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AD-763 879 PREDICTION OF SAFE LIFE OF PROPELLANTS N. S. Garman, et al Picatinny Arsenal Dover, New Jersey May 1973 DISTRIBUTED BY: National Technical Informatin Service U. S. DEPARTMENT OF COMMERCE 5285 Port Royal Road, Springfield Va. 22151 COPY NO. TECHNICAL REPORT 4505 PREDICTION OF SAFE LIFE OF PROPELLANTS N. S. GARMAN J. P. PICARD S. POLAKOSKI J. M. MURPHY rN2(cid:127) ~O KMAY 1973I APPROVED FOR PUBLIC RELEASE: DISTRIBUTION UNLIMITED :,, NAI-IONA L TECHNICAL S~INFORMATION SERVICE (cid:127);!PICATINNY ARSENAL DOVER, NEW JERSEY UNCLASSIFIED Securit% C'lassifjcation DOCUMENT CONTROL DATA -R & D (Sec.urty .ei ton ol title, body 0t abstracl and Indexing annotation must be entered when the -ralJ reponr Is claselifed) ORIGINATING ACT-ITTV (Cospotate authot) A*e. REPORT SECURITY CLASSIFICATION UNCLASSIFIED Picatinny Arsenal, Dover, New Jersey 07801 2b. GRouP 3 REPORT TITLE PREDICTION OF SAFE LIFE OF PROPELLANTS 4 OESCRIPTIVE NOTES (ype o ofrport and Inclu.lve dates) S AU THORISI (First name, middle initial, last name) N. S. Garman J. M. Murphy J. P. Picard S. Polakoski 0. REPORT DATE70TOA rPAE 17.N.F IS May 1973 T .. N9?V$GS b. NO. OF 5.R EPS So. CONTRACT OR GRANT NO- 5l ORIGINATOR'S REPORT NUM'SERIS) b. PROJECT NO. Technical Report 4505 €.AAMCC. MS S CCooed41e. 62458.S1b0.. 16. 2954.1 tOheT.Ho(cid:127)sEc Ra pRoEnPO) RT NoOMsS (A(cid:127)(cid:127)oney other n.,minb,e,fe th,a t mayy (cid:127) be a.s(cid:127)signed d. tO. OIsTRIBevrioN STATEMENT Approved for Public Release: Distribution unlimited It. SUPPLEMENTARY NOTES 12. SPONSORING MILITARY ACTIVITY IS, AMSTRACT The measure of chemical stability and the prediction of safe storage life is of prime interest to the manufacturer and use of propellants. This report will discuss the re- suits obtained with standard artillery propellant when exposed to artificial ageing at various temperatures. The measurements of residual stabilizer versus time have been used as the criteria for propellant deterioration. A kinetic interpretation of this deterioration phenomena employing Berthelot's Law demonstrates that a family of straight lines can be plotted characterizing the length of time necessary at the various test temperatures to obtain a given variation of stabilizer content. By establishing realist c cut-off points in regard to stabilizer content, propellant safe life may be safely calculated at any storage temperature. DD , l1473 m1 P: '00"414101 1AN s4 "'9• s UNCLASSIFIED A,) | security Classiflcation UNCLASSIFIED Security Classification I4. LINK A LINK 0 LINK C KEY WORDS OLE SWIT ROLE SW T ROLE WY Propellant Safe storage life prediction Propellant chemical stability Artificial ageing Propellant stabilizers Berthelot's Law of deterioration Propellant stabilizer analysis Propellant surveillance practices Propellant temperature resistance A Il0kiUtyN CLASSIFIED Clasesiication V Technical Report 4505 PREDICTION OF SAFE LIFE OF PROPELLANTS By N. S. Garman J. P. Picard S. Polakoski J. M. Murphy May 1973 Approved for Public Release: Distribution Unlimited AMCMS Code 4810.16.2954.1 Propellants Division Feltman Research Laboratory Picatinny Arsenal Dover, New Jersey 07801 TABLE OF CONTENTS Page Abstract 1 Object 2 Summary 2 Introduction 2 Results 4 Discussion 5 Conclusions 10 Recommendations 10 References 10 Tables 1. Representation of Arrhenius' and Berthelot's Law 7 2. Propellant Compositions 11 3. Prediction of Propellant Safe Life 12 Figures 1. Stabilizer Depletion Rate for M6 Propellant 13 Conditioned at 900 and 100C. 2. Stabilizer Depletion Rate for M6 Propellant 14 Conditioned at 600, 700 and 800C. 3. Stabilizer Depletion Rate for M9 Propellant 15 Conditioned at 80' and 90*C. 4. Stabilizer Depletion Rate for M9 Propellant 16 Conditioned at 600 and 70*C. 5. Stabilizer Depletion Rate for M30 Propellant 17 Conditioned at 90' and 100*C. TABLE OF CONTENTS (Cont) Figures 6. :' bilizer Depletion Rate for M30 Propellant 18 Conditioned at 60%, 70* and 80'C. 7. Stabilizer Depletion Rate for MIO Propellant 19 Conditioned at 900 and 100*C. 8. Stabilizer Depletion Rate for M1O Propellant 20 Conditioned at 600, 700 and 800C. 9. Deterioration Phenomena Expressed by Berthelot's 21 Law for M6 Propellant 10. Deterioration Phenomena Expressed by Berthelot's 22 Law for M9 Propellant 11. Deterioration Phenomena Expressed by Berthelot's 23 Law for M30 Propellant 12. Deterioration Phenomena Expressed by Berthelot's 24 Law for M1O Propellant 13. Comparing Data from Arrhenius'vs. Berthelot's 25 Equations Distribution List ii F ABSTRACT The measure of chemical stability and the prediction of safe storage life is of prime interest to the manufacturer and userof pro- pellants. This report will discuss the results obtained with standard artillery propellant when exposed to artificial ageing at various temperatures. The measurements of residual stabilizer versus time have been used as the criteria for propellant deterioration. A kinetic interpretation of this deterioration phenomena employing Berthelot's Law demonstrates that a family of straight lines can be plotted characterizing the length of time necessary at the various test temperatures to obtain a given variation of stabilizer content. By establishing realistic cut-off points in regard to stabilizer content, propellant safe