EP0078249B1 - Additif améliorant la combustion et réduisant la formation de noir de fumée des huiles combustibles, carburant diesel et autres combustibles et carburants liquides ainsi que ce combustible et carburant liquide en soi - Google Patents

Additif améliorant la combustion et réduisant la formation de noir de fumée des huiles combustibles, carburant diesel et autres combustibles et carburants liquides ainsi que ce combustible et carburant liquide en soi Download PDF

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Publication number
EP0078249B1
EP0078249B1 EP19820890134 EP82890134A EP0078249B1 EP 0078249 B1 EP0078249 B1 EP 0078249B1 EP 19820890134 EP19820890134 EP 19820890134 EP 82890134 A EP82890134 A EP 82890134A EP 0078249 B1 EP0078249 B1 EP 0078249B1
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EP
European Patent Office
Prior art keywords
combustion
fuels
oil
additive
polymerization
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.)
Expired
Application number
EP19820890134
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German (de)
English (en)
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EP0078249A1 (fr
Inventor
Gertrude Dipl.-Ing. Kaes
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
LANG & CO., CHEMISCH-TECHNISCHE PRODUKTE KOMMANDIT
Original Assignee
Lang & Co Chemisch-Technische Produkte KG
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Publication date
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Publication of EP0078249A1 publication Critical patent/EP0078249A1/fr
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Classifications

    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/10—Liquid carbonaceous fuels containing additives
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/10—Liquid carbonaceous fuels containing additives
    • C10L1/14—Organic compounds
    • 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
    • F02B3/00—Engines characterised by air compression and subsequent fuel addition
    • F02B3/06—Engines characterised by air compression and subsequent fuel addition with compression ignition

