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Syngas production from wood pellet using filtration

combustion of lean natural gaseair mixtures
Karina Araus, Felipe Reyes, Mario Toledo*
Department of Mechanical Engineering, Universidad Tecnica Federico Santa Mara, Av. Espana 1680,
Valparaso, Chile

article info

abstract

Article history:

A common method for the production of hydrogen and syngas is solid fuel gasification.

Received 16 December 2013

This paper discusses the experimental results obtained from the combustion of lean nat-

Received in revised form

ural gaseair mixtures in a porous medium composed of aleatory alumina spheres and

17 March 2014

wood pellets, called hybrid bed. Temperature, velocity, and chemical products (H2, CO, CO2,

Accepted 19 March 2014

CH4) of the combustion waves were recorded experimentally in an inert bed (baseline) and

Available online 16 April 2014

hybrid bed (with a volume wood fraction of 50%), for equivalence ratios (4) from 0.3 to 1.0,
and a constant filtration velocity of 15 cm/s. Upstream, downstream and standing com-

Keywords:

bustion waves were observed for inert and hybrid bed. The maximum hydrogen conversion

Hydrogen

in hybrid filtration combustion is found to be w99% at 4 0.3. Results demonstrate that

Syngas production

wood gasification process occurs with high temperature (1188 K) and oxygen available, and

Hybrid filtration combustion

the lean hybrid filtration process can be used to reform solid fuels into hydrogen and

Wood

syngas.

Gasification

Copyright 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights
reserved.

Introduction
Currently hydrogen (H2) is considered the fuel of the future as
a possible replacement for hydrocarbons. It is a clean fuel,
primarily to its low level of contamination when is burned. It
more energy per unit mass than any other fuel and applications of H2 as an energy source include electricity via fuel cell
[1]. Also hydrogen has disadvantages as low energy content
per unit volume, stored as liquid or compressed forms requires special and expensive infrastructure, and safety aspects. Hydrogen can be obtained from either renewable or
non-renewable sources. Reforming methane (CH4) with the
addition of water vapors is the industrial process most utilized
and economically feasible for the H2 production [2,3].

However, carbon dioxide (CO2) is generated during its production contributing to greenhouse gases and the subsequent
global warming. The main challenge competing energy
requirement and environmental protection is to find the balance between sustainable energy while reducing CO2 emissions generated by fossil fuels. As such, biomass can be
considered an excellent alternative to the production of
energy.
Biomass is considered a renewable source of energy
with zero emissions of CO2 to the atmosphere. It is available
in a diverse array of forms and types; animal refuse, forestry
residues and agriculture waste. There are also a number
of technologies available for the production of H2, syngas,
electricity, and generation of heat using biomass as the
starting feedstock; these include combustion, gasification,

* Corresponding author.
E-mail address: mario.toledo@usm.cl ( Mario Toledo).
http://dx.doi.org/10.1016/j.ijhydene.2014.03.140
0360-3199/Copyright 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.

7820

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liquefaction, hydrolysis, super-critical conversion, and pyrolysis [4e9]. However, some of these techniques are far from
being efficient. Lack of stable production of gases, limited
flexibility to operate a wide range of biomass, difficulties to
scale-up and low quality of obtained products are a few of the
disadvantages [5]. Recently, new technologies have been reported to convert biomass into H2; for example, gasification
under super-critical conditions and catalytic partial oxidation,
techniques which are not commercially available [10e14].
For other hand, research has been devoted to the benefits
of combustion in packed reactors with a porous matrix for the
production of H2, also known as filtration combustion.
Comparing this technique with conventional combustion in
an open flame, filtration combustion offers a wider power
range, higher efficiency, compact structure of higher energy
concentration per unit volume, stable combustion over a wide
range of equivalence ratios (4), due to the capacity of the
porous media to recirculate the heat within the reactor. This
method produces temperatures exceeding adiabatic values at
equilibrium, due to a large superficial area offered by the
porous media, which is responsible for heat transfer between
gaseous and inert solid phases [15e19]. Combining the benefits of filtration combustion and addressing requirements of
sustainable energy and minimal environmental impact, an
excellent proposal is hybrid filtration by homogenous mixing
of inert porous media and a solid fuel [20]. Thus, converting
solid and gas fuels into energy or H2 and syngas simultaneously [21].
Salganskii et al. [20] modeled gasification in a fixed bed
formed by a mixture of coal with an inert component. The
results of the thermodynamic model of the exhaust-gas
composition should be interpreted as the upper estimate in
terms of the CO and H2 contents in the gaseous products. On
the other hand, Salgansky et al. [22] performed theoretical and
experimental studies on combustion of coal/inert mixtures

