CN1199771A - The use of lubricity additives for reducing foam in fuels - Google Patents

The use of lubricity additives for reducing foam in fuels Download PDF

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Publication number
CN1199771A
CN1199771A CN 98107011 CN98107011A CN1199771A CN 1199771 A CN1199771 A CN 1199771A CN 98107011 CN98107011 CN 98107011 CN 98107011 A CN98107011 A CN 98107011A CN 1199771 A CN1199771 A CN 1199771A
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Prior art keywords
fuel
acid
composition
additive
suds suppressor
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CN 98107011
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Chinese (zh)
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CN1090230C (en
Inventor
G·C·杰弗里
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Afton Chemical Ltd
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Afton Chemical Ltd
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    • C10L10/08—Use of additives to fuels or fires for particular purposes for improving lubricity; for reducing wear
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    • 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
    • C10L1/30—Organic compounds compounds not mentioned before (complexes)
    • C10L1/305—Organic compounds compounds not mentioned before (complexes) organo-metallic compounds (containing a metal to carbon bond)

Abstract

The present invention relates to fuel additives for improving the foam behavior of fuel compositions containing said additives. The objective of the invention is obtained by the addition of a lubricity additive to fuel additive compositions containing colloidally dispersed metals and conventional antifoam agents. The present invention further relates to fuel concentrates and fuel compositions containing the fuel additive.

Description

Reduce the application of foamy oiliness improver in fuel
The fuel that is used for the middle runnings boiling spread in the preparation for example compositions of additives control foam of gas oil, diesel oil, gas turbine fuel, burner fuel etc. is the very important problem that needs are considered.If be transferred to fuel foaming the process of another jar from a jar at fuel, it just becomes is difficult to control flow velocity and volume.Same, foaming just may produce various other problems in the process of tanks tinning, for example is not transported in the jar conforming to an amount of fuel, and is perhaps opposite, in the local fuel overflow of tinning with overflow.
In order to overcome the problem of these foaming, diesel oil and a whole set of various suds suppressors of filling a prescription of additive that are used to prepare the finished product diesel oil fuel, for example polyacrylic ester and polysiloxane have been proposed to be used for.
When production is used for improving some multifunctional additive for lubricating oils of characteristic of midbarrel fuel, have been found that and in this enriched material, to comprise quite a large amount of suds suppressors, to guarantee that finished product fuel has the suds suppressor of q.s, foamy forms in the fuel so that suppress effectively in by the process of aforesaid operations.General, the amount at least 0.5% of needed suds suppressor (weight) in multifunctional additive for lubricating oils.In fact, in order effectively to use some multifunctional additive for lubricating oils, in this enriched material, can need 10% (weight) or the suds suppressor of volume more.
Have been found that when this multifunctional additive for lubricating oils contains a large amount of silicone suds suppressors and high alkaline detergent, may produce serious inconsistent problem.Aspect a lot of, proved this problem.On the one hand, may in multifunctional additive for lubricating oils, particularly in the process that stores, produce insoluble throw out or particulate matter.In addition, experimental result shows, even the interaction between high alkaline detergent and the silicone suds suppressor does not produce the solid of visible energy, this uncompatibility still may cause the considerable damage of suds suppressing properties in the finished product fuel that obtains.The manifestation of these two kinds of adverse consequences also may take place simultaneously.This inconsistent situation always can not take place in the composition that contains suds suppressor and high alkaline detergent.The HiTEC that has bought from EthylCorporation on the market for example 4043L fuel dope product contains polyethers polysiloxane suds suppressor, and it can be dissolved in 25 ℃ the water, for example the TEGOPREN that has bought from T.H.Goldschmidt AG on the market 5851 silicone surfactant products and overbased calcium sulfonate detergent do not present above-mentioned uncompatibility, so not within the scope of the invention.
Therefore, needs have been increased to a kind of like this method, promptly this method can effectively overcome for example such problem of uncompatibility between high alkaline metal detergent and the silicone suds suppressor of additive, particularly when the fuel composition situation of silicone suds suppressor to be used for a whole set of prescription of additive than higher concentration and to generate.
Have been found that now that in the presence of various suds suppressors adding oiliness improver can improve significantly and contain for example high alkaline metal detergent or improve the foam performance of fuel of the additive of metal matrix discharge of colloidal dispersion metallic material.
In realizing this process that needs, the present invention provides a kind of multifunctional additive for lubricating oils in an one embodiment preferred, as its component, this enriched material contains (i) oiliness improver, (ii) at least a high alkaline metal detergent and (iii) be insoluble to the suds suppressor of 25 ℃ water basically.
Another embodiment is included in the above-mentioned multifunctional additive for lubricating oils and contains the molten dispersion agent of (iv) at least a hydrocarbon and/or (v) improve the additive of metal matrix discharge as its component, by active ingredient, (iv) with (iii) weight ratio usually (iv) at the (iii) about 0.25-300 weight part of every weight part.
Be included in above-mentioned arbitrary enriched material can and preferably other component comprise liquid hydrocarbon diluent (particularly liquid rich arene diluent) or liquid alcohol thinner or emulsion splitter or sanitas or above-mentioned any two or more mixture.
Also have another embodiment, comprise the liquid fuel combination that contains above-mentioned any multifunctional additive for lubricating oils component, for example the fuel composition in the middle runnings boiling spread.
Of the present invention above-mentioned with other embodiment and advantage from behind description and appending claims can see more obvious.Component (i)
The carboxylic acid or derivatives thereof that oiliness improver of the present invention preferably randomly replaces with at least one hydroxyl.Preferred carboxylic acid derivative is carboxylic acid amide and carboxylicesters.
