Classifications

• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M109/00—Lubricating compositions characterised by the base-material being a compound of unknown or incompletely defined constitution
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M107/00—Lubricating compositions characterised by the base-material being a macromolecular compound
  • C10M107/02—Hydrocarbon polymers; Hydrocarbon polymers modified by oxidation
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M143/00—Lubricating compositions characterised by the additive being a macromolecular hydrocarbon or such hydrocarbon modified by oxidation
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M169/00—Lubricating compositions characterised by containing as components a mixture of at least two types of ingredient selected from base-materials, thickeners or additives, covered by the preceding groups, each of these compounds being essential
  • C10M169/04—Mixtures of base-materials and additives
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M2203/00—Organic non-macromolecular hydrocarbon compounds and hydrocarbon fractions as ingredients in lubricant compositions
  • C10M2203/10—Petroleum or coal fractions, e.g. tars, solvents, bitumen
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M2203/00—Organic non-macromolecular hydrocarbon compounds and hydrocarbon fractions as ingredients in lubricant compositions
  • C10M2203/10—Petroleum or coal fractions, e.g. tars, solvents, bitumen
  • C10M2203/104—Aromatic fractions
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M2205/00—Organic macromolecular hydrocarbon compounds or fractions, whether or not modified by oxidation as ingredients in lubricant compositions
  • C10M2205/02—Organic macromolecular hydrocarbon compounds or fractions, whether or not modified by oxidation as ingredients in lubricant compositions containing acyclic monomers
  • C10M2205/026—Butene
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M2205/00—Organic macromolecular hydrocarbon compounds or fractions, whether or not modified by oxidation as ingredients in lubricant compositions
  • C10M2205/17—Fisher Tropsch reaction products
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M2205/00—Organic macromolecular hydrocarbon compounds or fractions, whether or not modified by oxidation as ingredients in lubricant compositions
  • C10M2205/17—Fisher Tropsch reaction products
  • C10M2205/173—Fisher Tropsch reaction products used as base material
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
  • C10M2207/00—Organic non-macromolecular hydrocarbon compounds containing hydrogen, carbon and oxygen as ingredients in lubricant compositions
  • C10M2207/02—Hydroxy compounds
  • C10M2207/023—Hydroxy compounds having hydroxy groups bound to carbon atoms of six-membered aromatic rings
  • C10M2207/026—Hydroxy compounds having hydroxy groups bound to carbon atoms of six-membered aromatic rings with tertiary alkyl groups
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
  • C10N2030/00—Specified physical or chemical properties which is improved by the additive characterising the lubricating composition, e.g. multifunctional additives
  • C10N2030/02—Pour-point; Viscosity index
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
  • C10N2030/00—Specified physical or chemical properties which is improved by the additive characterising the lubricating composition, e.g. multifunctional additives
  • C10N2030/04—Detergent property or dispersant property
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
  • C10N2030/00—Specified physical or chemical properties which is improved by the additive characterising the lubricating composition, e.g. multifunctional additives
  • C10N2030/06—Oiliness; Film-strength; Anti-wear; Resistance to extreme pressure
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
  • C10N2030/00—Specified physical or chemical properties which is improved by the additive characterising the lubricating composition, e.g. multifunctional additives
  • C10N2030/50—Emission or smoke controlling properties
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
  • C10N2040/00—Specified use or application for which the lubricating composition is intended
  • C10N2040/25—Internal-combustion engines
  • C10N2040/255—Gasoline engines
  • C10N2040/26—Two-strokes or two-cycle engines

Definitions

• the present invention relates to the use of a lubricating oil composition comprising a Fischer-Tropsch derived base oil for reducing exhaust port blocking of a two-stroke engine and to a two-stroke lubricating engine oil composition having reduced exhaust port blocking.
• Two-stroke gasoline engines are used in motorcycles as well as in garden and recreational equipment such as lawn mowers, chain saws, string trimmers, mopeds, snow ⁇ mobiles, outboard marine motors and the like.
