CA2152671C - Apparatus and method for decreasing nitrogen oxide emissions from internal combustion power sources - Google Patents
Apparatus and method for decreasing nitrogen oxide emissions from internal combustion power sourcesInfo
- Publication number
- CA2152671C CA2152671C CA002152671A CA2152671A CA2152671C CA 2152671 C CA2152671 C CA 2152671C CA 002152671 A CA002152671 A CA 002152671A CA 2152671 A CA2152671 A CA 2152671A CA 2152671 C CA2152671 C CA 2152671C
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- CA
- Canada
- Prior art keywords
- fuel
- air
- combustion chamber
- burner
- mixture
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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Classifications
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/36—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using oxygen or mixtures containing oxygen as gasifying agents
- C01B3/363—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using oxygen or mixtures containing oxygen as gasifying agents characterised by the burner used
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
- F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
- F02B43/00—Engines characterised by operating on gaseous fuels; Plants including such engines
- F02B43/08—Plants characterised by the engines using gaseous fuel generated in the plant from solid fuel, e.g. wood
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
- F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
- F02B43/00—Engines characterised by operating on gaseous fuels; Plants including such engines
- F02B43/10—Engines or plants characterised by use of other specific gases, e.g. acetylene, oxyhydrogen
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
- F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
- F02M25/00—Engine-pertinent apparatus for adding non-fuel substances or small quantities of secondary fuel to combustion-air, main fuel or fuel-air mixture
- F02M25/10—Engine-pertinent apparatus for adding non-fuel substances or small quantities of secondary fuel to combustion-air, main fuel or fuel-air mixture adding acetylene, non-waterborne hydrogen, non-airborne oxygen, or ozone
- F02M25/12—Engine-pertinent apparatus for adding non-fuel substances or small quantities of secondary fuel to combustion-air, main fuel or fuel-air mixture adding acetylene, non-waterborne hydrogen, non-airborne oxygen, or ozone the apparatus having means for generating such gases
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
- F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
- F02B1/00—Engines characterised by fuel-air mixture compression
- F02B1/02—Engines characterised by fuel-air mixture compression with positive ignition
- F02B1/04—Engines characterised by fuel-air mixture compression with positive ignition with fuel-air mixture admission into cylinder
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/10—Process efficiency
- Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/10—Internal combustion engine [ICE] based vehicles
- Y02T10/12—Improving ICE efficiencies
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/10—Internal combustion engine [ICE] based vehicles
- Y02T10/30—Use of alternative fuels, e.g. biofuels
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10S123/00—Internal-combustion engines
- Y10S123/12—Hydrogen
Abstract
Apparatus is disclosed herein for reducing engine nitrogen oxide emissions by mixing hydrogen prepared from a portion of engine fuel within a simple burner The apparatus includes a burner (20) having an internal combustion chamber (25) for receiving either a portion of a gaseous fuel or liquid fuel (24) for mixture with air (26) and subsequent ignition by a spark plug. A mixing chamber (30) is included having a series of baffles against which injected air and fuel vapors impinge causing thorough and complete air/fuel blending into a mixture subsequently ignited and burned. and then discharged into the combustion chamber of the engine itself A pre-heating arrangement is provided for raising the temperature of the air/fuel mixture via a heat exchanging process with the combustion gases in the combustion chamber.
Description
2 1 5 2 6 7 ~ PCTIUS93112576 APPARATIJS AND METIIQ~ FQR
. DE('T~T'A.sING NITT~ T~N OXrnE T'MTssToNs FROM INTE~NAT ~ r~u~llON POWT~T~ sorTT;~T~s BA~ ,~Ou~U oF T~TT~' TNVT~'NTION
l. Field of the Invention The present invention relates to the f ield of reducing nitrogen oxide emission from internal combustion engines and turbines, and more particularly to a novel means of adding 1~YdLOg~1I prepared by means of a novel burner from a portion or part of the main engine fuel whether it be gaseous or liquid.
2. Brief DescriT~tion of the Priox Art It i5 well known that nitrogen oxides (NOX) foxm at the high temp~L u~t:s normally associated with combustion processes and that operating an engine at lean conditions with excess air lowers ~ <ItUL~ and, therefore, decreases NOX. However, decades of engine and turbine studies have shown that lean combustion limits for all fuels are above those where NOX emissions are below specified goals.
Natural gas and gasoline are examples where lean combustion has been pushed to its limit and where it has been f ound that hydrogen addition increase6 this limit to where NOX
output is acceptably low. However, means to obtain 1.~dl~,g~
for this purpose are beset with problems.
21~2~ 2-Problems and dif~iculties have been encountered when the 6upply of hydrogen is provided by materials carried in a separate tank which can be extremely heavy and requires pres6urization. As examples, methanol, llydru~ or ammonium nitrate can produce hydrogen when added to an engine combustor. However, these add to the fuel and so reduce the volumetric storage capacity which lowers overall performance, and results in complications through use of secondary materials. Hydrogen stored in the pressurized container which holds methane (Hythane) can also be used, but this causes about .75 percent reduced engine range for each percent l~ydLuu,c:~l used because of its very low energy content on a volumetric basis, and also re~uires special means to enable safe storage of 1IYdLUIJen.
A more f avorable method to obtain hydrogen is by properly treating a portion of the main engine fuel itself.
This does not require storing and using a new PYrPn~l~hlP and can be accomplished with little or no loss of fuel energy.
Hydrogen may be produced from fuels by high-temperature ~e -~ition, such as those listed in Greiner, U.S. Letters Patent 4, 350 ,133 . ~he actual patent discloses a fuel burner and rl~P ~cr combination on which hot gases produced from the burner heat a cPconA~ry flow of fuel within a heat exchanger to temperatures where it flPI _-~- of form hydrogen. It is intended for ~use with methanol as fuel, which can uniquely decompose without formation of solid carbon "soot" which can harm the engine process. The burner 21~2~71 of the aforementioned patent cannot efficiently combust when fuel rich, where otherwise hydrogen is produced. Hydrogen can also be produced by reacting the fuel with water to produce hydrogen through a "reforming" process. Such a process, however, requires involved catalytic means to bring about the water-fuel reaction, a heat input for its endothermic reaction, stored water or means to obtain it from the engine exhaust, etc. In addition, it often is difficult to obtain rapid and accurate flow response.
Because of such factors, the reformer process does not lend itself to an engine process.
The fuel may also be reacted with a deficiency of air to produce hydrogen. Doing so, however, is challenging because the excess fuel is not highly reactive and therefore difficult to involve in the reaction. For this reason, such previous processes relied on catalysts and complex hardware, which tended to make the process virtually 1lnllS~hle. Thus, ~ on~ et al., U.S. Letters Patent 4,033,133 teaches the use of special high temperature catalyst coupled with intensive preheat of the reactants to combust fuel with air to produce 11YI1L ~g~l . Such catalytic devices, by their nature are complex, dif f icult to control, and require undesirably long start-up times. Thus, they do not lend themselves to an engine process.
Therefore, a long-standing need has existed to provide a novel apparatus and means for accomplishing a technology breakthrough for a simple means of producing llydLl:)g~ll from WO 94/15082 ~2 _4_ PCTIUS93/12576 fuel in a simple burner without the catalyst or special pressurized hydrogen or related storage means normally considered .
-~ 2 1 5267 1 ~I~MMARY OF TTT~ I~VE~TION
Accordingly, the above problems and difficulties are obviated by the present invention which provides a novel means and method utilizing a burner for combusting air and hydrocarbons at fuel-rich stoichiometric air/fuel ratios.
In a f irst aspect, the present invention provides in an internal combustion apparatus, the ilu~L~V~ t which comprises:
a burner means having a combustion chamber for combusting air and hydrocarbons at fuel-rich air/fuel ratios from 0.3 to I to provide air/fuel vapors; and said burner means within said combustion chamber includes a mixer means intimately combining said air/fuel vapors for injection into said internal combustion apparatus .
The mixer means lncludes means Eor diverting a portion of the amin ~uel into the burner along with a portion of the amin air so that the fuel portion and air portion impinge against a first and second baffle arrangement whereby impingement thoroughtly mixes the fuel/air combination preparatory for ignition in the combustion chamber. Ignition means are provided for exhausting the burned gases from the burner into the combustion chamber of an engine. The .~ nt mixing provided by said impingements results in close to theoretical equilibration of the fuel-rich reaction, despite the low reactivity of the excess fuel.
In one ~orm of the invention, hydrogen gas is produced by employing a portion of methane gas which is mixed with the air by the baffle assembly, and in another form of the invention, liquid fuel, such as gasoline, is vaporized in a heat exchanger in the burner combustor prior to mixture ~t~
with air in the baffle assembly for subsequent ignition and discharge to the engine combustion compartment.