The carboxylic acid that hydroxyl replaces or carboxylic acid derivative can use separately or mix use with acid and/or acid derivative that any other hydroxyl replaces.The acid that is used for hydroxyl replacement of the present invention usually contains up to 60 carbon atoms.The acid that this hydroxyl replaces can be list or poly carboxylic acid or dimeracid.When using the monocarboxylic acid of hydroxyl replacement, they usually contain 10-40 carbon atom, more generally 10-30 carbon atom, a particularly 12-24 carbon atom.Such preferred acid is lipid acid, ricinolic acid.When the poly carboxylic acid that uses hydroxyl to replace, for example two or tricarboxylic acid, they usually contain 3-40 carbon atom, more generally 3-30 carbon atom, a particularly 3-24 carbon atom.The polycarboxylic example that such hydroxyl replaces comprises ricinolic acid, oxysuccinic acid, tartrate and citric acid.The acid that also can use hydroxyl to replace, dimeracid.So herein compound is called dimeracid and trimer acid.When using dimeracid, they usually contain 10-60, preferred 20-60, most preferably 30-60 carbon atom.By the dimerization unsaturated acid and introduce a hydroxy functional group and prepare such acid.The sour general mixture by a poly-acid, dimeracid and trimer acid is like this formed.According to an embodiment preferred of the present invention, this acid is the dimer (fatty acid) yl that hydroxyl replaces, for example oleic acid and linolic acid.This general dipolymer is with the mixture existence of the trimer of the dipolymer and 15% (weight) of single polymers, 83% (weight) of 2% (weight) and more high-grade acid.Above-described preferred dimeracid and other acid can have been bought from the market maybe and can have been prepared by adopting technique known.
As mentioned above, used oiliness improver component can be the form with carboxylic acid derivative.Can with one type derivative be the ester of this acid and polyvalent alcohol.Polyvalent alcohol that can derived ester usually contains 2-7 carbon atom.The example of suitable alcohol comprises aklylene glycol for example ethylene glycol, Diethylene Glycol, triethylene glycol and dipropylene glycol, glycerol, arabitol, Sorbitol Powder, mannitol, tetramethylolmethane, sorbitan, 1,2-butyleneglycol, 2,3-hexylene glycol, 2, the 4-hexylene glycol, quite which is pure and mild 1, the 2-cyclohexanediol.These alcohol can obtain easily.In the middle of the alcohol of being mentioned, preferably use glycerol or sorbitan.In preferred embodiments, this ester has at least one free hydroxyl group in the part by polyol derivative, promptly is not that all hydroxyls of polyvalent alcohol are all esterified.Particularly preferredly be to use single ricinolic acid glyceryl ester.
Operable other carboxylic acid derivative is the ester of the alkanolamine of the acid that replaces of hydroxyl and following formula:
R 1[N (R 1) (CH 2) p] qY wherein, p is 2-10, q is 0-10, Y is-N (R 1) 2, 4-morpholinyl or by R 11-piperazinyl or group-[(CH that group N-replaces 2) pN (R 1) qR 1, wherein the definition of p and q is the same, each substituent R 1Independently be selected from the group of alkyl with 1-6 carbon atom and following formula:
-(R 2O) rR 3Wherein r is 0-10, R 2Be alkylidene group with 2-6 carbon atom, R 3Be the hydroxyalkyl with 2-6 carbon atom, condition is at least one R 1Be-(R 2O) rR 3So alkanolamine is nitrogen-atoms the sort of that does not contain any band hydrogen.The existence expection of this free hydrogen atom can cause forming acid amides with acid-respons the time.Operable alkanolamine is can buy from the market maybe to prepare by adopting technique known.
According to embodiment preferred, in the alkanolamine of above-mentioned formula, Y is-N (R 1) 2, p be 2 and q be 0-3.Each R more preferably 1Be C 24Hydroxyalkyl, C 2Or C 3Hydroxyalkyl is particularly preferred.The object lesson of such compound comprises trolamine, triisopropylamine and the 1 and the diethylenetriamine that are replaced by hydroxyethyl or hydroxypropyl of each nitrogen-atoms wherein.
In another preferred embodiment, in alkanolamine, Y is the 1-piperazinyl of 4-morpholinyl or replacement, and p is that 2-6 and q are 0 or 1.The example of such alkanolamine comprises aminoethylpiperazine, two-(amino-ethyl) piperazine and the morpholine that is replaced by hydroxypropyl N-.These alkanolamines can have been bought from the market maybe and can prepare by adopting technique known.
Acid amides, for example the acid amides of the nitrogenous compound reaction formation of the carboxylic acid of hydroxyl replacement and ammonia or following formula also can be used as carboxylic acid derivative:
R 1[N (R 1) (CH 2) p] qY wherein, p is 2-10, q is 0-10, Y is-N (R 1) 2, 4-morpholinyl or arbitrarily by R 11-piperazinyl or group-[(CH that group N-replaces 2 pN (R 1) qR 1, wherein the definition of p and q is the same, each substituent R 1Independently be selected from hydrogen and have the alkyl of 1-6 carbon atom and the group of following formula:
-(R 2O) rR 3Wherein r is 0-15, R 2Be alkylidene group with 2-6 carbon atom, R 3Be the hydroxyalkyl with 2-6 carbon atom, condition is at least one R 1Be hydrogen.
According to embodiment preferred, in nitrogenous compound, Y is-N (R 1) 2, p be 2 and q be 0-3.The example of such compound comprises diethanolamine, three (methylol) aminomethane, Triethylenetetramine (TETA) or the diethylenetriamine that is at random replaced by two hydroxypropyl N.
In another embodiment, in nitrogenous compound, Y is the 1-piperazinyl of 4-morpholinyl or N-replacement arbitrarily, and p is 2-6, and q is 0 or 1, R 1Be hydrogen.The example of such compound comprises aminoethylpiperazine, two-(amino-ethyl) piperazine and morpholine.
The compound that is used to form these acid amides can have been bought from the market maybe and can prepare by adopting technique known.
In the nitrogenous compound of alkanolamine and above-mentioned formula, r is 1 or bigger, promptly contains those of an ehter bond or polyethers key, can prepare by one or more alkylene oxide reactions of suitable amine, morpholine or diethylenediamine compound and molar excess.When using the alkylene oxide of same type, R 2And R 3Be to contain same alkylene moiety.When using dissimilar alkylene oxides, R 2And R 3Can contain same or different alkylidene groups.
