PETROPHYSICS, VOL. 49, NO. 1 (FEBRUARY 2008); P.

2835; 6 FIGURES, 1 TABLE

Low Salinity Oil Recovery - An Experimental Investigation1

A. Lager2, K. J. Webb3, C. J. J. Black2, M. Singleton4, and K. S. Sorbie4

ABSTRACT

The idea of injecting low salinity water into a petroleum reservoir is not novel and was often used in the 70s
prior to the injection of surfactant. Recently it was
shown that simply injecting sufficiently low salinity
water improves oil recovery. Many possible mechanisms concerning low-salinity waterflood have been
proposed in the literature. This paper describes an
experimental investigation into some of the factors controlling the increased oil recovery observed when low
salinity brine is injected into oil saturated reservoir core
samples. Extensive chemical analyses were performed
on the effluent showing the extent of interaction
between the injected brine, the oil and the rock matrix.
Keywords: Low-salin ity waterflood, cat ion
exchange, clay mineralogy

INTRODUCTION

It has been 10 years since Yildiz and Morrow (1996)

pushed forward the research started by Jadhunandan
(Jadhunandan, 1990; Jadhunandan and Morrow, 1991;
Jadhunandan and Morrow, 1995) and published their paper
on the influence of brine composition on oil recovery,
which showed that changes in injection brine composition
can improve recovery. Tang and Morrow (1999) advanced
the research on the impact of brine salinity on oil recovery,

followed by other researchers such as Webb et al. (2004;

2005) and McGuire et al. (2005), which carried out an
extensive research program on low salinity injection. This
program included numerous core floods at ambient and reservoir conditions (e.g. temperature and pressure with live
fluid) both in secondary and tertiary mode, single well
tracer tests and log inject log, which resulted in a series of
publications (McGuire et al., 2005; Webb et al., 2004;
Webb et al., 2005) and the registration of the LoSal EOR
process trademark.
Numerous hypotheses have been devised to explain the
increase in oil production associated with low salinity water
injec tion, including increas ing pH leading to in-situ
saponification and interfacial tension reduction, emulsion
for ma tion, clay migra tion, and wettability alteration
(McGuire et al., 2005; Tang and Morrow, 1999; Yildiz and
Morrow, 1996). In this paper the fines migration and pH
increase mechanism are reviewed and discussed in the light
of new data obtained during ambient and reservoir condition low salinity floods. Also a new mechanism based on
the extended DLVO theory and cation exchange is discussed.
EXPERIMENTS

All corefloods discussed in this paper were performed on

nominally 3" long by 1.5" diameter plug samples from
sandstone oil reservoirs. Plug samples were loaded into
hydrostatic coreholders and miscibly solvent cleaned with
cycles of toluene and methanol, prior to saturation with

Revised Manuscript received by the Editor, November 16, 2007.

Paper originally presented at the International Symposium o the Society of Core Analysts, Trondheim Norway, September 12-16, 2006,
Paper SCA2006-36.
2
BP Exploration (Alaska), 900 Benson Blvd, Anchorage, AK 99519, USA; E-mail: [email protected].
3
BP Exploration Production Technology Group/Pushing Reservoir Limits, Sunbury, UK; E-mail: [email protected],
[email protected].
4
FAST-rac, Institute of Petroleum Engineering, Heriot-Watt University, Research Park, Riccarton, Edinburgh EH14 4AS, UK; E-mail:
[email protected], [email protected].
2008 Society of Petrophysicists and Well Log Analysts. All rights reserved.
1

