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`FLOW-THROUGH OXYGENATOR
`
`RELATED APPLICATIONS
`
`This application is a continuation-in-part of United States Patent Application Number
`10/872,017, now United States Patent Number 6,xxx,xxx, which claimspriority to United States
`Provisional Patent Application Number 60/358,534,filed February 22, 2002.
`
`FIELD OF THE INVENTION
`
`This inventionrelates to the electrolytic generation of microbubbles of oxygen for increasing the
`oxygen content of flowing water. This invention also relates to the use of superoxygenated
`water to enhance the growth andyield of plants. The flow-through modelis useful for
`oxygenating water for hydroponicplantculture, drip irrigation and waste watertreatment.
`
`BACKGROUND OF THE INVENTION
`
`Manybenefits maybe obtained through raising the oxygen content of aqueous media. Efforts
`have been madeto achieve highersaturated or supersaturated oxygenlevels for applications such
`as the improvementof water quality in ponds, lakes, marshes and reservoirs, the detoxification
`of contaminated water, culture offish, shrimp and other aquatic animals, biological culture and
`hydroponic culture. For example,fish held in a limited environmentsuch as an aquarium,a bait
`bucket or a live hold tank may quickly use up the dissolved oxygen in the course of normal
`respiration and are then subject to hypoxic stress, which can lead to death. A similar effectis
`seen in cell cultures, where the respiring cells would benefit from higher oxygen contentofthe
`medium. Organic pollutants from agricultural, municipal and industrialfacilities spread through
`the ground and surface water and adversely affectlife forms. Manypollutantsare toxic,
`carcinogenic or mutagenic. Decomposition ofthese pollutants is facilitated by oxygen, both by
`direct chemical detoxifying reactions or by stimulating the growth of detoxifying microflora.
`Contaminated water is described as having an increased biological oxygen demand (BOD) and
`water treatmentis aimed at decreasing the BOD so as to make more oxygen available for fish
`and otherlife forms.
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`The most common methodofincreasing the oxygen content of a medium is by sparging with air
`or oxygen. While this is a simple method, the resulting large bubbles produced simply break the
`surface andare discharged into the atmosphere. Attempts have been madeto reducethe size of
`the bubbles in order to facilitate oxygentransfer by increasing the total surface area of the
`oxygen bubbles. United States Patent Number 5,534,143 discloses a microbubble generatorthat
`achieves a bubble size of about 0.10 millimeters to about 3 millimeters in diameter. United
`States Patent Number 6,394,429 (“the ‘429 patent’) discloses a device for producing
`microbubbles, ranging in size from 0.1 to 100 micronsin diameter, by forcingair into the fluid at
`high pressure through a small orifice.
`
`Whentheobject of generating bubblesis to oxygenate the water, either air, with an oxygen
`content of about 21%, or pure oxygen maybe used. The production of oxygen and hydrogen by
`the electrolysis of water is well known. A currentis applied across an anode and a cathode
`which are immersed in an aqueous medium. Thecurrent maybe a direct current from a battery
`or an AC/DC converter from a line. Hydrogen gasis producedat the cathode and oxygen gasis
`produced at the anode. Thereactionsare:
`
`4H,0 + 4¢ + 40H’ +2H,
`AT THE CATHODE:
`2H,0 - 0, + 4H* + 4e
`AT THE ANODE:
`6H,O ~ 40H+ 4H* + 2H, + 0,
`NET REACTION:
`286 kilojoules of energy is required to generate one moleof oxygen.
`
`Thegasses form bubbles whichrise to the surface ofthe fluid and maybe collected. Either the
`oxygen or the hydrogen maybecollected for various uses. The “electrolytic water” surrounding
`the anode becomesacidic while the electrolytic water surrounding the cathode becomes basic.
`Therefore, the electrodes tend to foul or pit and have a limitedlife in these corrosive
`environments.
