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Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584

Contents lists available at ScienceDirect

Journal of Natural Gas Science and Engineering


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

Rate enhancement in unconventional gas reservoirs by wettability


alteration
Saurabh Naik, Zhenjiang You*, Pavel Bedrikovetsky
Australian School of Petroleum, The University of Adelaide, Adelaide, SA 5005, Australia

a r t i c l e i n f o a b s t r a c t

Article history: In unconventional water-wet gas reservoirs with extremely low permeability, water blockage due to the
Received 4 February 2015 capillary end effect near the fracture face and in the wellbore vicinity is a severe obstacle to gas pro-
Received in revised form duction. Wettability alteration of rock surface is discussed as an effective way to reduce water blockage
21 May 2015
and enhance gas production. It can also be applied to accelerating dewatering and preventing drilling
Accepted 9 June 2015
and fracturing uid leak-off. The current paper develops analytical models for steady-state two-phase
Available online 25 June 2015
linear and radial ows, accounting for the contact-angle-dependent capillary pressure and relative
permeability. The model has been validated by comparison with laboratory test. Applications of the
Keywords:
Wettability alteration
proposed model to porous media with constant and piecewise-constant contact angles are presented.
Production rate The modelling shows that the competition between the viscous and capillary effects on productivity
Unconventional gas reservoirs results in an optimal contact angle for the maximum well productivity indexes for water and gas. The
Capillary end effect productivity index increases with the capillary-viscous ratio and the altered zone length.
Two phase ow 2015 Elsevier B.V. All rights reserved.
Contact angle

1. Introduction retention is wettability alteration (Barenblatt et al., 1990). Wetta-


bility modication of rock surface towards less water-wet results in
Natural gas from the unconventional reservoirs is one of the key decrease of capillary pressure and mitigation of the water-blockage
energy resources that can meet the current world's energy and effect.
environmental objectives (Economides and Wood, 2009). However, Altering wettability to more water-wet increases the relative
the unconventional reservoirs have extremely low well produc- permeability for gas (Anderson, 1987), which is a positive factor for
tivity. Therefore, hydraulic fracturing is commonly used to stimu- gas production. However, it is accompanied by the increase of water
late wells in coal seam, shale and tight gas reservoirs (Wang et al., blocking effect which restricts gas ow from reservoir matrix to-
2012). For reservoirs with very low permeability, fracturing and wards well or fractures (Xie et al., 2009). These two competitive
drilling uid leak-off along with capillary end effect leads to an factors suggest the existence of the optimal contact angle (wetta-
increase of water saturation in the near wellbore or fracture-wall bility), corresponding to the maximum ow rate during gas pro-
regions (Xie et al., 2009; Bahrami et al., 2011; Odumabo et al., duction. Yet, the existence of the optimal contact angle for gas
2014). Fluid invasion into the reservoir is greatly affected by the production has not been reported in the literature.
contact angle (Li et al., 2014). Two competitive factors also suggest the existence of the con-
The increased water saturation in the fracture or wellbore tact angle that maximises water rate with gas-water production.
neighbourhood throttles gas ow from reservoir to the well. This Fast dewatering in coal seams or shale gas reservoirs is required at
water entrapment is referred to as water blockage. A few studies the beginning of the reservoir exploitation, in order to facilitate
have been conducted on water block clean-up (Mahadevan et al., rapid decrease of the reservoir pressure which intensies gas
2007, 2009) and the long-term effects on production (Bahrami desorption from the matrix. Numerous experimental studies on
et al., 2011). One of the most effective methods to reduce water wettability alteration have been performed. The contact angle of
rock surfaces can be altered articially through injection of sur-
factants (Adibhatla et al., 2006; Bryant et al., 2006; Kumar et al.,
* Corresponding author. 2008; Chen and Mohanty, 2014), high temperature steam
E-mail address: zyou@asp.adelaide.edu.au (Z. You).

http://dx.doi.org/10.1016/j.jngse.2015.06.016
1875-5100/ 2015 Elsevier B.V. All rights reserved.
1574 S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584

