US3670649A - Combustible cartridges - Google Patents

Combustible cartridges Download PDF

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Publication number
US3670649A
US3670649A US63537A US3670649DA US3670649A US 3670649 A US3670649 A US 3670649A US 63537 A US63537 A US 63537A US 3670649D A US3670649D A US 3670649DA US 3670649 A US3670649 A US 3670649A
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Robert C Hartlein
James D Kiles
Willard D Larson
Carl R Olson
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Dow Silicones Corp
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Dow Corning Corp
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    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F42AMMUNITION; BLASTING
    • F42BEXPLOSIVE CHARGES, e.g. FOR BLASTING, FIREWORKS, AMMUNITION
    • F42B5/00Cartridge ammunition, e.g. separately-loaded propellant charges
    • F42B5/02Cartridges, i.e. cases with charge and missile
    • F42B5/18Caseless ammunition; Cartridges having combustible cases
    • F42B5/192Cartridge cases characterised by the material of the casing wall
    • F42B5/196Coatings
    • CCHEMISTRY; METALLURGY
    • C06EXPLOSIVES; MATCHES
    • C06BEXPLOSIVES OR THERMIC COMPOSITIONS; MANUFACTURE THEREOF; USE OF SINGLE SUBSTANCES AS EXPLOSIVES
    • C06B23/00Compositions characterised by non-explosive or non-thermic constituents
    • C06B23/009Wetting agents, hydrophobing agents, dehydrating agents, antistatic additives, viscosity improvers, antiagglomerating agents, grinding agents and other additives for working up
    • CCHEMISTRY; METALLURGY
    • C06EXPLOSIVES; MATCHES
    • C06BEXPLOSIVES OR THERMIC COMPOSITIONS; MANUFACTURE THEREOF; USE OF SINGLE SUBSTANCES AS EXPLOSIVES
    • C06B25/00Compositions containing a nitrated organic compound
    • C06B25/18Compositions containing a nitrated organic compound the compound being nitrocellulose present as 10% or more by weight of the total composition
    • C06B25/20Compositions containing a nitrated organic compound the compound being nitrocellulose present as 10% or more by weight of the total composition with a non-explosive or a non-explosive or a non-thermic component
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10STECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S102/00Ammunition and explosives
    • Y10S102/70Combustilbe cartridge

Definitions

  • Nonmetallic cartridges having a porous casing of fiber-reinforced nitrocellulose are rendered oil and water resistant by first incorporating into the casing an organosilicon compound which renders the casing material essentially impervious to liquid water but which does not substantially alter the porosity of the material and then providing a continuous coating on the surface of the casing, the coating beinga room'temperature curing resinous organosiloxane having from 1.2 to 1.8 organic substituents per silicon atom, the major portion of the organic substituents being lower alkyl and/or phenyl radicals.
  • This invention relates to an improved combustible cartridge.
  • the invention relates to a fiber-reinforced nitrocellulose cartridge casing which is resistant to penetration by oil and water.
  • Combustible cartridge cases composed of low-nitrogen nitrocellulose, reinforcing fibers and a resinous binder have been developed.
  • the combustible case functions as a container for a propellant charge and is fitted with a metal projectile to provide a cartridge.
  • Such a cartridge has the advantages of lighter weight and lesser cost because of the elimination of the conventional metal casing.
  • the cartridge case When dry, the cartridge case is truly combustible leaving a little or no residue in the breech of a gun after firing.
  • the combustibility of the nitrocellulose case is adversely affected and, upon firing, a substantial amount of residue is left in the breech of the gun.
  • contact with oily substances, such as hydraulic fluid adversely affects the firing characteristics of the combustible cartridge.
  • a combustible cartridge having a porous casing composed of a fiberreinforced nitrocellulose which forms an exterior cartridge surface
  • the improvement consisting essentially of a. a water-repellent organosilicon compound incorporated into the casing in an amount sufficient to render the casing substantially impermeable to liquid water
  • the organosilicon compound being selected from the group consisting of alkali metal salts of a monoorganosiliconates in which the organic group is a lower alkyl radical of from one to three inclusive carbon atoms and silanes of the formula R,,SiX and water-soluble hydrolyzates thereof, in which R is a monovalent hydrocarbon radical of from 1 to 30 carbon atoms, X is a hydrolyzable group and n is an integer having a value of 1 to 3; and
  • FIG. 1 is a schematic cross-section of an assembled combustible cartridge and FIG. 2 is a broken cross-section of a portion of the cartridge casing.