with filtration of a gaseous oxidant. Experimental results

suggested that as the coal content in the bed exceeded 60%,
the volume concentration of CO and H2 were increased by
25%. The results of Salgansky et al. [22] demonstrated that
more studies are needed. Toledo et al. [21,23,24] have reported
a number of applications related to reforming gaseous and
solid fuels into H2 and syngas by using hybrid filtration combustion technology. Particularly, for rich and ultra-rich combustion of butane inside porous media composed of
homogeneous wood pellets and alumina spheres, they
observed that syngas yield in hybrid filtration combustion is
essentially higher than for butane filtration combustion in an
inert porous medium. Whereas rich and ultra-rich combustion of natural gas in a porous medium composed of homogeneous coal particles and alumina spheres, they reported
that syngas yield in hybrid filtration combustion was found to
be higher than for the inert porous medium case. The
maximum H2 conversion was 55% for the hybrid coal and
alumina bed at a volumetric coal value of 75%. Wood and
Harris [25] have reviewed research on lean CH4 combustion in
porous burners, specifically on ultra-lean combustion, and the
advanced of premixed fueleair mixtures burning inside of an
inert bed. This technology is capable of burning low-calorific
value fuels and very lean fueleair mixtures that would not
normally be flammable, potentially allowing the exploitation
of what would otherwise be wasted energy resources. However, above researchers still indicates that further studies are
required for investigation on filtration combustion related to
lean combustion for gaseous and solid fuels.
In this work, the results on H2 and syngas production in
lean filtration combustion of natural gaseair mixtures in
packed beds formed by wood pellets and alumina spheres are
reported. Temperature profiles, combustion wave velocities,
and chemical products were measured experimentally for
beds with wood content of 50%. Particular interest is the

Fig. 1 e Schematic of the experimental setup.

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 9 ( 2 0 1 4 ) 7 8 1 9 e7 8 2 5

concept and utilization of hybrid filtration combustion for

conversion of solid fuel to hydrogen and syngas.