In the formula of chain triacontanol amine compound, p is 2-10, preferred 2 or 3, and q is 0-10, preferred 0-5, r is 0-15, preferred 0-10.Work as R 1Be to contain 1-6, during the moieties of preferred 2-4 carbon atom, R 2Be to contain 2-6, the alkylidene group of preferred 2-4 carbon atom, R 3Be to contain 2-6, the hydroxyalkyl of preferred 2-4 carbon atom.This hydroxyalkyl usually contains 1-3 hydroxyl.When r greater than 0 the time, R 3Generally be monohydroxyalkyl group, for example hydroxyethyl or hydroxypropyl.When r is 0, R 3Generally be to have the nearly monohydroxyalkyl group or a multi-hydroxy alkyl of 4 hydroxyls, for example hydroxyethyl, hydroxypropyl or 1-hydroxyl-2, two (methylol) ethyls of 2-.P, q, r select independently.This just means, for example, when q greater than 0 the time, p can be different value in each repeating unit.In addition, when r greater than 0 the time, R in each ether repeating unit 2Can be identical or different.
Preferred carboxylic acid amide is oil base glycollic amide and oil base diglycollic amide.
Used in the present invention acid, it does not contain any hydroxyl substituent in sour skeleton, and it usually contains nearly 60 carbon atoms.This acid can be monocarboxylic acid or poly carboxylic acid or dimeracid.When using monocarboxylic acid, they usually contain 10-40 carbon atom, more generally 10-30 carbon atom, a particularly 12-24 carbon atom.Such example comprises aliphatic lipid acid for example lauric acid, tetradecanoic acid, margaric acid, palmitinic acid, stearic acid, oleic acid, linolic acid, linolenic acid, nondecylic acid, eicosanoic acid and mountain Yu acid.In the middle of this, preferably use oleic acid, linolic acid or their mixture.When using poly carboxylic acid, for example dicarboxylic acid or tricarboxylic acid, they usually contain 3-40 carbon atom, more generally 3-30 carbon atom, a particularly 3-24 carbon atom.Such polycarboxylic example comprises dicarboxylic acid for example succsinic acid, pentanedioic acid, hexanodioic acid, suberic acid, nonane diacid or sebacic acid, tricarboxylic acid for example 1,3,5-hexanaphthene tricarboxylic acid and tetracarboxylic acid for example 1,2,3,4-BTCA.
Also can use the not substituent acid of hydroxyl in skeleton, dimeracid.At this, such compound is dimeracid or trimer acid.When using dimeracid, they usually contain 10-60, preferred 20-60, most preferably 30-60 carbon atom.Such acid prepares by the dimerization of unsaturated acid, and they usually are made up of the mixture of monomer acids, dimeracid and trimer acid.According to embodiment preferred of the present invention, this acid is the lipid acid for example oleic acid and the linolic acid of dimerization.Such dimeracid usually exists with the trimer acid of the dimeracid and 15% (weight) of the monomer acids, 83% (weight) of 2% (weight) and the mixture of more high-grade acid.Above-described preferred dimeracid and other acid can have been bought from the market maybe and can have been prepared by adopting technique known.
This not the substituent carboxylic acid of hydroxyl can prepare by reaction with alkanolamine.The general formula of this alkanolamine is:
R 1[N (R 1) (CH 2) p] qY wherein, p is 2-10, preferred 2 or 3, q is 0-10, preferred 0-5, Y is-N (R 1) 2, 4-morpholinyl or by R 11-piperazinyl or group-[(CH that group N-replaces 2) pN (R 1)] qR 1, wherein the definition of p and q is the same, each R 1Independently be selected from and have 1-6 carbon atom, the group of the alkyl of preferred 2-4 carbon atom and following formula:
-(R 2O) rR 3Wherein r is 0-15, preferred 0-10, R 2Be to have 2-6 carbon atom, the alkylidene group of preferred 2-4 carbon atom, R 3Be to have 2-6 carbon atom, the hydroxyalkyl of preferred 2-4 carbon atom, condition is at least one R 1Be-(R 2O) rR 3This hydroxyalkyl usually contains 1-3 hydroxyl.When r greater than 0 the time, R 3Generally be monohydroxyalkyl group, for example hydroxyethyl or hydroxypropyl.When r is 0, R 3Generally be monohydroxyalkyl group or have multi-hydroxy alkyl, for example hydroxyethyl, hydroxypropyl or 1-hydroxyl-2, two (methylol) ethyls of 2-until 4 hydroxyls.This p, q and r value are to select independently.This just means, for example, when q greater than 0 the time, p can be different value in each repeating unit.In addition, when r greater than 0 the time, R in each ether repeating unit 2Can be identical or different.So alkanolamine is nitrogen-atoms the sort of that does not contain any band hydrogen.The existence expection at the free hydrogen atom on the nitrogen-atoms like this can cause forming acid amides with fatty acid response the time.
The alkanolamine that can be used to form ester is can buy from the market maybe to prepare by adopting technique known.For example r is 1 or bigger, promptly contains those alkanolamines of an ehter bond or polyethers key, can prepare by one or more alkylene oxide reactions of suitable amine, morpholine or diethylenediamine compound and molar excess.When using the alkylene oxide of same type, R 2And R 3Contain same alkylene moiety.When using dissimilar alkylene oxides, R 2And R 3Can contain same or different alkylidene groups.
According to embodiment preferred, state in the use in the alkanolamine of formula, Y is-N (R 1) 2, p be 2 and q be 0-3.Preferably this alkanolamine is trolamine or triisopropylamine or the 1 and the diethylenetriamine that are replaced by hydroxyethyl or hydroxypropyl of each nitrogen-atoms wherein.
According to another embodiment preferred, in the middle of the formula shown in above-mentioned, Y is the 1-piperazinyl of 4-morpholinyl or replacement, and p is that 2-6 and q are 0 or 1.The example of such alkanolamine comprises aminoethylpiperazine, two-(amino-ethyl) piperazine and the morpholine that is replaced by hydroxypropyl N-.
Described ester can be easy to from the market buy maybe and can maybe can adopt technique known to prepare by the application.
