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Manuscript_cdc289358a67c55f79bd5cd19a828e28

Numerical Estimations of Storage Efficiency for the Prospective CO2 Storage

Resource of Shales
Evgeniy M. Myshakin,a,b* Harpreet Singh,a Sean Sanguinito,a,b Grant Bromhal,a
Angela L. Goodmana
a
U.S. Department of Energy, National Energy Technology Laboratory, 626 Cochrans Mill Road,
Pittsburgh, PA 15236 and 3610 Collins Ferry Road, Morgantown, WV 26507
b
AECOM, 626 Cochrans Mill Road, P.O. Box 10940, Pittsburgh, PA 15236

Highlights:

 Hydraulically fractured shale formations may serve as reservoirs for carbon dioxide
sequestration
 Numerical simulations applied to estimate carbon dioxide storage efficacy in shales
 Intended for national-scale prospective resource estimation and screening

Abstract
Hydrocarbon-bearing shale formations might be an attractive geologic reservoir
for permanent carbon dioxide (CO2) storage. Shale formations applicable for
storage require previous hydrocarbon production to deplete a reservoir, hydraulic
fracturing to provide a highly-permeable stimulated zone, sufficient depths
(generally > 800 m or 2,600 feet) to maintain CO2 in a supercritical state, and an
overlying seal to prevent CO2 migration to underground sources of drinking water
and into the atmosphere. CO2 is stored in shale as a free phase within fractures
and matrix pores, and as a sorbed phase on organic matter and clay minerals.
Recently in our previous work, we presented a screening-level assessment
methodology for CO2 storage in shales using a volumetric approach. The
approach deals with reduction of CO2 storage through estimations of efficiency
factors based on petrophysical properties (i.e., bulk volume, porosity, sorption,
etc.) and their limitations on fluid transport. Here, we conducted numerical

*
Corresponding author.
Telephone: 1-412-386-5741; Fax: 1-412-386-5870
E-mail address: evgeniy.myshakin@netl.doe.gov

© 2018 published by Elsevier. This manuscript is made available under the Elsevier user license
https://www.elsevier.com/open-access/userlicense/1.0/
simulations using the FRACGEN/NFFLOW simulator to study the CO2 injection
into a depleted hydro-fractured shale reservoir to estimate storage efficiencies
using a range of reservoir parameters and injection scenarios. Specifically, the
ranges for two efficiency factors, 𝐸𝜙 and 𝐸𝑆 , measure the effectiveness of free and
sorbed CO2 storage. These efficiency factors were estimated to have P10 to P90
probability ranges of 0.15 to 0.36 for 𝐸𝜙 and 0.11 to 0.24 for 𝐸𝑆 , reported after 60
years of CO2 injection.

Keywords: carbon storage; storage resource; shale, storage efficiency

I. Introduction

Emissions of CO2 from industrial sources to the atmosphere can be prevented by

capturing CO2 from its emission source and injecting it into the subsurface, e.g., deep saline
formations, depleted conventional hydrocarbon reservoirs, and unmineable coal seams (Koide et
al., 1992; Harpalani et al., 2006; Bachu et al., 2007; Zhou et al., 2008; Goodman et al., 2011).
Due to the recent boom of shale hydrocarbon production in the United States, availability of
depleted shale reservoirs presents a promising opportunity for storing CO2. Unlike conventional
reservoirs, shale reservoirs have a relatively shorter production life (~5 years) (Zuo et al., 2016)
due to fast depletion of hydrocarbons through fractures, which can be extended to a maximum of
~20 years through enhanced recovery methods (Singh and Cai, 2018). Once these reservoirs are
depleted, they would present an economical advantage for CO2 storage as these reservoirs tend to
have thousands of wells that can be converted to CO2 injectors. CO2 injected in shales is
expected to be stored by sorption on organic matter and clay minerals and as free phase in
permeable matrix pores and both hydraulic and natural fractures. Few predictions for CO2
storage in specific shale plays have been reported by various researchers using a dynamic
approach (Kang et al., 2011; Tao and Clarens, 2013; Godec et al., 2013; Chen et al., 2015; Chen
et al., 2016). A static approach to screen shale formations for prospective CO2 storage that
applies a volumetric equation with petrophysical parameters and efficiency factors was proposed
recently by a few studies (Goodman et al., 2014; Senger et al., 2015; Levine et al., 2016). As per
the Levine et al. (2016) methodology, the prospective storage resource of CO2 in shales at a
national and regional scale is estimated using the following volumetric equations:

