Ultrasonics - Sonochemistry 57 (2019) 185–192

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Ultrasonics - Sonochemistry
journal homepage: www.elsevier.com/locate/ultson

Research on ultrasound-assisted demulsification/dehydration for crude oil T

a,1 b,1,⁎ c d e
Xianzhen Xu , Dan Cao , Jin Liu , Jun Gao , Xiaoyi Wang
a
College of Chemistry and Chemical Engineering, Shandong Sino-Japanese Center for Collaborative Research of Carbon Nanomaterials, Collaborative Innovation Center for
Marine Biomass Fiber Materials and Textiles, Laboratory of Fiber Materials and Modern Textile, Qingdao University, Qingdao 266071, China
b
College of Engineering, Ocean University of China, Qingdao 266100, China
c
Qingdao Geo-Engineering Surveying Institute, Qingdao 266071, China
d
College of Chemical and Environmental Engineering, Shandong University of Science and Technology, Qingdao 266590, China
e
Shanghai Ocean University, Shanghai 201306, China

A R T I C LE I N FO A B S T R A C T

Keywords: Crude oil demulsification and dehydration are important links in the process of crude oil exploitation, trans-
Ultrasound portation, and refining. In recent years, with the development of crude oil exploitation, the content of colloid and
Demulsification asphaltene in crude oil has been increasing, and the properties of crude oil emulsion have become more stable. In
Dehydration addition, the development and application of oil recovery technology and the use of a large number of oilfield
chemicals have made the composition of crude oil more complicated. The water content and salt content of oil
produced fluid increase year by year, which aggravates the task of crude oil dehydration and desalination.
Therefore, it is particularly important to study the demulsification and dehydration of crude oil. In this paper.
Research on ultrasound-assisted demulsification/dehydration for crude oil in investigated. Results indicate that
the demulsification effect varies with the increase of ultrasonic radiation time, but the difference is not sig-
nificant; with the increase of temperature, the effect of ultrasonic on the demulsification of crude oil emulsion is
decreased, or the advantages of ultrasonic can be fully displayed only at low temperature; ultrasonic power has a
critical value, when it is lower than this critical value, ultrasonic wave acts as demulsifying agent, and with the
increase of power, dehydration rate of the crude oil emulsion increases; when higher than the critical value, the
separated oil and water can be re-emulsified; ultrasonic demulsification can both shorten settling time and
reduce the amount of demulsifier; ultrasound is suitable for demulsification and dehydration of crude oil
emulsions with high water content. Results also prove that chemical demulsifier has a better effect for crude oil
demulsification /dehydration than that of ultrasonic treatment alone. In addition, recent progress on ultrasonic
demulsification equipment is introduced. The purpose of this paper is to offer equipment and technical support
for crude oil demulsification/ dehydration.

1. Introduction efficient response of the dispersed water phase to ultrasonic irradiation

to drive, coalesce, and segregate was similar to the behavior of sus-
Researches on chemical demulsification of waste oil have been pended particle [6], droplet [7], and bubbles [8,10] in sound field.
further developed in recent years. However, the dehydration process is As an easier, simpler and more efficient method, ultrasonic treat-
not ideal yet. In addition, chemical demulsifiers have poor adaptability ment has recently been used to separate water–oil emulsion in many
and may cause environmental pollution in the progress of water treat- works of literature [14,16,17,18,20,22,23,26,28,31]. These researches
ment [1]. Up to recently, ultrasonic irradiation was considered as an all indicate that ultrasonic treatment is a good method for crude oil
efficient method in desalting of heavy crude oil [2,3]. This method was demulsification/dehydration than a chemical agent from the viewpoint
first used in refinery oil dehydration by Yu et al. [4] to remove water in of environmental protection [5,9,15,21]. In a standing wave field, when
crude oil emulsion, which is mostly made by deliberate injection of ultrasonic irradiation is applied to water droplets in crude oil, at one
water into the crude oil in order to dissolve soluble salts especially NaCl time, the drops migrate toward the pressure nodes of the standing wave
[2]. Their experimental study on the influence of sound field para- field under the influence of the primary acoustic force. Since the density
meters on the water in crude oil emulsion behavior indicated that the of the droplet phase is more than that of the continuous phase (crude

