Enhanced thermal decomposition of nitromethane on functionalized graphene sheets: Ab initio molecular dynamics simulations

Li Min Liu, Roberto Car, Annabella Selloni, Daniel M. Dabbs, Ilhan A. Aksay, Richard A. Yetter

Research output: Contribution to journalArticle

65 Citations (Scopus)

Abstract

The burning rate of the monopropellant nitromethane (NM) has been observed to increase by adding and dispersing small amounts of functionalized graphene sheets (FGSs) in liquid NM. Until now, no plausible mechanisms for FGSs acting as combustion catalysts have been presented. Here, we report ab initio molecular dynamics simulations showing that carbon vacancy defects within the plane of the FGSs, functionalized with oxygen-containing groups, greatly accelerate the thermal decomposition of NM and its derivatives. This occurs through reaction pathways involving the exchange of protons or oxygens between the oxygen-containing functional groups and NM and its derivatives. FGS initiates and promotes the decomposition of the monopropellant and its derivatives, ultimately forming H2O, CO2, and N2. Concomitantly, oxygen-containing functional groups on the FGSs are consumed and regenerated without significantly changing the FGSs in accordance with experiments indicating that the FGSs are not consumed during combustion.

Original languageEnglish (US)
Pages (from-to)19011-19016
Number of pages6
JournalJournal of the American Chemical Society
Volume134
Issue number46
DOIs
StatePublished - Nov 21 2012

Fingerprint

Graphite
Molecular Dynamics Simulation
Graphene
Molecular dynamics
Pyrolysis
Hot Temperature
Computer simulation
Monopropellants
Oxygen
Derivatives
Functional groups
nitromethane
Vacancies
Protons
Ion exchange
Carbon
Decomposition
Defects
Catalysts
Liquids

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Liu, Li Min ; Car, Roberto ; Selloni, Annabella ; Dabbs, Daniel M. ; Aksay, Ilhan A. ; Yetter, Richard A. / Enhanced thermal decomposition of nitromethane on functionalized graphene sheets : Ab initio molecular dynamics simulations. In: Journal of the American Chemical Society. 2012 ; Vol. 134, No. 46. pp. 19011-19016.
@article{edaedec5bec84a12b9e4f01fff227ca7,
title = "Enhanced thermal decomposition of nitromethane on functionalized graphene sheets: Ab initio molecular dynamics simulations",
abstract = "The burning rate of the monopropellant nitromethane (NM) has been observed to increase by adding and dispersing small amounts of functionalized graphene sheets (FGSs) in liquid NM. Until now, no plausible mechanisms for FGSs acting as combustion catalysts have been presented. Here, we report ab initio molecular dynamics simulations showing that carbon vacancy defects within the plane of the FGSs, functionalized with oxygen-containing groups, greatly accelerate the thermal decomposition of NM and its derivatives. This occurs through reaction pathways involving the exchange of protons or oxygens between the oxygen-containing functional groups and NM and its derivatives. FGS initiates and promotes the decomposition of the monopropellant and its derivatives, ultimately forming H2O, CO2, and N2. Concomitantly, oxygen-containing functional groups on the FGSs are consumed and regenerated without significantly changing the FGSs in accordance with experiments indicating that the FGSs are not consumed during combustion.",
author = "Liu, {Li Min} and Roberto Car and Annabella Selloni and Dabbs, {Daniel M.} and Aksay, {Ilhan A.} and Yetter, {Richard A.}",
year = "2012",
month = "11",
day = "21",
doi = "10.1021/ja3058277",
language = "English (US)",
volume = "134",
pages = "19011--19016",
journal = "Journal of the American Chemical Society",
issn = "0002-7863",
publisher = "American Chemical Society",
number = "46",

}

Enhanced thermal decomposition of nitromethane on functionalized graphene sheets : Ab initio molecular dynamics simulations. / Liu, Li Min; Car, Roberto; Selloni, Annabella; Dabbs, Daniel M.; Aksay, Ilhan A.; Yetter, Richard A.

In: Journal of the American Chemical Society, Vol. 134, No. 46, 21.11.2012, p. 19011-19016.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Enhanced thermal decomposition of nitromethane on functionalized graphene sheets

T2 - Ab initio molecular dynamics simulations

AU - Liu, Li Min

AU - Car, Roberto

AU - Selloni, Annabella

AU - Dabbs, Daniel M.

AU - Aksay, Ilhan A.

AU - Yetter, Richard A.

PY - 2012/11/21

Y1 - 2012/11/21

N2 - The burning rate of the monopropellant nitromethane (NM) has been observed to increase by adding and dispersing small amounts of functionalized graphene sheets (FGSs) in liquid NM. Until now, no plausible mechanisms for FGSs acting as combustion catalysts have been presented. Here, we report ab initio molecular dynamics simulations showing that carbon vacancy defects within the plane of the FGSs, functionalized with oxygen-containing groups, greatly accelerate the thermal decomposition of NM and its derivatives. This occurs through reaction pathways involving the exchange of protons or oxygens between the oxygen-containing functional groups and NM and its derivatives. FGS initiates and promotes the decomposition of the monopropellant and its derivatives, ultimately forming H2O, CO2, and N2. Concomitantly, oxygen-containing functional groups on the FGSs are consumed and regenerated without significantly changing the FGSs in accordance with experiments indicating that the FGSs are not consumed during combustion.

AB - The burning rate of the monopropellant nitromethane (NM) has been observed to increase by adding and dispersing small amounts of functionalized graphene sheets (FGSs) in liquid NM. Until now, no plausible mechanisms for FGSs acting as combustion catalysts have been presented. Here, we report ab initio molecular dynamics simulations showing that carbon vacancy defects within the plane of the FGSs, functionalized with oxygen-containing groups, greatly accelerate the thermal decomposition of NM and its derivatives. This occurs through reaction pathways involving the exchange of protons or oxygens between the oxygen-containing functional groups and NM and its derivatives. FGS initiates and promotes the decomposition of the monopropellant and its derivatives, ultimately forming H2O, CO2, and N2. Concomitantly, oxygen-containing functional groups on the FGSs are consumed and regenerated without significantly changing the FGSs in accordance with experiments indicating that the FGSs are not consumed during combustion.

UR - http://www.scopus.com/inward/record.url?scp=84869483092&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84869483092&partnerID=8YFLogxK

U2 - 10.1021/ja3058277

DO - 10.1021/ja3058277

M3 - Article

C2 - 23101732

AN - SCOPUS:84869483092

VL - 134

SP - 19011

EP - 19016

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 46

ER -