(Bruining and Van Duijn, 2006), brine with various salinities


s  swc
(Nasralla et al., 2013) and water with different pH (Morsy et al., Ss (1)
2014). Signicant change of contact angle in sandstones and car- 1  swc  sgr
bonates with variations of salinity and pH has been reported with
regards to low salinity waterooding (Fogden et al., 2011; Morrow where s is the water saturation, and swc and sgr are the connate
and Buckley, 2011). Presently, intensive research is ongoing for water and irreducible gas saturations, respectively.
wettability alteration using nanoparticles (Roustaei et al., 2012; The contact angle at rock surface q is measured between the
Arab and Pourafshary, 2013; Hendraningrat et al., 2013; Assef wateregas interface and the wateresolid interface. The rock is
et al., 2014). To some extent, surface contact angle can be water-wet (hydrophilic) if q < p/2 and is hydrophobic if q > p/2.
controlled by varying concentrations and compositions of injected Therefore, saturation of the wetting phase Sw can be expressed as:
agents. It inspires the investigation of contact angle as a continuous 8 p
parameter, controllable by surface treatment. Although wettability >
< Ss; q<
2
alteration has been extensively studied in sandstone and carbonate Sw S; q (2)
>
: 1  Ss; p
reservoirs, research on unconventional rocks such as coals and q>
2
shales is still very limited. There are a few studies on shale (Morsy
et al., 2014) and tight sandstone (Kathel and Mohanty, 2013) oil Unconventional reservoirs exhibit a variety of mineralogy and
reservoirs. However, comprehensive research on wettability alter- surface types such as organic matter (e.g. kerogen), aluminosilicate
ation in unconventional gas reservoirs is unavailable in the clays and silica sands; each mineral has its own wettability. This
literature. leads to the necessity of using fractional wettability to describe the
Rate enhancement by wettability alteration has been dis- rock surface.
cussed by Kathel and Mohanty (2013). Piecewise wettability In the present work, the LeveretteCassie equation (O'Carroll
alteration may lead to saturation shock on the boundary of et al., 2005) is applied to describe a porous medium which has
altered and unaltered zones similarly to those on the boundary of three fractions of surface area (f1, f2, f3) with different contact an-
rocks with piecewise permeability (Barenblatt et al., 1990; gles. The major fraction f1 has the contact angle which is considered
Bedrikovetsky, 1993; Van Duijn et al., 1995). The saturation alterable from 0 to p by some wettability altering agent. A small
shock may highly affect well productivity index. However, fraction f2 is considered permanent water wet with contact angle
steady-state solutions for two-phase linear ows have been 0 and another small fraction f3 is permanently hydrocarbon wet
presented for uniform rock wettability only (Barenblatt et al., with contact angle p. The overall capillary pressure of porous me-
1990; Chaouche et al., 1993; Van Lingen et al., 1996; Huang and dium with fractional wettability is:
Honarpour, 1998). Analytical models accounting for wettability
2s
variation along the core or near to fracture face and wellbore are Pc s; q s Js; q;
not available in the literature. k
In the current study, the effects of contact angle alteration on f
well productivity for both water and gas are investigated using
Js; q f1 cosqCSw s; q a f2 CSs a f3 C1  Ss a
1 1 1
the analytical model. The formulae for steady-state saturation
distribution in heterogeneous rocks with piecewise-constant (3)
contact angle and for well index are derived. It is found that
there does exist an optimal contact angle to maximise the water where s is the interfacial tension, k is the rock permeability, f is the
production rate; another value of the contact angle maximises porosity, f1, f2, f3 are the major fraction and two minor fractions of
the production rate for gas. Calculations using the analytical rock surface respectively, f1 f2 f3 1; C and a are empirical
model show that the wettability alterations cause increase in model parameters.
productivity index 2.0e4.7 times for gas and around 2.0 times for The relative permeabilities of water (krw) and gas (krg) are
water. expressed as functions of water saturation as (Chen et al., 2013):
The structure of the paper is as follows: Section 2 presents the
Z S
contact-angle-dependent models for capillary pressure and two-
w2 sds
phase relative permeabilities, which are then applied in Section 3 h 0
krw s Ss Z (4)
for derivation of analytical model for steady-state two-phase 1
ows in rocks with piecewise-constant contact angle. Laboratory w2 sds
0
data of two coreood tests obtained from literature are analysed for
the model validation in Section 4. Analysis of the results from
Z1
developed analytical model is then conducted in both linear and
radial ows (Section 5). Section 6 presents application of nano- w2 sds
technology to rock surface treatment for enhanced dewatering and krg s 1  Ssh ZS (5)
gas production from unconventional reservoirs. Discussions of the 1
w2 sds
model validity and conclusions on optimal contact angle nalise 0
the paper (Sections 7 and 8).
where h is the tortuosity index and w(S) pis the cleat height or
capillary radius, expressed as wS k=f=CS 1=a according to
2. Contact-angle-dependent model for capillary pressure and YoungeLaplace model (Barenblatt et al., 1990; Bedrikovetsky, 1993).
relative permeability In this model, the rock is assumed to be water-wet and water
occupies smaller cleats or pores. As water saturation increases, the
This section presents the models for water-saturation- and cleats or pores are lled by water in order of increase of their
contact-angle-dependent capillary pressure and relative perme- aperture (radius). Conversely, if the rock is hydrophobic, the water
ability. To introduce the capillary pressure model, let us dene the lling sequence occurs from the largest to the smallest cleats and
normalised water saturation S as: pores. While this model is applicable to uniformly-wet media, it
S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584 1575

cannot explain the behaviour of intermediately-wet natural rocks 3. Analytical model for steady-state two-phase ow
where the fractional or mixed wettability is more likely due to

