US20050188605A1 - Reduced-emissions combustion utilizing multiple-component metallic combustion catalyst - Google Patents

Reduced-emissions combustion utilizing multiple-component metallic combustion catalyst Download PDF

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Publication number
US20050188605A1
US20050188605A1 US11/038,371 US3837105A US2005188605A1 US 20050188605 A1 US20050188605 A1 US 20050188605A1 US 3837105 A US3837105 A US 3837105A US 2005188605 A1 US2005188605 A1 US 2005188605A1
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United States
Prior art keywords
fuel
ppm
cerium
diesel
platinum
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Abandoned
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US11/038,371
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English (en)
Inventor
James Valentine
Barry Sprague
Jeremy Peter-Hoblyn
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Clean Diesel Technologies Inc
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Clean Diesel Technologies Inc
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Priority claimed from PCT/US2001/014789 external-priority patent/WO2001085876A1/en
Priority claimed from US10/290,798 external-priority patent/US7063729B2/en
Application filed by Clean Diesel Technologies Inc filed Critical Clean Diesel Technologies Inc
Priority to US11/038,371 priority Critical patent/US20050188605A1/en
Publication of US20050188605A1 publication Critical patent/US20050188605A1/en
Priority to SG200803902-6A priority patent/SG143272A1/en
Priority to CN2006800086843A priority patent/CN101160379B/zh
Priority to EP06718828A priority patent/EP1846540A4/en
Priority to BRPI0606586-4A priority patent/BRPI0606586A2/pt
Priority to PCT/US2006/001815 priority patent/WO2006078764A2/en
Priority to CA002595315A priority patent/CA2595315A1/en
Priority to MX2007008818A priority patent/MX2007008818A/es
Priority to KR1020077018828A priority patent/KR101077015B1/ko
Priority to JP2007552249A priority patent/JP5020830B2/ja
Priority to RU2007129120/04A priority patent/RU2007129120A/ru
Priority to AU2006206468A priority patent/AU2006206468A1/en
Assigned to CLEAN DIESEL TECHNOLOGIES, INC. reassignment CLEAN DIESEL TECHNOLOGIES, INC. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: PETER-HOBLYN, JEREMY D., SPRAGUE, BARRY N., VALENTINE, JAMES M.
Priority to ZA200706580A priority patent/ZA200706580B/en
Priority to NO20074181A priority patent/NO20074181L/no
Priority to HK08110458.6A priority patent/HK1114875A1/xx
Abandoned legal-status Critical Current

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    • C10L1/00—Liquid carbonaceous fuels
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    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/105—General auxiliary catalysts, e.g. upstream or downstream of the main catalyst
    • F01N3/106—Auxiliary oxidation catalysts
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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    • F02D19/00—Controlling engines characterised by their use of non-liquid fuels, pluralities of fuels, or non-fuel substances added to the combustible mixtures
    • F02D19/06—Controlling engines characterised by their use of non-liquid fuels, pluralities of fuels, or non-fuel substances added to the combustible mixtures peculiar to engines working with pluralities of fuels, e.g. alternatively with light and heavy fuel oil, other than engines indifferent to the fuel consumed
    • F02D19/0639—Controlling engines characterised by their use of non-liquid fuels, pluralities of fuels, or non-fuel substances added to the combustible mixtures peculiar to engines working with pluralities of fuels, e.g. alternatively with light and heavy fuel oil, other than engines indifferent to the fuel consumed characterised by the type of fuels
    • F02D19/0649—Liquid fuels having different boiling temperatures, volatilities, densities, viscosities, cetane or octane numbers
    • F02D19/0652—Biofuels, e.g. plant oils
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    • 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
    • F02M25/14—Engine-pertinent apparatus for adding non-fuel substances or small quantities of secondary fuel to combustion-air, main fuel or fuel-air mixture adding anti-knock agents, not provided for in subgroups F02M25/022 - F02M25/10
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    • F02M27/00—Apparatus for treating combustion-air, fuel, or fuel-air mixture, by catalysts, electric means, magnetism, rays, sound waves, or the like
    • F02M27/02—Apparatus for treating combustion-air, fuel, or fuel-air mixture, by catalysts, electric means, magnetism, rays, sound waves, or the like by catalysts
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    • C10L1/1241—Inorganic compounds oxygen containing compounds, e.g. oxides, hydroxides, acids and salts thereof metal carbonyls
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    • C10L1/1888—Carboxylic acids; metal salts thereof tall oil
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    • F01N2430/00—Influencing exhaust purification, e.g. starting of catalytic reaction, filter regeneration, or the like, by controlling engine operating characteristics
    • F01N2430/04—Influencing exhaust purification, e.g. starting of catalytic reaction, filter regeneration, or the like, by controlling engine operating characteristics by adding non-fuel substances to combustion air or fuel, e.g. additives
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    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
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    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
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    • F01N3/033—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters in combination with other devices
    • F01N3/035—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters in combination with other devices with catalytic reactors, e.g. catalysed diesel particulate filters
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    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
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    • Y02T10/10—Internal combustion engine [ICE] based vehicles
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    • Y02T10/30—Use of alternative fuels, e.g. biofuels

Definitions

  • the invention concerns new compositions and a new process for improving the efficiency of fossil fuel combustion sources.
