INSTITUTE OF PHYSICS PUBLISHING JOURNAL OF PHYSICS D: APPLIED PHYSICS

J. Phys. D: Appl. Phys. 34 (2001) 2798–2803 PII: S0022-3727(01)23229-X

Syngas production via methane steam

reforming with oxygen: plasma reactors
versus chemical reactors
Jean Marie Cormier1 and Iulian Rusu2
1
GREMI, Université d’Orléans, 14 rue d’Issoudun, BP 6744-45067, Orléans Cedex 2, France
2
Faculty of Industrial Chemistry, Technical University ‘Gh Asachi’,
Bd Dimitrie Mangeron 71, Iasi 6600, Romania
E-mail: jean-marie.cormier@univ-orleans.fr

Received 22 March 2001, in final form 8 July 2001

Published 5 September 2001
Online at stacks.iop.org/JPhysD/34/2798

Abstract
Steam reforming with oxygen (SRO) is a combination of non-catalytic
partial oxidation and steam reforming of methane, industrially used for
syngas production. There are several models of the chemical reactors used
for this purpose but in the last decade a new direction has
developed—plasma devices. The aim of the present paper is to make a
comparative analysis between the autothermal reformers, including their
improved variants, and the plasma reactors. The study is conceived in terms
of advantages and disadvantages coming from the exploitation parameters,
methane conversion, selectivity, energy efficiency and investment costs.
Although SRO by means of chemical reactors may be the most efficient,
plasma reactors represent an incisive approach by their simplicity,
compactness and low price.

1. Introduction production of hydrogen for automotive applications [1, 2].

Synthesis gas or syngas is a mixture of hydrogen and carbon
monoxide used as a major intermediary for the production of
pure hydrogen or other chemical compounds. Among these
we have to mention ammonia with its inestimable utility for
industry and agriculture and the liquid products derived by
the process known as SCL (syngas conversion to liquids) (e.g.
methanol and other alcohols, solvents, diesel fuel, jet fuel,
gasoline, etc).
The growing demand for chemicals derived from syngas
has led to the development of several technologies (e.g.
Fischer–Tropsch synthesis, NH3 or oxygenate production).
These processes are of strategic importance for any country.
For example, the synthesis developed by Fischer and Tropsch
was used by the Germans during the Second World War to
produce fuel from coal. South Africa also produced fuel this
way during the political sanctions against the apartheid regime.
Today, as the fuels obtained from syngas do not contain sulphur
or nitrogen compounds, their combustion in engines leads to
reduced environmental pollution. Hydrogen itself was taken
into account in the last period as a clean fuel, important steps
being made in the research in recent years on the on-board
Syngas is also the main source of carbon monoxide, which
is used in an expanding list of carbonylation reactions.
Originally, coal was the primary source of carbon for
syngas, but today natural gas has replaced it for economic
reasons. Despite the fact that coal reserves are large and
the price of coal is lower than that of the hydrocarbons, the
investment in a coal-based syngas plant is about three times
higher than that required for a natural-gas-based plant [3].
However, there are also technologies producing syngas from
petroleum coke, heavy residuals and even biomasses [4, 5].
Natural gas can be processed by several methods, e.g.
partial oxidation with oxygen (PO), steam reforming (SR),
steam reforming with oxygen (SRO), CO2 reforming (CDR)
and CO2 reforming with oxygen (CDRO) [6]. One of the
most attractive technologies seems to be the SRO, which is
also known as autothermal reforming. The main reasons for
recommending this technology over the other variants are the
low energy requirements, the high space velocity (at least one
order of magnitude relative to traditional SR), a lower process
temperature than PO and the H2 /CO ratio is easily regulated
by the inlet gas ratio [7–9]. The process can be performed by
means of various reactor models including plasma reactors.