In a second aspect, the present invention provides an apparatus for reducing nitrogen oxide cnnt~mln~ntR emitted from an internal combustion power source comprising:
a main fuel supply;
an air supply;
a non-driving burner means haying a combustion chamber operably coupled to said fuel supply and said air supply for receiving a portion of said main fuel and air in close proximity within said burner means;
mixer means carried in said burner means combustion chamber for thoroughly ,~ ~ ;n;n~ said fuel and said air together to form a blend; and ignition means adj acent said mixer means in said combustion chamber and secured to said burner means for igniting said fuel/air blend for di~charge into said nt~rn~l combustion power source.
In a still further aspect, the present invention provides a method of reducing NOX conti~m;n~ntR in an interral combustion power source comprising the steps of:
withdrawing a portion of fuel from a main fuel source;
introducing a quantity of air with said portion of fuel to produce an air/fuel flow;
conducting said air/fuel flow into a mixing assembly by forcibly urging said air/fuel flow into engagement with walls causing flow reversal and thorough mixing of air and fuel to produce a combustible vapor;
igniting said combustible vapor in a burner chamber to produce combustion products; and exhausting said combustion product f rom the burner into the combustion power source for mixing with main fuel.
A.
WO 94/15082 21~ 2 67 1 PCT/US93/12576 RRTT ~ DE~CRTPTION QF rrT~ AwINGs The features of the present invention which are believed to be novel are set forth with particularity in the ~rPPn'lPd claims- The present invention, both as to its organization and manner of operation, together with further objects and advantages thereof, may best be understood with reference to the following description, taken in connection with the a~ ying drawings in which:
FIGURE 1 is a schematic drawing of a combustion engine incorporating the novel hydrogen generation means of the present invention effective to reduce nitrogen oxide in the engine emissions;
FIGURE 2 is an enlarged diagrammatic view in section illustrating the novel burner means employed in the engine system shown in FIGURE 1 for IIYdLOS~ generation;
FIGURES 3 and 3A are diagrammatic sectional views of the I1YdL ~-g,a-l generator employing a pre-heater means using heat exchange principles;
FIGURE 4 is a chart pertaining to f actors contributing to nitrogen oxide formation involving reaction between methane (CH4) and air ( 2 + 4Nz);
FIGURE 5 is a chart similar to the chart of FIGURE 4 involving the ~1P~ -sition of methane at various temperatures based on equilibrium species per mole of methane;
21~2~71 ~ WO 94/15082 PCT/US93/12576 FIGURE 6 is a chart presenting further information on major species at equilibrium versus air/fuel stoichiometric ratio;
FIG~RE 7 is a chart which amplifies the section of FIGURE 6 below a ratio of l; and FIGURE 8 is a chart including experimental points for a methane-air burner where lllm; n~c~nt carbon appears.
WO 94/15082 ~ ~ ~ 2 ~ 7 ~ 9 PCT/US93/12576 ~
~ES('RTPTION OF THE PREFERRE~ EMBODIMENT
Referring to FIGU~E 1, a schematic illustration is present wherein numeral 10 represents a conventional combustion engine having an exhaust 11 which normally emits gases having a high level of nitrogen oxide, as well as other contaminants. However, by employment of the present invention, these contaminants are greatly reduced or eliminated . The engine 10 includes a manif old 12 into which engine fuel from a storage tank 13 is introduced to the engine main combustion chamber. The fuel contained within tank 13 is mainly introduced to the manifold 12 through a carburetor 14 via a regulating valve 15 connected to ~ main fuel line 16. Ambient air is introduced to the carburetor for mixture with the main fuel supply vla a valve 17 and an air inlet 18. Thus, it can be seen that the combustion engine 10 is employed with fuel from tank 13 via the ~.dlbuLc:tor 14 wherein the main fuel supply is mixed with air according to a proper ratio to permit efficient combustion in the engine 10.
However, the conventional system described is ~nh~nced by utilization of the novel burner apparatus of the present invention, indicated in the general direction of arrow 20 which may be ref erred to as a llydL og~ll generator f or supplying a hydrogen vapor to the manifold 12 in order to reduce or eliminate nitrogen oxide in the combustion engine exhaust . It can be seen in FIGURE 1 that the ~IydL oye~l ~ \/0 94/15082 2 1 5 Z 6 7 .~ PCT/US93/12576 --lv generator, indicated by numeral 21, is supplied with a portion of the main fuel supply by means of a bypass line 22 connected to main line 16, and which is coupled to the llyd~ug~ generator 21 through a valve 23. Line 24 connects the valve 23 with the generator 21.
Referring now in detail to FIGURE 2, the ~l~dLog~
generator 21 includes a housing having an internal combustion chamber 25 in which the hydrogen generating means are located. When the main fuel is a gas, 6uch as methane, a portion of the gas is introduced via line 24 in combination with air supplied via line 26 so that the gas/air is initially . in~-l in a tube 27 within the combustion chamber 25. The tube 27 is u~ cnded 50 that the combined gas/air is directed towards a baffle 28 carried on the end of a cup 3 0 . The combined gas/air impinges against the baffle 28, as indicated by the flow of arrows such that the flow is reversed upon itself and exits through the open end of the cup 30, indicated by numeral 31. The two streams of air and gas move together through the tube 27 so as to finally exit inside the cup 30 where the streams impinge on the baffle 28. This causes flow direction changes, first go degrees radially outward and then 90 degrees to the opening 31. This process induces mixture of the air and gas . The reversed f low exits the cup at the orif ice or opening 31 and immediately impinges on the end of the burn wall, indicated by numeral 32, serving as a second baffle where the flow is again abruptly caused to move at -W0 94/15082 2 ~ 6 7 ~ PCT/US93/12576 S~lrr~?qcive right angles producing further mixing. The thoroughly mixed gas and air is now within the combustion chamber 25 wherein ignition of the mixed gases by gases already burning in the burner combu~stion chamber takes place . The initial ignition of thè f irst entry of unignited gases occurs upon operation of a spark plug 34 having its electrodes within the combustion chamber 25. The flame continue6 through the burner and f inally exits at a discharge duct 35 from which it is introduced to the combustion chamber of the engine 10.
In another instance, when the main fuel is a liquid, such as gasoline, the fuel is introduced through a line 36 and moves through the heat exchanger coils 33. Heat from the burning gases is properly ~Yrh~n~ l to the liquid fuel causing it to vaporize. The latter vaporized gases then pa6s through a tube 3 7 eventually being conducted through op~n~n~c, such as opening 38, where the gases meeting ~n~ ing air in the line 26 with resultant consequences as described immediately above.
Referring now in detail to FIGI~RE 3, a fuel pre-heating arrangement is illustrated. The hydrogen generator 20 includes a housing 21 having an internal combustion chamber 25 in which the llydLog~rl generator means are located. The main fuel, liquid or gas, is ill~r o-lucel in the combustion chamber 25 via an input fuel line 39 so that the gas/air mixture is initially combined in spiral tube ~1. Tube 41 is in heat exchange re~ationship with the hot gases 31 f ormed 2152~1 in the chamber 25 after com~ustion has taken place. The tube is of sufficient length so that the internal air/fuel mixture is heated within the range of 500 to 1000F, which insures vaporization of the liquid fuel. The length of tubing required for such heating effects virtually completes thorough mixing of the air/fuel mixture in the tube 41. A
tube 43 is attached to tube 41 having an open end 42 located in close proximity to the insulated housing end plate 32.
The pre-heated and pre-mixed mixture impinges upon end plate 32 and travels along the plate 32 to the corners of the housing where the flow abruptly is changed 90 to further enhance the mixing of the vapors and gases- The ~1IOLUUY1I1Y
mixed gases are then ignited by spark ignitor 3g. After initial ignition, spark ignition 34 may be turned off and ignition will occur as the gases exiting tube opening 42 contact the burning flame. Opening 42 at the end of tube 43 is dimensioned so that the gas mixture exits at a linear f low rate greater than its burning rate so ignition does not f lash back into the tube . The Pmh~rl; r -nt of FIGURE 3 includes means for pre-heating the air/fuel mixture prior to combustion. This results in a higher combustion temperature which aids the equilibration process, PSp~'; A 1 l y with regard to the unoxidized fuel fragments. A cup, such as cup 31 in FIGURE 2, may be used for further mixing if separate pre-heater devices are used for the air/fuel mixture.
Because normal burners have an excess of very reactive air, it is no real chore to bring about efficient reaction.
r W094/15082 21s26rtl ~ PCTIUS93112576 The inventive burner has a def iciency of air, 50 its reaction occurs in two steps . The f irst is oxidation of part of the fuel with all the oxygen present, which occurs with good ef f iciency because of the intrinsic reactivity of oxygen. The second is ~ itipn` of the unreacted excess fuel on absorbing heat provided from the o~ ti'm reaction.
Since fuels are inherently stable, thermal A~ Fition to e~uilibrium products is ~ f;r~llt to achieve. Instead, it generally leads to partially ~ ecl fuel ~ s, inc:luding some original fuel. This does not provide the theoretical equilibrium products which are needed.