⁎
Corresponding author.
E-mail address: [email protected] (D. Cao).
1
Co-first author on this work.

https://doi.org/10.1016/j.ultsonch.2019.05.024
Received 16 April 2019; Received in revised form 15 May 2019; Accepted 21 May 2019
Available online 22 May 2019
1350-4177/ © 2019 Elsevier B.V. All rights reserved.
X. Xu, et al. Ultrasonics - Sonochemistry 57 (2019) 185–192

oil), the net effect of gravity-buoyant forces will cause droplets to move
downward, in direction of gravity [12,25,29,34]. However, the lift
forces can be neglected when a droplet is falling in a stagnant fluid. The
magnitude of the above-mentioned body forces is much more than the
surface tension forces which resist the drops to move freely. Therefore,
the comparison of them derives an inequality which demonstrates the
relatively fast movement of drops to the collection plane
[13,33,34,37,38].
In this paper, the comparison of demulsifying and dehydrating
crude oil using natural sedimentation, ultrasonic irradiation, chemical
agent and sonochemistry method are investigated. The important con-
clusion can provide an important reference for on-site application of
sonochemistry demulsification/dehydration technique. In addition, re-
cent progress on ultrasonic demulsification/ dehydration equipment is
summarized.

Fig. 2. The structure of time-controlled stable power ultrasonic demulsification

2. Recent progress on ultrasonic demulsification equipment device 1-Ultrasonic power control cabinet, 2-ultrasonic transducer, 3-ultrasonic
cable, 4-tank, 5-crude oil imports, 6-sewage outfall, 7-inspection mouth, 8-
In view of the shortcomings of the existing ultrasonic demulsifica- crude oil exports.
tion technology, such as the small area of ultrasonic action, the in-
complete demulsification, and the secondary emulsification after
separate. If the ship's oily wastewater is not properly disposed of and
emulsification, etc., in 2013, Rui Hu invented an ultrasonic demulsifi-
discharged directly, it will cause pollution of the oceans and rivers. The
cation and dewatering device [39], its structure is as Fig. 1 shows.
decomposition of the oil produces toxic substances such as benzo and
Experimental results show that the emulsion can be emulsified more
other polycyclic aromatic hydrocarbons, which have a direct toxic ef-
fully, thereby improving the demulsification efficiency and reducing
fect on the organism. In order to solve the above problems, a device for
the side effect of the secondary emulsification of oil and water after
the treatment of marine oily wastewater by ultrasonic enhanced film
ultrasonic demulsification.
combined with photoelectric catalytic technology was invented by
In order to solve the problem exist in the current methods of de-
Linan Zhu et al. [41]. The diagram of the invented device is as Fig. 3
mulsification and heavy oil viscosity reduction, such as high cost and
shows. The oily wastewater of the ship enters the ultrasonic demulsi-
high energy consumption, difficulty in oil and water separation, a time-
fication device through the collection pipeline, then enters the mem-
controlled stable power ultrasonic demulsification device, shown in
brane filter device, and then enters the photoelectrocatalytic oxidation
Fig. 2, was invented by Weizhong Ding and Yueling Zhang in [40]. The
device. It will be discharged and reused when it's every index measured
device includes an ultrasonic power control cabinet, ultrasonic trans-
by the indicators meets the requirement. The invention has the ad-
ducer, an ultrasonic tank. The ultrasonic power control cabinet contains
vantages of simple and compact structure, small occupation area,
several ultrasonic power. Ultrasonic transducers are arranged in the
convenient use and operation, and management, and also realizes the
tank according to the design requirements, ensuring the efficient dis-
recycling of oil and the reuse of sewage treatment, thus achieving the
tribution of the ultrasonic waves in the tank. The invented device can
purpose of energy saving and emission reduction.
keep the required ultrasonic power in a stable state without any at-
Oil-bearing solid waste, known as oily sludge, will be produced in
tenuation due to the use of the time control technology to ensure that
oil extraction, transportation, refining, oily wastewater treatment, and
the demulsification dehydration or the heavy oil viscosity reduction is
tank cleaning. Oily sludge is a large and wide range of pollution
continuously effective; at the same time, it can greatly reduce the
sources, including pathogenic bacteria, parasites (eggs), heavy metals,
working failure rate of ultrasonic transducers, which can ensure the
salts, and PCBs, dioxins, radionuclides and other refractory toxic and
normal production of oil fields.
harmful substances. As oily sludge is a hazardous waste, it can cause
Ship sewage treatment is an important part of the field of ship
pollution to groundwater, surface water, atmosphere, and surrounding
pollution prevention and control. Marine oil contains many kinds of oil,
vegetation if it is discharged or piled up at will. Therefore, strict
including lubricating oil, cylinder oil, and hydraulic oil, cleaning agent,
management has been put into practice in all countries. In order to
blowing agent (AFFF), paint and Solvents. A portion of the oil in the
solve the above problem, equipment for oil sludge treatment was
oily wastewater of the ship is emulsified in water and difficult to

