CN101319154A - Conductivity improving combination of cerium oxide and detergents for diesel fuels - Google Patents
Conductivity improving combination of cerium oxide and detergents for diesel fuels Download PDFInfo
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- CN101319154A CN101319154A CNA2007101528749A CN200710152874A CN101319154A CN 101319154 A CN101319154 A CN 101319154A CN A2007101528749 A CNA2007101528749 A CN A2007101528749A CN 200710152874 A CN200710152874 A CN 200710152874A CN 101319154 A CN101319154 A CN 101319154A
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- 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
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- C10L10/02—Use of additives to fuels or fires for particular purposes for reducing smoke development
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Abstract
The disclosure provides conductivity improving concentrates and methods for improving conductivity and reducing risks associated with static discharge in middle distillate fuel composition compositions, particularly diesel fuels. The conductivity improvement is provided with the combination of cerium oxide nanoparticles and dispersant/detergent and shows aged conductivity comparable to or higher than that obtained with conventional antistatic agents.
Description
The cross reference of related application
This application is the part continuation that application on September 19th, 2006, name are called the U. S. application US 11/533,200 of the diesel-dope that contains cerium or manganese and washing composition.
Technical field
The present invention relates to give the diesel-dope of the fuel stability of burning that finished diesel fuel machine fuel improves and raising.The invention still further relates to and be used to improve intermediate oil fuel composition, the particularly composition of the specific conductivity of diesel-fuel, the most particularly low-sulfur and ultra low sulfur diesel fuel and method.
Background technology
In diesel-fuel, used cerium oxide nanoparticles as the convertor catalyzer of eliminating the poisonous fume discharge.Cerium oxide is also having application aspect the particle emission that reduces diesel motor.Envirox
TMFuel Borne Catalyst is a kind of diesel-fuel ignition dope that reduces fuel consumption and reduce the harmful exhaust discharging.
Have been found that some organometallic compound is effective as the ignition dope of distillate fuel such as household fuel wet goods.For example, U.S. Pat 3,112,789 have described cyclopentadienyl tricarbonyl manganese have been used for this purpose, and methyl cyclopentadienyl tricarbonyl manganese (MMT) compound are sold as this type of ignition dope that distillates fuel with the form of the solution in hydrocarbon diluent.Two (cyclopentadienyl) iron is also as ignition dope propaganda and the sale used for this fuel.
U.S. Pat 3,883,320 and US 3,891,401 instructed in jet fuel the salt that adds transition metal such as manganese and alkaline-earth metal such as calcium to reduce settling and cigarette.Manganese/calcium the weight ratio of these patents needs about 5/1 and the metal group resultant of 200-600ppm are (in ' 401 patents, 200-500ppm).
Yet, in some additive combination preparation diesel-fuel, can encounter difficulties, thereby cause muddiness, precipitation, insoluble, inadequate fuel economy and inadequate cigarette to reduce.Appearance is to the demand of hydrocarbon matter fuel with the compositions of additives that dissolves in fuel, the dust that described composition produces in the time of not only can reducing fuel combustion, cigarette and/or carbonaceous product, and can improve the solvability in fuel and improve the fuel economy that fuel combustion produces.In this demand of realization, it also is important that a kind of like this additive is provided, this additive prevents from or suppresses residue at least to be deposited on the crucial engine or burner part or surface, and the fuel composition with gratifying physicals such as thermostability and stability in storage is provided.It also is extremely desirable that a kind of like this compositions of additives is provided, said composition can reduce or be suppressed at the toxic discharge (for example, carbon monoxide, unburned hydrocarbon, polyaromatic and/or particulate) that forms when using fuel in engine or burner or the similar combustion unit.It also is very desirable purpose that the compositions of additives that can reduce fuel consumption is provided.Therefore, there are the improved diesel-fuel additive of the fuel economy that reduces and improve for the organo-metallic fuel dope solvability of the burning that raising is provided, raising, the turbidity of reduction, improved cigarette and the needs of diesel-fuel additive combination.
Some intermediate oil fuel composition, particularly diesel-fuel can produce static, particularly when quick travel when this fuel being assigned in tank vessel or other free flowing bulk material container (bulkcontainer) or the container.Though diesel-fuel is not very volatile, the tank vessel that is used to transport diesel-fuel also is used for transport gasoline, kerosene and other more volatile and inflammable liquid.Even distribute more volatile fuel from oil tank after, steam also still exists, thus the burning that the spark that brings static by fuel composition to discharge to produce causes or the danger of blast.
These danger become more serious in the universal day by day and use along with low-sulfur fuel in recent years, even become more serious along with the introducing of ultra low sulfur diesel fuel in recent months.The method that is used for removing from fuel desulfuration has also reduced the concentration of other polar compound the fuel, and this has reduced the ability of fuel dissipation static charge.
In order to alleviate the burning that brings by low-sulfur fuel and super low sulfur fuel or the danger of blast, normally in being assigned to fuel in the free flowing bulk material container or before in fuel, add conductivity improver.Conductivity improver as its name suggests, improves the specific conductivity of fuel, thereby makes any build-up of static charges safety in fuel large volume transportation dissipate and do not produce spark.Conductivity improver has another name called static inhibitor.
The conductivity improver or the static inhibitor of the common species of using in the fuel, particularly diesel-fuel are Innospec Fuel Specialties, LLC, and Newark, Delaware sells
The board static inhibitor.Yet
Board static inhibitor sulfur-bearing.Therefore, in diesel-fuel, add
Static inhibitor has reduced some benefit of using super low sulfur fuel.In addition, these static inhibitor are very expensive.
And the static inhibitor of sulfur-bearing has brought another problem when using with additive concentrate that contains basic nitrogen or fuel.Specifically, the applicant has been noted that when using in additive concentrate that is containing basic nitrogen or the fuel mixture conduction that conventional static inhibitor provides is improved very rapidly and consumed.This is disadvantageous because its overslaugh these static inhibitor premixs are incorporated in the additive concentrate that contains basic nitrogen.Many components in the general fuel dope concentrate such as dispersion agent, washing composition, cetane number improver etc. all comprise nitrogenous compound.Therefore, the usually essential static inhibitor that adds sulfur-bearing separately by other component in the additive concentrate.Therefore, the static inhibitor of these kinds must be remained in the independent container in warehouse, and join in the fuel separately.Therefore, the static inhibitor of these kinds also needs additional expenses and the complicacy aspect storage, operation and distribution except that their inherent extra-expenses.
