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Article history: In the present article, ASPEN Plus is used to develop a process model of the hydrogen-rich gas production
Received 2 January 2019 through cleaning and catalytic conditioning of producer gas. The process includes producer gas cleaning
Received in revised form using venturi scrubber and sand bed filter followed by compression of the gas to 0.6 MPa using
16 February 2019
compressor. The clean producer gas along with steam undergoes high temperature water gas shift re-
Accepted 18 February 2019
action to produce hydrogen-rich gas. The power law kinetic model for commercial HTS catalysts reported
Available online 19 February 2019
in the literature is used in the model. Experimental results from our previous study and those reported in
the literature are used to validate the developed model for the compositions of CO & H2 in the product
Keywords:
Producer gas
gas. The validated model is further simulated to study the effects of parameters such as reactor tem-
Water gas shift reaction perature, catalyst bed length and steam to CO ratio on the product gas composition. The optimum
Hydrogen operating conditions for maximizing CO conversion are found and reported. The maximum H2
Process model composition and CO conversion predicted by the model are 27.029% 97.5479% respectively and the
ASPEN corresponding operating conditions are reactor; temperature of 350 C, S/CO of 8 and GHSV 1000 h1.
© 2019 Elsevier Ltd. All rights reserved.
https://doi.org/10.1016/j.energy.2019.02.136
0360-5442/© 2019 Elsevier Ltd. All rights reserved.
T.K. Patra et al. / Energy 173 (2019) 1130e1140 1131
clean up, water or liquid absorbents are use to remove contami- balance, water gas shift reaction and the methanation reaction. The
nants. Wet scrubbers such as spray scrubbers, wet dynamic model predicts the syngas composition and its heating value, char
scrubbers, cyclonic spray scrubbers, impactor scrubbers, venturi and tar yield during the process. The developed model was vali-
scrubbers, and electrostatic scrubbers are the most common and dated with experimental results of two different agricultural resi-
effective method to remove both particulate matter and tar from dues at different moisture contents and process operating
the contaminated gas stream [14]. This clean producer gas can be conditions.
directly used in gas engines, turbines and as a feedstock to produce The prime objective of the present study is to model and study
liquid fuels and electricity. Apart from the quality of the gas in the downstream section of the H2 rich gas production unit, which
terms of tar and SPM content, the composition of the producer gas comprises of the gas cleaning system and the fixed bed water gas
mixture also plays a vital role in deciding its application in various shift reactor. The study also aimed at finding the optimum oper-
processes [15]. The producer gas generated from the biomass ating conditions for maximization of H2 composition in the product
gasification process is a potential source of hydrogen-rich gas gas. The model development and simulation have been carried out
production provided a proper quality and composition are main- using ASPEN Plus software. The simulated model predictions are
tained. In this process, the raw producer gas generated undergoes validated for CO conversion and H2 composition with experimental
water gas shift reaction for hydrogen enrichment. It is a highly data from the previous experimental study and also the experi-
economical and efficient process which uses one of the most mental results reported by Marono et al. [30]. Apart from this,
important reactions in the process industry. The reaction equilib- various parameters affecting the composition of the final product
rium depends significantly on the temperature and also requires gas are also studied using the sensitivity analysis tool. Various
the presence of the catalyst [16]. The Arrhenius law states that the operating parameters such as the steam/CO ratio (S/CO) and gas
rate of reaction increases with the increase in temperature, at the hourly space velocity (GHSV) are incorporated in the model using
same time according to Le Chatelier's principle, the equilibrium the design specification tool. Power law kinetic model is chosen
moves in a forward direction with a decrease in temperature, for an and the reaction kinetics of commercial high temperature shift
exothermic reaction and vice versa for endothermic reaction [17]. catalyst reported in literature is used for the simulation. An opti-
Thus, operating condition for the reaction under consideration is mization study is also carried out to find out the optimum oper-
decided by the trade-off between the kinetics and the thermody- ating conditions for the hydrogen production process. The results of
namics of this reaction. In an industry, the water gas shift reaction is the present study can be used for process design and scale up of
carried out at two different temperature ranges, low temperature various syngas to methanol and hydrogen production processes. It
shift (LTS) from 150 C to 250 C and high temperature shift (HTS) will also help is deciding the optimum range for variation of
from 350 C to 500 C [17,18]. A numerous studies are reported for operating parameters to get maximum conversion.
