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United States Patent (19) 11 3,954,528 Chang Et Al

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United States Patent (19) 11 3,954,528 Chang Et Al United States Patent (19) 11 3,954,528 Chang et al. (45) May 4, 1976 (54) SOLID GAS GENERATING AND GUN I51 Int. Cl’.......................................... C06B 45/10 PROPELLANT COMPOSITION 58 Field of Search............. 149/92, 19, 19. 1, 19.4, CONTAINING TRAMINOGUANDINE 149/19.5, 19.6, 19.9, 19.91 NTRATE AND SYNTHETIC POLYMER BNDER 56 References Cited 75 Inventors: Marguerite S. Chang, Forest UNITED STATES PATENTS Heights; John H. Highby, Indian 2,929,699 3/1906 Audrieth et al................... 149/92 X Head, Gerald L. Mackenzie, Port 3, 117,044 1/1964 Sauer et al............................ 149/19 Tobacco, all of Md. 3,123,507 3/1964 Butts et al......................... 149/92 X (73) Assignee: The United States of America as represented by the Secretary of the Primary Examiner-Edward A. Miller Navy, Washington, D.C. Attorney, Agent, or Firm-R. S. Sciascia; J. A. Cooke ar 22) Filed: Nov. 6, 1970 57 ABSTRACT 21 Appl. No.: 97,444 Solid gas generating and gun propellant compositions employing triaminoguanidine nitrate as a propellant ingredient in admixture with an oxidant and a suitable 52 U.S. Cl............................... 149/19.4; 149/19.1; compatible binder material. 149/19.5; 149/19.6; 149/19.9; 149/1991; 149/92 7 Claims, No Drawings 3,954,528 1. 2 as a propellant ingredient, it imparts a low flame tem SOLID GAS GENERATING AND GUN perature, provides for good burning characteristics, PROPELLANT COMPOSITION CONTAINING and increases the amount of gas produced upon com TRIAMINOGUANIDINE NITRATE AND bustion of the instant propellant compositions. SYNTHETIC POLYMER BENDER 5 Triaminoguanidine nitrate may be synthesized accord ing to known processes and is commercially available BACKGROUND OF THE INVENTION in hydrochloride salt form. This invention relates generally to solid composite The optimum amount of the triaminoguanidine ni propellant compositions and more particularly to solid composite propellant compositions especially useful as trate salt utilized in the propellant compositions of this gas generators and gun propellants. invention is generally dependent upon the application Recently, there has been a great demand for new gas of the composition. For gas generator purposes, the generating propellants and gun propellants which are TAGN content should not exceed about 50 percent by cool burning, noncorrosive and yield a high amount of weight of the total composition, while for gun propel gas since attempts to improve existing gas generating 15 lant use higher quantities are applicable. compositions and gun propellants have been unsuc The oxidant and TAGN of the present invention may cessful for various reasons. For example, while the be incorporated into any compatible conventional addition of certain modifiers has lowered the flame binder matrix material. Generally, these are, for exam temperature and increased gas production, these same ple, gum rubbers of polyisoprene, . polyisobutylene, modifiers have contributed to the production of unde 20 butyl rubber, polyesters, polybutandienes, polyure sirable corrosive products. In turn, other modifiers thanes, polyglycols, polybutadienes with hydroxy or utilized in the past, while not producting corrosive carboxy functionality, polyesters with hydroxy func materials, have not succeeded to significantly lower the tionality, polyethers, vinyltetrazole polymers, glycidyl flame temperature or increase gas evolution. ether epoxy resins, and copolymers, etc. 25 More specifically, binder materials such as polyglycol SUMMARY OF THE INVENTION adipate, Butarez CTL I (a mixture of carboxyl-ter Accordingly, it is one object of this invention to pro minated polybutadiene and non-functional polybutadi vide a new solid composite gas generating and gun ene) Butarex CTL II (carboxyl-terminated polybutadi propellant composition. ene), the terpolymer of 2-methyl-5-vinyltetrazole: Another object of the present invention is to provide 30 a solid composite gas generating and gun propellant butyl acrylate: acrylic acid, and R-45M (a hydroxyl-ter composition which is cool burning and produces a high minated polybutadiene) are within the scope of this percentage of gas upon combustion. invention. Still another object of the instant invention is to pro A number of other materials may also be added in vide a solid composite gas generating and gun propel 35 minor amounts to the propellant compositions of this lant which yields only non-corrosive materials upon invention. These include for examples, coolants like combustion. oxamide, ammonium oxalate, oxilic acid, and guani These and other objects are achieved by providing a dine nitrate; plasticizers such as dioctyladipate, wetting composite propellant composition