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Gas Flotation of Petroleum Produced Water: A Review on Status, Fundamental

Aspects, and Perspectives

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DOI: 10.1021/acs.energyfuels.0c03262

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Gas Flotation of Petroleum Produced Water: A Review on Status,

Fundamental Aspects, and Perspectives
Martina Piccioli, Svein Viggo Aanesen, He Zhao, Marcin Dudek, and Gisle Øye*

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ABSTRACT: Produced water is a major byproduct in oil production and the largest waste stream generated in the petroleum
industry. At the Norwegian Continental Shelf, produced water is still mostly discharged to the sea, but some installations re-inject
produced water into the reservoir for pressure support or disposal. Gas flotation is a separation technology widely used both onshore
and offshore that generally reduces the oil concentration to <25 ppmv. It is also a promising technology for subsea water treatment.
The aim of this review is to give an overview and provide a link between the industrial use and the fundamental aspects of gas
flotation. The industrial analysis examines the development and design of gas flotation technologies: induced, dissolved, and compact
flotation units. Several aspects of subsea water separation are also discussed. The fundamental aspects are dedicated to the fluid
dynamics of bubble−droplet collisions and the phenomena involved after their encounter, i.e., film drainage, forces involved in this
process, and spreading of oil on the surface of gas bubbles. Moreover, a detailed analysis of parameters that can affect gas flotation,
like gas bubble and oil droplet sizes, droplet−bubble attachment mechanisms, interfacial properties, water composition, oil and gas
properties, pressure, and temperature, is provided.

1. INTRODUCTION Recently, however, more emphasis has been put on removing

Petroleum is still a major source of energy for most countries,
and it is estimated that the daily petroleum consumption in the
world will increase from 85 million barrels in 2006 to 106.6
million barrels by 2030.1 The production of oil generates 3−5
barrels of produced water (PW) for each barrel of oil.2 Already
in 1999, the daily water production was estimated to be over
210 million barrels worldwide.3 To reduce the environmental
footprint of the industry, efficient separation during water
treatment is essential.
PW is extracted from the reservoirs together with the
hydrocarbons. In the offshore production, it is often a mix of
formation and injection water. The composition is highly
complex and dependent upon the location, age, and
production history of the reservoir. Typically, PW contains a
wide variety of dissolved and dispersed components. The
dispersed components can be oil droplets, various types of
inorganic particles, and bubbles formed by nucleation and
growth of dissolved gas upon pressure reduction. The
dissolved constituents can be inorganic ions, water-soluble oil
components, and various production chemicals added to
optimize operations. Different components can also interact
and form complex and poorly defined constituents, sometimes
referred to as “schmoo”. Moreover, the composition can be
altered by chemical processes (scaling), physical processes
(sedimentation and biofilm attachment), or microbial
processes (reservoir souring, degradation of organics, and
formation of biomass).4
Before discharge to the sea or reinjection into a reservoir,
PW must be treated to a certain level of purity. The treatment
can be a multistage process of different technologies, where,
conventionally, the main goal has been to remove dispersed oil.
dissolved organic components, to reduce their potential
negative effects on the environment, and inorganic solids, if
the water is to be reinjected.
The environmental impact factor (EIF),5 used by operators
in the Convention for the Protection of the Marine
Environment of the North-East Atlantic (OSPAR) region to
assess the environmental risk and toxicity of PW discharges,
has shown that the dissolved components result in high EIF
values, while the contribution from dispersed oil can be
minimal.6,7 The composition and concentration of dissolved
organic compounds can depend upon different factors, such as
the type of oil, produced water volume and composition,
maturity of the field, or process conditions.8
In comparison to other oil and grease removal technologies,
gas flotation offers advantages, such as (i) shorter retention
time and higher loading rate, (ii) less sensitivity to oil density
and viscosity, (iii) compact and smaller footprint, and (iv)
better separation of small and light particles.9 Before going into
details of gas flotation, a brief overview of the offshore
petroleum production process is given. During offshore
production, the fluids produced from a well typically enter a
three-phase separator, where the gravity separates the fluids
into gas, oil, and water based on the density differences and the
Received: September 28, 2020
Revised: November 19, 2020

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size distributions of the dispersed phases. Different internals separation technology, as subsea petroleum production and
can also be installed to optimize the performance. Next, the processing facilities are increasingly used.22 Next, the collisions
crude oil and natural gas are treated in secondary and tertiary and attachment mechanisms of gas bubbles and oil droplets are
stages to reach export quality, while the PW has to be purified outlined. Finally, the importance of the interfacial properties
before discharge to the sea or reinjection into a reservoir. and the impact of the chemical composition of the oil/water/
One of the most common PW treatment methods, especially gas phases on the attachment process are highlighted. These
offshore, is with hydrocyclones. Subsequently, gas flotation aspects have not been systematically reviewed in the literature.
systems are typically used to further reduce the oil
concentration. However, the combination of separation 2. CURRENT STATUS OF GAS FLOTATION FOR PW
technologies depends upon the production site. Hydrocyclones TREATMENT
can be useful to reduce the oil concentration before PW enters 2.1. Gas Flotation Methods. There are three main
gas flotation systems, but can also be subject to clogging or methods of gas flotation: induced gas flotation (IGF),
fouling, and gravity separators can be followed directly by gas dissolved gas flotation (DGF), and electroflotation. Only the
flotation systems. first two, normally employed in the oil field practice, will be
Additional polishing steps, such as media filtration or considered here. IGF and DGF differ fundamentally in the way
membrane separation, can be used to target the smallest of generating gas bubbles, also leading to differences in their
droplets and particles remaining in the water phase and, to sizes, the mixing conditions, the hydraulic loading rate, and the
some extent, also dissolved components. As mentioned above, retention times. A comparison of the methods is summarized
the options available to handle the PW are1,2: reinjection, in Table 1.
where the PW is injected into the same formation from which
the oil is produced or to a disposal formation; and discharge to Table 1. Comparison between Induced and Dissolved Gas
the environment, where treatment of the PW must meet Flotation Systems Based on Ref 16
discharge regulations. According to the OSPAR requirements,
the oil content must be lower than 30 ppm to discharge the parameter IGF DGF
PW to the sea. However, the European Commission currently bubble size 100−1000 μm 10−100 μm
aims to reduce this limit to 15 mg/L for the existing generation velocity based, entrainment pressure based, saturation
installations and zero discharge on new facilities.10 If the PW method and dispersion and depressurization
is going to be reinjected, the threshold of the dispersed operating turbulent and less quiescent; quiescent; usually single-cell
condition multi-cell configuration configuration
components is typically determined by their concentration and
retention <5 min 5−15 min
size distribution that can be injected into the reservoir. This time
means that removal of both oil and solids is essential in this footprint compact (as a result of the high large (as a result of the high
case.11 At the Norwegian Continental Shelf (NCS), water residence time) residence time)
discharged to the sea peaked at 160 million standard cubic capital cost low high (large tank and
saturation system)
meter (scm) in 2007 and declined to 138 million scm in 2016.