0022-3727/01/182798+06$30.00 © 2001 IOP Publishing Ltd Printed in the UK 2798


If syngas processing is of strategic importance, research
regarding the use of plasma reactors has also become strategic
for different countries. For example, Germany, Japan and the
USA employ large funding regarding automotive applications
of plasma reactors. The Russian Federal R&D programme
in the field of hydrogen energy and technology for the period
1994–96 also included in the eight most promising processes
for the production and use of hydrogen two concerning plasma-
chemical technologies [10].
Therefore, the aim of the present paper is to make a
comparative analysis of the chemical and plasma reactors used
for SRO, in order to estimate the real prospects for plasma
processes in this field.
2. Syngas production by SRO
SRO is a combination of non-catalytic partial oxidation and
steam reforming developed by Haldor Topsøe in the late 1950s
in order to perform reforming in a single reactor [9]. There
are probably five main chemical reactions in the reforming
process:
CH4 + H2 O ⇔ CO + 3H2
H298 = 206 kJ (1)
CH4 + 2H2 O ⇔ CO2 + 4H2
H298 = 164.9 kJ (2)
CH4 + O2 ⇔ CO2 + 2H2
H298 = −318.9 kJ (3)
2CH4 + O2 ⇔ 2CO + 4H2
H298 = −71.8 kJ (4)
CO + H2 O ⇔ CO2 + H2
H298 = −41 kJ. (5)
Partial oxidation is an exothermic process, while steam
reforming is endothermic. The thermal energy generated by
the former can be adjusted by its molar air/methane ratio
so that the overall autothermal process can be carried out
without an extra external heat source for the SR process.
Classic thermodynamic analysis performed by Chan and Wang
[11] indicated that the optimal operating regime is with an
air/methane molar ratio of 3.5 and a 2.5 to 4 water/methane
molar ratio. Under these operating conditions, the number
of moles of hydrogen per mole of natural gas consumed is
2.19–2.22. The results also showed that under these conditions,
the solid carbon is suppressed, the mole fraction of CO ranges
from 2.24–4.38%, the methane conversion rate is 99.04–
99.45% and the operating temperature is between 820 and
871 K.
Taking into account the use of plasma reactors, Bromberg
and co-workers [12] have simulated the homogeneous SRO
process (CH4 + 0.5O2 + 1.88N2 + H2 O) by means of non-
equilibrium thermodynamics [13]. This method has been used
to determine the reaction trajectory in an adiabatic reactor.
The calculations performed for initial temperatures of 500,
1500 and 2000 K indicate that the reaction is characterized
by two distinct stages. During the first stage, complete
combustion of part of the methane occurs, producing mainly
CO2 and water, increasing the temperature of the system. In the
second stage, the remaining methane reacts with CO2 and H2 O
producing syngas and decreasing the system’s temperature.
The calculated rate of methane conversion ranged between 97.5
and 100%, leading to a final hydrogen mole fraction of about
35% and for the CO 8–16%.
Syngas production with SRO: plasmas or chemicals
However, since a plasma is a mixture of electrons, highly
excited atoms and molecules, ions, radicals, photons, etc, the
chemistry is very complex and the present understanding of
it is quite limited. It is difficult to predict theoretically the
final products and their concentration. Unfortunately, most
practical achievements are based on experiments.
3. Other methods of syngas production
There is an entire literature concerning the chemical
technologies used or proposed for syngas production.
Therefore, in this section we shall briefly summarize only
reports on syngas production by means of plasma methods.
The plasmatron experiments performed at Michigan
Institute of Technology (MIT) on the PO of methane revealed
that for energy inputs of less than 25 MJ kg−1 CH4 , hydrogen
output reaches 38% of equilibrium levels and the CO output
is 65% of equilibrium [14]. In these conditions the resulting
energy cost was as high as 267 MJ kg−1 H2 because most of
the hydrogen turns into water. Czernichowski et al used a
gliding arc installation for this process with a similar energy
cost [15–17].
Chapelle et al have used a classic gliding arc reactor
for syngas generation by SR [18]. For an electric power of
1.4 kW and a steam-to-methane ratio of 2–4, the maximum
CH4 conversion was 44%, with an output energy efficiency of