28

PETROPHYSICS

February 2008

Low Salinity Oil Recovery - An Experimental Investigation

simulated formation brine. Initial water saturation was

acquired by constant pressure oil flood. Initial water saturation values were found to be matched to those corresponding to the height of the sample above the oil water contact.
From analyses of sister samples using in-situ saturation
data, the distribution of water was uniform across the length
of the core samples. In all cases simulated formation water
was used for the initial water.
Samples were then loaded into hydrostatic coreholders,
prior to taking the samples to the conditions of the test.
Refined laboratory oils were displaced with the crude oil,
via a slug of toluene to provide a buffer between the lab oil
and the crude oil. The sample was then shut in for a period
of time (ageing).
Waterfloods were then performed on the samples by
injecting brine at constant flow rate at elevated temperature
and with nominal back pressure on the plug samples, to
ensure no gas production from the oil. For tertiary low
salinity waterfloods, high salinity connate brine was first
injected. Differential pressure and oil production were continuously monitored, and brine was injected until no further
oil production or change in pressure was recorded, at which
time low salinity water injection commenced from the low
oil saturation achieved after high salinity brine injection.
Once again differential pressure and oil production were
monitored. Secondary low salinity waterfloods were performed in an identical manner, but low salinity brine was
injected into the sample at initial water saturation. During
the course of the low salinity injection pH was monitored in
the effluent by taking aliquots of produced brine. In some
cases, which are described later, aliquots of the effluent
were also taken for ion analyses using inductively coupled
plasma mass spectroscopy (ICP-MS).
Mechanistic studies were performed at reduced conditions of pressure and elevated temperature.
RESULTS & DISCUSSION
Fines migration

An attempt to explain the low salinity production mechanism was put forward by Tang and Morrow (1999). They
noticed fines (mainly kaolinite) being eluted dur ing
low-salinity waterfloods on Berea core samples. They concluded that fines mobilization resulted in exposure of
underlying surfaces, which increased the water-wetness of
the sys tem. Ear lier work had shown that opti mum
waterflood displacement efficiency occurs under weakly
water wet conditions (Tang and Morrow, 1999; Yildiz and
Morrow, 1996). In the presence of high salinity brine, clays
are undisturbed and retain their oil wet nature leading to
poorer displacement efficiency. When contacted with
February 2008

low-salinity water, clay particles detach from the pore surface. Lever and Dawe (1984) showed that the released fines
migrate with flowing fluid and are subsequently captured at
pore throats or pore constrictions, causing formation damage. Tang and Morrow (1999) supposed that the detachment of mixed-wet clay particles from pores mobilized previously retained oil droplets attached to these clays, allowing an increase in oil recovery. They also reported a reduction in permeability when the injection brine salinity was
less than 1550 ppm TDS. This reduction in permeability
was observed when the low-salinity brine replaced the initially permeating high-salinity brine. Valdya and Fogler
(1992) showed that the release process is primed by a combination of extremely low-salinity and high pH. They
reported little change in permeability when fluids with
increasing pH were injected until an injection pH of 9 was
reached. At a pH > 11 a rapid and drastic decrease in the
permeability was observed implying that severe damage
was caused on contact with the high-salinity fluid and the
absence of salts in the solution.
The mechanism of fines migration was explained by the
Deryaguin-Landau-Verwey-Overbeek (DLVO) theory of
colloids (Deryaguin and Lan dau, 1941; Verwey and
Overbeek, 1948). The permeability reduction occurs if the
ionic strength of the injected brine is equal to or less than,
the critical flocculation concentration (CFC), which is
strongly dependent on the relative concentration of divalent
cations such as Ca2+ and Mg2+ (Khilar et al., 1990; Kia,
1987). Divalent cations have been known to stabilize the
clay by lowering the zeta potential resulting in the lowering
of the repulsive force. Also Bazin and Labrid (1991) indicated that water sensitivity is related to the cation exchange
capacity (CEC) of clay sandstones. They concluded that
high CEC sandstone will lead to a high potential for permeability reduction.
As Tang and Morrow (1999) showed, it is possible to
have fines migration during low salinity injection. However, during numerous low-salinity, reduced condition and
full reservoir condition core floods in our laboratory, in
which all have shown increased oil recovery, no fines
migration or significant permeability reductions were
observed. These results question the link between fines
migration and oil recovery.
pH Variation

Some studies have shown a rise in pH during low salinity

production laboratory experiments (Figure 1). This rise in
pH is due to two concomitant reactions: carbonate dissolution and cation exchange. The dissolution of carbonate (i.e.
calcite and/or dolomite) results in an excess of OH- and cation exchange occurs between clay minerals and the invad-

