Extreme nonequilibrium thermodynamics via quantum-chemical kinetics in multicomponent systems
Abstract
Energetic materials store high density of chemical energy, which can only be released through non-equilibrium chemical process, an exothermic reaction (typically, oxidation). For rapid release, from a (subsonic) deflagration to (supersonic) detonation and explosion, this must be a highly non-equilibrium process. Nevertheless, use of thermodynamic equations of states has been a tremendous success in continuum description of propellants and explosive dynamics. In the quest for novel, controlled or accelerated energy-release reactions, such methods have clear limitations- variations at length-scales below the mean-free paths call for explicit atomistic-molecular representation. Opportunely, the adequate methods of quantum chemistry and molecular dynamics have been developed over years. This project objective is to harness the modern theory-modeling methods and high-performance computing in order to gain insights into dynamics of reactive materials and explore rapid energy release processes. The approach to finding novel ways of reaction control and acceleration is by generalizing and extending the eutectics principles to (i) multicomponent mixtures and (ii) beyond equilibrium thermodynamics and towards exothermic chemical reactions. Technical approach relies on large-scale atomistic simulations and quantum chemistry, enabling to screen the possibilities- very large scale (104-106 atoms) simplistic-potentials melting simulations for A1-xBx mix, while keeping an eye on sublimation acceleration; multicomponent A, B, C… systems, with focus on interface solid||gas, sublimation rates as kinetic non-equilibrium metrics. The outcome will include, in addition to generic solid-liquid-gas model behaviors and trends, also understanding of topochemistry and morphology effects on reaction kinetics, with key examples being ammonium perchlorate oxidant or Zn-S propellant. Obtained insights should impact basic understanding and thus offer guidance for novel energy materials design.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Feb 06, 2025
- Source ID
- FA95502410093
Entities
People
- Boris I Yakobson
Organizations
- Air Force Office of Scientific Research
- Rice University
- United States Air Force