The amount of reinjected water, on the other hand, has
increased, and in 2016, approximately a quarter of all of the
PW was reinjected.12 For new installations, PW reinjection is 2.1.1. Induced Gas Flotation (IGF). In IGF processes, the
often considered the primary option of dealing with PW. gas bubbles can be introduced into the influent by either
As a result of its complexity and the need to handle large mechanical or hydraulic methods. In the mechanical-based
volumes of PW during petroleum production process, the IGF, the gas is introduced in the water through flow eddies
importance of topics related to PW has increased in the recent created by a mechanical impeller. The hydraulic units, on the
years, in both academia and industry. This is reflected in a other hand, use an eductor device to entrain the gas into the
number of review papers: the composition and treatment of water and have fewer moving parts than the mechanical units.
PW has been reviewed by several authors.1,2,13,14 Judd et al.15 Usually, gas bubbles generated through this method have a
examined the performance of several PW treatment diameter in the range of 100−1000 μm.19 An illustration of
technologies, including gas flotation. Rubio et al.16 investigated hydraulic IGF is given in Figure 1. Nowadays, offshore
the use of flotation in environmental applications, while Bennet flotation units have a compact hydraulic IGF design with a
et al.17 discussed the usage of air flotation for the separation of vertical orientation and no moving parts.23
oil from wastewater. Moosai and Dawe18,19 and more recently
Saththasivam et al.20 reviewed the oil droplet−gas bubble
attachment process, while Niewiadomski et al.21 described the
different mechanisms of bubble and droplet encounters. These
reviews are focused on either the macro- or microscopic
aspects of gas flotation, without discussing them in connection
with one another. The aim of this review is to combine both
large- and small-scale perspectives of gas flotation, first by
reviewing the current gas flotation technologies available for
the treatment of offshore PW and then by investigating the
fundamental aspects of gas flotation. In the first part, we focus
on the design of various compact flotation units (CFUs).
CFUs are a relatively recent advancement in the field of Figure 1. Illustration of hydraulic IGF. This figure was reproduced
flotation and have largely been omitted in the literature. with permission from ref 30. Copyright 2019 American Chemical
Moreover, we emphasize the recent improvements of subsea Society.

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2.1.2. Dissolved Gas Flotation (DGF). In DGF, fine bubbles
are formed by nucleation and growth of gas dissolved in both
water and oil phases when the pressure is reduced24 (Figure 2).
Figure 2. Illustration of bubble generation during DGF. This figure
was reproduced with permission from ref 30. Copyright [2019
American Chemical Society.
Nucleation of supersaturated gas could be either hetero- or
homogeneous, where heterogeneous is, by far, the most
efficient mechanism as a result of the lower energy barriers
when existing surfaces are the nucleation sites. Another
element to consider in DGF is the higher gas solubility in
the oil phase. The gas volume released at pressure reductions
will be higher within the oil droplets than in the surrounding
water phase. Expansion of gas bubbles in the oil droplets
should therefore also be considered during DGF. The
generated bubbles are much smaller compared to IGF: 10−
100 μm.19 Because the size of gas bubbles is smaller, the
retention time will also be higher. The gas/oil ratio and
hydraulic loading are also important factors to consider in
DGF.25
Recently, attention has been given to nanosized bubbles and
their role in DGF. Studies have shown that they can adhere
and/or entrain inside oil droplets, generating capillary bridges
between the droplets. This improved the hydrophobicity of the
droplets and the probability of adhesion to microbubbles and,
thereby, increased the overall flotation efficiency.26−28
2.1.3. Comparison of DGF to IGF. The main differences
between the two gas flotation techniques are the ways of
generating the gas bubbles, resulting in different mechanisms
and total surface areas of bubbles. Eftekhardadkhah et al.11
compared the removal of dispersed oil from PW during
induced, dissolved, and mixed IGF−DGF modes.
At two PW flow rates, the IGF had better removal efficiency
than the DGF, while the combination of the modes showed the
best removal. Clearly, the way of generating the bubbles
influenced the separation efficiency and the attachment
mechanisms between oil droplets and gas bubbles. During
IGF, gas bubbles are usually fully or partially encapsulated by
oil droplets. In contrast, during DGF, gas bubbles nucleate at
the surface or inside oil droplets and grow to sufficient size to
aid the separation. This process occurs if the partial pressure is
lower in the gas phase than in the liquid phase, meaning that
enough gas must be released from the solution, and a pressure
drop at the inlet is needed. The amount of released gas can
also depend upon the temperature and pressure difference
between the upstream piping and the operation condition of
the cell.
2.2. Compact Flotation Units (CFUs). A gas flotation
system used offshore should be designed for (i) minimal
footprint and weight, (ii) reduced motion sensitivity, (iii)
optimal oil removal efficiency, and (iv) simple operation.
pubs.acs.org/EF Review
This led to the development of the CFUs. These are
hydraulic units that can use both IGF and DGF advantages to
remove oil droplets from PW.29 Performing gas flotation in
single mode would result in disadvantages: in IGF systems, the
oil droplets much smaller than 100 μm may escape flotation,
while in DGF systems, the oil droplets larger than 100 μm
cannot be floated.30
Vertical vessels are usually preferred, because they require
less space and are less affected by wave motion. The retention
time is typically less than 1 min.31 The first CFU was
introduced to the oil and gas industry at the NCS in 2001.32
Today, the method has become well-proven and is used
worldwide. New designs of CFUs have also been developed to
maximize the performance and minimize the footprint and
weight.