Therefore, the composition and the method for electrostatic accumulation and discharging in the needs solution intermediate oil fuel composition.
Summary of the invention
An embodiment of Ti Chuing provides the diesel-fuel additive that contains cerium source such as cerium oxide particle or nano particle and diesel-fuel washing composition combination herein.
In one embodiment, diesel-fuel additive combination oxidation-containing cerium nano particle, cetane number improver, diesel-fuel washing composition and demulsifying compound.More particularly; another embodiment can oxidation-containing cerium particle or nano particle, contain diesel-fuel washing composition/dispersion agent, the demulsifying compound of alkylating (HR-PIB) succinimide polyamine and cetane number improver (for example nitric acid 2-ethylhexyl), can also the containing metal deactivator.
In one embodiment, can use the additive combination of oxidation-containing cerium particle or nano particle to handle diesel-fuel with the processing rate (treat rate) of the about 200ppm of about 1-in diesel-fuel.It is desirable that higher and cerium oxide lower aq is used for some.
Diesel-fuel additive combination of the present invention can also contain blended metal ignition dope such as cerium/manganese and cerium/manganese/iron cpd, alloy or mixture.The alloy that embodiment is herein used form of nanoparticles or contained two or more metals of nano particle improves solvability or the dispersiveness in fuel.
Another embodiment herein provides the diesel-fuel of oxidation-containing cerium nano particle, cetane number improver and washing composition and low-phosphorous demulsifying compound.
In another embodiment in this article, propose a kind of method that improves the efficient of diesel fuel for internal combustion engines machine fuel, in this fuel, add the diesel-fuel additive combination of oxidation-containing cerium nano particle, washing composition and demulsifying compound before this method is included in and is incorporated into fuel in the vehicles that comprise oil engine or other device.
Other embodiment herein comprises method, the method that improves diesel-fuel stability, the method that reduces cigarette in the diesel combustion that improve diesel-fuel efficient (fuel economy), improve the deliquescent method of organo-metallic fuel dope in diesel-fuel, reduce the turbidity of diesel-fuel with diesel-fuel additive method, reduce foamy method in the diesel-fuel and reduce the method for the filter stoppage of filter for diesel fuel.
In other embodiment, the invention provides a kind of middle runnings oil fuel additive concentrate, described concentrate comprises static inhibitor, this static inhibitor comprises compound cerium oxide particle and dispersion agent/washing composition; Fuel contains the combination as the cerium oxide particle and the dispersion agent/washing composition of static inhibitor.
In another embodiment, the invention provides a kind of method of distributing the middle runnings oil fuel, comprise the step that in fuel, adds the static inhibitor that contains compound cerium oxide particle and dispersion agent/washing composition.
In another embodiment, the invention provides a kind of reduction by electrostatic discharged catching fire or the method for explosion hazard of causing, may further comprise the steps: the middle runnings oil fuel is provided, add and the specific conductivity of cerium oxide particle compound dispersion agent/washing composition, thereby reduce electrostatic discharged danger with raising fuel.
Should be understood that: top general introduction and following detailed all are exemplary with illustrative, are the further explanations that is used to provide as the present invention for required protection.
Embodiment
In one embodiment, the invention provides a kind of solvable diesel-fuel additive combination that maybe can be scattered in cerium oxide particle in the diesel-fuel or nano particle that contains.More importantly, in one embodiment, the diesel-fuel additive combination contains the demulsifying compound compound to reduce or eliminate at pumping, distribution, filling jar and to use and add usually observed foam and/or emulsion problem in the thinner diesel-fuel.
In one embodiment, the demulsifying compound that uses in this diesel-fuel additive has the phosphorus content greater than 30 mg/kg demulsifying compounds.Yet, have been found that at present phosphorus content by reducing demulsifying compound in the diesel-fuel additive (no matter be have a mind to exist or exist with the form of pollutent) has improved fuel additive composition greatly and the stability of the fuel that obtains, and turbidity reduces obviously.Therefore, can in demulsifying compound, use the phosphorus content of about 30 mg/kg at most, or use the phosphorus content of about 24 mg/kg, in another embodiment, use the phosphorus of about 8 mg/kg, in another prescription, in the diesel-fuel demulsifying compound, use about 0.12 mg/kg phosphorus content.Along with phosphorus content descends, obtaining astonishing and unexpected improvement aspect turbidity reduction and the fuel stability.
Demulsifying compound herein (or cleaning agent) can be any one commercially available material, such as but not limited to oxyalkylated novolac polymer, as with commercially available those of the title of " NALCO " (trade mark) 7007 (not comprising Nalco) and " TOLAD " (trade mark) 2683 (not comprising Petrolite), alkylating phenol and by its deutero-resin, the alkyl phenol resin of-oxylization (oxylated) and yuban with 4-(1, the 1-dimethyl ethyl) phenol, propylene oxide (methyloxirane) and oxyethane, the EO/PO resin of ethoxylation, macrogol ester, ethylene oxide resin.
Therefore, this paper proposes a kind of diesel-fuel additive combination of oxidation-containing cerium nano particle, described cerium oxide nanoparticles has usually and is no more than 1 micron size, be no more than 300 nanometers in one embodiment, 1-300 nanometer for example, for example 1-150 nanometer, particularly 1-50 nanometer, especially 1-20 nanometer.This diesel-fuel additive combination can also contain at least a diesel-fuel washing composition/dispersion agent that is selected from succinimide, Mannich base, acid amides, amine and the polyetheramine.
In addition, this diesel-fuel additive combination can contain phosphorus content reduction, for example the highest about 24 mg/kg, or about 8 mg/kg-Yue 24 mg/kg, or the demulsifying compound of about 0.1 mg/kg-Yue 8 mg/kg.Obtained by this way to give the diesel-fuel additive combination that the outstanding turbidity decline of diesel-fuel, the raising of additive solvability, fuel stability raising, cigarette minimizing, combustion modifications and fuel economy improve.