  • Utilizing a fuel containing a fuel-soluble catalyst comprised of platinum and at least one additional metal reduces production of pollutants of the type generated by incomplete combustion, e.g., particulates, unburned hydrocarbons and carbon monoxide.
  • Diesel engines have a number of important advantages over engines of the Otto type. Among them are fuel economy, ease of repair and long life. From the standpoint of emissions, however, they present problems more severe than their spark-ignition counterparts. Emission problems relate to particulates, nitrogen oxides (NO x ), unburned hydrocarbons (HC) and carbon monoxide (CO). As engine operation modifications are made to reduce particulates and unburned hydrocarbons on diesel engines, the NO x emissions tend to increase.
  • NO x nitrogen oxides
  • HC unburned hydrocarbons
  • CO carbon monoxide
  • DPFs diesel particulate filters
  • DOCs diesel oxidation catalysts
  • FBCs fuel borne catalysts
  • particulate emissions are limited to 100,000 ⁇ g/hp-hr (0.1 gram/hp-hr).
  • a cerium FBC used at 30 ppm in fuel represents a metal catalyst input loading to the engine of 6000 ⁇ g/hp-hr of metal or roughly 6% of untreated engine emissions.
  • the fuel employed according to the invention comprises carbonaceous fuel, e.g., fossil fuel, containing low or ultra low levels of catalyst metal additives.
  • the catalyst metal additives will preferably be soluble or dispersible in the fuel and contain platinum and cerium and/or iron compositions.
  • the invention provides a diesel fuel for powering a diesel engine with reduced emission of particulates without the need for an after treatment device, comprising: a base fuel comprising distillate, and a fuel borne catalyst comprising platinum and cerium and/or iron, wherein the platinum is employed at a level of from 0.05 to 0.5 ppm, e.g., 0.1 to 0.5 ppm, and the levels of cerium or iron being from 5 to 10 ppm.
  • the diesel fuel contains less than 0.05% sulfur.
  • the cerium and/or iron are present at total concentrations of from 0.5 to less than 8 ppm.
  • the invention provides a method for reducing the emissions of particulates, hydrocarbons and carbon monoxide from a diesel engine directly out of the engine prior to contact with an oxidizer or particulate trap comprising: adding a fuel-soluble platinum group metal composition and at least one other catalytic compound comprising fuel-soluble compounds of cerium and/or iron to a diesel fuel to lower the emissions of particulates, unburned hydrocarbons and carbon monoxide, wherein the platinum is employed at a level of from 0.05 to 0.5 ppm, e.g., 0.1 to 0.5 ppm, and the levels of cerium and/or iron being from 5 to 10 ppm; and operating a diesel engine with the fuel.
  • the invention can be described as providing a process for improving combustion of pilot fuel in a dual-fuel diesel engine, which operates principally on natural gas, comprising: adding to a pilot fuel, a multi catalyst composition comprising platinum at concentrations of from only 0.0005 to less than 0.15 ppm and cerium and/or iron at total concentrations of from only 0.5 to less than 8 ppm.