𝐺𝐶𝑂2 = 𝐴𝑡 𝐸𝐴 ℎ𝑔 𝐸ℎ [𝜌𝐶𝑂2 𝜙𝐸𝜙 + 𝜌𝑠𝐶𝑂2 (1 − 𝜙)𝐸𝑆 )] (1)

and

𝑉𝑒 = 𝐴𝑡 𝐸𝐴 ℎ𝑔 𝐸ℎ (2)

where, GCO2 is the CO2 storage resource (mass) of the shale formation; At is the total area (map
view) of the shale formation being assessed for CO2 storage; hg is the gross thickness of the shale
formation; Ve is the net effective volume of the formation (𝐴𝑡 𝐸𝐴 ℎ𝑔 𝐸ℎ ); CO2 is the density of CO2
at the (averaged) pressure (𝑃̅) and (averaged) temperature (𝑇̅) of Ve prior to production;  is the
percentage of bulk volume that is void volume; 𝜌𝑠𝐶𝑂2 is the maximum mass of CO2 sorbed per
unit volume of solid rock, e.g., the asymptotic value of a sorption isotherm; 𝐸𝐴 is the fraction of
shale formation total area available for CO2 storage; 𝐸ℎ is the fraction of shale formation gross
thickness available for CO2 storage; 𝐸𝜙 is the fraction of shale porosity within the net effective
volume of the formation, Ve, available for CO2 storage; and 𝐸𝑆 is the fraction of the total
potential sorbed volume of CO2 within the net effective volume of the formation, Ve. The intent
of this methodology is to inform stakeholders and decision makers about the potential for CO2
storage in shale systems. A great deal of uncertainty is inherent in the terms represented by
Equation (1), specifically the efficiency factor terms which accommodate the complexities of the
fundamental processes associated with production, injection, and storage within shales due to a
lack of knowledge of shale systems.

As discussed in Levine et al. (2016) a set of principles and methods was developed to
estimate prospective CO2 storage in shales. At this national scale, prospective storage resources
are defined during the exploration phase when potential sub-regions are identified, as analogous
to the exploration process applied in the petroleum industry. A national scale methodology must
rely on limited data that is expected to be available at the earliest project stage and not detailed
geophysical and geochemical information. Thus, two broad categories for CO2 storage in shale
were determined – storage of CO2 as a fluid phase in the fractures and matrix pores and as an
adsorbed phase on organic matter and clays (Levine et al., 2016). Other storage mechanisms,
such as dissolution in an aqueous phase, are considered to be much smaller than free phase or
sorbed phase storage, and are thus not included in the methodology. The purpose of this paper is
to continue method development by determining a range of the efficiency factor terms
introduced by Levine et al. (2016) and shown in Equation (1) that can be used to estimate
prospective CO2 storage in shale. Each efficiency factor term in Equation (1) is given by a
fraction, p, that ranges between 0 and 1. The ranges of the efficiency factor terms 𝐸𝜙 and 𝐸𝑠
were calculated numerically using FRACGEN and NFFLOW (FRACGEN/NFFLOW, 2014).
The results of these simulations are intended to provide ranges of the p values reported at the P10
and P90 interval as input values for the CO2 storage methodology introduced by Levine et al.
(2016) and shown in Equation (1). The simulated storage efficiency factor ranges developed in
this paper are applicable to dry gas shales characterized by mainly one phase flow in pore space
and fractures.
II. Methodology and Definitions

2.1. Simulated CO2 Storage Efficiency Factor Terms, 𝐸𝜙 𝑎𝑛𝑑 𝐸𝑠

Equation (1) introduces four efficiency factor terms, 𝐸𝐴 , 𝐸ℎ , 𝐸𝜙 , and 𝐸𝑠 . Two of them, 𝐸𝐴
and 𝐸ℎ , are used to define a net effective volume (Ve) of the formation accessible for CO2
storage. As described in detail by Levine et al. (2016), 𝐸𝐴 reduces the storage resource by
accounting for both regional proximity and social data attributes that affect area, while 𝐸ℎ
reduces the storage resource by discounting geologic storage features that change with depth.
Information for assigning the terms needed to calculate the net effective volume of the formation
is determined from publicly available data sources and field data at the national and regional
scale. The remaining two efficiency factors, 𝐸𝜙 and 𝐸𝑠 , are calculated at the well-scale and are a
subset of the net effective volume where undesirable areal and vertical features have been
disqualified. The efficiency factor terms, 𝐸𝜙 and 𝐸𝑠 , reflect the fraction of the maximum amount
of CO2 that can be stored in a net effective formation volume as a free phase within fractures and
matrix pores and as a sorbed phase on organic matter and clay minerals.

In these simulations, the reservoir model is designed to represent the net effective volume
by simulating the fracture network and pore space available for CO2 to flow. The focus of this
effort is to calculate representative ranges for the terms 𝐸𝜙 and 𝐸𝑠 . In the simulations, those
factors are calculated using the following equations:

