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Title: Evolution of Carbon Clusters in the Detonation Products of the Triaminotrinitrobenzene (TATB)-Based Explosive PBX 9502

Abstract

Here, the detonation of carbon-rich high explosives yields solid carbon as a major constituent of the product mixture and, depending on the thermodynamic conditions behind the shock front, a variety of carbon allotropes and morphologies may form and evolve. We applied time-resolved small angle x-ray scattering (TR-SAXS) to investigate the dynamics of carbon clustering during detonation of PBX 9502, an explosive composed of triaminotrinitrobenzene (TATB) and 5 wt% fluoropolymer binder. Solid carbon formation was probed from 0.1 to 2.0 μs behind the detonation front and revealed rapid carbon cluster growth which reached a maximum after ~200 ns. The late-time carbon clusters had a radius of gyration of 3.3 nm which is consistent with 8.4 nm diameter spherical particles and matched particle sizes of recovered products. Simulations using a clustering kinetics model were found to be in good agreement with the experimental measurements of cluster growth when invoking a freeze-out temperature, and temporal shift associated with the initial precipitation of solid carbon. Product densities from reactive flow models were compared to the electron density contrast obtained from TR-SAXS and used to approximate the carbon cluster composition as a mixture of 20% highly ordered (diamond-like) and 80% disordered carbon forms, which willmore » inform future product equation of state models for solid carbon in PBX 9502 detonation product mixtures.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1];  [1];  [2];  [2];  [2];  [2];  [2];  [3];  [3];  [4];  [4]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. Washington State Univ., Pullman, WA (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Washington State Univ., Pullman, WA (United States). Inst. for Shock Physics
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1400254
Grant/Contract Number:
NA0002442
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 41; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Watkins, Erik B., Velizhanin, Kirill A., Dattelbaum, Dana M., Gustavsen, Richard L., Aslam, Tariq D., Podlesak, David W., Huber, Rachel C., Firestone, Millicent A., Ringstrand, Bryan S., Willey, Trevor M., Bagge-Hansen, Michael, Hodgin, Ralph, Lauderbach, Lisa, van Buuren, Tony, Sinclair, Nicholas, Rigg, Paulo A., Seifert, Soenke, and Gog, Thomas. Evolution of Carbon Clusters in the Detonation Products of the Triaminotrinitrobenzene (TATB)-Based Explosive PBX 9502. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.7b05637.
Watkins, Erik B., Velizhanin, Kirill A., Dattelbaum, Dana M., Gustavsen, Richard L., Aslam, Tariq D., Podlesak, David W., Huber, Rachel C., Firestone, Millicent A., Ringstrand, Bryan S., Willey, Trevor M., Bagge-Hansen, Michael, Hodgin, Ralph, Lauderbach, Lisa, van Buuren, Tony, Sinclair, Nicholas, Rigg, Paulo A., Seifert, Soenke, & Gog, Thomas. Evolution of Carbon Clusters in the Detonation Products of the Triaminotrinitrobenzene (TATB)-Based Explosive PBX 9502. United States. doi:10.1021/acs.jpcc.7b05637.
Watkins, Erik B., Velizhanin, Kirill A., Dattelbaum, Dana M., Gustavsen, Richard L., Aslam, Tariq D., Podlesak, David W., Huber, Rachel C., Firestone, Millicent A., Ringstrand, Bryan S., Willey, Trevor M., Bagge-Hansen, Michael, Hodgin, Ralph, Lauderbach, Lisa, van Buuren, Tony, Sinclair, Nicholas, Rigg, Paulo A., Seifert, Soenke, and Gog, Thomas. 2017. "Evolution of Carbon Clusters in the Detonation Products of the Triaminotrinitrobenzene (TATB)-Based Explosive PBX 9502". United States. doi:10.1021/acs.jpcc.7b05637.
@article{osti_1400254,
title = {Evolution of Carbon Clusters in the Detonation Products of the Triaminotrinitrobenzene (TATB)-Based Explosive PBX 9502},
author = {Watkins, Erik B. and Velizhanin, Kirill A. and Dattelbaum, Dana M. and Gustavsen, Richard L. and Aslam, Tariq D. and Podlesak, David W. and Huber, Rachel C. and Firestone, Millicent A. and Ringstrand, Bryan S. and Willey, Trevor M. and Bagge-Hansen, Michael and Hodgin, Ralph and Lauderbach, Lisa and van Buuren, Tony and Sinclair, Nicholas and Rigg, Paulo A. and Seifert, Soenke and Gog, Thomas},
abstractNote = {Here, the detonation of carbon-rich high explosives yields solid carbon as a major constituent of the product mixture and, depending on the thermodynamic conditions behind the shock front, a variety of carbon allotropes and morphologies may form and evolve. We applied time-resolved small angle x-ray scattering (TR-SAXS) to investigate the dynamics of carbon clustering during detonation of PBX 9502, an explosive composed of triaminotrinitrobenzene (TATB) and 5 wt% fluoropolymer binder. Solid carbon formation was probed from 0.1 to 2.0 μs behind the detonation front and revealed rapid carbon cluster growth which reached a maximum after ~200 ns. The late-time carbon clusters had a radius of gyration of 3.3 nm which is consistent with 8.4 nm diameter spherical particles and matched particle sizes of recovered products. Simulations using a clustering kinetics model were found to be in good agreement with the experimental measurements of cluster growth when invoking a freeze-out temperature, and temporal shift associated with the initial precipitation of solid carbon. Product densities from reactive flow models were compared to the electron density contrast obtained from TR-SAXS and used to approximate the carbon cluster composition as a mixture of 20% highly ordered (diamond-like) and 80% disordered carbon forms, which will inform future product equation of state models for solid carbon in PBX 9502 detonation product mixtures.},
doi = {10.1021/acs.jpcc.7b05637},
journal = {Journal of Physical Chemistry. C},
number = 41,
volume = 121,
place = {United States},
year = 2017,
month = 8
}