  • the invention is seen as providing a process for combusting a carbonaceous fuel comprising: mixing with fuel or combustion air a multi-component combustion catalyst comprising a platinum composition and cerium and/or iron compositions at levels reduced to as low as 0.0005 ppm for platinum and levels as low as 0.5 ppm for the cerium and iron; and combusting fuel with air in the presence of the catalyst in a regimen of treatment that will utilize effective catalyst levels for a time and under conditions, which will achieve one or more of the noted improvements.
  • a process for combusting a carbonaceous fuel comprising: mixing with fuel or combustion air a multi-component combustion catalyst comprising a platinum composition and cerium and/or iron compositions at levels of from about 0.0005 to 2 ppm for platinum and levels of from about 1 to 25 ppm for the cerium and iron; combusting fuel with air in the presence of the catalyst in a regimen of treatment that will utilize effective catalyst levels for a time and under conditions, which will achieve one or more of the noted improvements; then, for at least a period of time changing the amount of catalyst utilized by mixing with fuel or combustion air a multi-component combustion catalyst comprising a platinum composition and cerium and/or iron compositions at levels reduced to as low as 0.0005 ppm for platinum and levels as low as 0.5 ppm for the cerium and iron; and combusting fuel with air in the presence of the catalyst in a regimen of treatment that will utilize effective catalyst levels for a time and under conditions, which will achieve one or more of the noted improvements.
  • the invention provides a process for combusting a carbonaceous fuel comprising: for at least a part of a treatment regimen utilizing higher catalyst concentrations, e.g., platinum at 0.5 to 2.0 ppm and cerium at 7.5 to 15 ppm; mixing with fuel a multi-component combustion catalyst comprising a platinum composition and cerium and/or iron compositions at levels of 0.0005 to less than 0.15 ppm for platinum and levels of 0.05 to less than 1.0 ppm for the cerium and iron; and combusting the fuel with air in a regimen of treatment that will achieve one or more of the noted improvements.
  • a multi-component combustion catalyst comprising a platinum composition and cerium and/or iron compositions at levels of 0.0005 to less than 0.15 ppm for platinum and levels of 0.05 to less than 1.0 ppm for the cerium and iron
  • FIG. 1 is a graph summarizing the data from Example 3, wherein a platinum/cerium fuel borne catalyst (FBC) at low concentrations was evaluated on several fuels on a diesel engine.
  • FBC platinum/cerium fuel borne catalyst
  • FIG. 2 is a graph summarizing the data from Example 6, wherein a platinum/cerium fuel borne catalyst (FBC) at low concentrations was evaluated on several fuels on a diesel engine.
  • FBC platinum/cerium fuel borne catalyst
  • FIG. 3 is a graph summarizing the data from Example 7, wherein a platinum/cerium fuel borne catalyst (FBC) at low concentrations was evaluated on several fuels on a diesel engine.
  • FBC platinum/cerium fuel borne catalyst
  • the use of low and ultra-low individual and combined catalyst levels is significant in several regards, including the great reduction in catalyst solids which can accumulate within a system or are exhausted.
  • the invention can reduce pollutants without the use of after-treatment devices and can enhance after treatment due to the reduced production of particulates and the increased ability to burn off carbon deposits.
  • Cerium and iron levels are reduced to levels as low as 0.05 ppm and platinum levels are reduced to levels as low as 0.0005 ppm.
  • a regimen of treatment will utilize effective levels within the low and ultra-low ranges for a time and under conditions, which will achieve one or more of the noted improvements.
  • the invention relates to improving combustion of diesel fuels, which typically comprise a fossil fuel, such as any of the typical petroleum-derived fuels including distillate fuels.
  • the diesel fuel can be of any of those formulations disclosed in the above priority patent applications, which are incorporated by reference herein in their entireties.
  • a fuel can be one or a blend of fuels selected from the group consisting of distillate fuels, including diesel fuel, e.g., No. 2 Diesel fuel, No. 1 Diesel fuel, jet fuel, e.g., Jet A, or the like which is similar in boiling point and viscosity to No.
