Microbubble Generation

William B Zimmerman1*, Vclav Tesa 2, Simon Butler1, HC Hemaka Bandulasena1

Department of Chemical and Process Engineering, University of Sheffield, Mappin
Street, Sheffield S1 3JD, United Kingdom
2
Institute of Thermomechanics, Academy of Sciences of the Czech Republic, Prague,
Czech Republic.
*
Corresponding author. Email: [email protected]
1

Abstract
In general, there are three ways of generating microbubbles. The most common class
uses compression of the air stream to dissolve air into liquid, which is subsequently
released through a specially designed nozzle system, to nucleate small bubbles as
potentially nanobubbles, based on the cavitation principle.
These bubbles
subsequently grow into much larger bubbles through the rapid dissolution of the
supersaturated liquid. The second class uses power ultrasound to induce cavitation
locally at points of extreme rarefaction in the standing ultrasonic waves. The third
class uses an air stream delivered under low offset pressure, and airs to break off the
bubbles due to an additional feature, whether it be mechanical vibration, or flow
focussing, or fluidic oscillation. Conventional air diffusers rely on the structure of
porous material for the nozzles to generate small bubbles, but fluidic oscillation in
general promises to break off the forming bubble while it is still a hemispherical cap
the smallest shape for which bubble formation from a pore is likely to occur given the
strong adverse affect of surface tension at higher curvatures. The first two classes of
microbubble generation are usually associated with high power densities and power
consumption by either the compression or ultrasonic treatment. The third class should
have the lowest power consumption, provided it achieves the application targets of
bubble size distribution, air phase holdup, and bubble dispersion. In this paper, recent
patents in microbubble generation are categorized into the first and the third classes
above. The subject area is reviewed for its importance in several fields of application,
particularly generalized flotation processes and bioreactor treatments.

1. Introduction
1.1 The challenge of small bubble generation.
Naively, one would expect that when blowing small bubbles through an aperture,
making the aperture as small as possible would be sufficient for generating bubbles
correspondingly small . But there are a number of reasons why this does not suffice.
For instance, when a bubble is formed from a single aperture, the liquid attached to
the perimeter of the aperture serves as an anchor as the wetting force attaches the
growing bubble to the solid surface. Unless this anchoring force is disrupted, the
bubble will grow until the buoyant force on the bubble (which is proportional to its
volume) exceeds the anchoring restraint on the bubble (typically proportional to its
contact perimeter), and therefore breaks off. In this low pressure offset scenario, the
force balance usually breaks off the bubble at a size an order of magnitude larger than
the diameter of the aperture. Furthermore, the wetting properties of the solid surface
are extremely important. Should the bubble contact the surface over a larger region

than the aperture perimeter, if the solid surface is hydrophobic, the gas phase of the
growing bubble will form a second anchor force with the solid surface over a wider
area, increasing the buoyant force and thus bubble volume required to overcome it. If
the surface is hydrophilic, then this attractive force is absent.
A second reason for forming larger bubbles from small apertures is polydispersity of
bubble sizes and irregularity of the spacing between bubbles leading to quick
coalescence of the bubble cloud. Even if small bubbles are formed, then coalescence
can rapidly reduce the benefit.
The third reason for not forming small bubbles from small apertures is channelling in
a nozzle bank of pores or through a porous ceramic material. This is described in
Figure 1. The largest bubble that forms then provides the path of least resistance,
preferentially growing against all other bubbles in the parallel percolation process in a
nozzle bank or porous ceramic material.

(a)

(b)

Figure 1 Instability of parallel percolation. (a) If one of the bubbles increases beyond the
hemispherical shape, its growth becomes easier: air entering overcomes a lower pressure difference
P. It grows at the expense of the other bubbles. (b) The basic reason: Young-Laplace surface tension
law. Pressure difference across the air/water surface is inversely proportional to the curvature radius r.