`
`Manycathodes and anodes are commercially available. United States Patent Number 5,982,609
`discloses cathodes comprising a metalor metallic oxide ofat least one metal selected from the
`groupconsisting ofruthenium,iridium, nickel, iron, rhodium, rhenium,cobalt, tungsten,
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`manganese, tantalum, molybdenum,lead,titanium,platinum, palladium and osmium. Anodes
`are formed from the same metallic oxides or metals as cathodes. Electrodes may also be formed
`from alloys of the above metals or metals and oxides co-deposited on a substrate. The cathode
`and anodes may be formed on any convenient support in any desired shapeorsize. It is possible
`to use the same materials or different materials for both electrodes. The choiceis determined
`according to the uses. Platinum and ironalloys(‘‘stainless steel”) are often preferred materials
`dueto their inherentresistance to the corrosive electrolytic water. An especially preferred anode
`disclosed in U. S. Patent Number 4,252,856 comprises vacuum deposited iridium oxide.
`
`Holding vessels for live animals generally have a high population of animals which use up the
`available oxygen rapidly. Pumpsto supply oxygen have high power requirements and the noise
`and bubbling mayfurtherstress the animals. The available electrolytic generators likewise have
`high power requirementsandadditionally run at high voltages and produceacidic and basic
`water which are detrimental to live animals. Manyofthe uses of oxygenators, such as keeping
`bait or caught fish alive, would benefit from portable devices that did not require a source of
`high power. The need remainsfor quiet, portable, low voltage meansto oxygenate water.
`
`It is
`It has also been knownthat plantroots are healthier when oxygenated wateris applied.
`thought that oxygen inhibits the growth of deleterious fungi. The water sparged with air as in
`the ‘429 patent was shown to increase the biomass of hydroponically grown cucumbers and
`tomatoes by about 15%.
`
`The need remains for oxygenator models suitable to be placed in-line in water distribution
`devices so as to be appliedto field as well as hydroponicculture.
`
`SUMMARYOF THE INVENTION
`
`This invention provides an oxygen emitter whichis an electrolytic cell which generates very
`small microbubbles and nanobubbles ofoxygen in an aqueous medium,whichbubbles are too
`small to break the surface tension of the medium,resulting in a medium supersaturated with
`oxygen.
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`The electrodes may be a meta! or oxide of at least one metal selected from the group consisting
`
`of ruthenium,iridium,nickel, iron, rhodium, rhenium,cobalt, tungsten, manganese, tantalum,
`
`molybdenum,lead, titanium, platinum, palladium and osmium or oxides thereof. The electrodes
`
`5
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`may be formed into open grids or may be closed surfaces. The most preferred cathodeis a
`
`stainless steel mesh. The most preferred mesh is a 1/16 inch grid. The most preferred anodeis
`
`platinum and iridium oxide on a support. A preferred support is titanium.
`
`In order to form microbubbles and nanobubbles, the anode and cathodeare separated by a
`
`10
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`critical distance. Thecritical distance ranges from 0.005 inches to 0.140 inches. The preferred
`
`critical distance is from 0.045 to 0.060 inches.
`
`Models of different size are provided to be applicable to various volumes of aqueous medium to
`
`be oxygenated. The public is directed to choose the applicable model based on volumeand
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`15
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`power requirements of projected use. Those models with low voltage requirementsare
`
`especially suited to oxygenating water in which animalsare to be held.
`
`Controls are provided to regulate the current and timingofelectrolysis.
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`A flow-through model is provided which may be connectedin-line to a watering hoseorto a
`
`hydroponic circulating system. The flow-through model can be formedinto a tube with
`
`triangular cross-section. In this model, the anode is placed toward the outside of the tube and the
`
`cathode is placed on the inside, contacting the water flow. Alternatively, the anodes and
`
`cathodes maybein plates parallel to the long axis of the tube, or may be plates in a waferstack.
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`Alternately, the electrodes may be placedin a side tube (“‘T” model) out ofthe direct flow of
`
`water. Protocols are provided to produce superoxygenated water at the desired flow rate and at
`
`the desired power usage. Controls are inserted to activate electrolysis when wateris flowing and
`
`deactivate electrolysis at rest.
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`This invention includes a method to promote growth and increase yield ofplants by application
`
`of superoxygenated water. The watertreated with the emitter of this invention is one example of
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`superoxygenated water. Plants may be grown in hydroponic culture or in soil. The use of the
`
`flow-through model for drip irrigation of crops and waste water treatmentis disclosed.
`
`DESCRIPTION OF THE DRAWINGS
`
`Figure 1 is the O, emitter of the invention.
`
`Figure 2 is an assembled device.
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`5
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`Figure 3 is a diagram ofthe electronic controls of the O, emitter.
`
`Figure 4 showsa funnel or pyramid variation of the O, emitter.
