Introduction
The use of diesel vehicles is constantly increasing
mainly due to their inherent advantages, which in-
clude fuel economy, durability, driveability, etc. [1].
The main issue concerning their use are the increased
nitrogen oxides (NO
x
) and particulate matter emis-
sions (PM) [2]. Specifically, diesel PM represents an
important health hazard a fact that has led the legisla-
tion to adopt stringent emission standards. Diesel par-
ticulate filters (DPF) are becoming wide spread as an
effective measure to reduce PM emissions from diesel
vehicles as they have filtration efficiencies close to
100% [3]. Due to the fuel penalty induced by the
gradual loading of the filter, its periodical regenera-
tion, i.e. the combustion of the accumulated
particulates, is necessary [3]. It is therefore vital to
fully understand, model and control the regeneration
process in order to optimize the application and oper-
ation of DPFs both for lifetime durability and fuel
economy purposes. Consequently, the study of soot
combustion for the extraction of kinetic data that can
be coupled in modelling tools is very important. Dif-
ferent experimental approaches have been used in the
literature including thermogravimetric analysis (TG)
[4–13], flow and bed reactors, etc. [14, 15].
When TG is used for the extraction of chemical
kinetics data it has known experimental and computa-
tional difficulties that include control of the reactant
atmosphere [16], rate-controlling mass and heat trans-
fer limitations [7, 8] as well as the choice of the opti-
mal calculation method of the kinetic parame-
ters, e.g. [17], which have led to extended debating
about the reliability of its results. However, although
TG cannot substitute in situ experiments, it is still an
important experimental tool that has been used exten-
sively for soot and carbon oxidation studies
[e.g. 10, 13, 18], mainly because it represents a fast,
economical and easy to use experimental solution.
Although it is common to run non-isothermal TG
using the same reaction gas throughout soot oxidation
[6, 13], also a number of isothermal studies of soot re-
activity are found in literature [4, 5, 7]. Non-isother-
mal protocols are preferred because isothermal exper-
iments necessitate more experimental time and more
sample mass, while identical experimental conditions
and homogeneous sample are also necessary. Also, in
the case of exothermal reactions, such as soot oxida-
tion, self-heating of the sample may occur leading to
deviation from the desired isothermal conditions.
However, the temperature gradients within the sam-
ple are often neglected. This can be justified for
smaller initial sample masses [7] and/or slower reac-
tion [19], e.g. at lower O
2
concentration. Then the de-
coupling of the effect of temperature and progress of
reaction on the reaction rate and rate constant is possi-
ble. Finally and despite the above mentioned limita-
tions, isothermal studies are considered generally
better for determining kinetic rates [18] while they
also facilitate the investigation and modelling of
reaction gas diffusion in the solid sample.
1388–6150/$20.00 Akadémiai Kiadó, Budapest, Hungary
© 2008 Akadémiai Kiadó, Budapest Springer, Dordrecht, The Netherlands
Journal of Thermal Analysis and Calorimetry, Vol. 95 (2009) 1, 141–147
ISOTHERMAL SOOT OXIDATION EXPERIMENTS WITH
INTERMEDIATE GAS CHANGE IN A PERKIN-ELMER TGA6
Maria Kalogirou, P. Pistikopoulos, L. Ntziachristos and Z. Samaras
*
Laboratory of Applied Thermodynamics, Mechanical Engineering Department, Aristotle University Thessaloniki, P.O. Box 458
GR 541 24 Thessaloniki, Greece
Two isothermal soot oxidation protocols were tested in a Perkin–Elmer TGA6: (1) the sample was heated under N
2
and then the re-
action gas was introduced and (2) the sample was introduced after the empty furnace was heated under the reaction gas. The first
protocol is common in soot oxidation studies, it gives a measure of the volatiles and is easier to handle, but as it is shown the deter-
mined reaction rate may be falsified by the O
2
concentration. Using gas analysis it was found that ~2000 s are necessary for the
complete gas change in the instrument. An instrument specific correction function involving the O
2
concentration and reaction order
n with respect to O
2
was developed which allowed the correlation of the rates measured with both protocols.
Keywords: evolved gas analysis, isothermal, oxidation, soot, TG
* Author for correspondence: zisis@auth.gr