EP1252270B1 - Temperaturstabiler emulsionsbrennstoff - Google Patents

Temperaturstabiler emulsionsbrennstoff Download PDF

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Publication number
EP1252270B1
EP1252270B1 EP00993629A EP00993629A EP1252270B1 EP 1252270 B1 EP1252270 B1 EP 1252270B1 EP 00993629 A EP00993629 A EP 00993629A EP 00993629 A EP00993629 A EP 00993629A EP 1252270 B1 EP1252270 B1 EP 1252270B1
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Prior art keywords
carbon atoms
additives
fuel
group
linear
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French (fr)
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EP1252270A1 (de
Inventor
Philippe Schulz
Laurent Dalix
Frédéric Tort
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Total Marketing Services SA
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Total France SA
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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
    • C10L1/32—Liquid carbonaceous fuels consisting of coal-oil suspensions or aqueous emulsions or oil emulsions
    • 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
    • C10L10/00—Use of additives to fuels or fires for particular purposes
    • C10L10/02—Use of additives to fuels or fires for particular purposes for reducing smoke development
    • 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
    • C10L1/32—Liquid carbonaceous fuels consisting of coal-oil suspensions or aqueous emulsions or oil emulsions
    • C10L1/328—Oil emulsions containing water or any other hydrophilic phase
    • 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
    • C10L10/00—Use of additives to fuels or fires for particular purposes
    • C10L10/18—Use of additives to fuels or fires for particular purposes use of detergents or dispersants for purposes not provided for in groups C10L10/02 - C10L10/16