PETROPHYSICS

29

Arnaud et al.

ing water. The dissolution reactions are relatively slow and

dependent on the amount of carbonate material present in
the rock

However, cation exchange occurring on the clay minerals, and to a much lesser extent quartz, is faster (Appelo and
Postma, 2005). The mineral surface will exchange H+ present in the liquid phase with cations previously adsorbed.
This will lead to a decrease in H+ concentration inside the
liquid phase resulting in a pH increase.
If a pH above 9 was achieved inside a petroleum reservoir this would be equivalent to an alkaline waterflood.
According to Jensen and Radke (1988), the mechanisms
active at the front where alkaline water is displacing acidic
crude oil include: (1) a reduction of oil/water interfacial
tension, (2) wetting alteration of the matrix grains, (3) formation of water drops inside the oil phase, and (4) drainage
of oil from the volume between alkaline water drops to produce an emulsion containing very little oil.
The initial results from Tang and Morrow (1999) on
Berea sandstone and early experiments performed at our
laboratory on a North Sea reservoir system clearly exhibit a
rise in pH (Figure 1). The explanation given at the time for
this increase was that carbonate dissolution was sufficient
to generate this order of pH. The evidence showing a pH
increase during low salinity floods suggested that low salinity waterflood worked like an alka line waterflood
(McGuire et al., 2005).
However, conflicting evidence throws doubt on this
mechanism being the cause of the low salinity production
effect. The best low salinity coreflood results obtained to
date come from a North Sea reservoir (ca. 40% increase in

oil recovery), which has crude oil with a very low acid number (AN < 0.05). Experience with alkaline waterflooding
indicates that a high AN (AN > 0.2) is needed to generate
enough surfactant to induce wettability reversal and/or
emulsion formation (Ehrlich and Wygal, 1977). No direct
correlation has been found between the increase in oil
recovery due to low salinity waterfloods and the acid number of the crude oil (Figure 2). As the number of low salinity
waterfloods performed increased, some evi dence has
started to emerge that the benefit of low salinity production
mechanism could be achieved at a pH below 7.
Heriot Watt University (HW) performed an experiment
on a North Slope core sample where the pH rose from 5 to 6
(Figure 3a) with an increase in oil recovery. A model using
the geochemical modeling code, PHREEQC, was created
simulate a low salinity waterflood (Appelo and Postma,
2005). The model gave only an approximation of the pH
variation as the organic phase is extremely difficult to
model accurately. Interestingly, when the model contained
traces of carbonate, the pH increased and then slowly
decreased as observed in the HW experiment (Figure 3).
But when the carbonate trace amounts were removed, the
pH dropped. This disputes the earlier hypothesis that the
main drive for the pH variation is the carbonate dissolution.
The injection of fresh water in a saline aquifer is accompanied by a loss of Na+ and Mg2+ from the exchanger and an
increase in Ca2+ at the exchanger surface (Appelo, 1994). In
principle the loss of Ca2+ from solution is sufficient to drive
the dissolution reaction which should increase the pH up to
10. However, this is not observed in an aquifer due to proton buffering, which will keep pH at about 7 to 8. Proton
buffering is due to the desorption of proton (H+) from
oxides and organic matter. It is also due to the desorption of
complexes, in combination with reactions from oxides
(Griffioen, 1993). Furthermore, due to technical limita-

FIG. 1 pH variation during a low salinity flood (pH versus pore

volumes).

FIG. 2 Lack of correlation between acid number and the

increase in oil recovery due to low-saliniy waterflood.

CaCO 3
CO 2-3 + H 2O

30

Ca 2+ + CO 2-3
HCO -3 + OH - .