the kinetic simulation of downdraft biomass gasification [19e23]
however, a few researches have used Aspen Plus to develop a model 2. Process description
for the downdraft gasification process. Ramzan et al. [24] devel-
oped a steady state simulation model for a hybrid biomass gasifier. The raw producer gas from the gasification process contains
The model developed was based on Gibbs free energy minimization impurities such as tar, SPM, soot and dust particles which need to
method and chemical equilibrium in the reactions. The authors also be removed from it for its utilization in different industrial appli-
carried out a sensitivity analysis of the gasification process and cations such as power production, production of fuels and chem-
reported the effects of gasifier temperature, Equivalence ratio (ER), icals. Cleaning is necessary as because these impurities cause
moisture content and steam/biomass on syngas composition, HHV various problems in further downstream processes such as clog-
of the syngas, Cold gas efficiency (CGE) and hydrogen production. ging of the engine, corrosion, environmental pollution etc. The
Begum et al. [25] developed a model for fixed bed gasification of experimental setup used for model development is shown in Fig. 1.
Municipal solid waste (MSW) using Aspen Plus. The model calcu- The producer gas cleaning unit basically consists of two equip-
lations were based on Gibbs free energy minimization method to ments: venturi scrubber and sand bed filter. Venturi scrubber
predict the product gas composition, was validated with experi- effectively eliminates the impurities comprising of tar and SPM. The
mental data reported in literature. Kuo et al. [26] carried out a solvent passes through the venturi scrubber in a co-current fashion
comparative thermodynamic analysis for gasification of raw and and impurities from the gas phase get transferred to the liquid
torrified bamboo in a downdraft gasifier using Aspen Plus. The phase. Water is used as a solvent in the present system. The venturi
authors used two operating parameters modified equivalence ratio scrubber consists of a converging section, throat, diverging section
and steam supply ratio to study the gasification performance by and a cyclonic chamber. Water and gas enter separately from the
cold gas efficiency and carbon conversion. Formica et al. [27] re- top of the converging section and their velocity increases. The high
ported a zero dimensional steady state model for a downdraft velocity liquid gets atomized upon discharge into the throat section
biomass gasification plant. The model also included all the plant and comes in contact with gas phase. When the fluid passes
equipments such as gasifier, cyclone, heat exchangers and piping through the diverging section, its velocity decreases and the tiny
and validated with the experimental results. The authors have liquid droplets get mixed with the gas stream. The increased sur-
carried out simulations using various operating parameters such as face area of the solvent molecules enhances the mass transfer and
equivalence ratio, biomass moisture content and gasifying air thus the separation of impurities takes place efficiently [31]. In the
temperature. Tapasvi et al. [28] proposed a two stage gasification cyclonic chamber, the clean gas goes out of the top and the dirty
model for comparing torrified and non torrified biomass gasifica- water gets collected from the bottom. A sand bed filter is used to
tion. The authors reported a better model predictions by incorpo- remove the moisture and remaining impurities in the product gas.
rating tar, biomass decomposition products and char composition In the sand bed filter, the gas passes through a bed of thin wood
data in the model. Three process parameters i.e. steam to biomass shavings followed by of coarse and fine sands. The wood shavings
ratio, Gibbs reactor temperature and equivalence ratio were varied and sand bed collectively remove the moisture and remaining tar
and the model was validated with CeHeO ternary diagrams and particles. The outlet gas from the cleaning system is compressed
other reported experimental results. Recently Gagliano et al. [29] and sent to the fixed bed catalytic reactor. In this reactor water gas
proposed an equilibrium based model for co-current gasification of shift reaction is carried out to enhance the hydrogen content in the
agricultural residues. The model incorporates mass and energy producer gas. The water gas shift reaction involves the reaction of
1132 T.K. Patra et al. / Energy 173 (2019) 1130e1140
LEGEND:
steam with carbon monoxide. The heating coils are wrapped over a represent raw syngas, which is an impure producer gas; four
stainless steel pipe and temperature is controlled by using PID streams are mixed viz. GASIFIED, TAR, CSPM and FINESPM in a
controller (Make: Selec, Model: TC 513). The water is pumped mixer block (MIXER). The enthalpy of mixing is considered to be
through stainless steel pipe using HPLC pump (Make: Lab Alliance, zero as in reality, only one producer gas stream exists. The