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`15
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`Figure 5 shows a multilayer sandwich O, emitter.
`
`Figure 6 showsthe yield of tomato plants watered with superoxygenated water.
`
`Figure 7 shows an oxygenation chambersuitable for flow-through applications. Figure 7A is a
`cross section showing arrangementofthree plate electrodes. Figure 7B is a longitudinal section
`showingthe points of connection to the powersource.
`
`Figure 8 is a graph showing the oxygenation of waste water.
`
`DETAILED DESCRIPTION OF THE INVENTION
`
`20
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`Definitions:
`
`Forthe purposeofdescribing the present invention, the following terms have these meanings:
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`30
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`“Critical distance” means the distance separating the anode and cathode at which evolved
`
`oxygen forms microbubbles and nanobubbles.
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`“Critical distance” meansthe distance separating the anode and cathode at which evolved
`oxygen forms microbubbles and nanobubbles.
`
`“O, emitter” meansa cell comprised ofat least one anode and at least one cathode separated by
`the critical distance.
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`“Metal” means a metal or an alloy of one or more metals.
`
`“Microbubble” means a bubble with a diameterless than 50 microns.
`
`““Nanobubble” meansa bubble with a diameterless than that necessary to break the surface
`tension of water. Nanobubbles remain suspendedin the water, giving the water an opalescent or
`milky appearance.
`
`“Supersaturated” means oxygen at a higher concentration than normalcalculated oxygen
`solubility at a particular temperature and pressure.
`
`“Superoxygenated water” means water with an oxygencontentat least 120% ofthat calculated
`to be saturated at a temperature.
`
`“Water” means any aqueous medium withresistance less than one ohm per square centimeter;
`that is, a medium that can support theelectrolysis of water. In general, the lowerlimit of
`resistance for a medium that can support electrolysis is water containing more than 2000 ppm
`total dissolved solids.
`
`The present invention produces microbubbles and nanobubbles of oxygenvia the electrolysis of
`water. As molecular oxygen radical (atomic weight 8) is produced,it reacts to form molecular
`oxygen, O,.
`In the special dimensionsofthe invention, as explained in moredetail in the
`following examples, O, forms bubbles which are too small to break the surfacetension of the
`fluid. These bubbles remain suspended indefinitely in the fluid and, whenallowed to build up,
`make the fluid opalescent or milky. Only after several hours do the bubbles begin to coalesce on
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`the sides of the container and the waterclears. During that time, the water is supersaturated with
`oxygen. In contrast, the H, formedreadily coalesces into larger bubbles which are discharged
`into the atmosphere, as can be seen by bubble formationat the cathode.
`
`5
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`Thefirst objective of this invention was to make an oxygen emitter with low power demands,
`low voltage and low current for use with live animals. Forthat reason, a small button emitter
`was devised. The anode and cathode wereset at varying distances. It was foundthat electrolysis
`took place at very short distances before arcing of the current occurred. Surprisingly, at slightly
`larger distances, the water became milky and no bubbles formedat the anode, while hydrogen
`continued to be bubbled off the cathode. At distance of 0.140 inches between the anode and
`cathode, it was observed that the oxygen formed bubblesat the anode. Therefore, the critical
`distance for microbubble and nanobubble formation was determined to be between 0.005 inches
`and 0.140 inches.
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`Example 1. Oxygen emitter.
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`As shown in Figure 1, the oxygen evolving anode 1 selected as the mostefficientis an iridium
`oxide coated single sided sheet of platinum on a support oftitanium (Eltech, Fairport Harbor,
`OH). The cathode 2 is a 1/16 inch mesh(size 8 mesh) marinestainless steel screen. The
`anodeand cathode are separated by a non-conducting spacer3 containing a gap 4 for the passage
`of gas and mixing of anodic and cathodic water and connected to a powersource through a
`connection point5. Figure 2 showsa plan view of the assembled device. The O, emitter 6 with
`the anode connecting wire 7 and the cathode connecting wire 8 is contained in an enclosure 9,
`connected to the battery compartment 10. The spacerthicknessiscriticalasit sets the critical
`distance.
`It mustbe ofsufficient thickness to prevent arcing ofthe current, but thin enough to
`separate the electrodes by no more than 0.140 inches. Abovethat thickness,the power needs are
`higher and the oxygen bubbles formed at higher voltage will coalesce and escapethe fluid.