(1)
(2)

PETROPHYSICS

February 2008

Low Salinity Oil Recovery - An Experimental Investigation

tions, none of the experiments showing a change in pH were

performed at reservoir conditions with live fluids. The
majority of petroleum reservoirs contain CO2, which will
act as a pH buffer, rendering an increase of pH up to 10
unlikely if not impossible in most reservoirs.
The results obtained unequivocally prove that despite
previous evidence, high pH is not responsible for the
increase in oil recovery due to the injection of low salinity
water. This is important as it would have been very unlikely
that such an increase would have been sustainable in a
petroleum reservoir due to the proton buffering from oxides
present in the reservoir rocks and the significant amount of
CO2 present in some petroleum reservoirs.
Multi-component Ionic Exchange (MIE)

At the same time as pH measurements were carried out,

geochemical analysis of the low salinity effluents were performed. These high lighted the pre dom i nant role of
multicomponent ionic exchange (MIE) chromatography on
the water chemistry during waterflooding. Multicomponent
ionic exchange is the basis of geochromatography. It
involves the competition of all the ions in pore water for the
mineral matrix exchange sites. Because natural exchangers
show different selectivity for different cations, the ratio of
sorbed over solute concentration is variable for individual
cations. This theory was applied to enhanced oil recovery in
the 70s by Pope et al. (1978) but the best application of this
theory was done by a hydrogeologist who studied the invasion of saline aquifers by fresh water. Valocchi et al. (1981)
injected fresh water into a brackish water aquifer and
noticed that the concentration of Ca2+ and Mg2+ in different
control wells were lower than the invading water and the
connate brine. Similar results were witnessed during low

FIG. 3 a) pH variation during a low salinity waterflood in an Endicott core. b) PHREEQC model of the pH variation during a low salinity waterflood with the presence of calcite. c) PHREEQC model of the pH variation during a low salinity waterflood without the presence of calcite.

February 2008

PETROPHYSICS

31

Arnaud et al.

TABLE 1 Mechanism of association between organic functional groups and soil minerals (from Sposito, 1989).
Mechanism

Organic functional group involved

Cation exchange

Amino, ring NH, heterocyclic N

(aromatic ring)
Amino, heterocyclic N, carbonyl,
carboxylate
Carboxylate
Amino, Carboxylate, carbonyl,
alcoholic OH
Carboxylate, amines, carbonyl,
alcoholic OH
Carboxylate
Amino, carbonyl, carboxyl, phenolic
OH
Uncharged organic units

Protonation
Anion exchange
Water bridging
Cation bridging
Ligand exchange
Hydrogen bonding
Van der Waals interaction

salinity floods done at BP and Heriot Watt (Figure 4). The

evidence of MIE came from the effluent analysis of a North
Slope low-salinity coreflood. The injected brine had a
lower salinity than the connate water. However the effluent
analysis showed a sharp decrease in Mg2+ and Ca2+ concentration. Their concentration dropped lower than the concentration in the invading brine. This indicates that Mg2+ and
Ca2+ were strongly adsorbed by the rock matrix. Similar

FIG. 4 Variation in Ca2+ and Mg2+ in the effluent during

low-salinity corefloods. The two HS lines show the concentration
in the high-salinity connate brine and the LS lines show the concentration in the low-salinity connate brine. Cation exchange
caused the concentration in the effluent (diamond and square
points) to decrease below the two LS curves and then return to
the same concentration as the low-salinity brine once equilibrium was reached. All concentrations are in parts per millions

32

results were obtained by Heriot Watt University on two

different floods performed on the same system.
Following these results a mechanism was formulated
around the possibility that MIE was responsible for the
increase in oil recovery. According to the extended DLVO
theory (Amarson and Keil, 2000) and Sposito (1989), eight
different possible mechanisms of organic matter adsorption
onto clay mineral are possible depending on the organic
function of the organic matter and the condition of the clay
surfaces (Table 1). Out of those eight mechanisms, four are
strongly affected by cation exchange occurring during a
low salinity brine injection; cation exchange, ligand bonding and cation and water bridging (Figure 5).
Adsorption by cation exchange occurs when molecules
con tain ing quaternized nitro gen or heterocyclic ring
replace exchangeable metal cations initially bound to clay
surface. Ligand bonding refers to the direct bond formation
between a multivalent cation and a carboxylate group.
These bonds are stronger than cation bridging and cation
exchange bonds and lead to the detach ment of
organo-metallic complexes (RCOO-M; where M represents
the multivalent cation) from the mineral surface. Cation
bridging is a weak adsorption mechanism between polar
functional group and exchangeable cations on the clay surface. It is to note that on some occasion if the exchangeable
cation is strongly solvated (i.e Mg2+) water bridging will
occur. It involves the complexation between the water molecule solvating the exchangeable cation and the polar functional group of the organic molecule. In several studies
regarding organic matter adsorption onto clay minerals in
seawater (Amarson and Keil, 2000; Hedges and Hare,
1987; Henrichs and Sugai, 1993; Kia, 1987), it has been
found that Van der Waals interactions, ligand exchange and
cation bridging are the dominant adsorption mechanisms.
On an oil-wet surface, multivalent cations at a clay surface will bond to polar compounds present in the oil phase
(resin and asphaltene) forming organo-metallic complexes.

