TY - JOUR
T1 - Effect of nanostructure, oxidative pressure and extent of oxidation on model carbon reactivity
AU - Jaramillo, Isabel C.
AU - Gaddam, Chethan K.
AU - Vander Wal, Randy L.
AU - Lighty, Jo Ann S.
N1 - Funding Information:
The authors acknowledge support by the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy under Award Number 10016259 . This material is based upon work while Dr. Lighty served at the National Science Foundation. Any opinions, findings, and conclusions expressed in this publication are those of the authors and do not necessarily reflect the views of the National Science Foundation. The authors thank Joseph D. Levinthal at the University of Utah for providing some of the samples.
Publisher Copyright:
© 2014 The Combustion Institute.
PY - 2015/5/1
Y1 - 2015/5/1
N2 - Oxidation kinetics and fringe analysis studies of three "model" carbons, ranging from fullerenic to onion-like nanostructures and a reference diesel soot were performed in a thermogravimetric analyzer. The samples were oxidized isothermally at temperatures ranging from 575 to 775. °C in air. Multiple tests were performed to obtain the most favorable operating conditions to minimize mass-transfer diffusion limitations in the experiments.First-order reaction kinetics and an Arrhenius-type equation were used to extract the rate constants at each temperature. The activation energies for the oxidation of the carbon samples ranges from 124 to 204. kJ/mol, and it was approximately 140. kJ/mol for the reference diesel soot sample. The onion-like structure exhibited a slower kinetic rate compared to the other carbons. Similar kinetic parameters were found for "intermediate structure" model carbon and reference diesel soot.Fringe analysis explained the differences in the kinetic parameters between carbon samples studied. The onion-like carbon "nascent" sample had a broader range of lamellae length with smaller tortuosity distribution, suggesting stacking; the "nascent" fullerenic carbon had much shorter mean lamella length distribution and broader tortuosity, suggesting more curvature. Nanostructure metrics of the reference diesel soot and intermediate model carbon were between the other two carbons. Results confirm a structure-property relationship between oxidative reactivity with carbon nanostructure.
AB - Oxidation kinetics and fringe analysis studies of three "model" carbons, ranging from fullerenic to onion-like nanostructures and a reference diesel soot were performed in a thermogravimetric analyzer. The samples were oxidized isothermally at temperatures ranging from 575 to 775. °C in air. Multiple tests were performed to obtain the most favorable operating conditions to minimize mass-transfer diffusion limitations in the experiments.First-order reaction kinetics and an Arrhenius-type equation were used to extract the rate constants at each temperature. The activation energies for the oxidation of the carbon samples ranges from 124 to 204. kJ/mol, and it was approximately 140. kJ/mol for the reference diesel soot sample. The onion-like structure exhibited a slower kinetic rate compared to the other carbons. Similar kinetic parameters were found for "intermediate structure" model carbon and reference diesel soot.Fringe analysis explained the differences in the kinetic parameters between carbon samples studied. The onion-like carbon "nascent" sample had a broader range of lamellae length with smaller tortuosity distribution, suggesting stacking; the "nascent" fullerenic carbon had much shorter mean lamella length distribution and broader tortuosity, suggesting more curvature. Nanostructure metrics of the reference diesel soot and intermediate model carbon were between the other two carbons. Results confirm a structure-property relationship between oxidative reactivity with carbon nanostructure.
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U2 - 10.1016/j.combustflame.2014.12.006
DO - 10.1016/j.combustflame.2014.12.006
M3 - Article
AN - SCOPUS:84938744747
SN - 0010-2180
VL - 162
SP - 1848
EP - 1856
JO - Combustion and Flame
JF - Combustion and Flame
IS - 5
ER -