𝑓𝑟𝑒𝑒
𝑉𝑖
𝐸𝜙 = 𝑓𝑟𝑒𝑒 (3)
𝑉𝑚𝑎𝑥

𝑉 𝑠𝑜𝑟𝑏
𝐸𝑆 = 𝑉𝑖𝑠𝑜𝑟𝑏 (4)
𝑚𝑎𝑥

𝑓𝑟𝑒𝑒
where 𝑉𝑖 is the simulated CO2 volume stored in a reservoir volume contacted by the
propagating CO2 plume as a free gas, 𝑉𝑖𝑠𝑜𝑟𝑏 is the simulated CO2 volume stored in the same
𝑓𝑟𝑒𝑒
reservoir volume as a sorbed phase, 𝑉𝑚𝑎𝑥 is the maximum CO2 volume that can be stored in a
reservoir volume as a free gas at initial (avearged) 𝑃̅ and 𝑇̅ conditions before gas production, and
𝑠𝑜𝑟𝑏
𝑉𝑚𝑎𝑥 is the maximum CO2 volume that can be stored in the reservoir volume as a sorbed phase
at initial (averaged) 𝑃̅ and 𝑇̅ conditions before gas production. This is consistent with the
recommendation by Levine et al. (2016) where all properties should be calculated at the average
reservoir pressure and temperature prior to hydrocarbon production. The initial 𝑃̅ (30.34 MPa)
and 𝑇̅ (62.8oC) conditions of the shale reservoir before production of hydrocarbons were
estimated from average values of the following top ten shale systems in North America:
Marcellus, Haynesville, Bossier, Barnett, Fayetteville, Muskwa, Woodford, Eagle Ford, Utica,
𝑓𝑟𝑒𝑒
and Montney (Jarvie, 2012). The values of 𝑉𝑖 and 𝑉𝑖𝑠𝑜𝑟𝑏 are the output of the simulations on
CO2 injecton into the depleted shale reservoir model. The reservoir volume contacted by the CO2
plume is estimated using the “convex hull” method for accessible reservoir volume (Gorecki et
al., 2009).

As noted by Bachu et al. (2014) efficiency factors can change both temporally and
spatially, thus the time scale of storage efficiency should be reported with prospective storage
estimates. They indicate that CO2 storage capacity has a time dependency over the lifetime of a
CO2 storage project. For CO2 injection into saline formations, Gorecki et al. (2009) opted to
estimate storage coefficients at the end of CO2 injection. In this work, besides estimation of the
efficiency factors at the end of injection, the factors were also estimated between selected time
points “dynamically through injection” in notation of Gorecki et al. (2009). This was done to
deliver better applicability of the efficiency terms to various operational time intervals at an
injection site.

𝑓𝑟𝑒𝑒 𝑠𝑜𝑟𝑏
The estimations of 𝑉𝑚𝑎𝑥 and 𝑉𝑚𝑎𝑥 were made using two methods. In Method I,
𝑓𝑟𝑒𝑒 𝑠𝑜𝑟𝑏
𝑉𝑚𝑎𝑥 and 𝑉𝑚𝑎𝑥 , based on the total reservoir volume, are used to calculate theoretical maxima of
CO2 that can be stored as free and sorbed phases, respectively. The resulted efficiency factors
increase as injection time progresses since CO2 continuously accumulates in the defined total
reservoir volume. These factors produce a reservoir size dependancy, and to apply them to a
target reservoir size, a transition coefficient is needed to adapt values esimated in this work for
the selected reservoir drainage area (1,370 x 1,370 m) to a particular target reservoir drainage
𝑓𝑟𝑒𝑒 𝑠𝑜𝑟𝑏
area. In Method II, 𝑉𝑚𝑎𝑥 and 𝑉𝑚𝑎𝑥 are computed based on the same reservoir volume contacted
by the CO2 plume at selected time points. In other words, the CO2 volume quantities in
Equations (3) and (4) are related to the same rock volume contacted by CO2 at selected time
points. The factors calculated using Method II are free from size dependancy and provide insight
into flow evoluton as CO2 propagates through stimulated (hydraulically-fractured) and non-
stimulated (natural fractures and pore matrix) reservoir volumes, and the result is the
understanding of a shale reservoir’s capability to accomodate CO2 with time.

III. Simulation Details

3.1 Description of the Reservoir Model

FRACGEN and NFFLOW (FRACGEN/NFFLOW, 2014), two explicit-fracture reservoir

modeling software programs developed by the National Energy Technology Laboratory (NETL)
to characterize discrete-fracture networks and simulate fluid flow, respectively, are specifically
developed for reservoirs where flow pathways are dominated by a network of discrete fractures.
FRACGEN generates stochastically a realization of a natural fracture network using three
different models to sample fitted statistical distributions for various fracture set attributes. This
realization is controlled by natural fracture orientations, lengths, apertures, spacings between
fractures, and fracture network connectivity. To build the model of the fractured shale reservoir,
Model 1 was used (FRACGEN/NFFLOW, 2014) that randomly distributes the centers of
fractures over the entire region using a uniform probability density. The fracture connectivity
control functions can tune the range of the fracture length distribution keeping the input mean
fracture lengths the same. The hydraulic fractures located perpendicular to the horizontal well are
specified deterministically.