surface roughness, mineral heterogeneity and different adsorbed In this section, analytical solution to the system of immiscible
compounds (Bradford et al., 1997). steady-state two-phase ow is derived, accounting for the effects of
In order to describe the relation between relative permeability contact angle on capillary pressure and relative permeability. The
and contact angle, we apply the model that accounts for wettability analytical model will be applied to the treatment of laboratory
heterogeneity of natural cores at the pore scale, which results in a coreood data (Section 4) and sensitivity study on gas-water pro-
difference in pore lling sequence for intermediate wettability ductivity (Section 5).
(McCaffery and Bennion (1974); see also Bradford et al. (1997) for
experimental validation of the model). An empirical weighting
function g(q) represents the portion of pores exhibiting hydro- 3.1. Analytical model
phobic surfaces:
Darcy's law applies to the ow of each phase (Barenblatt et al.,
gq 1  cosq=2 (6) 1990; Cinar and Riaz, 2014):
As it follows from Eqs (4) and (5), the contact-angle-dependent
kkrw s; q kkrg s; q
relative permeabilities for water and gas become: uw  VPw ; ug  VPg ; U uw ug
mw mg
Z S Z 1 (11)
1  gq w2 sds gq w2 sds
krw s; q Ssh 0
Z 1
1S
(7) where uw and ug stand for ow velocities of water and gas,
w2 sds respectively; U is the total velocity; krw and krg are relative per-
0 meabilities of water and gas, respectively; mw and mg are viscosities
of water and gas, respectively; Pw and Pg are phase pressures.
Z 1S Z1 Capillary pressure Pc is dened as the difference between the
gq w2 sds 1  gq w2 sds gas and water pressures:
0
krg s; q 1  Ssh Z 1
S
Pc Pg  Pw (12)
2
w sds
0 Substituting Darcy equation for water in (11) and capillary
(8) pressure equation (12) into Darcy equation for gas in (11), we
obtain:
Particularly, for gas ow in tight formation, especially in nano-
!
porous media, molecular scale interactions can have signicant krg s; q krg s; qmw
impact on gas ow (Shapiro and Wesselingh, 2008). Gas velocity is k VPc uw 1 U (13)
mg krw s; qmg
non-zero at the distance from the pore wall less than the mean free
path of gas (Wu and Pruess, 1998). At this scale, the collision fre- Fractional ow function f is calculated as the ratio of water
quency between gas molecules and the pore walls increases if mobility krw/mw to the total mobility l:
compared with gas molecularemolecular collisions, yielding
higher gas ux than that calculated from no-slip condition at the krw s; q=mw krw s; q krg s; q
pore wall. This effect is referred to as the Klinkenberg (gas slip) f s; q ; ls; q (14)
ls; q mw mg
effect. It is evaluated by multiplying the Klinkenberg term
1 b= Pg to the gas permeability (8) as: Substituting Eqs. (14) and (3) into (13) results in:

Z 1S Z1
0 1 gq w2 sds 1  gq w2 sds
0
b A
krg s; q @1 1  Ssh Z 1
S
(9)
Pg 2
w sds
0

where Pg is the average gas pressure along the distance, and b is the
Zs Zy
Klinkenberg factor. For tight gas reservoirs with permeability below f s; qkrg s; qJ 0 s; q
c ds xa dx (15)
1 md, formula for Klinkenberg factor is given by Jones and Owen f s; q  f 0
(1980) as: s0 y0

b 0:86k0:33 (10) p
where c is the capillary-viscous
p ratio, dened as c s kf=mg jUjL
in linear ow and c 2ps kf=mg jqj in radial ow. Water ux ratio
where k is the gas permeability at innite pressure.
f0 uw/U. For linear ow, distance y X, y0 0, a 0, and s0 is
Contact-angle-dependent models for capillary pressure and
water saturation at the core outlet or fracture face. For radial ow,
relative permeability presented in this section will be applied to the
y R, y0 Rw, a 1, and s0 is water saturation at wellbore. Eq. (15)
governing system of two-phase ow in the next section.
1576 S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584

denes the analytical solution for saturation prole in both linear


and radial ows.
The ow direction is inverse to increasing distance y, from y 1
to y0. At the ow exit point y y0, capillary pressure is Pc 0. As
capillary pressure is a monotonic function of saturation, the exit
point saturation s0 can be determined from Pc (s0, q) 0 for various
contact angles. The saturation also tends to a certain value s0 at the
distance far away from the exit, i.e., as y / , s/s0. Inlet point
saturation s0 can be determined from f 0 f (s0, q) for various
contact angles.
The productivity index (PI) for each phase is calculated as the
ow rate divided by the phase pressure drawdown:

PIi qi =DPi (16)


Fig. 2. Matching of the measured saturation proles by the analytical model.
in which i stands for either w (for water) or g (for gas). DP is the
pressure drop calculated from Darcy equation (11) by integration
over the distance from inlet to outlet: The region where y  b is considered the unaltered zone and the
contact angle is set as the initial contact angle; q q0 (Fig. 1). The
Z1 solution procedure for piecewise-constant wettability case is
ui m i xa
DPi dx (17) similar to that for uniform wettability. Water saturation at ow
k kri sx; q
y0 outlet s0 is obtained from Pc(s0) 0. Then the saturation prole is
calculated from y0 up to b for given c and f0. Capillary pressure and
3.2. Solution procedure pressures for both phases are continuous across the boundary y b.
The saturation on the outer side of the boundary s, is calculated
For uniform wettability with known contact angle, the solution from the value on the inner side of the boundary s as: Pc(s,
procedure is as follows. First, water saturation at ow outlet s0 q0) Pc(s, qa). Afterwards, the saturation prole is calculated in the
is determined from capillary pressure function Pc (s0, q) 0. unaltered zone from y b to the inlet y 1. Pressure drops of water
Second, saturation prole is calculated from (15) for given c and and gas are calculated from (17). Finally, productivity indexes for
f 0. Third, pressure drops of water and gas are calculated from both phases are obtained from (16).
(17). Finally, productivity indexes for both phases are obtained
from (16). 4. Treatment of laboratory coreood data
Let us consider piecewise-constant wettability in which the
contact angle alteration is applied up to a fraction of the full length. In this section, the laboratory coreooding carried out by Bazin
The region y0  y < b is considered the altered zone, where b is the et al. (2010) under two ow rates are analysed in order to validate
altered zone length. The contact angle in this zone is q qa (Fig. 1). the model proposed in Sections 2 and 3.