33% at an energy cost of about 97 MJ kg−1 H2 .
CDR is currently of great interest both for the
transformation of natural gas and for environmental control.
Chapelle et al [18] has performed the reaction in both
transferred arc and gliding arc reactors. In the first case the
hydrogen concentration in the exit gases decreased from 48
to 22% for a CO2 /CH4 ratio increasing from 0.5 to 2. The
necessary energy for the production of 1 kg of hydrogen
was of 234 MJ, corresponding to an energy efficiency of
about 27%. In the second case the energy cost decreased to
226 MJ kg−1 H2 , with an energy efficiency of about 31%. The
same reaction was performed by means of glow discharges,
micro-arc plasmas and dielectric-barrier discharges, but with
low energy efficiency [19, 20].
The advantage of oxygen addition in the CDRO process
is the supply of additional energy for methane conversion, due
to a parallel reaction of methane oxidation. Laboratory-scale
experiments gave 100% conversion but at a very high energy
expenditure (190–270 MJ kg−1 H2 ), the energy efficiency
ranging between 23 and 42% [17]. In order to promote an
efficient reforming process, Fridman’s team has used a pulsed
corona discharge reactor with preheating of the inlet gases at
about 900 ◦ C [21]. They succeeded in lowering the plasma
energy cost to 34 MJ kg−1 H2 . However, the energy spent for
preheating the mixture was about 340 MJ kg−1 H2 .
The literature also presents results regarding the use of
thermal plasmas for syngas production starting from gasoline
and diesel fuel, biofuels (canola and corn oil) and even used
tires [22, 23].
4. Chemical reactors
The reformer basically consists of a ceramic lined tube and
a Ni-based fixed catalyst bed for equilibration of the gas
2799
J M Cormier and I Rusu
(figure 1(a)). The preheated feed streams (CH4 + H2 O and
H2 O + O2 ) are mixed in a burner placed at the top where partial
oxidation of the methane occurs. The final steam reforming
takes place in the catalyst bed below the burner. Typically, the
SRO reactor operates at about 2200 K in the combustion zone
and 1200–1400 K in the catalytic zone. Operating pressures
range from 12 to 70 atm. Tests carried out on fixed bed reactors
revealed that one of the most important features concerns the
adiabatic working conditions. Methane conversions up to 90%
with residence times of up to 0.1 s have been found.
Exxon developed a fluidized-bed system in which the
CH4 /H2 O mixture is fed to the bottom of the reactor and
oxygen is fed into the middle of a fluidized bed of catalyst
(figure 1(b)). The fluidized bed offers the advantage of an
optimal temperature distribution, with the absence of radial
and axial gradients and a lower pressure drop with respect to a
fixed bed operating at the same dimension and space velocity.
The usual catalyst is a Ni catalyst supported on a refractory
material containing a variety of promoters. The additives are
potassium and/or calcium alkali ions, which mainly serve to
suppress excessive carbon deposit on the catalyst [24]. Recent
studies show that catalysts based on noble metals seem to be
more active for SRO [7, 25].
There are several studies presenting comparisons between
different processes of syngas synthesis and the implied
economics [9, 26–30]. The basis of comparisons rested
mainly on four points: raw material consumption, energy
consumption and energy recovery, investments and operational
costs. The conclusion that one can draw from these studies is
that autothermal reforming improves the steam reforming cost
by 10–20%. This means that the investment varies between
750 and 900 euro per N m3 h−1 and a final hydrogen cost of
0.05–0.08 euro per Nm3 .
The shortcomings of the chemical autothermal reformers
concern size, the large investments, the limitations on rapid
response, the extreme operating conditions that limit the
lifetime of a reactor, heat management (during the front end
of the catalyst bed as the methane undergoes total oxidation),
safety and operability.
Possible improvements of the SRO include the use
of membrane technology, the achievement of integrated
autothermal reforming/fuel cell systems and periodically
operated fluidized bed reactors.
Conventional SRO often leads to low hydrogen yield since
the formed H2 may react with oxygen to yield water. To avoid
this problem several authors have proposed a periodic system
