Syngas production from methane using AC gliding

arc reactor

Guofeng Xu
School of Chemical Engineering, Dalian University of
Technology,
Dalian Liaoning, PR China
Xinwei Ding
School of Chemical Engineering, Dalian University of
Technology,
Dalian Liaoning, PR China

Abstract AC gliding arc reactor producing syngas (H
2
+CO) for
partial oxidation of methane in an atmospheric gliding arc
discharge has been designed and constructed. In this case, no
catalysts are used to assist reforming; the plasmas play a role as
catalyst and provide the energy for such reactions. The oxygen in
the air is used for the partial oxidation of methane. The methane
conversion and the energy efficiency are within 50 %-87 % and
30 %-48 % for different experiment conditions, respectively.
Characteristics of the gliding arc reactor are influenced by the
ratio of the outer diameter and the inner diameter. When this
value is 0.56, the methane conversion and the energy efficiency
are 87 % and 46 %, respectively, that is much higher than other
experiment conditions. The experiment results show that
hydrogen concentration remains constant when the O
2
/C
increases from 0.8 to 1.2, as the methane conversion is increased.
Keywords- Gliding arc, Syngas, Plasma, partial oxidation
I. INTRODUCTION
When hydrogen (H
2
), as fuel has a very high flame speed,
mixed with other fuels, hydrogen addition increases flame
speed and improves engine combustion stability. Also
hydrogen production plays an important role in the
development fuel cell (FC) technology. At least at short-term
and medium-term, conventional catalytic technology for H
2

production is unable to supply all requirements, because the
major drawbacks for it is relatively low specific productivity,
high metal capacity, sluggish response, and the large size and
weight equipment[1]. During recent years the non-thermal
plasma technology in the production of hydrogen or syngas (a
gas mixture of H
2
and CO) is focused on by the scientific
workers in all countries [2-10]. Non-thermal plasma, special
gliding arc, can overcome the shortcoming of conventional
technology for H
2
production[10, 11]. The plasma way of
hydrogen production has almost no inertia, lower the reaction
temperature, high electivity, and small equipment[12]. The
long-chain reactions of fuel (Methane, CH
4
) conversion and
hydrogen production are produced by the non-thermal plasma
generated active species (electrons, H, OH and O radicals).
Recently, plasma reformers for methane conversion
applications have been investigated by several research
groups. Bromberg researched the low current plasmatron fuel
converted (Gen 2) in which fuels and oxidants are injected
near the electrode gap for syngas production. This 2 l, 3 kg
converter was supplied power ranges in the 50-300 W, in the
partial oxidation mode of operation the reforming efficiency
was around 60-76 %[13]. Kalra et al. reported a new gliding
arc system using a reverse vortex flow for reforming methane.
The experiment results showed plasma energy cost for this
conversion could be as small as 0.66k Wh/m
3
of syngas.
Additionally, the new gliding arc system provided near-perfect
thermal insulation from the reactor wall, indicating that this
system did not require the withstand high-temperature
materials for reactor wall [14]. Rollier et al. studied the
gasoline reforming by non-thermal plasma reactor. They
found that the improvements reactor geometry, such as inner
diameter, converging-diverging nozzle and channel long,
increased the synthesis gas production[15, 16]. Lee and Kim
investigated a three-dimensional version of a typical gliding
arc and noted that non-thermal plasma characteristics of the
rotating gliding arc can be increased by rotating an elongated
arc string and hydrogen selectivity can reach almost 100
%[17]. Horng and Chang developed a plasma fuel converter
for producing a hydrogen rich gas fuel. It consisted of a 100
mm height with a 7.3-29 ml volume and 5mm length arc. The
GAR produced a maximum hydrogen concentration of 48 %
and a hydrogen volume flow rate of 70 ml/min [15, 16].
From the above review, it is clear that different converter
has different performances. The ratio of outer diameter and the
inner diameter of the gliding arc reactor (GAR) should be
maintained in a proper value to keep a good reaction process
in the GAR. One of the reasons is attributed to the
hydrodynamics inside the converter. This paper aims to
improve operation condition and converter geometry for
maximum energy efficiency and methane conversion using the
GAR. This device with low current and high voltage is used to
convert methane into syngas or hydrogen rich gas.
II. EXPERIMENTAL SETUP
A scheme of the experimental setup specially developed
for this application is shown in Figure 1. This experimental
setup allows the reformer feeding with different methane/air
mixture. The main apparatus consists of a gliding arc reactor
(GAR), a power supply, flow controls and measurement
systems. For the GAR, an inner elector, which is connected to
high voltage, is placed inside a circular cylinder that serves as
a ground electrode. The inner electrode and the outer electrode
are made of stainless steel. The narrowest gap distance
between inner and outer electrode is 2 mm to generate the
initial ignition of the arc channel. An AC power supply is used
978-1-4244-6255-1/11/$26.00 2011 IEEE
for the plasma generation. The frequency of the power supply
is 5 kHz and the high voltage is 8 KV. The feed gas is a
mixture of pure methane (99.99% Guangming Co.) and air,
both at ambient temperature. The feed gas is injected
tangentially into the GAR to form a swirling flow field within
the converter. Mass flow controllers (MFCD07-7B) control
the flow rates of methane and air. The dry compositions of the
gaseous products, like methane and oxide products, are
analyzed using a GC (Gas chromatograph, Agilent 1790N-
TCD) which has a TCD detector, the other hydrocarbon and
hydrogen were analyzed by another GC (Agilent 6890N, TCD
and FID). The carrier gases are N
2
for hydrogen and hydrogen
for permanent gas (O
2
, N
2
, CO, CO
2
el at), respectively. The
current and voltage signals are determined by an oscilloscope
(LeCroy LT-332). To verify the effect of the converter outlet
on a fuel reforming performance, the diameter range of the
outlet is from 5mm to 30 mm and the diameter of inner is 30
mm.