Another benefit of the present invention is that demulsifying compound is with regard to its improved performance with regard to the performance of expecting in fuel dope and the finished product fuel.In having the fuel of washing composition/dispersion agent, be easy to form milk sap, therefore need demulsifying compound.Make the demulsifying compound passivation or all reduce the emulsion breaking effect, thereby cause more emulsification with any reaction of demulsifying compound reaction.Thereby the deemulsification that provides a kind of method to improve fuel dope by this way, this method comprise add cerium oxide nanoparticles, washing composition and demulsifying compound that in fuel dope wherein demulsifying compound has the phosphorus less than about 30 mg/kg.In another embodiment, this demulsifying compound has the phosphorus of the highest about 24 mg/kg, or the phosphorus that in an independent embodiment, has about 8 mg/kg-Yue 24 mg/kg, or In yet another embodiment, has the phosphorus of about 0.1 mg/kg-Yue 8 mg/kg.
The amount of cerium oxide nanoparticles, washing composition and the demulsifying compound that uses in present disclosed embodiment can change according to other required component in the character of required purposes, diesel-fuel and additive combination or the finished product fuel.
A kind of diesel fuel composition that contains the compositions of additives of a large amount of diesel-fuels and less improvement quantity combusted is provided in another embodiment, this compositions of additives comprises: a) one or more dissolve in the component of fuel, comprise in manganese and/or cerium compound, mixture or the alloy one or more; B) one or more dissolve in washing composition fuel, alkali metal containing or alkaline-earth metal, neutral or alkaline basic metal or the alkaline earth salts of one or more in for example at least a sulfonic acid and/or at least a carboxylic acid and/or at least a Whitfield's ointment and/or at least a alkylphenol and/or at least a sulfurized alkylphenol; And c) demulsifying compound that reduces as the phosphorus content that limits above, wherein component a) thinks that fuel provides the amount of 0.1-5ppm manganese, cerium or manganese and cerium to have components b) think that fuel composition provides the amount of 5-50ppm basic metal and/or alkaline-earth metal to exist.This embodiment can also contain one or more alkyl nitrate ester selected cetane number improvers.
By improving the specific conductivity of fuel, fuel can dissipate preferably by the static charge of large volume transfer the fuel generation as in fuel being assigned to tanker truck or light rail car (rail car) time.The static charge because fuel can dissipate preferably, so fuel seldom can produce spark, and spark can light exist in the zone, by fuel itself or the volatile cigarette that causes by the fuel of the front of once in tank vessel, transporting.
Certain embodiments of the invention are based on the applicant's discovery, and promptly the compound of cerium oxide nanoparticles and dispersion agent/washing composition provides unexpected and surprising collaborative antistatic benefit for the middle runnings oil fuel.These embodiments also provide the specific conductivity benefit and need not add the sulfocompound picture in super low sulfur fuel
Static inhibitor, thus the environmental protection benefit also is provided.
These embodiments are particularly suitable for the intermediate oil fuel composition.The intermediate oil fuel composition includes but not limited to jet fuel, diesel-fuel and kerosene.In one embodiment, fuel is the low-sulfur fuel that sulphur is lower than about 50ppm.In one embodiment, fuel is the diesel-fuel of super low sulfur or the kerosene of super low sulfur.It is generally acknowledged that super low sulfur fuel has the sulphur of about 15ppm at the most, more preferably the sulphur of 10ppm at the most.It is generally acknowledged that term " diesel-fuel " is the common name that comprises diesel oil (diesel), biofuel (biodiesel), biofuel deutero-fuel, artificial diesel oil and their mixtures.Although biofuel is not distillate fuel technically, it also still comprises in the definition that is the term " intermediate oil fuel composition " that uses in whole application and claims.
The present invention includes jet fuel, although conventionally it is not considered as " low-sulfur " or " super low sulfur " fuel, because their sulphur content is relatively very high.Yet the specific conductivity that jet fuel also can be benefited from these embodiments is improved and irrelevant with their sulphur content.
The term that uses among the present invention " firing system " and " device " comprise any device, machine or the engine that utilizes combustible fuel to produce power wholly or in part.For example, this term comprises diesel oil-cell mixed power automobile, gasoline-cell mixed power automobile, two-stroke engine, all burners or combustion unit, comprises for example fixed burner, waste incinerator, diesel-fuel burner, diesel-fuel engine, transportation diesel engine, Fuel Petroleum burner, gasoline engines, power station generator etc.Benefit from all combustion units, system, equipment and/or engine that hydrocarbon matter fuel combustion system of the present invention comprises combustion fuel.Term " firing system " also comprises the inside and outside combustion equipment that can burn or wherein can burn hydrocarbon matter fuel, machine, engine, turbine engine, jet engine, boiler, incinerator, evaporation burner, plasma burner system, plasma arc, fixed combustion device etc.
In diesel-fuel, used cerium oxide nanoparticles as the convertor catalyzer of eliminating the poisonous fume discharge.Cerium oxide is also having application aspect the particle emission that reduces diesel motor.For example, Oxonica, Ltd. (Oxfordshire, Envirox England)
TMFuel BorneCatalyst is a kind of diesel-fuel ignition dope that reduces fuel consumption and reduce the harmful exhaust discharging.Cerium oxide particle has also shown the benefit that reduces muddy and foam formation in the diesel-fuel.
Although can use common cerium oxide particle, have been found that in certain embodiments of the invention it is useful using the cerium oxide that is doped with the component that causes forming the excess oxygen room.This often means that for the oxygen room is provided, doping agent is a divalence or tervalent.For the oxygen room is provided, this dopant ion must be divalence or tervalent element ion, and it is the metal of IIA, IIIB, VB or group vib in rare earth metal, transition metal or the periodictable.They also must have and allow the size of ionic bond within the cerium oxide nanoparticles surf zone.Therefore, should not use the big metal of ionic radius.
Generally, doping oxide has formula Ce
1-xM
xO
2Or [(CeO
2)
1-n(REO
y)
n]
1-kM '
kM is described metal or metalloid, particularly Rh, Cu, Ag, Au, Pd, Pt, Sb, Se, Fe, Ga, Mg, Mn, Cr, Be, B, Co, V, Zr, Ti and Ca and Pr, Sm and Gd in the preceding formula, and the value of x is up to 0.3, be generally 0.01 or 0.1-0.2, M ' is described metal or the metalloid except that rare earth in the back formula, and RE is a rare earth, and y is 1 or 1.5, n and k can be identical or different, the value of each is up to 0.5, and is preferably the highest by 0.3, is generally 0.01 or 0.1-0.2.In applicant's PCT/GB2002/005013, can find more details, as a reference with it.