NFFLOW models fluid flow in the fracture network on a segment-by-segment basis,

accounting for flow into or from the matrix for each segment as a function of one-dimensional
models and the fluid flow history. The discrete fractures are modeled by connecting three
different domain types: fracture intersections, fracture midpoints, and matrix rock. Fractures are
treated as a gap between two parallel surfaces, giving a cubic law relationship to the volumetric
flow rates within fractures:

hw3  dP
Q (5)
12  ds

where Q is the flow rate, h is the formation thickness, w is the fracture aperture, µ is the fluid
viscosity, and dP/ds is the pressure gradient. Fracture intersections are considered to have zero
volume and therefore no accumulation term, so the material balance for a fracture intersection I
is given by:

QI n  QI s  QI e  QI w  QI u  QI d  0 (6)

where n, s, e, w, u, d are the connecting mid-point sections to the north, south, east, west,
upward, and downward respectively. Fracture section mid-points are where the volume of the
fractures is accounted for and where fluid transfer to and from the matrix rock occurs. Fracture
segment mid-points are governed by the material balance equation:

hw d P
 dl  QI e  Qe E  QR  QL
RC RC
(7)
RT dt I  E Z

where I and E are the two connecting fracture intersections, and R and L are the two connecting
matrix blocks. Rock matrix blocks are only connected to a single fracture mid-point, so no cross-
matrix flow is modeled. Matrix flow is modeled with Darcy’s law given the governing material
balance equation:

( ) ( A  )
A  0 (8)
t x
where A is the cross-sectional area of the matrix block, φ is the porosity of the matrix,
and ρ is the density of the fluid.

The NFFLOW code treats gas residing in the matrix as a free phase in the hydraulic and
natural fractures, and the matrix pore space as a sorbed phase on the solid rock. Sorption is
represented by the Langmuir sorption function and assumes isothermal conditions where the gas
component can adhere as a monolayer. A competitive sorption process is not accounted for in the
current version of the code. Although it is known from several experimental studies that
isothermal surface diffusion in shales might show an abnormal decrease in adsorption at high
pressures (Beaton et al., 2010a; Beaton et al., 2010b; Rexer et al., 2013; Lutynski et al., 2016).
Here, we assume that the Langmuir sorption function is adequate to model the sorption behavior
for screening prospective storage in shales at the regional and national scales. The total amount
of gas in each matrix block is considered to be the mass sum of free and sorbed gas. Details of
the FRACGEN/NFFLOW development and its application can be found elsewhere (FRACGEN/
NFFLOW, 2014; McKoy and Sams, 1997; Myshakin et al., 2015).

Figure 1 shows three different plan-views of the shale reservoir, including the natural
network distributions and locations of hydraulic fractures labeled as SHAPES 0-2. Three plan-
view shapes of hydraulic fractures were chosen as typical plan-view shapes following the
guidance by Suliman et al. (2013). SHAPE 0 shows the rectangular stimulated reservoir volume
(SRV) defined by the hydraulic fracture of a simple bi-wing geometry (uniform wing length,
152 m), the shape that would be commonly considered in simulators. SHAPES 1 and 2 provide
variable fracture lengths (wing lengths, 91 – 213 m) and are represented by elongated hydraulic
fractures at the ends of the lateral and an oval-like pattern. For each shape realization, the sum of
all hydraulic fracture lengths remains the same. In spite of different shapes defining SRV, it is
important to set the same total hydraulic fracture lengths to provide consistency. The dimensions
of the rectangular reservoir drainage area were selected as 1,370 x 1,370 m. The well lateral
shown as a black line in Figure 1 is placed in the middle of the reservoir domain. The hydraulic
fractures shown as red lines in Figure 1 are represented by the parallel fractures located
perpendicular to the lateral and provide communication between the natural fracture network
(shown as green lines in Figure 1) and the horizontal well.

SHAPE 0 (rectangular) SHAPE 1 (elongated at lateral ends) SHAPE 2 (oval-like)

Figure 1. The horizontal cross-section of the shale reservoir model showing natural (green) and hydraulic
(red) fractures. The lateral (black) is placed in the middle of the reservoir. Three different hydraulic
fracture realizations are depicted (SHAPES 0-2).

Table 1. Hydraulic and Natural Fracture Parameters for the Shale Reservoir Model*

Parameters of Natural Fracture Network Values

 Effective fracture aperture, m 3.8 x 10-6 and 3.7 x 10-6 **
Fracture lengths, m 61 – 122 and 30 – 91 **

15300 (high density)

Number of fractures
6300 (low density)

Parameters of Hydraulic Fractures Values

Effective fracture aperture, m 1.39 x 10-5
Spacing between clusters, m 15 m
Spacing between stages, m 107 m
Number of stages (Figure 1) 8
Number of clusters/well lateral 24
Hydraulic fracture half-length (wing length, Figure 1), m 91 – 213
Total number of hydraulic fractures 72
Total length of the lateral, m 876
* **
ICMI report, 2013; Kulga et al., 2014. Two fracture sets (green lines in Figure 1)