FIG. 5 Representation of the diverse adhesion mechanism

occurring between clay surface and crude oil.

PETROPHYSICS

February 2008

Low Salinity Oil Recovery - An Experimental Investigation

Such complexes have been shown to promote oil-wetness

in petroleum reservoirs (Rueslatten et al., 1994). At the
same time, some organic polar compounds will be adsorbed
directly to the mineral surface displacing the most labile
cations present at the clay surface, enhancing the oil wetness of the clay surface. During the injection of low salinity
brine, MIE will take place, removing organic polar compounds and organo-metallic complexes from the surface
and replacing them with uncomplexed cations. In theory,
the desorption of polar compounds from the clay surface
should lead to a more water-wet surface, resulting in an
increase in oil recovery.
To test this mechanism, an experiment was devised to
replace all the multivalent cations present on the mineral
surface by Na+. A North Slope core sample was flushed
repeatedly with brine containing only NaCl until the effluent showed only traces of Ca2+ and Mg2+. Two shut-ins were
performed to make sure that no carbonate was left undissolved. Once the core surface was fully saturated with Na+,
oil was flooded until a Swi of 12% was obtained. After
aging, high salinity brine, containing only NaCl was
flushed through the core followed by low salinity brine containing only NaCl. Finally a tertiary flood was performed
using low salinity brine containing Ca2+ and Mg2+.
By doing so, the formation of organo-metallic complexes on the mineral surfaces due to the presence of
multivalent cations on the mineral surface, was prevented
and only van der Waals interactions occurred. If MIE is the
predominant mechanism, the primary high salinity flood
should yield a higher oil recovery due to the absence of oil
adsorption by ligand formation and multivalent cation bridging and exchange. Also the secondary low salinity flood
should not produce any oil as all the mobile oil would have
been displaced by the primary flood and no organo-metallic
complexes are present to be desorbed. Finally a tertiary low
salinity flood containing divalent cations should not produce
any oil as only non-complexable monovalent cations (i.e.
Na+) will be desorbed from the mineral surface by the divalent cations present in the invading brine.
The results of the experiments matched the predictions.
First, the North Slope core sample was prepared to a representative initial water saturation and aged in dead crude oil.
The initial screening experiments were conducted at 25C.
A conventional high salinity waterflood gave a recovery of
42% OOIP and a tertiary low salinity flood resulted in a
total recovery of 48% OOIP (i.e. an additional 5% OOIP). A
second suite of experiments were conducted at reservoir
tem per a ture (102C). A con ven tional high salin ity
waterflood resulted in a recovery of 35% OOIP. The core
was flushed with brine containing only high salinity NaCl
until Ca2+ and Mg2+ was effectively eluted from the pore
surface. Initial water saturation was re-established and the
February 2008

sample aged in crude oil. A high salinity waterflood consisting of NaCl (no Ca2+ and Mg2+) resulted in a recovery of
48% OOIP. A tertiary low salinity flood was then conducted
(again no Ca2+ and Mg2+) and no additional recovery
observed (Figure 6). This was followed by a low salinity
flood with Ca2+ and Mg2+ present and again no additional
recovery was observed. This sequence indicated that high
salinity connate brine containing Ca2+ and Mg2+ resulted in
poor recovery. Removing the Ca2+ and Mg2+ from the rock
surface before waterflooding led to higher recovery irrespective of salinity. This is noteworthy in that this is the first time
that no improve oil recovery is observed when low salinity
water is injected into a clastic reservoir where the mineral
structure was preserved. This has confirmed the importance
of MIE in the low salinity production mechanism.
CONCLUSION