Model: series II) which gets converted to steam at saturated con- PRODGAS (impure producer gas leaving the mixer) enters the
ditions. The flow rate of the gas is based on S/CO ratio. The steam venturi scrubber (VSCRUB). Another stream which is entering in the
generated is mixed with the feed gas in a mixer to preheat the venturi scrubber is the WATER. The outlet streams are DIRWATER
reactants. The mixed gas is then passed to a preheater, where the (water þ impurities) and GAS þ SPM. VScrub is a solid separator
feed mixture is further heated to 200 C. The preheated feed gas is block used for cleaning impurities from gaseous streams. Many
then passed through a catalyst bed in a tubular reactor. The outlet theoretical models are available to predict the particle collection
gas from the reactor is at a high temperature ranging from 300 C to efficiency of venturi scrubber such as Calvert, Yung, Boll etc. For the
450 C. This gas passes through a condenser to cool down the hot present study, CALVERT calculation method is chosen and the grade
hydrogen-rich gas. When the hot outlet gas is passed through the efficiency parameter (f) is chosen as 0.31. For predicting particle
condenser, the excess steam gets condensed and gets separated collection efficiency Calvert assumed that venturi scrubber consists
from the product gas in a gas-liquid separator. entirely a throat and the gas droplets accelerates in the throat to
achieve highest gas velocity. f is a correlative parameter used to
3. Model development calculate the penetration and its value lies in the range between 0.2
and 0.7 [35]. GAS þ SPM stream goes into the solid separator, where
3.1. Assumptions most of the SPM is separated on the basis of the parametric values.
It is a cyclone type solid separator block. The solid fraction of solid
Tar is a mixture of various hydrocarbons and represented as a outlet is chosen as 1 and the separation sharpness as 0.85. The
mixture of four different chemicals, i.e. 25% Toluene, 58% Phenol, classification characteristic for the separation is based on particle
15% Naphthalene and 2% Pyrene [32,33]. SPM is generally size. The GAS stream from the solid separator goes into the
comprised of unconverted carbon and ash. In the present simula- SNDBFLT (sand bed filter), where further separation is done. A Sep2
tion study, SPM is assumed to contain 100% of Ash [34].The system block is used to model the sand bed filter unit. The efficiency of
is assumed to be ideal and at steady state without any disturbances. separation for the sand bed filter is taken from literature as 97%
The loss of material from the system is negligible. Pressure and heat [36]. So the sand bed filter removes the remaining tar and the
loss have been incorporated in the model. The shift reactor is moisture present in the product gas with an outlet gas split fraction
assumed to remain at a constant temperature. of 0.03 for tar components and H2O. The pure gas, represented by
CLEANGAS is compressed in COMPRSOR. A compressor model
3.2. Model description which is available in the ASPEN Plus simulator was used. In order to
incorporate the heat loss during the compression process, a heat
Fig. 2 describes the complete process flow diagram of the pro- exchanger (Heater model) denoted by HEATLOSS is used. The heat
posed system developed using ASPEN Plus. Table 1 lists all the exchanger block is used to reduce the temperature of compressed
streams and blocks used in the ASPEN PLUS simulation. In order to product gas stream from 294.308 C to 40 C. The pressure of the inlet
T.K. Patra et al. / Energy 173 (2019) 1130e1140 1133
and outlet streams remains constant at 6 bars, the vapour fraction is stream (COLD) goes into the gas liquid separator (GLS), a Flash2
taken as 1 and the net het duty for the heat exchanger is 363.513 block is chosen.
Cal/sec. The outlet gas of the cleaning system going into the tank is To model it. The final outlet stream coming out from GLS is
represented by COMPGAS stream. A Splitter model (SPLITTER) is represented as FINALGAS. Table 2 describes the various model pa-
used which splits the COMPGAS stream into two fractions, one that rameters used for different blocks in the process flow diagram.
goes into the shift reactor system (CLNGASIN) and the other that An optimization study for the water gas shift reactor has been
remains in the tank. The amount of the gas going into the reactor carried out. The operating parameters such as reactor temperature,
system is decided by split fraction. The Split fraction is the fraction steam to CO ratio and GHSV are considered for the study and the
of inlet stream going into the outlet stream.. The split fraction for output parameter chosen is CO conversion. Three different levels
the CLNGAS stream is set as 0.1 i.e. only a small fraction of the clean for all the input parameters are taken and a full factorial design
producer gas has been fed into the water gas shift reactor. In our method is adopted to consider all possible combination of the
case, this split fraction is based on the steam/CO ratio. This is ach- operating conditions.