`Preferably, the spacer is from 0.005 to 0.075 inches thick. At the lower limits, the emitter tends
`to foul more quickly. Most preferably, the spacer is about 0.050 inches thick. The spacer may
`be any nonconductive material such as nylon,fiberglass, Teflon® polymerorotherplastic.
`Becauseofthecriticality of the space distance,it is preferable to have a non-compressible
`spacer. It was found that Buna, with a durometer measure of 60 wasnot acceptable due to
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`decomposition. Viton, a commonfluoroelastomer, has a durometer measure of 90 and was
`foundto holdits shape well.
`
`In operation, a small device with an O, emitter 1.485 inches in diameter was driven by 4AA
`batteries. Thecritical distance was held at 0.050 inches with a Viton Spacer. Five gallons of
`water becamesaturated in seven minutes. This size is suitable for raising oxygen levels in an
`aquarium orbait bucket.
`
`It is convenientto attach a control circuit which comprises a timerthatis thermostatically
`controlled by a temperature sensor whichdeterminesthe off time for the cathode. When the
`temperature of the solution changes,the resistance ofthe thermistor changes, which causes an
`off time ofa certain duration. In cool water, the duration is longer so in a given volume, the
`emitter generates less oxygen. Whenthe wateris warmer and therefore hold less oxygen,the
`duration of off time is shorter. Thus the device is self-controlled to use power most
`economically. Figure 3 showsa block diagram ofa timer control with anode 1, cathode 2,
`thermistor temperature sensor 3, timer control circuit 4 and wire from a direct current power
`source 5.
`
`Example 2. Measurement of O, bubbles.
`Attempts were made to measure the diameter of the O, bubbles emitted by the device of
`Example |.
`In the case ofparticles other than gasses, measurements can easily be made by
`scanning electron microscopy, but gasses do not survive electron microscopy. Large bubble may
`be measuredby pore exclusion, for example, whichis also not feasible when measuring a gas
`bubble. A black and white digital, high contrast, backlit photograph oftreated water with a
`millimeter scale reference was shot ofwater produced by the emitter of Example 1. About 125
`bubbles were seen in the area selected for measurement. Seven bubbles ranging from the
`smallest clearly seen to the largest were measured. The area was enlarged, giving a scale
`multiplier of 0.029412.
`
`Recorded bubble diameters at scale were 0.16, 0.22, 0.35, 0.5 1, 0.76, 0.88 and 1.09 millimeters.
`The last three were considered outliers by reverse analysis of variance and were assumedto be
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`hydrogen bubbles. When multiplied by the scale multiplier, the assumed O, bubbles were found
`to range from 4.7 to 15 microns in diameter. This test was limited by the resolution ofthe
`camera and smaller bubbles in the nanometer range could not be resolved. It is known that white
`light cannot resolve features in the nanometersize range, so monochromatic laser light may give
`resolution sensitive enough to measure smaller bubbles. Efforts continue to increase the
`sensitivity of measurementso that sub-micron diameter bubbles can be measured.
`
`Example 3. Other models of oxygen emitter
`Depending on the volumeoffluid to be oxygenated, the oxygen emitter of this invention may be
`shaped asa circle, rectangle, cone or other model. One or more maybeset in a substrate that
`maybe metal, glass, plastic or other material. The substrate is notcritical as long as the current
`is isolated to the electrodes by the nonconductorspacer material of a thickness from 0.005 to
`0.075 inches, preferably 0.050 inches.
`It has been noticed that the flow of water seems to be at
`the periphery ofthe emitter, while the evolved visible bubbles (H,) arise at the center of the
`emitter. Therefore, a funnel or pyramidal shaped emitter was constructedto treat larger volumes
`of fluid. Figure 4 is a cross sectional diagram of such an emitter. The anode | is formed as an
`open grid separated from a marinegradestainlesssteel screen cathode 2 by the critical distance
`by spacer 3 aroundthe periphery of the emitter and at the apex. This flow-through embodiment
`is suitable for treating large volumes of waterrapidly.
`
`Thesize may be varied as required. A round emitter for oxygenating a bait bucket may be about
`2 inches in diameter, while a 3-inch diameter emitter is adequate for oxygenating a 10 to 40
`gallon tank. Thelive well of a fishing boat will generally hold 40 to 80 gallons of water and
`require a 4-inch diameter emitter. It is within the scopeofthis invention to construct larger
`emitters or to use several in a series to oxygenate larger volumes.