Figure 1 Schematic diagram of experimental setup.

III. REACTION PERFORMANCE ASSESSMENT
Methane conversions is defined as
4
4
CH
4
moles of CH consumed
X 100%
moles of CH introduced
= (1)
The hydrogen selectivity and the carbon monoxide
selectivity are, respectively, defined
2
4
H
2
moles of H produced
S 100%
2 moles of CH consumed
=

(2)
4
CO
moles of CO produced
S 100%
moles of CH consumed
= (3)
The specific energy input (SEI, kJ/l) and the energy
efficiency are defined, respectively, as follows:
discharge
TVF
P
SEI
Q
= (4)
H CO H
2 2
CH CH
4 4
(Q Q LHV
100%
P +Q LHV
)

+
(5)
Where Q
TVF
is the total volume flow of the feed of the
converter (l/s), P is the power input of the GAR (kW), Q
H2
is
the volume flow rate of hydrogen (l/s), Q
CO
is the volume flow
rate of carbon monoxide (l/s), LHV
H2
is the lower heating
value of hydrogen (kJ/l).
The conversion rate evaluates the efficiency of methane
decomposition, while information on rich hydrogen gas
production in terms of available energy is given by the energy
efficiency. For energy of the non-thermal GAR, SEI can be
used to effectively estimate the economic evaluation.
IV. RESULTS AND DISCUSSION
A. Influence of O
2
/C ratio
As shown in Figure 2, using the total gas flow rate of 6
l/min, the O
2
/C ratio in terms of the conversions of methane is
investigated. It can be seen in this figure that, as the O
2
/C ratio
increases, the conversion of methane increases. The hydrogen
concentration is slightly increased from O
2
/C=0.8 to
O
2
/C=0.9, and then its reduce. As seen, at the proportion
O
2
/C=1.1 the maximum conversion of methane is 87 % and
the thermal efficiency is 40 %. The O
2
/C ratio has an
important effect on the fuel reforming process in the GAR.
The high O
2
/C ratio is, the more oxygen is held in the same
total flow rate gas and the more heat is produced to improve
the conversion of methane.
Figure 3 show effect the selectivity of hydrogen and
carbon monoxide on the different O
2
/C under P = 80 W and
P= 40 W, respectively. As given in Figure 3, when the input
power is 80 W, the selectivity of hydrogen reduces with
increasing O
2/
C ratio from 0.8 to 1.0. The selectivity of carbon
monoxide increases with increasing O
2
/C at the P = 40 W. For
this GAR, maintain the selectivity of carbon monoxide in the
range 71 %-74 % at the P=80 W. The selectivity of hydrogen
decreases, like shown Figure 3 because of the excess oxygen
reacts with hydrogen and carbon monoxide to form water and
carbon dioxide. As the input power can supply enough energy
to transform fuel, the GAR is heated by the partial oxidation
released heat and its temperature increase. It should be noted
that continuous operation of the GAR resulted in no erosion of
the electrode surface. Partial oxidation of methane in the GAR
completely avoids soot formation, because the soot is not
found in the GAR.
B. Effect of SEI
Figure 4 shows the effect of SEI on the methane
conversion and the hydrogen selectivity. When the other
experiment conditions are fixed, the methane conversion and
the hydrogen selectivity are increase with the increasing SEI.
When the SEI>0.72 kJ/l, however, the methane conversion
and the hydrogen selectivity hold 85% and 45%, respectively.