2.2.1. Advances in CFU Design. In the original CFU design
(left panel of Figure 3), the process takes place in a single-
Figure 3. Schematic representation of the original CFU design (left)
and a more recent development (right).
compartment vessel, where water is introduced from the upper
part and mixing, flotation, and separation are all done in the
open settings. This results in a countercurrent flow: smaller oil
droplets tend to follow the gravity and stream of treated water,
affecting the efficiency of flotation.
Later a multistage single-vessel CFU was introduced,33
where the number of internal stages can be adjusted to the PW
quality at the inlet. PW enters the vessel near the bottom, and
the gas is added just upstream the vessel inlet. Then, the
mixture is distributed into the vessel through several tangential
pipes. The continuous mixing through the different tangential
pipes increases the flotation efficiency in each stage by
promoting the coalescence of oil droplets.
A CFU with internal swirl design has also been reported to
improve the gas separation efficiency.29 The swirl design
features a lower terminal velocity in certain areas and a flow
eddy that aids collisions between gas bubbles and oil droplets
and separates residual crude oil from PW in a second treatment
stage, allowing for separation of more of the smaller gas
bubbles with attached oil droplets.
A recent development in the design of CFU is a separate
inlet chamber with water flow at the bottom of the vessel (right
panel of Figure 3). The water is distributed in the vessel
through several tangential distribution pipes that promote oil
droplet coalescence, improving the process efficiency. In
comparison to the old design, in the inlet chamber, where
water and gas are mixed, there is no countercurrent flow,
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allowing for higher concentrations of bubbles and droplets for
an extended period of time. This normally has a positive
influence on the coalescence efficiency. Dedicated drain points
or short pulses of increased flow are used to mitigate
accumulation of large solid particles in the inlet drum.
In Table 2, the range values of important operating
parameters of the most recent CFU designs are listed with
their range values.
Table 2. CFU’s Operating Parameters
parameter range value
capacity (m3/h) 10−900
vessel dimension (m) diameter of 1.5−3.5
height of up to 7.5
residence time (min) 0.5−1
Bubble size distributions in CFUs can vary according to the
bubble creation method. In Table 3, typical bubble generation
Table 3. CFU Gas Bubble Distribution According to the
Generation Method
gas bubble
generation method size (μm) additional remarks
boosted recycle motive 200−300 most reliable method: stable and
water stream and powering independent of feed flow
liquid driven ejectors
sparge mix method that uses 300−600 simple approach but not robust
feedwater pressure
break outgas 20−50 quality of bubbles depends upon
flow, upstream piping/valving, etc.
multiphase pump (DGF 50−80 at a high temperature, the dissolution
pumps) is poor and most of the gas is
sheared with the impeller
methods and corresponding bubble sizes are given. Two
important factors can be noted: (i) if too small bubbles are
generated, they could cause insufficient buoyancy for the
separation, meaning that the residence time would also be
increased, and (ii) the bubbles from all of the generation
techniques can have different size distributions.34
2.3. Subsea Separation and CFUs. Nowadays, significant
attention is given to subsea production and processing. Seabed
water treatment can also result in a substantial decrease of CO2
emissions.33 The conditions at the seabed level are extreme
compared to topside, and the high pressure can change the
fluid behavior. The higher values of absolute pressure can raise
the density difference between water and oil and reduce the
viscosity of the fluids. As a result, the separation performance
may be enhanced. These conditions also imply some changes
in the process units compared to topside (offshore) design.
Subsea separators and hydrocyclones for PW treatment are
currently in operation or test use,35−39 while new separation
concepts have been proposed.40,41 When it comes to CFUs,
however, their performance at high outer pressure is still a key
gap for possible subsea use. Moreover, the marinization, gas
and production chemical logistics, and reject handling are
other important reasons why subsea CFUs are not yet
qualified. One main challenge is that they rely on direct
injection of pressurized gas or the use of recirculation pumps
to drive eductors.36 Lately, a new type of eductor was
introduced, which lets the flotation unit operate without the
need of energy input or pressurized gas feed. This brings CFUs
one step closer to subsea application.
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A CFU module design has been recently tested for subsea
use at the expected fluid properties (Figure 4).
Figure 4. Illustration of design and components in the CFU module
design. This figure was reproduced with permission from ref 42.
Copyright 2020 Society of Petroleum Engineers.
This subsea CFU module uses IGF, where the ejectors
create the bubbles. The outlet for the clean water is at the
bottom of the vessel, while two tangential inlets for oil and gas
are located at the top. At the headers, flotation gas and motive
water are split into four branches connected to the ejectors,
where the gas is mixed and sheared by the motive water. The
water−gas mixture is then routed to the main water inlet and
three side inlets on the CFU vessel.
Overall, the results obtained with this subsea CFU are
comparable to a topside unit.42
3. MICROSCOPIC ASPECTS OF GAS FLOTATION
From a microscopic perspective, the formation of a stable
bubble−droplet agglomerate is generally considered to be the
rate-controlling step during gas flotation.43 There are two
mechanisms in which the bubble−droplet agglomerate can
form: (i) nucleation of gas bubbles at the surface or inside the
oil droplets or (ii) droplet−bubble coalescence after drainage
of the aqueous film between them.
Several sub-processes are involved during the film drainage
mechanism: the approach of gas bubbles and oil droplets, the
drainage and rupture of the aqueous film formed between
them upon close approach, and the rise of the coalesced
phases. Upon coalescence of oil droplets and bubbles, the
effective density of the oil is reduced and the increased density
difference between the agglomerates and water is used to
enhance the separation.19 The separation rate can be described
by Stokes’ law (eq 1)
2
2 R (ρo − ρw )
v=
9 η (1)
where v is the velocity of the droplets, ρo is the density of the
dispersed phase, ρw is the density of the continuous phase (i.e.,
water), R is the radius of the dispersed entity, η is the viscosity
of the continuous phase, and g is the gravitational constant.
From this, it can be seen that the size of the dispersed entity
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Figure 5. Mechanisms for gas bubble capture of oil droplets suspended in water: (A) direct impingement, (B1) gas bubble nucleation, coalescence,
and growth of the bubbles on the surface of the oil droplet, (B2) gas bubble nucleation and growth of the bubbles inside the oil droplet, (C)
clustering of gas bubbles to form a buoyant aggregate, and (D) hydrodynamic capture of oil droplets in the wake of rising bubbles. This figure was
based on ref 23.
and the density difference are the key factors for promoting
separation.
