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
  • C10L1/00—Liquid carbonaceous fuels
  • C10L1/10—Liquid carbonaceous fuels containing additives
  • C10L1/14—Organic compounds
  • C10L1/18—Organic compounds containing oxygen
  • C10L1/188—Carboxylic acids; metal salts thereof
  • C10L1/1886—Carboxylic acids; metal salts thereof naphthenic acid
• • 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
  • C10L1/20—Organic compounds containing halogen
  • C10L1/201—Organic compounds containing halogen aliphatic 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
  • C10L1/00—Liquid carbonaceous fuels
  • C10L1/10—Liquid carbonaceous fuels containing additives
  • C10L1/14—Organic compounds
  • C10L1/20—Organic compounds containing halogen
  • C10L1/202—Organic compounds containing halogen aromatic 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
  • 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)
  • C10L1/306—Organic compounds compounds not mentioned before (complexes) organo-metallic compounds (containing a metal to carbon bond) organo Pb compounds
• • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
  • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
  • F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
  • F02B3/00—Engines characterised by air compression and subsequent fuel addition
  • F02B3/06—Engines characterised by air compression and subsequent fuel addition with compression ignition

Definitions

• the present invention relates to improved fuels for internal combustion engines, and more particularly to a metal-containing motor fuel which, due to its content of particular metals, in particular form, and at particular concentrations, has improved characteristics and increases the performance of gasoline (spark ignition) or diesel (compression ignition) engines operated therewith.
• motor fuel is used to designate all liquid hydrocarbon fuels suitable for use in internal combustion engines of all type, including gasoline, kerosene, and diesel fuel.
• Such fuels are composed of a mixture of various types of hydrocarbons boiling within the range of about 80 to about 800 F.
• Another object of this invention is to provide a fuel whose deposits in the engine improve anti-knock properties.
• a further object of this invention is to provide gasolines and diesels fuels of improved combustion characteristics.
• a still further object of this invention is to provide a process of making improved motor fuels by the addition of a special composition containing zinc, copper and lead compounds in certain amounts and proportions.
• the present invention provides for the preparation of concentrated solutions of the additive to be incorporated into the fuel.
• the present invention mainly comprises the provision of a motor fuel comprising per each liter of fuel about 0.5-15 mg. of zinc in the form of zinc naphthenate, about 0.5-25 mg. of copper in the form of copper napht-henate, and lead in the form of lead naphthenate in an amount at least about 2 times the weight of the sum of the zinc and copper content, the total amount of zinc, copper and lead being between about 3 and 200 mg. per liter of fuel.
• brominated and/or chlorinated hydrocarbon in an amount such as to obtain a 10% to preferably 35% to 50% bromination of the added metals in the case of brominated hydrocarbons, and a 20% to 200%, preferably 70% to 100% chlorination of the added metals in the case of the chlori nated hydrocarbons.
• bromin-ation and chlorination are used herein to designate the conversion of the added metals into their maximum valency halogen compounds. If brominated and chlorinated hydrocarbons are used concurrently, they should be added in such proportions as to provide the amounts of bromine and chlorine required for the above stated halogenation levels.
• brominated benzene brominated ethylene, chlorinated benzene or chlorinated ethylene as the halogenated hydrocarbons.
• bromo benzene, ethylene dibromide, ohloro benzene and/or ethylene dichloride will give the most desirable results.
• the additive composition of the present invention which contains 05-15 mg. of zinc in the form of zinc naphthenate, about 05-25 mg. of copper in the form of copper naphthenate, and lead in at least double the amount of the total of the zinc and copper, the total amount of the zinc, copper and lead being greater than 3 mg., and being as high as a total of 200 mg., are suitable not only for gasoline for internal combustion engines, but for diesel oils and for fuels in general for all types of internal combustion engines.
• a preferred motor fuel in accordance with the present invention comprises per each liter of hydrocarbon fuel about 3.5-8 mg., most preferably about 7.2 mg., of zinc in the form of zinc naphthenate, about 0.55 mg.,
• composition of the additives with reference to the metals (mg/l.)
• the composition of the present invention has the efiect of forming a film between the cylinder walls and the piston which improves the compression and reduces the friction between the cylinder and piston, thus improving the entire operation of the engine and rendering the operation of the same much more economical.