with a feed composition alternating between CH4 /O2 and
CH4 /H2 O mixtures [31–33]. It was envisaged that this would
promote independent methane oxidation and steam reforming
steps, and thus minimize hydrogen reconversion. The results
indicate that under periodic cycling, SRO proceeds via the
interaction of entities derived from the dissociative adsorption
of CH4 and H2 O leading predominantly to CO2 and H2 .
A membrane reactor combines the separation properties
of a membrane with the performance of a catalytic system
(figure 1(c)). The combined efforts of Amoco, BP Chemicals,
Praxair, Sasol and Statoil developed an innovative technology,
named OTM (oxygen transport membrane) that can convert
natural gas to syngas with very high selectivity [7]. In this
process, a ceramic perovskite type membrane permits SRO
2800
with separation of oxygen. Air and methane are introduced
into opposite sides of the membrane, the oxygen dissociated
into ions diffuses through the membrane reacting with methane
to give oxidation products.
Air Products, the US Department of Energy, Ceramatec
and other partners have developed a similar reactor technology
[34, 35]. The laboratory-scale apparatus has operated with
methane at 7–30 atm and an air feed to the interior membrane
at atmospheric pressure. In the second phase, an engineering
process development unit will test subscale membranes under
full operating conditions at a nominal 700 m3 per day.
The weak point of the membrane reactors is the mass
transfer, which is limited if the membrane does not have
sufficient flux to satisfy the productivity of the catalyst. Other
practical issues, such as membrane pore blockage and thermal
and mechanical stability have limited for the moment the
usefulness of these systems.
Variants of the membrane reactors are the solid oxide
fuel cells (SOFC) and, in the last decade, there has been
an increased interest in the use of SOFC to produce H2
[1, 36, 37]. The membrane in this case is also an electrode (the
anode), made of porous carbon plates laced with a catalyst.
The hydrogen combines with HO− ions to produce water
vapour and electric power. Therefore, the chemical energy
is converted directly into electricity. On the anode side, the
natural gas is first ejected into a reforming chamber where it
draws waste thermal energy from the stack and is converted
into H2 and CO. It then flows into the anode manifold where
most of the H2 and CO is oxidized. This gas stream is then
partly recycled to the reforming chamber where the resulting
water is used as a reagent. On the cathode side, air is first
blown into a heat exchanger where it reaches nearly operating
temperature. The air is brought up to the operating temperature
by combustion of the remaining H2 and CO from the anode.
The oxygen in the cathode manifold is converted into an
oxygen ion that travels back to the anode. For hydrogen users,
the CO can be converted by the established mode into CO2 and
H2 using a shift reactor followed by CO2 separation.
For a cell voltage ranging between 0.5 and 0.8 V, the
thermodynamic calculations show an efficiency of electricity
and hydrogen generation of about 80% [37]. The system
is simple, efficient, tolerant to impurities and uses cheap
catalysts. Due to the high operating temperatures air
compression is not required. Another advantage is that both
hydrogen and CO are used in the cell. While in other cases,
CO is a poison, in SOFC it is a fuel. Moreover, SOFCs can
provide an effective energy conversion system even for small-
scale plants.
Tanaka et al [38] have designed a combined cycle system
with a solid oxide fuel cell and gas turbine. According to
their economic calculations the total electricity generation
efficiency can rise up to 60–70%. The gas turbine accounts for
the greatest investment input (35%), with the next highest being
the fuel cell module (including the reformer—23%), followed
by the heat exchanger (20%). Although the unit investment
cost is higher than that for a large-scale coal power plant it can
still be considered as a competitive alternative for urban areas.
However, a cheaper reformer would decrease the investment
costs.
Among the disadvantages we have to mention that the
SOFCs run at temperatures of 800–1000 ◦ C and, therefore,
 Syngas production with SRO: plasmas or chemicals