Given these difficulties of forming small bubbles from air flow through a nozzle or
nozzle bank, high power density techniques have been developed. In general, there
are three ways of generating microbubbles. The most common class uses
compression of the air to dissolve air into liquid, which is subsequently released
through a specially designed nozzle system, to nucleate small bubbles as potentially
nanobubbles, based on the cavitation principle. These bubbles subsequently grow
into much larger bubbles through the rapid dissolution of the supersaturated liquid.
The second class uses power ultrasound to induce cavitation locally at points of
extreme rarefaction in the standing ultrasonic waves.
The third class uses an air stream delivered under low offset pressure, and aims to
break off the bubbles due to an additional feature, whether it be mechanical vibration,
or flow focussing, or fluidic oscillation. Conventional air diffusers rely, fruitlessly,
due to the instability described in Figure 1, on the structure of porous material used
for the nozzles to generate small bubbles, but fluidic oscillation in general promises to
break off the forming bubble while it is still a hemispherical cap the smallest shape
for which bubble formation from a pore is likely to occur given the strong adverse
affect of surface tension at higher curvatures. The first two classes of microbubble
generation are usually associated with high power densities and power consumption
by either the compression or ultrasonic treatment. The third class should have the
lowest power consumption, provided it achieves the application targets of bubble size

distribution, air phase holdup, and bubble dispersion. In this paper, we review recent
patents in microbubble generation, giving substantial exposition to a new technique
for generating microbubbles with low power density just offset pressure linked
with fluidic oscillation to overcome the three major difficulties highlighted above
creating bubbles of the scale of the aperture diameter, rather than an order of
magnitude higher.
1.2 The benefit of microbubbles.
In many instances, miniaturization is sought for the purposes of convenience
smaller devices are more portable, or require fewer uses of resources. Why would
microbubbles be a benefit? In the case of consumer products which use
microbubbles, it might be the texture of the product (frequently a foam) is perceived
better; possibly the processing of microfoams is better with lower viscosity or better
rheological features. Separations processes such as for minerals or biotech materials
might be enhanced, or for the flotation or air-lift of wastes or oil recovery. A
common thread among the benefits of microbubbles is in their transport behaviour
mass, momentum, and heat transport at the interface of microbubbles is influenced by
the interfacial surface area. Figure 2 depicts the key feature of high surface area to
volume ratio.

(a)

(b)

(c)

Figure 2. The transfer benefit of microbubble generation. (a) Division of a volume into n smaller,
equally sized objects, productes additional surface area that scales with the cube root of the dividing
number. (b) For a single bubble, the surface area and transfer rate scale as the square of the bubble size
l, but bubble volume scales with its cube. (c) Therefore, the total transfer rate with the number of
bubble adjusted to keep the air phase volume constant, scales inversely with the bubble size l smaller
bubbles lead to greater transfer.

The argument given in Figure 2 for the benefit in transfer efficiency is typified by the
common chemical engineering phenomenological description of interphase mass
transfer flux J (moles per second):
(1)
J = K l a ( cg cl )
where Kl is the mass transfer coefficient (units of velocity), a is the interfacial area,
and cg and cl are molar concentrations. There is a direct analogy to heat transfer flux
Q where the roles of the concentrations are played by temperature, i.e. Newtons Law
of Cooling. What is not so intuitive, however, is that there is a similar transfer effect
for momentum, where the role of J is taken by the force F in the vertical direction
induced by velocity changes in the horizontal direction, which follows from Newtons
law of viscosity:
w
F = a
(2)
x
The interpretation of equation (2) is that the momentum transfer by a cloud of rising
bubbles increases with the surface area of the cloud dragging more of the ambient
liquid with it than a larger bubble with less surface area. This feature opposes the
more intuitive feature that smaller bubbles rise less quickly than a single larger bubble
that matches its volume. The rise velocity is a linear effect with bubble size as shown
in Figure 3.

Figure 3. The rise velocity of bubbles as shown theoretically (Levich) and experimentally. As transfer
rates are shown to increase inversely proportionally to bubble size, but the velocity difference rises
proportionally to bubble size, one would expect momentum transfer by the cloud of bubbles to be
relatively constant. The total amount of momentum transferred, however, should be larger by the
smaller bubbles due to the finite height of the liquid layer. The slope of the above graph shows that
bubbles three fold smaller stay in the liquid ten fold longer, thus having longer time to transfer the
same momentum rate.

The stirring effect by a rising cloud of small bubbles, according to Figure 2,

exceeds that of the passage of a single larger bubble if nonlinearity is neglected
(Stokes regime).
The canonical chemical engineering application for such
microbubble dispersal is called surface aeration, frequently the most important
process in bioreactors and fermentors (see Grammatika and Zimmerman, 1999).