The chemical composition, the physicochemical properties
of the fluids, and the interfaces between the fluids will also
influence the bubble and droplet sizes in a gas flotation system.
The interfacial tension is an important parameter for
determining the extent of breakup of bubbles and droplets,
while the interfacial viscoelasticity will affect the film drainage
and rupture steps and, thereby, the formation of droplet−
bubble agglomerates.44
Moreover, the pressure and temperature will have effects on
the interfacial composition and behavior. Clearly, there are
many factors that will affect the separation process, and a deep
understanding of them is essential to obtain optimal and
reliable gas flotation processes. In this section, we will first
briefly review different droplet−bubble attachment mecha-
nisms, followed by a description of approach and film drainage
and rupture mechanisms. Finally, interfacial properties and
parameters affecting these will be considered.
3.1. Fluid Dynamics and Physical Aspects of Gas
Flotation. 3.1.1. Droplet−Bubble Attachment Mechanisms.
Four main droplet−bubble attachment mechanisms were
suggested, where the way the oil droplets and the gas bubbles
attach differs23 (Figure 5).
The first mechanism is full or partial encapsulation (Figure
5A).18,21 The rising gas bubbles create a water flow (illustrated
by streamlines) that the droplets tend to follow. If the droplets
are big enough, they will approach the gas bubbles, and a thin
aqueous film is formed between them, which can drain and
rupture. To evaluate if the oil droplet will spread and cover the
gas bubble, the spreading coefficient (S0) has to be taken into
account (eq 2)
pubs.acs.org/EF Review
S0 = γwg − γow − γog (2)
where γwg is the water−gas interfacial tension, γow is the oil−
water interfacial tension, and γog is the oil−gas interfacial
tension. It is important to distinguish between the initial
spreading coefficient (SIN), which indicates the initial spread-
ing affinity and is defined in the absence of the spread oil on
the gas surface, and the equilibrium spreading coefficient
(SEQ), which gives information about the thickness of the
spread oil layer, defined with γwg in the presence of spread
oil.45 A negative value of SIN means that SEQ is also negative,
and the oil does not spread on the surface of the bubble. A
positive value of SIN means that, when the three phases come
into contact, the oil phase will spread and form a continuous
film between the gas and water. In the latter case, two different
situations are possible, according to the value of SEQ. If SEQ = 0
(meaning that γwg = γow + γog, i.e., condition of complete
wetting), the oil spreads as a thick layer, while if SEQ < 0, there
is initial rapid spreading of the oil phase, followed by the
retraction of the oil film into a lens in the aft part of the gas
bubble. This means that SIN > SEQ and that if SIN can have
either a positive or negative value, SEQ can only be negative or
equal to 0.46 In fact, the equilibrium γwg is lower than the initial
γwg because of the presence of the spread oil but also because
of the adsorption of dissolved components at the gas−water
interface. An overview of all of the possible cases is given in
Table 4.
Clearly, the direct impingement with full encapsulation is
the best mechanism for oil flotation. This creates the strongest
droplet−bubble agglomerates and prevents detachment caused
by the shear forces occurring in the flotation unit. The
approach and drainage mechanisms will be described in more
detail below.
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Table 4. Bubble−Droplet Configuration According to the
Values of SIN and SEQ
SIN SEQ bubble−droplet configuration
<0 <0 no spreading
0 spreading
>0
<0 oil lens
In the second mechanisms depicted in Figure 5, the
dissolved gas nucleates on the surface of the oil droplets
(B1) or within the droplets (B2) and coalesces to form a
bigger bubble.47 The result will be a full or partial
encapsulation depending upon the bubble size and the initial
spreading coefficient.
The third mechanism (Figure 5C) consists of physical lifting
of the oil droplets by the flocculated gas bubbles.47 This can
lead to physical entrapment of rising gas bubbles.
The last mechanism (Figure 5D) occurs when the gas
bubbles are considerably bigger (hundreds of μm) than the oil
droplets. Here, the oil droplets are too small to break the water
layer between the bubble surface and droplets. Instead, they
will be entrapped in the turbulent wake created by the rising
bubbles. This is also called “hydrodynamic capture” and does
not lead to very stable bubble−droplet aggregates.48
3.1.2. Influence of Droplet and Bubble Sizes on Removal
Efficiency. The size ratio between droplets and bubbles can
influence the mechanisms by which oil droplets will be
removed during gas flotation, as outlined in the previous
section. The size distribution of oil droplets and gas bubbles
can also play a central role in the flotation efficiency. The
collision efficiency has been shown to depend upon particle
and bubble sizes.49 Several studies have also demonstrated that
oil removal by gas flotation is improved by decreasing the gas
bubble sizes, which has been attributed to larger surface areas
available for droplet attachment.49−51 Small gas bubbles also
lead to an increase in the collision frequency, considered a
crucial factor in oil droplet capture.52 Conversely, larger
bubbles result in lower collision efficiency.28 Moreover, a
recent study conducted by Lim et al.53 shows a reduction of
the oil attachment efficiency with the increase of the sizes of
gas bubbles as a result of a reduction of the contact angle. It is
important to keep in mind that gas bubbles are generally much
bigger than oil droplets. Flotation often works well with
droplets with a diameter above 20 μm, while smaller droplets
can result in too long retention times.18 Because the PW in gas
flotation units usually has been through a primary water
treatment stage, most of the oil droplets are usually less than
20 μm.18 If these small droplets are hard to separate,
flocculants can be added to the system, to improve the oil
removal efficiency.54,55 A parameter that can help in under-
standing if flocculants are needed in the system is the induction
time (defined later). If the induction time is considerably
reduced by their addition, flocculants are desirable. Further-
more, water treatment aided by flocculants can be needed if
Figure 6. Stages of the bubble−droplet interaction. From left to right: approaching (first two pictures), contact, thin-film breakage, spreading, and
an oil-coated bubble.