comprising an oxi agents such as lecithin, crosslinking and curing agents dant, such as cyclotetramethylenetetranitramine 40 such as di and trifunctional epoxides and ferric acetyl (HMX), triaminoguanidine nitrate (TAGN), and a acetonate (FeAA), other burning rate and ballistic modifiers, such as lead chromate, and vulcanizing suitable binder. agents like sulfur and sulfur containing compounds. DESCRIPTION OF THE PREFERRED Having generally described the invention the follow EMBODIMENTS 45 ing examples are set forth for purposes of illustration. It Pursuant to the present invention, an improved gas will be understood that the invention is not limited to : generating and gun propellant is provided by an admix these examples, but is susceptible to different modifica ture of an oxidant, preferably, cyclotetramethylenetet tions that will be recognized by one of ordinary skill in ranitramine (HMX) in an amount of from about 5 to the art. about 85 percent by weight, triaminoguanidine nitrate 50 in an amount of from about 5 to about 70 percent by EXAMPLE 1 weight and a suitable compatible organic polymeric binder in an amount of from about 5 to about 30 per Composition % weight cent by weight of the total composition. HMX 75.0 Although, HMX is the preferred oxidant of the in 55 TAGN 13.0 R 45M (hydroxyl-terminated 11.2 stant composition, other oxidants, which are tradition polybutagdiene, molecular ally employed for this purpose and are compatible with weight 2600, OH functionality the TAGN propellant ingredient of this invention, may 2.4, a product of Sinclair also be employed. Some of these are, for example, Petrochemicals, N.Y., N.Y.) cyclotrimethylenetrinitramine (RDX), ammonium ni 60 toluene diisocyanate ().8 trate, 5-aminotetrazole nitrate, ammonium perchlorate and mixtures thereof. It should be noted, however, that where the absence of non-corrosive gases upon com Theoretical Calculations bustion is desired ammonium perchlorate is not partic ularly suitable. 65 Chamber temperature at constant P(1000 psi): The triaminoguanidine nitrate ingredicnt of the in 2255K stant invention is a nitrogen rich compound with a Chamber temperature at constant V: 2800°K reasonably high melting point. When employed herein Moles of gas: 5.155 3,954,528 3 4. -continued Experimental Data Composition % weight Thermal stability at 95°C: one month without a Conco Oil 2.25 change in weight (in another formulation which was prepared the R45M binder was treated with 1 percent 5 phenyl-g-naphthylamine at 140°F. The propellant was The propellant compositions of the instant invention exceptionally stable and had a better retention of physi are readily formulated according to conventional pro cal properties). pellant mixing procedures; i.e., the solids, e.g., TAGN, Flame temperature in Closed Bomb Test: HMX etc., are mixed with the organic binder and cur 2208°K (300 psi), about 2358°K at 1000 psi 10 ing or crosslinking agent, extruded or compression molded, and subsequently heat cured. EXAMPLE 2 Having thus described the invention, what is claimed as new and desired to be secured by Letters Patent of Composition % weight the United States is: 15 1. A composite propellant composition comprising 5-aminotetrazole nitrate 75 TAGN 8.5 (1) an oxidant selected from the group consisting of binder (45 percent 1-methyl-5- 20.() cyclotetramethylene tetranitramine, cyclotrimethylene vinyltetrazole 45 percent methoxyethyl trinitramine, ammonium nitrate, 5-aminotetrazole ni methyl-tetrazole trate, ammonium perchlorate and mixtures thereof, (2) 6 percent ethylene dimethylacrylate triaminoguanidine nitrate, and a compatible synthetic 4 percent cumene hydropcroxide) 20 DTA Ti: 1480 polymer binder. Burning rate 1000 psi; 77°F : 0.634 in./sec. 2. The composite propellant composition of claim 1 wherein said oxidant is present in an amount within the range of from about 5 to about 85 percent by weight, said triaminoguandine nitrate is present in an amount EXAMPLE 3 25 within the range of from about 5 to about 70 percent by weight and said binder is present in an amount within Composition % weight the range of from about 5 to about 30 percent by TAGN 10.0 weight of the total composition. ammonium nitrate 748 3. The composite propellant composition of claim 2 polyisoprene rubber - 305 (Shell Oil Co.) 12.75 30 wherein said oxidant is selected from the group consist sulfur (). p-quinone dioxime (). ing of cyclotetramethylenetetranitramine, ammonium Conco Oil 2.25 nitrate, 5-aminotetrazole nitrate, and mixtures thereof. 4. The composite propellant composition of claim 3 wherein said compatible binder is a polymer selected 35 from the group consisting of polyisoprene, polyisobu EXAMPLE 4 tylene, butyl rubber, a polyester, a polyurethane, a polyglycol, a polybutadiene, a polybutadiene having Composition % weight carboxy functionality, a polybutadiene
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