The paper is organized as follows. In section 2, the two classes of high power
consumption formation of microbubbles compression followed by release, and
power ultrasound are discussed, with an eye to the high value added products from
the processes that utilize microbubbles. In section 3, the third class of low power
consumption microbubble generation is discussed. In recent patents, this class has
included the use of porous materials, flow focussing, and fluidic oscillation actuated
microbubble generation. In section 4, speculations about current and future trends are
discussed, particularly with regard to the future promise of miniaturization and power
efficiency.

2. Applications and high power nucleation of microbubbles.

Applications of small bubbles

As the Introduction made clear the generic benefits of microbubbles for transfer
processes, one of the key application areas for microbubbles are generalized flotation
processes (see e.g. Grammatika and Zimmerman, 2001) for which microbubbles
collect on larger particle, forming a floc which is lense dense than the surrounding
fluid, thus rising due to buoyancy. The larger particle may be a solid waste or an oil
droplet in the common application area of dissolved air flotation.
Generating small bubbles is important in many industrial applications. Low density
particulates are separated from potable water and wastewaters by small bubbles
produced by either dissolved air flotation or dispersed air flotation. Also biological
treatment of wastewater requires aeration systems with high oxygen transfer
efficiencies. Electroflotation is commonly used in mineral industry to separate fine
particles from solutions and oil industry to separate oil-water emulsions. In adsorbing
colloid flotation, heavy metals are removed by fine microbubbles. In yeast industry,
bio mass production mainly depends of oxygen transfer efficiency of the aeration
system. In the production process of some biopharmaceutical products, bioreactors
require fine bubble aeration systems.
For biomolecular separations, very small microbubbles, termed aphrons, have shown
particularly useful extraction properties. Lye and Stuckey (2001), for instance, report
large mass transfer coefficients in the extraction of erythromycin using colloidal
liquid aphrons, an emerging technique for the recovery of microbial secondary
metabolites, such as antibiotics in pre-dispersed solvent extraction (PDSE) processes.
More typically, microbubbles at the micron scale form colloidal gas aphrons are used
for gas phase extraction, such as for lactoferrin and lactoperoxidase from sweet whey
(Fuda et al. 2004). Protein separations are typically by interfacial affinity, rather than
phase transfer. For instance, Noble et al. (1998) showed that protein affinity to foams
was largely chemical interactions, but to gas aphrons, electrostatic and hydrophobic
interactions dominated. Oil recovery could benefit from gas-lift technology if
sufficiently small microbubbles can be generated in situ downhole (Guet and Ooms
2006), driving such innovations as new pump cavitation mechanisms (Samuel and
Saveth, 2006).
Burns et al.(1997) compared three common bubble generation mechanisms namely ,
DAF, electroflotation and air spraying, for bubble size and surface area produced per
time as a function of power input to the system. The study revealed that DAF
produced the narrowest bubble size distribution with largest average bubble size, but
promised highest surface area/unit time/power compared to other two methods. Also