  • the assembled combustible cartridge includes a metal projectile 10, attached either mechanically or adhesively to the upper rim portion 11 of the cylindrical combustible case which is designated generally by the numeral 12.
  • a propellant 13, such as nitrocellulose, is contained in casing 12 and is ignited by a fast burning explosive 14, such as black powder, which is detonated by means of a primer element 15.
  • the cartridge case 12 consists of a tubular casing 16 and a base member 17 which can be attached to the bottom portion of casing 16 by mechanical or adhesive means 18. If desired, the case 12 can be molded as one piece.
  • the exact configuration of the above described elements forms no part of the present invention and can be varied according to design specification.
  • the case 12 is composed of low-nitrogen nitrocellulose, reinforcing fibers and a resinous binder. To ensure combustibility, the casing material must be porous. The porosity or void content is thought to allow flame propagation thru the case upon ignition of the main propellant charge 13 and provide for complete burning of the material.
  • the nitrocellulose can vary in nitrogen content, but is what is generally known as lownitrogen nitrocellulose, being combustible rather than explosive in its burning characteristics.
  • the amount of nitrocellulose incorporated into the casing material can vary depending upon the burning characteristics desired, but is generally in the range of from 50 to weight percent.
  • the nitrocellulose can be in the form of powder, fibers and the like.
  • Fibers in staple or continuous form are used to reinforce the casing and improve its dimensional stability.
  • the fibers must be combustible at the ignition temperature and can be of synthetic or natural origin.
  • Acrylics such as acrylonitrile; polyolefins, such as polypropylene; polyamides and polyesters are all exemplary of synthetic fibers which can be used.
  • the faster burning natural fibers such as cotton, hemp, jute, kraft fibers or other cellulosic materials are preferred.
  • the amount of fiber depends upon the casing strength desired and usually is in the range of 10-25 weight percent.
  • a resinous component such as polyvinyl formal, polyvinylacetate, polyacetal, polymethylmethacrylate or acrylonitrile, is employed as a binder for the nitrocellulosefiber mixture.
  • the amount of binder will vary depending upon the manufacturing technique and the desired strength characteristic, but will generally be in the range of 10-25 weight percent.
  • additives such as burn promoting agents and crystalline explosives can be incorporated into the casing material. Diphenylamine, cyclotetramethylene tetranitramine and diaminotrinitrobenzene are burn promoting additives which can be used.
  • the nitrocellulose-fiber-resin mixture can be formed into a casing 12 by many conventional methods such as compression molding, felting, injection molding and the like. If molded as separate elements, the tubular casing 16 and base 17 should be joined and sealed in such a manner as to prevent penetration of water or oil into the casing 12.
  • the above-described combustible cartridge is improved and rendered practical for use under a variety of field conditions by first incorporating a water repellent organosilicon compound in the casing material and then applying a substantially continuous coating to at least the exterior casing surface, the coating being a room temperature curing organosiloxane resin.
  • the resin coating acts as a primary barrier to moisture, in the form of liquid or vapor, and oil.
  • the water repellent organosilicon which is incorporated into the porous casing, serves to prevent wicking or transmission of liquid water throughout the casing in the event that the surface coating is damaged but does not destroy the porosity of the material.
  • the water repellent organosilicon compounds (a) used in the practice of the invention include alkali metal siliconate salts for example any lithium, sodium, potassium or cesium salt of the monomethyl siliconate, monoethyl siliconate, monopropyl siliconate, monovinyl siliconate, or monoallyl siliconate.
  • alkali metal siliconate salts for example any lithium, sodium, potassium or cesium salt of the monomethyl siliconate, monoethyl siliconate, monopropyl siliconate, monovinyl siliconate, or monoallyl siliconate.
  • These salts can contain an average from less than one to three inclusive alkali metal atoms per silicon atom.
  • the salts contain an average of from one to two alkali metal atoms per silicon atom.
  • two or more salts can be employed.
  • the sodium salts are preferred, in particular the sodium salt of monomethyl siliconate which contains about one sodium atom per silicon atom.