  • Diesel fuel, ultra low sulfur diesel fuel (ULSD) and biologically-derived fuels such as those comprising a “mono-alkyl ester-based oxygenated fuel”, i.e., fatty acid esters, preferably methyl esters of fatty acids derived from triglycerides, e.g., soybean oil, Canola oil and/or tallow.
  • a “mono-alkyl ester-based oxygenated fuel” i.e., fatty acid esters, preferably methyl esters of fatty acids derived from triglycerides, e.g., soybean oil, Canola oil and/or tallow.
  • Jet A and Diesel No. 1 are deemed equivalent for applications of the invention, but are covered by different American Society For Testing and Materials (ASTM) specifications.
  • the diesel fuels are covered by ASTM D 975, “Standard Specification for Diesel Fuel Oils”. Jet A has the designation of ASTM D 1655, “Standard Specification for Aviation Turbine Fuels”.
  • the term ultra low sulfur diesel fuel (ULSD) means No. 1 or No. 2 diesel fuels with a sulfur level no higher than 0.0015 percent by weight (15 ppm) and some jurisdictions require a low aromatic hydrocarbon content e.g., less than ten percent by volume.
  • low aromatic content ultralow sulfur diesel (LA ULSD) fuel as used herein means that this component of the fuel will have an aromatic content in volume percent of less than 10%, and preferably of from 1 to 8%, particularly in the range of from 2 to 5%.
  • the table below shows typical analyses of a No. 2 diesel and low aromatic ultralow sulfur diesel fuels LA ULSD, in addition to a formulation also containing a biodiesel component (LA ULSD with FBC and 20% Bio-Diesel). Typical No.
  • Biodiesel typically comprises a minor proportion of a diesel fuel blend, typically from about 1 to 35%, e.g., on the order of 15 to 25%. Blends will typically contain about 20% biodiesel, wherein this biologically-derived fuel component will be comprised of a “mono-alkyl ester-based oxygenated fuel”, i.e., fatty acid esters, preferably from fatty acids derived from triglycerides such as soybean oil, Canola oil and/or tallow.
  • a “mono-alkyl ester-based oxygenated fuel” i.e., fatty acid esters, preferably from fatty acids derived from triglycerides such as soybean oil, Canola oil and/or tallow.
  • fatty acid ester(s) is intended to include any compound wherein the alcohol portion is easily removed, including polyols and substituted alcohols, etc., but are preferably esters of volatile alcohols, e.g., the C 1 -C 4 alcohols (preferably methyl), 2-methoxy ethyl and benzyl esters of fatty acids containing about eight or more (e.g., 8 to 22) carbon atoms, and mixtures of such esters. Volatile alcohols are highly desirable. Methyl esters are the most highly preferred ester reactants. Suitable ester reactants can be prepared by the reaction of diazoalkanes and fatty acids, or derived by alcoholysis from the fatty acids naturally occurring in fats and oils.
  • Suitable fatty acid esters can be derived from synthetic or natural, saturated or unsaturated fatty acids and include positional and geometrical isomers.
  • Suitable preferred saturated fatty acids include caprylic, capric, lauric, myristic, palmitic, stearic, arachidic, behenic, isomyristic, isomargaric, myristic, caprylic, and anteisoarachadic.
  • Suitable preferred unsaturated fatty acids include myristoleic, palmitoleic, ricinoleic, linoleic, oleic, elaidic, linolenic, eleasteric, arachidonic, erucic, and erythrogenic acids.
  • fatty acids derived from soybean oil, palm oil, safflower oil, rapeseed oil, Canola (low erucic acid), and corn oil are especially preferred for use herein.
  • the fatty acids can be used “as is,” and/or after hydrogenation, and/for isomerization, and/for purification.
  • rapeseed provides a good source for C 22 fatty acids
  • C 16 -C 18 fatty acids can be provided by tallow, soybean oil, or cottonseed oil
  • shorter chain fatty acids can be provided by coconut, palm kernel, or babassu oils.
  • Lard, olive oil, peanut oil, sesame seed oil, and sunflower seed oil, are other natural sources of fatty acids.
  • Preferred esters comprised in the biodiesel are lower alkyl esters, e.g., methyl, ethyl, propyl and butyl, particularly methyl esters of soybean and or tallow fatty acids.
