Classifications

• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
  • C10L1/00—Liquid carbonaceous fuels
  • C10L1/10—Liquid carbonaceous fuels containing additives
  • C10L1/14—Organic compounds
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
  • C10L10/00—Use of additives to fuels or fires for particular purposes
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
  • C10L10/00—Use of additives to fuels or fires for particular purposes
  • C10L10/02—Use of additives to fuels or fires for particular purposes for reducing smoke development
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
  • C10L10/00—Use of additives to fuels or fires for particular purposes
  • C10L10/04—Use of additives to fuels or fires for particular purposes for minimising corrosion or incrustation
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
  • C10L10/00—Use of additives to fuels or fires for particular purposes
  • C10L10/06—Use of additives to fuels or fires for particular purposes for facilitating soot removal
• • 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
  • C10L1/26—Organic compounds containing phosphorus
• • 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
  • C10L1/26—Organic compounds containing phosphorus
  • C10L1/2633—Organic compounds containing phosphorus phosphorus bond to oxygen (no P. C. bond)
  • C10L1/2641—Organic compounds containing phosphorus phosphorus bond to oxygen (no P. C. bond) oxygen bonds only
• • 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)
• • 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
  • C10L2230/00—Function and purpose of a components of a fuel or the composition as a whole
  • C10L2230/22—Function and purpose of a components of a fuel or the composition as a whole for improving fuel economy or fuel efficiency
• • 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
  • C10L2250/00—Structural features of fuel components or fuel compositions, either in solid, liquid or gaseous state

Definitions

• the present invention relates to the use of a composition containing ferrocene and lecithin as a fuel additive to improve combustion promotion.
• ferrocene and derivative(s) thereof are used as an additive for various liquid fuels.
• ferrocene, derivative(s) thereof and a improvement combustion method of a liquid hydrocarbon in the presence of a fuel additive composition consisting of an aromatic solvent, an aliphatic solvent and/or a petroleum solvent which are liquid organic carriers capable of dissolving the ferrocene and derivative(s) thereof are described in JP02-132 188A .
• a method of conditioning of diesel engines is described in US Patent 4389220 specification. In accordance with the method, a deposit containing carbon in the combustion chamber is removed, and the fuel consumption per distance traveled is reduced by about 5%, by adding 20-30ppm of ferrocene to the fuel.
• JP Patent 3599337 a method of reducing carbonaceous deposition on the engine and ancillary equipment thereof is proposed in JP Patent 3599337 specification.
• 1-100ppm of ferrocene and derivative(s) thereof, as additives for fuel oil consisting of a heavy residual oil for an internal combustion, are added to a fuel directly, without blending other additives.
• ferrocene and ferrocene derivative(s) used for these inventions have a drawback of very low solubility in an aromatic solvent, an aliphatic solvent and a petroleum solvent.
• ferrocene is in the solid state.
• a large quantity of agitation power and long time which depend on the size of the solid, are needed.
• solid ferrocene doesn't dissolve easily either. The trouble occurs in the internal combustion engine when solid ferrocene isn't dissolved beforehand before it adds to the fuel. Therefore, under the present situation, the solid ferrocene is added to a fuel after it is dissolved in a solvent in a solution tank with an agitator.
• the present invention is made in view of the aforementioned problems of the conventional technology and has an object to provide a fuel additive containing ferrocene, which can easily and stably be dissolved in a fuel and improves the combustion.
• the present inventors found the object to be accomplished by using ferrocene in combination with lecithin.
• composition according to the present invention is characterized by containing ferrocene and lecithin which is used as fuel additive for improving combustion.
• the solid fuel additive composition used according to the present invention for improving the combustion is characterized by containing 80 to 99 % by mass of ferrocene and 1 to 20 % by mass of lecithin.
• the particulate fuel additivecomposition used according to the present invention is characterized by containing 78 to 99 % by mass of ferrocene 0.9 to 20 % by mass of lecithin and 0.1 to 2 % by mass of water.
• liquid fuel additive composition used according to the present invention for improving the combustion is characterized by containing mineral oil containing ferrocene and lecithin dissolved therein, and having the ferrocene content of 2 to 5 % by mass and the lecithin content of 5 to 50 % by mass.
• the fuel additive composition used according to the present for improving the combustion invention is characterized by being used by being added into a fuel so as to make the concentration of the ferrocene and the lecithin in ranges of 1 to 50 ppm, and 0.01 to 500 ppm, respectively.
• composition used as a fuel additive according to this invention for improving the combustion will be explained in detail.