life may be safely calculated at any storage temperature. OBJECT To apply standard analytical methods to propellant stabilizer determination in order to establish the rate of loss of stabilizer during periods of high temperature propellant ageing, applying Berthelot's Law of deterioration phenomena to the resulting data in an effort to predict propellant chemical safe life at any storage temperature., - SUMMARY As part of a project entitled "Long Range Study of Prediction of Safe Life of Propellants", benefits which may be derived by the appli- cation of testing procedures or concepts are reviewed and evaluated to determine their relevance. To this end, the testing technique described in this report and the kinetic interpretation of the resulting test data have shown much promise as a method of forecasting propellant chemical safe life on small samplings of standard single-, double- and triple-base U. S. Army artillery propellant formulations. However, work must be expanded to make a more comprehensive review of pro- pellants of U. S. Army interest and to study and refine the approach so that full application of this testing routine can be included in the propellant surveillance effort. INTRODUCTION One of the major problems concerned with the manufacture and use of propellants is the measurement of their chemical stability and the prediction of their safe storage life. The U. S. Army has substantial quantities of artillery propellants in storage. These various artillery propellants are subject to degradation with ageing, the end result being spontaneous ignition. Therefore, it is mandatory that a con- tinuous knowledge of the stability status of this stock be acquired. The Propellants Division, Picatinny Arsenal, has the responsibility for this mission, and currently maintains control over these stocks by conducting the 65.5*C. Surveillance Test and the propellant stock activity described in references (1) and (2) respectively. These two programs involve all lots of artillery propellant manufactured for the U. S. Army. The 65.5%C. Surveillance Test depends upon an end-point which is defined as the appearance of visible red fumes of nitrogen dioxide over the propellant sample stored at 65.5%C. It has been established through years of experience that the development of the end-point in 20 days or less denotes a storage hazard of the ambient stored stock but with an ample safety margin for disposition action on any remnant 2 of that lot of propellant. The propellant stock program has only very recently been implemented, the scope of this activity now relating to propelling charges and/or bulk propellant actually on hand in Field Service and Industrial Stock installations. Stabilizer content determinations of representative samples of each lot forwarded to this installation from the storage facilities form the basis for safe life determinations of this active stock. From the data developed by this program, in addition to those results observed in the 65.5*C. Surveillance Test, a sound, comprehensive stability control of all U. S. Army propellant stock is accomplished. The benefits derived from such programs far outweigh the costs of testing, in that these measurements are the controlling factor in pre- venting loss of property and possibly life. The results of these programs can be translated into money, material and manhour savings by insuring the use of only acceptable propellant in loading and re- blending operations, and by reducing storage costs through the dis- posal of unserviceable propellants. Additionally, a technical advan- tage is realized from conducting the 65.5'C. Surveillance Test in that opportunity is provided to perform related studies concerned with the safe life properties of propellants. It is widely recognized in the study of propellant chemical deterioration that the measurement of residual stabilizer content offers the best means of establishing the stability potential of these materials. The method of analysis is, of course, of the greatest im- portance. It must be analytically sound, reproducible, relatively simple and capable of providing results which can be meaningfully interpreted. In the last few years, such a method was developed and is presently replacing some of the older wet chemical methods whose results were questionable when applied to aged propellants. This method is described in detail in Reference 3. The available propellant stabijizer is separated from hot alkali by steam distillation and analyzed spectrophotometrically. For this, the distillate is diluted to a standard volume with ethanol and the absorbance of the solution measured at 285 and or 247 mu for the determination of available stabilizer as diphenylamine or ethyl centralite respectively. This method of analysis is employed to accomplish the surveillance activity described in Reference 2. Recently the NATO countries were in need of an evaluation pro- cedure that would assure acceptor countries that propellants receive-d from others would have a proven chemical stability for a given period of time Then stored at ambient conditions. After many stability tests were reviewed and evaluated through the conduct of round robins to insure that strict analytical agreement could be realized among 3

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