  • R can be any monovalent hydrocarbon radical of from 1 to 30 inclusive carbon atoms, such as alkyl radicals such as methyl, ethyl, isopropyl, hexyl, octadecyl or myricyl; alkenyl radicals such as vinyl, allyl, hexenyl; alkynyl radicals such as propargyl; cycloaliphatic radicals such as cyclopentyl, cyclohexyl or cyclohexenyl; aromatic hydrocarbon radicals such as phenyl, tolyl, xylyl, xenyl, naphthyl or anthracyl and aralkyl hydrocarbon radicals such as benzyl, beta-phenylethyl, beta-
  • X can be any hydrolyzable group such as halogen atoms such as F, Cl, Br or 1; groups of the formula OZ when 2 is any hydrocarbon or halogenated hydrocarbon group such as methyl, ethyl, isopropyl, octadecyl, allyl, hexenyl, cyclohexyl, phenyl, benzyl, beta-phenylethyl, 2-ch1oroethyl, chlorophenyl, 3,3,3-trifluoropropyl or bromocyclohexyl; any hydrocarbon ether radical such as Z-methoxyethyl, 2-ethoxyisopropyl, 2-butoxyisobutyl, p-methoxyphenyl or (CH CH O) CH any acyl radical such as acetyl, propionyl, benzoyl, cyclohexoyl, acrylyl, methacrylyl, stearyl, naph
  • any amino radical such as Nl-l dimethylamino, diethylamino, methylphenylamino or dicyclohexylamino
  • X can also be the sulfate group or sulfate ester groups of the formula OSO OM) where M is defined above; the cyano group; the isocyanate group; and the phosphate group or phosphate ester groups of the formula --OPO(OM) in which M is defined above.
  • hydrolyzable group means any group attached to the silicon which is hydrolyzed by water at room temperature to form 5 SiOH.
  • a relatively inexpensive source of the water repellent silanes are the chlorosilicon compounds produced as by-products in the direct process method for preparing alkyl silicon chlorides by the reaction of alkyl chlorides with silicon.
  • a mixture of by-product chlorosilicon compounds contained in the residue from this direct process can by hydrolyzed to provide water soluble hydrolyzate which is neutralized by the addition of calcium hydroxide.
  • the above described water repellents can be incorporated into the casing material by a variety of methods, such as by impregnating, for example dipping or spraying; mixing the organosilicons into a pulp mixture which is then molded or felted to form the casing or by pretreating the reinforcing fiber component of the mixture with the defined organosilicon compounds.
  • the water repellents can be incorporated into the casing material by exposing the molded casing to the organosilicon compound which is entrained in steam.
  • the casing must be dried to remove free water.
  • the amount of organosilicon compound which is incorporated is sufficient to render the casing substantially impermeable or nontransmittive of liquid water. This amount will vary with the density and porosity of the casing material, but is generally in the range of 0.1 to 3 percent by weight of the casing material.
  • substantially impermeable to liquid water it is meant that the casing material, after incorporation of the water repellent, does not transmit liquid water through a 100 mil thickness after having sustained the efi'ects of a 12- inch head of water for 1 hour.
  • the defined water repellent organosilicon compounds are very poor film formers, thus the porosity of the casing is lowered by only a small amount, for example by 20 percent of its untreated value.
  • the retention of the substantial amount of porosity throughout the casing material is necessary to flame propagation and complete combustion of the casing during firmg.
  • organosiloxane resin on the exterior surface of the casing serves as the primary barrier to penetration by oil and moisture.
  • Silicones in general are considered poor candidates in material applications where combustibility is a necessary characteristic and the above described organosiloxane resin cannot be considered combustible.
  • the resin is tailored, by means of controlling the degree and type of substitution on the silicon atom, to provide a flexible film which will not crack during normal handling, yet had sufiicient rigidity to shatter upon firing. This flexible frangible film is shattered into fine particles and carried away by the hot combustion gases during firing of the cartridge, thus eliminating a major source of residue in the breech of the gun.
  • the organo substituents in the siloxane resin must be either lower alkyl of one to six carbon atoms or phenyl radicals.