Table 1 compiles parameters of hydraulic and natural fractures explicitly considered to

build the shale reservoir model and taken from various literature sources for shale systems in
North America. For the natural fracture network characterization, the values representing two
sets of fractures (joints) were collected or estimated from multiple sources (Kulga et al., 2014;
Engelder, 2008; Bruner and Smosna, 2011; Inks et al., 2014; Lash et al., 2004; Zagorski et al.,
2011; Ejofodomi et al., 2011; Zhang et al., 2014; Soeder, 1988; Eastern Gas Shale Project,
1981). The effective apertures of hydraulic and natural fractures were estimated based on history
matching gas production rates and flowing bottom-hole pressures (FBHP) for the commercial
Marcellus shale lateral wells in Southwestern Pennsylvania (Kulga et al., 2014). The parameters
characterizing the hydraulic fracture spacings, lengths, and numbers were taken from the
Industrial Carbon Management Initiative report (ICMI report, 2013). In that report,
PSU‐SHALECOMP (Kulga et al., 2014), FRACGEN/NFFLOW (FRACGEN/NFFLOW, 2014),
and two commercial simulators, Eclipse (Eclipse, 2018) and CMGGEM (CMGGEM, 2018),
were validated against field data. The four simulators provided consistent predictions for carbon
dioxide injection into a depleted shale reservoir over a period of 60 years.

CO2 injection into the depleted shale reservoir was assumed to occur over a period of 60
years using selected time points, 5, 10, 20, 30, 40, 50, and 60 years, while noting that the CO2
storage resource of a shale reservoir varies according to local site conditions and specifics of
infrastructure in place. As a general requirement, CO2 injection should be commercially and
technically viable on the time scale of site operation. At present, it is difficult to use a common
approach to estimate a time frame required for CO2 injection into shale reservoirs due to lack of
information. With a growing number of field projects, a generalized method to estimate those
quantities for well-characterized storage sites is expected to emerge.

3.2 Simulation Cases

To calculate simulated efficiency factor terms, 𝐸𝜙 and 𝐸𝑠 , for CO2 injection, typical
ranges of parameters relevant for shales were selected based on the literature data. The boundary
values of the parameters were used to simulate the amount of CO2 injected in the shale reservoir
and the reservoir volume that is contacted by the CO2 plume. These parameters are initial
reservoir pressure, matrix permeability, Langmuir volume, density of natural fracture center
points which is a reciprocal product of average fracture spacing and mean fracture length,
injection pressure, matrix porosity, and shale thickness (Table 2). As discussed in the literature,
these parameters are considered to be the most important in controlling the fluid transport in
shale reservoirs (Goodman et al., 2014; ICMI report, 2013). The values for these parameters
were taken as measured or evaluated quantities for the shale plays. The selection of the lower
and upper values listed in Table 2 is limited to the literature data discussed in detail in
Supplemental Materials for each parameter. Each simulation case is constituted of a combination
of symbols indicating corresponding parameters and each symbol is augmented with “L” or “H”
referrring to lower or upper value, respectively, as listed in Table 2. In total, 57 simulation cases
were run with FRACGEN/NFFLOW, and the designation of the cases and corresponding
efficiency factor values are given in Table S1 (Supplementary Materials).

Table 2. Range of Input Parameters to Estimate CO2 Storage Efficiency in the Shale Reservoir Model

Values
Parameter Symbol References
LOW (L) HIGH (H)
Initial reservoir pressure, MPa R 3.45 6.90 [1,2]
Matrix permeability, m2 M 5.92 x 10-21 5.92 x 10-19 [3-9]
Langmuir volume, m3/ton V 3.40 9.35 [10-14]
-5 -4
Density of natural fracture center D 6.35 x10 and 2.03 x10 and [4-6,15-24]
 points, m-2 3.81 x10-5 * 1.91 x10-4 *
Injection pressure, MPa I 20.68 27.58 [15,25-29]
Matrix porosity P 0.045 0.125 [3-8]
Thickness, m T 30 152 [15]
*
Two natural fracture sets (Figure 1); [1] Zhang et al., 2017a, [2] Zhang et al., 2017b; [3] Kulga et al., 2014; [4]
Engelder, 2008; [5] Bruner and Smosna, 2011; [6] Zhang et al., 2014; [7] Hildenbrand and Kroos, 2003; [8]
Ruppert et al., 2013; [9] Nuttall et al., 2005; [10] Inks et al., 2014; [11] Vermylen, 2011; [12] Jin and Firoozabadi,
2014; [13] Busch et al., 2008; [14] Chareonsuppanimit et al., 2012; [15] Jarvie, 2012; [16] Lash et al., 2004; [17]
Zagorski et al., 2011; [18] Ejofodomi et al., 2011; [19] Soeder, 1988; [20] Ataman, 2008; [21] Yu et al., 2014; [22]
Laderia and Price, 1981; [23] Wiltschko et al., 1991; [24] Nelson, 2001; [25] Zhou et al., 2008; [26] Gorecki et al.,
2009; [27] ICMI report, 2013; [28] Hildenbrand et al., 2002; [29] Hildenbrand et al., 2004.

