2. Size Discrepancy of Bubble and Aerator Pore
The advantages obtained by the division of input gas volume into the large number of very small bubbles are based on the resultant large area of the total phase boundary between the gas and liquid phases. Since the intensity of transport processes (such as heat and/or mass transfer) across this phase boundary is proportional to the total surface area, it always seemed a quite obvious idea to increase the transfer intensity by making the bubbles very small. The simplest approach seemed to use for their generation an aerator with a large number of small parallel pores through which the gas is percolated. Typical present day commercially available aerators are mostly made by sintering a large number of very small objects (e.g., small spheres of thermos plastic polymer or glass spheres). Serving as the pores are then the small empty spaces left between these objects in the sintering process. Unfortunately, the experience with a usual aerator with steady gas flow percolation is almost universally disappointing. Irrespective of how small are the pore cross-sections, the generated bubbles are practically always substantially larger.
This discrepancy between the size of the pores and the size of generated bubbles was only relatively recently explained in [
3]. The explanation was found in the conjunctions of the bubbles, schematically presented in
Figure 1. An important role is the small bubble rise velocity law, presented in
Figure 2, evaluated as a power-law fit through the data points for microbubbles from several experiments [
4,
5,
6,
7,
8]. The equation of this law is:
where
(m/h) is the terminal velocity of the upwards motion and
d (mm) is the microbubble diameter. This Equation (1) assumes steady flow conditions in which the velocity is governed by equivalence of two acting forces, the hydraulic friction force on the microbubble boundary and of the driving force generated by the difference of specific volumes of the gas and liquid.
Evidently, the small microbubbles move very slowly. It may be noted in
Table 1 that the 50 μm microbubble (certainly not the smallest) moves so slowly that for traversing the whole height of a typical bioreactor vessel it needs the time scale of an hour. These long durations, of course, can have consequences such as the full finishing of transfer processes, for which there is not enough time during the fast moving rise of larger bubbles. In the situation presented in
Figure 1, the onset of very low velocity of the microbubble after leaving the aerator pore exit, forms a bunch of very small bubbles near one another. As presented in the drawing, inside the aerator pore the microbubbles are initially fast moving and thus their size corresponds to the size of the pore cross section area. They move inside the pore at a relatively high velocity dictated by properties of the gas supply source. This velocity is generally much higher than the value in Equation (1). On leaving the pore exit, the bubble velocity suddenly decreases to the value smaller than the value shown in
Figure 2, which means a near halt of motion. The microbubble only slowly increases its upwards motion velocity to the fully developed terminal velocity given by Equation (1).
The nonlinearity of this velocity law is seen from several evaluated data points:
This sudden velocity decrease and very slow motion at the pore exit means the newly emerging microbubble on leaving the pore inevitably collides with its predecessor microbubble, which is still dwelling near the pore exit. The collision and subsequent conjunction into a single larger bubble is more inevitable because the formation of a larger bubble is associated with decrease of total energy of surface tension (note that the total surface energy is smaller in the single larger bubble than in the sum of the two original microbubbles of the same total volume) and all passive processes always move into the direction of energy decreasing.
The energy released in the conjunction is used for oscillating the resultant larger bubble after the conjunction is over. This way, the energy is dissipated. Bubble oscillation increases its hydrodynamic resistance, which is an additional effect that decreases and almost stops the rising motion [
10]. The microbubble thus stays at or near the pore exit for some time. This results in conjunction with yet another of the later coming follower microbubbles. Thus at the pore exit dwells a bunch of bubbles, each of them stepwise increasing in diameter with each performed collision. The repeated processes finally end with a large bubble, substantially larger than the size of an aerator pore exit and capable of rising sufficiently fast away from the aerator pore.
The reason for the capability to keep the size of generated bubbles small by gas flow oscillation at the aerator was discovered from high-speed camera images. The original idea of why the oscillation is useful was the expectation of it breaking the larger bubbles into smaller ones by oscillatory decomposing. Later detailed studies of camera images, however, have shown the importance of a different mechanism. What happens is the repeated conjunctions discussed above are prevented by the oscillation. This prevention is due to increasing the distances between each pair of predecessor and follower microbubbles. The distance is made so large that the conjunction ceases to be possible.
