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Title: Moisture Outgassing Rates from TATB-Formulations: Experiments and Kinetic Model Development

Conference ·
OSTI ID:967290

Moisture outgassing rates from materials are of interest and importance to a variety of different fields. Because water can attack and accelerate decomposition, aging, or rusting of various parts, the assembly of an apparatus with 'wet' materials can shorten the lifetime of the apparatus. Outgassing of moisture from materials can be quite slow and a material that is seemingly dry at the time of assembly may slowly release water over years. This slow release of water will compromise the other constituents of the apparatus (e.g. electrical components, metals, organic materials) and shorten the lifetime of the apparatus. For apparatuses that are expensive or laborious to construct, it is especially important to understand and be able to predict the mechanisms and rates of water release from various materials. Such an understanding can support the development of accurate estimates of the apparatus's serviceable age and may allow for mitigation strategies in order to protect other parts from water. Energetic materials such as TATB based PBX-9502 (95% TATB, 5% Kel-F 800) and LX-17 (92.5% TATB and 7.5% Kel-F) pose a particularly challenging problem because they are heterogeneous materials with potentially many different sources and mechanisms of water release. Water molecules could be adsorbed into the polymeric binder matrix, trapped in occlusions within the polymer and the TATB crystals/particles, or trapped within defect sites in the TATB crystal. Finally, many studies indicate that water is a decomposition product under rapid heating conditions, at high temperatures and/or high pressure. Previous studies have measured the water release rate(s) from LX-17 or PBX-9502 prill/powder in order to establish oven drying times prior to use. These studies limited their time frame to a few days or a week of drying. Other studies have looked at the rate of water release of large pressed parts contained in sealed containers. Finally, some studies have looked at the rate of water diffusion through pressed parts, or the effects of wet vs. dry machining, or the influence of the synthesis methods in the amount of water present. There are a few different models that have been developed to predict the rate of water release from LX-17 or PBX-9502. These models are, to some extent, limited by the limitations of the experiments. Because all these experiments looked at water release over a relatively short period of time and left the samples relatively undamaged, they serve as a lower bound. In this work, we perform experiments and develop models that can serve as an upper bound on the rate and amount of water that can be released. Our experimental approach is to use temperature programmed desorption (TPD) and monitor the rate and amount of water release as a function of temperature. We analyzed our experimental data using two different kinetic analysis methods (isoconversional analysis and nth-order Arrhenius kinetic fits) and used the results to make predictions. The suitability of these kinetic analysis methods as well as the applicability of these experiments to long term aging (e.g. years) issues are discussed. Using the kinetics from our experiments, we predict the water release at temperature and timescales relevant to the existing literature. Based on our analysis and comparison with older data, the kinetic model(s) developed in this work serve as a relatively accurate (i.e. order of magnitude) method for predicting the water release under a variety of thermal histories.

Research Organization:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
W-7405-ENG-48
OSTI ID:
967290
Report Number(s):
LLNL-PROC-415199; TRN: US200923%%304
Resource Relation:
Conference: Presented at: Compatibility, Aging, and Stockpile Stewardship, Albuquerque, NM, United States, Sep 29 - Oct 02, 2009
Country of Publication:
United States
Language:
English