  • the siloxy units of the resin include Cfl SiO C H SiO C H (Cl-l )SiO, (C H SiO, (Cl-1 SiO units, C H-,(C H )Si0 and C H SiO It is preferred that at least 50 percent of the substituents be phenyl radicals. Those resins have a degree of substitution of less than 1.2 are brittle and easily cracked during handling.
  • the resin having a degree of substitution of greater than 1.8 have elastomeric properties, thus are not frangible, and leave a great amount of residue after firing. Because of these limitations the resin is a combination of the monoorganosiloxy units and diorganosiloxy units described above with the preferred resins having a degree of substitution of from 1.3 to 1.6
  • the organosilicon resin must be one that cures at room temperature to form the flexible frangible coating.
  • the described resins cure at room temperature as a result of the remaining functionality, for example acetoxy or methoxy substituents which condense upon exposure to atmospheric moisture.
  • the resins are generally prepared by hydrolysis of the corresponding chlorosilanes. The hydrolyzate contains uncondensed hydroxyl groups which can then be reacted with functional silanes, such as trimethoxychlorosilane or triacetoxysilanes, to obtain the room temperature curing properties.
  • the room temperature curing properties of materials containing functionality, such as acetoxy functional resins are well known and illustrated in US. Pat. Nos. 2,934,519 and 3,032,529.
  • condensation catalysts such as dibutyltin dilaurate, can be used to accelerate the curing at room temperature.
  • One preferred resin for use in the invention is a ketoxime functional organosiloxane block copolymer consisting essentially of (a) 5 to 25 inclusive mol percent of diorganosiloxane units wherein the diorganosiloxane units are bonded through silicon-oxygen-silicon bonds forming a polydiorganosiloxane block having an average from 6 to 15 inclusive diorganosiloxane units per block, the polydiorganosiloxane being at least mol percent dimethylsiloxane or phenylmethylsiloxane units, any remaining units being selected from the group consisting of phenylmethylsiloxane and monomethylsiloxane units (b) 50 to 75 inclusive mol percent organosiloxane units having an average formula R,SiO wherein at has a value of from 1 to 1.3 inclusive and R" is an organic group selected from the group consisting of phenyl radicals, methyl radicals, ethyl radicals and prop
  • This room temperature curable composition can be prepared by several methods. The best method is to couple a hydroxyl-terminated polydiorganosiloxane with an aromaticcontaining organosiloxane resin having hydroxyl groups by reaction with a trifunctional organosilane. The resulting block copolymer is itself hydroxylated and then reacted with monoorganotriketoximesilane to yield the described composition. Alternatively, the hydroxylated terminated polydiorganosiloxane can be cohydrolyzed with a trifunctional organosilane in the proper proportion. Examples of Q and Q can be found in US. Pat. Nos. 3,184,427 and 3,189,576.
  • the resin is applied from a solution to the surface of the casing 12 by any conventional means such as spraying, dipping or brushing.
  • any suitable solvent which does not react with functional groups of the resin and which have no adverse effect on the casing material can be employed to form the coating solution.
  • solvents include benzene, toluene, xylene, perchloroethylene, mineral spirits and chlorobenzene.
  • thixotropic agents such as silica can be added to the solution to provide for a uniform coating. Care should be taken during the coating operation to avoid pin holes in the thin film.
  • the amount of resin coated onto the shell casing will vary but is generally in the range of from 2 to 15 weight percent, thus providing 1 to 5 mil thickness of coating.
  • a heat conductive substance such as carbon black, silicon carbide, or powdered metal, for example aluminum, be incorporated in the resin coating. These materials serve to transfer the heat of a point of combustion, such as a small piece of burning char or cigarette, over a large area thus minimizing fire hazards from such materials.
  • the invention contemplates, as an ar ticle of manufacture, combustible fiber-reinforced nitrocellulose products having incorporated therein a water repellent organosilicon compound as previously defined in an amount sufi'rcient to render the material substantially impermeable to liquid water and having a continuous coating on the surface thereof of the described room temperature curable organosiloxane resin.
  • a water repellent organosilicon compound as previously defined in an amount sufi'rcient to render the material substantially impermeable to liquid water and having a continuous coating on the surface thereof of the described room temperature curable organosiloxane resin.
  • FIG. 2 fiber-reinforced nitrocellulose prepared in accordance with the invention is illustrated.