• Slow speed two-stroke diesel engines are used for marine propulsion in very large ships.
• crankcase To operate a two-stroke gasoline engine the crankcase holds a mixture of two-stroke gasoline
• Conventional two-stroke gasoline engine lubricants are typically formulated with a mineral oil base oil or synthetic base oil and a low-viscosity, low-boiling hydrocarbon solvent to enhance the miscibility of the lubricant with the gasoline.
• Some two-stroke engine oils have used ester base oils with no low boiling solvent to reduce flammability and minimize smoky emissions. However these lubricants often suffer from poor oxidation stability.
• Other two- stroke engine oils have used polyalphaolefin base oils having improved low temperature properties. Both PAOs and ester base oils suffer from the disadvantage of being limited in supply and very expensive.
• a variety of performance additives can be added to improve the overall performance of the lubricant.
• a two-stroke engine oil should meet the requirements set by standards setting organizations, including Japanese Automobile Standard JASO M345 2003 and International Standard ISO 1373832000(E).
• smoke-reducing additives are often added to the lubricant.
• smoke-reducing additives include those that contain metals, but these tend to be undesirable from an environmental viewpoint.
• Other examples include synthetic basestocks, but these tend to be expensive.
• Polybutenes and polyisobutylenes are also commonly added for reducing smoke and as anti-scuffing agents. It is taught in WO2007/050352 that
• polyisobutylenes contribute to exhaust port deposits and clogging .
• Fischer-Tropsch derived base oil as a base oil in a two- stroke engine lubricating oil composition, an improved two-stroke engine lubricating oil composition is provided which exhibits, in particular, a reduction in exhaust port blocking.
• a lubricating oil composition comprising at least one Fischer-Tropsch derived base oil for reducing exhaust port blocking of a 2-stroke engine.
• a 2-stroke lubricating engine oil composition comprising (i) at least one Fischer-Tropsch derived base oil having a kinematic viscosity at 100°C in the range of from 2 to 30 mm 2 /s and (ii) 5 wt% or greater of a hydrocarbon solvent; wherein the lubricating engine oil composition has a Blocking Index of greater than 130 as measured by the JASO M343-92 Exhaust System Blocking Test Method.
• a 2-stroke lubricating engine oil composition comprising (i) a first Fischer-Tropsch derived base oil having a kinematic viscosity at 100°C in the range of from 2 mm 2 /s to 10 mm 2 /s and (ii) a second Fischer-Tropsch derived base oil having kinematic
• the weight ratio of the first Fischer- Tropsch base oil to the second Fischer-Tropsch base oil is in the range of from 10:1 to 1:5, and wherein the lubricating engine oil composition has a Blocking Index of greater than 130 as measured by the JASO M343-92
• Fischer-Tropsch derived base oil preferably heavy
• lubricating oil compositions herein provides reduced exhaust port blocking.
• Fischer-Tropsch derived base oil allows replacement of polyisobutylenes on a viscometric basis.
• the 2-stroke lubricating oil compositions according to the present invention also provide reduced engine wear, increased lubricity, reduced pollution, an improved smoke index, good low-temperature performance,
• the 2-stroke engine oil of the present invention also meets the requirements of Japanese Automobile
• the 2-stroke lubricating oil composition for use herein comprises at least one Fischer-Tropsch derived base oil.
• Fischer-Tropsch derived base oils are known in the art.
• Fischer-Tropsch derived is meant that a base oil is, or is derived from, a synthesis product of a Fischer-Tropsch process.
• a Fischer-Tropsch derived base oil may also be referred to as a GTL (Gas-To- Liquids) base oil.
• GTL Gas-To- Liquids
• Suitable Fischer-Tropsch derived base oils that may be conveniently used as the base oil in the lubricating composition are those as for example
• the Fischer-Tropsch derived base oil preferably has a kinematic viscosity at 100°C in the range of from 2 mm 2 /s to 30 mm 2 /s.