Fig. 1. Schematic of piecewise-constant wettability inow cases: (a) linear ow in coreooding; (b) linear ow towards fracture face; (c) radial ow towards wellbore.
S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584 1577

Cylindrical Mo^liere sandstone core from tight gas reservoir increase in fractional ow function with contact angle (viscous
with diameter of 3.8 cm and length of 7 cm is used. The initial core effect), which increases water production and decreases gas
permeability is extremely low (0.01 md) and is typical for un- production.

conventional reservoirs; the porosity is 0.144. The tortuosity for The dimensionless total mobility is dened as the product of
tight sandstone is taken as h 2.0 (Barenblatt et al., 1990). The total mobility and water viscosity: L lmw. Fig. 3c presents
laboratory procedure is as follows: rst, the core was fully satu- dimensionless total mobility versus water saturation s at different
rated with water under vacuum. Second, nitrogen was injected contact angles. At small contact angle q, increase of saturation leads
into the core until irreducible water saturation was reached. Third, to increase of relative permeability for water krw and decrease of
water was injected into the core with constant pressure until relative permeability for gas krg. The dominance of gas permeability
breakthrough. Fourth, nitrogen backow was performed with due to large wateregas viscous ratio causes reduction of dimen-
constant pressure drawdown 10 bars in Test 1 and 15 bars in Test sionless total mobility L with saturation.
2, respectively. The measured saturation proles are shown in At large contact angle q, krw is high and krg is low at large water
Fig. 2. Measured irreducible saturation for water was swc 0.22 saturation. The effect of krw increase dominates over that of krg
and for gas was sgr 0.2. decrease, which yields increase of L at large water saturation.
The mathematical model presented in Sections 2 and 3 is Fig. 4 presents the saturation proles s(X) for different contact
applied to the calculation of saturation prole under the laboratory angles with small (Fig. 4a) and large (Fig. 4b) capillary-viscous ra-
conditions. s0 values are approximated from the saturation proles tios in linear ow. The curves start at X 0 from saturation value S0.
of each test; 0.320 and 0.295 for test 1 and test 2, respectively. The For X / , the proles tend to s0. The curves are monotonic. The
values of tuned parameters as obtained by least-square method conditions at X 0 and X / , as determined by the rock wetta-
(Chalk et al., 2012; You et al., 2013) are: capillary pressure model bility and by the rates of both phases, are independent. At a certain
parameters C 104, a 0.4 and contact angle q 57.3 . The ob- contact angle, s0 > s0 yields decreasing saturation proles (blue,
tained saturation proles for the two tests (blue and red curves (in green and red curves) and s0 < s0 yields increasing saturation
the web version) in Fig. 2) are in good agreement with measured proles (grey and cyan curves). The slope of s(X) increases with q,
proles (green and cyan points in Fig. 2). from low negative value at q 0 (blue curves) to high positive value
at q p (cyan curves). The capillary-viscous ratio c determines the
5. Analysis of the results signicance of capillary end effect. The magnitude of slope of s(X)
curve decreases with c (Fig. 4). The same behaviour occurs in radial
In this section, the analytical model developed in Section 3 is ow.
applied to investigating the effect of contact angle on the produc- The productivity index (Eq. (16)) can be used to evaluate the
tivity behaviour of both phases in linear and radial ows. The linear total effect of contact angle on productivity for each phase. The full
case applies to ow towards a fracture or coreood in the labora- range of contact angle from 0 to p is examined (Fig. 5). PI values for
tory; while the radial case applies to ow towards wellbore in the gas and water at contact angle of p/2 are used as scales to obtain
eld. Sensitivities of productivity for gas and water to the capillary- dimensionless PIs. The saturation prole is constant for all c values
viscous ratio and altered zone length are analysed. at this contact angle, which corresponds to the condition s0 s0
The values of rock and uid properties used in this study to (intersection between blue and green curves in Fig. 3b). Therefore,
portray unconventional reservoirs with low permeability are listed relative permeabilities (7, 8) are independent of c. PIs for both gas
in Table 1. The well radius is: rw 0.15 m. and water at q p/2 are independent of c (Fig. 5).
The contact angle affects boundary saturation and relative For large values of c, the effect of saturation decrease with
permeability curves. Sensitivity of the contact angle to fractional contact angle (capillary effect) dominates over the effect of frac-
ow function and boundary saturations s0 and s0 is analysed. tional ow increase (viscous effect) on PI. Increase of contact angle
Fractional ow function f(s) calculated from (14) is presented in leads to the increase of PI for gas (blue and green (in the web
Fig. 3a. The fractional ow decreases with contact angle for any version) curves in Fig. 5a) and decrease of PI for water (blue and
given saturation in the range swc < s < 1  sgr. green curves in Fig. 5b). As c decreases, the capillary and viscous
Fig. 3b shows the contact angle dependences of s0 calculated effects become comparable. The two competitive effects lead to an
from Pc(s0,q) 0 and s0 calculated from f(s0,q) f0. Both saturations optimal PI at an intermediate contact angle (red and cyan curves in
s0 and s0 decrease with contact angle; s0 and s0 are equal at an Fig. 5a and b). The optimal contact angle increases with c for gas
intermediate contact angle (Fig. 3b), which results in a constant and decreases with c for water. Larger value of c yields higher
saturation prole at this contact angle. increase in PI for both gas and water (Fig. 5).
Alteration of contact angle introduces two competitive effects Let us investigate the effect of altering the contact angle of a
on the productivity for water and gas. One effect is the reduction of fraction of the production zone on the PI-contact angle prole. We
saturation prole with contact angle (capillary effect), which de- consider an example where the rock surface is partially treated by a
creases water production and increases gas production; the other is wettability alteration agent from the ow exit y0 up to a certain
distance y1. The zone from y1 to the inlet y2 remains unaltered.
Without losing generality, the rock surface is assumed water wet
before treatment and the initial contact angle is zero. After the
Table 1
Values of rock and uid properties. treatment, the contact angle of the altered zone qa is shifted to a
chosen value ranging from 0 to p.
Parameter Value
Fig. 6 shows the saturation prole at different altered contact
k (md) 1 angles qa for low (Fig. 6a) and high (Fig. 6b) capillary-viscous ratios.
f 0.05
Saturation decreases with contact angle in the wettability alter-
h 0.75
s (N/m) 0.08 ation zone (0 < X < b). Capillary pressure continuity is satised
C 0.5 across the boundary between wettability altered and unaltered
a 0.9 zones (X b), which yields discontinuous saturation at this
mg(Pa s) 1.5  105 boundary (Fig. 6). Increase of contact angle in the zone near to core
mw (Pa s) 1  103
outlet or fracture face (0 < X < b) of water-wet rocks results in
1578 S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584