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the flotation process is placed a long distance from the well,
but flocculants are not necessary required if the process is close
to the production well (for example, subsea). In fact, it has
been demonstrated that separation can be more efficient when
the process is conducted at the seabed conditions.42
Higher collision probability can also be realized with a large
sweep factor (SF).20 The sweep factor describes the number of
times per unit time a given volume of water is swept by a gas
bubble and is defined as follows (eq 3):56
AgasFgas
SF =
Acell (3)
where Agas is the total cross-sectional area of bubbles per unit
volume, Fgas is the volumetric flow rate, and Acell is the cross-
sectional area of the flotation cell. Lee and Frankiewicz showed
the following relationship between the size of the gas bubbles
and the SF:57 The sweep factor increases as the size of the gas
bubbles decreases.
Notably, the sweep factor increases with decreasing bubble
size. In CFUs, however, the retention times must be taken into
account as well, which means that the oil removal efficiency
cannot be evaluated solely based on bubble sizes.
3.1.3. Fluid Dynamics of Bubble−Droplet Collisions. In
this section, the droplet−bubble attachment mechanism from
Figure 5A is described in more details. Images of the approach,
drainage, rupture, and coalescence steps are also shown in
Figure 6.
An encounter can be defined as the point when the oil
droplet is close enough in the path swept by a gas bubble, so
that a thin film is formed.21 The encounter can occur in four
different ways: gravity action, interception, inertial impact, and
turbulent motions.58,59
Starting with the gravity mechanism, both the oil droplets
and gas bubbles will flow upward in the gravitational field
because they are lighter than water. The gas bubbles are
generally bigger than the oil droplets and have a higher density
difference with water, which leads to a higher rising velocity
(eq 1). Therefore, oil droplets appear to fall on the gas
bubbles. Following the streamlines (depicted as dashed lines in
Figure 7), the oil droplets will initially move away from air
bubbles, before they get closer when passing around the aft
part of the bubbles.
If the oil droplets are big enough, they will come into
contact with the surface of the bubbles, and this is defined as
the interception mechanism. Encounters by inertial impact
occur when the oil droplet and the gas bubble approach each
other with such a high enough velocity that the droplet does
not have enough time to deviate from its path around the
bubble.
Finally, in turbulent motion, both the oil droplet and the gas
bubble are in turbulent eddies when they approach each other.
If the gas bubble is larger and the droplet is smaller than the
turbulent eddy (or the other way around), the droplet cannot
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Figure 7. Encounter of an oil droplet with a gas bubble in the Earth’s
gravitational field.
reach the bubble surface because it stays inside the eddy. This
mechanism is believed to increase the chance of the encounter.
Furthermore, Flint and Howarth60 showed that adjacent gas
bubbles have a positive impact on the gas flotation efficiency.
They can force the liquid streamlines closer to the bubble,
bringing the droplet trajectory closer.
3.1.4. Film Drainage. When oil droplets and gas bubbles
approach each other with any of the mechanisms outlined in
the previous section, a thin water film is formed between them.
This film should drain and rupture as quickly as possible to
form a stable droplet−bubble aggregate, which contributes to
achieve efficient gas flotation. The drainage of the film is
usually expressed in terms of the induction time, i.e., the time
required for the liquid film to reach the critical film thickness,
where it ruptures.61 Droplet−bubble adhesion has been
reported to occur at a (critical) film thickness of 0.1 μm.43
Studies by Gu et al.62 on air−bitumen systems showed that the
induction time increased with increasing the bubble size.
Moreover, Yan et al.51 observed that both the induction time
and spreading time increased as the size of the bubbles
increased.
Eftekhardadkhah et al.11 demonstrated that low induction
times improved the oil removal efficiency. The rate of film
drainage is determined by a combination of capillary pressure
and disjoining pressure.63 In addition, the Marangoni effect can
impair the film drainage process. This slowdown is due to a
concentration gradient of interfacial components that occurs
when they are pulled along with water as the film starts to
drain. This will create a flux in the opposite direction of the
film drainage inside the droplets/bubbles to resist the
concentration gradient at the interface.18
When the gas bubble and the oil droplet approach each
other, their interfaces are deformed and the pressure in the film
is different from the surrounding pressure by a quantity that is
equal to the capillary pressure.64,65 The capillary pressure is the
external force of the meniscus of the thin film, which forces the
liquid out of the film when the critical thickness is reached.
The disjoining pressure (Π) is the pressure inside the film and
is the internal force that disjoins the interfaces.44 It is the result
of surface forces acting at distances comparable to the thin-film
thickness.5 To balance the capillary pressure, the disjoining
pressure must increase in magnitude as the thickness of the
film decreases.66 Dependent upon the value of the disjoining
pressure, there can be different situations:44 If Π > 0, the
repulsive forces dominate and an external force is needed to
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drain the film to the critical thickness, where it ruptures. If Π <
0, the attractive forces dominate, leading to a spontaneous
drainage of the film, which will rupture after reaching the
critical thickness. The surface forces determining the disjoining
pressure are summarized in Figure 8.
Figure 8. Summary of the surface forces that affect the disjoining
pressure.
3.1.5. Spreading. After rupture of the film has occurred, the
oil can start to spread over the gas bubble. The spreading
coefficient of a fluid, S0, can be used to evaluate the process67
(eq 2).
The spreading velocity can be expressed in terms of the
coverage time, i.e., the time required for an oil droplet to
spread on a bubble after rupture of the film. Eftekhardadkhah
et al.68 showed that the coverage time is shorter than the
induction time and that it increases with the oil viscosity.
Kinetic studies have also demonstrated that, at higher viscosity
ratios (viscosity of water to the viscosity of the oil), the
spreading is faster.69
3.1.6. Strength of Bubble−Droplet Aggregates. Once
droplet−bubble aggregates have been formed, they must rise to
the top of the flotation unit, where they will be skimmed off as
a froth. To be stable, the adhesive force between the phases
must be large enough to prevent detachment under the
dynamic conditions of the flotation processes.44 Typically, it is
drag and turbulent forces that can contribute to detachment,
especially if the oil forms a lens at the aft of the bubble. The
detachment of droplet−bubble agglomerates can be viewed as
an emulsification process. If the bubbles are large, the water
flow in the aft part of them is expected to be highly turbulent
and can disperse the attached oil lens into smaller particles,
given enough energy. Also, the oil film spreading on the surface
of the gas bubble is exposed to a water drag. It has been shown
that emulsification of the attached oil makes oil flotation in
centrifugal devices, with a high energy dissipation rate,
inefficient.21
3.2. Interfacial Properties and Factors Influencing
Them. 3.2.1. Interfacial Tension and Interfacial Dilatational
Rheology. Adsorption of interfacially active components will
alter the interfacial properties of droplets and bubbles.