IV. Results and Discussion

The minimum and maximum values of the simulated efficiency factors, 𝐸𝜙 and 𝐸𝑠 ,
calculated using Equations (3) and (4) together with P10 and P90 values are listed in Table 3. The
P10 notation reflects there is a 10 percent probability that an estimated value is less than the P10
value, and the P90 notation reflects there is a 90 percent probability that the estimated value is
less than the P90 value). The values reported in Table 3 were collected after analyzing efficiency
factors calculated using the combinations of input parameters given in Table 2. Table 3 shows
that efficiency factors calculated by Method I gradually increase from 5 to 60 years of injection
time. The efficiency factors estimated through Method II demonstrate maxima within the 20- to
40-year time interval. That suggests that effectiveness of carbon storage declines with time as
more CO2 propagates into untreated areas beyond the SRV where natural fractures and pore
network are the only conduits for flow.

Table 3. Ranges of Eϕ and ES Efficiency Factor Terms for Carbon Dioxide Storage in Shales Calculated
Using Method I and Method II (values in the parentheses)

E
Years Minimum Maximum P10 P90
5 0.04 (0.17) 0.12 (0.56) 0.04 (0.25) 0.12 (0.53)
10 0.06 (0.22) 0.18 (0.59) 0.07 (0.31) 0.18 (0.57)
20 0.08 (0.27) 0.23 (0.60) 0.09 (0.34) 0.23 (0.59)
30 0.10 (0.28) 0.28 (0.60) 0.11 (0.36) 0.27 (0.58)
40 0.11 (0.28) 0.31 (0.59) 0.13 (0.37) 0.30 (0.56)
50 0.14 (0.27) 0.34 (0.58) 0.14 (0.34) 0.33 (0.55)
 60 0.15 (0.26) 0.37 (0.57) 0.15 (0.34) 0.36 (0.54)
ES
5 0.02 (0.09) 0.07 (0.36) 0.03 (0.14) 0.07 (0.34)
10 0.04 (0.13) 0.11 (0.48) 0.05 (0.16) 0.11 (0.44)
20 0.06 (0.16) 0.17 (0.57) 0.07 (0.20) 0.17 (0.53)
30 0.08 (0.15) 0.21 (0.59) 0.09 (0.20) 0.20 (0.56)
40 0.09 (0.15) 0.25 (0.58) 0.10 (0.21) 0.22 (0.57)
50 0.10 (0.15) 0.26 (0.57) 0.11 (0.20) 0.23 (0.56)
60 0.11 (0.14) 0.27 (0.55) 0.11 (0.19) 0.24 (0.55)

Although Method II provides useful insight into how flow within SRV, natural fractures and
matrix pore space affects efficiency factors, Equation (1) is intended to be used with a total shale
reservoir volume (see, the definitions of the At and hg terms in that equation given above). Thus,
for the estimations of the overall storage efficiency expressed by Equation (1), the values
obtained by Method I are recommended to be used. Specifically, the ranges for two efficiency
factors, 𝐸𝜙 and 𝐸𝑆 , were estimated to have P10 to P90 probability ranges of 0.15 to 0.36 for 𝐸𝜙
and 0.11 to 0.24 for 𝐸𝑆 , reported after 60 years of CO2 injection. A description of the U.S. DOE-
NETL methods for estimating prospective storage can be found in Goodman et al. (2011) and
Goodman et al. (2016). In these methods, overall storage efficiency is calculated using a log-
odds approach with Monte Carlo sampling. Ranges of the efficiency factor terms defined in
Equation (1) at the P10 and P90 probability interval are required as inputs to estimate an overall
storage efficiency and ultimately prospective storage resource. At the prospective scale, it is
assumed that the storage efficiency terms are independent and not correlated. The ranges of the
simulated efficiency factor terms, 𝐸𝜙 and 𝐸𝑠 , can be applied to Equation (1) to estimate
prospective storage of CO2 in targeted shale systems. Representative ranges of the remaining
efficiency factor terms, 𝐸𝐴 and 𝐸ℎ , that are used to define a net effective volume of the formation
accessible for CO2 storage, can be assigned from publicly available data sources and field data
available at the national and regional scale.

Figure 2 displays the 𝐸𝜙 and 𝐸𝑆 efficiency factors computed using Method I over 60
years of injection time. From 5 to 20 years, the values demonstrate a steeper increase when
compared to the subsequent 20- to 60-year period where a nearly linear trend is found in the
dependency of the minimum/maximum values with time. In Method II, variations in
𝐸𝜙 and 𝐸𝑆 reflect the transport heterogeneity of CO2 through shale media for a free phase storage
in hydraulic fractures, natural fractures, and matrix pores and a sorbed phase storage on organic
matter and clay minerals. The transport through the reservoir is a strong function of the pressure
gradient and absolute pressure controlling the CO2 flow as free and sorbed phases. The analysis
of simulated efficiency factors obtained by Method II indicates that low/high natural fracture
density, injection pressure, and high/low initial reservoir pressure are mainly responsible for the
decrease/increase of the 𝐸𝜙 and 𝐸𝑆 factors shown in Figure 3. Additionally, variability in matrix
permeability and Langmuir volume is also important for 𝐸𝜙 and 𝐸𝑆 . Both Table 3 and Figure 3
show that for the lower limits, the largest factors appear over 20-30 years for 𝐸𝜙 and 20-40 years
for 𝐸𝑆 , while for the upper limits the maximum is reached after 20 years of injection for storage
in pore space and fractures, and the largest value occurs during 20-30 years of injection for
storage as a sorbed phase.
 0.40
a) a)
0.35 0.6