• porous sealing ring which is level at the top, that is pressed flat and which is about 1-2 mm. (depending on the size of the engine) wide, is conical towards the bottom and which fills the space between the piston head and the motor block in a wedgeshaped manner.
• This ring can be taken off and upon analysis is found to have essentially always the same composition.
• the presence of these metals is, however, of critical importance for the formation of the film, and their amount is likewise decisive for the formation and the efficiency of the film in accordance with the present invention.
• the copper content influences the combustion and thereby the amount and proportion of C and H in the deposits.
• the content of C and H in the deposits in order to achieve the most desirable effects has been found to be about 30- 35%, whereby the ratio of C:H is about 1:1.
• the additives of the present invention may be added not only to unleaded fuels, but also to leaded motor fuels, that is fuels containing soluble lead compounds, particularly lead tetraethyl, as anti-knock agents. It is common practice to use in conjunction with lead tetraethyl certain halogenated hydrocarbons as scavenging agents. In the normal leaded motor fuel the contents of lead tetraethyl and halogenated hydrocarbons are balanced in such Way that in the combustion chamber theoretically the total amount of lead becomes volatile as lead-bromide or lead chloride, and is expelled with the exhaust gases.
• Gasoline as used in connection with the present invention is a well known article of commerce for use in internal combustion engines operating on the Otto cycle. It is composed of a mixture of various types of hydrocarbons, including aromatics, olefins, parafims, isoparafiins and naphthenes. These mixtures are obtained from petroleum by refining processes including fractional distillation, catalytic cracking, hydroforming, alkylation and extraction. Motor gasoline boils between 80 F. (initial boiling point) and about 450 .F., when tested by A.S.T.M. method 86. Its vapor pressure by A.S.T.M. method D323 varies for use at different seasons between 7 and 15 lbs. per square inch at 100 F.
• diesel fuels used in the practice of the present invention are all of the commonly sold grades including kerosene. Kerosenes normally have boiling ranges between 100 F. and about 600 F. and are sometimes referred to in the petroleum industry as No. 1 fuel oils. Diesel. fuels in general have boiling ranges between F. and are described more fully in A.S.T.M. specification D-975-53T as amended.
• Such fuels are derived from petroleum crude oils by a variety of processing operations which may include atmospheric and vacuum distillation, catalytic and thermal cracking, catalytic and thermal reforming, visbreaking, hydrotreating and the like.
• processing operations which may include atmospheric and vacuum distillation, catalytic and thermal cracking, catalytic and thermal reforming, visbreaking, hydrotreating and the like.
• diesel fuel is composed of a mixture of various types of hydrocarbons including parafiins, isoparafiins, naphthenes and aromatics.
• the efliciency in accordance with the present invention can be impaired through acids of the sulfur formed during combustion, Which partly bind amounts of metals added.
• the amounts of metals added in accordance with the present invention should be increased according to the content of sulfur, e.g. the content of sulfur of 2%, the
• naphthenates of copper, lead and zinc were carried out with naphthenates of copper, lead and zinc.
• commercial naphthemates of lead, copper and zinc made by Hoechster Farbwerke, Frankfurt-am-Main were used. These naphthenates were individually dissolved in a gasoline having a boiling range of 100 C. in such amount as to obtain (1) a lead solution containing 58.8 g. of lead per liter, (2) a copper solution containing 13.6 g. of copper per liter, and (3) a zinc soluton containing 28.8 g. of zinc per liter.
• the gasoline contained 29.4 mg. of lead, 3.4 mg. of copper, 7.2 mg. of zinc and 0.03 cc. of mono bromo benzene per liter.
• the amount of gas blown through into the crankcase was substantially reduced and stabilized at a minimum, which was measured and found to be 50% of the amount of gas blown through and measured when the same motor was operated without the additive of the present invention.
• the amount of gas blown through with standard gasoline was measured to be 88 cc. per second at 3000 r.p.m. and 11.6 H.P. output, and this blown through amount dropped for the same number of revolutions and the same output to 44 cc. when the gasoline with the additive of the present invention was used.
• the increase of the output or efiiciency corresponded to the improved sealing effect obtained according to the present invention and to a corresponding increase of the compression pressure with a simultaneous improvement of the combustion.