  • biodiesel B100
  • biodiesel is defined as the mono alkyl esters of long chain fatty acids derived from vegetable oils or animal fats, for use in compression-ignition (diesel) engines. This specification is for pure (100%) biodiesel prior to use or blending with diesel fuel.
  • One product of this type is available under the trademark BioDiesel by Members of the National BioDiesel Board and is identified as “Methyl Soyate, Rapeseed Methyl Ester (RME), Methyl Tallowate”.
  • the manufacturer also refers to the fuel as “a mono-alkyl ester-based oxygenated fuel, a fuel made from vegetable oil or animal fats.” It is said to contain 11% oxygen by weight. They describe the product as Methyl esters from lipid sources, CAS Number 67784-80-9.
  • the process of the invention employs a fuel-soluble, multi-metal catalyst, preferably comprising fuel-soluble platinum and either cerium or iron or both cerium and iron.
  • the cerium and/or iron are typically employed at concentrations of from 0.5 to 20 ppm and the platinum from 0.0005 to 2 ppm, with preferred levels of cerium and/or iron being from 5 to 10 ppm, e.g., 7.5 ppm, and the platinum being employed at a level of from 0.0005 to 0.5 ppm, e.g., less than 0.15 ppm, and in some cases less than 0.1 ppm, say 0.01 to 0.09 ppm.
  • the treatment regimen can call for the utilizing higher catalyst concentrations initially or at defined intervals or as needed—but not for the whole treatment as has been necessary in the past.
  • platinum concentrations can be as high as 1 ppm or even up to 2 ppm, as needed.
  • the cerium and/or iron are preferred at levels of cerium and/or iron being from 2 to 10 ppm, e.g., 3-8 ppm, and the platinum being employed at a level of from 0.05 to 0.5 ppm, e.g., from 0.1 to 0.5 ppm, e.g., 0.15 ppm, for typical operations. The tests below, run at these levels show surprising results in terms of engine out emissions.
  • a preferred ratio of cerium and/or iron to platinum is from 100,000:1 to 3:1, e.g., in the range of from 100:1 to 20,000:1, but more typically will be from 50,000:1 to 500:1.
  • a preferred ratio within the above ranges and shown surprisingly effective by testing will have a ratio of cerium and/or iron to platinum at from 75:1 to 10:1.
  • a formulation using 0.15 ppm platinum with 10 ppm of cerium and 5 ppm of iron is exemplary.
  • Another, preferred formulation will contain 0.15 ppm platinum and 7.5 ppm cerium.
  • Another advantage of low levels of catalyst (about 3 to 15 ppm total), preferably below 12 ppm and more preferably below 8 ppm, is the reduction in ultra fine particles resulting from metal oxide emissions.
  • a cerium FBC used at 30 ppm in fuel represents a metal catalyst input loading to the engine of 6000 ⁇ g/hp-hr of metal or roughly 6% of untreated engine emissions. Therefore, low levels of catalyst used in the present invention of less than 8 ppm and preferably 4 ppm as a bimetallic or trimetallic FBC will, for example, contribute only 800-1600 ⁇ g/hp-hr of catalyst loading to the engine or 0.8-1.6% of baseline soot emissions. This has the advantage of reduced metal ash emissions and reduces the contribution of the FBC to overall particulate mass emissions or loading of metal ash to downstream emission control devices.
  • the fuel can contain detergent (e.g., 50-300 ppm), lubricity additive (e.g., 25 to about 500 ppm), other additives, and suitable fuel-soluble catalyst metal compositions, e.g., 0.1-2 ppm fuel soluble platinum group metal composition, e.g., platinum COD or platinum acetylacetonate and/or 2-20 ppm fuel soluble cerium or iron composition, e.g., cerium as a soluble compound or suspension, cerium octoate, ferrocene, iron oleate, iron octoate and the like.
  • the fuel as defined, is combusted without the specific need for other treatment devices although they can be used especially for higher levels of control on diesels.
  • a combination of platinum with iron and/or cerium at low concentrations in fuels is as effective as much higher concentrations of cerium, iron or other metals without platinum in reducing carbon or soot deposits or emissions. Concentrations of a few ppm metals in combination are as effective as 30-100 ppm of iron and/or cerium used alone.