Fig. 1. The structure of an ultrasonic demulsifica-

tion and dewatering device 1-tank, 2-inlet port, 3-
oil distribution tube, 4-head, 5-first ultrasonic de-
mulsification chamber, 6-second ultrasonic de-
mulsification chamber, 7-first ultrasonic trans-
ducer, 8-second ultrasonic transducer, 9-out port,
10, 11, 12-outlet, 13-weir plate, 14- distribution
subsidence area, 15-crude oil demulsification zone,
16-oil–water separation zone, 17-separation of
water settling zone, 18-heater, 19-support plate,
21-demulsification chamber channel.

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X. Xu, et al. Ultrasonics - Sonochemistry 57 (2019) 185–192

Fig. 3. The diagram of A device for the treatment of

marine oily wastewater by ultrasonic enhanced film
combined with photoelectric catalytic technology
1-Grille, 2-ultrasonic demulsification device, 3-ul-
trasonic probe, 4-dosing device, 5-sewage outfall,
6-inclined plate structure, 8-Oil generator, 9-ex-
haust pipe, 10-membrane filter device, 11-modified
filter, 12-backwashing device, 13-photoelec-
trocatalytic oxidation device, 14-UV lamp, 15-
anode, 16-cathode, 17-aeration device, 18-detec-
tion device, 19-drain.

device for demulsifying the oily sludge, a centrifuge for the solid–liquid
separation of the oily sludge, and an ultrafiltration system for oil–water
separation of oily wastewater, and a sludge storage tank for storing oily
sludge, a mud tank for storing mud, a centrifugal reservoir for storing
oily effluent, for storing oil and the filtrate pool used to store moisture.
The invention has the advantages of novel design and reasonable rea-
lization, low cost, fast processing speed, thorough separation of oil,
mud, and water, and the invention can make the oil sludge be resource-
utilized, thereby reducing environmental pollution and waste of re-
sources [35].

3. Research on demulsifying and dehydrating crude oil using

ultrasonic irradiation, natural sedimentation, chemical agent and
sonochemistry method