DAF experiments showed slight improvement of bubble size with increasing pressure
requiring 60-90 psi to produce 46 to 57.5 m bubbles.
Makuta et al. (2006) reported an ultrasonic method to produce microbubbles of
uniform diameter from 4 to 15 m at a constant periodic rate. A bubble protruded at
the tip of a needle was oscillated by ultrasonic waves and projections were formed by
the surface waves to give a continuous stream of tiny bubbles. The stability of bubble
generation was limited by the gas viscosity to approximately 20.0 Pa s in a highly
viscous liquid of kinematic viscosity between 5 and 100mm2 s1 and surface tension
between 20 and 34 mNm1.
In all these generalized flotation processes, the high value added of the substance,
typically an economically viable product, to be separated justifies the use of high
power techniques to generate microbubbles. But given that high power is required to
generate microbubbles with conventional techniques of nucleation from compression
or power ultrasound, all of the processes mentioned above would benefit from
inventions and innovations that are energy efficient, while still achieving target
bubble sizes and hold-ups.
Several recent patents fall into this category of using high power compression effects
to dissolve air and then, upon releasing the pressure, nucleating or otherwise creating
small bubbles. For example, In US20070108640, Takahashi et al. (2007) claim a
device which first dissolves air under pressure and then draws, using suction through
a mixer unit, the dissolved air enriched water and a stream of air, using a nozzle and a
bubble generating cartridge. The key feature of this is that the dissolved air enriched
water stream becomes supersaturated and requires less pressurization overall in
creating microbubbles. This patent is specific for a hair-washing unit, and therefore
can be termed a process patent the fundamental mechanisms may well have been
known already in, say, wastewater treatment, but then have never been applied, in
such an embodiment, for a hair washing system.
In US20070119987, Vion (2007) demonstrates a three staged compression system
with a prerelease stage with modest decompression, a nozzle release stage, and a
transition chambre which brings the pressure to saturation, before a final outlet tube
which confines cavitation and limits the reattachment to the tube walls, thus opposing
initial coalescence. By staging the releases, this technology should reduce the initial
compression required so that energy costs for supersaturation of the dissolved air are
minimized. This is a promising technology for retrofitting existing dissolved air
flotation plant for separating solids and immiscible oily effluent.
In US7199085, Rea et al. (2007) do not claim, per se, a microbubble generation
methodology, but rather a recipe for creating a colloidal liquid and gas aphron
composite fluid which has a long enough shelf-life to be pumped downhole, which
in particular is valued for its thixotropic rheological properties. Given our discussion
at the beginning of this section of the value of microbubbles for enhanced oil
recovery, one possible delivery method would be through a sufficiently stabilized
composite liquid with colloidal emulsion and or aphron constituents which would
release the microbubbles as the complex liquid stability fails in the oil sands. This

latter claim is not made in the patent, but rather it does not limit the range of
downhole activities for which such a complex fluid could be applied.
In US7214508, Hucklenbroich and Mueller (2007) do not actually claim a
microbubble generation technique. They describe a technique for cell lysate coarse
level separation that involves compression of the lysate which forms flocs, and then
decompression which results in a coarse phase separation between the flocs and a
lower, clear liquid layer. This clarification technique appears rapid, and it is difficult
to imagine that the compression-decompression cycle does not nucleate microbubbles
that integrate into the organic material flocs, thus improving the buoyancy difference
between the floc and clear liquid phases. Analysis suggests that this separation is a
microbubble mediated flotation process.
In WO/2007/068446: Eichler et al. (2007) describe an integrated biogas production
and separation process, where the biogas generated is combined with the process
liquid in a microbubble generation stage to use the biogas enriched bubbles in a
recycle stage to separate the biodegradable material, by flotation, from which it was
formed. As the major idea of this patent is process integration simultaneous use of
the product in its own processing it is not necessary to specify any novel
microbubble generation scheme to achieve this. Consequently, one would expect that
in the first instance, implementation has been done with convention compression
methods for dissolved gas flotation.