Definitions

  • the present invention relates more specifically to the composition of fuels consisting of water / liquid hydrocarbon emulsions of water / diesel emulsions which are economically interesting and limit the problems of environmental pollution. So it's going to be in the present exposed water / hydrocarbon stabilized emulsions, including surfactants to promote and maintain the stable emulsion for variations in temperatures between -10 ° C and above 70 ° C.
  • phase separation phase shift / demixing
  • Out of phase oil (separated) at the end of this period may represent up to 3% by volume of the emulsion. It is easy to imagine that after a few days of storage, the phase shift of this emulsion according to the application No. 2,470,153 is sufficiently important for become unacceptable to operation, under normal conditions of application.
  • the fuel emulsified according to this patent also suffers from a lack of stability, especially at low temperatures.
  • the Applicant has also been able to this clearly evident by reproducing the preferred example of implementation of the emulsified fuel according to this US patent. It turned out that the emulsion separated (shift) in one hour. The phenomenon is further accentuated at low temperature less than 5 ° C. One can hardly imagine then, what could happen in Vehicle tanks containing this emulsion during a harsh winter.
  • Japanese Patent Abstract No. 77-69,909 given in the chemical abstract 87: 138 513 x concerns an emulsified fuel (kerosene: water) comprising sorbitan sesquioleate and polyethylene glycol ether of nonylphenol as emulsifiers.
  • the size of the dispersed phase droplets aqueous is ⁇ 20 ⁇ and on average of the order of 10 ⁇ .
  • This technical proposal does not does not allow it to meet the stability objectives appropriately physicochemical, pollution control, economy and reduction of fuel consumption.
  • This technical education can not be of any relief for a person skilled in the art who places himself in the prospective approach of the invention.
  • emulsified fuels which can be fuels, include specific quantities of hydrocarbons and a set of additives minor amount, including an emulsifying system comprising at least one sorbitol ester, at least one polyalkoxylated fatty acid ester of higher HLB or equal to 9, and at least one alkylphenol-polyalkoxylated HLB of between 10 and 15, the respective concentration ratios of these components ranging from 2.5 - 3.5; 1.5 - 2.5; 0.5 - 1.9.
  • the dispersed phase of these emulsified fuels is constituted 5 to 35% by weight of the water, while the additives are present at 0.1 to 2% by weight.
  • the present invention aims at a stable emulsified fuel during the less than four days at more than 70 ° C, cold fuel stability, that is to say - 10 ° C or storage up to 40 ° C being maintained for at least three months without untimely decantation. In addition, it aims to obtain an emulsified fuel satisfactory to all levels of government in terms of the environment.
  • the preferred sorbitol esters are selected from sorbitol oleates, taken alone or as a mixture, the sesquioleate of sorbitol having the preference.
  • the fatty acid esters of formula (II) are chosen from oleates, stearates and ricinoleates of polyethylene glycol.
  • the preferred esters are those whose polyethylene glycol fraction has a molecular weight less than or equal to 600, and preferably less than 450.
  • the polyalkoxylated compounds of formula (III) which in combination with the other two components of the system emulsifying fuel stability when hot, are chosen from iso di and trialkyl alcohols, each alkyl radical having 1 to 15 carbon atoms, preferably among the alcohols Alkyl radicals comprise from 5 to 12 carbon atoms. Preferably they are chosen from isotridecyl alcohols comprising from 3 to 10 groups ethoxylates.
  • the hydrocarbon liquid constituting the part major fuel is selected from the group consisting of species, middle distillates, synthetic fuels, animal or vegetable oils, esterified or not, and their mixtures.
  • the emulsified fuel according to the invention also comprises the phase hydrocarbon, water and emulsifier system other additives such as procetanes chosen preferably from peroxides and / or nitrates and their mixtures, and optionally a metal catalyst for post-combustion so-called metal, being one of those of the group consisting of magnesium, calcium, barium, cerium, copper, iron or their mixtures. It can contain in in addition to the aqueous phase a biocide, preferably a bactericide and / or a fungicide, and also antifreeze.
  • the fuel according to the invention may contain usual additives such as filterability additives, cloud point improvement, lubricant and anti-sedimentation additives, anti-wear additives, anti-foam additives, anti-corrosion additives, additives detergents, and / or additives or additive compositions to improve the operability to cold.
  • additives such as filterability additives, cloud point improvement, lubricant and anti-sedimentation additives, anti-wear additives, anti-foam additives, anti-corrosion additives, additives detergents, and / or additives or additive compositions to improve the operability to cold.
  • a second object of the invention is the composition of additives for fuel containing essentially the emulsifier system and possibly at minus another additive selected from compounds of the group consisting of procetanes, catalytic promoters of combustion and soot, biocides, anti-gels, detergents, lubricity additives, anti-foam additives, anti-corrosion additives, anti-wear additives and additives or additive compositions to improve cold operability.
  • the purpose of this example is to present the stability results of the emulsified fuels of the invention compared to those of the known art.
  • compositions of the emulsifying systems are given in Table I below: Surfactant Composition AT B VS D E F F ' BOY WUT H I J K The M NOT Sorbitan sesquioleate 3 3 1.5 3 3 1 1.5 1.5 1 3 Sorbitan mono-oleate 3 3 1.5 1.5 1.5 1.5 Sorbitan Laurate 1.5 Sorbitan Stearate 1.5 PEG 300 1 PEG 6EO Monooleate 2 2 2 2 Monooelale PEG 7.4 EO 2 2 2 2 2 2 2 Monooleate PEG 600 1 Nonylphenol ethoxylated 9 EO 1 1 1 1 3 Nonylphenol ethoxylated 12 EO 1 Nonylphenol ethoxylated 30EO 1 1.5 1.5 Ethylated decyl alcohol 3EO 1 Isotridecyl alcohol ethoxylated 7.5 EO 1 1 1 1 HLB emulsifier system 7.2 7.5 7.6 7.6 7.6 7.6 8.2 10.1 8.1 9.2 9.6 9.6 10.1 10.1
  • compositions A, C and F are compositions according to In the invention, compositions B, D, E and N serve as comparative examples.
  • the quality of the emulsions were assessed according to criteria of granulometry, storage stability regardless of the ambient temperature, stability in use, storage stability and temperature stability.
  • the stability of the emulsion in use is characterized by an absence of demixing / decantation or other disruption of the emulsion in a 1 liter beaker having undergoes a stimulating cycle corresponding to the presumed diesel recirculation cycle in a car tank.
  • Storage stability is determined by an absence of demixing / decantation after three months of static storage in vials frustoconical sections of three samples maintained at 0 ° C, 20 ° C and 40 ° C, respectively.
  • the demixion is characterized by the separation into two phases not necessarily clear.
  • the hot stability is characterized by a total absence of demixing / settling after four days of static storage at 75 ° C.
  • Stabilities are assessed by the more or less long time separating the preparation of the emulsion and the time of demixing / decantation. This time appraise according to the stability appreciated in hours (h), days (j), weeks (s) and months (M).