According to an aspect of the present invention, improving the butyrous additive compound is the derivative of the acid of hydroxyl replacement, and it partly contains at least one free carboxyl at sour deutero-.Such compound can for example dicarboxylic acid or dimeracid or trimer acid form as the acid that initial hydroxyl replaces by using poly carboxylic acid.Suitable is that control is used to form the acid of reacting of acid derivative and the mole number of compound makes the compound that forms contain at least one free carboxy functional group at sour derivative moiety.For example, if use acid with two carboxyl functional groups, for example dicarboxylic acid or dimeracid, this mol ratio should be about 1: 1.
According to another aspect of the present invention, this ester contains at least one free carboxy at sour derivative moiety, and does not have hydroxyl substituent on sour skeleton.Such compound can for example dicarboxylic acid or dimeracid or trimer acid form as initial acid by using poly carboxylic acid.The acid that control that suitable is is used to react and the mole number of alkanolamine make the ester that forms contain at least one free carboxy functional group at sour derivative moiety.For example, if use acid with two carboxyl functional groups, for example dicarboxylic acid or dimeracid, this mol ratio should be about 1: 1.
Acid moieties this acid derivative contains under the situation of at least one free carboxy, itself just can use or it can further be derived to improve its performance.The type that is used for the compound of this purpose depends on the type of acid of initial usefulness and the performance of the acid derivative that needs influence usually.For example, can increase the fuel dissolution degree of acid derivative by the part of in its molecule, introducing a dissolved fuel.As such example, what can mention is chain alkyl or alkenyl.For this reason, this acid derivative can with alcohol roh or amine, RNH2 reaction, wherein, R has nearly 30 carbon atoms for example alkyl or the alkenyl of 4-30 carbon atom.Carbonatoms in alkyl or the alkenyl may depend on the number of the carbon atom in acid derivative itself.The free carboxy functional group reactions of these compounds and acid derivative forms another one ester bond or amido linkage.The example of operable special pure and mild acid amides comprises oleyl alcohol and oleylamide.
In addition, this acid derivative can further react, and introduces one or more polarity headgroups in its molecule.This just has the result who increases the oiliness effect, and this increase butyrous effect is that acid derivative is shown.This is considered to because this polarity headgroup increases the affinity of acid derivative and metallic surface.The example that can be used for introducing the compound of one or more polarity headgroups comprises those that introduced above polyamines (for example 1 and diethylenetriamine), monohydroxy-alcohol (for example ethanol and propyl alcohol) and alkanolamine and polyvalent alcohol are for example.
Unless this carboxylic acid derivative is by dimeracid or trimer acid deutero-, this general derivative further reacts the part of introducing fuel dissolution.Dimeracid derivative and trimer acid derivative have contained chain alkyl or alkenyl part often on sour skeleton, it is enough to the fuel dissolution degree that provides suitable.
Though above by the agency of this acid derivative further react, but at first react by polycarboxylic free carboxy functional group, introduce the group or the polarity headgroup of fuel dissolution, the product reaction that generates then forms acid derivative, just forms same last part probably.Certainly, this has just guaranteed that the product that forms after the initial reaction partly contains at least one free carboxy at sour deutero-, so that the formation of acid derivative is still possible.Component (ii)
The example of metallic washing composition is the oily molten high alkalinity salt of basic metal or alkaline-earth metal and the acidic substance below one or more (or its mixture): (1) sulfonic acid, (2) carboxylic acid, (3) alkylphenol, (4) sulfenyl phenolate and (5) feature are the organic phosphoric acids that has a direct C at least.Such organic phosphoric acid comprises by with phosphorization agent for example phosphorus trichloride, phosphorus heptasulfide, thiophosphoric anhydride, tri-chlorination p and s, white phosphorus and halogenation sulphur, or prepared those of phosphorus chloride sulphuring treatment olefin polymer (for example polyisobutene).The most general salt of above-mentioned acid is the salt of sodium, potassium, lithium, calcium, magnesium, strontium and barium.
This metal additive is the oily molten high alkalinity salt of basic metal or alkaline-earth metal preferably.High alkalinity salt is preferred, because metal adds with spissated form, so expense is suitable, but metal need not add with this form.Using term " high alkalinity " is to show the stoichiometric metal-salt of the amount of metal wherein greater than organic acidic group.This comprises low alkalinity washing composition (promptly have TBN and be about those of 6-40) and high alkalinity (promptly have TBN and be about those of 250-500) material.Prepare the common used method of high alkalinity salt and comprise the solution that adds hot acid and surpass the mineral oil of stoichiometric metal neutralizing agent, the metal neutralizing agent is metal oxide, metal hydroxides, metal carbonate, alkali metal bicarbonate salt or metallic sulfide for example, this mixture of carbonating in the presence of promotor, and filter the material that generates.The example that is used as the compound of promotor comprises aldehydes matter, for example the condensation product of phenol, naphthols, alkylphenol, thiophenols, sulfenyl phenolate, formaldehyde and aldehydes matter; Alcohol is methyl alcohol, 2-propyl alcohol, octyl group alcohol, cellosolvo, carbitol, ethylene glycol, stearyl alcohol and hexalin for example; Amine is aniline, phenylenediamine, thiodiphenylamine, Phenyl beta naphthylamine and n-Laurylamine for example.The special effective means for preparing this high alkalinity salt comprises acid mixed with excessive basic alkaline earth metal neutralizing agent and at least a suitable promotor, at the temperature of raising 60-200 ℃ of this mixture of following carbonating for example.
The example of overbased sulfonate comprises high alkalinity sulfonic acid lithium, high alkaline azochlorosulfonate acid sodium, high alkalinity potassium sulfonate, high alkaline calcium sulfonate and overbased magnesium sulphonates, wherein each sulfonate radical is partly linked on the virtue nuclear, it contains one or more aliphatic substituting groups usually successively, so that hydrocarbon solubleness to be provided.