Experimental apparatus and procedure

Fig. 1 shows the experimental apparatus, having three main
components: reactor, control system, and data logging. Lean
filtration combustion of natural gaseair mixtures was carried
out in a quartz tube 260  39  44 mm (length, ID, and OD,
respectively). The tube was packed with an equal volumetric
mixture of cylindrical wood pellets (5.6  5.6 mm, length  D)
and alumina spheres (Al2O3, 5.6 mm D). This hybrid bed has
40% porosity, occupying 80 mm of the length of the tube.
Wood pellets have a calorific value of 4406 kcal/kg, 0.6 g/ml of
apparent density, and 14.05% of moisture. Internal and
external surfaces of the tube were covered with thermal
insulation (Fiberfrax, 1.5 and 2.0 mm, respectively): thus,
allowing minimum heat loss and resulting to temperature
profiles almost uniformly, as well as protecting the tube from
excessive thermal expansion due to elevated temperatures.
Mass flow controllers (Aalborg, Orangeburg, USA) were
used to measure flow of natural gas (96% CH4) and air,
generated by an industrial air compressor (Qualitas, Florida,
USA). Reactants were mixed in a pre-reactor chamber, assuring a homogeneous gaseous mixture into the reactor.
Mixture is fed through the bottom of the burner and the
reactor is open to the atmosphere.
Combustion temperature data was collected by five S-type
(platinum/rhodium) thermocouples (T1eT5, see Fig. 1)
(OMEGA Engineering, Inc., Stamford, USA), shielded inside a
multi-bore ceramic tube running axially in the center of the
reactor, which provided temperature values in close proximity to the solid phase. Voltages measured by the thermocouples were recorded by an OMB DAQ 54 acquisition module
and converted by the Personal DaqView Software (OMEGA
Engineering, Inc., Stamford, USA). The thermocouple junctions were equally spaced at 4 cm interval along the length of
the shell, leaving 5 cm at each end of the reactor. Propagation
rates were obtained from thermocouple tracing. The experimental error in the temperature measurements was estimated at 50 K. Wave velocity measurements were based on
displacement of thermal profile along the reactor length,
having an error less than 10%.
Combustion products were sampled at the reactors exit by
using a ceramic tube, which is inserted 5 cm inside the packed
reactor (discrete sampled). The tube was connected to a vacuum line used as a sample probe. The exhausted gas was
filtered in a gas wash bottle and finally stored in Tedlar bags
for quantitation. The sample gas was taken when the flame
front was positioned in the middle length of the reactor.
Concentrations of H2, CO, CH4, and CO2 were quantified
directly by gas chromatography (GC), using a slightly modified
method reported by Pedersen-Mjaanes et al. [26]. Briefly, a
Clarus 500 GC (PerkineElmer, Massachusetts, USA) fitted with
two packed S/S columns (HayeSep Q, 3 m  1/8 in OD and
Molecular Sieve 5A, 1 m  1/8 in OD, Supelco, New Jersey,
USA), one detector (TCD), and helium (Linde Gas Chile, S.A.) as
carrier gas. Errors in GC analysis were estimated to be 15%.

7821

Before studying the combustion wave in the hybrid reactor,

a combustion wave in porous media with alumina spheres
(inert bed) only was studied, establishing validation and
baseline for the experimental procedure.
Using wood pellets in the packed reactor at 0 and 50%,
with 4 from 0.5 to 1.0, direction of the combustion wave
propagation was upstream (from T1 to T5). Ignition was
initiated at the reactors exit and propagation was recorded.
As the wave reached the reactor bottom, the flame was
turned off. However, using 4 of 0.4 and 0.3, in the presence/
absence of wood pellets, direction of the combustion wave
was downstream in propagation (from T5 to T1). Ignition
was initiated at position T5 (50 mm of inert packing, Fig. 1).
Once combustion progressed to position T4, reactor was
packed with hybrid bed until position T2 (solid particle and
alumina spheres were mixed aleatory before filtrate in the
reactor), and finally inert bed from T2 to the exit of the
reactor. The downstream propagation was recorded. As the

Fig. 2 e Combustion temperature profiles depicted at

various propagation times at 4 [ 0.6. Two cases are
presented: A) upstream inert bed and B) upstream hybrid
bed.

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wave reached the reactor exit, the flame was turned off. In
both cases (upstream and downstream propagation) the
alumina spheres were slowly shifted downwards occupying
the space of the wood pellets consumed by the moving
combustion wave. It was found that in both cases the wood
pellets were completely consumed through oxidation and
gasification. The operation of the reactor is a batch process.

Results and discussion

Experimental results are presented in terms of combustion
temperature, propagation rate, composition of combustion
products, and degree of conversion to H2 for mixtures of
natural gaseair in a packed reactor with a porous media either
inert (no wood pellets) or hybrid (50% wood pellets), within
equivalence ratio (4) range from 0.3 to 1.0, with a constant
velocity of filtration of 15 cm/s. Comparative data was

Fig. 3 e Combustion temperature profiles depicted at

various propagation times at 4 [ 0.4. Two cases are
presented: A) downstream inert bed and B) downstream
hybrid bed.

considered between measurements T2 to T4 in the packed

reactor.

