demonstration calculations.

Flow parameters

Mean of Ln travel time distribution, mln Normal distribution for mln 18.87676 (ln(s)) 18,87676, 0.8

Std. Dev. of Ln travel time distribution, sln Normal distribution for sln ¼ sln =mln 0.026487 0.026487, 7.946 10 3

Geometric parameters

Aperture (m) Constant 1 10 3 1 10 3

Fracture spacing (m) Constant 5 5

Free-water diffusion coefﬁcient Dfree (m2/s), 243

Am Constant 9.49 10 10 9.49 10 10

Dfree (m2/s), 239Pu Constant 1.30 10 9 1.30 10 9

Dfree (m2/s), 235U Constant 6.64 10 10 6.64 10 10

Dfree (m2/s), 239Pa Constant 6.04 10 10 6.04 10 10

Diffusive tortuosity tD, all species Normal distribution for tD ¼ D=Dfree 0.0144 0.0144, 4.176 10 3

Matrix sorption coefﬁcient Kd (cc/g), 243Am Cumulative distribution function CDF 400 (100,0) (400,0.5) (1000,1)

Kd (cc/g), 239Pu CDF 100 (10,0) (100,0.5) (200,1)

Kd (cc/g), 235U CDF 0.2 (0,0) (0.2, 0.5) (3,1)

Kd (cc/g), 231Pa Truncated normal distribution 5500 Range: 103–104, 5500, 1500

a

Parameter values were selected as representative of a fractured rock under oxidizing conditions. Actual values used in an analysis would be site-speciﬁc, depending

on the hydrologic and geochemical conditions at the site. For illustrative purposes, values from the Yucca Mountain Project nuclear waste repository have been adopted in

this study (SNL, 2008).

1 1 1

Normalized Breakthrough

Normalized Breakthrough

Normalized Breakthrough

0.01 0.01 0.01

1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05 1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05 1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05

Time since release, years Time since release, years Time since release, years

1 1 1

Normalized Breakthrough

Normalized Breakthrough

Normalized Breakthrough

1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05 1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05 1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05

Time since release, years Time since release, years Time since release, years

Fig. 4. Sensitivity analyses varying the far ﬁeld model parameters plus and minus two standard deviations from their mean values. Left column: 243Am, Center column:

239

Pu, right column: 235U. Solid curves: base case parameters. Dotted curves: parameters reduced by two standard deviations. Dashed curves: parameters increased by two

orders of magnitude. Top row: mean residence time is varied. Bottom row: log of standard deviation of residence time is varied.

In each set of six ﬁgures, a row denotes the change in a particular the input is able to reach the outlet before decaying. This fraction

parameter, and a column denotes a particular radionuclide (left is strongly inﬂuenced by the early-arriving portion of the inven-

column: 243Am, center column: 239Pu, right column: 235U, 231Pa tory, as inﬂuenced by the parameters of the lognormal RTD. This

not shown). In each individual ﬁgure, the base case simulation is is seen in the bottom row of Fig. 4, which indicates that for

the solid curve, the dotted curve is the parameter reduced by two smaller spreads in the lognormal distribution of residences times,

standard deviations, and the dashed curve is the parameter there is a lessening of the early breakthroughs of 243Am, which in

increased by two standard deviations. turn leads to a smaller fraction of the mass arriving at the outlet

The top row of Fig. 4 indicates that uncertainty in the mean before decaying. By contrast, most parameters have a very small

residence time has a large inﬂuence on the breakthrough curve effect on the breakthrough of 235U because the breakthrough of

through the far ﬁeld model. The largest effect is on 243Am, with a this weakly sorbing radionuclide is controlled principally by the

moderate effect on 239Pu, and a small effect on 235U. The dramatic transport delays of the parent species as well as radioactive decay.

effect on 243Am is controlled by the degree to which a portion of Essentially, 235U travels rapidly through the model once it is

B.A. Robinson, S. Chu / Computers & Geosciences 52 (2013) 155–163 161

1 1 1

Normalized Breakthrough

Normalized Breakthrough

Normalized Breakthrough

0.01 0.01 0.01

1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05 1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05 1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05