Fig. 3. Effects of contact angle on steady-state two-phase ow: (a) fractional ow curve for water at different contact angles; (b) boundary saturations versus contact angle at
different fractional ow for water f0; (c) dimensionless total mobility versus saturation at different contact angles.

decrease of saturation near the exit, but the capillary end effect still optimal contact angle for the maximum gas productivity (Fig. 7a).
occurs in the unaltered zone (X > b). The optimal contact angle is around p/2.
Restriction of gas ow due to capillary end effect occurs at the However, the water ow is only restricted at high contact an-
exit (X 0) for low qa and at the boundary between wettability gles. As capillary-viscous ratio increases, the end effect increases. It
altered and unaltered zones (X b) for high qa (Fig. 6). Despite the reduces the water productivity at high contact angles (Fig. 7b).
intention of reducing the end effect by wettability alteration in the Water production from water-wet reservoirs can be maximised by
zone near to wellbore or fracture face, end effect at the altered zone altering the contact angle in wettability alteration zone (0 < X < b)
boundary can still occur. Higher capillary-viscous ratio results in towards the optimal value qa < p/2, and can be minimised by
larger end effect. It reduces the productivity for gas at both high and altering the contact angle towards qa p (Fig. 7b).
low contact angles (Fig. 7a). Contact angle alteration affects satu- The sensitivity of productivity index to the altered zone length b
ration in the altered zone signicantly (Fig. 6). In this zone the is investigated. PI for gas versus contact angle in the case of
competing capillary and viscous effects yield an intermediate piecewise-constant contact angle in linear ow is shown in Fig. 8a.

Fig. 4. Saturation proles for different contact angles in linear ow (f0 0.01): (a) c 0.1; (b) c 10.
S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584 1579

Fig. 5. Productivity index versus contact angle at different capillary-viscous ratios c in linear ow (f0 0.01): (a) gas; (b) water.

Fig. 6. Saturation prole at different altered contact angle qa in linear ow with piecewise alteration of contact angle (f0 0.01, b 0.5): (a) c 0.1; (b) c 10.

Fig. 7. Productivity index versus piecewise alteration of contact angle in water-wet rock at different c in linear ow (f0 0.01, b 0.5): (a) gas; (b) water.

The maximum value of PI for gas increases with b, since the vari- Increase of contact angle in the zone near to wellbore (0 < R < b) of
ation of saturation and relative permeability in altered zone occurs water-wet rocks results in decrease of saturation near the exit, but
over a larger distance with b. The increase of b from 0.005 to 0.5 the capillary end effect still occurs in the unaltered zone (R > b)
results in the increase of productivity index for gas from 0.1% to 7% (Fig. 9). The pressure drop across the altered zone near the wellbore
at qa p/2 (green curve in Fig. 8b). is much higher compared to that in linear case, causing the altered
Saturation proles in radial ow towards well at different qa for zone properties to be more inuential over the total ow in radial
low (Fig. 9a) and high (Fig. 9b) c are presented in the case of than in linear case. Therefore, PI prole is more sensitive to b in
piecewise alteration of contact angle. Saturation decreases with radial case than that in linear case (Fig. 10a). Higher b leads to
contact angle qa in the wettability alteration zone (0 < R < b). higher productivity index; the increase of b from 5  104 to 0.05
1580 S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584

Fig. 8. Productivity index for gas in the case of piecewise-contact angle in linear ow (f0 0.01, c 0.1): (a) PIg versus qa; (b) PIg versus b.

Fig. 9. Saturation proles at different altered contact angle qa in radial ow with piecewise alteration of contact angle (f0 0.01, b 5.0  104): (a) c 0.01; (b) c 0.5.