0.30
0.5
0.25
E 

E 
0.20 0.4

0.15
0.3
0.10

0.05 0.2
0.00
0.25 b) b)
0.6

0.20
ES

ES
0.4
0.15

0.10
0.2
0.05

0.00 0.0
0 10 20 30 40 50 60 0 10 20 30 40 50 60
years years

Figure 2. Simulated efficiency factors for carbon Figure 3. Simulated efficiency factors for carbon
dioxide storage a) in pore space and fractures dioxide storage a) in pore space and fractures and
and b) in a sorbed phase calculated using b) in a sorbed phase calculated using Method II.
Method I.

The injected carbon dioxide travels throughout the wellbore in induced fractures and
natural fracture networks as the primary conduit versus the negligible flow through matrix pore
volume with permeability on the order of nano-darcy. Because of low matrix permeability, it
takes a long time for the pressure pulse to travel from the matrix to the outer parts of the
reservoir, and as a result, transient flow is expected to last for long periods of time within a shale
reservoir as if it is infinite in size. At late times, flow is expected to be at pseudo-steady state
when the reservoir boundaries are reached and flow continues in a state of pseudo-equilibrium
(Bello, 2009). The analysis has revealed that during continuous active transport from the
wellbore into the SRV, the efficiency factor terms increase. After flow continues into untreated
zones through natural fracture network as a main conduit, the efficiency factor terms decline.
Thus, the presence of the maxima on efficiency factor curves can be attributed to change of flow
regimes and the ability of the SRV to efficiently transmit and store fluids.
 After comparing the efficiency factor ranges corresponding to different regimes, an
important observation is deduced. A high efficiency factor does not always mean high bulk
formation permeability (Table S1). In other words, the ability of a reservoir with high matrix
porosity that can transmit fluids faster would not necessarily result in a reservoir with high CO 2
storage potential. This is attributed to permeabilities as the measurement of the ability of porous
media to transmit fluids, while the factors are relative quantities involving estimates of the
theoretical maxima of stored gas. For the high porosity cases, the corresponding theoretical
maxima are also high, and injected CO2 utilizes the available volume to a lesser extent than cases
with low porosity and low theoretical maxima.

There are assumptions and limitations of the model influencing transport of injected CO2
at small spatial scales in shale reservoirs that could refine the accuracy of the reported efficiency
factors. Knudsen diffusion and slip flow are known to affect gas flow at low pressure within the
confined pores of the shale matrix (Singh and Javadpour, 2013; Singh and Javadpour, 2016;
Singh et al., 2014) and coupled matrix-fracture system (Singh and Azom, 2013). These two flow
and transport mechanisms can affect the overall mass transport (generally dominated by
convective flux given by Darcy’s law) depending on pore size distributions, pressure and
temperature conditions, and the chemical nature of pore walls (Heller et al., 2014). The reactive
nature of CO2 is known to significantly impact the pore structure of the conventional reservoir
rock (Singh, 2017), something that could be even more important in the case of shale rocks with
extremely tight pore space. Kang et al. (2011) studied the ability of shale core samples to store
CO2, and concluded that although transport in the inorganic matrix is viscous (Darcy) flow,
transport in the organic pores is not due to flow but mainly to molecular transport mechanisms:
pore and surface diffusion. Heller et al. (2014) indicated that contribution of slip flow could be
above Darcy flux at low pressures corresponding to conditions in the beginning of injection into
a depleted shale reservoir. Several other mechanisms of fluid transport in shale have recently
been investigated in the laboratory and reviewed by Singh (Singh, 2016), for example, (i)
counter-current imbibition due to osmotic potential created by the difference of salinities
(Fakcharoenphol et al., 2014; Fakcharoenphol et al., 2016) may force the trapped fluid out of the
nanopores; and (ii) imbibition of fluids in shale matrix can create micro-fractures (Makhanov et
al., 2014; Roshan et al. 2015; Sun t al., 2015; Yang et al., 2015; Zhou et al., 2016; Meng et al.,
2015), which increases the local permeability of matrix. Accounting for these transport
mechanisms are expected to improve the accuracy of efficiency factors presented in this study,
although these mechanisms are rarely accounted by researchers (Sun et al., 2015; Yang et al.,
2016; Yan et al., 2017). Most reservoir simulators developed for tight fractured rocks like shale
tend to focus more on fracture networks (Yang et al., 2016; Yan et al., 2017). Several
mechanisms of fluid transport found to be important at small scales in shales as discussed above
are not included in the simulators because their importance has not been explored at field scale.