Indigenous crude oil components, like asphaltenes and resins,
will adsorb onto the oil−water interface of oil droplets, while
water-soluble oil components will also adsorb on the surface of
gas bubbles. In addition, production chemicals can adsorb onto
all available interfaces (gas−oil−water). Adsorption is a
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dynamic phenomenon that will lead to a decay in the
interfacial tension until the adsorption and desorption fluxes
are equal and an equilibrium is reached. A reduction of the
oil−water and gas−water interfacial tensions entails that less
energy is required to break up the oil droplets and gas bubbles.
Hence, the interfacial tension will influence droplet and bubble
size distributions.
The interfacial adsorption will also lead to viscoelastic effects
at the interfaces. Experimentally, the interfacial dilatational
moduli E′, which is related to the elasticity of the interface, and
E″, which is related to the viscosity of the interface, can be
determined.70 Often, it is the interfacial dilatational elasticity
(E′) that is of interest, because increasing elasticity as a result
of adsorption of components and buildup of interfacial layers
can oppose coalescence between droplets and bubbles. The
dilatational rheological properties have been considered most
relevant for short-term emulsion stability.71,72 An example is
the study by Prins et al.73 that found that a mixture of sodium
dodecyl sulfate (SDS) and dodecyl alcohol produced a more
stable oil-in-water (O/W) emulsion compared to emulsions
prepared using SDS alone as a result of the higher interfacial
dilatational elasticity in the first case. It has also been reported
that the adsorption of asphaltenes at O/W interfaces leads to
the formation of viscoelastic interfacial layers,74−76 which can
retard the drainage process and affect the oil spreading.
The interfacial dilatational elasticity will also affect the
Marangoni effect (described in section 3.1.4), which can
oppose the drainage of the thin aqueous film between droplets
and bubbles (Figure 9).
Figure 9. Marangoni effect between an oil droplet and a gas bubble in
water.
High dilatational elasticity can oppose the interfacial
concentration gradient and, thereby, increase the film drainage
time and oppose coalescence.
It is clear from this that the interfacial properties play an
important role for the flotation efficiency by influencing both
the attachment process between oil droplets and gas bubbles
and the size distributions. The interfacial properties will
depend upon the chemical composition of the oil, gas, and
water phases as well as the temperature and pressure. This and
the effect on the separation efficiency are described in the
following sections.
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3.2.2. Water Composition. 3.2.2.1. Dissolved Organics in
PW. The dissolved organic components in PW originate from
the crude oil, and their solubility depends upon the molecular
weight, type, and extent of polar functional groups formed by
heteroatoms in the structure and salinity and pH of the water
phase. The adsorption of these dissolved components at the
gas−water interface has been reported in several studies.77−80
Furthermore, it has been demonstrated that the adsorption of
dissolved components on the bubble prevents bubble
coalescence and reduces the attachment efficiency between
oil droplets and bubbles.81 This can be attributed to an
increased potential energy, which prolongs or prevents the
rupture of the thin liquid film. Moreover, the adsorption of the
dissolved organic compounds at the gas−water interface leads
to a decrease in the interfacial tensions, affecting the size of gas
bubbles. The presence of dissolved organic components can
also increase the viscosity of the aqueous phase, which could
prolong the film drainage time.68 In either case, the result will
be reduced oil removal during gas flotation.11
3.2.2.2. Salinity of PW. Salinity of water, i.e., the amount
and type of ions in the water phase, is an important parameter
for efficient gas flotation. It can promote the gas bubble−oil
droplet attachment and oil droplet coalescence and prohibit
the merging between gas bubbles.18,23
It has been reported that, at sufficiently low salinity, the
presence of electrical double layer interactions will reduce the
attachment efficiency of oil droplets and bubbles,81 while no
rupture of the thin films was seen in ultrapure water.68 The
removal of the repulsive double layer between oil droplets and
gas bubbles by increasing the salinity decreases the induction
time, favoring the oil attachment on gas bubbles.43 Chakibi et
al.64 also showed that the rupture times of the film decrease
considerably at high ionic strength.
The ionic composition of water can also influence the
adsorption of the dissolved organic compounds at the gas−
water interface,82 affecting the gas bubble−oil droplet
attachment.
It has been shown that metal cations, such as Ca2+, Mg2+,
Na+, and K+, can increase the droplet−bubble attachment
efficiency,83 by reacting with the dissolved organic compounds
adsorbed at the oil−water interface. The hydrophobic
complexes can act as “bridges” between the two coalescing
units, favoring the attachment process. Moreover, the divalent
ions can form complexes with the dissociated naphthenic acids
at the oil−water interface.84 These complexes are less
hydrophilic than the charged species and can partition from
the interface and back to the oil phase, reducing the amount of
interfacially active components at the oil−water interface.
To promote droplet−droplet coalescence, coagulants
containing the trivalent ions Al3+ and Fe3+ can be added to
the system.85−87 However, in PW systems, polymeric
flocculants are more popular.88
It has also been widely reported that the electrolyte
concentration affects bubble sizes.50,89−92 Furthermore, it has
been demonstrated that the gas bubbles become much smaller
above a certain critical salinity concentration, leading to more
efficient gas dispersion.93−95
The valency of the ions also plays an important role, and
studies have shown that the concentration of salt required to
inhibit coalescence varies in the sequence: Al3+ < Mg2+ <
Na+.96−98 There is still no agreement on explaining the
reduced coalescence between bubbles caused by electrolytes,
but different explanations have been proposed.93 Hydration
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repulsions, electrical double-layer repulsions, gas solubility,
hydrophobic attractions, and the Gibbs−Marangoni effect have
all been suggested as possible mechanisms for the inhibition of
coalescence between bubbles. Recently, Firouzi and Nguyen99
also presented a modeling approach where non-DLVO forces
together with the Gibbs−Marangoni stress and Casimir−van
der Waals attraction were used to understand the bubble
coalescence in salt solutions.