• a drop of the CO percentage and an increase of the CO percentage was found. Irrespective of the increased compression pressure, no tendency to knock could be determined or found.
• EXAMPLE 2 25 cc. of the lead solution, 12.5 cc. of the copper solution, and 12.5 cc. of the zinc solution were mixed with 0.935 cc. of ethylene dibromide and the mixture was added to 50 litres of the gasoline of Example 1. The additives thus contained with respect to the metal contents the same composition as in Example 1. However, the ha1ogenof 0.0187 cc. of ethylene dibromide instead of 0.03 cc. liter.
• the diesel oil had a specific weight of 0.840 and a sulfur content of 0.96%.
• EXAMPLE 4 An additive was added to 50 liters of the same diesel oil as in Example 3 so that the composition with respect to the metals was the same as in Example 3. However, the addition of the halogenated hydrocarbon amounted to 0.045 cc. and in another case to 0.06 cc. of mono bromo benzene per liter.
• EXAMPLE 5 The following test was carried outwith unleaded ARAL Super gasoline to which per liter of fuel were added 29.4 mg. lead, 0.6 mg. copper and 3.6 mg. zinc, and furthermore 0.006 cc. ethylene dibromide and 0.011 cc. ethylene dichloride, whereby corresponding amounts of the above described master solutions of the respective metals were used.
• EXAMPLE 6 16 cc. of the lead solution, 25 cc. of the copper solution and 25 cc. of the zinc solution were added to 100 liters of commercial gasoline which had been leaded with 10 0.3 cc. per liter of lead tetraethyl.
• the gasoline has the following characteristics: Specific wt. at C. 0.726 Initial boiling 32 15 Boiling until 55 percent 14.5 Boiling until 70 do.. 31 Boiling until 100 do 55 End of boiling 192 Olefin content percent 21 Aromatic content do 15 Each liter of the gasoline thus contained 9.4 mg. of lead, 3.4 mg. of copper and 7.2 mg. of zinc.
• the first drive was taken with a regular gasoline not containing the additives of this invention.
• the fuel consumption amounted to 25.746 liter/100 km.
• the following eight drives were taken with the above described gasoline according to this invention and gave the following results:
• the fuel consumption decreased by 25.99% after going a total distance of 1608 km. as compared with the fuel consumption observed when operating the bus on a regular fuel without thev additives of this invention.
• EXAMPLE 7 A gasoline containing 0.45 cc. per liter of lead tetraethyl and having the following characteristics:
• EXAMPLE 8 8 cc. of the lead solution, 12.5 cc. of the copper solution and 12.5 cc. of the zinc solution were mixed with 100 liters of a commercial leaded super gasoline con- Table I [Percentage changes of measurements indicating the engine performance when using gasoline containing the additive of the present invention as compared to the use of normal gasoline] Measurements at full load Revolutions Before the overhaul After the overhaul per minute Performance, Specific Amount of gas Specific Amount of gas Horsepower percent consumption, blown Horsepower Performance consumption, blown percent through, percent through, percent percent Table 11 Measurements with partial load Revolutions per Before the overhaul After the overhaul minute Performance, Specific consump- Amount of gas Specific consump- Amount of gas Horsepower percent tion, percent blown through, Horsepower tion, percent blown through,
• This incrustation was black and hard, that is a typical oil crust. The residue was left in the engine when the gasoline with additives was introduced into the engine. After the test with the gasoline containing the additive the incrustation on the piston head was reduced to about 0.2 min; it be- EXAMPLE 9 17.5 cc. of the lead solution, 4.5 cc. of the copper solution and 12.5 cc. of the zinc solution, 0.3 cc. ethylene dibromide and 0.6 cc. ethylene dichloride were added to of one of the common Volume percent Content of olefins 3 Content of aromatics 30:9 Content of paraifins and naphthenes 66.0 Content of sulfur 0.034
• Cylinder 8.6 10. Cylinder 2 7. 8 9. 4 Cylinder 3 8. 9. 3 Cylinder 4".-- 8. 8 10. 0
• Cylinder 1- 8. 5 8.0 Cylinder 2 7.8 7. 6 Cylinder 3. 8.7 8. 1 Cylinder 4... 9. 0 8.1
• halogenated hydrocarbons as scavenging agents.