FIGT~RE 3A illustrates a modified pre-heater with the addition of an exit tube 70 over the exhaust 42 so that gases exist via a horizontal slit 71 at the top and then curve towards the end wall. This curve is known as a "Coanda" curve. The combination causes the flow to bend over and follow down the outside of the attached tube. The Coanda device is used to induct air from the surroundings into the lamina made by a smaller f low of air pumped into the Coanda. Up to lOO times the air flow can be so educted.
Using thi6 in the burner will cause circulation of the burning gases, which decreases the length of the combustion chamber .
The inventive concept shows that equilibration in excess-fuel burners is achieved if the air and fuel are very h~ -3elleously mixed prior to ignition. Apparently, within this intimate mixture, heat supplied from oxidation of part WO 94/1~082 21~ 2 6 7 ~ PCT/US93/12~76 of the fuel is simultaneously absorbed by unreacted fucl in immediate contact, which then do ~ rc to equilibrium products .
This intimate premixing is achieved by bringing the air and fuel together in a separate chamber, where the flow is made to move back and forth. This intimate mixture then enters the combustion chamber wherein ignition occurs. It is necessary that burning does not travel back into the mixing chamber, despite the burning gases at their exit, which normally is an excellent ignition source.
This is prevented by the velocity of the stream that leaves the mixing chamber, taking advantage of the fact that the rate of burning through a mixture of fuel and air occurs at a finite rate. Thus, if the burning rate is 1 ft. /sec., then the gas mixture exiting the mixing chamber must travel at a higher rate. Otherwise, the burning gases in the burner would cause a burning lamina to travel back into the mixing chamber, which would be destructive.
The dimension of the burner 21 in inches used is:
I . D . Insulated Burner 21 5 . 373 Diameter of Cup 30 Height of Cup 30 Distance between Cup 30 and Rear Wall 32 0.875 Diameter Tube 26 0.5 Distance from end of Tube 26 and Bottom 28 of Cup 30 0.75 No Annulus or other hardware added to Orif ice 31 W0 94115082 2 ~ ~ 2 ~ 7 ~ PCT/US93/12576 From the above, the annulus that sets the flow ~rom mixing chamber into burner chamber has O . D . of 1. 0 and I . D . of 0 . 5, so its area, A, is .59 in or .0041 ft . Fuel wa6 gaseous methane, so a ~l~vc~puLizing assembly was not used. Oxidizer was laboratory air taken f rom c ~S~uL at maximum pressure of 50 psig.
The linear flow, LF, in ft. at the annulus was estimated from the air flow, AF, and fuel flow, FF, both in standard cubic feet per hour (SCFH) at the t ~ uL~ and pressure, and the area, A, using, LF = (AF + FF) / (A x 3600) .
Flow data from the tests at minimum and maximum flows, and as derived therefrom are in the following table:
Test Flow Rates ft3hr ft/sec FF AF Total LF
Nin 20.75 105.2 126.0 8.53 Nax 39.2 219.1 258.3 17.5 Linear burning rates for air-fuel mixtures can be found in standard engineering texts, such as the "Chemical ~n~in-~rs~
T~An-lhonk", John H. Perry, Editor (1963). These vary from about 1 ft/sec for most ~uels to maximum of about 8 for hydrogen .
The linear burning rates in the table always exceed the linear burning velocity of the ~ir-fuel mixture, so flash back burning into the mixing hardware was not likely, and it was not found. Had problems UCuurLed due to too low a gas WO 94/15082 2 ~ S 2 6 71 PCT/US93/12576 ~6 velocity, which could not be solved by other means, a fine metal screen would have been attached over the annulus.
Experience has shown this to prevent flARhha~-k at rates about 2/3 the actual linear burning rate due to a radical-trapping effect that inhibits ignition.
Factors ~ontributinq to NQx Form~tion FIGURE 3 is constructed from data calculated ~y the ~h~miCAl equilibrium program for reaction between methane (CH4) and air ( 2 + 4N2) (la) ( 2 + 4Nz), where n is stoi--hi~ ~LiC ratio. At n = l, the air contains just sufficient oxygen to react with all carbon and 11ydLu~
atoms, producing carbon dioxide (CO2) and water (HzO) in the ratio, (lb) CO2 + H2O.
The lower curve of FIGURE 3 is volume percent NOX in the combustion mix, the upper curve is equilibrium reaction temperature in F (divided by lO to fit the ordinate), and the slant line from the origin is air/fuel ratio by weight (divided by lOO).
Results show that temperature and excess air e~fect the formation of NOX, which peaks just beyond the stoil-h;, LLic ratio of l, where the air/fuel ratio is about 12. This is near the conditions where many engine comhustors operate.
At stoi~hi LLic ratios greater than two, Nûx is substantially tl;m;ni~hP-9, as temperature drastically 2 ~ ~ 2 PCT/US93/12576 decreases. The air/fuel ratio~ is about 20 or greater.
Practical experience has shown that methane combusts poorly at the latter high air-fuel ratios where NOX is low, and that this can be remedied by adding an appropriate amount of hydrogen .
HYdL~ell Production ~sinq a Burner Two means of producing IIYdLV~II from fuels generally using a burner are aiscussed below. The hydrogen so produced would be co-injected into the engine combustion chamber with the L- inrl~r of the fuel.
1. HYdroqen Produced b'~ Thermal Decomposition of Methane The CH4 molecule contains, in effect, two moles of 11YXILVg~::ll per atom of carbon, so the fuel is a candidate as hydrogen source. On the other hand, its }IydLvg~ll content is only 25% by weight, with the rc--;nin~ 75% being solid carbon. Complete reaction is, (2) CH4 = C(~) + 2 Hz.
FIGURE 4 has equilibrium data on the above reaction at various temperatures, calculated with the theoretical program. In this analysis, only methane (CH4), solid carbon (C(s) ), and ~IydLug~ll were ;nrl~
At above 700F, notab`le r~ oc;Ation occurs, approaching 50% at 1000 and 100% at 1500F. Each mole of },ydLvJall iS AC- _~n;ed by 0.5 moles of carbon.
2~ ~2671 ~ WO 94/15082 PCT/US93/12576 Experience shows that dissociation approaching equilibration requires the fuel pass through special catalysts while being heated, which represents an engineering complexity.
Energy input is required to heat the methane and effect d; ~CQ~ tion at the given conditions. Such data are in the curve labeled kNT-hr/lb. To refer this to an automobile, prPlim;n~ry as6umptions were made of 20 miles/6 lb. of methane (at, say, 60 mph) and need for 10% by volume of 11ydL~y~l~ to improve engine emissions. Results for these conditions are in the curve labeled kNT (multiplied by lO to fit the ordinate). As an example, if dP~ ition by heating to 1000F is called for, where one mole of methane converts to one of 11ydr ~yt~ there i5 a continuous need for . 016 kN thermal, or 16 watts.
If the latter energy is supplied electrically from the auto alternator, various inefficiencies would result in a 6-fold drain to the engine or about lO0 watts, if the energy is from a battery recharged by the engine. This energy would add to the other electrical needs of the engine and heat transfer from electrical heaters is difficult to carry out.
Energy for the process may be supplied by a separate burner, as in Greiner, U. S . Letters Patent 4, 350 ,133 . Here, energy from hot burner gases produced by burning some of the fuel is used to heat another portion of fuel in a separate heat exchanger to flP~ 05ition WO 94115082 2~S~6r1 i PCTII~S93/12576 q_ temperature, and the gases f rom the exchanger then passed to the engine. The spent burner gases are exhausted, resulting in energy losses resembling those discussed above. The patent was intended for u~e with methanol as fuel, which can uniquely ~ , Ee without formation of solid carbon "soot".
The f ormation of carbon by dissociation of all fuels which are not methanol results in severe h~n~l;C;-rfi.
Most important, as a solid carbon can severely clog various engine parts. Also as a solid, it is difficult to burn which reduces the energy output of the engine.
The overall conclusion is that formation of }1ydLucJ~1~ by thermal ~;qc~ci~tion of fuels for subsequent injection into an engine is fraught with problems. These nre uv~;~, ~ by the alternative method of producing 11~dLUU~
by reaction of fuel in a burner at sub-stoirhi1 LLic at/fuel ratio, as next 9ie~ Csec~.
2. Hydroqen Produced bY Sub-6toichiometric Air/Fuel Reaction Further information on major species theoretically formed in a burner at equilibrium vs. stoirh; ~ ~LiC ratio is given in FIGURES 5 and 6. (Nitrogen and oxygen are not shown since they are not important to the analysis and their high concentrations overpower those of the other species. ) FIGURE 6 amplif ie6 the data below a ratio of l. Note that above a ratio of about O . 4, about l . 55 moles of ~IydL ug~
form per mole of methane, while carbon does not form. This suggests that if a combustion technique could be developed _ .... _ _ . _ . . . , . . . _ _ _ _ _ _ .