Fig. 10. Productivity index for gas in the case of piecewise contact angle in radial ow (f0 0.01, c 0.01): (a) PIg versus qa; (b) PIg versus b.

results in the increase of productivity index for gas from 1% to 9% at and Torsaeter, 2014). The adsorption of nanoparticles onto rock
qa p/2 (green curve in Fig. 10b). surface is dependent on DLVO forces exerting on NPs (Li and
Torsaeter, 2015), which indicates that different types of NPs and
6. Nanoparticle injection for wettability alteration in surface materials exhibit different interactions. The wettability
unconventional rocks alteration of rock surface is affected by the types of NPs and the
underlying mineralogy, leading to different resultant contact angles
Presently, nanoparticles (NPs) are extensively applied to based on their combinations.
wettability alteration of reservoir rocks for waterooding (Maghzi The main minerals present in unconventional coal seam and
et al., 2012; Giraldo et al., 2013; Ju and Fan, 2013; Hendraningrat shale reservoirs are sand, clays and organic matter. Karimi et al.
S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584 1581

(2012) applied zirconium dioxide (ZrO2) NPs to decrease carbonate 7. Discussions


contact angle from 90 to 0 . Li and Torsaeter (2015) used
hydrophilic silica NPs to decrease contact angle of sandstone rock The analytical model for steady-state ow is based on equality of
surface from 54 to 22 . Hendraningrat and Torsaeter (2014) the pressure and capillary-pressure gradients. The exact solution
investigated three metal oxides NPs: aluminium (Al2O3), titanium for steady-state ow with piecewise-constant contact angle is
(TiO2) and silicon (SiO2). Nano uids used in the experiment expressed by implicit analytical formulae, allowing for explicit ex-
with the concentration 0.05 wt% result in the contact angles pressions for the well productivity index.
measured in brine (NaCl 3 wt%) lowered from 53.68 to 28.6 , The saturation prole for steady-state ow in the rock with
21.64 and 38.82 for Al2O3, TiO2 and SiO2, respectively. To in- constant contact angle starts at the boundary value s0, which cor-
crease the contact angle, lipophilic polysilicon NPs with surface responds to zero capillary pressure, and tends to constant s0 as X
modication can be used (Ju and Fan, 2009). Hydrophobic and tends to innity, where the constant saturation is determined by
neutral wet polysilicon nano uids with concentration 4 g/L suc- fractional ow. Size of the end effect zone, where the signicant
cessfully altered sandstone contact angle from 50 to 84.56 and fraction of variation s0  s0 occurs, is equal to cL. Therefore, at low
98.12 , respectively (Roustaei et al., 2012). Cupric oxide (CuO) NPs capillary-viscous ratio, the saturation prole is almost uniform,
increased water contact angles from less than 5 up to 130 and while the saturation varies along the distance at high capillary-
150 with amine- and thiol-modied surfaces, respectively (Basu viscous ratio. In the rocks with piecewise-constant contact angle,
et al., 2011). the above proles are valid in constant-contact-angle intervals; the
Lebedeva and Fogden (2011) investigated the wettability alter- proles in different intervals are matched by the continuity con-
ation of kaolinite clay surface, due to the deposition of asphaltene dition for capillary pressure yielding the saturation jumps.
nanoparticles. The clay surface was altered from hydrophilic to A plane-parallel-ow analytical model is applied to the treat-
hydrophobic with contact angle 140 . ment of coreood data, and also to ow and saturation prediction
To the best of our knowledge, application of NPs to the wetta- near to the fractured well. The axi-symmetric model is applied for
bility alteration of organic matter has not been reported in the vertical and horizontal wells.
contemporary literature. Let us discuss the limitations of the analytical model (15). It
Let us estimate the effects of contact angle alteration by assumes gas is incompressible. Since the gas density is a function of
applying different NPs using the analytical model (Section 3) for pressure, the incompressibility assumption is valid if the pressure
the above-mentioned cases. Productivity index values versus drawdown is much less than the reservoir pressure:
contact angle are shown in Figs. 5 and 7 for f0 0.01. For low
water fractional ow f0 0.01 and the contact angle altered from DP
1 (18)
50 to 90 (Roustaei et al., 2012), c 5 and 0.05 result in PIg P
increase by 2.0 and 1.08 times, respectively. For high water frac-
For linear ow during coreooding, substitution of Darcy's law
tional ow f0 0.95 and the contact angle altered from 0 to 130
U k=mDP=L into the condition (18) yields:
(Basu et al., 2011), gas productivity index PIg can be increased by
4.7 and 1.25 times for high (c 5) and low (c 0.05) capillary- DP UmL
viscous ratios, respectively. Given f0 0.01 with contact angle 1 (19)
P kP
alteration from 0 to 50 (Vafaei et al., 2006), water productivity
index PIw is increased by 2.1 and 1.96 times for c 5 and 0.05, or
respectively.
Different types of NPs affect wettability of shale- or coal- kp
U (20)
minerals differently; hence, a mixture (cocktail) of NPs must be mL
developed for multi-mineral rocks. The corresponding technol-
For core length L 0.1 m, permeability k varying from 0.01 to 10
ogy includes adding nanoparticles that increase the resulting
md, gas viscosity m varying from 105 to 4  105 Pa s, and pressure
contact angle, into a drilling or fracturing uid. The contact angle
P varying from 5  105 to 107 Pa, the maximum velocity where the
increase yields the pore-scale deviation of water into larger
incompressibility assumption is valid varies from 1.2  105 to 1 m/
pores, increasing water rate during dewatering, and decreasing
s. The typical ow velocities in cores have the order of magnitude
water saturation to facilitate the gas ow in the future. Injection
106e105 m/s (Barenblatt et al., 1990; Bazin et al., 2010). There-
of nanoparticles, making the rock more water-wet, after the
fore, gas compressibility is negligible under the conditions of these
dewatering, leads to water displacement into smaller pores with
laboratory studies by Bazin et al. (2010), so the incompressibility
the consequent gas rate increase. The fast pore pressure decrease
assumption is valid.
in both scenarios results in more intensive gas desorption. To
For fractured wells, velocity at the fracture face is calculated using
summarise, the well treatment described above includes adding
Eq. (20). For permeability variation k 0.01e10 md, m 105e4 
NPs into drilling or fracturing uids with the consequent in-
105 Pa s, reservoir pressure P 5  106e108 Pa, and length of linear
crease of the contact angle (rst stage); at the second stage,
ow region towards the fracture L 10e250 m, the maximum ve-
hydrophilic NPs are injected into the reservoir in order to
locity where the incompressibility assumption is valid varies from
decrease the contact angle after dewatering during gas produc-
5  108 to 0.1 m/s. Typical velocities at fracture faces in gas reser-
tion. Therefore, two different cocktails must be developed for
voirs have the order of 105e104 m/s (see Shaoul et al., 2012).
two stages. The delivery of nanoparticles is performed by the
Therefore, there are some unconventional eld cases where the
injection together with fast deteriorating gas-based foam
incompressibility assumption is valid, and where it is not. Inequality
(Farajzadeh et al., 2011).
(20) denes the conditions where the analytical model (15) is valid.
The analytical model for steady-state gas-water ow in rocks
For radial ow towards well, the rate of incompressible uid per
with piecewise-constant contact angle can be used for design of
unit height of reservoir (Q) is calculated as:
the treatment technology, including dening volumes of injected
uids and their compositions. The analytical model can also be
2pkDP
applied to the upscaling of laboratory data for well index Q (21)
prediction. mlnre =rw
1582 S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584