CH4 + H2O H2O + O2 Syngas Exhaust

Syngas

Burner Cyclone

Membrane
O2
Catalyst
bed
Catalyst Fluidised
bed bed

Syngas CH4 + H2O

Reactants

(a) (b) (c)

Figure 1. Different kinds of chemical reformers.

Cathode (2)
W/2
Insulator
Air W

Anode
Cooling water W/2

(1) (4)
(3)
Cooling water
Figure 3. Diagram of a microwave plasmatron.

Reactants
Syngas
Figure 2. Diagram of a thermal plasma reactor.
several minutes of fuel burning is required to reach operating
temperature. This delay is considered to be a shortcoming for
automotive applications. However, most of the cells generate
H2 at 1 atm or less and for bulk production this will then require
higher compression to apply the chemical technology [24].
5. Plasma reactors
Depending on their energy, temperature and ionic density,
plasmas are usually classified as either thermal plasmas
or non-thermal (non-equilibrium) plasmas. Generally, the
plasma used for chemical applications is required to provide a
high operating power together with a very selective energy
input while simultaneously maintaining a non-equilibrium
condition [15].
Thermal plasma reactors (plasmatrons) have different con-
structive variants (induction, DC and microwave plasmatrons)
[18, 39]. Basically, the plasmatron comprises two water-
cooled metallic tubular electrodes (figure 2). A spark occurs
in the gap between the electrodes, and the incoming feedstock
gas blows the arc into the arc chamber. The working gas can
be injected directly or tangentially into the gap between elec-
trodes. Applying an external magnetic field can enhance the
gas rotation. The electrodes are usually made of copper but it
is possible to use some new improved alloys, such as beryllium
bronze and tungsten–copper–nickel.
The SRO reaction performed by Bromberg and his team
[40] by the means of a plasmatron, without a catalyst, resulted
in a hydrogen yield of 40% (defined as the ratio of hydrogen
released to hydrogen content in methane) for an input power
of 3.5 kW. At low values of input power, the homogeneous
plasma process resulted in low methane conversions (about
40%). The device’s productivity was about 4000 m3 h−1 H2
per cubic metre of reactor. The minimum power consumption
without heat recovery was about 100 MJ kg−1 H2 .
Furthermore, in order to decrease this specific power
consumption a nickel-based catalyst on an alumina support
was used through. The hydrogen yield increased by up to
80%, for an input power of 2.7 kW and a methane conversion
rate of 70%. The plasma composition of the reformate was
of 35%H2 , 5%CH4 , 3.7%CO, 15%CO2 , 41%N2 and traces of
C2 hydrocarbons. The required specific energy was reduced
to less than 17 MJ kg−1 H2 . The productivity also increased
to about 10 000 m3 h−1 H2 per cubic metre of reactor.
The main drawback of using thermal plasmas is the
overheating of the reaction media, when the reagents in all

