Sooting Behavior of Propane and n-butane in a Micro Flow Reactor with a Controlled Temperature Profile

DUBEY, Ajit Kumar*, Institute of Fluid Science, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, 980-8577, JAPAN
TEZUKA, Takuya, Institute of Fluid Science, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, 980-8577, JAPAN
HASEGAWA, Susumu, Institute of Fluid Science, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, 980-8577, JAPAN
NAKAMURA, Hisashi, Institute of Fluid Science, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, 980-8577, JAPAN
MARUTA, Kaoru, Institute of Fluid Science, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, 980-8577, JAPAN
Abstract: Sooting behavior of propane and n-butane were studied using a micro flow reactor with a controlled temperature profile where maximum
temperature was 1300 K. Effect of equivalence ratio at mean inlet velocity of 10 cm/s on flame and soot response was studied for both fuels. Four kinds of
responses are observed namely, FREI (Flame with repetitive extinction and ignition), flame, flame + soot, and soot. Critical sooting equivalence ratio
(equivalence ratio at which soot is first observed) for propane is lower than that for n-butane, indicating that propane is more sooting than n-butane which is
in contrast to earlier results. Steady state computations were performed for both fuels to understand underlying chemistry. Experimental flame positions for
rich flames were compared with computational maximum heat release rate positions and the agreement is better for n-butane than propane. Relationship
between computational PAH mole fraction profile and experimentally observed soot was studied qualitatively. (150 words)

Keywords: Sooting behavior, Propane, n-butane, Micro flow reactor with a controlled temperature profile
1. Introduction
Propane and n-butane form major component of LPG which has
widespread applications. Soot formation occurs at fuel rich
conditions and is undesirable from efficiency and maintenance
considerations in combustion devices. It is also a concern for
environment and human health. Hence it is important to study soot
formation in these widely used fuels. Sooting tendency of these fuels
are studied [13] and it is found that n-butane is more sooting than
propane. To study the effect of fuel structure on sooting behavior the
temperature and pressure must be well controlled.
In this work sooting behavior of propane and n-butane is studied
using a micro flow reactor with a controlled temperature profile [4,
5]. A micro flow reactor is a simple device which can be used to
study effects of fuel structure on oxidation characteristics as the
given temperature profile and pressure can be invariant across
experiments. In earlier works the micro flow reactor has been
applied to study sooting behavior of acetylene [4] and C-16 isomers
(n-cetane and iso-cetane) [5].
2. Experimental setup
The micro flow reactor setup shown in Fig. 1 employs a quartz
tube whose inner diameter is 2 mm which is less than ordinary
quenching diameter for fuels at standard state. The reactor tube is
heated externally using a premixed hydrogen-air flat flame
burner which creates a stationary temperature profile with
b
maximum temperature of 1300 K along the inner wall of
reactor tube. The temperature is measured using a K-type
c
thermocouple by inserting it from exit of the reactor. Direct
d
images are captured by a digital still camera, Nikon D-300.
Fuel and air are supplied to the reactor through separate mass
flow controller and are mixed before entering in the reactor.

3. Computational method
Flow in the micro flow reactor is modeled as one-dimensional,
atmospheric, premixed, steady and reactive flow field.
Computations are performed using CHEMKIN-PRO where
convective heat transfer between gas and reactor wall is added in the
energy equation.

dT 1 d dT A K
dT A K
A 4Nu
M

Y
V
C
k hkWk
(Tw T ) 0

k
k
pk

dx C p dx dx C p k 1
dx C p k 1
Cp d 2
In above equation, Nu = 4, d = 2 mm and Tw is derived from
experimental temperature profile. A detailed PAH formation
mechanism proposed by Wang et al. [6] is used to compute
chemistry.
4. Results and discussion
Experiments are performed for propane and n-butane at
equivalence ratio (1.54.5) and mean inlet velocity of 10 cm/s. Four
kinds of soot and flame responses were observed namely FREI
(flame with repetitive extinction and ignition), flame, flame + soot
(soot is observed downstream of flame) and soot. Representative
images for flame and soot response are shown in Fig. 2.