~ WO 94/15082 215 2 6 71 PCT/US93112576 to attain this equilibrium, it would not require an external heat input, catalysts or special heat exchange means, and all of its combustion products could pass into the engine to minimize thermal energy losses.
ExpERIMENTAT~ R~ ULTS
The ability of the instant burner to attain theoretical equilibration at sub-stoirhi~ LLic ratios required to attain the process goals of no carbon was experimentally ascertained by operating the burner whose design and irmC have previously been given, using methane as fuel. Visual observations were made of the sudden rl ~ cArp~Arance and reappearance of ; ncAnr~-~cr~nt carbon as the actual stoirh i ~ ~L iC ratios are also drawn on the Figure .
The points all fall on the line for stoirhi~ LLic ratio of 0.45, which is where theory predicts formation of carbon.
Cul~st:l v~tion of mass requires that the I ~ -; n i n~ species, including hyd- UU,~:ll, essentially also follows the theoretical predictions .
While particular pmhorl;--nts of the present invention have been shown and described, it will be obvious to those skilled in the art that changes and modifications may be made without departing from this invention in its broader aspects and, therefore, the aim in the Arp'`nrl~rl claims is to cover all such changes and modifications as fall within the tro~ spirit and scope of this invention.
. DE('T~T'A.sING NITT~ T~N OXrnE T'MTssToNs FROM INTE~NAT ~ r~u~llON POWT~T~ sorTT;~T~s BA~ ,~Ou~U oF T~TT~' TNVT~'NTION
l. Field of the Invention The present invention relates to the f ield of reducing nitrogen oxide emission from internal combustion engines and turbines, and more particularly to a novel means of adding 1~YdLOg~1I prepared by means of a novel burner from a portion or part of the main engine fuel whether it be gaseous or liquid.
2. Brief DescriT~tion of the Priox Art It i5 well known that nitrogen oxides (NOX) foxm at the high temp~L u~t:s normally associated with combustion processes and that operating an engine at lean conditions with excess air lowers ~ <ItUL~ and, therefore, decreases NOX. However, decades of engine and turbine studies have shown that lean combustion limits for all fuels are above those where NOX emissions are below specified goals.
Natural gas and gasoline are examples where lean combustion has been pushed to its limit and where it has been f ound that hydrogen addition increase6 this limit to where NOX
output is acceptably low. However, means to obtain 1.~dl~,g~
for this purpose are beset with problems.
21~2~ 2-Problems and dif~iculties have been encountered when the 6upply of hydrogen is provided by materials carried in a separate tank which can be extremely heavy and requires pres6urization. As examples, methanol, llydru~ or ammonium nitrate can produce hydrogen when added to an engine combustor. However, these add to the fuel and so reduce the volumetric storage capacity which lowers overall performance, and results in complications through use of secondary materials. Hydrogen stored in the pressurized container which holds methane (Hythane) can also be used, but this causes about .75 percent reduced engine range for each percent l~ydLuu,c:~l used because of its very low energy content on a volumetric basis, and also re~uires special means to enable safe storage of 1IYdLUIJen.
A more f avorable method to obtain hydrogen is by properly treating a portion of the main engine fuel itself.
This does not require storing and using a new PYrPn~l~hlP and can be accomplished with little or no loss of fuel energy.
Hydrogen may be produced from fuels by high-temperature ~e -~ition, such as those listed in Greiner, U.S. Letters Patent 4, 350 ,133 . ~he actual patent discloses a fuel burner and rl~P ~cr combination on which hot gases produced from the burner heat a cPconA~ry flow of fuel within a heat exchanger to temperatures where it flPI _-~- of form hydrogen. It is intended for ~use with methanol as fuel, which can uniquely decompose without formation of solid carbon "soot" which can harm the engine process. The burner 21~2~71 of the aforementioned patent cannot efficiently combust when fuel rich, where otherwise hydrogen is produced. Hydrogen can also be produced by reacting the fuel with water to produce hydrogen through a "reforming" process. Such a process, however, requires involved catalytic means to bring about the water-fuel reaction, a heat input for its endothermic reaction, stored water or means to obtain it from the engine exhaust, etc. In addition, it often is difficult to obtain rapid and accurate flow response.
Because of such factors, the reformer process does not lend itself to an engine process.
The fuel may also be reacted with a deficiency of air to produce hydrogen. Doing so, however, is challenging because the excess fuel is not highly reactive and therefore difficult to involve in the reaction. For this reason, such previous processes relied on catalysts and complex hardware, which tended to make the process virtually 1lnllS~hle. Thus, ~ on~ et al., U.S. Letters Patent 4,033,133 teaches the use of special high temperature catalyst coupled with intensive preheat of the reactants to combust fuel with air to produce 11YI1L ~g~l . Such catalytic devices, by their nature are complex, dif f icult to control, and require undesirably long start-up times. Thus, they do not lend themselves to an engine process.
Therefore, a long-standing need has existed to provide a novel apparatus and means for accomplishing a technology breakthrough for a simple means of producing llydLl:)g~ll from WO 94/15082 ~2 _4_ PCTIUS93/12576 fuel in a simple burner without the catalyst or special pressurized hydrogen or related storage means normally considered .
-~ 2 1 5267 1 ~I~MMARY OF TTT~ I~VE~TION
Accordingly, the above problems and difficulties are obviated by the present invention which provides a novel means and method utilizing a burner for combusting air and hydrocarbons at fuel-rich stoichiometric air/fuel ratios.
In a f irst aspect, the present invention provides in an internal combustion apparatus, the ilu~L~V~ t which comprises:
a burner means having a combustion chamber for combusting air and hydrocarbons at fuel-rich air/fuel ratios from 0.3 to I to provide air/fuel vapors; and said burner means within said combustion chamber includes a mixer means intimately combining said air/fuel vapors for injection into said internal combustion apparatus .
The mixer means lncludes means Eor diverting a portion of the amin ~uel into the burner along with a portion of the amin air so that the fuel portion and air portion impinge against a first and second baffle arrangement whereby impingement thoroughtly mixes the fuel/air combination preparatory for ignition in the combustion chamber. Ignition means are provided for exhausting the burned gases from the burner into the combustion chamber of an engine. The .~ nt mixing provided by said impingements results in close to theoretical equilibration of the fuel-rich reaction, despite the low reactivity of the excess fuel.
In one ~orm of the invention, hydrogen gas is produced by employing a portion of methane gas which is mixed with the air by the baffle assembly, and in another form of the invention, liquid fuel, such as gasoline, is vaporized in a heat exchanger in the burner combustor prior to mixture ~t~
with air in the baffle assembly for subsequent ignition and discharge to the engine combustion compartment.
In a second aspect, the present invention provides an apparatus for reducing nitrogen oxide cnnt~mln~ntR emitted from an internal combustion power source comprising:
a main fuel supply;
an air supply;
a non-driving burner means haying a combustion chamber operably coupled to said fuel supply and said air supply for receiving a portion of said main fuel and air in close proximity within said burner means;
mixer means carried in said burner means combustion chamber for thoroughly ,~ ~ ;n;n~ said fuel and said air together to form a blend; and ignition means adj acent said mixer means in said combustion chamber and secured to said burner means for igniting said fuel/air blend for di~charge into said nt~rn~l combustion power source.
In a still further aspect, the present invention provides a method of reducing NOX conti~m;n~ntR in an interral combustion power source comprising the steps of:
withdrawing a portion of fuel from a main fuel source;
introducing a quantity of air with said portion of fuel to produce an air/fuel flow;
conducting said air/fuel flow into a mixing assembly by forcibly urging said air/fuel flow into engagement with walls causing flow reversal and thorough mixing of air and fuel to produce a combustible vapor;
igniting said combustible vapor in a burner chamber to produce combustion products; and exhausting said combustion product f rom the burner into the combustion power source for mixing with main fuel.
A.
WO 94/15082 21~ 2 67 1 PCT/US93/12576 RRTT ~ DE~CRTPTION QF rrT~ AwINGs The features of the present invention which are believed to be novel are set forth with particularity in the ~rPPn'lPd claims- The present invention, both as to its organization and manner of operation, together with further objects and advantages thereof, may best be understood with reference to the following description, taken in connection with the a~ ying drawings in which:
FIGURE 1 is a schematic drawing of a combustion engine incorporating the novel hydrogen generation means of the present invention effective to reduce nitrogen oxide in the engine emissions;
FIGURE 2 is an enlarged diagrammatic view in section illustrating the novel burner means employed in the engine system shown in FIGURE 1 for IIYdLOS~ generation;
FIGURES 3 and 3A are diagrammatic sectional views of the I1YdL ~-g,a-l generator employing a pre-heater means using heat exchange principles;
FIGURE 4 is a chart pertaining to f actors contributing to nitrogen oxide formation involving reaction between methane (CH4) and air ( 2 + 4Nz);
FIGURE 5 is a chart similar to the chart of FIGURE 4 involving the ~1P~ -sition of methane at various temperatures based on equilibrium species per mole of methane;
21~2~71 ~ WO 94/15082 PCT/US93/12576 FIGURE 6 is a chart presenting further information on major species at equilibrium versus air/fuel stoichiometric ratio;
FIG~RE 7 is a chart which amplifies the section of FIGURE 6 below a ratio of l; and FIGURE 8 is a chart including experimental points for a methane-air burner where lllm; n~c~nt carbon appears.