Time since release, years Time since release, years Time since release, years

1 1 1

Normalized Breakthrough

Normalized Breakthrough

Normalized Breakthrough

0.01 0.01 0.01

1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05 1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05 1e-02 1e-01 1e+00 1e+01 1e+02 1e+03 1e+04 1e+05

Time since release, years Time since release, years Time since release, years

Fig. 5. Sensitivity analyses varying the far ﬁeld model parameters plus and minus two standard deviations from their mean values. Left column: 243Am, Center column:

239

Pu, right column: 235U. Solid curves: base case parameters. Dotted curves: parameters reduced by two standard deviations. Dashed curves: parameters increased by two

orders of magnitude. Top row: diffusive tortuosity is varied. Bottom row: all sorption coefﬁcients are varied.

generated from decay of 239Pu, so changes in its transport To gain further insight into the underlying uncertainties that

parameters or the ﬂow rate through the system have a relatively control the results, the importance analysis feature in the Gold-

small effect. The inﬂuence of uncertainties in the diffusion and Sim software is used. The importance measure, a metric with a

sorption parameters (Fig. 5) are similar to those for the mean normalized value between 0 and 1, represents the fraction of the

residence time. These parameters impart a delay in the travel variance in a result that is explained by the uncertainty in a

time that acts in a similar manner to an increase in mean particular variable. This measure is useful in identifying non-

residence time. For the parameter ranges selected here, the linear, non-monotonic relationships between an input variable

magnitude of the differences is less for the diffusion and sorption and the result, which conventional correlation coefﬁcients may

parameters than for the travel time parameters. not reveal. To ensure that 500 is a sufﬁcient number of realiza-

tions, additional simulation runs using 100, 1000, and 2000

realizations were performed. Signiﬁcant differences were found

4.3. Monte Carlo analysis in the 100 and 500 realization cases; however, average differences

in the importance measure were only about 3% when comparing

Using the same basic model setup, we ran a suite of Monte the 500 realization case to the 1000 or 2000 realization cases,

Carlo simulation runs with values for the seven uncertain hydro- suggesting that there are statistically insigniﬁcant differences in

logic and transport parameters (the two ﬂow parameters, tortu- the model runs for the cases with greater than 500 realizations.

osity for matrix diffusion, and the sorption Kd values for each Therefore, the 500-realization case is presented below.

species) sampled from stochastic distributions. Results presented In this example, the ‘‘result’’ we use to examine the impor-

below are for a simulation consisting of 500 Monte Carlo realiza- tance of different parameters is the total cumulative arrival of a

tions, with each realization run to a simulation time of 200 ky. species at the outlet at a particular time (i.e. the y-value of the

Note that, as described below, convergence testing using different breakthrough curve at the selected time). To gain further insight,

numbers of realizations indicated that 500 realizations was we selected three times at which to do the importance analysis:

sufﬁcient to obtain stable results. Descriptions of the 12 para- 103, 104, and 105 y. For illustration, we discuss the results for

235

meters are provided in Table 1. The mass ﬂuxes reaching the U. Fig. 7 shows the uncertainty in sorption coefﬁcient for 235U

outlet boundary in response to the unit input of 243Am were (KdU235) dominating the inﬂuence on 235U breakthrough for the

analyzed using the statistical analysis and breakthrough display earlier times (103 and 104 y), even to the extent that it becomes a

capabilities of GoldSim. A description of a few representative more inﬂuential uncertain parameter than the mean travel time.

results follows. This result changes for the longest time frame, with uncertainty in

Fig. 6 shows the composite uncertainty range for 243Am mean travel time (LnorMean) dominating by the end of simula-

breakthrough accounting for uncertainties in all parameters. This tion. The Kd values of the parent species in the decay chain also

range of breakthroughs represents how the uncertainty in the appear as somewhat important to the uncertainty in 235U break-

parameters associated with this species would propagate through through, reﬂecting the fact that retardation of the parent species

a probabilistic systems analysis, impacting bottom-line results lead to greater or lesser amounts of decay to 235U their transport

such as dose. through the system. Thus, while a complete presentation of this

162 B.A. Robinson, S. Chu / Computers & Geosciences 52 (2013) 155–163

1.0e00

1.0e-02

1.0e-04

(g/y r)

1.0e-06

1.0e-08

1.0e-10

1.0e-02 1.0e00 1.0e02 1.0e04 1.0e06

Time (yr)

Percentiles

Greatest Result 95% Percentile 75% Percentile

25% Percentile 5% Percentile Least Result

Mean Median

243

Fig. 6. Uncertainty ranges in the output mass ﬂux time-history curve for Am based on the 500 realization Monte Carlo simulation.