Substitution of rate expression in vertical well into the condition For rocks with permeability 1 md (corresponding dp 0.1 mm),
(18) yields: the calculated Kn 0.1 for gas pressure P 6.8  105 Pa. For rocks
with low permeability 0.01 md (dp 0.01 mm), the calculated Kn 0.1
2pkp for P 6.8  106 Pa. From this we conclude that the model neglecting
Q (22)
mlnre =rw Knudsen diffusion is applicable only for reservoirs at high reservoir
pressures (P > 6.8  105 Pa for 1 md, P > 6.8  106 Pa for 0.01 md).
For k 0.01e10 md, m 105e4  105 Pa s, P 107e108 Pa, The YoungeLaplace model for capillary pressure is valid if the
ratio between drainage and well radii re/rw 103e104, the disjoining pressure is negligible and surface tension is constant. It is
maximum rate per unit height, where the incompressibility inappropriate for pore/channel sizes in the range of nanometres. In
assumption is valid varies from 1.7  105 to 0.9 m2/s. Some typical this scale, applying the augmented YoungeLaplace equation, the
rates for tight gas reservoirs vary in the range 103e0.1 m2/s (see capillary pressure can be calculated as the sum of the traditional
McGowen et al., 2007). Thus, the gas compressibility can be ignored YoungeLaplace term and the disjoining pressure in the thin water
in some cases, and cannot be ignored in other cases. lm which can wet the surface. The disjoining pressure effects have
For the linear ow case in this paper, k 1 md, m 2  105 Pa s been used to describe the wetting lm behaviour of a meniscus in
and length of linear ow region is 103 m. For pressure varying from regions around 0.1 mm (Kelly, 2013). If pore sizes are above this size,
5  106 to 108 Pa, the maximum velocity where the incompressibility the YoungeLaplace equation can be used to calculate capillary
assumption is valid varies from 2.5  106 to 5  105 m/s. The ve- pressure. For the synthetic case study in Section 4, the average pore
locities in the synthetic case (Section 5) are in the order of 107 m/s, radius estimated from KozenyeCarman model is 0.3 mm. Therefore,
therefore the incompressibility assumption is valid. For the radial the capillary pressure calculated from YoungeLaplace model is valid.
ow regime, we use the same permeability, viscosity and pressure Good agreement between two saturation proles as obtained
range. For re/rw 6.67  103, the maximum rate per unit height from coreoods with different rates, and the prediction by the
where the incompressibility assumption is valid varies from 2  103 analytical model (15) with three tuning parameters C, a and q has
to 3.5  102 m2/s. The rates in the synthetic case have the order of been observed (Fig. 2). The two measured saturation proles can be
104 m2/s, therefore the incompressibility assumption is valid. approximated by exponential functions with three degrees of
In the case that the gas compressibility cannot be neglected, freedom each: s(X) A BeCX, giving the two curves six degrees of
such as for high rates or high pressure drawdowns, equation of freedom totally. Good match by tuning only three parameters val-
state for gas rg(Pg) is included in gas rate equation (10). The nal idates the analytical model.
expression for steady-state solution is a system of two ordinary A simplied model for relative permeability and capillary
differential equations with respect to pressure and saturation. pressure (Section 2) has been applied in this paper. The model
The gas slip effect can be signicant in porous media with low corresponds to pore-space geometry as a bundle of parallel capil-
pressure or low permeability (Wu and Pruess, 1998; Civan et al., lary with different wettability. In reality, natural rocks consist of
2011). According to gas permeability Equation (9), the slip effect numerous minerals with different wettability and grid-like pore-
is negligible if gas pressure is much larger than the Klinkenberg space geometry. One way around is the percolation-effective media
factor b. For typical permeability k 0.001 and 1 md, the value of model for the rocks with spotted micro heterogeneity in both
b is 3.3  105 and 2.8  105 Pa, respectively. A typical reservoir capillary pressure and relative permeability (Barenblatt et al., 1990;
pressures in coal seams are 106e107 Pa (Gaurav et al., 2012). The Bedrikovetsky, 1993).
corresponding error in calculated relative permeability for gas The obtained steady-state solutions provide the long-term as-
using (9) is 2e6%, if gas slip effect is ignored. In shallow gas res- ymptotics for non-steady state problems of immiscible Newtonian
ervoirs, pressure can be even lower, which leads to higher effect of and Now-Newtonian displacements, which is important informa-
gas slip. For shallow reservoirs or reservoirs with ultra-low tion for the transient analysis (Bedrikovetsky, 1993; Morrow and
permeability, the gas slip effect can cause rate miscalculation Buckley, 2011; Fogden et al., 2011). Since the long-term asymp-
around 10% if it is ignored. It can be especially prevalent in core- totic states are in thermodymanic equilibrium, the solutions are
ooding tests, where low pressures are commonly used. applicable for partly-miscible ows also (Farajzadeh et al., 2011;
Knudsen diffusion occurs where the gas with low enough Cinar and Riaz, 2014).
density ows in small enough capillaries, such that the gas particles Two scenarios are investigated for wateregas ow with well
collide more frequently with the solid walls than with other par- treatment by NPs. One scenario involves increasing contact angle
ticles (Bhatia et al., 2011). Knudsen diffusion can be evaluated by under high water saturation which corresponds to the processes of
the Knudsen number Kn, dened as the ratio between the mean dewatering and the fracturing-uid ow-back. The other scenario
free path of gas molecule and the pore size: involves decreasing contact angle under low water saturation,
which occurs during gas production.
l k T
Kn ; l p B (23) Based on the analytical model developed, the strategy of gas
dp 2Ppd2g productivity enhancement is as follows: For rocks with uniform
wettability, alter contact angle of rock surface towards p/2 for low
where l is mean free path of gas, dp is pore diameter, kB is Boltz- capillary-viscous ratio and p for high capillary-viscous ratio. For
mann constant (1.38  1023 J/K), T is gas temperature, dg is piecewise wettability alteration of water-wet rocks, optimal contact
diameter of gas molecule. Knudsen diffusion is negligible if Kn 0.1 angle is p/2 for both low and high capillary-viscous ratios. The
(He et al., 2014). We consider methane molecule diameter strategy targeting maximum water productivity is contact angle
4.14  1010 m and typical reservoir temperature 373 K. Pore sizes alteration towards p/2 for low capillary-viscous ratio and zero for
in coal seam reservoirs can range from a few angstroms to over a high capillary-viscous ratio.
micron. For pressure varying from 5  106 to 108 Pa, Kn in coal
seams can vary from 7  105 to 3. Pore sizes in shales range from 8. Conclusions
0.005 to 0.1 mm (Nelson, 2009). For pressure varying from 5  106 to
108 Pa, Kn in shale reservoirs can vary from 7  104 to 0.3. Analytical modelling and its application to enhancing the well
Therefore, Knudsen diffusion effect can be signicant in tight for- productivity for gas and water by wettability alteration allow
mation; however, it is not always the case. drawing the following conclusions:
S. Naik et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1573e1584 1583