It should be emphasized that the simulated efficiency factor terms, 𝐸𝜙 and 𝐸𝑆 , do not
encompass such processes, as the probability that CO2 will never reach some of the pore space
and fractures due to transport heterogeneities associated with fracture networks and low matrix
permeability. The simulation in this work addresses this inefficiency of transport as a function of
time where eventually CO2 will reach all pore space and fractures if simulated long enough. In
addition, the simulated efficiency factors are based on the finite set of the input parameters
representing key properties of shale formations across North America. As a result, the simulated
efficiency values reported here are likely to “overestimate” CO2 storage in depleted shale
formations and should be considered as the upper bound.

V. Conclusion

Numerical simulations of CO2 injection into a depleted fractured shale reservoir were carried
out to estimate representative ranges of efficiency factor terms, 𝐸𝜙 , and 𝐸𝑆 , to account for the
effectiveness of CO2 storage as free and sorbed phases, respectively. Specifically, the ranges for
two efficiency factors, 𝐸𝜙 and 𝐸𝑆 , were estimated to have P10 to P90 probability ranges of 0.15 to
0.36 for 𝐸𝜙 and 0.11 to 0.24 for 𝐸𝑆 , reported after 60 years of CO2 injection. Key reservoir
parameters from shale formations across North America (Marcellus, Haynesville, Bossier,
Barnett, Fayetteville, Muskwa, Woodford, Eagle Ford, Utica, and Montney) and various
injection scenarios were used to sample volumes of CO2 that can be stored in gas-dominant shale
reservoirs at the national and regional scale. The estimated P10 and P90 ranges for the simulated
efficiency factors are intended to be used in the generalized equations for CO2 storage in shales
that provide a net effective volume of a reservoir accessible for CO2 flow to calculate
prospective CO2 storage in shale formations. These results can help further development of the
methodology to assess prospective CO2 storage in depleted shale gas reservoirs.
Acknowledgment

This technical effort was performed in support of the National Energy Technology Laboratory's
ongoing research under RES Contract DE-FE0004000. The simulations were carried out on
NETL's High-Performance Computer for Energy and the Environment (HPCEE).

Disclaimer

This project was funded by the Department of Energy, National Energy Technology Laboratory,
an agency of the United States Government, through a support contract with AECOM. Neither
the United States Government nor any agency thereof, nor any of their employees, nor AECOM,
nor any of their employees, makes any warranty, expressed or implied, or assumes any legal
liability or responsibility for the accuracy, completeness, or usefulness of any information,
apparatus, product, or process disclosed, or represents that its use would not infringe privately
owned rights. Reference herein to any specific commercial product, process, or service by trade
name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its
endorsement, recommendation, or favoring by the United States Government or any agency
thereof. The views and opinions of authors expressed herein do not necessarily state or reflect
those of the United States Government or any agency thereof.

Nomenclature

𝐸𝜙 Efficiency factor for CO2 storage as a free phase

𝐸𝑆 Efficiency factor for CO2 storage as an adsorbed phase

𝐸𝐴 Fraction of shale formation total area available for CO2 storage

𝐸ℎ Fraction of shale formation gross thickness available for CO 2 storage

At Total area of a shale formation

hg Gross thickness of the shale formation

Ve Net effective volume of the formation

CO2 Density of CO2 at the (averaged) pressure (𝑃̅ ) and (averaged) temperature (𝑇̅)

𝜌𝑠𝐶𝑂2 Maximum mass of CO2 sorbed per unit volume of solid rock

𝜙 Porosity

GCO2 CO2 storage resource

 P10 10th percentile

P90 90th percentile

𝑓𝑟𝑒𝑒
𝑉𝑖 Simulated CO2 volume stored in a reservoir volume contacted by the propagating CO 2
plume as a free gas

𝑉𝑖𝑠𝑜𝑟𝑏 Simulated CO2 volume stored in the same reservoir volume as a sorbed phase
𝑓𝑟𝑒𝑒
𝑉𝑚𝑎𝑥 Maximum CO2 volume that can be stored in a reservoir volume as a free gas at initial
(averaged) 𝑃̅ and 𝑇̅ conditions before gas production
𝑠𝑜𝑟𝑏
𝑉𝑚𝑎𝑥 Maximum CO2 volume that can be stored in the reservoir volume as a sorbed phase at
initial (averaged) 𝑃̅ and 𝑇̅ conditions before gas production

Q Flow rate

h Formation thickness

w Fracture aperture

µ Fluid viscosity

ρ Density of the fluid

A Cross-sectional are of the matrix block

R Universal gas constant

T Temperature

P Pressure

𝑇̅ Averaged temperature before hydrocarbon produciton

𝑃̅ Averaged pressure before hydrocarbon produciton

t Time

x Distance
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