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

Claims (11)

  1. Emulgierter Brennstoff enthaltend einen größeren Teil an Kohlenwasserstoff-Flüssigkeit und einen kleineren Teil von 5 bis 35 Gew.-% Wasser, enthaltend ein Ensemble von Zusätzen, unter ihnen ein emulgierendes System, aufweisend:
    i) 2,5 bis 3,5 Gewichtsteile mindestens eines Sorbitolesters der nachfolgenden Formel (I):
    Figure 00140001
    in der die Reste X gleich oder verschieden sind und jeweils einer Gruppe entsprechen, die ausgewählt ist unter den Gruppen OR1, wobei R1 Wasserstoff oder ein aliphatischer Rest mit 1 bis 6 Kohlenstoffatomen ist, und den Gruppen R2-COO-, wobei R2 Wasserstoff oder ein gesättigter oder ungesättigter, linearer oder verzweigter, aliphatischer Kohlenwasserstoffrest ist, der gegebenenfalls mit mindestens einer Hydroxylgruppe substituiert ist und der 6 bis 22 Kohlenstoffatome aufweist, wobei mindestens ein Rest X R2-COO- entspricht,
    ii) 1,5 bis 2,5 Gewichtsteile mindestens eines polyalkoxylierten Fettsäureesters der nachfolgenden Formel (II):
    Figure 00150001
    in der R3 ein gesättigter oder ungesättigter, linearer oder verzweigter, aliphatischer Kohlenwasserstoffrest ist, der gegebenenfalls mit mindestens einer Hydroxylgruppe substituiert ist und der 6 bis 22 Kohlenstoffatome aufweist, R4 eine lineare oder verzweigte Alkylengruppe ist, die 1 bis 10 Kohlenstoffatome, bevorzugt 2 bis 3 Kohlenstoffatome, aufweist, n eine ganze Zahl ist, die größer oder gleich 6 ist, wobei sie bevorzugt zwischen 6 und 30 variiert, und schließlich R5 Wasserstoff, eine lineare oder verzweigte Alkylgruppe von 1 bis 10 Kohlenstoffatomen oder auch
    Figure 00150002
    ist, wobei R6 gleich R3 oder davon verschieden ist,
    iii) 0,5 bis 2,5 Gewichtsteile mindestens einer polyalkoxylierten Verbindung der nachfolgenden allgemeinen Formel (III)
    Figure 00150003
    in der R9 und R10 lineare oder verzweigte Alkylgruppen sind, die gleich oder verschieden sind, die 1 bis 20 Kohlenstoffatome aufweisen, wobei R7 ein lineares oder verzweigtes Alkylen ist, das 1 bis 10, bevorzugt 1 bis 3, Kohlenstoffatome aufweist, R8 ausgewählt ist aus der Gruppe, die aus Wasserstoff, den linearen oder verzweigten Alkylgruppen von 1 bis 10 Kohlenstoffatomen, und
    Figure 00160001
    besteht, wobei R11 ein gesättigter oder ungesättigter, linearer oder verzweigter, aliphatischer Rest ist, der gegebenenfalls mit Hydroxylfunktionen substituiert ist und der 7 bis 22 Kohlenstoffatome aufweist, m und p ganze Zahlen sind, die von 0 bis 20 bzw. von 3 bis 10 variieren,
    wobei das HLB des emulgierenden Systems von 6 bis 8 variiert.
  2. Brennstoff nach Anspruch 1, dadurch gekennzeichnet, daß die Konzentration an emulgierendem System kleiner oder gleich 2 Gew.-% ist.
  3. Brennstoff nach einem der Ansprüche 1 und 2, dadurch gekennzeichnet, daß die Sorbitolester der Formel (I) ausgewählt sind unter den Sorbitanoleaten, alleine oder im Gemisch, wobei das Sesquioleat bevorzugt ist.