  • the water repellent organosilicon compound 19 is incorporated throughout the casing material 12, while the organosiloxane resin 20 forms a continuous coating on the exterior surface.
  • EXAMPLE Combustible cartridges (152 mm) composed of 69 weight percent nitrocellulose, 15 weight percent kraft fibers, 15 weight percent formaldehyde resin binder and 1 weight percent of diphenylamine, were impregnated with a weight percent aqueous solution of the sodium salt of monomethyl siliconate having about one sodium atom per silicon atom. The cartridges were sprayed with the solution and allowed to dry. After drying the exterior surfaces of the cartridges were sprayed with a toluene solution of a ketoxime functional resin prepared by the reaction of monomethyldi(methylethylketoxime )siloxy terminated polydimethylsiloxane (d.p.
  • the cartridges were loaded with propellant primed and fitted with a projectile. A portion of the assembled cartridges were exposed to a simulated rain stonn for 12 hours. The cartridges, both dry and wet, were fired from a 155 mm howitzer. Muzzle velocities were comparable to those of untreated cartridges. The dry cartridges left no residue in the breech after firing. The cartridges which had been exposed to the rain left little or no residue in the breech, the largest fragment residue totaling only 3-4 square inches. Untreated cartridges fabricated from the same components leave a considerable amount of residue in the breech which must be removed prior to firing another round.
  • An article of manufacture having a surface of porous fiber-reinforced nitrocellulose, the fiber-reinforced nitrocellulose having incorporated therein a water-repellent organosilicon compound in an amount sufficient to render the nitrocellulose substantially impermeable to v liquid water, the or ganosilicon compound being selected from the group consisting of alkali metal salts of monoorganosilconates in which the organic group is a lower alkyl of from one to three inclusive carbon atoms and silanes of the formula R,,SiX., and watersoluble hydrolyzates thereof in which R is a monovalent hydrocarbon radical of from 1 to 30 inclusive carbon atoms, X is a hydrolyzable group and n is an integer having a value of l or 3; said surface having a continuous coating thereon of a room temperature curable organosiloxane resin, said organosiloxane resin having an average of from 1.2 to 1.8 organic groups per silicon atom, at least mol percent of the organic groups being selected
  • siloxane resin contains from 3 to 20 mol percent of ketoxime siloxy units.
  • organosiloxane resin consists essentially of a. 5 to 25 inclusive mol percent of diorganosiloxane units wherein the diorganosiloxane units are bonded through silicon-oxygen-silicon linkages to form a diorganosiloxane block having an average of from 6 to 15 inclusive siloxy units per block, the polydiorganosiloxane being at least mol percent dimethylsiloxane' or phenylmethylsiloxane units any remaining units being selected from the group consisting of phenylmethylsiloxane and monomethylsiloxane units;
  • organosiloxane units of the general formula R" ,.SiO wherein x has a value of from 1 to 1.3 inclusive and R" is selected from the group consisting of methyl, ethyl, propyl and phenyl radicals, at least 50 mol percent of the R" substituents being phenyl radicals, the organosiloxane units comprising a block of at least 3 siloxane units, the siloxane units being selected metal salt of a monoorganosiliconate in which the organic group is a lower alkyl of one to three inclusive carbon atoms.
  • a cartridge in accordance with claim 9 wherein the organosilicon compound is monomethyl sodium siliconate.
  • halogenated hydrocarbon radicals and Q is a divalent hydrocarbon radical; the mol percentages of (a), (b) and being based on the total number of siloxane units present.
  • a water repellent organosilicon compound incorporated into said casing in an amount sufficient to render said casing substantially impermeable to liquid water
  • said organosilicon compound being selected from the group consisting of alkali metal salts of a monoorganosiliconate in which the organic group is a lower alkyl radical of from one to three inclusive carbon atoms, and silanes of the formula R,,SiX.,-,, and water-soluble hydrolyzates thereof, in which R is a monovalent hydrocarbon radical of from 1 to 30 carbon atoms, X is a hydrolyzable group and n is an integer having a value of l to 3 inclusive; and
  • a cartridge in accordance with claim 7 wherein the or- 11 A cartridge in accordance with claim 9 wherein the organosiloxane resin contains ketoxime radicals.