• “%” means “mass percentage” unless otherwise specified.
• the composition used as a fuel additive according to this invention for improving the combustion contains ferrocene and lecithin.
• These fuel additives can be in the solid state, especially in the particle state, and in the liquid state.
• ferrocene is called bis(cyclopentadienyl)iron, and is also called dicyclopentadienyl iron.
• ferrocene may be a solid such as a fine powder, a coarse particle, a pellet and the like, and may be a liquid.
• the form of ferrocene can be suitably chosen depending on the form of a fuel additive of the present invention. It is explained in detail later.
• a fuel additive used in the present invention can have a combustion promotion effect, a soot reduction effect, a NOx reduction effect and the like, by containing ferrocene.
• a combustion promotion effect a soot reduction effect, a NOx reduction effect and the like
• ferrocene a cleaning effect of the combustion promotion that controls the formation of deposit on a valve, a piston ring, and a combustion chamber is observed. Since the deposit reduces engine output and increases attrition of parts by adhering, controlling formation of the deposit achieves stable driving of a diesel engine.
• several percent reduction of fuel consumption can be realized by preventing superfluous air at the time of combustion, by the reforming combustion such as combustion promotion, soot reduction, NOx reduction and the like.
• Lecithin is an animal and plant phospholipid of which the principal ingredients are a glycerophospholipid and a sphingophospholipid. It is obtained by the purification process of various kinds of vegetable oil such as soybean oil, rapeseed oil, rice-bran oil, palm oil, sunflower oil, cocoanut oil, cottonseed oil, corn oil, peanut oil, linseed oil, safflower oil, olive oil and the like. Usually, a vegetable oil is included 1 to 50%. Depending on the contained amount of the vegetable oil and the ratio between saturation acid and unsaturated acid in the vegetable oil, lecithin exists in the liquid form or in the solid form at normal temperature. Moreover, in recent years, a powder lecithin is manufactured from a liquid lecithin by carrying out oil extraction and vacuum drying.
• lecithin may be a liquid, and may be a solid such as a fine powder and the like.
• the form of lecithin can be suitably chosen depending on the form of a fuel additive of the present invention. It is explained in detail later.
• a fuel additive used in the present invention can be in the solid state, in the particle state, and in the liquid state.
• a solid fuel additive used in the present invention preferably contains 80 to 99% of ferrocene and 1 to 20% of lecithin. If the content of the lecithin is less than 1%, the ferrocene may not dissolve in the fuel easily. If the content of the lecithin is 20%, the ferrocene solubility enhancement effect may be obtained completely.
• the form of ferrocene is not especially limited as long as it is solid at normal temperature, mention may be made, for example, of a solid form such as a fine powder, a coarse particle, a pellet and the like.
• lecithin is preferably in the powder form at normal temperature, more preferably a fine powder of 1 mm or less in particle diameter. It is because the mixture with Ferrocene may be made more uniform.
• a particulate fuel additive used in the present invention is one aspect of the above-mentioned solid fuel additive, and is granulated from fine powder ferrocene compound into the shape of a coarse particle.
• the particle diameter it is preferable to be 0.5 mm to 15 mm, more preferably 1 mm to 10 mm. When the particle diameter is less than 0.5 mm, the handling workability may be inferior due to powder dust. When the particle diameter is more than 15 mm, the solubility may decrease due to decreased deflocculability.
• a particulate fuel additive preferably contains 78 to 99% of ferrocene, 0.9 to 20% of lecithin and 0.1 to 2 % of water.
• the ferrocenes may not dissolve in the fuel easily. If the content of the lecithin is 20%, the ferrocene solubility enhancement effect may be obtained completely.
• Ferrocene are preferably in the powder form at normal temperature, more preferably a fine powder of 2 mm or less in particle diameter.
• lecithin is also preferably in the powder form at normal temperature, more preferably a fine powder of 1 mm or less in particle diameter. It is for the convenience of granulation process.
• a powder lecithin used in this invention has high hygroscopicity, and obtains suitable tackiness for a granulation by mixed with small amount of water.
• the content of the water is less than 0.1%, the sufficient tackiness may not be obtained, and when the content of the water is more than 2%, the above-mentioned powder ferrocene and the above-mentioned powder lecithin may be agglomerated due to high water content.
• a liquid fuel additive of the present invention contains mineral oil containing ferrocene and lecithin dissolved therein, and preferably the content of the ferrocene is 2 to 5 % and the content of the lecithin is 5 to 50 %. If the content of the lecithin is less than 5%, the ferrocenes may not dissolve in the mineral oil easily. If the content of the lecithin is 50%, the effect of enhancing solubility of ferrocenes in mineral oil may be obtained completely.