Definitions

  • the invention relates to an additive with a combustion-promoting and soot-inhibiting effect on heating oils, diesel fuels and other liquid fuels, in particular with a boiling end at normal pressure above 300 ° C., the addition one or more oil-soluble and / or oil-dispersible compounds of transition metals such as combustion-catalytically active Contains iron, manganese, molybdenum, cobalt, nickel or copper, and / or alkaline earths, and one or more inhibitors against polymerization and oxidation of hydrocarbons.
  • the invention further relates to liquid fuels with such an additive.
  • soot deposits which due to their large surface area also adsorb acidic components, especially sulfuric acid, also cause increased corrosion and thus material losses in the exhaust system of such systems.
  • the oil When burning heating oils and diesel fuels, the oil is usually sprayed into the combustion zone in the form of droplets that are as finely divided as possible (except for small gasification burners).
  • the individual droplets are quickly heated up in this hot zone and at least partially evaporated.
  • these vaporized hydrocarbons mix with the atmospheric oxygen and maintain the flame formation, whereby the corresponding combustion products are formed.
  • As these droplets move through the combustion zone their size continuously decreases until the volatile components have evaporated (and burned).
  • a small or large remnant of non-volatile constituents remains, which consist of highly polymeric organic compounds, carbon and impurities.
  • hydrocarbons When hydrocarbons are heated to a high degree, they crack, whereby larger molecules are broken down into smaller ones.
  • organometallic, organic and inorganic compounds can serve as combustion-promoting additives.
  • organometallic compounds have proven to be favorable as combustion catalysts of hydrocarbons in certain cases, since on the one hand they can be finely divided into solution / dispersion in oil-soluble / oil-dispersible form and on the other hand compounds of transition and / or alkaline earth metals have shown good effects as combustion catalysts.
  • heating oils and diesel fuels from petroleum or synthetic oils
  • stabilization thereof during storage is to ensure that the application properties of these hydrocarbons do not deteriorate over time through oxidation and polymerization.
  • inhibitors can be added, which are widely used in practice especially in the case of carburetor fuels and lubricating oils, but can also be used in heating oils and diesel fuels, see below.
  • MMT methylcyclopentadienylmanganese tricarbonyl
  • ferrocene dicyclopentadienyl iron
  • a well-known short method for determining the stability of middle distillates is the accelerated stability test (also EDM diesel test, Union Pacific or Nalco and Du Pont test) at 149 ° C (300 ° Fahrenheit).
  • This test determines the relative stability of middle distillates under short-term aging conditions at high temperature and with access to air. The procedure consists in aging the distillate sample at 149 ° C (300 ° Fahrenheit) for 90 minutes with the entry of air and filtering off the residues formed.
  • the filter covering is rated with numbers from 1-20 and provides a comparison of the aging stability of the distillates tested. The lower the rating number, the more stable the distillate, whereby a number up to a maximum of 7 is usually considered to be satisfactory.
  • the color of the distillate is determined according to ASTM (D - 1500 - 58 T) before and after aging, which also allows a relative evaluation of the stability.
  • Polymerization and oxidation inhibitors are known per se and are used in a wide variety of products such as e.g. B. food, cosmetics, plastics, rubber and also used in mineral oil derivatives. It has been shown that these inhibitors are largely ineffective in the products for combustion promotion at issue here. For mineral oil distillates and residual oils, specific inhibitors have also been used to improve storage stability. All of these known oxidation and polymerization inhibitors have hitherto been used to stabilize the products at conventional storage temperatures. A temperature stress of these heating oil and diesel fuel inhibitors of over 150 ° C. has not been provided.
  • the object of the invention is to provide an additive for heating oils and diesel fuels and other liquid fuels, which hinders the polymerization at temperatures of in particular 300 ° C. and above.
  • there is a sharp increase in the reaction rate at temperatures above 300 ° C. the tendency of unsaturated hydrocarbons to polymerize being significantly further favored by the presence of metal compounds, in particular the transition group. It is therefore of particular interest to hinder precisely these high-temperature reactions, since they lead to the increased formation of unburned carbon and high-molecular tarry hydrocarbon compounds (which usually also contain polycyclic aromatics), which can have cancerogenic properties.
  • the inhibitors used for this purpose must neither decompose nor evaporate at this temperature at normal pressure (boiling point or sublimation above 300 ° C).
  • the antioxidants and antipolymerizers which are already known for the stabilization of heating oils and distillates cannot be used for the present purposes since they do not meet these conditions.
  • BHT 2,4-dimethyl-6-tert-butylphenol, 2,6-di-tert-butylp-cresol
  • BHA sterically hindered xylenols and trimethylphenols
  • BHA butylated hydroxyanisoles
  • TBHQ middle distillates
  • para-cresols and aromatic amines are used.
  • These inhibitors are only suitable for temperature ranges up to about 150 ° C.
  • Oxidation and polymerization inhibitors which are also intended for higher temperature loads, have already been used to stabilize plastics, lubricating oils and asphalts.
  • An anti-aging agent known for heat resistant rubber articles is e.g. the zinc salt of 2-mercapto-benzimidazole. However, this inhibitor is also decomposed at temperatures of 300 ° C and is not suitable for higher temperatures.
  • US Pat. No. 2,697,033 is known to include Zn-dicyclohexyldithiophosphate and Ca-petroleum sulfonate in oils to stabilize the storage.
  • the thermal-oxidative decomposition behavior of the Zn-dicyclohexyldithiophosphate is so unfavorable that the inhibitor function is not fulfilled.
  • the start of decomposition is at normal pressure, at 10 6 Pa and at 5 x 10 6 Pa far below 300 ° C.
  • A1kylphenole which serve oil-soluble for the preparation of alkaline earth metal salts.
  • these must be reactive phenols, preferably monoalkylphenols, which are consequently unsuitable as oxidation and polymerization inhibitors.
  • octyl- to dodecylphenols have a vapor pressure of the order of 101,000 Pa, which means that they evaporate completely or to a considerable extent at this temperature and are therefore unsuitable for polymerization-inhibiting catalysis at this temperature.
  • GB-A-800445 shows the use of Mg naphthenate and refractory oxides such as e.g. B. silicon oxide.
  • Mg naphthenate and refractory oxides such as e.g. B. silicon oxide.
  • refractory oxides such as e.g. B. silicon oxide.
  • such mixtures have disadvantages and are not suitable for producing the desired effect.