• a motor fuel for use in internal combustion engines comprising a liquid hydrocarbon motor fuel for internal combustion engines containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 05-15 mg. of zinc in the form of zinc naphthenate, about 0.5-25 mg. of copper in the form of copper naphthenate, and lead in the form of lead naphthenate in an amount equal to at least two times the total of the zinc and copper content, the total amount of zinc, copper and lead being not more than 200 mg.
• a motor fuel for use in internal combustion engines is provided.
• said motor fuel comprising a liquid hydrocarbon motor fuel for internal combustion engines containing as an essential co-active ingredient an additive for each liter of fuel consisting of about 0.5-15 mg. of zinc in the form of zinc naphthenate, about 0.5-25 mg. of copper in the form of copper naphthenate, and lead in the form of lead naphthenate in an amount equal to about two to three times the total of the zinc and copper content, and also containing a member selected from the group consisting of brominated and chlorinated benzene and ethylene in an amount sufficient for an about 10-100% bromination and an about 20-200% chlorination, respectively, of said copper, zinc and lead.
• a motor fuel for use in internal combustion engines comprising a liquid hydrocarbon motor fuel for internal combustion engines containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 0.5-15 mg. of zinc in the form of zinc naphthenate, about 0.5-25 mg. of copper in the form of copper naphthenate, and lead in the form of lead naphthenate in an amount equal to about two to three times the total of the zinc and copper content, and also containing a member selected from the group consisting of brominated and chlorinated benzene and ethylene in an amount sufficient for an about 35-50% bromination and an about 7 -100% chlorination, respectively, of said copper, zinc and lead.
• a motor fuel for use in internal combustion engines comprising a liquid hydrocarbon motor fuel for internal combustion engines containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 3.5-8 mg. of zinc in the form of zinc naphthenate, about 0.5- mg. of copper in the form of copper naphthenate, and lead in the form of lead naphthenate in an amount equal to about 2.5-3 times the total of the zinc and copper content per liter, and also containing a member selected from the group consisting of brominated and chlorinated benzene and ethylene in an amount sufficient for an about -100-% bromination and an about 20-200% chlorination, respectively, of said copper, zinc and lead.
• a motor fuel for use in internal combustion engines comprising a liquid hydrocarbon motor fuel for internal combustion engines containing as an essential co-active ingredient an additive per each liter of fuel consisting of 3.5-8 mg. of zinc in the form of Zinc naphthenate, about 0.5-5 mg. of copper in the form of copper naphthenate, and lead in the form of lead naphthenate in an amount equal to about 2.5-3 times the total of the zinc and copper content, and also containing a member selected from the group consisting of brominated and chlorinated benzene and ethylene in an amount sufficient for an about 35-50% bromination and an about 70-100% chlorination, respectively, of said copper, zinc and lead.
• a motor fuel for use in internal combustion engines comprising a liquid hydrocarbon motor fuel for internal combustion engines containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 7.2 mg. of zinc in the form of zinc naphthenate, about 3.4 mg. of copper in the form of copper naphthenate, about 29.4 mg. of lead in the form of lead naphthenate, and a member selected from the group consisting of brominated and chlorinated benzene and ethylene in an amount sufficient for an about 35-50% bromination and an about 70-100% chlorination, respectively, of said copper, zinc and lead.
• Diesel fuels boiling in the range between about 200 F. and about 600 F. containing as an essential oo-active ingredient an additive per each liter of fuel consisting of about 7.2 mg. of zinc in the form of zinc naphthenate, about 3.4 mg. of copper in the form of copper naphthenate, about 29.4 mg. of lead in the form of lead naphthenate, and about 0.045 to about 0.06 cc.
• a motor fuel for use in internal combustion engines comprising a liquid hydrocarbon motor fuel for internal combustion engines containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 3.6 mg. of zinc in the form of zinc naphthenate, about 0.6 mg. of copper in the form of copper naphthenate, about 29.4 mg. of lead in the form of lead naphthenate, and about 0.006 cc. of ethylene dibromide and 0.011 cc. of ethylene dichloride.