  • the organosiloxane resin consists essentially of a. 5 to 25 inclusive mol percent of diorganosiloxane units wherein the diorganosiloxane units are bonded through silicon-oxygen-silicon linkages to form a diorganosilox ane block having an average of from 6 to 15 inclusive siloxy units per block, the polydiorganosiloxane being at least mol percent dimethylsiloxane or phenylmethylsiloxane units any remaining units being selected from the group consisting of phenylmethylsiloxane and monomethylsiloxane units;
  • organosiloxane units of the general formula R",SiO wherein x has a value of from 1 to 1.3 inclusive and R" is selected from the group consisting of methyl, ethyl, propyl and phenyl radicals, at least 50 mol percent of the R" substituents being phenyl radicals, the organosiloxane units comprising a block of at least 3 siloxane units, the siloxane units being selected from the group consisting of monoorganoand diorganosilox y units; and

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CA (1) CA962841A (fr)
CH (1) CH574591A5 (fr)
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US20130172496A1 (en) * 2010-09-22 2013-07-04 Dow Corning Corporation High refractive index compositions containing resin-linear organosiloxane block copolymers
US20130168727A1 (en) * 2010-09-22 2013-07-04 Dow Corning Corporation Organosiloxane block copolymer
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US8776690B2 (en) 2009-08-04 2014-07-15 Nitrochemie Aschau Gmbh Sleeve for accommodating propellant charge powder
US20150001567A1 (en) * 2011-12-30 2015-01-01 Dow Corning Corporation Solid state light and method of forming
US20150031826A1 (en) * 2012-03-12 2015-01-29 Dow Corning Corporation Compositions of resin-linear organosiloxane block copolymers
US20150031841A1 (en) * 2012-02-29 2015-01-29 Dow Corning Corporation Compositions of Resin-Linear Organosiloxane Block Copolymers
US20150045486A1 (en) * 2011-12-02 2015-02-12 Dow Corning Corporation Curable compositions of resin-linear organosiloxane block copolymers
US20150045520A1 (en) * 2012-03-21 2015-02-12 Dow Corning Corporation Compositions of resin-linear organosiloxane block copolymers
US20150043241A1 (en) * 2012-03-20 2015-02-12 Dow Corning Corporation Light guide and associated light assemblies
US20150051356A1 (en) * 2012-03-28 2015-02-19 Dow Corning Corporation Amphiphilic Resin-Linear Organosiloxane Block Copolymers
US20150073077A1 (en) * 2012-03-21 2015-03-12 Dow Corning Corporation Compositions comprising resin-linear organosiloxane block copolymers and organopolysiloxanes
US20150087772A1 (en) * 2012-03-21 2015-03-26 Dow Corning Corporation Compositions of resin-linear organosiloxane block copolymers
US20150087771A1 (en) * 2012-03-21 2015-03-26 Dow Corning Corporation Process for preparing resin-linear organosiloxane block copolymers
US20150112011A1 (en) * 2012-03-21 2015-04-23 Dow Corning Corporation Compositions of resin-linear organosiloxane block copolymers
US20160009866A1 (en) * 2013-03-15 2016-01-14 Dow Corning Corporation Compositions of Resin-Linear Organosiloxane Block Copolymers
RU2781931C1 (ru) * 2021-11-29 2022-10-21 Федеральное казенное предприятие "Государственный научно-исследовательский институт химических продуктов" Способ нанесения защитного покрытия на сгорающий материал жесткого сгорающего картуза

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US3929074A (en) * 1974-04-05 1975-12-30 Us Navy Means for the elimination of a cartridge rim
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US8776690B2 (en) 2009-08-04 2014-07-15 Nitrochemie Aschau Gmbh Sleeve for accommodating propellant charge powder
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DE2140742C3 (de) 1974-10-03
AT316392B (de) 1974-07-10
BE771246A (fr) 1972-02-14
FR2102232A1 (fr) 1972-04-07
CH574591A5 (fr) 1976-04-15
CA962841A (en) 1975-02-18
GB1337340A (en) 1973-11-14
DE2140742A1 (de) 1972-03-30
DE2140742B2 (de) 1974-02-21
JPS5238360B1 (fr) 1977-09-28
SE373858B (fr) 1975-02-17
FR2102232B1 (fr) 1974-03-29
NL7111105A (fr) 1972-02-15

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