WO 94/15082 ~ ~ ~ 2 ~ 7 ~ 9 PCT/US93/12576 ~
~ES('RTPTION OF THE PREFERRE~ EMBODIMENT
Referring to FIGU~E 1, a schematic illustration is present wherein numeral 10 represents a conventional combustion engine having an exhaust 11 which normally emits gases having a high level of nitrogen oxide, as well as other contaminants. However, by employment of the present invention, these contaminants are greatly reduced or eliminated . The engine 10 includes a manif old 12 into which engine fuel from a storage tank 13 is introduced to the engine main combustion chamber. The fuel contained within tank 13 is mainly introduced to the manifold 12 through a carburetor 14 via a regulating valve 15 connected to ~ main fuel line 16. Ambient air is introduced to the carburetor for mixture with the main fuel supply vla a valve 17 and an air inlet 18. Thus, it can be seen that the combustion engine 10 is employed with fuel from tank 13 via the ~.dlbuLc:tor 14 wherein the main fuel supply is mixed with air according to a proper ratio to permit efficient combustion in the engine 10.
However, the conventional system described is ~nh~nced by utilization of the novel burner apparatus of the present invention, indicated in the general direction of arrow 20 which may be ref erred to as a llydL og~ll generator f or supplying a hydrogen vapor to the manifold 12 in order to reduce or eliminate nitrogen oxide in the combustion engine exhaust . It can be seen in FIGURE 1 that the ~IydL oye~l ~ \/0 94/15082 2 1 5 Z 6 7 .~ PCT/US93/12576 --lv generator, indicated by numeral 21, is supplied with a portion of the main fuel supply by means of a bypass line 22 connected to main line 16, and which is coupled to the llyd~ug~ generator 21 through a valve 23. Line 24 connects the valve 23 with the generator 21.
Referring now in detail to FIGURE 2, the ~l~dLog~
generator 21 includes a housing having an internal combustion chamber 25 in which the hydrogen generating means are located. When the main fuel is a gas, 6uch as methane, a portion of the gas is introduced via line 24 in combination with air supplied via line 26 so that the gas/air is initially . in~-l in a tube 27 within the combustion chamber 25. The tube 27 is u~ cnded 50 that the combined gas/air is directed towards a baffle 28 carried on the end of a cup 3 0 . The combined gas/air impinges against the baffle 28, as indicated by the flow of arrows such that the flow is reversed upon itself and exits through the open end of the cup 30, indicated by numeral 31. The two streams of air and gas move together through the tube 27 so as to finally exit inside the cup 30 where the streams impinge on the baffle 28. This causes flow direction changes, first go degrees radially outward and then 90 degrees to the opening 31. This process induces mixture of the air and gas . The reversed f low exits the cup at the orif ice or opening 31 and immediately impinges on the end of the burn wall, indicated by numeral 32, serving as a second baffle where the flow is again abruptly caused to move at -W0 94/15082 2 ~ 6 7 ~ PCT/US93/12576 S~lrr~?qcive right angles producing further mixing. The thoroughly mixed gas and air is now within the combustion chamber 25 wherein ignition of the mixed gases by gases already burning in the burner combu~stion chamber takes place . The initial ignition of thè f irst entry of unignited gases occurs upon operation of a spark plug 34 having its electrodes within the combustion chamber 25. The flame continue6 through the burner and f inally exits at a discharge duct 35 from which it is introduced to the combustion chamber of the engine 10.
In another instance, when the main fuel is a liquid, such as gasoline, the fuel is introduced through a line 36 and moves through the heat exchanger coils 33. Heat from the burning gases is properly ~Yrh~n~ l to the liquid fuel causing it to vaporize. The latter vaporized gases then pa6s through a tube 3 7 eventually being conducted through op~n~n~c, such as opening 38, where the gases meeting ~n~ ing air in the line 26 with resultant consequences as described immediately above.
Referring now in detail to FIGI~RE 3, a fuel pre-heating arrangement is illustrated. The hydrogen generator 20 includes a housing 21 having an internal combustion chamber 25 in which the llydLog~rl generator means are located. The main fuel, liquid or gas, is ill~r o-lucel in the combustion chamber 25 via an input fuel line 39 so that the gas/air mixture is initially combined in spiral tube ~1. Tube 41 is in heat exchange re~ationship with the hot gases 31 f ormed 2152~1 in the chamber 25 after com~ustion has taken place. The tube is of sufficient length so that the internal air/fuel mixture is heated within the range of 500 to 1000F, which insures vaporization of the liquid fuel. The length of tubing required for such heating effects virtually completes thorough mixing of the air/fuel mixture in the tube 41. A
tube 43 is attached to tube 41 having an open end 42 located in close proximity to the insulated housing end plate 32.
The pre-heated and pre-mixed mixture impinges upon end plate 32 and travels along the plate 32 to the corners of the housing where the flow abruptly is changed 90 to further enhance the mixing of the vapors and gases- The ~1IOLUUY1I1Y
mixed gases are then ignited by spark ignitor 3g. After initial ignition, spark ignition 34 may be turned off and ignition will occur as the gases exiting tube opening 42 contact the burning flame. Opening 42 at the end of tube 43 is dimensioned so that the gas mixture exits at a linear f low rate greater than its burning rate so ignition does not f lash back into the tube . The Pmh~rl; r -nt of FIGURE 3 includes means for pre-heating the air/fuel mixture prior to combustion. This results in a higher combustion temperature which aids the equilibration process, PSp~'; A 1 l y with regard to the unoxidized fuel fragments. A cup, such as cup 31 in FIGURE 2, may be used for further mixing if separate pre-heater devices are used for the air/fuel mixture.
Because normal burners have an excess of very reactive air, it is no real chore to bring about efficient reaction.
r W094/15082 21s26rtl ~ PCTIUS93112576 The inventive burner has a def iciency of air, 50 its reaction occurs in two steps . The f irst is oxidation of part of the fuel with all the oxygen present, which occurs with good ef f iciency because of the intrinsic reactivity of oxygen. The second is ~ itipn` of the unreacted excess fuel on absorbing heat provided from the o~ ti'm reaction.
Since fuels are inherently stable, thermal A~ Fition to e~uilibrium products is ~ f;r~llt to achieve. Instead, it generally leads to partially ~ ecl fuel ~ s, inc:luding some original fuel. This does not provide the theoretical equilibrium products which are needed.
FIGT~RE 3A illustrates a modified pre-heater with the addition of an exit tube 70 over the exhaust 42 so that gases exist via a horizontal slit 71 at the top and then curve towards the end wall. This curve is known as a "Coanda" curve. The combination causes the flow to bend over and follow down the outside of the attached tube. The Coanda device is used to induct air from the surroundings into the lamina made by a smaller f low of air pumped into the Coanda. Up to lOO times the air flow can be so educted.
Using thi6 in the burner will cause circulation of the burning gases, which decreases the length of the combustion chamber .
The inventive concept shows that equilibration in excess-fuel burners is achieved if the air and fuel are very h~ -3elleously mixed prior to ignition. Apparently, within this intimate mixture, heat supplied from oxidation of part WO 94/1~082 21~ 2 6 7 ~ PCT/US93/12~76 of the fuel is simultaneously absorbed by unreacted fucl in immediate contact, which then do ~ rc to equilibrium products .
This intimate premixing is achieved by bringing the air and fuel together in a separate chamber, where the flow is made to move back and forth. This intimate mixture then enters the combustion chamber wherein ignition occurs. It is necessary that burning does not travel back into the mixing chamber, despite the burning gases at their exit, which normally is an excellent ignition source.
This is prevented by the velocity of the stream that leaves the mixing chamber, taking advantage of the fact that the rate of burning through a mixture of fuel and air occurs at a finite rate. Thus, if the burning rate is 1 ft. /sec., then the gas mixture exiting the mixing chamber must travel at a higher rate. Otherwise, the burning gases in the burner would cause a burning lamina to travel back into the mixing chamber, which would be destructive.