  • the addition with combustion-promoting and soot-inhibiting effect to heating oils, diesel fuels and other liquid fuels is characterized in that the combustion-catalytically active oil-soluble and / or oil-dispersible compounds of alkaline earths are those of calcium, strontium and / or barium and that as Inhibitor is an oxidation and polymerization inhibitor based on sterically hindered heat-stable alkylphenols with an average molecular weight of 280 or based on N-phenylnaphtylamine (molecular weight 219), the inhibitor having a heat resistance so that it due to its vapor pressure and / or its decomposition temperature temperatures of 300 ° C and above can be exposed at least briefly at normal pressure without losing its polymerization-inhibiting effect.
  • the weight ratio metal: inhibitor 1: 0.1 to 10.
  • Liquid fuels according to the invention in particular those with a boiling end at normal pressure above 300 ° C., such as heating oils and diesel fuels, are characterized in that they contain the additive described above.
  • the metal content in the liquid fuel and propellant can be 0.1 to 1000 Ge parts by weight per million parts by weight of the fuels mentioned.
  • the addition according to the invention on the one hand improves the shelf life of the fuels mentioned and on the other hand also effectively inhibits the polymerizations described above, which are accelerated enormously at temperatures of over 300 ° C. At the same time, the advantage of more complete combustion is achieved even with less excess air. This is all the more important since the aforementioned trend towards using heavier cuts and products from conversion plants, in particular catalytic and thermal crackers and coking plants, in heating oils and diesel fuels is constantly increasing.
  • the polymerization inhibitors used according to the present invention are also effective at temperatures above 300 ° C. They are not only thermally stable under the effects of heat for as long as the hydrocarbon droplet to be burned passes through the combustion zone, but they also advantageously provide effective protection against oxidation for heating oils and diesel fuels at the normal normal storage temperatures.
  • Such inhibitors are high boiling phenols with longer chain, sterically hindering alkyl groups such as e.g. Nonyle.
  • the higher molecular weight organic amine compound N-phenyl-2-naphthylamine also fulfills the present condition. In practice, of course, any carcinogenic effects must always be observed and the harmful additives must be preferred, although heating oils and diesel fuels should normally not come into contact with the skin or with food.
  • Inhibitors based on highly alkylated or polymeric sterically hindered phenol compounds have proven to be particularly economical and advantageously do not result in any increases in pollutants by SO 2 / SO 3 or nitrogen oxides, phosphorus compounds etc. in the exhaust gas.
  • the soot number according to Bacharach was 3 with an air number of 1.4.
  • a soot number of 3.3 was measured for the Unitherm burner with the same air ratio.
  • the boiler efficiency, measured with the heat quantity measuring device, was 76.0-76.3% and 75.8-76.2% for the burners mentioned.
  • the soot number for the Olymp burner improved to 1.5 for the same air ratio (1.4) and even to 1.2 for the Unitherm burner.
  • the boiler efficiency of the additive heating oil was found to be 79.5-80.0% (Olymp burner) and 82.0-83.0% (Unitherm burner) when using the same heat measuring device.
  • the average gain in efficiency was 3.6 and 6.5% due to the additives.
  • composition of the additive according to the invention was:
  • Extra-light, light heating oil with the following analysis data is, with and without addition, according to the invention in a Vossmann, Duo Parola-E, steel boiler with a Weiswash oil burner type WL 2/3 with a heat output of max. 81 kW burned.
  • the soot number at 12.3-12.4% CO 2 and 16.4% CO 2 + 0 2 was reduced under analogous combustion conditions 0.01% CO in the exhaust gas reduced to an average of 1.06, ie improved by 2 points.
  • This gas oil complies with the European regulations for use as diesel fuel.
  • the following additives according to the invention were added to the gas oil, alkylated phenol according to Examples 1 and 2, sterically hindered tertnonyl-cresols, N-phenyl-2-naphthylamine and other highly evaporative polymerization and oxidation inhibitors with a boiling point (boiling range) of over 300 ° C. at normal pressure were included.
  • the finished additive was added with 1 part by weight of additive to 2000 parts by weight of gas oil.
  • the following improvements in the carbon black number were achieved for the following metal contents in the additive according to the invention:
  • This coker gas oil (without additive) was subjected to the accelerated aging text described above at 149 ° C (300 ° Fahrenheit) for 90 minutes.
  • the color number was 9.
  • the color number became 14 with the same accelerated aging, to 16 in the presence of 15 ppm manganese (from MMT) and in 15 ppm copper (from copper naphtenate) increased to 18.
  • the non-additive coker gas oil described in Example 4 was used in trucks as diesel fuel. Practical operation of these motor vehicles was not possible with the product, however, as these diesel engines showed very strong and unreasonable smoke emissions not only at full load, but also during normal operation, which may be due to the high content of aromatics and unsaturated hydrocarbons.
  • An additive according to the invention consisting of 15% by weight of MMT, 20% by weight of alkylated phenols according to Examples 1 and 2 and 65% by weight of paraffin-based petroleum, was used in a ratio of 1 part by weight of additive to 700 parts by weight of coker gas oil admitted.
  • the manganese content was 52.8 ppm, that of high-boiling alkylated phenols 28.6 ppm in the coker gas oil.
  • the smoke development of the diesel engines operated with it was drastically reduced and averaged 20 Hartridge units.
  • the residues in the combustion cylinders of the engines operated with it were negligible even after several months of use and the injection in excellent condition.
  • Residual heating oils containing heavy parts from visbreakers had the following analysis data:
  • This heavy residual oil was treated with 100 ppm manganese (from manganese naphtenate) and silicon dioxide obtained by flame hydrolysis of silicon tetrachloride with a BET surface area of approx. 200 (Aerosil 200) in an amount of 50 ppm plus aluminum oxide with a BET surface area of approx. 100 ( Aluminum oxide-C) also added in an amount of 50 ppm.
  • silanol groups on the surface of the highly disperse silica as well as analogous aluminum hydroxides in the highly disperse aluminum oxide are likely to be responsible for the polymerization inhibition at temperatures above 300 ° C, while the manganese may have catalytically favored the combustion of carbon or carbon-enriched particles in the colder zone of the combustion . It shows that the inorganic polymerization inhibitors according to the invention can also be used advantageously for the present purposes.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Liquid Carbonaceous Fuels (AREA)
  • Solid Fuels And Fuel-Associated Substances (AREA)