3. T-Z and D-Z Oscillators
The device used for study of this phenomenon was initially a fluidic oscillator available from earlier experiments described in [
11,
12,
13,
14,
15]. It made possible elucidating by high-speed camera images the mechanism of the empirically discovered conjunction suppression. Non-optimised initial investigations used a no-moving-part fluidic oscillator (from another project) with dominant geometric parameter, main nozzle exit width 2 mm. The progress made with it was satisfactory and justified making another, dedicated oscillator model as well as applying for the patent document [
2], filed in 2006 with colleague Prof. Zimmerman. The earliest publications about the conjunction suppressing phenomenon originated from the University of Sheffield, where the present author tested the design during his temporary stay. It was also there where the oscillator design known as Tesař-Zimmerman or T-Z oscillator was made.
This oscillator, intended for the extensive feasibility tests, consisted of two parts:
- (1)
An acrylic body with air flow cavity of a fluidic jet-deflection amplifier as shown in
Figure 3;
- (2)
A length of Tygon tube which provided the required delayed-flow negative feedback loop.
The amplifier body part, presented in
Figure 3, was in this case a stack of four rectangular polymethylmethacrylate (PMMA) plates, with the cavity for air flow made by numerically controlled laser cutting. The most important among these plates is the pair of identical central amplifier plates, each 2 mm thick. In them were made cavities laser-cut through the whole plate thickness and then the stacked (the reason behind the pair instead of a single thicker plate is a higher precision of generated shapes in thinner plates by the laser-cutting). Both from the bottom and top, the amplifier cavities were then closed by attached cover plates (
Figure 3 shows the top plate removed to show the cavities). Useful for identifying the internal flow processes in the amplifier and the role of its components is the schematic representation shown in
Figure 4.
Although differing in overall geometry as well as in most details, the fundamental idea on which the oscillation generation is based in [
2] was the mutual connection of the input terminals
X1 and
X2 by the feedback fluid flow channel presented in
Figure 5. This oscillator idea is not new [
17]. It is actually already more than 60 years old, as shown in
Figure 5 by the copy of original drawing made for patent application. Nevertheless, this earliest version [
17] has never been used in any larger scale application. There were only uses in laboratory tests. In 1964, four years later after the patent document from
Figure 5, a laboratory model of a similar oscillator was made (for an unidentified military purpose) by a researcher named C. E. Spyropoulos, who was then employed at the Ordnance Fuse Laboratories of Army Materiel Command in the USA. Details of his oscillator are not known, perhaps due to military secrecy. In some literature it is possible to find Spyropoulos mistakenly mentioned as the inventor of this fluidic single-loop oscillator principle.
The microbubble generation could be made also with a different fluidic oscillator design than the one in [
2]. Experience [
18,
19]. has shown, however, that this choice is almost perfect from many points of view, including the economy of oscillator manufacturing.
Figure 4 shows a schematic representation of the amplifier. In this drawing, the air flow comes from the supply terminal
S at the left-hand side into the main nozzle and leaves on the opposite right-hand side through one of the two output terminals
Y1 and
Y2 in periodic alternation. Inside the amplifier body, the flow from the supply nozzle forms a jet entering the device’s interaction cavity. This cavity is a constant-depth space gradually increasing in the flow direction in width and hence also increasing in a cross-sectional area. In the symbolic representations, like the one in
Figure 4, nozzles are represented by the black triangles gradually decreasing in width in the flow direction, which accelerates the flow. The jet issuing from the supply nozzle is quite sensitive to influences acting in the region where the air flow leaves the supply nozzle. This sensitivity is here used for the amplification effect. At this sensitive location are directed exits from two control nozzles oriented perpendicularly to the main jet flow and connected to control terminals
X1 and
X2. Immediately downstream from these two nozzles are two mutually inclined attachment walls. The jet from the main nozzle attaches to one of these walls by the aerodynamic phenomenon called the Coandă effect. In steady flow regimes, it keeps the jet stably attached. Further downstream from the two attachment walls are in
Figure 4 two collectors, one of them capturing the jet. Immediately from there, continuing from the collectors towards the exit terminals, are important components, the diffusers. In them the cross-sectional areas for air flow gradually increase. While the schematic symbol for the nozzle is a black triangle, as mentioned above, indicating the area decrease in flow direction and hence acceleration of the flow, the symbol for diffuser is a white triangle. It shows that in the direction of the flow, the flow velocity decreases. The angle between the attachment walls has to be so large that the flow cannot be attached simultaneously to both. Thus only one of the collectors captures the air flow and directs it through the diffuser to the appropriate output terminal. The air pressure in the rectangular region surrounding the amplifier cavities in the centre of
Figure 4 is low, usually lower than atmospheric. It is the result of the flow velocity increase in the nozzles at the cost of pressure. As the kinetic energy of the air flowing in the nozzle increases, the pressure inside the region must decrease. This means a low pressure inside the amplifier until the pressure recovery in the diffusers. In the inactive output terminal, this low pressure generates a suction reverse flow. In the oscillator, this means alternating the output flow between positive (in active terminal) to negative (inactive terminal).