This metal carboxylate can prepare from any organic carboxyl acid.Metal carboxylate preferably for example has those salt of the monocarboxylic acid of 4-30 carbon atom.These acid can be hydrocarbon aliphatic series, cyclic aliphatic or aromatic carboxylic acid.Those aliphatic carboxylic acids that monocarboxylic acid for example has about 4-18 carbon atom are preferred, particularly have those of 6-18 carbon atom.This ring grease acid usually can contain 4-12 carbon atom.Aromatic acid usually can contain one or two condensed ring and contain 7-14 carbon atom, and wherein carboxyl can or be free of attachment on this ring.This carboxylic acid can be the saturated or unsaturated fatty acids with about 4-18 carbon atom.The example that can be used for preparing some carboxylic acid of metal carboxylate comprises butyric acid, valeric acid, caproic acid, enanthic acid, hexahydrobenzoic acid, ring capric acid, naphthoic acid, phenylacetic acid, 2 methyl caproic acid, 2 ethyl hexanoic acid, suberic acid, sad, n-nonanoic acid, capric acid, undecanoic acid, lauric acid, tridecanoic acid, tetradecanoic acid, pentadecylic acid, palmitinic acid, linolenic acid, margaric acid, stearic acid, oleic acid, nondecylic acid, arachic acid, heneicosanoic acid, docosoic acid and erucic acid.
In order to prepare the molten salt of oil of the present invention, most preferred carboxylic acid is a Whitfield's ointment.The example of high alkaline salicylate is lithium salicylate, sodium salicylate, potassium salicylate, calcium salicylate and magnesium salicylate, and wherein the aromatics part is replaced by one or more aliphatic substituting groups usually, so that hydrocarbon solubleness to be provided.
The example of suitable high alkalinity containing metal phenates washing composition comprises, but be not limited thereto, for example high alkalinity phenol lithium, sodium phenylate, potassium phenylate, calcium phenylate, phenol magnesium, sulfuration phenol lithium, sulfuration sodium phenylate, sulfuration potassium phenylate, sulfuration calcium phenylate, sulfuration phenol magnesium, wherein each aryl has one or more aliphatic groups, so that hydrocarbon solubleness to be provided.Above-mentioned high alkalinity metal washing composition is commonly referred to " high alkalinity phenates " or " high alkalinity sulfuration phenates ".
Suitable in addition, though seldom preferred, be the phosphorus-sulfurized alcohol of phosphorus-olefine sulfide of (a) hydrolysis or hydrolysis and/or high alkalinity lithium, sodium, potassium, calcium and the magnesium salts of the phenolic compound that aliphatic series replaces with 10-2000 carbon atom with 10-2000 carbon atom.Other similarly oily molten organic acid high-alkaline base metal and alkaline earth salt is suitable, and for example the high alkalinity aliphatic sulfonate is commonly referred to " sulfonated petro-leum ".Can use the mixture of the salt of two or more different high-alkaline base metals and/or alkaline-earth metal.Equally, also can use the salt of the mixture of two or more different acid or two or more dissimilar acid (for example one or more high alkalinity calcium phenylates and one or more calcium sulphonate).Though rubidium, caesium and strontium salt are spendable, they are very expensive, make can not implement for most application.Equally, though barium salt is that effectively barium is heavy metal, is deleterious material, makes present application seldom select barium salt.
Metallic washing composition can be low alkalinity or overbasic type or its mixture.The total basicnumber of the washing composition of low alkalinity is approximately greater than 8, still less than about 200.The sulfonate that preferred metallic washing composition is high alkalinity calcium and magnesium, sulfuration phenates and Acid Thiosalicylique salt, the every ASTM D of its total basicnumber that has (TBN) 2896-88 at least 200 preferably is higher than 250.Component (iii)
Be used for suds suppressor of the present invention and comprise those suds suppressors that are generally used for fuel composition, for example silicone suds suppressor.When used suds suppressor and high alkalinity metal washing composition present seriously inconsistent the time, advantage of the present invention is tangible especially.With the uncompatibility of high alkalinity metal washing composition is certified by the serious foaming when suds suppressor mixes with this washing composition.At suds suppressor is a kind of utmost point when being insoluble to 25 ℃ the situation of suds suppressor of water, and this uncompatibility is modal.This problem solves by the oiliness improver that adds the above-mentioned type.
Preferred suds suppressor is the polysiloxane polyether copolymer of following formula:
Figure A9810701100131
Wherein R is independently selected from H, OH, C1-3 alkyl, poly-alkoxyl group, poly--(alkoxyl group)-X (wherein X is OH, methyl or ester) and poly-alkoxy derivative, and wherein aromatics, phenols or amphyl all are grafted on alkoxyl group or the polyether chain.Poly-oxyalkyl chain usually contains oxyethyl group or propoxy-unit or its mixture of two kinds.This polysiloxane polyether copolymer can be the organo-siloxane terpolymer, for example contains those and the polyethers that is grafted on the polysiloxane copolymer of alkylphenol or modification alkylphenol derivative.Preferably be insoluble to the suds suppressor of 25 ℃ water basically.
Be used for suitable polysiloxane polyether copolymer of the present invention and comprise the S911 suds suppressor, a kind of polyethers polydimethylsiloxane of having bought from WackerChemie GmbH; Dow Coming  Q2-2600 suds suppressor, a kind of polysiloxane polyether copolymer of having bought from Dow Coming; With the TP325 suds suppressor, a kind of organo-siloxane terpolymer of having bought from OSi Specialties Inc..
Be not that the polysiloxane polyether copolymer suds suppressor of the present invention part is included in 25 ℃ of water solubles and do not demonstrate with high alkaline metal detergent serious inconsistent those.The example of the multipolymer of these types comprises the AG from T.H.Goldschmidt, TEGOPREN  5851 silicone surfactants that Essen, Germany have bought.The suds suppressor of this specific type does not produce the effect of foam stabilization, for this reason, needs oiliness improver of the present invention as a kind of control method.Component (iv)
In embodiment preferred of the present invention, composition comprises the dispersion agent that at least a hydrocarbon is molten.These dispersion agents comprise the succinic diamide of long-chain, the succinate of long-chain, succsinic acid ester-acid amide, long-chain polyamine and the long-chain mannich base of long-chain.The long-chain of these washing composition-dispersion agents contains on average at least 20 carbon atoms, for example average 30-200 carbon atom or more carbon atoms.These long-chain substituting groups are normally from polyolefine oligopolymer or polymer-derived, this polyolefine oligopolymer or polymkeric substance have suitable number-average molecular weight for example about 800,950,1200,1350,1500,1700,2100 or 2300, it is that for example the polymerization or the copolymerization of the mixture etc. of propylene, butylene, iso-butylene, amylene, ethene and propylene form by olefinic monomer successively.
