DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Comprehensive End-to-End Design of Novel High Energy Density Materials: II. Computational Modeling and Predictions

Abstract

In this work, we have proposed a holistic approach to design novel energetic materials by bridging synthesis, experimental characterization, computational modeling, and validation. Multiscale computational modeling that combines first-principles calculations, analytical theory, and empirical statistical analysis served to further advance the proposed methodology. The established materials design guiding principles led to development of a set of new energetic molecules, PHE-1, PHE-2, and PHE-3, that represent improved variations of the heterocyclic energetics and are predicted to be superior to the existing conventional energetic materials. Molecular mechanisms of the enhanced performance and sensitivity of the proposed energetic materials as a function of their chemical composition and structure are discussed.

Authors:
 [1];  [2];  [3]; ORCiD logo [1]
  1. Univ. of Maryland, College Park, MD (United States). Materials Science and Engineering Dept.
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Energetic Materials Center
  3. Bakhirev Scientific Research Inst. of Mechanical Engineering, Dzerzhinsk, Nizhny Novgorod (Russia)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE
OSTI Identifier:
1483297
Grant/Contract Number:  
AC52-07NA27344; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 43; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Tsyshevsky, Roman, Pagoria, Philip, Smirnov, Aleksandr S., and Kuklja, Maija M. Comprehensive End-to-End Design of Novel High Energy Density Materials: II. Computational Modeling and Predictions. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.7b07585.
Tsyshevsky, Roman, Pagoria, Philip, Smirnov, Aleksandr S., & Kuklja, Maija M. Comprehensive End-to-End Design of Novel High Energy Density Materials: II. Computational Modeling and Predictions. United States. https://doi.org/10.1021/acs.jpcc.7b07585
Tsyshevsky, Roman, Pagoria, Philip, Smirnov, Aleksandr S., and Kuklja, Maija M. Mon . "Comprehensive End-to-End Design of Novel High Energy Density Materials: II. Computational Modeling and Predictions". United States. https://doi.org/10.1021/acs.jpcc.7b07585. https://www.osti.gov/servlets/purl/1483297.
@article{osti_1483297,
title = {Comprehensive End-to-End Design of Novel High Energy Density Materials: II. Computational Modeling and Predictions},
author = {Tsyshevsky, Roman and Pagoria, Philip and Smirnov, Aleksandr S. and Kuklja, Maija M.},
abstractNote = {In this work, we have proposed a holistic approach to design novel energetic materials by bridging synthesis, experimental characterization, computational modeling, and validation. Multiscale computational modeling that combines first-principles calculations, analytical theory, and empirical statistical analysis served to further advance the proposed methodology. The established materials design guiding principles led to development of a set of new energetic molecules, PHE-1, PHE-2, and PHE-3, that represent improved variations of the heterocyclic energetics and are predicted to be superior to the existing conventional energetic materials. Molecular mechanisms of the enhanced performance and sensitivity of the proposed energetic materials as a function of their chemical composition and structure are discussed.},
doi = {10.1021/acs.jpcc.7b07585},
journal = {Journal of Physical Chemistry. C},
number = 43,
volume = 121,
place = {United States},
year = {2017},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 20 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: Structures of (a) oxadizole fragments and functional groups as building blocks involved in constructing energetic materials, (b) 3,4- bis(4-nitro-1,2,5-oxadiazol-3-yl)-1,2,5-oxadiazole-2-oxide (BNFF), (c) 3,4-bis(4-nitro-1,2,5-oxadiazol-3-yl)-1,2,5-oxadiazole with (BNFF-1, LLM-172) and 3-(4-amino-1,2,5-oxadiazol-3-yl)-4-(4-nitro-1,2,5-oxadiazol-3-yl)-1,2,5-oxadiazole (ANFF-1, LLM-175), (d) 3,5-bis(4-nitro1,2,5-oxadiazol-3-yl)-1,2,4-oxadiazole (LLM-191) and 3-(4-amino1,2,5-oxadiazol-3-yl)-5-(4-nitro-1,2,5-oxadiazol-3-yl)-1,2,4-oxadiazole (LLM-192), and (e) 3,3′-bis(3-nitro-1,2,5-oxadiazol-4-yl)-5,5′-bi-1,2,4oxadiazole (LLM-200).

Save / Share:

Works referenced in this record:

A Comparison of Model Chemistries
journal, November 1995

  • Ochterski, Joseph W.; Petersson, George A.; Wiberg, Kenneth B.
  • Journal of the American Chemical Society, Vol. 117, Issue 45
  • DOI: 10.1021/ja00150a030

Recent Advances in the Synthesis of High Explosive Materials
journal, December 2015


Comprehensive End-to-End Design of Novel High Energy Density Materials: I. Synthesis and Characterization of Oxadiazole Based Heterocycles
journal, October 2017

  • Tsyshevsky, Roman; Pagoria, Philip; Zhang, Maoxi
  • The Journal of Physical Chemistry C, Vol. 121, Issue 43
  • DOI: 10.1021/acs.jpcc.7b07584

Design and Synthesis of Energetic Materials
journal, August 2001


Thermochemische untersuchungen an nitraminen
journal, July 1973


Thermal Decomposition of Energetic Materials. 66. Kinetic Compensation Effects in HMX, RDX, and NTO
journal, November 1994