Combustion temperature and propagation rate

Profiles obtained showed the potential use of lean mixtures to
produce simultaneously conversion of solid and gaseous fuel
to energy. Figs. 2 and 3 present the profile along the reactor (T1
to T5) for mixtures of natural gaseair with presence/absence
of wood pellets in the bed at various times of propagation
waves. The direction of propagation rate in the pack bed (inert
or hybrid), was upstream at 4 0.6 and downstream at 4 0.4.
Temperature peaks reached at T3 thermocouple in the
absence and presence of wood pellets were 1249 K and 1183 K
(Fig. 2, upstream propagation), and 1245 K and 1179 K (Fig. 3,
downstream propagation), respectively.
Experimental combustion temperature in a packed reactor
in either inert or hybrid media for natural gaseair mixtures
are presented in Fig. 4. Combustion temperature in the inert
bed reached a relatively constant value of 1275 K throughout
the tested 4 region. Temperatures obtained are basically independent from 4 or CH4 content, effect that is similar to
observed by Kennedy et al. [27]. However, temperatures
reached by hybrid bed were about 1188 K for 4 less than 0.8,
whereas temperatures diminished drastically for values (4)
above 0.8 (around 244 K). Drop in combustion temperature
suggest a change of kinetic mechanism due to reduce of oxygen available.
Propagation velocities of combustion are presented in
Fig. 5. Downstream and upstream propagation velocities were
observed, primarily depending on equivalence ratio. Close to
extinction limit, flame propagation is noticed as downstream.
Starting at 4 0.3, wave velocity decreases with an increase in
CH4, approaching zero at 4 0.45 for inert bed and 4 0.40 for
hybrid bed. A standing combustion wave is formed under
these experimental conditions. With further increase of the
CH4 amount, the regime of propagation changes to upstream.
The absolute value of velocity grows with the increase of 4 in

Fig. 4 e Combustion temperatures for inert and hybrid bed

as a function of equivalence ratios.

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 9 ( 2 0 1 4 ) 7 8 1 9 e7 8 2 5

Fig. 5 e Combustion wave velocity for inert and hybrid bed

as a function of equivalence ratios.

the lean mixtures, reaching the maximum at 4 1.0, using the

inert and hybrid bed.

7823

Fig. 7 e Carbon monoxide concentration of lean natural

gaseair mixtures for inert and hybrid bed.

The importance of this study is to evaluate the potential of

lean hybrid filtration combustion for the production of H2 and
syngas. Concentration of H2, CO, CH4, and CO2 measured
during the filtration combustion of natural gaseair with and
without wood pellets are presented as a function of 4 in Figs.
6e9, respectively. Specifically, for the inert bed and starting
from equivalence ratios below 1.0, complete combustion can
be achieved due to oxygen content in the mixtures. Therefore,
in this regime the concentrations of products such as H2 and
CO appear in insignificant concentrations in the exhaust
gases, as natural gas does not through partial oxidation under
these experimental conditions. As an example, H2 concentration remains null and independent from 4, for the range

4 0.3e4 0.9, for natural gaseair mixtures in inert bed.

Increasing 4 1.0, concentration of H2 reached 2.9% (Fig. 6),
similarly to reported by Toledo et al. [24]. For hybrid bed, H2
concentrations were independent from 4 for the range
0.3 < 4 < 0.8 reaching a constant value about 5.9%. Increasing
4 from 0.8 to 1.0, H2 concentration decreased from 6.8% to
1.5%, respectively (Fig. 6). The result shows that low combustion temperatures difficulties H2 production in hybrid
filtration combustion.
Fig. 7 shows the CO concentrations as a function of 4
for natural gaseair mixtures in the inert and hybrid bed. For
inert bed the concentration of CO measured remains
almost constant (w0.2%) and independent from 4 tested at the
range 0.3 < 4 < 0.8. While incrementing 4 from 0.8 to 1.0, CO
concentration increased from 0.2 to 3.4%, respectively. In the
hybrid bed, the concentrations of CO measured experimentally were slightly dependent of 4 and the maximum was 1.4%
reached at 4 1.0.

Fig. 6 e Hydrogen concentration of lean natural gaseair

mixtures for inert and hybrid bed.

Fig. 8 e Methane concentration of lean natural gaseair

mixtures for inert and hybrid bed.

Combustion products

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Fig. 9 e Carbon dioxide concentration of lean natural

gaseair mixtures for inert and hybrid bed.