3. Low power microfluidic microbubble generation.

In this section, three low power methods of generating microbubbles are discussed.
In general, the use of porous ceramic materials or slits in membranes is common in
aeration used in wastewater treatment. Flow focussing, particularly in microdroplet
formation, is known as a route to create microbubbles/microfoams as well. Finally,
fluidic oscillation has recently been demonstrated as a methodology for producing
microbubbles. All three methods of these methods are implemented by geometric
features with characteristic dimensions on the microscale. The latter two are likely to
be engineered microfluidic devices (see Zimmerman, 2005), whereas the random
porous nature of porous materials is likely to be a property of the material for which it
was selected.
Porous materials.
In US20070114176, Yamasaki et al. (2007) introduce a porous wood charcoal
material prior to a diaphragm in a diffuser system, which has the interesting
biochemical property of activating microorganisms on the wood charcoal which
digest wastewater faster. In this case, the micro/nano bubble generation mechanism is
subsidiary to the microorganism activation as the economic driver. If the sole goal
were microbubble generation, then porous materials generally suffer from the
difficulties discussed in the Introduction. However, porous materials do create a
range of bubble sizes, with sufficiently high population of the microbubble regime to
achieve the desired activation of the microorganisms for digestion.
Flow focussing.
In US20070114183: Lee and Muir (2007) focus on the use of microbubbles in
separating dispersions of immiscible liquids, such as oil and water, which is
conventionally done by dissolved air flotation with high power usage, but is done with
low power usage by clarification tanks (lowest) or by structured packings or parallel
plate packs, without the use of microbubbles. Combining the use of interesting
internal contacting patterns in their vessel to help induce buoyant segregation and
microbubble dispersal, with microbubbles generated by flow focussing, this patent
ingeniously joins the major features of the two extreme conventional techniques (high
energy dissolved air flotation and low energy parallel plate packs) to achieve a low
energy and relatively quick, active separation.
In US20070095937, Noguchi and Chuang (2007) demonstrate a series of devices
which use restrictions in flow, partitions in flow, flanges, and entrainment of air from
recesses in the walls to generate microbubbles laden fluid, which are then launched
against bouncing surfaces. They claim particular configurations, which achieve the
microbubble formulation. Flow focussing in general is know for foam (microbubbles)
and dispersion (microdroplet) generation (see Lorenceau et al. 2006), but any
particular configuration and process for which flow focussing has not yet been shown
to generate dispersions of microbubbles or microdroplets is fair game for a process
patent based on novel usage.
Fluidic oscillation.
Prior art in microbubble generation included a number of systems that cause
mechanical vibration oscillating of solid bodies and their surfaces but to our
knowledge, only in UK0621561, Tesa and Zimmerman (2006), it is the air that is
oscillated, particularly by its taking a completely different spatial path to alternative

exit nozzles. The device performing the vibration of the air flow is a fluidic oscillator
(or a bank of oscillators). It handles a continuous flow input, switching it into one of
two output channels with a regular frequency. Typically, oscillator is a no-moving
part amplifier based on the Coanda effect (see Tesa , 2007), Fig. 4a, provided with a
feedback loop. Although in UK0621561, Tesa and Zimmerman (2006) claim not to
be limited to any particular implementation of a fluidic oscillator as a methodology
for actuating microbubble formation from a hemispherical cap formed from an
aperture or nozzle bank, the oscillator of Tesa et al. (2006), Fig. 4b, was used in
demonstrator experiments for applications to wastewater treatment (Hu 2006), yeast
growth (Zhang, 2007), and oil recovery (Varma, 2007).

(a)
(b)

(c)

Figure 4. Fluidic oscillator used in experiments. (a) The amplifier made as cavities in a stack of laser
cut Perspex plates (b) In an oscillator, the feedback loop connects the two control terminals of the
amplifier. The pressure difference between them generates the flow in the loop than causes the main air
flow from the supply terminal to switch from one Coanda-effect attachment wall to the opposite one.
This is repeated periodically at 1-100Hz depending on the length of the feedback loop. (c) Flow rate
time history for the fluidic oscillator connected to a parallel percolation nozzle bank with apertures of
600 diameter. The bubble growth is limited by the duration of the oscillation pulse. Growth stops
while all generated bubbles are still smaller than the hemispherical stability limit (see Figure 1).

This fluidic oscillator was connected to two identical parallel percolation nozzle
banks, with fixed size apertures, Fig. 5a. One set of nozzle banks was used for
aeration tests to find the oxygen transfer efficiency with apertures of 600 micron
diameter (Hu, 2006). Oscillation, with careful selection of the materials for
construction to avoid strong hydrophobic forces anchoring bubbles, and selection of
the orientation with flow, lead to generation of small bubbles and order. Specific
measures were necessary to ensure forced separation of the not yet mature, small
bubbles from the percolation orifices. One layout, Fig. 5b achieves the separation by
the action of water pulses synchronised with the air pulsation. Another layout, Fig. 5c,
uses alternating liquid and air columns moving in a reciprocating manner in the
manifold.

(a)

(b)

(c)

Figure 5. Microbubble generation from nozzle banks with fluidic oscillation. (a) Artists conception of
the dual outlet bank feed by a single fluidic oscillator. (b) Image of fine mist microbubbles generated
by opposing nozzle banks for air and water flow. The air pulse separates the bubbles that would
otherwise relain attached to the exit apertures (c) Slower operation in oil with air microbubbles
generated. In this configuration, the air is injected into the manifold leading to the nozzles and its
pulsation leads to alternating filling the nozzle with air and liquid. Clearly shown is the fact that the
microbubbles are generated with even spacing. Hydrodynamics of viscous flow ensures that the
column of uniformly spaced, monodisperse rising air bubbles is stable in its rise rate no bubble
overtakes its predecessor and thus the cloud is non-coalescent in theory (Crabtree and Bridgewater,
1969). In practise, this approximation appears to hold well in (b).