Competition between the viscous and capillary effects on gas Greek letters
productivity results in non-monotonic contact-angle-de- a capillary model parameter
pendency of gas productivity index, suggesting the existence of b Altered zone length
optimal contact angle for enhanced gas production. c capillary-viscous ratio
For dewatering and fracturing uid ow-back, competition be- h tortuosity index
tween the viscous and capillary effects on water productivity q surface contact angle
yields the optimal contact angle which maximises the produc- L dimensionless total mobility
tivity index for water. l mean free path of gas, m; total mobility, 1/Pa s
In the case of wettability alteration over the full length, the m viscosity, Pa s
higher the capillary-viscous ratio c, the higher the capillary end r density, kg/m3
effect, the larger the end effect zone and the higher the s interfacial tension, N/m
maximum productivity indexes for gas and water. f porosity
In the case of wettability alteration on a fraction of water-wet
rock, increase of the capillary-viscous ratio c leads to the in- Abbreviations
crease of the maximum productivity index for water and DLVO DerjaguineLandaueVerweyeOverbeek
decrease for gas. This is because the capillary end effect at the NP nanoparticle
boundary between wettability altered and unaltered zones re- PI productivity index
duces gas ow more severely with higher c.
The larger the altered zone length b, the higher the contact angle Subscripts
effect on gas and water productivity index. This is due to alter- a altered
ation of saturation prole and relative permeability over a larger e drainage radius
distance. g gas
Productivity index is sensitive to small value of b in radial ow w water (for productivity index and relative permeability),
towards well, indicating that wettability alteration in small wetting (for saturation), well (radius)
neighbourhood of wellbore can effectively improve productivity 0 exit
indexes for gas and water.
Wettability alteration in the range achieved by nanoparticles,
Superscripts
leads to 2.0e4.7 times increase of well productivity for gas and
0 inlet
twice increase for water.
The maximum productivity index for water should be applied
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