  • the process of the invention will comprise: mixing with fuel or combustion air a multi-component combustion catalyst comprising a platinum composition and cerium and/or iron compositions at levels reduced to as low as 0.0005 ppm for platinum and levels as low as 0.5 ppm for the cerium and iron; and combusting fuel with air in the presence of the catalyst in a regimen of treatment that will utilize effective catalyst levels for a time and under conditions, which will achieve one or more of the noted improvements.
  • low catalyst levels can be employed for at least a portion of a treatment regimen, which can also include employing a higher initial dose and/or intermittently using higher catalyst levels.
  • the invention also has significant beneficial use in the area of dual-fuel diesel engines, which although they operate principally on natural gas, utilize a more smoke-producing pilot fuel such as regular diesel fuel.
  • the catalyst concentrations according to the invention can be the above-noted low catalyst levels for at least a part of a treatment regimen, with platinum concentrations of from only 0.6005 to less than 0.15, e.g., less than 0.1, ppm and cerium and/or iron at total concentrations of from only 0.5 to less than 8 ppm. In some cases, it will be useful to utilize less than 0.05 ppm platinum and a total catalyst level of less than 5 ppm.
  • bimetallic and trimetallic platinum combinations are compatible with standard additive components for distillate and residual fuels such as pour point reducers, antioxidant, corrosion inhibitors and the like.
  • cerium III acetylacetonate cerium III napthenate, and cerium octoate, cerium oleate and other soaps such as stearate, neodecanoate, and other C 6 to C 24 alkanoic acids, and the like.
  • the cerium is preferred at concentrations of 1 to 15 ppm cerium w/v of fuel, e.g., 4 to 15 ppm.
  • the cerium is supplied as cerium hydroxy oleate propionate complex (40% cerium by weight) or a cerium octoate (12% cerium by weight). Preferred levels are toward the lower end of this range.
  • iron compounds include ferrocene, ferric and ferrous acetyl-acetonates, iron soaps like octoate and stearate (commercially available as Fe(III) compounds, usually), iron napthenate, iron tallate and other C 6 to C 24 alcanoic acids, iron penta carbonyl Fe(CO) 5 and the like.
  • platinum group metal compositions e.g., 1,5-cyclooctadiene platinum diphenyl (platinum COD), described in U.S. Pat. No. 4,891,050 to Bowers, et al., U.S. Pat. No. 5,034,020 to Epperly, et al., and U.S. Pat. No. 5,266,083 to Peter-Hoblyn, et al., can be employed as the platinum source.
  • platinum COD 1,5-cyclooctadiene platinum diphenyl
  • platinum group metal catalyst compositions include commercially-available or easily-synthesized platinum group metal acetylacetonates, including substituted (e.g., alkyl, aryl, alkyaryl substituted) and unsubstituted acetylacetonates, platinum group metal dibenzylidene acetonates, and fatty acid soaps of tetramine platinum metal complexes, e.g., tetramine platinum oleate.
  • the platinum is preferred at concentrations of 0.05-2.0 ppm platinum w/v (mg per liter) of fuel, e.g., up to about 1.0 ppm.
  • Preferred levels are toward the lower end of this range, e.g., 0.15-0.5 ppm.
  • Platinum COD is the preferred form of platinum for addition to the fuel.
  • the cerium or iron are typically employed at concentrations to provide from 0.5 to 25 ppm of the metal and the platinum from 0.0005 to 2 ppm, with preferred levels of cerium or iron being from 5 to 10 ppm, e.g., 7.5 ppm, and the platinum being employed at a level of from 0.1 to 0.5 ppm, e.g., 0.15 ppm.
  • a preferred ratio of cerium and/or iron to platinum is from 100,000:1 to 10:1, e.g., from 50,000:1 to 500:1.
  • a formulation using 0.0015 ppm platinum with 10 ppm of cerium and 5 ppm of iron is exemplary, with a ratio of cerium plus iron to platinum of about 10,000:1.
  • An alternative exemplary composition will contain 0.0015 ppm platinum with 10 ppm of iron and 5 ppm of cerium.