On the basis of these experiments, the comparison of demulsifying

and dehydrating crude oil by ultrasonic wave, natural sedimentation,
demulsifier chemical and Sonochemistry method is further investigated
in this section. In order to make the experimental results more accord
with reality, SAGD watery crude oils (the freezing point is 67. 2 °C) is
selected as the oil sample to investigate which method is the best so-
lution for crude oil emulsification-dehydration.
Fig. 4. A schematic diagram of an oily sludge treatment system, an automatic
control cabinet, a power supply equipment and a fire fighting device arranged
3.1. Experimental apparatus and materials
in a vehicle-mounted oily sludge treatment box. oil storage tank 1 screw pump;
2-funnel, 3-mixer, 4-straight pump, 5-ultrasonic demulsification equipment, 6-
temperature control panel, 7-second in-line pump, 8-centrifuge, 9-mud pool, The main experimental apparatus are a high-speed mixer, stop-
10-centrifugal reservoir, 11-the first high pressure pump, 12-ultrafiltration watch, resistance heating furnace, densitometer, constant temperature
system, 13-thickener, 14-filtrate pool, 15-fire equipment, 16-controller, 17- waters, temperature controller, etc. High-speed mixer and temperature
power supply equipment. controller are shown in Figs. 5and 6 respectively.
The main experimental materials are SAGD watery crude oils shown
invented by Likun Zhou [42]. Fig. 4 is a schematic diagram of an oily in Fig. 7 and Type SP demulsifier (concentration is 250 mg/L).
sludge treatment system, an automatic control cabinet, a power supply
equipment and a fire fighting device arranged in a vehicle-mounted oily 3.2. Experimental procedures
sludge treatment box. The process of this invention includes the steps of
adding water, stirring, diluting, ultrasonic demulsification, solid–liquid (1) Heat the constant temperature water to the required temperature.
separation, and oil–water separation. The equipment includes an oil (2) Add the SP demulsifier to the prepared SAGD watery crude oil and
sludge treatment system, an automatic control system and a power stir the mixture of crude oil and demulsifier using a high-speed
supply device. The oily sludge treatment system comprises an agitator mixer.
for diluting the oily sludge with water, an ultrasonic demulsification (3) Process the mixed sample using the ultrasonic transducer.

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X. Xu, et al. Ultrasonics - Sonochemistry 57 (2019) 185–192

Fig. 8. The comparison chart of chemical agent demulsification/dehydration

and sonochemistry demulsification/dehydration at 40 °C.

(4) When the dewatering amount does not appear to add up, record the
total volumes of the dehydrated water and the whole mixed sample.

Fig.5. High-speed mixer. 3.3. Experimental results and discussion

3.3.1. The comparison of demulsifying and dehydrating crude oil using a

chemical agent and sonochemistry method respectively
Experiments of demulsifying and dehydrating crude oil using a
chemical agent and sonochemistry method respectively at different
temperatures are carried out. Results are shown in Figs. 8, 9 and 10
respectively. φw is dehydration rate.
In the above three figures, ultrasonic powers and the concentration
of chemical agents are all treatment 100 W and 250 mg/L respectively.
As can be seen in Figs. 8–10, sonochemistry method has a better effect
Fig. 6. Temperature controller. for crude oil demulsification/dehydration than that of using chemical
agent alone. The gap between the two effects has narrowed as the
temperature grows. However, the effect of sonochemistry method be-
comes better than that of chemical agent method with the increasing of
treatment duration.
Due to the poor flowability of heavy crude oil, chemical demulsifier
cannot be fully dispersible in the emulsion so that the good effect of
demulsification/ dehydration cannot be achieved. However, the mixed
role of ultrasonic wave and chemical demulsifier can produce syner-
getic effects: ultrasonic wave itself can demulsify and dehydrate crude
oil, meanwhile, chemical demulsifier can be adequately dispersed
under ultrasonic treatment so that chemical demulsify- cation/dehy-
dration can be fully promoted.

Fig. 7. SAGD watery crude oil.

Fig. 9. The comparison chart of chemical agent demulsification/dehydration

and sonochemistry demulsification/dehydration at 60 °C.