Especially the manufacture method that is suitable for such washing composition-dispersion agent of the additive make fuel composition be known and document in report is arranged.So operable general succinic diamide is described in disclosed PCT patent application WO 93/06194 and the disclosed EP patent application publication number 0441014 (1991.8.14).Cited disclosed succinate, succsinic acid ester-acid amide, people can reference example such as USP 3,184,474; 3,331,776; 3,381,022; 3,522,179; 3,576,743; 3,632,511; 3,804,763; 3,836,471; 3,862,981; 3,936,480; 3,948,800; 3,950,341; 3,957,854; 3,957,855; 3,991,098; 4,071,548; With 4,173,540.Long-chain polyamine dispersant-washing composition is described in for example USP 3,275,554; 3,394,576; 3,438,757; 3,454,555; 3,565,804; 3,671,511; 3,821,302; In EP patent publication No. 382405.The operable suitable molten mannich base washing composition-dispersion agent of fuel is disclosed in for example USP 3,948,619; 3,994,698 and particularly among the USP 4,231,759.
Being used for one group of preferred dispersing agent-washing composition of the present invention is the succinic diamide that forms by following reaction: i.e. polyisobutylene succinic anhydride and polyamines reaction, for example 1, diethylenetriamine, Triethylenetetramine (TETA), tetren, penten and N-[2-hydroxyethyl of the ethylidene polyamines that has an average 2-6 nitrogen-atoms with each molecule particularly] the ethylene diamine reaction.In the middle of these dispersion agents, the GPC number-average molecular weight that preferred polyisobutene has is 750-2300, preferred 800-1350.
Mannich base dispersion agent preferably in addition, it is to form by following substance reaction: (i) alkylphenol, wherein alkyl is to be 750-2300 by number-average molecular weight, preferred 80-1350, the olefin polymer deutero-of 800-1100 most preferably, (ii) polyalkylene polyamine and (iii) formaldehyde or formaldehyde precursor.Most preferably the alkyl of alkylphenol is to be the polypropylene deutero-of 800-1100 by number-average molecular weight, and polyalkylene polyamine is a diethylenetriamine.Dispersion agent reference example that other is useful such as EP 476,196 B1.Component (v)
The discharge that can be included in additional material in the composition of the present invention and be metal matrix improves for example cyclopentadienyl tricarbonyl manganese compound of additive.When such compound was present in the finished product fuel, such compound can reduce exhaust emissions, particularly particle emission and smog.In addition, in composition of the present invention, use the cyclopentadienyl tricarbonyl manganese compound to make the cleanliness factor of cleanliness factor, particularly inlet valve of inlet system further improve.The cyclopentadienyl tricarbonyl manganese compound that can be used for practice of the present invention comprises cyclopentadienyl tricarbonyl manganese, methyl cyclopentadienyl tricarbonyl manganese, the dimethyl cyclopentadienyl tricarbonyl manganese, the trimethylammonium cyclopentadienyl tricarbonyl manganese, the tetramethyl-cyclopentadienyl tricarbonyl manganese, the pentamethyl-cyclopentadienyl tricarbonyl manganese, the ethyl cyclopentadienyl tricarbonyl manganese, the diethyl cyclopentadienyl tricarbonyl manganese, the propyl group cyclopentadienyl tricarbonyl manganese, the sec.-propyl cyclopentadienyl tricarbonyl manganese, tertiary butyl cyclopentadienyl tricarbonyl manganese, the octyl group cyclopentadienyl tricarbonyl manganese, the dodecyl cyclopentadienyl tricarbonyl manganese, the ethyl-methyl cyclopentadienyl tricarbonyl manganese, indenyl manganese tricarbonyls etc. comprise the mixture of the compound that two or more are such.Preferably be the cyclopentadienyl tricarbonyl manganese of liquid in room temperature, mixture of the liquid mixture of methyl cyclopentadienyl tricarbonyl manganese, ethyl cyclopentadienyl tricarbonyl manganese, cyclopentadienyl tricarbonyl manganese and methyl cyclopentadienyl tricarbonyl manganese, methyl cyclopentadienyl tricarbonyl manganese and ethyl cyclopentadienyl tricarbonyl manganese etc. for example.The preparation method of these compounds is described in document for example among the US 2,818,417.
Though be not too preferred, other the manganic compound fuel dissolubility or breakdown of fuel can be included in the composition of the present invention.The illustrative example of these compounds is manganese oleate, manganese naphthenate, octyl group etheric acid manganese and ethylene diaminetetraacetic acid manganese.
In principle, in any liquid fuel that from oil, biological substance, coal, shale and/or oily sand, obtains, can obtain advantage of the present invention.If not exclusive, under most situation, under present environment, this basic fuel will mainly obtain from oil at least.
So, the present invention can be applied to such fuel for example kerosene, rocket engine fuel, aviation fuel, diesel oil, family warming oil, light cycle oil, heavy cycle oil, light gas oil, heavy gas oil, bunker fuel, residual oil fuel, overweight oil fuel, with general any liquid (or flowable) product that is applicable to fuel in engine (for example diesel oil, gas turbine fuel etc.) or combustion unit.Other suitable fuel comprise from biological substance for example the liquid fuel that obtains of vegetables oil (for example rape seed oil, Oil of jojoba, cotton seed wet goods) or waste material deutero-liquid fuel for example from municipal waste and/or industrial waste deutero-fuel.