pH-induced IFT reduction or emulsification and fines

migra tion are not ubiq ui tous dur ing low salin ity
waterfloods. They are an effect rather than the cause. Cation
exchange between the mineral surface and the invading
brine has been demonstrated to be the primary mechanism
underlying the improved waterflood recovery observed
with low salinity waterflood. This mechanism explains
many of the results that have been reported during 10 years
of research on low salinity injection. It explains why the
low salinity production mechanism does not work when a
core is acidized and fired as the cation exchange capacity of
the clay minerals is destroyed. It explains why low salinity
water injection has no effect on mineral oil as no polar compounds are present to strongly interact with the clay minerals. Also it explains why there is no direct correlation
between the oil acid number and the amount of oil recovered as quaternized nitrogen and heterocyclic ring also play
a role in the adsorption mechanism. Finally it explains why

FIG. 6 Effect of MIE on oil recovery percentage.

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33

Arnaud et al.

the low salinity production mechanism does not seem to

work on carbonate reservoirs.
NOMENCLATURE

AN
CEC
CFC
DLVO

Acid number
Cation exchange capacity
Critical flocculation concentration
Deryaguin-Landau-Verwey-Overbeek theory
of colloids
ICP-MS Inductively coupled plasma mass spectroscopy
MIE
Multicomponent Ionic exchange
OOIP
Original oil in place
pH
Potential of hydrogen
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ABOUT THE AUTHORS

Ken Sorbie is a professor of petro leum engineering at
H e r i o t - Wa t t U . i n E d i n b u rg h , S c o t l a n d . e - m a i l :
[email protected]. His research interests include the modeling of multiphase flow in porous media, particularly on the fun-

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February 2008

Low Salinity Oil Recovery - An Experimental Investigation

damentals of two- and three-phase flow at the pore level and on the
effects of wettability. He is also active in the study of chemical and
porous media transport aspects of mineral scale formation and prevention in oil fields. Sorbie holds a BS degree in chemistry from
Strathclyde U., Scotland, and a PhD degree in theoretical chemistry/applied mathematics from Sussex U.
Mike Singleton is a Research Associate at the Heriot-Watt
University Institute of Petroleum Engineering, where his research
interests include the chemical interactions that take place during
fluid flow through porous media. Mike also holds a BSc Degree in
Chemistry from Salford University (1991) and an MPhil in Petroleum Engineering from Heriot-Watt University (1998). He
co-ordinates (together with Ken Sorbie) the FAST-rac consultancy
arm of the Flow Assurance and Scale Team (FAST) joint industry
project (JIP). Mike joined the FAST group in December 2004 following ten years of service with Baker Petrolite, Liverpool, UK.
During this time he was involved in the manufacture and testing of
many oilfield service chemicals, ranging from demulsifiers to
scale, wax and corrosion inhibitors. He was also involved in inves-

February 2008

tigating the area of Chemical Water Control and Relative Permeability Modification (RPM).
Cliff Black is a Senior Advisor in Reservoir Management for
BP. He provides coaching and assurance for BP Major Projects and
Reservoir Management worldwide with particular focus on
waterflooding and IOR. He has held various leadership positions
in BPs E&P Technology organizations and has initiated many
technologies that are moving into field deployment today. He has
29 years experience in improving oil recovery.
Kevin Webb is currently the low salinity subsurface project
manager in the Pushing Reservoir Limits team which is part of BPs
E&P Technology organization in the UK. He has 22 years experience in oil recovery processes, especially waterflood, and has provided analyses and interpretation of laboratory data to many BP
projects worldwide.
Arnaud Lager is a reservoir engineer for BP in the Pushing
Reservoir Limits team which is part of BPs E&P Technology organization. He has a Msc degree in Petroleum Geochemistry from the
University of Newcastle (2000). He is currently working in Alaska
on the deployment of Low salinity waterflood.

PETROPHYSICS

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