Usually, cerium oxide particle has and is no more than 1 micron size, in special embodiment, is no more than 300 nanometers, for example 1-300 nanometer, for example 1-150 nanometer, particularly 1-50 nanometer, especially 1-20 nanometer.
In certain embodiments, preferably apply cerium oxide particle to prevent reunion.For this reason, can under the situation that coating-forming agent organic acid, acid anhydrides or ester or Lewis base are arranged, particle be pulverized in organic solvent.Have been found that in this mode that comprises that original position applies and significantly to improve oxide coating.And, in many cases, can directly use the product that obtains without intermediate steps.Therefore, in some coating methods, before the particles dispersed that will apply is in hydrocarbon flux, be necessary dry they.Therefore, cerium oxide particle can be dispersed or dissolved in the fuel or in the another kind of hydrocarbon compatible with this fuel.
The particle that is subjected to this processing should have big as far as possible surface-area, and preferably before coating, this particulate surface-area is at least 10m
2/ g, preferred surface is long-pending to be at least 50 or 75m
2/ g, for example 80-150m
2/ g or 100-300m
2/ g.
Coating processes comprises pulverizes this particle to prevent to form any aggregate.The method that can be used for this purpose comprises high-speed stirring or drum commentaries on classics and utilizes colloidal mill, ultrasonic wave or ball milling.Ball milling is preferred.Can in PCT/GB02/02312, find the more details of this coating.
The concentration of cerium oxide is generally 0.1-10% by weight in the additive, usually 0.5-5%.And cerium oxide nanoparticles has usually and is no more than 1 micron size, is no more than 300 nanometers in one embodiment, for example 1-300 nanometer, for example 1-150 nanometer, particularly 1-50 nanometer, especially 1-20 nanometer.
The existence that has been found that washing composition/dispersion agent can make cerium oxide particle stable in fuel or fuel dope combination.The special washing composition that can use in the present invention comprises the nitrogenous washing composition of alkalescence.Suitable ashless washing composition/dispersion agent comprises acid amides, amine, polyetheramine, Mannich base and preferred succinimide, although metallic in this article washing composition also is effective.
In many patent specifications, all described these dispersion agents, mainly be to use for lubricant compositions, but also described their uses in hydrocarbon fuel as additive.Ashless dispersion agent stays metallic resistates hardly or not when burning.They are only carbon containing, hydrogen, oxygen usually, and are in most of the cases also nitrogenous, but also contain other non-metallic element such as phosphorus, sulphur or boron sometimes.Useful especially in this article ashless dispersant/washing composition be by with the maleic anhydride of polyamine reaction on " hyperergy " polyisobutene (HR-PIB) of replacing and obtaining, thereby realize the dispersiveness of content to obtain to improve of about 5.4% nitrogen.This material is with HiTEC
(R)4007 purchase the Corporation in Afton Chemical.In the fuel dope combination of this paper, can use washing composition/dispersion agent with the content of about 20% weight of about 5-.
In one embodiment, washing composition is the succinimide that each molecule on average has at least 3 nitrogen-atoms.Succinimide is preferably aliphatic, can be saturated or undersaturated, and especially olefinic is undersaturated, for example the alkyl or alkenyl succinimide.Washing composition generally is to be formed by the alkylene polyamine mixture that the alkyl or alkenyl amber acylation agent that has at least 35 carbon atoms in alkyl or alkenyl usually and each molecule on average have at least 3 nitrogen-atoms.In another embodiment, polyamine has 4-6 nitrogen-atoms at each molecule.Preferably; it can be by being 500-10 derived from number-average molecular weight, the polyisobutenyl amber acylation agent of 000 polyisobutene and can comprise ring-type and non-annularity part, ethylidene polyamines with the average composition from the Triethylenetetramine (TETA) to the penten form.Therefore, chain generally has 500-2500, and the molecular weight of 750-1500 especially, and the chain with molecular weight of about 900 and 1300 is useful especially is that the succinimide of about 2100 aliphatic chain also is useful although have molecular weight.At US-A-5, can find more details in 932,525 and 6048373 and EP-A-432,941,460309 and 1,237,373.
The example of useful in this article suitable containing metal washing composition includes but not limited to such as following material: phenol lithium, sodium phenylate, potassium phenylate, calcium phenylate, phenol magnesium, sulfurized phenol lithium, sulfurized sodium phenylate, sulfurized potassium phenylate, sulfurized calcium phenylate and sulfurized phenol magnesium, wherein each aryl has one or more fatty group, thereby gives the hydrocarbon solvability; Any subsalt (usually being called " high alkalinity " phenolate or " high alkalinity sulfuration phenolate ") in above-mentioned phenol or the sulfuration phenol; Sulfonic acid lithium, sodium sulfonate, potassium sulfonate, calcium sulphonate and sulfonic acid magnesium, wherein each sulfonic acid partly invests and contains usually on the substituent aromatic proton of one or more aliphatics, thereby gives the hydrocarbon solvability; Any subsalt in the above-mentioned sulfonate (usually being called " overbased sulfonate "); Lithium salicylate, sodium salicylate, potassium salicylate, calcium salicylate and magnesium salicylate, thus wherein the aromatics part is given the hydrocarbon solvability by one or more aliphatics substituting groups replacements usually; Any subsalt in the above-mentioned salicylate (usually being called " high alkaline salicylate "); Have 10-2000 carbon atom hydrolysis sulphur phosphatization (phosphosulphurised) alkene or have the hydrolysis phosphorus sulfurized alcohol of 10-2000 carbon atom and/or lithium, sodium, potassium, calcium and the magnesium salts of the phenolic compound that aliphatics replaces; The cycloaliphatic carboxylic acid's that aliphatic carboxylic acid and aliphatics replace lithium, sodium, potassium, calcium and magnesium salts; The subsalt of above-mentioned carboxylic acid (usually being called " high alkalinity carboxylate salt ") and many other similar oily molten organic acid basic metal and alkaline earth salts.