ieved by using the design specification tool. A small FORTRAN code
is written, the ratio variable was defined as:
3.3. Model parameters
R ¼ H2 O=CO (1)
A bimodal particle size distribution (PSD) of the particulate
Where, H2O and CO are variables representing the mole flow
matter with a peak diameter of 0.155 mm reported by Jimenez and
rates of H2O and CO in the FEED stream respectively. Here, the split
Ballester [38] is used in this model. According to Laurence and
fraction parameter of SPLITTER block is varied to achieve the
Ashenafi [39] sand bed filter has a particle removal efficiency from
desired value of R.
70% to 99%, while the tar removal efficiency is about 50%e97%.
Before developing the model of the shift reactor system, the
Pathak et al. [36] reported the cleaning efficiency of the filter in the
reactions scheme and kinetic model are defined. A kinetic scheme
range of 83%e97%. In the present ASPEN model, the parametric
is defined for the water gas shift reaction. The reaction model
values of separation efficiencies of the sand bed filter have been
chosen is the reversible general type and the reaction class selected
considered to be 97%. Laurence and Ashenafi [39] reported the
is power law. The pre-exponential factor, activation energy and the
separation efficiency in the range of 85%e90%. In the present
exponent values reported by Hla et al. [37] are used. One of the raw
model, the parametric value of separation sharpness of solid
materials of the shift process is water (H2O stream). This goes into
separator has been considered to be 85%. The kinetic model for the
the steam generator (STEAMGEN) which is modeled using the
commercial water gas shift catalysts i.e. High Temperature Catalyst
heater block. STEAM is then mixed with the CLNGASIN stream in
(HTC) represented by equations (2) and (3) are reported in Hla et al.
MIXER2 (mixer block), the MIXED stream is then preheated by a
[37] is chosen in the present study. The equilibrium constant is
preheater (PREHEAT). The preheated stream (FEED) goes into the
calculated using the correlation given in equation (5).
REACTOR which is a Rplug reactor. The dimensions and other
specifications such as the reactor temperature and catalyst loading
88±2:18 0:9±0:041 0:31±0:056
are entered. For a particular simulation, the reaction kinetic model r ¼ 100:659±0:0125 exp P CO P H2 O
has been chosen accordingly. The outlet of the reactor (H2RICH) is
RT (2)
then condensed in a condenser (CONDENS) which is modeled using P 0:156±0:078
CO2 P 0:05±0:006
H2 ð1 bÞ
a HeatX block. The minimum temperature approach is set at 10 F
and the hot stream outlet temperature is 40 C. The condensed where b is the approach to equilibrium and is defined as:
1134 T.K. Patra et al. / Energy 173 (2019) 1130e1140
Table 1 Table 2
Description of steams and blocks in the ASPEN model. Various model input parameters used for simulation.
composition value is less than that of the results obtained from the Reactor Temperature(deg C)
experimental study. However, at higher GHSVs of 2712 h1 and Fig. 4. Comparison of experimental data of the present study with the model pre-
5425 h1, the model predicted CO composition values and the dicted H2 and CO compositions in the product gas for GHSV 2712 h1..
corresponding experimental values matches well. In fact for lower
reactor temperatures it exactly matches with the experimental CO
composition for all GHSVs. 50
Hydrogen
The developed model is also validated with experimental results Model Prediction
reported by Marono et al. [30] for CO and H2 composition in the Experimental
40 Carbon Monoxide
product gas at different reactor temperatures. The composition of
Product gas Composition(%)
product gas, space velocity, steam to CO ratio, catalyst weight and Model Prediction
Experimemtal
catalyst composition reported by Marono et al. [30] are used as
30
Table 4 20
Experimental data from present study used for simulation.
Table 5 100
Experimental data reported by Marono et al. [30] used for simulation. Hydrogen
90 Model Prediction
Feed gas composition Component Composition (%
Experimental
v/v, dry basis) 80
20
100 10
Hydrogen
90 Model Prediction 0
Experimental 280 300 320 340 360 380 400 420 440
80
Product gas composition (%)
Carbon Monoxide o
Reactor Temperature ( C)
70
Experimental
Model Prediction Fig. 7. Comparison of experimental data of Marono et al. [30] with the model pre-
60 dicted H2 and CO compositions in the product gas for GHSV 10,000 h1.