  • Another will contain from 3 to 10 ppm of a combination of Ce and Fe along with 0.1 to 0.5 ppm platinum.
  • Another fuel of preference will contain from 0.05 to 0.5 ppm platinum and the levels of cerium and/or iron of from 0.5 to 10 ppm, especially wherein the cerium and/or iron are present at total concentrations of from 3 to 8 ppm.
  • the combustion according to the invention can be of an emulsion with water, wherein an oil phase is emulsified with water, the water comprising from 1 to 30% water based on the weight of the diesel fuel.
  • the emulsion will be predominantly of the water-in-oil type and will preferably contain surfactants, lubricity additives and/or corrosion inhibitors in addition to the other components mentioned above.
  • surfactants lubricity additives and/or corrosion inhibitors in addition to the other components mentioned above.
  • suitable emulsion forms and additives is found in U.S. Pat. No. 5,743,922.
  • Combustion can improve combustion efficiency and reduce particulates without the use of oxidation catalysts or particulate filters for enhanced emissions control on diesel engines. Also, better carbon burn out in open flame combustion sources will lead to lower carbon deposits on heat transfer surfaces and lower soot oxidation temperatures on downstream heat recovery devices.
  • the fuels of the invention comprising a base fuel and low levels of fuel borne catalysts based on platinum and cerium and/or iron compounds, provide better engine out emissions than the prior art, yet further provide unexpectedly good results in terms of PM, HC, CO, NO x and NO 2 as a percentage of NO x when used with an after treatment device such as a diesel oxidation catalyst (DOC) or diesel particulate filter (DPF).
  • DOC diesel oxidation catalyst
  • DPF diesel particulate filter
  • Other devices including particulate reactors, partial filters or NO x adsorbers can also be used and benefit from reduced engine out emissions of the current invention.
  • diesel particulate filter is meant to refer to those devices known in the art as exhaust gas filters that reduce particulate emissions by trapping a portion of the particulates within a complex internal structure.
  • diesel oxidation catalyst is meant to refer to those devices known in the art as exhaust gas treatment catalysts that reduce particulate, hydrocarbon and carbon monoxide emissions by causing contact with catalyzed surfaces in lieu of trapping particulates as done in the diesel particulate filters. See the examples below, for the engine out results and the benefits of the FBC with catalyzed after treatment devices to reduce NO 2 and particulate emissions.
  • NO 2 is a strong lung irritant and can be generated in large quantities by traditional use of heavily catalyzed aftertreatment devices such as DOCs, DPFs or combinations.
  • This example describes the preparation of a low-emissions diesel fuel according to a preferred aspect of the invention a fuel is blended using the Colonial Pipeline Company fungible aviation kerosene grade 55 analyzed above (Jet A, and similar in boiling and viscosity to No. 1 Diesel), with additives (100 ppm of the TFA 4690-C detergent, 225 ppm of the noted Texaco lubricity additive) and a fuel borne catalyst (FBC) containing 0.15 ppm platinum supplied as platinum COD and 7.5 ppm cerium supplied as cerium hydroxy oleate propionate complex (solution containing 40% cerium by weight).
  • FBC fuel borne catalyst
  • ppm values are, again weight of metal in mg per volume of fuel in liters
  • the fuel was used in a test of a 1998 DDC Detroit Diesel Series 60, 400 hp engine and showed remarkably improved results as compared to a reference on highway No 2 or a CARB ULSD (California Air Resources Board Ultra Low Sulfur Diesel) fuel.
  • HCDOC heavily catalyzed diesel oxidation catalyst
  • LCWMF lightly catalyzed wire mesh filter
  • PGM platinum group metal
  • ULSD fuel produced reduction in particulates of 59%, but increased NO 2 emissions to 58% of total nitrogen oxide species.
  • the cerium additive was cerium hydroxy propionate oleate and the platinum additive was platinum COD.
  • This transient cycle is described by means of percent of maximum torque and percent of rated speed for each one-second interval over a test cycle of 1199 second duration.
  • the first five minutes of the cycle is designated as the New York Non-Freeway (NYNF) portion of the test and represents city operation with extensive idle time.
  • the second five minutes is called the Los Angeles Non Freeway (LANF) portion.