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Fig. 10. The comparison chart of chemical agent demulsification/dehydration Fig. 13. The comparison chart of ultrasonic demulsification/dehydration and
and sonochemistry demulsification/dehydration at 70 °C. sonochemistry demulsification/dehydration at 40 °C.

indicate that sonochemistry method is significantly better than natural

sedimentation for crude oil demulsification/ dehydration.
For sonochemistry method, on the one hand, chemical demulsifier
itself has the function of demulsification/dehydration; on the other
hand, in a standing wave field, when ultrasonic irradiation is applied to
water droplets in crude oil, at one time, the drops migrate toward the
pressure nodes of the standing wave field under the influence of the
primary acoustic force [4,23]. Since the density of the droplet phase is
more than that of the continuous phase (crude oil), the net effect of
gravity-buoyant forces will cause droplets to move downward in the
direction of gravity [2]. Synergetic effect of these two methods can
effectively improve dewatering ratio. Natural sedimentation demulsi-
fication/dehydration is, in fact, a time-consuming process and has no
good dehydration effect. That is why sonochemistry method is sig-
nificantly better than the natural sedimentation method for crude oil
Fig. 11. The comparison chart of natural sedimentation demulsification/de- demulsification/dehydration.
hydration and sonochemistry demulsification/dehydration at 40 °C.

3.3.3. The comparison of demulsifying and dehydrating crude oil using

ultrasonic treatment and sonochemistry method
Experiments of demulsifying and dehydrating crude oil using ul-
trasonic and sonochemistry method under different temperatures
(40 °C, 50 °C, 60 °C and 70 °C) are carried out. Results are shown in
Figs. 13, 14, 15 and 16 respectively.
As can be seen in the above Figures, the gap between these two
effects of crude oil demulsification/dehydration using ultrasonic treat-
ment and sonochemistry method has narrowed as the temperature
grows; sonochemistry method can shorten dehydration time. In a word,
sonochemistry method has a better effect for crude oil demulsification/
dehydration than that of ultrasonic treatment alone

Fig. 12. The comparison chart of natural sedimentation demulsification-dehy-

dration and sonochemistry demulsification-dehydration at 50 °C.

3.3.2. The comparison of demulsifying and dehydrating crude oil using

natural sedimentation and sonochemistry method
Experiments of demulsifying and dehydrating crude oil using nat-
ural sedimentation and sonochemistry method under different tem-
peratures (40 °C and 50 °C) are carried out. Results are shown in
Figs. 11 and 12 respectively.
As can be seen in Fig. 11, the maximum dehydration rate using
natural sedimentation is only 1.8%, while the maximum dehydration
rate using sonochemistry method can reach up to 18.01%. As can be
seen in Fig. 12, the maximum dehydration rate using natural sedi-
mentation is only 2.5%, while the maximum dehydration rate using
Fig. 14. The comparison chart of ultrasonic demulsification/dehydration and
sonochemistry method can reach up to 48.22%. The above two figures
sonochemistry Demulsification/dehydration at 50 °C.