Fig. 7. Importance analysis of the input parameters with respect to uncertainties in the 235U output mass ﬂux. Larger values for a parameter denote that the uncertainties

in that parameter have a larger inﬂuence on the overall uncertainty in the output mass ﬂux.

model is outside the scope of this paper, the illustrative results directly from a process model, using particle tracking or other

show the power of the RTDMM for enabling the groundwater methods, or by otherwise deﬁning the RTD using a simple,

pathway to be represented in a robust yet computationally parameterized representation of travel times such as a normal

efﬁcient manner. or lognormal distribution.

There are important potential beneﬁts to RTDMM approach.

First, in a probabilistic simulation study in which a different RTD

5. Conclusions is speciﬁed for each realization, the ﬂow rates unique to that RTD

can be mapped onto the same grid, with no other adjustments.

This paper presents the theoretical development and numerical Second, the model is easily implemented in any ﬂow and trans-

implementation of a new modeling approach for representing the port modeling code that is capable of accepting prescribed ﬂuid

groundwater pathway in an RA or PA model of a contaminant and solute source terms at multiple grid cells. Third, once the ﬂow

transport system. The model developed in the present study, model is set up, the computational burden of the calculation is no

called the RTD Mixing Model (RTDMM), allows for an arbitrary more onerous than a one-dimensional model with the same

distribution of ﬂuid travel times to be represented, to capture, number of grid cells, even though the model is able to represent

albeit indirectly, the effects of ﬂow processes such as channelized a wide variety of travel time distributions. Finally, for codes that

ﬂow and fast pathways and complex three-dimensional disper- also have reactive transport or other advanced transport options,

sion. This opens the door to be able to specify the RTD curve implementation of the RTDMM makes these features immediately

B.A. Robinson, S. Chu / Computers & Geosciences 52 (2013) 155–163 163

available. For example, use of the FEHM computer code allowed Becker, M.W., Charbeneau, R.J., 2000. First-passage-time transfer functions for

us to incorporate reactive transport and diffusion into the groundwater tracer tests conducted in radially convergent ﬂow. Journal of

Contaminant Hydrology 40, 299–310.

stagnant ﬂuid in the rock matrix away from the ﬂowing fractures, Becker, M.W., Shapiro, A.M., 2003. Interpreting tracer breakthrough tailing from

using that code’s generalized dual porosity model formulation. different forced-gradient tracer experiment conﬁgurations in fractured bed-

A suite of example calculations veriﬁed the correct implemen- rock. Water Resources Research 39 (1), 1024, http://dx.doi.org/10.1029/

tation of the method, and showed its utility for the case of a 2001WR001190.

Dagan, G., Cvetkovic, V., 1996. Reactive transport and immiscible ﬂow in geologic

radioactive decay chain, dual porosity transport and sorption. Our media I. General theory. Proceedings of the Royal Society of London, Series A

examples utilized the option of specifying an RTD with lognormal 452, 285–301.

distribution, which results in a very wide distribution of travel Danckwerts, P.V., 1953. Continuous ﬂow systems: distribution of residence times.

Chemical Engineering Science 2, 1–13.

times that might be more representative of a highly heteroge- Destouni, G., Sassner, M., Jensen, K.H., 1994. Chloride migration in heterogeneous

neous, fractured medium than the traditional 1D-ADE model. soil 2. Stochastic modeling. Water Resources Research 30 (3), 747–758.