Can use the mixture of the salt of two or more Different Alkali metals and/or alkaline-earth metal.Equally, also can use the salt (for example, one or more calcium phenylates and one or more calcium sulphonate) of the mixture of two or more different acid or two or more dissimilar acid.Though rubidium, caesium and strontium salt are feasible, their cost makes them use for great majority and becomes impracticable.
According to one embodiment of the invention, in early days cerium oxide nanoparticles is joined in the diesel-fuel by being incorporated in the diesel-fuel additive combination.Have been found that introduce particle in this way can be by preventing to reunite and preventing cerium particulate surface area losses thus and the fuel efficiency that in diesel engine, causes improving.The present invention embodies the above-mentioned performance that it is used for improving cerium oxide particle or nano particle more fully by making cerium oxide.This is to remove cerium by reducing owing to form throw out from fuel, thereby the cerium atom that keeps more can be used for combustion catalysis and reduce discharge or other benefit is realized.
Another benefit of the present invention is owing to having reduced or eliminated the precipitation that caused by the interaction between for example cerium atom or particle and fuel additive component and/or the pollutent, having separated out and/or the muddy filter stoppage that has reduced fuel filter.The fuel filter fault can cause the running of an engine difficulty, finally causes shutting down.An embodiment is that the interaction that reduces according to the present invention between phosphorus and cerium oxide particle or the nano particle reduces the fuel filter obstruction.The measurement of this benefit can be observed from IP 387 filtration tests.Therefore, a kind of method that reduces the filter stoppage of fuel filter in the vehicles that use diesel engine or other device is provided herein, this diesel combustion diesel-fuel also has fuel filter, and described method is included in diesel-fuel is incorporated into the vehicles or the diesel-fuel additive combination of adding oxidation-containing cerium nano particle, washing composition and demulsifying compound in this fuel before of other device.
Therefore, the invention provides a kind of method that improves the efficient of combustion engine fuel, this method adds oxidation-containing cerium and/or the metallic substance that dissolves in fuel in manganese source and the washing composition and the demulsifying compound of the additive that acts as a fuel before being included in fuel being incorporated into the vehicles that comprise oil engine or other device in this fuel.In this way introduce cerium oxide need hardly or not for other introducing method as the required any vehicle fuel management system of dosing (on-board dosing) in using.Fuel efficiency is that cerium oxide particle is incorporated into result in the fuel.
Therefore, the present invention also provides a kind of fuel additive composition, its oxidation-containing cerium nano particle and/or manganese source and be preferably the washing composition of aliphatics succinimide and phosphorus less than the demulsifying compound of about 8 mg/kg.In another embodiment, fuel additive composition also contains demulsifying compound and the cetane number improver reagent as limiting above.
The concentration of cerium oxide particle or nano particle is generally in the diesel-fuel additive, by weight, and 0.1-10%, 0.5-5% usually.
The fuel dope of introducing at refinery generally can contain cetane number improver, cold flow improver, antioxidant and metal passivator.Therefore, fuel additive composition of the present invention can be introduced one or more in these.Therefore, the invention provides a kind of like this fuel additive composition, its oxidation-containing cerium nano particle and/or colloid, washing composition, demulsifying compound, randomly, be selected from cetane number improver (being also referred to as ignition improver) (for example alkyl nitrate ester selected), cold flow improver (for example polyester) and antioxidant (as phenoplast, for example 2,6-DI-tert-butylphenol compounds or phenylenediamine such as N, N '-di-sec-butyl-p-phenyl enediamine) and metal passivator such as salicyclic acid derivatives, N for example, N-two salicylidenes-1, one or more components in the 2-propylene diamine.
In diesel-fuel additive combination of the present invention, also can use slip additive, rust-preventive agent and defoamer.
In another embodiment of the invention, fuel additive composition can contain the demulsifying compound that mixture, blend, compound or the alloy of two or more metals and washing composition/dispersion agent and phosphorus are up to about 30 mg/kg.The mixed metal catalyst system is known, but needs and provide it at present to use with washing composition and demulsifying compound and can reduce or eliminate muddiness, unstable or precipitation.
Therefore, the improved fuel additive composition of the present invention can comprise that the material, washing composition/dispersion agent and the phosphorus that contain two or more metallic combustioncatalystss are up to the demulsifying compound of about 30 mg/kg.In another embodiment, this demulsifying compound has the phosphorus of the highest about 24 mg/kg, or in an independent embodiment, has the phosphorus of about 8 mg/kg-Yue 24 mg/kg, or In yet another embodiment, has the phosphorus of about 0.1 mg/kg-Yue 8 mg/kg.For example, washing composition/dispersion agent and demulsifying compound can be as described above.These metallic combustioncatalystss can be cerium oxide particle or nano particle, manganese source such as methyl cyclopentadienyl tricarbonyl manganese and source of iron such as dissolved ferric oxide and ferrocene.
" manganese " refers to any manganese or manganiferous material, compound or precursor herein, such as but not limited to
Purchase methyl cyclopentadienyl tricarbonyl manganese and sulfonic acid manganese, phenol manganese, manganese salicylate, cyclopentadienyl tricarbonyl manganese, alkyl cyclopentadienyl manganese tricarbonyl, organic manganese tricarbonyl derivative, alkyl cyclopentadienyl manganese derivative, bicyclic pentadiene manganese, two alkyl cyclopentadienyl manganese, neutrality and high alkalinity bigcatkin willow acid manganese, neutrality and high alkalinity phenol manganese, neutrality and high alkalinity sulfonic acid manganese, manganese carboxylate, manganese oxide and their combination and mixture in Afton Chemical Corporation.
Therefore, can use cerium/manganese mixture or alloy in this article; Can use cerium/manganese/iron mixture or alloy in this article; Can use cerium/iron mixture or alloy in this article; Or can use manganese/iron mixture or alloy in this article.
A kind of fuel dope is provided, and its oxidation-containing cerium and manganese source, washing composition and phosphorus content mostly are the demulsifying compound of about 24 mg/kg most.In an independent embodiment, the phosphorus in the demulsifying compound is about 8 mg/kg-Yue 24 mg/kg, is the phosphorus of about 0.1 mg/kg-Yue 8 mg/kg In yet another embodiment.