`It is also within the scope of
`this invention to vary the modelto provide for low voltage and amperagein cases where the
`need for oxygen is moderate and longlasting or conversely, to supersaturate water very quickly
`at higher voltage and amperage.
`In the special dimensions ofthe presentinvention, it has been
`foundthat a 6 volt battery supplying a current as low as 40 milliamperesis sufficient to generate
`oxygen. Such a modelis especially useful with live plants or animals, while it is more
`convenient for industrial use to use a higher voltage and current. Table I shows a numberof
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`models suitable to various uses.
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`Emitter Model|Gallons __Volts
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`TABLEI
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`Waterpail
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`1.200
`1.200
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`
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` 250
`2
`1
`2.500
`5.000
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`10
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`0.980
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`0.410
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`Example 4. Multilayer sandwich O,emitter
`AnO, emitter was made in a multilayer sandwich embodiment. (Figure 5) An iridium oxide
`coated platinum anode1 wasformedinto a grid to allow good water flow and sandwiched
`betweentwostainless steel screen cathodes2. Spacing washeld atthecritical distance by nylon
`spacers 3. The embodimentillustrated is held in a cassette 4 which is secured by nylon bolt 5
`with a nylon washer 6. The dimensionsselected were:
`
`cathode screen
`
`0.045 inches thick
`
`nylon spacer
`
`0.053 inches thick
`
`anode grid
`
`0.035 inches thick
`
`nylon spacer
`
`0.053 inches thick
`
`0.045 inches thick,
`cathode screen
`for an overall emitter thickness of 0.231 inches.
`
`If a more powerful emitter is desired, it is within the scopeofthis invention to repeat the
`sequence of stacking. For example, an embodiment may easily be constructed with this
`sequence: cathode, spacer, anode, spacer, cathode, spacer, anode, spacer, cathode, spacer, anode,
`spacer, cathode. The numberoflayers in the sandwichis limited only by the power requirements
`acceptable for an application.
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`Example 5. Effect of Superoxygenated water on the growth of plants.
`It is known that oxygen is important for the growth of plants. Although plants evolve oxygen
`during photosynthesis, they also have a requirementfor oxygen for respiration. Oxygenis
`evolvedin the leaves of the plants, while often the roots are ina hypoxic environment without
`enough oxygen to support optimum respiration, which can bereflected in less than optimum
`growth and nutrient utilization. Hydroponically grown plants are particularly susceptible to
`oxygen deficit in the root system. United States Patent Number 5,887,383 describesa liquid
`supply pump unit for hydroponic cultures which attain oxygen enrichmentby sparging with air.
`Such a method has high energy requirements andis noisy. Furthermore, while suitable forself-
`contained hydroponic culture, the apparatus is not usable for field irrigation. In a report available
`on the web, it was shown that hydroponically grown cucumbers and tomatoes supplied with water
`oxygenated with a device similar to that described in the ‘429 patent had increased biomass of
`about 12% and 17% respectively. It should be noted that when sparged with air, the water may
`becomesaturated with oxygen,butit is unlikely that the wateris superoxygenated.
`
`Superoxygenated water in hydroponic culture.
`A.
`Two small hydroponic systems were set up to grow two tomato plants. Circulation protocols
`were identical exceptthat the 2 % gallon water reservoir for the Control plant was eroated with
`and aquarium bubbler andthat for the Test plant was oxygenated with a five-inch strip emitter for
`two minutesprior to pumping. The cycle wasset at four minutes ofpumping, followed by four
`minutes of rest. The control water had an oxygen content of about 97% to 103% saturation, that
`is, it was saturated with oxygen. The test water had an oxygen content of about 153% tol165%
`saturation, that is, it was supersaturated.
`Thetest plant wasat least four times the volume of the
`control plant and began to show whatlookedlikefertilizer burn. Atthat point the fertilizer for
`the Test plant was reduced byhalf. Since the plants were not exposedto naturallight but to
`continuousartificial light in an indoor environmentwithoutthe natural means of fertilization
`(wind and/orinsects), the experiment was discontinued after three months. At that time, the Test
`plant but not the Control plant had blossomed.
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