  • Brill, T. B.; Gongwer, P. E.; Williams, G. K.
  • The Journal of Physical Chemistry, Vol. 98, Issue 47
  • DOI: 10.1021/j100098a020

Using Hessian Updating To Increase the Efficiency of a Hessian Based Predictor-Corrector Reaction Path Following Method
journal, October 2004

  • Hratchian, H. P.; Schlegel, H. B.
  • Journal of Chemical Theory and Computation, Vol. 1, Issue 1
  • DOI: 10.1021/ct0499783

A review of energetic materials synthesis
journal, February 2002


Recent approaches to the synthesis of high explosive and energetic materials: A review
journal, March 1984


Comprehensive assessment of physicochemical properties of new energetic materials
journal, October 2016


Modeling Thermal Decomposition Mechanisms in Gaseous and Crystalline Molecular Materials: Application to β-HMX
journal, November 2011

  • Sharia, Onise; Kuklja, Maija M.
  • The Journal of Physical Chemistry B, Vol. 115, Issue 44
  • DOI: 10.1021/jp202733d

Inhomogeneous Electron Gas
journal, November 1964


Assessment of Gaussian-2 and density functional theories for the computation of enthalpies of formation
journal, January 1997

  • Curtiss, Larry A.; Raghavachari, Krishnan; Redfern, Paul C.
  • The Journal of Chemical Physics, Vol. 106, Issue 3
  • DOI: 10.1063/1.473182

Accurate reaction paths using a Hessian based predictor–corrector integrator
journal, June 2004

  • Hratchian, Hrant P.; Schlegel, H. Bernhard
  • The Journal of Chemical Physics, Vol. 120, Issue 21
  • DOI: 10.1063/1.1724823

Effect of Polar Surfaces on Decomposition of Molecular Materials
journal, September 2014

  • Kuklja, Maija M.; Tsyshevsky, Roman V.; Sharia, Onise
  • Journal of the American Chemical Society, Vol. 136, Issue 38
  • DOI: 10.1021/ja506297e

Thermochemistry of N-nitro- and N -nitrosoamines of the alicyclic series
journal, August 1974

  • Pepekin, V. I.; Matyushin, Yu. N.; Lebedev, Yu. A.
  • Bulletin of the Academy of Sciences of the USSR Division of Chemical Science, Vol. 23, Issue 8
  • DOI: 10.1007/BF00923193

Computational Design of Novel Energetic Materials: Dinitro-bis-triazolo-tetrazine
journal, April 2015

  • Tsyshevsky, Roman V.; Pagoria, Philip; Kuklja, Maija M.
  • The Journal of Physical Chemistry C, Vol. 119, Issue 16
  • DOI: 10.1021/acs.jpcc.5b01086

Ab Initio Kinetics of Gas Phase Decomposition Reactions
journal, December 2010

  • Sharia, Onise; Kuklja, Maija M.
  • The Journal of Physical Chemistry A, Vol. 114, Issue 48
  • DOI: 10.1021/jp108065c

Gaussian-3 theory using density functional geometries and zero-point energies
journal, April 1999

  • Baboul, Anwar G.; Curtiss, Larry A.; Redfern, Paul C.
  • The Journal of Chemical Physics, Vol. 110, Issue 16
  • DOI: 10.1063/1.478676

Surface-Enhanced Decomposition Kinetics of Molecular Materials Illustrated with Cyclotetramethylene-tetranitramine
journal, May 2012

  • Sharia, Onise; Kuklja, Maija M.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 20
  • DOI: 10.1021/jp301723j

Generalized transition state theory. Classical mechanical theory and applications to collinear reactions of hydrogen molecules
journal, April 1979

  • Garrett, Bruce C.; Truhlar, Donald G.
  • The Journal of Physical Chemistry, Vol. 83, Issue 8
  • DOI: 10.1021/j100471a031

Additivity rules for the estimation of thermochemical properties
journal, June 1969

  • Benson, Sidney W.; Cruickshank, F. R.; Golden, D. M.
  • Chemical Reviews, Vol. 69, Issue 3
  • DOI: 10.1021/cr60259a002

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965


LASL Explosive Property Data
book, December 1980


Works referencing / citing this record:

Accelerating the discovery of insensitive high-energy-density materials by a materials genome approach
journal, June 2018


Accelerating the discovery of insensitive high-energy-density materials by a materials genome approach
journal, June 2018


Azasydnone – novel “green” building block for designing high energetic compounds
journal, January 2018

  • Dalinger, Igor L.; Serushkina, Olga V.; Muravyev, Nikita V.
  • Journal of Materials Chemistry A, Vol. 6, Issue 38
  • DOI: 10.1039/c8ta06895j

N -(2-Fluoro-2,2-dinitroethyl)azoles: a novel assembly of diverse explosophoric building blocks for energetic compound design
journal, January 2019

  • Palysaeva, Nadezhda V.; Gladyshkin, Aleksei G.; Vatsadze, Irina A.
  • Organic Chemistry Frontiers, Vol. 6, Issue 2
  • DOI: 10.1039/c8qo01173g