And, also containing in the fuel additive composition of washing composition/dispersion agent and demulsifying compound in preparation, cerium oxide particle or nano particle can combine with ferrocene (source of iron).Therefore, for example provide a kind of fuel additive composition, its oxidation-containing cerium (Envirox of Oxonica for example
TM), ferrocene (generally on sale), succinimide washing composition/dispersion agent (Afton ChemicalCorporation's
4007, obtain by the 950MW polyisobutene and the polyamine reaction that have greater than 70% vinylidene and maleic anhydride, thereby realize that final N content is about 6.0%) and demulsifying compound (Tolad 9357 of Baker Petrolite), said composition has excellent ignition dope activity, no muddiness or precipitation, good cigarette reduces and the fuel economy of raising.
The composition of certain embodiments of the invention and method can provide the specific conductivity of 25pS/m at least for fuel under time of carrying and temperature.This specific conductivity is enough to reach the new ASTM standard (ASTM D975 and modification and annex thereof) of the diesel-fuel specific conductivity of suggestion, and it is according to any suitable test method, includes but not limited to what ASTM D2622 and ASTM D4951 measured.Obtain specific conductivity by independent adding cerium oxide particle and washing composition, thus avoided needing to add conventional static inhibitor as
Compound.The verified specific conductivity that is provided by these embodiments was kept 7 days after being in well and being compound to washing composition and cerium oxide particle together at least.The added advantage of embodiment of the present invention is to obtain antistatic effect and need not add unnecessary sulphur in fuel composition.For example, the combination of cerium oxide particle and washing composition/dispersion agent is contributed the sulphur of about 0.135ppm at the most to fuel composition, thereby keeps using the benefit of super low sulfur fuel.
Embodiment
Demonstration hybrid metal system
Following embodiment has further set forth viewpoint of the present invention, but does not limit the present invention.
Embodiment 1.
Embodiment 2.
Fuel stability for the product that improves embodiment 1, demulsifying compound (available from the Tolad 9338 of Baker Petrolite, the blend of the longer chain polyethylene glycols in Fatty Alcohol(C12-C14 and C12-C18) and aromatic solvent, oxyalkylated resol and oxyalkylated ethylene glycol/epoxy polymer adducts) combination with itself and 2.27% weight.The phosphorus content of Tolad 9338 is 23.95 mg/kg.Yet, depend on the required storage time and/or relate to the type of diesel-fuel that have the turbidity of height, this all is unacceptable product concerning nearly all purposes.When filtering, obtain the throw out of per 1 kilogram of 1.39 gram.
Embodiment 3
In order to improve fuel stability and solvability, with the product of embodiment 1 and the demulsifying compound of 2.27% weight (Tolad 2898, have the alkyl phenol resin than the-oxylization of low phosphorus content of 7.85 mg/kg) combination.Improved fuel stability, and reduced (seeing below), but be not for all fuel or all fuel purposes, all to be Utopian with respect to the turbidity as a result of embodiment 2.When filtering, obtain the throw out of per 1 kilogram of additive product, 0.35 gram.
(Tolad 9357 for the another kind of demulsifying compound that embodiment 4. is 0.199 mg/kg with product and 2.27% weight, the phosphorus content of embodiment 1, yuban with 4-(1, the 1-dimethyl ethyl) phenol, propylene oxide and oxyethane in aromatic solvent) combination.This fuel dope combination has excellent transparency, low-down turbidity and unconspicuous throw out (per 1 kilogram of fuel dope combination is 0.15 gram throw out only).This diesel-fuel additive combination that will obtain under the processing rate of 1350ppm combines with diesel-fuel and causes excellent fuel stability, do not precipitate and do not have muddiness.In this final diesel-fuel product, cerium oxide content is 0.37 weight % (5ppm), so phosphorus content is a trace.This final diesel-fuel product is being excellent aspect the burning of cigarette minimizing, fuel economy, fuel stability, solvability and raising.
As what can find out from top embodiment, when
4656 diesel-fuel additive (alkyl nitrate ester selected cetane number improver) and Tolad 9338 demulsifying compounds and Enivrox
TMWhen cerium oxide nanoparticles was mixed, the fuel dope product that obtains produced the throw out of per 1 kilogram of additive, 1.39 grams.When
4656 diesel-fuel additive (alkyl nitrate ester selected cetane number improver) and Tolad 2898 demulsifying compounds and Enivrox
TMWhen cerium oxide nanoparticles was mixed, product produced the throw out of per 1 kilogram of additive, 0.35 gram.When
4656 diesel-fuel additive (alkyl nitrate ester selected cetane number improver) and Tolad 9357 demulsifying compounds and Enivrox
TMDuring mixing, product produces the throw out of per 1 kilogram of additive, 0.15 gram.
Turbidimetry
Significantly, when combination cetane number improver, cerium oxide nanoparticles and phosphorous low demulsifying compound, unexpected improvement is that turbidity reduces." NTU " is the unit of measure that is commonly referred to as " non-arbitrary unit " in industry.
Froth breaking experiment general introduction
In addition, the applicant has carried out the froth breaking test to the fuel dope product of making, have astonishing result that contains alkyl nitrate ester selected cetane number improver and cerium oxide nanoparticles.Minimizing has active influence to foam to observe cerium oxide.Use Envirox separately
TMProduct, the fuel foam attenuation time reduces by half, but when with
When 4656 type products used jointly, the foaming properties improvement had surpassed common
4656 foaming properties.Therefore, when combination cerium oxide nanoparticles and alkyl nitrate ester selected cetane number improver, obtaining unexpected benefit aspect the minimizing of diesel-fuel foam.
Basis reference diesel-fuel has 45 seconds fall time and the foam height of 100mls; Use 250ppm Envirox
TMThe diesel-fuel of handling has 21.2 seconds fall time and the foam height of 100mls; Use 1100ppm
4656 diesel-fuels of handling have 6.9 seconds fall time and the foam height of 80mls; Use 250ppm Envirox
TMAdd 1100ppm
4656 diesel engine of handling have 2.8 seconds fall time and 55mls foam height.Significantly, for the foam minimizing that realizes by combination cerium oxide nanoparticles and alkyl nitrate ester selected cetane number improver in diesel-fuel unexpected excellent the improvement arranged.Therefore, the method that provides a kind of diesel-fuel foam to reduce by the fuel dope combination that oxidation-containing cerium nano particle and alkyl nitrate ester selected cetane improver additive are provided for fuel herein.
