Development of gas-phase reaction mechanism for ammonium perchlorate using quantum mechanics calculations

Tanusree Chatterjee, Stefan T. Thynell

Research output: Contribution to conferencePaper

Abstract

The chemical kinetics involved during the initiation and subsequent reactions of ammonium perchlorate (AP) in gas phase is studied using quantum mechanics (QM) based calculations. In this study, a gas-phase reaction mechanism is formulated where-in several new initiation steps are proposed between NH3 and HOCLO3. The developed reaction mechanism is further compared with existing gas-phase mechanisms developed by Beckstead and his group at Brigham Young University, and additional reactions proposed by Lin and his group at Emory University. Here-in, quantum mechanics calculations were performed using Gaussian 09 program package to identify reaction pathways via transition state theory (TST). Searches for transition states were performed using density functional theory (DFT) and low-level basis-sets such as B3LYP/6-31G(d). Once a transition state with a single negative frequency was identified, intrinsic reaction coordinate (IRC) calculations were then performed to link the reactants to the products. Higher level calculations were then performed using the compound method G4(MP2) to compute the thermodynamic properties of species at equilibrium or at transition states. This work elucidates how QM can contribute to further our understanding of the complex chemical kinetics involved during the decomposition of AP in the gas phase.

Original languageEnglish (US)
StatePublished - Jan 1 2018
Event2018 Spring Technical Meeting of the Eastern States Section of the Combustion Institute, ESSCI 2018 - State College, United States
Duration: Mar 4 2018Mar 7 2018

Other

Other2018 Spring Technical Meeting of the Eastern States Section of the Combustion Institute, ESSCI 2018
CountryUnited States
CityState College
Period3/4/183/7/18

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All Science Journal Classification (ASJC) codes

  • Mechanical Engineering
  • Physical and Theoretical Chemistry
  • Chemical Engineering(all)

Cite this

Chatterjee, T., & Thynell, S. T. (2018). Development of gas-phase reaction mechanism for ammonium perchlorate using quantum mechanics calculations. Paper presented at 2018 Spring Technical Meeting of the Eastern States Section of the Combustion Institute, ESSCI 2018, State College, United States.