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oil emulsion become abnormal and complex, and the structure can’t be
destroyed by simple ultrasonic wave and good demulsification effect
cannot be achieved only by ultrasonic treatment alone. He combined
the action of ultrasonic and demulsifier cannot only exert the respective
roles of ultrasonic and demulsifier but also can make the demulsifier
better dispersed in the crude oil emulsion and promote the further
exertion of demulsifier to achieve better demulsification effect [19].
Under the condition of 75 °C and 10 h of ultrasonic radiation, re-
search results indicate that the dehydration rate of the crude oil
emulsion gradually increases with the increase of ultrasonic power, and
the change tends to be gentle. When the power is increased to 100 W,
the dehydration rate of the crude oil emulsion reaches the maximum.
With the increase of power, the dehydration rate of the crude oil
emulsion gradually began to decrease. And from the quality of the re-
Fig. 15. The comparison chart of ultrasonic demulsification/dehydration and moved water, with the increase of ultrasonic power, the water released
sonochemistry Demulsification/dehydration at 60 °C. from the clear and transparent becomes cloudy, which indicates that
the removal of water contains a certain amount of oil.
The results show that the ultrasonic power is not as big as possible
but have critical value. When ultrasonic power is lower than this critical
value, ultrasonic wave acts as a demulsifying agent, and with the in-
crease of power, the dehydration rate of the crude oil emulsion in-
creases. When the ultrasonic power is higher than the critical value, the
ultrasonic wave will emulsify, and the separated oil and water can be
re-emulsified, thus reducing the dehydration rate of the crude oil
emulsion [24,27].
This is because, in general, to make the water particle start from the
static state relative to the oil movement, a certain sound radiation force
must be applied, and the sound intensity at this time is called the lower
critical sound intensity, and the power at this time is called the lower
critical power. Only when the critical power is lower than the critical
sound intensity, can the water particles start to accelerate the motion
and collision and condense with each other, thus separating the oil from
Fig. 16. The comparison chart of ultrasonic demulsification/dehydration and the oil. When the sound intensity exceeds a certain value, the water
sonochemistry demulsification/dehydration at 70 °C. particles move violently and collide with the surrounding oil particles
continuously. The agglomerated water particles are redispersed, which
4. Discussion on influence factors for sonochemistry in turn leads to mixing, new emulsification, and reduced demulsifica-
demulsification/dehydration tion. The sound intensity at this time is called upper critical sound in-
tensity, also called cavitation threshold, and the corresponding power is
Research results indicate that the demulsification and dehydration called upper critical power [32].
process of crude oil emulsion at different ultrasonic radiation time will Therefore, the ultrasonic demulsification power must be between
be stable after 300 min. This shows that ultrasonic radiation has a the upper and the lower critical power, and preferably near the upper
significant effect on the demulsification of crude oil emulsion, and the critical power. The demulsification effect at this time is the best.
ultrasonic method can reduce the demulsification temperature. It can When the ultrasonic radiation time is 10 min at 75 °C, research re-
also be seen from the diagram that the demulsification effect varies sults indicate that the final dehydration rate of crude oil emulsion with
with the increase of ultrasonic radiation time, but the difference is not 50 mg/L demulsifier dosage is the highest, and the final dehydration
significant. The final dehydration rate of ultrasonic demulsification is rate of crude oil emulsion with the demulsifier dosage of 25 mg/L,
about 79%. 100 mg/L, and 150 mg/L decreases in turn. This shows that ultrasonic
Research results indicate that the graph that the demulsification and demulsification can both shorten settling time and reduce the amount
dehydration process of crude oil emulsion at different ultrasonic ra- of emulsifier.
diation time will be stable after 200 min. The experimental results show Under the condition of 75 °C and ultrasonic irradiation time of
that with the increase of temperature, the effect of ultrasonic on the 10 min, research results indicate that with the increase of settling time,
demulsification of crude oil emulsion is decreased, or the advantages of the demulsification effect of crude oil emulsion with different water
ultrasonic can be fully displayed only at low temperature. The final content is quite different; both the initial demulsification rate and the
dehydration rate is up to 96%. final dehydration rate of crude oil emulsions increase with the increase
Research results indicate that for crude oil emulsions without of water content; the equilibrium time of demulsification dehydration
emulsions, both the initial demulsification rate and the final dehydra- process decreases with the increase of water content [30].
tion rate are much lower than those of crude oil emulsions with de- The results show that ultrasound is suitable for demulsification and
mulsifiers added and the time during which the emulsion dehydration dehydration of crude oil emulsion with high water content. This is
process tends to be stable is also long much longer. This indicates that explained by the fact that, under ultrasonic radiation, small water
the ultrasonic action alone cannot achieve the ideal demulsification droplets collide with each other and coalesce into relatively large water
effect. Only when combined with demulsifier can be the best demulsi- droplets. Water droplets subsequently collide and adhere to each other
fication effect be achieved [5,11]. to form large water droplets and settle under gravity. It takes a time
In the middle and late period of oil field exploitation, in order to process to separate oil from the oil. There are a large number of water
increase the production of crude oil, various oil displacement agents droplets in the crude oil emulsion with high water content. In the same
have been added into the crude oil, which makes the structure of crude time, water droplets are easier to coalesce to form large water droplets
and then to separate from oil emulsion with low water content.

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