  4. Brennstoff nach den Ansprüchen 1 bis 3, dadurch gekennzeichnet, daß die Fettsäureester der Formel (II) ausgewählt sind unter den Oleaten, den Stearaten und den Ricinoleaten von Polyethylenglykol, wobei die bevorzugten Ester diejenigen sind, deren Polyethylenglykol-Anteil ein Molekulargewicht von kleiner oder gleich 600, und bevorzugt kleiner als 450, aufweist.
  5. Brennstoff nach einem der Ansprüche 1 bis 4, dadurch gekennzeichnet, daß die polyalkoxylierten Verbindungen der Formel (III) ausgewählt sind unter den Iso-, Di- und Trialkyl-alkoholen, wobei jeder Alkylrest 1 bis 15 Kohlenstoffatome aufweist, bevorzugt unter den Alkoholen, deren Alkylreste 2 bis 12 Kohlenstoffatome enthalten.
  6. Brennstoff nach Anspruch 5, dadurch gekennzeichnet, daß die polyalkoxylierten Verbindungen der Formel (III) bevorzugt Isotridecyl-alkohole sind, die 3 bis 10 ethoxylierte Gruppen aufweisen.
  7. Brennstoff nach einem der Ansprüche 1 bis 6, dadurch gekennzeichnet, daß die Kohlenwasserstoff-Flüssigkeit ausgewählt ist aus der Gruppe, die aus den Benzinen, den Mitteldestillaten, den Synthesekraftstoffen, den tierischen oder pflanzlichen Ölen, verestert oder unverestert, und ihren Gemischen besteht.
  8. Brennstoff nach einem der Ansprüche 1 bis 7, dadurch gekennzeichnet, daß er die Cetanzahl verbessernde Zusätze, die bevorzugt unter den Peroxiden und/oder den Nitraten und ihren Gemischen ausgewählt sind, und gegebenenfalls einen Metallkatalysator für die Nachverbrennung von Rußen, wobei das Metall eines derjenigen aus der Gruppe ist, die aus Magnesium, Calcium, Barium, Cer, Kupfer, Eisen oder ihren Gemischen besteht, aufweist.
  9. Brennstoff nach einem der Ansprüche 1 bis 8, dadurch gekennzeichnet, daß die wässrige Phase ein Biozid, bevorzugt ein Bakterizid und/oder ein Fungizid, und gegebenenfalls ein Frostschutzmittel, enthält.
  10. Brennstoff nach einem der Ansprüche 1 bis 9, dadurch gekennzeichnet, daß er einen oder mehrere Zusätze für die Filtrierbarkeit, zur Verbesserung des Trübungspunkts, für die Schmierfähigkeit, gegen Sedimentierung, Verschleißschutz-Zusätze, Entschäumungs-Zusätze, Korrosionsschutz-Zusätze, Detergens-Zusätze und/oder Zusätze oder Zusatz-Zusammensetzungen zur Verbesserung der Kältfunktionsfähigkeit aufweist.
  11. Zusatz-Zusammensetzung für einen Brennstoff, insbesondere für einen Kraftstoff, dadurch gekennzeichnet, daß sie im wesentlichen das emulgierende System, wie es in einem der Ansprüche 1 bis 10 definiert ist, und gegebenenfalls mindestens einen weiteren Zusatz, der ausgewählt ist unter den Verbindungen der Gruppe, die aus den Cetanzahlverbesserern, den katalytischen Rußverbrennungs-Promotoren, den Bioziden, den Frostschutzmitteln, den Detergenzien, den Schmierfähigkeitszusätzen, den Verschleißschutz-Zusätzen, den Entschäumungs-Zusätzen, den Korrosionsschutz-Zusätzen und den Zusätzen oder Zusatz-Zusammensetzungen zur Verbesserung der Kältefunktionsfähigkeit besteht, enthält.
EP00993629A 1999-12-23 2000-12-12 Temperaturstabiler emulsionsbrennstoff Expired - Lifetime EP1252270B1 (de)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
FR9916380A FR2802941B1 (fr) 1999-12-23 1999-12-23 Combustible emulsionne stable en temperature
FR9916380 1999-12-23
PCT/FR2000/003483 WO2001048123A1 (fr) 1999-12-23 2000-12-12 Combustible emulsionne stable en temperature