By the present invention being incorporated into the remarkable improvement that used Machine Design and method are provided in the vehicles or the equipment.In one embodiment, provide a kind of emission control system that is used for aftertreatment diesel-fuel combustion processes exhaust flow herein, comprising: exhaust passageway is used for by containing the exhaust flow from diesel-fuel incendiary waste by-product; Particulate filter is selected from cyclic regeneration technology diesel particulate filter, diesel particulate filter and catalyzed diesel, is positioned at exhaust passageway and is suitable for contacting with exhaust flow; Wherein fuel has introducing additive combination wherein, and this additive combination oxidation-containing cerium and/or manganese, washing composition, alkyl nitrate ester selected cetane number improver and optional demulsifying compound are thus by making the dispersed maximum running that improves particulate filter of cerium oxide.This has prevented the reunion of cerium oxide particle, otherwise reunion reduces the interaction of cerium oxide and exhaust gas particle.And the dispersion of the cerium oxide particle of raising of the present invention has reduced their reunion, and makes the minimum or elimination of fuel filter possibility of jamming.In addition, also provide a kind of process useful that improves the diesel particulate filter performance: under the situation of not using fuel dope combination described herein, reduce negative impact to filter surfaces.
In some engine design, injector spray orifice right and wrong are columniform, but open outside the combustion chamber along with diameter increases, and purpose is behind each fuel injection injector holes to be kept dry.Find that these designs extremely are easy to coking, fuel flows, the incendiary homogeneity and the coking meeting influences negatively, and impels settling to gather, and the surface of injector holes can not be purged totally because fuel dynamics flows.Therefore, exist protect the needs of injector spray orifice by the exposure that the combustion chamber gas that comprises cerium atom and cerium oxide particle is at present improved.By the present invention, cerium and cerium oxide particle can be used for oxidation and remove carbonaceous sediment around the spray orifice neutralization.Therefore, this paper provides a kind of diesel-fuel additive to be combined in the method for using in the diesel engine with non-cylindrical injector spray orifice, and this diesel-fuel additive combination oxidation-containing cerium, washing composition/dispersion agent, phosphorus are less than the demulsifying compound of 24 mg/kg.In an independent embodiment, the phosphorus in the demulsifying compound is about 8 mg/kg-Yue 24 mg/kg, is the phosphorus of about 0.1 mg/kg-Yue 8 mg/kg In yet another embodiment.
Specific conductivity embodiment
Comparative Examples 1
Measure the specific conductivity of the reference fuel RF93-T-95 diesel-fuel sample that contains 50-500ppm sulphur according to IP 274 (ASTM D2624).Then, in cold environment (under 21 ℃) or thermal environment (under 50 ℃), fuel is carried out weathering test.Use two cold samples.After 7 days, measure specific conductivity again.Directly measure the specific conductivity of the hot sample that from baking oven, takes out.Before measuring specific conductivity, make a cold sample leave standstill at room temperature 1 hour, and another cold sample only vibrate it from refrigeration plant after shifting out.
Comparative Examples 2
Except cerium oxide nanoparticles (Envirox with 250ppm (volume)
TM, median size=12 nanometers) and repeat Comparative Examples 1 outside joining in the diesel-fuel.
Embodiment C 1
Except fuel dope concentrate with 1100ppm (volume)
Outside joining in the diesel-fuel, repeat 4656 (AftonChemical) Comparative Examples 1.
Embodiment C 2
Except before adding the additive concentrate also with the cerium oxide nanoparticles (Envirox of 250ppm (volume)
TM, median size=12 nanometers) and repeat the process of embodiment 1 outside joining in the diesel-fuel.
Embodiment C 3
Except with the conventional static inhibitor of 5ppm (volume) (Baker Petrolite's
3514) rather than the fuel dope concentrate repeat the process of embodiment 1 outside joining in the diesel-fuel.
Embodiment C 4
Except also joining the cerium oxide particle (in embodiment 2) of 250ppm (volume) in the diesel-fuel, repeat the process of embodiment 3.
Embodiment C 5
Except with the another kind of conventional static inhibitor of 5ppm (volume) (Innospec FuelSpecialties's
450) rather than T3514 repeat the process of embodiment 3 outside joining in the diesel-fuel.
Embodiment C 6
Except also joining the cerium oxide particle (in embodiment 2 and 4) of 250ppm (volume) in the diesel-fuel, repeat the process of embodiment 5.
Comparative Examples 3-4
The ultra low sulfur diesel fuel that contains 30ppm sulphur except use replaces repeating the RF93-T-95 diesel-fuel Comparative Examples 1-2.
Embodiment C 7-C12
Use the ultra low sulfur diesel fuel among the Comparative Examples 3-4 to repeat embodiment 1-6.
Reported the result of specific conductivity embodiment in the table 1.
Data presentation the synergistic effect of cerium oxide and washing composition combination to the diesel-fuel specific conductivity.And, to compare with the static inhibitor of routine, cerium oxide particle and washing composition combination have shown higher initial conductivity and comparable or better aging specific conductivity.Therefore, the present embodiment provides the specific conductivity that is beneficial to diesel-fuel and does not need to add special static inhibitor.
According to the consideration of specification sheets and the practice of the disclosure of disclosure herein, other embodiment of this specification sheets is apparent to those skilled in the art.When using in specification sheets and claim, " one " can refer to a kind of or a kind of incessantly.Unless otherwise stated, otherwise all numerals that are expressed as dosis refracta, performance such as molecular weight, per-cent, ratio, reaction conditions etc. of in specification sheets and claims, using be interpreted as under any circumstance all regulating by term " about ".Therefore, unless show on the contrary, the digital parameters of stating in specification sheets and claims all is can be according to the approximation of planning to change by the desired properties that the present invention obtains.At least, rather than attempt to limit the application of the principle that is equivalent to claims scope, each digital parameters all should be regarded as at least considering report significant figure number and by using the common method of rounding up makes up.Although the digital scope and the parameter of the scope statement that the present invention is wide are approximations, the numerical value of stating in the specific embodiment is still as far as possible accurately reported.Yet any numerical value must contain some error that is produced by the standard deviation of finding in their experimental measurements separately.It is exemplary that the meaning only is considered as specification sheets and embodiment, and the real scope and spirit in this aspect are to be shown by following claim.