• a motor fuel for use in internal combustion engines comprising a leaded liquid hydrocarbon motor fuel for internal combustion engines containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 0.5-15 mg. of zinc in the form of zinc naphthenate, about 05-25 mg. of copper in the form of copper naphthenate, and lead in the form of lead naphthenate in an amount equal to at least two times the total of the zinc and copper content, the total amount of zinc, copper and lead in the form of naphthenates being between about 3 and 200 mg.
• a motor fuel for use in internal combustion engines comprising a leaded liquid hydrocarbon motor fuel for internal combustion engines containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 3.5-8 mg. of Zinc in the form of zinc naphthenate, about 0.5-5 mg. of copper in the form of copper naphthenate, and lead in the form of lead naphthenate in an amount equal to about 2.5-3 times the total of the zinc and copper content, and also containing a member selected from the group consisting of brominated and chlorinated benzene and ethylene in an amount sufficient for an about 35-50% bromination and an about 70-100% chlorination, respectively, of said copper, zinc and lead in the form of naphthenates.
• a motor fuel for use in internal combustion engines comprising a leaded liquid hydrocarbon motor fuel for internal combustion engines containing between about 0.3-0.6 cc. of lead tetraethyl and halogenated hydrocarbon scavenging agents therefor, and also containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 05-15 mg. of Zinc in the form of Zinc naphthenate, about 0.5-25 mg.
• a motor fuel for use in internal combustion engines comprising a leaded liquid hydrocarbon motor fuel for internal combustion engines containing per liter 0.3-0.6 cc. of lead tetraethyl and halogenated hydrocarbon scavenging agents therefor in an amount up to 50% higher than necessary for halogenating the lead of the lead tetraethyl, and also containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 3.6 mg. of zinc in the form of zinc naphthenate, about 0.6 mg. of copper in the form of copper naphthenate, and about 10 mg. of lead in the form of lead naphthenate.
• a motor fuel for use in internal combustion engines comprising a leaded liquid hydrocarbon motor fuel for internal combustion engines containing per liter between about 0.3-0.6 cc. of lead tetraethyl and halogenated hydrocarbon scavenging agents therefor in an amount up to 50% higher than necessary for halogenating the lead of the lead tetraethyl, and also containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 05-15 mg. of zinc in the form of zinc naphthenate, about 05-25 mg. of copper in the form of copper naphthenate, and lead in the form of lead naphthenate in an amount of about 80-100% of the total of the zinc and copper content in the form of naphthenates.
• a motor fuel for use in internal combustion engines comprising a leaded liquid hydrocarbon motor fuel for internal combustion engines containing per liter 0.6 cc. of lead tetraethyl and halogenated hydrocarbon scavenging agents therefor in an amount up to 50% higher than necessary for halogenating the lead of the lead tetraethyl, and also containing as an essential co-active ingredient an additive per each liter of fuel consisting of about 7.2 mg. of zinc in the form of zinc naphthenate, about 0.6 mg. of copper in the form of copper naphthenate, and about 6.2 mg. of lead in the form of lead naphthenate.

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• Chemical & Material Sciences (AREA)
• Oil, Petroleum & Natural Gas (AREA)
• Engineering & Computer Science (AREA)
• Chemical Kinetics & Catalysis (AREA)
• General Chemical & Material Sciences (AREA)
• Organic Chemistry (AREA)
• Liquid Carbonaceous Fuels (AREA)
• Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
• Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

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• 0
  • NL NL243431D patent/NL243431A/xx unknown
  • BE BE581117D patent/BE581117A/xx unknown
  • LU LU37147D patent/LU37147A1/xx unknown
• 1958
  • 1958-09-26 AT AT676858A patent/AT210544B/de active
• 1959
  • 1959-04-10 DE DET16530A patent/DE1108005B/de active Pending
  • 1959-04-10 DE DET18942A patent/DE1220667B/de active Pending
  • 1959-04-16 CH CH7211359A patent/CH395641A/de unknown
  • 1959-06-30 FR FR798881A patent/FR1228798A/fr not_active Expired
  • 1959-07-20 ES ES0250914A patent/ES250914A1/es not_active Expired
  • 1959-09-28 GB GB32935/59A patent/GB919184A/en not_active Expired
• 1963
  • 1963-04-15 US US272880A patent/US3341310A/en not_active Expired - Lifetime

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