Sadeghi and Vissers100 studied the breakup of bubbles at
different salt concentrations. They showed that, at 5 g/L of
NaCl, only smaller bubbles (50 μm diameter) were broken,
and their diameters were halved. On the other hand, at a
salinity of 40 g/L, only the bigger bubbles (100 μm diameter)
were affected and broken down to 25−30 μm, while the
smaller bubbles (20−30 μm diameter) remained stable and did
not change with the further increase of salinity.
Furthermore, Fanaie and Khiadani101 studied the effect of
salinity on the size distribution of microbubbles of a dissolved
air flotation system and observed a reduction from 40−250 μm
(freshwater) to 20−160 μm (saline water).
3.2.2.3. pH. The oil attachment efficiency on gas bubbles is
also affected by the pH of the water phase. Varying the pH
significantly influences the solubility of certain organic
compounds and their interfacial properties.80,102 The pH of
the aqueous phase determines whether the acids or bases
govern the interfacial properties.103 Dependent upon pH,
charged species can accumulate at the oil−water or gas−water
interfaces, reduce the interfacial tension, and form viscoelastic
interfacial layers. At low pH values, the basic compounds
adsorb at the interfaces and become protonated, while at
neutral or higher pH, the acids govern the interfacial activity.
Still, acidic components of crude oils are typically considered
to be more surface-active than their basic counterparts.102,104
Li et al.105 performed experiments to study the effect of pH on
the gas flotation efficiency for a dissolved air flotation system.
Their results showed that the highest removal efficiency is
reached at pH values between 6 and 9. On the other hand, a
study performed on the attachment between crude oil droplets
and bubbles showed higher efficiency at the lower values of pH
(4 and 6).81 This difference might be due to the presence of
dissolved components in their systems. In fact, at neutral or
high pH values, the acids accumulate at the oil−water and
gas−water interfaces, reducing the attachment efficiency. The
salinity must be included in the discussion as well. At low
salinities, where the electrostatic repulsion is higher and
prevents the approach of oil droplets and gas bubbles, pH will
have a stronger impact. Moreover, as explained in the previous
paragraph, multivalent metal ions can act as bridges between
oil droplets and gas bubbles and improve the attachment.
3.2.3. Oil Properties. The chemical composition of the
crude oil will obviously influence the separation process. Crude
oils are in fact mixtures of hydrocarbons and a wide range of
other organic components. Moreover, crude oil compounds
can have different degrees of polarity, affected by the presence
of heteroatoms, like nitrogen, sulfur, and oxygen.106,107 These
polar compounds can adsorb at the oil−water interface,
influencing the drainage and rupture of the film separating the
oil droplet and the gas bubble.68 Moreover, as outlined above,
the adsorption of the dissolved components on bubbles will
reduce the gas bubble−oil droplet attachment.81 In addition,
the oil-in-water concentration and density and viscosity of the
oil are other important parameters that can affect the oil
removal during gas flotation. In general, flotation units
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underperform when the influent has more than 500−1000
mg/L dispersed oil.19 Several studies have demonstrated that
lower initial oil concentrations lead to better oil removal
efficiency.81,98,105,108,109 It is also worth mentioning that, at
high oil concentrations, droplet−droplet coalescence can
become quite efficient and facilitate separation. Introducing
gas improves this process, because the attachment of droplets
to bubbles can both enhance the overall separation and lower
the separation times.
3.2.4. Gas Properties. Natural gas and nitrogen are most
widely used during gas flotation in PW treatment. The
attachment efficiency of two crude oils using methane and
nitrogen with and without dissolved components in the water
phase was studied.81 The results showed that, in the absence of
the dissolved components, the best performance was obtained
with methane.
When the dissolved compounds are present, however, the
attachment efficiency was better for the nitrogen system. This
was attributed to higher affinity of water-soluble components
to the methane bubbles, which reduced the attachment.
3.2.5. Temperature and Pressure. 3.2.5.1. Temperature.
Decreasing or increasing the temperature can influence
different factors, like density, viscosity, interfacial tensions,
solubility of gas and oil components, and dimensions of gas
bubbles. Raising the temperature decreases the viscosity and
density of all phases. The reduced water viscosity leads to
higher rising velocity of bubbles and droplets and increased
film thinning rates when bubbles and droplets approach.
Moreover, the coalescence frequency of oil droplets
increases.110,111 Altogether, these effects tend to enhance the
separation, and Radzuan et al.109 observed an increased oil
removal efficiency when operating at higher temperatures.
On the other hand, a rise of the temperature will also reduce
the oil−water interfacial tension.23 The solubility of oil
components in the water phase can increase, resulting in
more components adsorbing on the gas bubbles and reducing
the gas−water interfacial tension. These reductions will
facilitate breakup of droplets and bubbles and, thereby, reduce
the separation. Mândrea et al.112 studied the generation of gas
bubbles by orifices in a water column and showed that the
bubble diameter is directly proportional to the surface tension
of water. Sadeghi and Vissers100 showed that the increase of
the temperature slightly reduces the size of the bigger bubbles,
while it has no significant effect on smaller bubbles. The
reduction of bubble size with the temperature has also been
reported by other authors.113,114 Moreover, the increased
adsorption of dissolved components on gas bubbles can also
reduce the droplet−bubble attachment.11 Finally, considering
the CFU temperature application range, an increased temper-
ature can also reduce the solubility of gas in both oil and water
phases, which will reduce the possibility of using the DGF in
the treatment process.
3.2.5.2. Pressure. The effect of the pressure on the gas
flotation has not been widely investigated. However, it is
expected to influence the separation efficiency, because it can
alter densities, viscosities, interfacial properties, solubilities, and
the size of the bubbles and droplets. Increased pressure will
only slightly increase the oil−water interfacial tension.115,116
However, it has a major effect on the gas density, which leads
to a slower rise of the gas bubbles, and the longer retention
time will increase the probability of the encounter with oil
droplets.113,116 It has also been shown that increased pressure
leads to more breakage of nitrogen bubbles because of the
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increase in the gas density, which was attributed to larger
inertia of the gas in the fluctuating bubble.113 Also, the
coalescence time has been shown to increase with the pressure,
resulting in higher stability of the bubbles.117 The hydrostatic
pressure created by the liquid depth can also affect the size of
the gas bubbles and the frequency of bubble generation, and
increased bubble sizes have been demonstrated when bubbles
rise through the flotation column.18,100 Decreased frequency of
bubble generation by increasing the hydrostatic column
pressure was also observed.