• the total amount of Fischer-Tropsch derived base oil in the lubricating oil composition is preferably in the range of from 5 wt% to 99 wt ⁇ 6 , more preferably from 10 wt% to 99 wt%.
• Tropsch derived base oil having a kinematic viscosity at 100°C in the range of from 2 mm 2 /s to 10 mm 2 /s,
• the light Fischer-Tropsch derived base oil is present at a level of from 5 wt% to 60 wt%, preferably at a level of from 20 wt% to about 60 wt%.
• the lubricating oil composition comprises a heavy Fischer- Tropsch derived base oil having a kinematic viscosity at 100°C in the range of from 12 mm 2 /s to 30 mm 2 /s,
• the heavy Fischer-Tropsch derived base oil is preferably present at a level of from 5 wt% to about 60 wt%, preferably from 10 wt% to 50 wt%.
• Fischer-Tropsch derived base oil having a kinematic viscosity at 100°C in the range of from 12 mm 2 /s to 30 mm 2 /s, preferably in the range of from 18 mm 2 /s to 22 mm 2 /s, and less than 2 wt% of a light Fischer-Tropsch base oil having a kinematic viscosity at 100°C in the range of from 2 mm 2 /s to 10 mm 2 /s.
• a kinematic viscosity at 100°C in the range of from 12 mm 2 /s to 30 mm 2 /s, preferably in the range of from 18 mm 2 /s to 22 mm 2 /s, and less than 2 wt% of a light Fischer-Tropsch base oil having a kinematic viscosity at 100°C in the range of from 2 mm 2 /s to 10 mm 2 /s.
• the lubricating oil composition is preferably free of light Fischer-Tropsch derived base oil having a kinematic viscosity at 100°C in the range of 2 mm 2 /s to 20 mm 2 /s.
• the lubricating oil composition comprises a mixture of a first Fischer-Tropsch oil which is a light Fischer
• Tropsch base oil having a kinematic viscosity at 100°C in the range of from 2 mm 2 /s to 10 mm 2 /s, preferably in the range of from 2 mm 2 /s to 4 mm 2 /s
• a second Fischer- Tropsch base oil which is a heavy Fischer-Tropsch base oil having a kinematic viscosity at 100°C in the range of from 12 mm 2 /s to 30 mm 2 /s, preferably in the range of from 18 mm 2 /s to 22 mm 2 /s.
• the weight ratio of the first Fischer- Tropsch derived base oil and the second Fischer-Tropsch derived base oil is in the range of from 10:1 to 1:5, more preferably in the range of from 1.98:1 to 0.01:1.
• the lubricating composition herein may comprise one or more additional base oils.
• additional base oil s
• various conventional mineral oils, synthetic oils as well as naturally derived esters such as vegetable oils may be conveniently used.
• the additional base oil may conveniently comprise mixtures of one or more mineral oils and/or one or more synthetic oils; thus, the term “base oil” may refer to a mixture containing more than one base oil or base stock.
• Mineral oils include liquid petroleum oils and solvent- treated or acid-treated mineral lubricating oil of the paraffinic, naphthenic, or mixed paraffinic/naphthenic type which may be further refined by hydrofinishing processes and/or dewaxing.
• Suitable base oils for use in the lubricating oil compositions herein are Group I-III mineral base oils, Group IV poly-alpha olefins (PAOs) , and Group V base oils.
• Group I lubricating oil base oils according to the definitions of American Petroleum
• API API for categories I-V. These API categories are defined in API Publication 1509, 16th Edition,
• Synthetic oils include hydrocarbon oils such as olefin oligomers (including polyalphaolefin base oils; PAOs) , dibasic acid esters, polyol esters, polyalkylene glycols (PAGs) , alkyl naphthalenes and dewaxed waxy isomerates.