The dimension of the burner 21 in inches used is:
I . D . Insulated Burner 21 5 . 373 Diameter of Cup 30 Height of Cup 30 Distance between Cup 30 and Rear Wall 32 0.875 Diameter Tube 26 0.5 Distance from end of Tube 26 and Bottom 28 of Cup 30 0.75 No Annulus or other hardware added to Orif ice 31 W0 94115082 2 ~ ~ 2 ~ 7 ~ PCT/US93/12576 From the above, the annulus that sets the flow ~rom mixing chamber into burner chamber has O . D . of 1. 0 and I . D . of 0 . 5, so its area, A, is .59 in or .0041 ft . Fuel wa6 gaseous methane, so a ~l~vc~puLizing assembly was not used. Oxidizer was laboratory air taken f rom c ~S~uL at maximum pressure of 50 psig.
The linear flow, LF, in ft. at the annulus was estimated from the air flow, AF, and fuel flow, FF, both in standard cubic feet per hour (SCFH) at the t ~ uL~ and pressure, and the area, A, using, LF = (AF + FF) / (A x 3600) .
Flow data from the tests at minimum and maximum flows, and as derived therefrom are in the following table:
Test Flow Rates ft3hr ft/sec FF AF Total LF
Nin 20.75 105.2 126.0 8.53 Nax 39.2 219.1 258.3 17.5 Linear burning rates for air-fuel mixtures can be found in standard engineering texts, such as the "Chemical ~n~in-~rs~
T~An-lhonk", John H. Perry, Editor (1963). These vary from about 1 ft/sec for most ~uels to maximum of about 8 for hydrogen .
The linear burning rates in the table always exceed the linear burning velocity of the ~ir-fuel mixture, so flash back burning into the mixing hardware was not likely, and it was not found. Had problems UCuurLed due to too low a gas WO 94/15082 2 ~ S 2 6 71 PCT/US93/12576 ~6 velocity, which could not be solved by other means, a fine metal screen would have been attached over the annulus.
Experience has shown this to prevent flARhha~-k at rates about 2/3 the actual linear burning rate due to a radical-trapping effect that inhibits ignition.
Factors ~ontributinq to NQx Form~tion FIGURE 3 is constructed from data calculated ~y the ~h~miCAl equilibrium program for reaction between methane (CH4) and air ( 2 + 4N2) (la) ( 2 + 4Nz), where n is stoi--hi~ ~LiC ratio. At n = l, the air contains just sufficient oxygen to react with all carbon and 11ydLu~
atoms, producing carbon dioxide (CO2) and water (HzO) in the ratio, (lb) CO2 + H2O.
The lower curve of FIGURE 3 is volume percent NOX in the combustion mix, the upper curve is equilibrium reaction temperature in F (divided by lO to fit the ordinate), and the slant line from the origin is air/fuel ratio by weight (divided by lOO).
Results show that temperature and excess air e~fect the formation of NOX, which peaks just beyond the stoil-h;, LLic ratio of l, where the air/fuel ratio is about 12. This is near the conditions where many engine comhustors operate.
At stoi~hi LLic ratios greater than two, Nûx is substantially tl;m;ni~hP-9, as temperature drastically 2 ~ ~ 2 PCT/US93/12576 decreases. The air/fuel ratio~ is about 20 or greater.
Practical experience has shown that methane combusts poorly at the latter high air-fuel ratios where NOX is low, and that this can be remedied by adding an appropriate amount of hydrogen .
HYdL~ell Production ~sinq a Burner Two means of producing IIYdLV~II from fuels generally using a burner are aiscussed below. The hydrogen so produced would be co-injected into the engine combustion chamber with the L- inrl~r of the fuel.
1. HYdroqen Produced b'~ Thermal Decomposition of Methane The CH4 molecule contains, in effect, two moles of 11YXILVg~::ll per atom of carbon, so the fuel is a candidate as hydrogen source. On the other hand, its }IydLvg~ll content is only 25% by weight, with the rc--;nin~ 75% being solid carbon. Complete reaction is, (2) CH4 = C(~) + 2 Hz.
FIGURE 4 has equilibrium data on the above reaction at various temperatures, calculated with the theoretical program. In this analysis, only methane (CH4), solid carbon (C(s) ), and ~IydLug~ll were ;nrl~
At above 700F, notab`le r~ oc;Ation occurs, approaching 50% at 1000 and 100% at 1500F. Each mole of },ydLvJall iS AC- _~n;ed by 0.5 moles of carbon.
2~ ~2671 ~ WO 94/15082 PCT/US93/12576 Experience shows that dissociation approaching equilibration requires the fuel pass through special catalysts while being heated, which represents an engineering complexity.
Energy input is required to heat the methane and effect d; ~CQ~ tion at the given conditions. Such data are in the curve labeled kNT-hr/lb. To refer this to an automobile, prPlim;n~ry as6umptions were made of 20 miles/6 lb. of methane (at, say, 60 mph) and need for 10% by volume of 11ydL~y~l~ to improve engine emissions. Results for these conditions are in the curve labeled kNT (multiplied by lO to fit the ordinate). As an example, if dP~ ition by heating to 1000F is called for, where one mole of methane converts to one of 11ydr ~yt~ there i5 a continuous need for . 016 kN thermal, or 16 watts.
If the latter energy is supplied electrically from the auto alternator, various inefficiencies would result in a 6-fold drain to the engine or about lO0 watts, if the energy is from a battery recharged by the engine. This energy would add to the other electrical needs of the engine and heat transfer from electrical heaters is difficult to carry out.
Energy for the process may be supplied by a separate burner, as in Greiner, U. S . Letters Patent 4, 350 ,133 . Here, energy from hot burner gases produced by burning some of the fuel is used to heat another portion of fuel in a separate heat exchanger to flP~ 05ition WO 94115082 2~S~6r1 i PCTII~S93/12576 q_ temperature, and the gases f rom the exchanger then passed to the engine. The spent burner gases are exhausted, resulting in energy losses resembling those discussed above. The patent was intended for u~e with methanol as fuel, which can uniquely ~ , Ee without formation of solid carbon "soot".
The f ormation of carbon by dissociation of all fuels which are not methanol results in severe h~n~l;C;-rfi.
Most important, as a solid carbon can severely clog various engine parts. Also as a solid, it is difficult to burn which reduces the energy output of the engine.
The overall conclusion is that formation of }1ydLucJ~1~ by thermal ~;qc~ci~tion of fuels for subsequent injection into an engine is fraught with problems. These nre uv~;~, ~ by the alternative method of producing 11~dLUU~
by reaction of fuel in a burner at sub-stoirhi1 LLic at/fuel ratio, as next 9ie~ Csec~.
2. Hydroqen Produced bY Sub-6toichiometric Air/Fuel Reaction Further information on major species theoretically formed in a burner at equilibrium vs. stoirh; ~ ~LiC ratio is given in FIGURES 5 and 6. (Nitrogen and oxygen are not shown since they are not important to the analysis and their high concentrations overpower those of the other species. ) FIGURE 6 amplif ie6 the data below a ratio of l. Note that above a ratio of about O . 4, about l . 55 moles of ~IydL ug~
form per mole of methane, while carbon does not form. This suggests that if a combustion technique could be developed _ .... _ _ . _ . . . , . . . _ _ _ _ _ _ .
~ WO 94/15082 215 2 6 71 PCT/US93112576 to attain this equilibrium, it would not require an external heat input, catalysts or special heat exchange means, and all of its combustion products could pass into the engine to minimize thermal energy losses.
ExpERIMENTAT~ R~ ULTS
The ability of the instant burner to attain theoretical equilibration at sub-stoirhi~ LLic ratios required to attain the process goals of no carbon was experimentally ascertained by operating the burner whose design and irmC have previously been given, using methane as fuel. Visual observations were made of the sudden rl ~ cArp~Arance and reappearance of ; ncAnr~-~cr~nt carbon as the actual stoirh i ~ ~L iC ratios are also drawn on the Figure .
The points all fall on the line for stoirhi~ LLic ratio of 0.45, which is where theory predicts formation of carbon.
Cul~st:l v~tion of mass requires that the I ~ -; n i n~ species, including hyd- UU,~:ll, essentially also follows the theoretical predictions .
While particular pmhorl;--nts of the present invention have been shown and described, it will be obvious to those skilled in the art that changes and modifications may be made without departing from this invention in its broader aspects and, therefore, the aim in the Arp'`nrl~rl claims is to cover all such changes and modifications as fall within the tro~ spirit and scope of this invention.
Claims (21)
1. In an internal combustion apparatus, the improvement which comprises:
a burner means having a combustion chamber for combusting air and hydrocarbons at fuel-rich air/fuel ratios from 0.3 to I to provide air/fuel vapors; and said burner means within said combustion chamber includes a mixer means intimately combining said air/fuel vapors for injection into said internal combustion apparatus.
a burner means having a combustion chamber for combusting air and hydrocarbons at fuel-rich air/fuel ratios from 0.3 to I to provide air/fuel vapors; and said burner means within said combustion chamber includes a mixer means intimately combining said air/fuel vapors for injection into said internal combustion apparatus.
2. The invention as defined in Claim 1 including:
means for preventing flame flash back into said air/fuel mixer means.
means for preventing flame flash back into said air/fuel mixer means.