The amplifier discussed above is converted into a fluidic oscillator by the addition of the feedback loop channel or tube, connecting the two control nozzles. The earliest found idea in the literature is in patent [
17]. The original illustration from this document is shown in
Figure 5. It might be said that the aerodynamic design applied there is not really good. Firstly, the gas flow in the feedback loop will experience sudden changes in each of the four sharp corners of the feedback loop. The air flow in them loses its regularity, separates from the wall and generates aerodynamic noise likely to interfere with the carried signal. The second evident disadvantage is the “island” produced by the cutting of the feedback channel. Because of the cutting through the whole plate thickness this part falls out from the PMMA plate during the cutting process. Putting it back and placing it and fixing into the correct position requires another, not easy step in the manufacturing process. A third disadvantage of the drawing in
Figure 5 indicates that the designer failed to understand basic problems of internal aerodynamics. He designed the collector and the diffuser connected to it with short and curved walls, with which it is impossible to expect a reasonable pressure recovery. Instead, the diffusers must be long and with a small opening angle.
These shortcomings of Warren’s original design [
17] were in the T-Z oscillator corrected so that the aerodynamic performance was very much better, as was proven in the performed laboratory experiments. One of the essential improvements made in the T-Z oscillators over the version in
Figure 5 is their controllability by varying the feedback loop length, as indicated in
Figure 6. This property is particularly of importance with the oscillator output connected to the aerator.
The frequency of generated oscillation is dependent on the feedback tube length, air flow rate, magnitude of the air bleed off through the inactive output terminal, liquid column height in the reactor vessel, and finally also, of course, on the aerator as well as amplifier aerodynamic resistances. These parameters had to be all finely tuned if the bubble coalescence was to be eliminated without any large energetic loss. The results, however, were encouraging. With a standard commercially available sintered alumina aerator, as they are used in aquaculture, the capability to generate small microbubbles with an average diameter of 7 μm was demonstrated [
20]. It demands identifying the so called “sweet spot” [
20] of the adjustment. Favourable properties of the T-Z oscillators are demonstrated in the list of successful solutions, those obtained in recent research projects listed below. All cases listed there are of a large future economic potential.
Present development has added to the repertoire of fluidic oscillators in [
19] the new jet-deflection design. It is the novel Desai-Zimmerman or D-Z oscillator developed recently at the University of Sheffield, U.K. [
21]. Its design was specifically adapted to the conditions prevailing microbubble generating aerators—
Figure 7. The new oscillator version is of two-sided relaxation type, in principle following the one-sided oscillator design of Zalmanzon [
22], the earliest known fluidic oscillator but very little is known. The feedback effect is obtained by filling compressed air into its two accumulation chambers
C1, C2 in this particular design is connected to the middle of the attachment walls.
4. Microbubbles Generated by Mediation of the Oscillator
Initial targets, at which aimed the microbubble generation mediated by the fluidic oscillators were the obvious advantages obtained from the increase of total mass transport from gas to liquid (or vice versa in gas stripping). This was the result of the increase in the total surface boundary. The sum of mass transport surfaces increases, of course, with increasing the number of bubbles (and hence decreasing their mean diameter) generated from the same gas volume. From the fundamental patent [
2], the basis of further developments, is shown in
Figure 8 a picture of a typical configuration used in the tests [
21,
22] with a simple bioreactor (at right-hand side of the picture) and the oscillator (in picture centre). For the photosynthetic growing of primitive organisms [
25,
26,
27,
28,
29], the reactor walls are transparent and the water inside illuminated by spectrally suitable light. The aerator body is positioned in the centre of the vessel bottom and the bubble motion thus generates a paraxial rising water column. Downwards moving annular water flow is near the reactor walls. This circulation brings the microorganisms periodically to the external illumination.
In this particular early case, the advantages resultant from the small size of the microbubbles were just used. Their small dimensions correspond to the very small rising velocities according to Equation (1). There was no physically different behaviour from what is known about larger bubbles, just the increased geometric extrapolation to the smaller size. Even then, the enhanced interface area is an obvious benefit for a large number of chemical and biological processes with thus increased heat and mass transfer.