Claims (4)

1. Additif ayant une action favorisant la combustion et inhibant la formation de noir de carbone, pour fuels, carburants Diesel et autres combustibles et carburants liquides, en particulier ceux ayant un point final de distillation sous la pression normale de plus de 3000e, l'additif contenant un ou plusieurs composés de métaux de transition tels que fer, manganèse, molybdène, cobalt, nickel ou cuivre et/ou de métaux alcalino-terreux, solubles et/ou dispersables dans les huiles, ayant une action de catalyse de la combustion, et un ou plusieurs inhibiteurs contre la polymérisation et l'oxydation des hydrocarbures, caractérisé par le fait que les composés de métaux alcalino-terreux, solubles et/ou dispersables dans les huiles, ayant une action de catalyse de la combustion, sont des composés du calcium, du strontium et/ou du baryum et par le fait que l'additif contient comme inhibiteur un inhibiteur d'oxydation et de polymérisation à base d'alkylphénols thermostables stériquement encombrés, ayant une masse moléculaire moyenne de 280, ou à base de N-phényl- naphtylamine (masse moléculaire 219), l'inhibiteur présentant une stabilité thermique, de telle sorte qu'il peut être exposé au moins pendant une courte durée, en raison de sa tension de vapeur et/ou de sa température de décomposition, sous la pression normale, à des températures de 300 °C et davantage sans perte de son action d'inhibition de la polymérisation.
2. Additif selon la revendication 1, caractérisé par le fait que le rapport pondéral métal : inhibiteur est de 1 : 0,1 à 10.
3. Combustibles et carburants liquides, en particulier ayant un point final de distillation sous la pression normale de plus de 300 °C, tels que fuels et carburants Diesel, caractérisés par le fait qu'ils contiennent un additif selon l'une des revendications 1 ou 2.
4. Combustibles et carburants liquides selon la revendication 3, caractérisés par le fait que la teneur en métal est de 0,1 à 1000 parties en poids par million de parties en poids de ces combustibles et carburants.
EP19820890134 1981-10-12 1982-09-24 Additif améliorant la combustion et réduisant la formation de noir de fumée des huiles combustibles, carburant diesel et autres combustibles et carburants liquides ainsi que ce combustible et carburant liquide en soi Expired EP0078249B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
AT4379/81 1981-10-12
AT437981A AT373274B (de) 1981-10-12 1981-10-12 Zusatz mit verbrennungsfoerdernder und russhemmender wirkung zu heizoelen, dieselkraftstoffen und sonstigen fluessigen brenn- und treibstoffen, sowie fluessige brennund treibstoffe mit diesem zusatz

Publications (2)

Publication Number Publication Date
EP0078249A1 EP0078249A1 (fr) 1983-05-04
EP0078249B1 true EP0078249B1 (fr) 1987-10-28

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Country Status (4)

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EP (1) EP0078249B1 (fr)
AT (1) AT373274B (fr)
CA (1) CA1188891A (fr)
DE (1) DE3277537D1 (fr)

Cited By (3)

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Publication number Priority date Publication date Assignee Title
US5360459A (en) 1991-05-13 1994-11-01 The Lubrizol Corporation Copper-containing organometallic complexes and concentrates and diesel fuels containing same
US5376154A (en) 1991-05-13 1994-12-27 The Lubrizol Corporation Low-sulfur diesel fuels containing organometallic complexes
US5534039A (en) 1991-05-13 1996-07-09 The Lubrizol Corporation Organometallic complex-antioxidant combinations, and concentrates and diesel fuels containing same