Fig. 2 Representative images for flame and soot responses at mean

inlet velocity of 10 cm/s (a) FREI (n-butane, = 1.6) (b) Flame
(propane, = 1.7) (c) Flame + Soot (propane, = 1.9) (d) Soot
(propane, = 4).
Flame and soot responses for propane and n-butane are shown for
the experimental range in Fig. 3. Propane shows four and n-butane
shows three different kinds of soot and flame response.
The equivalence ratio at which soot is first observed is termed
critical sooting equivalence ratio. Critical sooting equivalence ratio
of propane, 1.9, is lower than that of n-butane, 2.4. This is in contrast
to earlier observed results [1-3] where n-butane is found to be more
sooting than propane. The maximum flame temperature in earlier
experiments are more than 1600 K. In current experiments the

Fig. 1 Micro flow reactor setup.

maximum temperature is 1300 K. So, the difference in order of

sooting tendency can be due to lower temperature.

Figure 5 shows experimental flame position and computational heat

release rate profile for n-butane at equivalence ratio of 2.2. The
difference between wall temperature at experimental flame position
and maxima of computational heat release rate is 6 K. The used
mechanism fares well for n-butane compared to propane.

Fig. 3 Soot and flame response for propane and n-butane.

In experiments, soot is first observed downstream of a flame. The
first soot particles are formed by nucleation from higher PAHs
(Polycyclic Aromatic Hydrocarbon). The computational flame
structure reveals that the precursors for PAH formation start to form
just downstream of flame. So, the flame position in experiments are
important attributes of sooting flames and give information about
position where PAH production starts. Figure 4 shows experimental
flame and computational heat release profile for propane at
equivalence ratio of 1.7 and mean inlet velocity of 10 cm/s. The
agreement between experimental flame position and maximum heat
release rate position is not so good. The difference in wall
temperature at experimental flame and wall temperature at
computational maximum heat release rate is more than 100 K.

Fig. 4 Experimental flame and computational heat release rate

profile for propane at equivalence ratio of 1.7 and mean inlet
velocity of 10 cm/s.

Fig. 6 Experimental flame and soot image and computational heat

release rate and A4 (Pyrene) mole fraction profile.
Figure 6 shows experimental image and computational heat release
rate and mole fraction of pyrene (A4) for n-butane at equivalence
ratio of 4.0 and mean inlet velocity, 10 cm/s. The wall temperature
at experimental flame position agrees within 2 K with computational
maximum heat release rate. The agreement of flame position
improves with increasing equivalence ratio. In principle, soot
nucleation can start with any PAH higher than A4 but in current
computations A4 mole fractions are much higher than other higher
PAHs combined. Therefore, the mole fraction profile of A4 is
similar to that of sum of all higher PAHs. The computed mole
fraction of A4 at the experimentally observed upstream edge of soot
is 510-6, which gives an approximate concentration of higher PAHs
required to form first soot particle at temperature of 1300 K.
4. Conclusions
Sooting behavior of propane and n-butane was studied using a
micro flow reactor with a controlled temperature profile with
maximum temperature of 1300 K.
Critical sooting equivalence ratio for propane was lower than that
of n-butane.
Used chemical mechanism compares well with n-butane but not
with propane flames.
The computed mole fraction of pyrene at the upstream edge of
soot was expected to be the order of a ppm.
Acknowledgements
This work was partially supported by Council for Science,
Technology and Innovation (CSTI), Cross-ministerial Strategic
Innovation Promotion Program (SIP), Innovative Combustion
Technology (Funding agency: JST).

Fig. 5 Experimental flame and computational heat release rate

profile for n-butane at equivalence ratio of 2.2 and mean inlet
velocity of 10 cm/s

References
1. Glassman, I., Sympo. (Int.) on Combust. 22:295-311(1988).
2. Olson, D.B., Pickens, J.C., Combust. Flame 57:199-208(1984).
3. Calcote, H.F., Manos, D.B., Combust. Flame 49: 289-304
(1983).
4. Nakamura, H., Tanimoto, R., Tezuka, T., Hasegawa, S., Maruta,
K., Combust. Flame 161: 582-591( 2014).
5. Nakamura, H., Suzuki, S., Tezuka, T., Hasegawa, S., Maruta, K.,
Proc. Combust. Inst., 35 (3): 3397-3404 (2014).
6. Wang, Y., Raj, A., Chung, S. H., Combust. Flame 160:16671676 (2013).