Figure 2 Conversion of methane and hydrogen concentration for O2/C
under various input power (6 L/min of total volume flow, 10 mm long
and 30 mm inner diameter GAR ).

Figure 3 Selectivity of hydrogen and carbon monoxide ratio for O2/CH4
under various input power.

Figure 4 Effect of the SEI on the methane conversion (--) and the
hydrogen selectivity (--).

Figure 5 Effect of the SEI on the energy efficiency.
The energy efficiency of the GAR is presented in Figure
5 as a function of specific energy input (SEI) input to the
gliding discharge. The energy efficiency rapidly rises with the
SEI due to an increase of the effective input power, but at
SEI>0.7 kJ/l the energy efficiency starts slowly growing
because of CO
2
and water formation. In the range of SEI from
0.75 to 1.1 kJ/l, the energy efficiency holds about 40 %. It is to
be noted that the optimum SEI in the present study is 0.75 kJ/l
for P = 80 W and Q
TVF
= 6 l/min. This test result implies that
the energy efficiency is invalid through only increasing the
input power or reducing the total flow rate, when the
geometrical configuration of the converter plasma is fixed.
There are, in fact, two ways to increase the energy efficiency:
optimization of the converter configuration and conjunction
with the gliding arc and catalyst.
C. The outer geometry of the GAR
Figure 6 shows the effect of the Do/Di on the CH
4

conversion, energy efficiency, and hydrogen selectivity. The
experiment results of the GAR with 10 mm long and 30 mm
inner diameter are shown in the solid line. The Do/Di has a
significant effect on the GAR, which the other parameters,
such as the electric power, current, voltage and the flow rate of
reaction gas, remain constant. As shown in the figure, the CH4
conversion increases with the Do/Di increase and the
maximum conversion locate near the Do/Di = 0.5, and then
the conversion is slowly reduced. The H
2
electivity remains
constant about 45%, when the Do/Di value is from 0 to 1.
When the outer diameter of the GAR is changed from small to
big, the rate of gas rotate is progressively reduced. The high
rate of rotation is too strong in the outside for blowing out the
arc, and this cannot remain rotation steadily. As a result, arc
moves only at the range of low rate of gas rotate. In contrast,
because the low rate of rotation is too weak to blow arc to
rotate around the outer electrode, arc is remained on a fixed
point. The too high or too low rate of rotation degrades
performance of GAR. In the condition of normal charge of
GAR, when the ratio of Do and Di is 0.5 in this experiment,
the GAR has the best performance.

Figure 6 Changes of Do/Di versus energy efficiency, CH4 conversion, and
H2 selectivity.
Figure 6 shows the effect of a on the energy efficiency.
Increasing Do/Di value causes the same effect on energy
efficiency and conversion of methane. The best energy
efficiency equal to 43 % is obtained for Do/Di value around
0.5. When the inner diameter of the GAR is nearly 6 times as
length as the outer diameter, the energy efficiency is 27 % and
the methane conversion is 55 %. Although, the methane
conversion can be increased by the way of the increasing the
power, this method should reduce the energy efficiency and
increase the erosion on the electrodes. More importantly, the
test results strongly prove that the role of the converter
structure is major dominant in the present experiment.
Otherwise, the conversion and selectivity with the same
specific power density and length arc should be similar due to
the similar thermal conditions of the different converter.
Optimizing the structure of the GAR and analyzing
hydrodynamics in the converter are important work in the
future.
V. V CONCLUSION
The performance of a Gliding arc reactor (GAR) for partial
oxidation of methane, like methane conversion, hydrogen
selectivity and energy efficiency, is investigated to use the
GAR with a high voltage, low current. The results show the
GAR is able to generate rich hydrogen gas under stationary
conditions in this paper. The best conversion rates and energy
efficiency are 85 % and 48 %, respectively, at the operating
condition which is power of 80 W, feed supply rate of 6 l/min
and O
2
/C of 0.9. The results show that the geometry of GAR,
especially focused on the outer geometry, affects the
characteristics of the GAR. The ratio of the outer diameter and
the inner diameter should be maintained in a suitable value
(Do/Di=0.5) to guarantee the energy efficiency. The energy
efficiency and hydrogen selectivity values are remarkably
small, which are mainly attributed to generate water and CO
2
.
For improving performance of the GAR, the further work is to
combine plasma with catalyst (Ni) in this experiment system.
At the same time, the hydrodynamics inside the converter is
investigated by mathematical modeling for improving
performance and geometry optimization.
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