General, in fuel, use the component of the compositions of additives of a spot of performance that is enough to improve combustionproperty and its used basic fuel.Therefore, this amount will be according to some following factors vary, for example: the working conditions of the type of basic fuel and the finished product fuel that will use.But in general, the concentration (ppm) of this component (active ingredient) in basic fuel is as follows:
General range Preferable range Particularly preferred scope
Component (i) oiliness improver ?????10-400 ????15-200 ?????20-100
Component is metal detergent (ii) The metal component of 1-100ppm The metal component of 5-50ppm The metal component of 10-30ppm
Component is suds suppressor (iii) ??????1-30 ?????2-15 ??????3-8
Contain in addition one or more components (iv) and (under the situation of fuel v), (ppm) is as follows for the concentration of general active ingredient:
General range Preferable range Particularly preferred scope
Component is dispersion agent (iv) ??????10-500 ??????20-200 ?????40-100
Component (the v) discharge improving agent of metal matrix 0.1-50ppm metal The metal of 1-10ppm The metal of 2-10ppm
People can recognize, if you are using, and can be one component (i), (ii) and (iii) and (iv) and/or (v) be blended into respectively in the fuel, perhaps if necessary, they can be blended in the fuel with auxiliary mixed form.Usually, the particular order of such blending step is not crucial.In addition, these components can be with the form blending of solution or diluent.But, preferably,, reduced contingent blending error, and the advantage of consistency and dissolubility property aspect be provided by total enriched material because simplified this blending operation like this with the form blending component utilized of multifunctional additive for lubricating oils of the present invention.A kind of like this enriched material is a part of the present invention, this enriched material usually contains the additive of 99-1% (weight) and solvent that is used for additive or the thinner of 1-99% (weight), wherein solvent or thinner and fuel are miscible and/or can be dissolved in the fuel, will use this enriched material in this fuel.Certainly, this solvent or thinner can be this fuel itself.But the example of other solvent or thinner comprises petroleum solvent, kerosene, alcohol (for example 2-Ethylhexyl Alcohol, Virahol and isodecyl alcohol), aromatic solvent (for example toluene and dimethylbenzene) and cetane number improver (for example 2-ethylhexyl nitric ether).They can use or mix use separately.
Composition of the present invention can further contain the component of optional routine used in fuel composition, for example fuel stabilizer, cetane number improver, deicing agent, combustion improving agent, cold flow improving agent, anti static additive, biocide, antioxidant, sanitas, anti-wax precipitation additives and metal passivator.
The various optional component that can be included in the fuel composition of the present invention is used with the amount of routine.Therefore, the amount of such optional components is not crucial in practice of the present invention.Used amount all is enough to provide fuel composition needed functional performance under any special situation, and such amount is that the those skilled in the art of this area are known.
The following examples further specify the present invention.Embodiment
List the embodiment 1 and 2 and the basic recipe of comparative example 1-4 of listed suds suppressor of eliminating table 2 and oiliness improver below.Its amount is based on a milliliter additive/1000 milliliter fuel.
Table 1
Basic recipe Gram number in the mixture Weight %
Solvent 1 ?????250.77 ????50.14
Emulsion splitter 2 ?????4.62 ????0.92
Sanitas 3 ?????4.12 ????0.82
Metal detergent 4 ?????149.02 ????29.8
Dispersion agent 5 ?????71.02 ????14.2
???MMT/LP62 6 ?????20.55 ????4.11
The 1:2-ethylhexanol; 2: the OFRIC that has bought from Baker Performance Chemical The D5021 emulsion splitter; 3:HiTEC 536 anticorrosive agents, it is the succinimide/acid amides of the low-molecular-weight polyalkylene polyamine bought from Ethyl Corporation; 4:HiTEC 611 washing composition, it is the high alkalinity alkyl benzene calcium sulfonate of having bought from Ethyl Corporation with nominal total alkali number about 300; 5: based on the ashless polyisobutenyl succinimide dispersion agent of polyisobutene, succinyl oxide and the tetren of 950 number-average molecular weights; 6: the cyclopentadienyl tricarbonyl manganese compound in the xylene/heptane solvent mixture.
The fuel additive treating of all processing makes in this basic recipe per 1000 milliliters of fuel 0.44 ml of formulation of having an appointment.
In order to estimate various additives and they effects, measure lather volume and arrive first foamless time of fuel surface fuel composition.The bubble effect that presses down that less lather volume and the short time representation to first improve.Used in these embodiments basic fuel is low-sulfur diesel-oil (sulphur of＜0.05% weight).
The oiliness improver of measured quantity and different suds suppressors are joined in other part of branch of basic components, then the multifunctional additive for lubricating oils that obtains is blended in the basic fuel, produce fuel composition, the amount of the multifunctional additive for lubricating oils that fuel composition in each case contains is equivalent to the suds suppressor and the oiliness improver of about 0.44 milliliter and specified amount of the fuel of per 1000 milliliters basic components, and suds suppressor and oiliness improver have been included in the complete prescription.Then, vibrate rapidly, and measure the needed time of dissipation of foaming in each case at following various fuel of condition of controlling.This method comprises as used in ASTM D1094, uses graduated glass cylinder, and this glass cylinder cleaned minimum one hour with chromic acid, then used the acetone rinsing with water rinse, and is dry then.With fuel these cylinders are installed to 100 milliliters of marks.Tight their lids then, and vibrate 1 minute under the situation of 2-3 stroke of per second, each stroke is a 15-30 cm long and on vertical plane.Then the cylinder of vibration is put in one plane, avoided vibration, maximum lather volume (foamy milliliter number) and the fuel of record forms the first peace and quiet some time of (to first time (second)).