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  • The detonation of carbon-rich high explosives yields solid carbon as a major constituent of the product mixture and, depending on the thermodynamic conditions behind the shock front, a variety of carbon allotropes and morphologies may form and evolve. We applied time-resolved small angle x-ray scattering (TR-SAXS) to investigate the dynamics of carbon clustering during detonation of PBX 9502, an explosive composed of triaminotrinitrobenzene (TATB) and 5 wt% fluoropolymer binder. Solid carbon formation was probed from 0.1 to 2.0 μs behind the detonation front and revealed rapid carbon cluster growth which reached a maximum after ~200 ns. The late-time carbon clustersmore » had a radius of gyration of 3.3 nm which is consistent with 8.4 nm diameter spherical particles and matched particle sizes of recovered products. Simulations using a clustering kinetics model were found to be in good agreement with the experimental measurements of cluster growth when invoking a freeze-out temperature, and temporal shift associated with the initial precipitation of solid carbon. Product densities from reactive flow models were compared to the electron density contrast obtained from TR-SAXS and used to approximate the carbon cluster composition as a mixture of 20% highly ordered (diamond-like) and 80% disordered carbon forms, which will inform future product equation of state models for solid carbon in PBX 9502 detonation product mixtures.« less
  • Triaminotrinitrobenzene (TATB) is a highly anisotropic molecular crystal used in several plastic-bonded explosive (PBX) formulations. A complete understanding of the orientation distribution of TATB particles throughout a PBX charge is required to understand spatially variable, anisotropic macroscale properties of the charge. Although texture of these materials can be measured after they have been subjected to mechanical or thermal loads, measuring texture evolution in situ is important in order to identify mechanisms of crystal deformation and reorientation used to better inform thermomechanical models. Neutron diffraction measurements were used to estimate crystallographic reorientation while deuterated TATB (d-TATB) powder was consolidated into amore » cylindrical pellet via a uniaxial die-pressing operation at room temperature. Both the final texture of the pressed pellet and the in situ evolution of texture during pressing were measured, showing that the d-TATB grains reorient such that (001) poles become preferentially aligned with the pressing direction. A compaction model is used to predict the evolution of texture in the pellet during the pressing process, finding that the original model overpredicted the texture strength compared to these measurements. The theory was extended to account for initial particle shape and pore space, bringing the results into good agreement with the data.« less
  • The sensitivity of TATB-based explosive PBX-9502 is affected by non-reversible thermal expansion, or {open_quotes}ratchet growth.{close_quotes} PBX-9502 is a plastic-bonded explosive consisting of 95 wt{percent} TATB (2,4,6-trinitro-1,3,5-benzenetriamine) and 5 wt{percent} Kel-F 800 binder (chlorotrifluoroethylene/vinylidine 3:1 copolymer). The magnitude of the increase in size and the corresponding increase in sensitivity is reported here for a particular pressing of PBX-9502, after repeated thermal cycling. The physical morphology of the expanded material is examined using scanning electron microscopy, in an effort to determine the increase in intergranular holes, intragranular cracks and fissures in the TATB crystals, and the change in the distribution of themore » Kel-F, all of which are suspected to affect the sensitivity of the material. These images support the proposed mechanism for ratchet growth. Sensitivity, growth of the reactive wave behind the shock front, and Hugoniot data are obtained from in-material particle velocity gauge records of the shock initiation process. Increases in sensitivity with growth and with elevated temperature are summarized in Pop plots. Sensitivity increases commensurate with the increase in voids. {copyright} {ital 1998 American Institute of Physics.}« less