The 600 micron nozzle bank showed the formation of nearly mono-dispersed,
uniformly well spaced clouds of microbubbles, nearly all submillimetre size. Oxygen
transfer efficiency rates were shown to be 8-fold higher with the fluidic oscillator
operating than without (Hu, 2006). A subsequent study found that yeast cultures had
exponential growth rates at least 20% higher with the fluidic oscillation than without
(Zhang, 2007). Implementation of nozzle banks in microchips with oriented outlets of
60 micron diameter also demonstrated bubble clouds with sizes of the scale of the
aperture diameter when actuated by air flow through the fluidic oscillator with a range
of offset pressures from 0.1 to 1.5 bar, but approximately 8-fold larger without the
fluidic oscillation (Varma, 2007). The latter result suggests that high hold-ups can be
achieved given the slow rise time of the microbubbles and low coalescence rates, with
the potential for low power dissipation.

4. Current and future developments

Microbubble generation is a hot topic, but it is possible that the future applications are
even smaller. Cameron (2005) reports in the trade press about the development of
nanobubble generation in the labs of Masatoshi Takahashi at the Institute for
Environmental Management Technology at the National Institute of Advanced
Industrial Science and Technology (AIST). Takahashis 200 nanometer diameter
bubbles have been reported to have no propensity to rise and are stable for months,
having been formed by a process involves physical stimulation leading to violent
adiabatic collapse. Insufficient information has yet been revealed for primary
disclosure to validate the claims, which, however, are striking concerning the possible
metabolic and medical uses of nanobubbles, which carry more of the advantages with
regards to transfer efficiency than microbubbles, but potentially others as well.
Nanoparticles are supposedly highly reactive, which suggests that nanobubbles will
make for excellent interfacial reactions in heterogeneous catalysis. Mass transfer will
be dominated by interfacial interactions, which are different with different chemical
species. Deshpande and Zimmerman (2005) have already demonstrated that such
asymmetry in mass transfer kinetics can be exploited in optimizing heterogeneous
chemical reactors.
In this review, we categorized microbubble generators into high power consumption
processes which are tolerated by the value of the product produced, and low power
consumption approaches that attempt to generate microbubbles using little more than
the offset pressure driving the air flow to form the microbubbles. Given the economic
drivers in industries using high power consumption, the current trends in patents are
to incrementally cut the usage of power with improved designs and design concepts.
The major challenge is to shift from high power consumption regimes to low power
consumption methodologies without sacrificing the desired microbubble size and
distribution through coalescence or channelling instabilities. Fluidic oscillation is one
approach that promises minimal power losses and low power consumption with
desirable bubble size properties and nearly uniform spacing to oppose coalescence.
The approach is not yet sufficiently characterized to know if the concept will work
with all types of nozzles used in microbubble formation, whether it scales up to large
sparging requirements of fermentors and bioreactors, or scales down to microfluidic

bioreactors, as the combination of oscillation frequencies and flow rates must be

sufficient to limit the bubble growth to the hemispherical cap and to interact
favourably with mechanisms to detach the hemispherical cap semi-formed bubble by
overcoming the anchoring force subcritical buoyancy. These studies, as well as
potential application areas, are underway.
Many of these questions must simply be answered by experimentation. Multiphase
flow and interfacial phenomena at three phase boundaries are insufficiently developed
to shed much light on the questions of transient oscillation in three-dimensional,
complex geometries.

Acknowlegdements

WZ would like to thank support from the EPSRC for the development of the
acoustic actuated fluidic oscillator (Grant No. GR/S67845) and for financial
support from the Food Processing Faraday Partnership, Yorkshire Water, and
Sheffield University Enterprises Ltd. WZ would like to acknowledge the Royal
Academy of Engineering / Leverhulme Trust Senior Research Fellow programme.
The authors acknowledge helpful discussions with Marianne Grammatika.

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