• the ferrocene may be a solid such as a fine powder, a coarse particle, a pellet and the like, or may be a liquid, preferably a liquid or a fine powder from the viewpoint of shape that dissolves easily in mineral oil.
• the lecithin may also be a liquid, or a solid such as a fine powder and the like, preferably a liquid or a fine powder, because of the shape thereof that dissolves easily in mineral oil.
• mineral oil includes hydrocarbon fuel oil , gas oil, kerosene and the like.
• grade A heavy oil, grade B heavy oil, gas oil, kerosene and the like can be preferably used, and grade A heavy oil can be more preferably used.
• Lecithin in the present invention mainly provides the effect as follows.
• fuel includes fuels used as a fuel for diesel engines, oil incinerators, boiler devices and the like, such as grade A heavy oil, light oil such as kerosene, gas oil and the like, heavy oil, heavy residue oil, lubricating oil, waste oil and mixed oil thereof, and also fuel emulsion thereof, and solid fuel such as coal and the like, but are not limited thereto, as long as the fuel is not in gaseous form.
• Lecithin has an oleophilic portion and a hydrophilic portion, and is known to act as a surfactant agent. However, in the present invention, it is considered that lecithin enhances the solubility due to the action of an oleophilic portion. That is, it is considered as follows. When ferrocene and lecithin are dissolved in a fuel, one part of oleophilic portions of the lecithin promptly adsorb to the surface of the ferrocene, and another oleophilic portions of the lecithin enhance lipophilic property on the surface of the ferrocene, therefore, lecithin contribute to the solubility enhancement of ferrocene in a fuel. These actions are not seen in any other surfactant agents such as nonionic surfactant and the like, and are peculiar to lecithin.
• Lecithin itself acts as a fuel additive, and contributes to long-term stable operation of the combustion facility including a diesel engine.
• Sludge is an insoluble matter, which exists in a fuel oil, especially in a heavy oil, and causes clogging of a strainer and incomplete combustion since it is easy to precipitate.
• a generation of the sludge arises from change into a hydrocarbon polymer having few hydrogen atoms by oxidation, polymerization and condensation of hydrocarbon that remains in a oil residue in a tank, because of heat-treatment, catalytic cracking, pyrolysis and the like during a purification process of crude oil.
• hydrocarbon malthene, asphaltene, carbine, carboid and carbon.
• These polymers initially exist in a heavy oil as a macromolecular colloid. It is considered that the colloid has a hydrocarbon such as carbine, carboid and the like as a core with an extremely high C/H ratio, surrounded by some asphaltenes, and covered sequentially with hydrocarbon polymer with a low C/H ratio.
• An asphaltic substance that exists in a heavy oil as such a colloidal particle will not be precipitated and cause the problem of clogging of a strainer, incomplete combustion and the like, as long as it is floating dispersedly as stable colloid.
• this colloidal particle has polarity and adsorptivity property. Therefore, if equilibrium condition is disrupted by heating, adding an oil of a different kind, prolonged storage and the like, the colloidal particles agglutinate together one after another, and get into an aggregate of big particles (micelle colloid), and form sludge by precipitating.
• Lecithin infiltrates and absorbs to binding portion and/or association of sludge such as carbon, asphaltene and the like, and has a mincing action of sludge by dispersion force by acting as a surfactant agent. Lecithin also has the effect of preventing separation and precipitation of sludge, by preventing mixing of different-type fuels, association of the colloidal particles by heating and the like, by this action.
• Binder action at the time of granulation to prepare a particulate fuel additive is iii) Binder action at the time of granulation to prepare a particulate fuel additive.
• lecithin when a particulate fuel additive is granulated, lecithin obtains suitable tackiness for a granulation by mixed with small amount of water, and bears a role of a binder.
• Lecithin contained in particulate fuel additives has deflocculation action to make particles easy to crush when the additive is fed into a fuel.
• the crushed additive comes to dissolve very easily by solubility enhancement effect of lecithin.
• Ferrocene has a very low solubility in mineral oil, and are soluble only up to about 2.5% in concentration. However, by adding the prescribed amount of lecithin, it is possible for ferrocene to be dissolved up to 5% in concentration, and the stability of the solution is good in a broad temperature region.