Concentrations of CH4 are shown in Fig. 8 as a function of

equivalence ratio. Unburned CH4 is practically not measured
in the products starting from 4 0.3 to 1.0 for natural gaseair
mixtures using the inert bed. Contrary, CH4 is slightly detected
using natural gaseair mixtures with the hybrid bed. Its concentration grows with increasing 4, achieving w2.6% for
4 1.0. In fact, the filtration combustion of lean natural
gaseair mixtures under the experimental conditions tested is
capable of inducing chemical transformation of wood in the
mixtures with excess oxygen concentration, but this content
of oxygen is not sufficient to transformer all the CH4 content
in the mixture (unburned CH4 or incomplete combustion). In
comparison for the hybrid bed case the CH4 concentrations
increase for equivalence ratio of 0.9 and 1.0 (CH4 unreacted)
that suggests that CO concentrations is not higher than the
inert bed case.

Fig. 10 e Conversion degree of fuels to hydrogen for inert

and hybrid bed.

For natural gaseair mixtures using the inert bed the concentrations of CO2 increased with equivalence ratio (Fig. 9).
The maximum concentration of CO2 measured was w7.9% at
4 0.9. For hybrid bed the maximum concentrations of CO2
were 7.8% and 8.5% which were reached at 4 0.3 and 4 0.8,
respectively.
Fig. 10 shows the degree of conversion of solid fuel to H2 for
natural gaseair mixtures in the inert and hybrid bed, as
function of the equivalence ratio. The yield is calculated using
the initial H2 content in the natural gas and wood pellets for
the case of the hybrid bed. The maximum yield recorded for
the hybrid bed was w99% at 4 0.3. In fact, a lean wave is
capable of inducing chemical transformation of CH4 in mixtures with very high oxygen concentration, using inert bed,
whereas, in packed bed with wood and inert medium and
using lean wave prevails more the chemical transformation of
the wood than CH4 in the mixtures with very high oxygen
concentration. Thus, the results show that lean hybrid filtration can be used to reform solid fuels into H2 and syngas.
Furthermore, the hybrid filtration of lean burn offers advantages where the energy content of the fuel is extremely low,
because the porous matrix can potentially provide high heat
recirculation.

Conclusions
Hydrogen and syngas production in lean filtration combustion
were studied experimentally for natural gaseair mixtures
using a packed bed with an inert medium and/or hybrid. The
hybrid bed was randomly arranged of wood pellets plus inert
medium, at volumetric wood content of 50%. The experimental conditions tested were at equivalence ratio (4) from 0.3
to 1.0, for a filtration velocity of 15 cm/s. The focus of research
was to analyze on combustion temperatures, combustion
wave velocities, the chemical products, and conversion of
solid fuel (wood) to H2 and syngas.
The combustion temperatures recorded for the inert bed
was practically independent of equivalence ratio (1275 K). For
hybrid bed the combustion temperature (1188 K) decreases at
4 > 0.8. Drop in combustion temperature suggest a change of
kinetic mechanism due to reduce of oxygen available.
Downstream and upstream wave propagation was
observed for lean natural gaseair mixtures. Close to the
extinction limit, downstream propagation was observed. The
velocity of the wave decreases with an increase of the CH4
concentration, approaching zero at 4 0.45 for inert beds and
4 0.40 for hybrid beds. A standing combustion wave is
formed under these experimental conditions. With further
increase of the CH4 amount, the regime of propagation
changes to upstream. The absolute value of velocity grows
with the increase of equivalence ratio in the lean mixtures,
reaching the maximum at 4 1.0, using the reactor with and
without wood pellets.
The maximum degree of conversion of fuels to H2 for the
hybrid bed was w99% at 4 0.3. A lean filtration wave is
capable of inducing chemical transformation of wood in
mixtures with very high oxygen concentration. The results
show that lean hybrid filtration combustion can be used to
reform wood into H2 and syngas.

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Acknowledgments
The authors wish to acknowledge the support by the CONICYT-Chile (FONDECYT 1121188).

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