  • the third five minute section of the test is called the Los Angeles Freeway (LAF) portion. This is representative of high speed freeway operation.
  • the final five minutes is a repeat of the NYNF portion.
  • Results represent the mean of triplicate “hot-start” repeat tests for each fuel.
  • Results are presented graphically for reduction in emissions of hydrocarbons (HC), carbon monoxide (CO), nitrogen oxides (NO x ) and particulates (PM) for each fuel tested relative to emissions from a standard No. 2 on-highway reference fuel containing 386 ppm sulfur.
  • HC hydrocarbons
  • CO carbon monoxide
  • NO x nitrogen oxides
  • PM particulates
  • Additive A delivered 0.15/4/4 ppm Pt/Ce/Fe; Additive B delivered 0.15 ppm/7.5 ppm Pt/Ce; and Additive C delivered 0.15/5.6/2.4 ppm Pt/Ce/Fe. All additives contained the same commercial detergent package to assist with stability of the catalyst. Results show similar reductions for all three additives in HC, CO, NOx and NO 2 . Particulate reductions for bimetallic Additive B appear slightly better at 32% versus baseline No. 2D while Additives A and C both delivered PM reduction of 25%. In all cases the blend of additive with the ULSD provided unexpectedly good reduction in NOx and NO 2 .
  • a trimetallic may present cost advantages versus a bimetallic or may be preferred for use in regeneration of exhaust aftertreatment devices such as DOCs, DPFs, wire mesh filters or combined systems.

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US11/038,371 US20050188605A1 (en) 2000-08-01 2005-01-19 Reduced-emissions combustion utilizing multiple-component metallic combustion catalyst
JP2007552249A JP5020830B2 (ja) 2005-01-19 2006-01-19 多成分金属燃焼触媒を使用する低排出物燃焼
RU2007129120/04A RU2007129120A (ru) 2005-01-19 2006-01-19 Использование многокомпонентного металлосодержащего катализатора для горения с более низкими выбросами
AU2006206468A AU2006206468A1 (en) 2005-01-19 2006-01-19 Reduced-emissions combustion utilizing multiple-component metallic combustion catalyst
CA002595315A CA2595315A1 (en) 2005-01-19 2006-01-19 Reduced-emissions combustion utilizing multiple-component metallic combustion catalyst
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EP06718828A EP1846540A4 (en) 2005-01-19 2006-01-19 REDUCED EMISSION COMBUSTION OBTAINED BY MEANS OF A MULTI-COMPONENT METAL COMBUSTION CATALYST
BRPI0606586-4A BRPI0606586A2 (pt) 2005-01-19 2006-01-19 combustão de emissões reduzidas utilizando catalisador de combustão metálico de múltiplos componentes
PCT/US2006/001815 WO2006078764A2 (en) 2005-01-19 2006-01-19 Reduced-emissions combustion utilizing multiple-component metallic combustion catalyst
SG200803902-6A SG143272A1 (en) 2005-01-19 2006-01-19 Reduced-emissions combustion utilizing multiple-component metallic combustion catalyst
MX2007008818A MX2007008818A (es) 2005-01-19 2006-01-19 Combustion de emisiones reducidas que utiliza catalizador metalico de combustion de varios componentes.
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CA2595315A1 (en) 2006-07-27
KR20070094861A (ko) 2007-09-21
WO2006078764A3 (en) 2007-10-04
NO20074181L (no) 2007-10-12
EP1846540A2 (en) 2007-10-24
EP1846540A4 (en) 2009-12-30
AU2006206468A1 (en) 2006-07-27
HK1114875A1 (en) 2008-11-14
RU2007129120A (ru) 2009-02-27
CN101160379B (zh) 2012-05-02
JP5020830B2 (ja) 2012-09-05
CN101160379A (zh) 2008-04-09
KR101077015B1 (ko) 2011-10-26
MX2007008818A (es) 2007-09-27
ZA200706580B (en) 2008-06-25
JP2008526510A (ja) 2008-07-24
SG143272A1 (en) 2008-06-27
BRPI0606586A2 (pt) 2009-07-07
WO2006078764A2 (en) 2006-07-27

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