50
CO conversion (%)
study, the GHSV is varied from 1000 h1 to 20,000 h1 at reactor 10
CO conversion (%)
60
20
L ¼ 4*W/7.74
V ¼ L*194.729*10
40
VFLOW ¼ MFLOW/DENSITY
10
VFLOW ¼ VFLOW*(P*273.15/T)
SPACEV ¼ VFLOW*1000/V
20
X ¼ (COIN-COOUT)*100/COIN
0
CO ¼ CO*100/ (1-H2O)
CO2 ¼ CO2*100/ (1-H2O) 0
H2 ¼ H2*100/ (1-H2O) 250 300 350 400 450 500 550 600
o
Reactor temperature ( C)
Fig. 9 shows the effect of catalyst bed length on the product gas
composition and CO conversion at S/CO ratio of 8. It is observed that Fig. 10. Variation of product gas composition (CO, CO2, and H2) with reactor
with the increase in catalyst bed length H2 and CO2 composition temperature.
composition of CO, CO2 and H2. From the figure it is seen that with
CO conversion (%)
25
60 the increase in S/CO ratio the composition H2 and CO2 increases and
that of CO decreases. At S/CO ratio of 8 the maximum amount of H2
20
and CO2 obtained in the product gas stream are 26.64% and 21.40%
40 respectively. The maximum amount of H2 and CO2 produced at S/
15
CO of 8 are 26.64% and 21.40%. Fig. 12 shows the effect of S/CO on CO
10 conversion at different reactor temperatures. It can be seen that
20 higher S/CO gives higher CO conversion. While increasing the S/CO
5 from 2 to 4, the CO conversion value goes up from 69.27% to 86.13%
and the further rise in S/CO to 8 results in increase in CO conversion
0 0
to a maximum value of 93.48%. By analyzing the outlet gas
0 2 4 6 8 10 12 14
composition profiles, the S/CO ratio of 8 is found to be the optimum
catalyst bed length (cm)
at all reactor temperatures for maximum CO conversion and H2
Fig. 9. Variation of product gas composition (CO, CO2 and H2) and CO conversion with production since there is no significant variation is observed in the
catalyst bed length. product gas composition beyond this value.
1138 T.K. Patra et al. / Energy 173 (2019) 1130e1140
Table 6
S/CO=2 List of different factors with their levels.
25 CO
Factor Level-1 Level-2 Level-3
CO2
H2 GHSV (h1) 1000 1500 2000
Product gas composition (%)
20 S/CO=4 S/CO 2 4 8
CO Reactor temperature (C) 300 350 400
CO2
15 H2
S/CO=6 has 3 levels. So, accordingly, the total number of experiments which
CO
is given by (level) factor becomes 27. The results of all the 27 ex-
10 CO2
H2
periments are shown in the following Table 7. The response variable
S/CO=8 considered in the experiment is the product gas composition and
5 CO CO conversion.
CO2 On examining the above results, it is observed that highest CO
H2 conversion of about 97.55% and H2 composition of 27.026% are
0 achieved for GHSV 1000 h1, S/CO ratio of 8 and temperature
250 300 350 400 450 500 550 600 350 C. The GHSV 2000 h1, S/CO ratio of 2 and the reactor tem-
Reactor temperature ( C)
0
perature of 300 C corresponds to the lowest CO conversion of
63.35% and the lowest H2 composition of 23.687%. Unlike the
Fig. 11. Effect of steam to CO ratio on outlet gas composition.
temperature dependence trend observed before, the conversion of
CO is not higher at temperatures as high as 400 C. For instance, the
100
conversion at a specific GHSV and S/CO ratio is higher at 350 C
S/CO 2 than at 400 C. From this it can be inferred that at low GHSVs,
S/CO 4 unlike in the previous study, the optimum temperature for the shift
80
S/CO 6 reaction is 350 C. ̊Note that the temperature dependence is still
S/CO 8
followed as the conversion at 300 C is lower than that at 400 C
and 350 C. The conversion of CO also increases with the S/CO ratio.
CO conversion (%)
Table 7
Experimental matrix for factorial design study.
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