Similarly, two-region or other models often yield complex, Erickson, N., Destouni, G., 1997. Combined effects of dissolution kinetics, second-

perhaps bimodal RTD curves, yet the RTDMM can implement this ary mineral precipitation, and preferential ﬂow on copper leaching from

mining waste rock. Water Resources Research 33 (3), 471–483.

type of model with no additional computational burden than is Ginn, T.R., 2001. Stochastic-convective transport with nonlinear reactions and

encountered with the 1D-ADE model. Finally, though not the mixing: ﬁnite streamtube ensemble formulation for multicomponent reaction

focus of the present study, it would be possible to use the systems with intra-streamtube dispersion. Journal of Contaminant Hydrology

47 (1), 1–28.

experimentally measured breakthrough curve from a conserva-

GoldSim Technology Group, 2010. Goldsim Probabilistic Simulation Environment

tive tracer as direct input to the RTDMM, so that more complex User’s Guide, Version 10.5, December, 2010.

reactive tracers can be modeled. In this way, the advective Gupta, A., Destouni, G., Jensen, M.B., 1999. Modelling tritium and phosphorus

processes would be captured directly without the preliminary transport by preferential ﬂow in structured soil. Journal of Contaminant

Hydrology 35, 389–407.

step of ﬁtting the conservative tracer to an idealized model, which Maloszewski, P., Zuber, A., 1993. Tracer experiments in fractured rocks: matrix

can add a level of uncertainty to the interpretation of reactive diffusion and the validity of models. Water Resources Research 29 (8),

transport experimental results. 2723–2735.

Rainwater, K.A., Wise, W.R., Charbeneau, R.J., 1987. Parameter estimation through

The RTDMM implementation was further demonstrated by

groundwater tracer tests. Water Resources Research 23, 1901–1910.

presenting a multi-realization result that used the importance Robinson, B.A., Tester, J.W., 1984. Dispersed ﬂuid ﬂow in fractured reservoirs: an

sampling method provided by GoldSim to investigate the degree analysis of tracer-determined residence time distributions. Journal of Geo-

to which uncertainties in each parameter inﬂuence the overall physical Research 89 (B12), 10374–10384.

Robinson, B.A., Tester, J.W., 1986. Characterization of ﬂow maldistribution using

uncertainty of the contaminant breakthrough results. Because of inlet–outlet tracer techniques: an application of internal residence time

the deceptively simple yet very ﬂexible and computationally distributions. Chemical Engineering Science 41 (3), 469–483.

efﬁcient formulation, we anticipate that the RTDMM may ﬁnd Robinson, B.A., Viswanathan, H.S., Valocchi, A.J., 2000. Efﬁcient numerical techni-

ques for modeling multicomponent ground-water transport based upon

wide application as a method for representing the groundwater

simultaneous solution of strongly coupled subsets of chemical components.

pathway in RA and PA systems models. Advances in Water Resources 23, 307–324.

Robinson, B.A., Viswanathan, H.S., 2003. Application of the theory of micromixing

to groundwater reactive transport models. Water Resources Research 39, 11, h

Acknowledgments ttp://dx.doi.org/10.1029/2003WR002368.

Robinson, B.A., Li, C.H., Ho, C.K., 2003. Performance assessment model develop-

ment and analysis of radionuclide transport in the unsaturated zone, Yucca

Funding for portions of this work was provided by the Mountain, Nevada. Journal of Contaminant Hydrology 62–3, 249–268.

Department of Energy, Ofﬁce of Nuclear Energy Advanced Fuel SNL, 2008. Particle Tracking Model and Abstraction of Transport Processes. MDL-

Cycle Initiative. The authors thank the anonymous reviewers of NBS-HS-000020 REV 02 ADD 02. Sandia National Laboratories, Las Vegas,

Nevada.

our manuscript for their constructive and thorough reviews, Tang, D.H., Frind, E.O., Sudicky, E.A., 1981. Contaminant transport in fractured

which enabled us to strengthen the paper considerably. porous media: analytical solution for a single fracture. Water Resources

Research 17 (3), 555–564.

Viswanathan, H.S., Robinson, B.A., Valocchi, A.J., Triay, I.R., 1998. A reactive

References transport model of neptunium migration from the potential repository at

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Arnold, B.W., Hadgu, T., Sallaberry, T.J.M., 2008. Sensitivity Analyses of Radio- Zyvoloski, G.A., Robinson, B.A., Dash, Z.V., Trease, L.L., 1997. Summary of the

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