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US4690687A (en) * 1985-08-16 1987-09-01 The Lubrizol Corporation Fuel products comprising a lead scavenger
EP0579339B1 (fr) * 1985-08-16 1997-06-04 The Lubrizol Corporation Produits combustibles
FR2616795B1 (fr) * 1987-06-19 1989-10-27 Inst Francais Du Petrole Procede ameliore de production de chaleur par combustion d'un fuel lourd
EP0358734B1 (fr) * 1988-01-27 1994-06-15 The Lubrizol Corporation Composition de carburant
US5160350A (en) * 1988-01-27 1992-11-03 The Lubrizol Corporation Fuel compositions
US4908045A (en) * 1988-12-23 1990-03-13 Velino Ventures, Inc. Engine cleaning additives for diesel fuel
GB2239258A (en) * 1989-12-22 1991-06-26 Ethyl Petroleum Additives Ltd Diesel fuel compositions containing a manganese tricarbonyl
US5944858A (en) * 1990-09-20 1999-08-31 Ethyl Petroleum Additives, Ltd. Hydrocarbonaceous fuel compositions and additives therefor
EP0476196B1 (fr) * 1990-09-20 1993-11-18 Ethyl Petroleum Additives Limited Compositions combustibles hydrocarburées et additifs pour celles-ci
EP0482253A1 (fr) * 1990-10-23 1992-04-29 Ethyl Petroleum Additives Limited Compositions de combustible bonnes pour l'environnement, et additifs pour
TW230781B (fr) * 1991-05-13 1994-09-21 Lubysu Co
IT1254456B (it) * 1992-02-14 1995-09-25 Basf Italia Composizione marcante-denaturante particolarmente adatta per marcare edenaturare bitumi combustibili o prodotti affini.
US5551957A (en) * 1992-05-06 1996-09-03 Ethyl Corporation Compostions for control of induction system deposits
US5511517A (en) * 1994-02-10 1996-04-30 Ethyl Corporation Reducing exhaust emissions from otto-cycle engines
CA2205143C (fr) * 1996-05-14 2003-07-15 Ethyl Corporation Procede et produits permettant d'ameliorer l'efficacite de combustion de combustibles de chauffage hydrocarbones
GB2321906A (en) * 1997-02-07 1998-08-12 Ethyl Petroleum Additives Ltd Fuel additive for reducing engine emissions
DE19701961A1 (de) * 1997-02-22 1998-12-24 Adolf Dipl Chem Metz Automobil-Bio-Katalysator-Additiv Flüssig-Katalysator als Zugabe in den Kraftstoff zur regenerativen Erneuerung der Natur und Entsäuerung der Böden
WO2001016257A1 (fr) * 1999-09-01 2001-03-08 The Associated Octel Company Limited Additif pour carburant permettant de prevenir la recession des sieges de soupape
IT1318868B1 (it) 2000-08-03 2003-09-10 Cesare Pedrazzini Additivo per ridurre il particolato nelle emissioni derivanti dallacombustione di gasolio ed olio combustibile e composizione carburante
US7300477B2 (en) 2003-08-14 2007-11-27 Afton Chemical Corporation Method and fuel additive including iron naphthenate
US7332001B2 (en) * 2003-10-02 2008-02-19 Afton Chemical Corporation Method of enhancing the operation of diesel fuel combustion systems
GB0700534D0 (en) * 2007-01-11 2007-02-21 Innospec Ltd Composition
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CN102337169B (zh) * 2010-07-16 2013-07-03 甘肃黑马石化工程有限公司 锅炉多元除渣清灰节能剂组合物及其制备工艺

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5360459A (en) 1991-05-13 1994-11-01 The Lubrizol Corporation Copper-containing organometallic complexes and concentrates and diesel fuels containing same
US5376154A (en) 1991-05-13 1994-12-27 The Lubrizol Corporation Low-sulfur diesel fuels containing organometallic complexes
US5534039A (en) 1991-05-13 1996-07-09 The Lubrizol Corporation Organometallic complex-antioxidant combinations, and concentrates and diesel fuels containing same

Also Published As

Publication number Publication date
CA1188891A (fr) 1985-06-18
ATA437981A (de) 1983-05-15
DE3277537D1 (en) 1987-12-03
AT373274B (de) 1984-01-10
EP0078249A1 (fr) 1983-05-04

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