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EP1252270A1 EP1252270A1 (de) 2002-10-30
EP1252270B1 true EP1252270B1 (de) 2005-11-02

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US (1) US6793694B2 (de)
EP (1) EP1252270B1 (de)
JP (1) JP2003518550A (de)
KR (1) KR100730067B1 (de)
AT (1) ATE308602T1 (de)
AU (1) AU2855001A (de)
BR (1) BR0016907A (de)
CA (1) CA2394784A1 (de)
DE (1) DE60023749T2 (de)
DK (1) DK1252270T3 (de)
ES (1) ES2246934T3 (de)
FR (1) FR2802941B1 (de)
HU (1) HUP0204073A2 (de)
MX (1) MXPA02006265A (de)
MY (1) MY127900A (de)
PL (1) PL191935B1 (de)
WO (1) WO2001048123A1 (de)
ZA (1) ZA200204659B (de)

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US7276093B1 (en) 2000-05-05 2007-10-02 Inievep, S.A. Water in hydrocarbon emulsion useful as low emission fuel and method for forming same
US20060130394A1 (en) * 2004-12-22 2006-06-22 Flint Hills Resources, L.P. Performance diesel fuels and additives
RU2008146727A (ru) * 2006-04-27 2010-06-10 Нью Дженерейшн Байофьюэлз, Инк. (Us) Композиция биологического топлива и способ получения биологического топлива
FR2925909B1 (fr) * 2007-12-26 2010-09-17 Total France Additifs bifonctionnels pour hydrocarbures liquides obtenus par greffage a partir de copolymeres d'ethylene et/ou de propylene et d'esters vinyliques
FR2925916B1 (fr) * 2007-12-28 2010-11-12 Total France Terpolymere ethylene/acetate de vinyle/esters insatures comme additif ameliorant la tenue a froid des hydrocarbures liquides comme les distillats moyens et les carburants ou combustibles
KR101071204B1 (ko) 2011-03-08 2011-10-10 이영서 중유용 연료첨가제 및 이를 포함하는 연료유
JP2023552062A (ja) * 2020-11-04 2023-12-14 ビーエーエスエフ ソシエタス・ヨーロピア 燃料エマルジョン用の短鎖界面活性剤及び任意選択により長鎖界面活性剤を含む乳化剤パッケージ

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US4877414A (en) * 1988-03-31 1989-10-31 Kenneth Mekonen Fuel compositions
FR2746106B1 (fr) * 1996-03-15 1998-08-28 Combustible emulsionne et l'un de ses procedes d'obtention
JP2001508117A (ja) * 1997-01-16 2001-06-19 クラリアント・ゲゼルシャフト・ミト・ベシュレンクテル・ハフツング 燃料−水−エマルジョン
US6648929B1 (en) * 1998-09-14 2003-11-18 The Lubrizol Corporation Emulsified water-blended fuel compositions
TW589369B (en) * 2001-07-11 2004-06-01 Kune-Muh Tsai Emulsion fuel oil additive

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PL191935B1 (pl) 2006-07-31
DK1252270T3 (da) 2006-03-20
HUP0204073A2 (en) 2003-05-28
JP2003518550A (ja) 2003-06-10
US6793694B2 (en) 2004-09-21
ATE308602T1 (de) 2005-11-15
PL355490A1 (en) 2004-05-04
FR2802941B1 (fr) 2002-04-05
CA2394784A1 (en) 2001-07-05
KR100730067B1 (ko) 2007-06-20
BR0016907A (pt) 2002-10-29
MY127900A (en) 2006-12-29
AU2855001A (en) 2001-07-09
ZA200204659B (en) 2002-12-23
EP1252270A1 (de) 2002-10-30
WO2001048123A1 (fr) 2001-07-05
US20040107633A1 (en) 2004-06-10
MXPA02006265A (es) 2003-01-28
FR2802941A1 (fr) 2001-06-29
DE60023749D1 (de) 2005-12-08
ES2246934T3 (es) 2006-03-01
KR20020071900A (ko) 2002-09-13
DE60023749T2 (de) 2006-07-13

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