CaltechAUTHORS
  A Caltech Library Service

Increasing Oxygen Balance Leads to Enhanced Performance in Environmentally Acceptable High-Energy Density Materials: Predictions from First-Principles Molecular Dynamics Simulations

Guo, Dezhou and Zybin, Sergey V. and Chafin, Andrew P. and Goddard, William A., III (2022) Increasing Oxygen Balance Leads to Enhanced Performance in Environmentally Acceptable High-Energy Density Materials: Predictions from First-Principles Molecular Dynamics Simulations. ACS Applied Materials & Interfaces, 14 (4). pp. 5257-5264. ISSN 1944-8244. doi:10.1021/acsami.1c20600. https://resolver.caltech.edu/CaltechAUTHORS:20220119-817310000

[img] PDF (Bond order cutoff values for different atom pairs and evolution of the system pressure during constant temperature simulation of eight times volume expansion over 20 ps) - Supplemental Material
See Usage Policy.

95kB

Use this Persistent URL to link to this item: https://resolver.caltech.edu/CaltechAUTHORS:20220119-817310000

Abstract

Environmental concerns have stimulated the development of green alternatives to environmentally pollutive nitramine compounds used for high-energy density materials (HEDMs). The excellent energetic properties of CL20 make it a promising candidate, but its negative oxygen balance limits its efficiency for industrial and military applications. We predict here that CL20-EO formed by introducing ether links into the CC bonds of the original CL20 structure to attain balanced CO₂ and H₂O production leads to improved performance while minimizing the formation of carbonaceous clusters and toxic gases. To test this concept, we predicted the detonation properties at the Chapman–Jouguet (CJ) state using reactive molecular dynamics simulations with the ReaxFF force field combined with quantum mechanics based moleculear dynamics. We predict that CL20-EO enhances energetic performance compared to CL20 with a 6.0% increase in the CJ pressure and a 1.1% increase in the detonation velocity, which we attribute to achieving the correct oxygen balance to produce fully oxidized gaseous products. After expansion to normal conditions from the CJ state, CL20-EO leads only to nontoxic fully oxidized gases instead of forming the carbonaceous clusters and toxic gases found with CL-20. Thus, CL20-EO is predicted to be environmentally green. These results indicate that oxygen balance plays an important role in both energy availability and end-product toxicity and that balanced CO₂ and H₂O production systems provide promising candidates for the next generation of environmentally acceptable alternatives to toxic HEDMs while also enhancing the detonation performance.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acsami.1c20600DOIArticle
ORCID:
AuthorORCID
Guo, Dezhou0000-0003-2094-9195
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2022 American Chemical Society. Received: October 25, 2021; Accepted: January 4, 2022; Published: January 18, 2022. This research was funded by a grant from the ONR (N00014-19-1-2081, program manager, Chad Stoltz). D.G. and W.A.G. thank S.Z. for communicating his predictions about the structures and energetics of CL20-EO in advance of publications. Author Contributions. D.G. and S.V.Z. carried out the atomistic simulations. D.G., W.A.G., and S.V.Z. wrote the manuscript and contributed to the data analysis. A.P.C. carried out the CHEETAH calculations. All authors discussed the results and commented on the manuscript. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Office of Naval Research (ONR)N00014-19-1-2081
Subject Keywords:Chapman−Jouguet, CL20, QM-MD, ReaxFF, oxygen balance, energetic performance
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1509
Issue or Number:4
DOI:10.1021/acsami.1c20600
Record Number:CaltechAUTHORS:20220119-817310000
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20220119-817310000
Official Citation:Increasing Oxygen Balance Leads to Enhanced Performance in Environmentally Acceptable High-Energy Density Materials: Predictions from First-Principles Molecular Dynamics Simulations. Dezhou Guo, Sergey V. Zybin, Andrew P. Chafin, and William A. Goddard. ACS Applied Materials & Interfaces 2022 14 (4), 5257-5264; DOI: 10.1021/acsami.1c20600
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:113000
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:20 Jan 2022 16:47
Last Modified:23 Apr 2022 05:09

Repository Staff Only: item control page