3. The invention as defined in Claim 2 wherein:
said burner includes a combustion chamber having an inlet means for receiving separate supply of fuel and air;
and said mixer means includes a baffle assembly disposed in said burner means combustion chamber for receiving said combined air/fuel supply in forced impingement relationship to create a mixed vapor.
said burner includes a combustion chamber having an inlet means for receiving separate supply of fuel and air;
and said mixer means includes a baffle assembly disposed in said burner means combustion chamber for receiving said combined air/fuel supply in forced impingement relationship to create a mixed vapor.
4. The invention as defined in Claim 3 wherein:
said baffle assembly includes a cup-like member having a wall adapted to interfere with flow of said combined air/fuel mixture to blend said mixture and redirect the flow; and said burner means having a back wall for receiving said redirected mixture flow adapted to further blend said air/fuel mixture.
said baffle assembly includes a cup-like member having a wall adapted to interfere with flow of said combined air/fuel mixture to blend said mixture and redirect the flow; and said burner means having a back wall for receiving said redirected mixture flow adapted to further blend said air/fuel mixture.
5. The invention as defined in Claim 4 including:
said burner means having an ignition means adjacent to said mixer means for selectively igniting said air/fuel mixture.
said burner means having an ignition means adjacent to said mixer means for selectively igniting said air/fuel mixture.
6. The invention as defined in Claim 5 including:
heat exchanger means disposed in said burner means combustion chamber for vaporizing liquid fuel;
a source of liquid fuel operably connected to said heat exchanger means.
heat exchanger means disposed in said burner means combustion chamber for vaporizing liquid fuel;
a source of liquid fuel operably connected to said heat exchanger means.
7. Apparatus for reducing nitrogen oxide contaminants emitted from an internal combustion power source comprising:
a main fuel supply;
an air supply;
a non-driving burner means haying a combustion chamber operably coupled to said fuel supply and said air supply for receiving a portion of said main fuel and air in close proximity within said burner means;
mixer means carried in said burner means combustion chamber for thoroughly combining said fuel and said air together to form a blend; and ignition means adjacent said mixer means in said combustion chamber and secured to said burner means for igniting said fuel/air blend for discharge into said internal combustion power source.
a main fuel supply;
an air supply;
a non-driving burner means haying a combustion chamber operably coupled to said fuel supply and said air supply for receiving a portion of said main fuel and air in close proximity within said burner means;
mixer means carried in said burner means combustion chamber for thoroughly combining said fuel and said air together to form a blend; and ignition means adjacent said mixer means in said combustion chamber and secured to said burner means for igniting said fuel/air blend for discharge into said internal combustion power source.
8. The invention as defined in Claim 7 wherein:
said mixer means includes spaced-apart walls within said combustion chamber having a first wall adapted to receive impinging fuel portion and air flow adapted to achieve flow reversal to a second wall adapted to receive and redirect impinging fuel portion and air flow to produce a thorough mixture of said fuel/air flow.
said mixer means includes spaced-apart walls within said combustion chamber having a first wall adapted to receive impinging fuel portion and air flow adapted to achieve flow reversal to a second wall adapted to receive and redirect impinging fuel portion and air flow to produce a thorough mixture of said fuel/air flow.
9. The invention as defined in Claim 8 wherein:
said fuel is in a gaseous state.
said fuel is in a gaseous state.
10. The invention as defined in Claim 9 including:
a source of liquid fuel;
heat exchanger means disposed in said burner means for receiving and vaporizing said liquid fuel.
a source of liquid fuel;
heat exchanger means disposed in said burner means for receiving and vaporizing said liquid fuel.
11. The invention as defined in Claim 10 including:
means in said burner means to prevent ignition of said air/fuel mixture in said mixer means.
means in said burner means to prevent ignition of said air/fuel mixture in said mixer means.
12. The invention as defined in Claim 11 including:
means in said mixer means for inducing sudden flow reversals of said fuel/air mixture.
means in said mixer means for inducing sudden flow reversals of said fuel/air mixture.
13. A method of reducing NOX contaminants in an internal combustion power source comprising the steps of:
withdrawing a portion of fuel from a main fuel source;
introducing a quantity of air with said portion of fuel to produce an air/fuel flow;
conducting said air/fuel flow into a mixing assembly by forcibly urging said air/fuel flow into engagement with walls causing flow reversal and thorough mixing of air and fuel to produce a combustible vapor;
igniting said combustible vapor in a burner chamber to produce combustion products; and exhausting said combustion product from the burner into the combustion power source for mixing with main fuel.
withdrawing a portion of fuel from a main fuel source;
introducing a quantity of air with said portion of fuel to produce an air/fuel flow;
conducting said air/fuel flow into a mixing assembly by forcibly urging said air/fuel flow into engagement with walls causing flow reversal and thorough mixing of air and fuel to produce a combustible vapor;
igniting said combustible vapor in a burner chamber to produce combustion products; and exhausting said combustion product from the burner into the combustion power source for mixing with main fuel.
14. The method as defined in Claim 13 wherein: said main fuel is methane and said step of igniting combustible vapor produces hydrogen vapor for discharge into the combustible power source.
15. The method as defined in Claim 14 including the step of:
introducing air and fuel portion vapors into the mixing assembly where said vapors are produced in a heat exchanger converting liquid fuel into said vapors.
introducing air and fuel portion vapors into the mixing assembly where said vapors are produced in a heat exchanger converting liquid fuel into said vapors.
16. The method as defined in Claim 15 including the step of:
preventing flash back ignition if said air/fuel mixture is in the mixing assembly.
preventing flash back ignition if said air/fuel mixture is in the mixing assembly.
17. The method as defined in Claim 16 wherein:
said main fuel is selected from a group of liquid hydrocarbons including gasoline and diesel.
said main fuel is selected from a group of liquid hydrocarbons including gasoline and diesel.
18. In an internal combustion apparatus, the improvement which comprises:
a burner means for combusting air and hydrocarbons at fuel-rich air/fuel ratios within ranges of 0.3 to 1 to provide air/fuel vapors;
said burner means includes a mixer Means intimately combining said air/fuel Vapors for injection into said internal combustion apparatus;
said burner includes a combustion chamber having an inlet means for receiving a supply of fuel and air;
a pre-heater means for heating the supply of fuel and air;
said mixer means includes a baffle wall disposed in said burner means combustion chamber for receiving said pre-heated and combined air/fuel supply in forced impingement relationship to create a mixed vapor;
said baffle wall receiving and re-directing said pre-heated and combined air/fuel mixture within said combustion chamber to further blend said air/fuel mixture;
said mixer means includes a tubular coil for receiving and mixing said air/fuel supply; and said pre-heater means constitutes a heat exchanger employing combusted gases in said combustion chamber to be conducted adjacent to said tubular coil to raise the temperature of said air/fuel mixture preparatory to entering said combustion chamber.
a burner means for combusting air and hydrocarbons at fuel-rich air/fuel ratios within ranges of 0.3 to 1 to provide air/fuel vapors;
said burner means includes a mixer Means intimately combining said air/fuel Vapors for injection into said internal combustion apparatus;
said burner includes a combustion chamber having an inlet means for receiving a supply of fuel and air;
a pre-heater means for heating the supply of fuel and air;
said mixer means includes a baffle wall disposed in said burner means combustion chamber for receiving said pre-heated and combined air/fuel supply in forced impingement relationship to create a mixed vapor;
said baffle wall receiving and re-directing said pre-heated and combined air/fuel mixture within said combustion chamber to further blend said air/fuel mixture;
said mixer means includes a tubular coil for receiving and mixing said air/fuel supply; and said pre-heater means constitutes a heat exchanger employing combusted gases in said combustion chamber to be conducted adjacent to said tubular coil to raise the temperature of said air/fuel mixture preparatory to entering said combustion chamber.
19. The invention as defined in Claim 18 wherein:
said coil terminates in an exit tube opening immediately adjacent to said baffle wall.
said coil terminates in an exit tube opening immediately adjacent to said baffle wall.
20. The invention as defined in Claim 19 wherein:
each coil is of sufficient length so that the air/fuel mixture within the coil is heated within the range of 500 to 1000°F.
each coil is of sufficient length so that the air/fuel mixture within the coil is heated within the range of 500 to 1000°F.