Laboratory experiments have, however, demonstrated various potential improvements resultant from the fact that the properties do not follow a simple linear proportionality law. The patent drawing configuration in
Figure 8 presents the setup as it was actually used in laboratory experiment, i.e., with various measurement instrumentations (rotameter for flow rate, pressure gauges) and the bioreactor connected to only one oscillator terminal [
2]. The other terminal, in
Figure 8, is connected to a bleed-off valve used for “sweet spot” adjustments. It is, of course, not economical to lose in this way a substantial proportion of the compressed air, but this was inevitable for gaining experience with the amplifier loading and matching. Once such an experience was obtained, it became possible to design the T-Z oscillators properly matched to the aerator as the aerodynamic loading. A detailed discussion of (slightly different) fluidic matching problems is available in [
30].
The result of the fully matched adjustments, without the lost air flow, is configured with two reactor vessels operated in anti-parallel (suction on one side at the same time as the output flow on the opposite side) as shown in
Figure 9.
7. Biotechnology of Micro-Organisms
An extremely promising application of microbubbles generated with the fluidic oscillator [
32] are photobioreactors for growing micro-organisms: algae, bacteria, yeast, and lower fungi. Of particular importance are single-cell microalgae, especially those known as green microalgae, performing photosynthesis. Like the higher green plants they derive the energy for their growth from light—mostly, of course, sunlight. As reactants, they use carbon, C, from CO
2 in atmosphere and hydrogen, H, from H
2O. The reaction products are higher hydrocarbons used to build plant body. They are now mostly seen as source of biomass for further processing into biofuels [
33]—or even the substrate for food (so far for animal and not human consumption, which may come later). Of particular promise is the photosynthetic generation of lipids, with the advantage of the high speed of biomass growth. Under optimum conditions, the microalgae can double their mass within a few days. An important fact is this is a promising way to decrease carbon in the emissions into the atmosphere and reduce dependence on fossil fuels. In [
27,
28] was demonstrated their potential to decrease CO
2 in the atmosphere—and use it as carbon source together with the produced biomass as feedstock for chemical industry.
At present the largest percentage of investigated microalgae biomass growing is done in open raceways, usually shallow channels aerated by a paddlewheel which simultaneously forces the water to circulate. The aeration effect is poor and yet consumes much energy. More expensive, but with a better future perspective, are closed vessel photobioreactors. They make possible a close control of the growth process and it is in this way that they can demonstrate the microbubble aerator with mediating advantages of the fluidic oscillator [
29,
34].
While green microorganisms need a supply of CO2 microbubbles for photosynthesis growth, they also need stripping from water inhibiting dissolved O2. This is also a task that can be fulfilled by microbubbles.
Some of the bioreactor application ideas were in principle already mentioned in the literature, but were at that time considered impractical for several reasons. Apart from the most important factor of high costs—running as well capital cost—, the microbubbles generated by the earlier known methods received a quite high input of energy, which in contact with the liquid surface in the top of the bioreactor, caused lysis of living cells. In the microbubbles generated in mediation by fluidic oscillators, this cause of lysis has been practically eliminated, as was found already in the first studies, e.g., [
25,
26,
27,
28,
29,
34,
35]. This, together with low cost, simplicity, and absence of driving mechanisms has significantly increased interest in the new generation method. An important factor in the success of the fluidic oscillator in its various roles is its controllability, discussed in [
20].
9. Some Recent Results
An excellent detailed survey of microbubble intensification of bioprocessing by microbubbles was recently published in [
20]. What seems to be a different physical process, but in fact is only a consequence of widely different time scales of competing parallel processes, is the evaporation dynamics of microbubbles [
37,
38]. It results in the absence of the so far unavoidable heating of the liquid, thus making most efficient the “cold distillation”. It is likely to become economically of extreme importance, considering the huge quantities of worldwide alcohol production, which thus may be made at a significantly lower cost.
In [
41] are presented laboratory tests results of biodiesel production with the microbubble removal of water, as well as esterification, which is important for biodiesel production with a phantom catalyst. There is already a monograph [
33] published on the problems associated with biofuels from algae. Several current projects with successful solutions of important tasks are listed in
Figure 11.
Microbubbles made with oscillator mediation of anaerobic digestion were reported by the authors of [
31], demonstrating an increase by 25%–100% in the production rate of biogas.
Interesting results were obtained by comparison in [
31] of aeration by 3 mm diameter bubbles with and without the upstream fluidic oscillation according [
42]. The authors’ measurements without optimisation have shown at least a 50% increase in the coefficient of mass transfer. A later optimised study has shown an even substantially higher improvement—a 90% increase obtained with oscillation. The project [
31] was oriented towards the wastewater treatment.
Remarkable increase by as much as 100% of biogas production was reported with the microbubble mediation of anaerobic digestion of biomass.
Microbubbles were already used in preparation of nanoparticles [
43], indicating another association with another rapidly developing area.