• the fuel additive according to the present invention for various fuels used for diesel engines, oil incinerators, boiler devices and the like, which are used in a marine vessels, power generating facilities and the like, is added into the fuels so as to make the concentration of ferrocene and lecithin in ranges of 1 to 50 ppm, and 0.01 to 500 ppm, respectively. More specifically, as for usual concentration of ferrocene, it is preferred that the fuel additive is added sequentially into the fuels in order that the fuels in oil incinerators and boiler devices have ferrocene concentration of 1-10 ppm and the fuels in diesel engine have ferrocene concentration of 10-50 ppm.
• soot reduction, NOx reduction and the like several fold to dozens of the continuous additive amount can be temporarily added while a short time, based on the condition of a combustion engine.
• the above-mentioned lecithin has advantageous concentration to dissolve easily and stably ferrocene in a fuel oil and in fuel additive itself, and to disperse sludge further, in a heavy fuel oil especially.
• Liquid fuel additive (Example 5 - 7 and Comparative example 2)
• the fuel additives were prepared by compositions shown in Table 3, and the rate of solution until ferrocene is completely dissolved in grade A heavy oil was evaluated by measuring the number of seconds. Stability of the obtained solution after still standing for one week at room temperature was evaluated. The test was done on a 200 g scale. The results are shown in Table 3.
• Example Comparative Example 5 6 7 2 additive composition [%] Ferrocene 3.5 5.0 4.0 2.5 Lecithin (Liquid) 5 20 50 --- Water --- --- --- Grade A Heavy Oil 92 75 46 97.5 Total 100 100 100 100 solubility rate 180 370 290 580 dissolved concentration 4.8 3.5 4.1 2.5 stability test very good good good passed Lecithin(Solid) means a powdered lecithin in the solid state, lecithin (liquid) means a lecithin in the liquid state. Stability test: "very good” mesns complete dissolution, "good” mesns almost dissolution, "passed” mesns a little insoluble matter was observed, “no good” mesns too much insoluble matter was observed.
• Example 1 4 The rate of solution of solid fuel additives of the present invention (Example 1 4) until ferrocene concentration reaches 3% is very fast as compared with comparative example 1.
• the concentration of a stable solution of comparative example 1 is 3% but with many insoluble matters, while the concentration of a stable solution of example 1-4 is allowed to be 3.5 to 5.0%.
• the evaluations of stability after storing for one week of Example 1 - 4 are "very good" or "good”. Thus, it was confirmed that a solid fuel additive of this invention was very excellent in all aspects of solution rate of ferrocene, dissolved concentration and stability evaluation.
• a solid fuel additive of this invention (Examples 1-4) and a liquid fuel additive of this invention (Examples 5-7) have a very excellent effect of sludge dispersion as compared with comparative example 1, 2 and additive-free.
• Comparative examples 1 and 2 which do not contain lecithin, had no effect at all and were the same as additive-free grade C heavy oil.
• An effect of lecithin was the result of being proportional to an additive amount in general.
• the system examination was done, namely, in a solution tank with an agitator, 9.0Kg of solid fuel additive was dissolved in 360 liters of grade A heavy oil, and was added of 1/1000 into the fuel (grade C heavy oil) line from this solution tank with injection pump. (The additive amount of fuel additive was 25ppm.)
• Example 3 or comparative example 1 A solid fuel additive of Example 3 or comparative example 1 was added by the above-mentioned method over four months alternately per one month (30 days) (one month x 2 times for each solid fuel additive). Then, a fuel consumption and condition of dirt of a heat exchanger by visual observation was compared. Next, water-wash was performed and dirt removal performance was compared.
• Example 3 Comparative Example 1 fuel consumption first 2.597 KL 2,660 KL second 2,566 KL 2,647 KL dirt of a heat exchange mechanism first Very little deposit adhered to the surface, A deposit almost adhered to the entire surface thinly. second same as above same as above removability of dirt of a heat exchange mechanism by flushing with water first removed by easy rinsing with water A lot of time of washing with water was needed until removed. second same as above same as above General Properties of a fuel oil (Grade C heavy oil) Density(15°C) : 0. 984 Viscosity(50°C) :401 cst Sulfer content(%);3. 61 Carbon Residueworth(%) : 13. 4 Asphaltene(%):8, 98
• the fuel additive in which the ferrocene contained can be dissolved easily and stably can be provided.

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• 2008
  • 2008-01-16 JP JP2008007269A patent/JP4131748B1/ja active Active
  • 2008-02-21 US US12/305,317 patent/US20100050503A1/en not_active Abandoned
  • 2008-02-21 EP EP08711738A patent/EP2107103B1/en active Active
  • 2008-02-21 ES ES08711738T patent/ES2383623T3/es active Active
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• 2009
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