4. CHALLENGES AND FUTURE RESEARCH
PERSPECTIVES
Nowadays, more attention is given to subsea production and
processing because oil reserves in easily accessible locations are
slowly running out, but also because it has several potential
advantages compared to topside processing.118−120
The development of subsea systems needs to meet the
design specifications and requires understanding of the oil
production process, the possible environmental risks, reservoir
flow, seabed conditions, costs, and performance require-
ments.22 Moreover, the design of subsea equipment introduces
several challenges, because installations are different from each
other in terms of reservoir fluid composition, sea depth,
pressure and flow, distance to shore, seabed topography, etc.
As mentioned previously, some subsea separators and
hydrocyclones are applied technologies, while subsea CFUs
are still in the development stage. The available subsea
hydrocyclones present turndown issues with low flow rates and
are additionally plagued by small reject orifices, susceptible to
blockage and requiring frequent backflush.42 In general,
minimal intervention and maintenance are vital for subsea
processes, and there is a need for alternative technologies.
In the literature, gas flotation at a high pressure has not been
thoroughly investigated; therefore, more research at relevant
process conditions is needed to understand the fundamental
mechanisms, effects of solids, production chemicals, and fluid
properties particularly in combination with a varying temper-
ature. Furthermore, because the high pressure seems to favor
bubble breakage, studies relating gas flotation performances
and gas bubble sizes would be of interest. The low surrounding
temperature in a subsurface environment is a challenge for the
subsea CFUs. The temperature at the subsea CFU may be
significantly lower than at the wellhead, depending upon the
distance between them. Temperature-maintaining measures,
such as direct electric heating and insulations, can be employed
but at the cost of both increased capital investment and system
complexity. These considerations are critical for designing a
cost-effective, robust subsea process system and, eventually,
can benefit the environment. This also includes optimized gas
injection methods and gas volumes needed for good flotation
efficiency at subsea operational conditions. When it comes to
structural requirements, subsea CFUs are expected to be larger
(with wider outer diameters) than the topside equipment as a
result of both increased internal and external pressure. This,
however, should not largely affect the separation process.
5. CONCLUSION
The volume of PW is expected to increase annually because of
the increasing number of oil fields and their extended lifetimes.
It is of extreme importance to have proper and efficient water
treatment processes to comply with the strict water discharging
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regulations. Gas flotation has proven to be a valuable technique
in the upstream petroleum processing and is a strong candidate
for subsea water treatment. It is firmly believed that a deep
understanding of the colloidal aspects involved in this process
is crucial to enhance the technology. In general, efficient
separation can be achieved by increasing the attachment
efficiency between bubbles and droplets and promoting
coalescence. Moreover, a deep understanding of the interfacial
phenomena involved in the process is crucial. Further
knowledge on how extreme conditions at the seabed affect
gas flotation is also needed to assess the possibility of applying
gas flotation for subsea PW treatment.
■
AUTHOR INFORMATION
Corresponding Author
Gisle Øye − Ugelstad Laboratory, Department of Chemical
Engineering, Norwegian University of Science and Technology
(NTNU), N-7491 Trondheim, Norway; orcid.org/0000-
0002-6391-3750; Email: gisle.oye@ntnu.no
Authors
Martina Piccioli − Ugelstad Laboratory, Department of
Chemical Engineering, Norwegian University of Science and
Technology (NTNU), N-7491 Trondheim, Norway;
orcid.org/0000-0001-9482-4745
Svein Viggo Aanesen − Equinor Research Centre, N-3905
Porsgrunn, Norway
He Zhao − Aker Solutions AS, N-1366 Lysaker, Norway
Marcin Dudek − Ugelstad Laboratory, Department of
Chemical Engineering, Norwegian University of Science and
Technology (NTNU), N-7491 Trondheim, Norway;
orcid.org/0000-0001-6444-7109
Complete contact information is available at:
https://pubs.acs.org/10.1021/acs.energyfuels.0c03262
Notes
The authors declare no competing financial interest.
Biographies
Martina Piccioli holds a master of science degree in chemical science
and technology from the University of Milano-Bicocca of Milan, Italy.
She is currently employed as a Ph.D. candidate at the Norwegian
University of Science and Technology. The project is focused on gas
flotation for subsea produced water treatment. Her key interests
include surface and colloid chemistry, phase separation, and water
treatment technologies.
Svein Viggo Aanesen holds a master of science degree in organic
geochemistry from the University of Tromso, Norway. He is currently
employed as a principle researcher in Equinor Research and
Technology. The main responsibility is technology qualifications of
both internally and externally developed technologies for water
treatment, with a special focus on produced water from oil and gas
fields. Key interests include the understanding of fundamental
mechanisms of water treatment technologies and water quality
analysis.
He Zhao holds a Ph.D. degree in the multiphase flow phenomena in
gas processing equipment from the Norwegian University of Science
and Technology. He is currently employed as a senior specialist
engineer in Subsea System and Product Engineering at Aker
Solutions. His main responsibilities are subsea process and boosting
system design, technology qualification, and R&D programs. His key
interests include bulk liquid−gas separation, water and gas treatment
technologies, and CO2-EOR.
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Marcin Dudek holds a Ph.D. degree in chemical engineering from the
Norwegian University of Science and Technology. After obtaining his
Ph.D. degree, he continues to work in Ugelstad Laboratory as a
postdoctoral researcher, studying the effect of production chemicals
on produced water treatment and crude oil production. His key
interests include produced water, colloidal and surface chemistry
(dispersion and emulsions), and microfluidics.
Gisle Øye received his M.Sc. and Ph.D. degrees within surface and
colloid chemistry at University of Bergen, Norway. In 2002, he started
at the Norwegian University of Science and Technology, where he
currently is professor and leader of Ugelstad Laboratory, the group of
surface, colloid, and polymer chemistry at the Department of
Chemical Engineering. His research interests include fundamental
interfacial phenomena, complex fluid characterization, separation, and
microfluidic methods. Although fundamental, the research is often
driven by industrial needs.
■
ACKNOWLEDGMENTS
This work was carried out as a part of SUBPRO, a Research-
Based Innovation Centre within Subsea Production and
Processing. The authors gratefully acknowledge the financial
support from SUBPRO, which is financed by the Research
Council of Norway, major industry partners, and NTNU.
■
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