• API Group III hydrocarbon base oils sold by the Shell Group under the designation "Shell XHVI” (trade mark) may be conveniently used.
• PAOs Poly-alpha olefin base oils
• lubricating compositions may be derived from linear C2 to C32, preferably C6 to Ci6, alpha olefins.
• Particularly preferred feedstocks for said poly-alpha olefins are 1- octene, 1-decene, 1-dodecene and 1-tetradecene .
• the total amount of base oil incorporated in the lubricating composition is preferably present in an amount in the range of from 60 to 99 wt.%, more preferably in an amount in the range of from 65 to 98 wt . % and most preferably in an amount in the range of from 70 to 95 wt.%, with respect to the total weight of the lubricating composition.
• the finished lubricating composition has a kinematic viscosity in the range of from 2 to 30 mm 2 /s at 100 °C, more preferably in the range of from 3 to 20 mm 2 /s, most preferably in the range of from 4 to 15 mm 2 /s .
• the lubricating oil composition Preferably, the lubricating oil composition
• a volatile hydrocarbon solvent comprises 5 wt% or greater of a volatile hydrocarbon solvent.
• the inclusion of such a solvent is for the purpose of improving the miscibility and/or solubility of base oil and additives with gasoline or other fuel.
• the volatile hydrocarbon solvent is present in the composition at a level in the range of 5 to 40 wt%, preferably in the range of 10 wt% to 30 wt%, more preferably in the range of from 20 wt% to 30 wt%, by weight of the total composition.
• Suitable volatile hydrocarbon solvents include kerosene, Exxsol D80 commercially from Exxon Mobil Chemical Company, Shellsol D70 commercially
• the smoke-suppression agent is an olefinically unsaturated polymer selected from the group consisting of polybutene, polyisobutylene or a mixture of polybutene and polyisobutylene, which has a number average molecular weight of 400 to 2200 and a terminal olefin content of at least 60 mol%, based on the total number of double bonds in the polymer.
• olefinically unsaturated polymer selected from the group consisting of polybutene, polyisobutylene or a mixture of polybutene and polyisobutylene, which has a number average molecular weight of 400 to 2200 and a terminal olefin content of at least 60 mol%, based on the total number of double bonds in the polymer.
• a smoke-suppression agent is that commercially available from BASF Corporation under the tradename Glissopal (RTM) 1000, an approximately 1000
• Dalton poly-isobutylene examples would be poly- butylenes of similar molecular weight supplied by Ineos Oligomers under the trade name Indopol.
• the smoke-suppression agent is preferably present in the composition at a level in the range of from 5% to
• One or more detergent/dispersant additive packages may be included in the lubricating oil composition of the present invention, preferably in an amount of from 1 to
• Ashless, low-ash or ash- containing additives may be used for this purpose.
• Suitable ashless additives include polyamide, alkenylsuccinimides , boric acid-modified
• additives include alkaline earth metal (e.g. magnesium, calcium, barium) , salicylate, sulfonate, phosphonates or phenates or combinations of any two or more such
• detergent/dispersant additive packages include, for example,
• the lubricating composition may further comprise additional additives such as anti-wear additives,
• lubricity additives extreme pressure agents, anti ⁇ oxidants, friction modifiers, viscosity index improvers, pour point depressants, rust or corrosion inhibitors, defoaming agents and seal fix or seal compatibility agents .
• the above-described additives may be present at a level in the range of from 0.005% to 15%, preferably from 0.005% to 6%, by weight of the lubricating oil
• crankcase holds a mixture of two-stroke gasoline
• the recommended mix ratio of two- stroke gasoline engine lubricant and fuel are specified by the engine manufacturer.
• the fuels useful in two- stroke gasoline engines are well known to those skilled in the art and usually contain a major portion of a normally liquid fuel such as a hydrocarbonaceous
• gasoline as defined by ASTM D439-89.
• fuels can also contain non-hydrocarbonaceous materials such as alcohols, ethers, organo nitro compounds and the like.