21. In an internal combustion apparatus, the improvement which comprises:
a non-driving burner means having a combustion chamber for combusting air and hydrocarbons at fuel-rich air- fuel ratios within range of 0.3. to 1 to provide air/fuel vapors;
said burner means includes a mixer means in said combustion chamber intimately combining said air/fuel vapors for injection into said internal combustion apparatus;
said burner means includes said combustion chamber having an inlet means for receiving a supply of fuel and air;
a pre-heater means in said combustion chamber for heating the supply of fuel and air;
said mixer means includes a baffle wall disposed in said burner means combustion chamber for receiving said pre-heated and combined air/fuel supply in forced impingement relationship to create a mixed vapor; and said baffle wall receiving and re-directing said pre-heated and combined air/fuel mixture within said combustion chamber to further blend said air/fuel mixture.
a non-driving burner means having a combustion chamber for combusting air and hydrocarbons at fuel-rich air- fuel ratios within range of 0.3. to 1 to provide air/fuel vapors;
said burner means includes a mixer means in said combustion chamber intimately combining said air/fuel vapors for injection into said internal combustion apparatus;
said burner means includes said combustion chamber having an inlet means for receiving a supply of fuel and air;
a pre-heater means in said combustion chamber for heating the supply of fuel and air;
said mixer means includes a baffle wall disposed in said burner means combustion chamber for receiving said pre-heated and combined air/fuel supply in forced impingement relationship to create a mixed vapor; and said baffle wall receiving and re-directing said pre-heated and combined air/fuel mixture within said combustion chamber to further blend said air/fuel mixture.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US07/997,450 US5299536A (en) | 1992-03-27 | 1992-12-28 | Apparatus and method for decreasing nitrogen oxide emissions from internal combustion power sources |
| US07/997,450 | 1992-12-28 |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CA2152671A1 CA2152671A1 (en) | 1994-07-07 |
| CA2152671C true CA2152671C (en) | 1997-02-25 |
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA002152671A Expired - Fee Related CA2152671C (en) | 1992-12-28 | 1993-12-23 | Apparatus and method for decreasing nitrogen oxide emissions from internal combustion power sources |
Country Status (8)
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| US (1) | US5299536A (en) |
| EP (1) | EP0677144A4 (en) |
| KR (2) | KR0148195B1 (en) |
| CA (1) | CA2152671C (en) |
| DE (1) | DE677144T1 (en) |
| ES (1) | ES2080707T1 (en) |
| SG (1) | SG47045A1 (en) |
| WO (1) | WO1994015082A1 (en) |
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| US5441546A (en) | 1993-11-08 | 1995-08-15 | Moard; David | Apparatus and method for decreasing nitrogen oxide emissions from internal combustion power sources |
| US5666923A (en) * | 1994-05-04 | 1997-09-16 | University Of Central Florida | Hydrogen enriched natural gas as a motor fuel with variable air fuel ratio and fuel mixture ratio control |
| KR100294307B1 (en) * | 1994-09-20 | 2001-10-25 | 엠. 모어드 데이비드 | Low oxidation burner with improved injector |
| US5546701A (en) * | 1994-09-20 | 1996-08-20 | Hydrogen Burner Technology, Inc. | Underoxidized burner utilizing improved injectors |
| US6126908A (en) * | 1996-08-26 | 2000-10-03 | Arthur D. Little, Inc. | Method and apparatus for converting hydrocarbon fuel into hydrogen gas and carbon dioxide |
| US6245303B1 (en) | 1998-01-14 | 2001-06-12 | Arthur D. Little, Inc. | Reactor for producing hydrogen from hydrocarbon fuels |
| US6033793A (en) * | 1996-11-01 | 2000-03-07 | Hydrogen Burner Technology, Inc. | Integrated power module |
| US5944510A (en) * | 1996-11-01 | 1999-08-31 | Greiner; Leonard | Dynamic fluid injector |
| US5938800A (en) * | 1997-11-13 | 1999-08-17 | Mcdermott Technology, Inc. | Compact multi-fuel steam reformer |
| US5947063A (en) * | 1997-11-18 | 1999-09-07 | Southwest Research Institute | Stoichiometric synthesis, exhaust, and natural-gas combustion engine |
| DE69910334T2 (en) * | 1998-03-26 | 2004-06-24 | Pugachev, Aleksandr Vasilievič | METHOD AND DEVICE FOR TREATING AN AIR-FUEL MIXTURE FOR INTERNAL COMBUSTION ENGINES AND HEAT EXCHANGERS |
| US6089859A (en) | 1998-06-19 | 2000-07-18 | Hydrogen Burner Technology, Inc. | Reduced carbon from under oxidized burner |
| WO2000012888A2 (en) * | 1998-08-27 | 2000-03-09 | Tyma, Inc. | Fuel supply system for a vehicle including a vaporization device for converting fuel and water into hydrogen |
| US6641625B1 (en) | 1999-05-03 | 2003-11-04 | Nuvera Fuel Cells, Inc. | Integrated hydrocarbon reforming system and controls |
| JP4393002B2 (en) * | 2001-02-01 | 2010-01-06 | ヤンマー株式会社 | Gas engine |
| CA2410927A1 (en) * | 2002-11-05 | 2004-05-05 | Michel Petitclerc | Electrically heated reactor for reforming in gaseous phase |
| US6739125B1 (en) | 2002-11-13 | 2004-05-25 | Collier Technologies, Inc. | Internal combustion engine with SCR and integrated ammonia production |
| AU2003903283A0 (en) * | 2003-06-26 | 2003-07-10 | H.A.C. Technologies Pty Ltd | Reformate assisted combustion |
| WO2015182694A1 (en) * | 2014-05-28 | 2015-12-03 | 日野自動車 株式会社 | Burner and fuel vaporizing device |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4036186A (en) * | 1973-06-04 | 1977-07-19 | Nippon Soken, Inc. | Air-fuel mixture ratio correcting system for carburetor |
| US3982910A (en) * | 1974-07-10 | 1976-09-28 | The United States Of America As Represented By The Administrator Of The National Aeronautics And Space Administration | Hydrogen-rich gas generator |
| JPS58584B2 (en) * | 1975-03-05 | 1983-01-07 | カブシキガイシヤ ニツポンジドウシヤブヒンソウゴウケンキユウシヨ | ``Ninenkikan'' |
| DE2614670A1 (en) * | 1976-04-05 | 1977-10-13 | Siemens Ag | GAS GENERATOR FOR THE CATALYTIC CONVERSION OF LIQUID, HYDROCARBON-CONTAINING FUEL WITH AN OXYGEN-CONTAINING GAS AT INCREASED TEMPERATURE INTO A FUEL GAS, IN PARTICULAR FROM FUEL FUEL |
| US4090485A (en) * | 1977-03-28 | 1978-05-23 | Antonio LaCreta | Fuel systems for internal combustion engines |
| US4157084A (en) * | 1977-09-20 | 1979-06-05 | Wallis Marvin E | Fuel injection system and method for internal combustion engine |
| US4350133A (en) * | 1980-05-19 | 1982-09-21 | Leonard Greiner | Cold start characteristics of ethanol as an automobile fuel |
| US5002481A (en) * | 1986-08-08 | 1991-03-26 | Forschungszentrum Julich Gmbh | Apparatus for generating a combustible gaseous mixture |
| US4861348A (en) * | 1986-10-08 | 1989-08-29 | Hitachi, Ltd. | Fuel reforming apparatus |
| US4737161A (en) * | 1987-01-27 | 1988-04-12 | International Fuel Cells Corporation | Compact hydrogen generator |
| US5115787A (en) * | 1991-09-24 | 1992-05-26 | Texas Instruments Incorporated | Spark ignition combustion engine of the fuel injection type and heating element therefor |
| US5207185A (en) * | 1992-03-27 | 1993-05-04 | Leonard Greiner | Emissions reduction system for internal combustion engines |
-
1992
- 1992-12-28 US US07/997,450 patent/US5299536A/en not_active Expired - Fee Related
-
1993
- 1993-12-23 KR KR1019950702679A patent/KR0148195B1/en active
- 1993-12-23 EP EP94905521A patent/EP0677144A4/en not_active Withdrawn
- 1993-12-23 DE DE0677144T patent/DE677144T1/en active Pending
- 1993-12-23 ES ES94905521T patent/ES2080707T1/en active Pending
- 1993-12-23 SG SG1996004084A patent/SG47045A1/en unknown
- 1993-12-23 WO PCT/US1993/012576 patent/WO1994015082A1/en not_active Application Discontinuation
- 1993-12-23 CA CA002152671A patent/CA2152671C/en not_active Expired - Fee Related
- 1993-12-23 KR KR1019950702679A patent/KR960700397A/en not_active IP Right Cessation
Also Published As
| Publication number | Publication date |
|---|---|
| US5299536A (en) | 1994-04-05 |
| KR960700397A (en) | 1996-01-20 |
| EP0677144A4 (en) | 1995-12-20 |
| SG47045A1 (en) | 2000-02-22 |
| WO1994015082A1 (en) | 1994-07-07 |
| KR0148195B1 (en) | 1998-08-17 |
| ES2080707T1 (en) | 1996-02-16 |
| CA2152671A1 (en) | 1994-07-07 |
| DE677144T1 (en) | 1996-09-19 |
| EP0677144A1 (en) | 1995-10-18 |
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Legal Events
| Date | Code | Title | Description |
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| EEER | Examination request | ||
| MKLA | Lapsed |