Fracture of crystals and frictional heating are associated with the formation of “hot spots” (localized heating) in energetic composites such as polymer bonded explosives (PBXs). Traditional high speed optical imaging methods cannot be used to study the dynamic sub-surface deformation and the fracture behavior of such materials due to their opaque nature. In this study, high speed synchrotron X-ray experiments are conducted to visualize the in situ deformation and the fracture mechanisms in PBXs composed of octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX) crystals and hydroxyl-terminated polybutadiene binder doped with iron (III) oxide. A modified Kolsky bar apparatus was used to apply controlled dynamic compression on the PBX specimens, and a high speed synchrotron X-ray phase contrast imaging (PCI) setup was used to record the in situ deformation and failure in the specimens. The experiments show that synchrotron X-ray PCI provides a sufficient contrast between the HMX crystals and the doped binder, even at ultrafast recording rates. Under dynamic compression, most of the cracking in the crystals was observed to be due to the tensile stress generated by the diametral compression applied from the contacts between the crystals. Tensile stress driven cracking was also observed for some of the crystals due to the transverse deformation of the binder and superior bonding between the crystal and the binder. The obtained results are vital to develop improved understanding and to validate the macroscopic and mesoscopic numerical models for energetic composites so that eventually hot spot formation can be predicted.

Composite energetic materials have been shown to generate heat under certain ultrasonic excitations, enough to drive rapid reactions in some cases. In an attempt to isolate the proposed heat generation mechanisms of frictional and viscoelastic heating at crystal-crystal and crystal-binder interfaces, a systematic study was conducted with cyclotetramethylene-tetranitramine crystals arranged as discrete inclusions within Sylgard 184 binder. Groups of three embedded crystals, or “triads,” were arranged in two geometries with the crystals either in contact or slightly separated. Additionally, samples with good crystal-binder adhesion as well as ones mechanically debonded using compression were considered. The samples were excited ultrasonically with a contact piezoelectric transducer, and the top surface of each sample was monitored via infrared thermography. The contacting triads showed evidence of an intense localized heat source conducting to the polymer surface above the crystal locations in contrast to the separated triads. The debonded samples of both types reached higher maximum surface temperatures, on average. The results of both two-way and nested analysis of variance indicate a statistically significant difference for both adhesion and separation distance on temperature rise. We conclude that friction between crystal contact points and a debonded, moving binder at the crystal interface (also a mode of friction) play a significant role in localized heat generation, while viscoelastic/viscoplastic heating appears comparatively minor for these specific excitation conditions. The significance of frictional heat generation over viscoelastic heating in these systems may influence future design considerations related to the selection of binder materials for composite energetic materials.

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