• suitable fuels include, but are not necessarily limited to methanol, ethanol, diethyl ether, methylethyl ether, nitro methane and liquid fuels derived from vegetable and mineral sources such as corn, switch grass, alpha shale and coal. Examples of such fuel mixtures are
• the fuel is preferably lead-free gasoline.
• Two-stroke gasoline engine lubricants are typically used in admixture with fuels in amounts of about 20 to 250 parts by weight of fuel per 1 part by weight of lubricating oil, preferably in the range from 30 to 100 parts by weight of fuel per 1 part by weight of
• lubricating oil compositions of the present invention provide an improved benefit in terms of reduced exhaust port blocking. Such a benefit can be measured by the standard test method JASO 343-92.
• lubricating oil compositions of the present invention have a Blocking Index of greater than 130, preferably greater than 140, as measured by JASO 343-92.
• the lubricating compositions may be conveniently prepared by admixing the additives that are usually present in lubricating compositions, for example as herein before described, with mineral and/or synthetic base oil.
• formulations were prepared by mixing the additives with the base oils according to conventional preparation methods. To determine the effect of each composition on exhaust system port blocking the Blocking Index for each example was measured using the Exhaust System Blocking test method JASO M343-92.
• two-stroke motorcycle oils were prepared having the formulations set out in Table 2 below.
• the formulations were prepared by mixing the additives with the base oils according to conventional preparation methods.
• Various measurements were made on each of the engine lubricants using the test methods detailed in Table 2. The results of these tests are set out in Table 2.
• 2-stroke performance additive package containing aminic dispersant, antioxidants (mixed hindered phenols and aminic antioxidants) , over-based detergents from the range calcium phenates and calcium salicylates
• Fischer-Tropsch base stock having a kinematic viscosity at 100°C of 19 cSt prepared according to the method of US-A-7354508.
• Fischer-Tropsch base stock having a kinematic viscosity at 100°C of 3 cSt prepared according to the method of US-A-7354508.
• 2-stroke performance additive package containing aminic dispersant, antioxidants (mixed hindered phenols and aminic antioxidants) , over-based detergents from the range calcium phenates and calcium salicylates
• Example 1 the major change in the formulation compared to Comparative Example A was to reduce PB and replace with a heavy residual GTL base oil.
• a minor modification was made to the API Gp I high viscosity index (HVI) base stock to maintain iso- viscometrics .
• HVI high viscosity index
• Tropsch base oil GTL-3 together with heavy Fischer- Tropsch base oil GTL-19, gives an exceptional improvement in port blocking performance compared to the standard (API Gp I) mineral oil based formulation under iso- viscous conditions.
• API Gp I mineral oil based formulation under iso- viscous conditions.
• Examples 2 to 4 are all 2 stroke oil formulations containing no PB, and yet suitable port blocking behaviour is obtained.

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• Chemical & Material Sciences (AREA)
• Chemical Kinetics & Catalysis (AREA)
• General Chemical & Material Sciences (AREA)
• Oil, Petroleum & Natural Gas (AREA)
• Organic Chemistry (AREA)
• Lubricants (AREA)

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• 2012
  • 2012-05-03 EP EP12718220.2A patent/EP2705126A1/de not_active Withdrawn
  • 2012-05-03 US US14/115,365 patent/US20140128303A1/en not_active Abandoned
  • 2012-05-03 CN CN201280021846.2A patent/CN103547660A/zh active Pending
  • 2012-05-03 BR BR112013028321A patent/BR112013028321A2/pt not_active IP Right Cessation
  • 2012-05-03 RU RU2013153814/04A patent/RU2013153814A/ru not_active Application Discontinuation
  • 2012-05-03 JP JP2014508793A patent/JP2014517097A/ja not_active Withdrawn
  • 2012-05-03 WO PCT/EP2012/058076 patent/WO2012150283A1/en active Application Filing

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