2801
J M Cormier and I Rusu
V1
C a tho d e
D isc ha rge s
T°
M ea su re
G a s inle t
Figure 4. Diagram of a three-discharge glidarc reactor.
Table 1. Comparative data for SRO reactors.
Investment cost
(euro/Nm3 h−1 H2 )
Chemical reactors 750–900
Plasma reactors 65
degrees of freedom uniformly consume energy. It is the high
electron temperature that determines the reaction evolution in
non-thermal plasmas, while the gas temperature can remain as
low as room temperature. Non-thermal plasmas have several
types if discharge: glow, corona, dielectric barrier, microwave,
radiofrequency and gliding arc [41, 42].
The microwave discharge operates at very high
frequencies, with which only light electrons can follow the
oscillations of the electric field. Therefore, this discharge is far
from local thermodynamic equilibrium and has the advantage
that it can be used in a wide pressure range.
The electron temperatures in a microwave discharge are
mainly defined by the electric field (Eel ) in the discharge and
by the pressure (P ); however the maximization of the Eel /P
ratio at the discharge axis may be sufficient for electrodynamic
stabilization [43]. This can be achieved by the interference
of microwaves. Practically, the radiation is introduced into
the microwave device along a waveguide (1), the power W
being divided into two identical coherent components (W/2)
by means of a metal pin (2) mounted in a metal cylinder (3)
(figure 3). The discharge is formed into a dielectric tube (4),
Eel taking the highest value in its central plane. This is
due to the fact that the system is symmetrical with respect
to the electric field. Scientists from Kurchatov Institute of
Moscow have studied the SRO experimentally (5% oxygen
for a ratio H2 O/CH4 < 1) using such a continuous microwave
discharge plasmatron [43, 44]. The discharge power was up to
200 kW, the frequency was 915 MHz, the gas-flow rate up to
200 m3 h−1 , and the gas pressure in the reaction zone varied
in the range 0.1–1 atm. In this case the energy consumption
was of 42–47 MJ kg−1 H2 for a methane conversion rate higher
than 90%.
Quite recently, a simpler alternative approach for plasma
SRO has been proposed–the gliding arc [15, 45]. In this cold
plasma the ionization processes induced by the electric field
dominate the thermal ones and give relatively high-energy
2802
A no d e s
V2 V3
G a s o utle t
T°
M e a su r e
C he m ic a l
d ia gno stic s
Investment cost
H2 cost SOFC-GT-SRO system
(euro/Nm3 ) (euro/W)
0.05–0.08 5.12
0.23 4.59
electrons as well as excited ions, atoms or molecules that
promote selective chemical transitions efficiently. Such a
gliding arc occurs when the plasma is generated between two
or more diverging electrodes placed in a fast gas flow [46].
The average residence time of the reagents in the reaction
zone is about 10−3 s. This fact allows very high specific
throughputs in the reaction zone, which generally exceed, by
four orders of magnitude, other chemical methods, including
electrochemical and thermal ones. The literature presents
several studies modelling the behaviour of glidarcs trying
to predict the working parameters in different experimental
conditions [47–53].
The electrical circuit of a gliding arc consists of a high
voltage generator (up to 10 kV) used to ignite the discharge
and a second power generator with a voltage up to 1 kV and
a total current up to 10 A. Current limitation is achieved by
means of inductance.
The experiments for generating syngas by SRO in gliding
arc reactors have only been performed in the laboratory.
Researchers from GREMI, Université d’Orléans, have used a
reactor with an inner cone-shaped electrode and an external
metallic tube as a second electrode. This plasma reactor
generates turning gliding arc discharges, produced by the radial
injection of the gas mixture. Approximately 40% of the
methane submits to chemical transformation at a conversion
cost of about 89 MJ kg−1 H2 and to 125 kJ mole−1 of converted
methane, when a ratio of H2 O/CH4 = 4.5 was used through.
The electric power ranged between 0.1 and 0.3 kW with an
output energy efficiency of 40%. The productivity was as high
as 10 000 m3 h−1 H2 per m3 of reactor, operating at atmospheric
pressure. Further tests started in Spring 2001 with a multiple
discharge reactor (figure 4) using various catalysts.
We now present some preliminary results concerning the
costs of syngas production by means of plasma reformers.
There are three major costs in the manufacturing of hydrogen-
rich gas: the natural gas cost, the electricity cost and the

investment for the reactor system. For both the plasmatron
and the turning gliding-arc reactor a capital cost of 0.6 euro
per Watt of electrical power, that means about 65 euro per
Nm3 h−1 of hydrogen is estimated. This includes the cost
of the power supply and the reactor. The calculation assumes
that the capital equipment depreciates over a three-year period.
For a specific energy consumption of 16 MJ kg−1 H2 the cost
of the produced hydrogen is about 0.23 euro m−3 . However,
larger systems will produce hydrogen at lower costs and one
must appreciate the high productivity of plasma reactors, due
to their low dimensions.
6. Conclusion
SCL is becoming increasingly important for economic,
environmental and strategic reasons. Different authors admit
that a 25% capital cost reduction in current technology
would have a major impact on the overall economics of SCL
[11, 17, 54]. Plasma reactors represent an incisive approach by
their simplicity, compactness and low price (see table 1). For
small-scale units providing hydrogen for fuel cells, not only
for automotive applications, the choice of technology may be
dictated by such parameters as simplicity and quick response
to transients. Although SRO by means of chemical reactors
may be the most efficient, the use of plasma reactors may quite
soon become the preferred choice. Much more work has to be
done on the use of catalysts and reactor design (including heat
recovery).
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