Table 2
Press down foam system The amount ml/1000ml fuel of suds suppressor ?H2658 7Amount ml/1000ml fuel Lather volume (ml) To first time (second)
Embodiment 1 ????S911 8 ???0.011 ???0.045 ????1.7 ????15.7
Comparative example 1 ????S911 ???0.011 ?????0 ?????40 ????＞900
Embodiment 2 ??Q2-2600 9 ???0.011 ???0.045 ?????3 ?????13
Comparative example 2 ??Q2-2600 ???0.011 ?????0 ?????40 ???＞1560
Comparative example 3 There is not suds suppressor ?????0 ???0.045 ????33.3 ????32.3
Comparative example 4 There is not suds suppressor ?????0 ?????0 ????33.3 ?????34
Comparative example 5 Basic fuel is only arranged ?????0 ?????0 ?????33 ?????28
7:HiTEC 2658 oiliness improvers, the oil base diglycollic amide of having bought from Ethyl Corporation.The 8:S911 suds suppressor, the silicone suds suppressor of having bought from Wacker Chemie GmbH.The 9:Q2-2600 suds suppressor, the silicone suds suppressor of having bought from Dow Coming.
Result in the table 2 shows, with the composition that only contains basic fuel (comparative example 5) or the fuel composition (comparative example 1-4) that contains the additive agent mixture outside the scope of the present invention relatively, fuel additive composition of the present invention (embodiment 1 and 2) provides tangible demonstration to reduce volume of foam and to the fuel composition of time of first, as the lather volume of embodiment 1 and 2 resulting tangible less values and to first experimental tests time proved.
Table 3 explanation is resulting in the favourable effect aspect the foam performance by lipid acid oiliness additive being added in the system that contains suds suppressor and high alkalinity washing composition.
Table 3
Component Embodiment 3 Comparative example 6
Solvent 1 ????????24.4g ????????20.83g
Metal detergent 4 ????????17.86g ????????20.3g
Suds suppressor 8 ????????1.63g ????????1.87g
Oiliness improver 10 ????????6.09g ??????????-
Processing speed: be added to the volume in the fuel Every 1000ml fuel 0.41ml preparation Every 1000ml fuel 0.36ml preparation
To first lather collapse time 25.7 second ＞11 minutes
Lather volume/ml ????????8.7ml ????????30ml
10: the oleic acid that obtains from Aldrich Chemical Company.
Result in the table 3 shows, compare with the additive agent mixture (comparative example 6) that contains outside the scope of the present invention, fuel additive composition of the present invention (embodiment 3) provides tangible demonstration to reduce volume of foam and to the fuel composition of time of first, as the lather volume of embodiment 3 resulting tangible less values and to first experimental tests time proved.
The present invention can allow very big variation in its practice, therefore, the invention is not restricted to above-mentioned specific embodiment.And the present invention is in the spirit and scope of appended claim, comprises available legally its equivalent.
The patentee does not want to contribute any disclosed embodiment to give the public, and any disclosed improvement and variation can not fall within the scope of the claims fully, and they are considered under the principle that is equal to is a part of the present invention.

Claims (15)

1. fuel additive composition, it comprises (i) oiliness improver, (ii) high alkalinity metal washing composition and (iii) be insoluble to the suds suppressor of 25 ℃ water basically.
2. the fuel additive composition of claim 1, wherein oiliness improver is carboxylic acid, carboxylic acid amide or carboxylicesters.
3. the fuel additive composition of claim 2, wherein oiliness improver is selected from oil base glycollic amide and oil base diglycollic amide.
4. the fuel additive composition of claim 1, wherein the high alkalinity metal washing composition is selected from calcium sulphonate, sulfonic acid magnesium, sulfuration calcium phenylate, sulfuration phenol magnesium, calcium salicylate, magnesium salicylate, and wherein the total basicnumber of this washing composition (TBN) is pressed ASTM D2896-88 and is at least 200.
5. the fuel additive composition of claim 1, wherein suds suppressor is the silicone suds suppressor that is insoluble to 25 ℃ water basically.
6. the fuel additive composition of claim 5, wherein silicone suds suppressor is the polysiloxane polyether copolymer that is insoluble to 25 ℃ water basically.
7. the fuel additive composition of claim 1, it also contains the material that at least a discharge that is selected from dispersion agent, metal matrix improves additive, emulsion splitter and sanitas.
8. the fuel additive composition of claim 7, wherein dispersion agent is the molten dispersion agent of hydrocarbon, this dispersion agent is selected from long-chain succinimide, long-chain succinate, long-chain succsinic acid ester-acid amide, long-chain polyamine and long-chain mannich base.
9. the fuel additive composition of claim 7, wherein to improve additive be the cyclopentadienyl tricarbonyl manganese compound to the discharge of metal matrix.
10. multifunctional additive for lubricating oils, it contains the additive of claim 1 of 99-1% (weight) and solvent that is used for additive or the thinner of 1-99% (weight), and this solvent or thinner are miscible and/or can be dissolved in the fuel that will use this enriched material.
11. a fuel composition, it contains (a) a large amount of basic fuel and (b) fuel dope of a spot of claim 1, and wherein the amount of this fuel dope is enough to improve the foam performance of this fuel.
12. by mixing (a) a large amount of basic fuel and (b) fuel composition that obtains of the fuel dope of a spot of claim 1, wherein the amount of this fuel dope is enough to improve the foam performance of this fuel.
13. a minimizing contains the high alkalinity metal washing composition and is insoluble to foamy method in 25 ℃ the fuel composition of silicone suds suppressor of water basically, wherein oiliness improver and said fuel composition is mixed.
14. the method for claim 13, wherein oiliness improver is carboxylic acid, carboxylic acid amide or carboxylicesters.
15. the method for claim 13, wherein silicone suds suppressor is the polysiloxane polyether copolymer that is insoluble to 25 ℃ water basically.
CN98107011A 1997-02-17 1998-02-17 The use of lubricity additives for reducing foam in fuels Expired - Fee Related CN1090230C (en)

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DE10251312A1 (en) * 2002-11-04 2004-05-19 Basf Ag Additive mixture useful for improving antifoam performance of fuels comprises a silicone antifoam and a lubricity improver selected from neutralized fatty acids and long-chain carboxylic acids and their esters
US20050005506A1 (en) * 2003-07-08 2005-01-13 Henly Timothy J. Distillate fuel compositions for improved combustion and engine cleanliness
US7696136B2 (en) 2004-03-11 2010-04-13 Crompton Corporation Lubricant compositions containing hydroxy carboxylic acid and hydroxy polycarboxylic acid esters
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