Claims (35)
1. additive concentrate that is used for the intermediate oil fuel composition, described additive concentrate comprises static inhibitor, described static inhibitor comprises compound dispersion agent and cerium oxide particle.
2. the additive concentrate of claim 1, wherein said fuel comprises diesel-fuel.
3. the additive concentrate of claim 1, wherein said static inhibitor is contributed the sulphur of 0.135ppm at the most for the additive concentrate.
4. the additive concentrate of claim 1, wherein cerium oxide particle comprises nano particle.
5. the additive concentrate of claim 1, wherein said dispersion agent comprises succinimide dispersants.
6. the additive concentrate of claim 7, wherein said succinimide dispersants is formed by tetren.
7. use the additive concentrate of claim 1 under 21 ℃, to provide the conductivity measurements of 500pS/m at least in the middle runnings oil fuel after aging 7 days.
8. the intermediate oil fuel composition that improves of a specific conductivity, described fuel comprises static inhibitor, described static inhibitor comprises compound dispersion agent and cerium oxide particle.
9. the fuel of claim 8, wherein said fuel comprises diesel-fuel.
10. the fuel of claim 8, wherein said static inhibitor is that fuel composition is contributed the sulphur of 0.135ppm at the most.
11. the fuel of claim 8, wherein said fuel had the specific conductivity of 500pS/m at least after under 21 ℃ aging 7 days.
12. the fuel of claim 8, wherein cerium oxide particle comprises nano particle.
13. the fuel of claim 8, wherein said dispersion agent comprises succinimide dispersants.
14. the fuel of claim 13, wherein said succinimide dispersants is formed by tetren.
15. the application of the fuel of claim 8 in combustion unit.
16. method of distributing the intermediate oil fuel composition, comprise adding the step that quantity is enough to provide for described fuel the static inhibitor of specific conductivity benefit in the intermediate oil fuel composition, described static inhibitor comprises compound dispersion agent and cerium oxide particle.
17. being reduced to, the method for claim 16, the specific conductivity that also is included in described fuel composition be lower than the step of distributing described fuel composition before the 50pS/m.
18. the method for claim 17, wherein said allocation step comprise described fuel composition is assigned in the free flowing bulk material container.
19. the method for claim 16 wherein was mixed in described dispersion agent and described cerium oxide particle in the additive concentrate before joining described fuel in advance.
20. the method for claim 16, wherein said fuel comprises diesel-fuel.
21. being fuel composition, the method for claim 16, wherein said static inhibitor contribute the sulphur of 0.135ppm at the most.
22. the method for claim 16, wherein cerium oxide particle comprises nano particle.
23. the method for claim 16, wherein said washing composition comprises the succinimide washing composition.
24. the method for claim 23, wherein said succinimide dispersants is formed by tetren.
25. a reduction be may further comprise the steps by electrostatic discharged catching fire or the method for explosion hazard of causing, and the intermediate oil fuel composition is provided; In described fuel composition, add the combination of dispersion agent and cerium oxide particle to improve the specific conductivity of described fuel composition; Reduce danger electrostatic discharged in the described fuel composition thus.
26. the method for claim 25 also comprises the step of distributing fuel composition.
27. the method for claim 26, wherein said allocation step comprise described fuel composition is assigned in the free flowing bulk material container.
28. the method for claim 26, the specific conductivity of wherein said fuel composition is at least 50pS/m under time of carrying and temperature.
29. the method for claim 25 wherein was mixed in dispersion agent and described cerium oxide particle in the additive concentrate before joining described fuel composition in advance.
30. the method for claim 25, wherein said fuel composition comprises diesel-fuel.
31. the method for claim 25, wherein said intermediate oil fuel does not have the sulfur-bearing conductivity improver basically.
32. the method for claim 25, the wherein compound sulphur that in fuel composition, is added to many 0.135ppm of dispersion agent and cerium oxide particle.
33. the method for claim 25, wherein cerium oxide particle comprises nano particle.
34. the method for claim 25, wherein said dispersion agent comprises succinimide dispersants.
35. the method for claim 34, wherein said succinimide dispersants is formed by tetren.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US11/811637 | 2007-06-08 | ||
| US11/811,637 US20080098644A1 (en) | 2006-09-19 | 2007-06-08 | Conductivity improving combination of cerium oxide and detergents for diesel fuels |
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|---|---|
| CN101319154A true CN101319154A (en) | 2008-12-10 |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101892101A (en) * | 2010-08-09 | 2010-11-24 | 北京斯伯乐科技发展有限公司 | Ashless high-efficiency oil antistatic agent and using method thereof |
| CN103103000A (en) * | 2013-03-06 | 2013-05-15 | 济南恒致达新能源科技有限公司 | Multifunctional oil-saving and emission-reducing compound diesel fuel additive composition |
| CN106147891A (en) * | 2015-05-14 | 2016-11-23 | 英菲诺姆国际有限公司 | To compositions of additives and the improvement of fuel oil |
-
2007
- 2007-09-18 CN CNA2007101528749A patent/CN101319154A/en active Pending
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101892101A (en) * | 2010-08-09 | 2010-11-24 | 北京斯伯乐科技发展有限公司 | Ashless high-efficiency oil antistatic agent and using method thereof |
| CN101892101B (en) * | 2010-08-09 | 2013-01-30 | 北京斯伯乐科技发展有限公司 | Ashless high-efficiency oil antistatic agent and using method thereof |
| CN103103000A (en) * | 2013-03-06 | 2013-05-15 | 济南恒致达新能源科技有限公司 | Multifunctional oil-saving and emission-reducing compound diesel fuel additive composition |
| CN106147891A (en) * | 2015-05-14 | 2016-11-23 | 英菲诺姆国际有限公司 | To compositions of additives and the improvement of fuel oil |
| CN106147891B (en) * | 2015-05-14 | 2019-06-28 | 英菲诺姆国际有限公司 | Improvement to compositions of additives and fuel oil |
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