Article

Cite This: Ind. Eng. Chem. Res. 2020, 59, 299−307 pubs.acs.org/IECR

Experimental and Numerical Investigation of Biosolid Gasification:

Equilibrium-Based Modeling with Emphasis on the Effects of
Different Pretreatment Methods
Ashraf Abdelrahim,*,† Paola Brachi,‡ Giovanna Ruoppolo,‡ Simona Di Fraia,† and Laura Vanoli†
†
Dipartimento di Ingegneria, Università degli Studi di Napoli “Parthenope”, 80143 Napoli, Italy
‡
Istituto di Ricerche sulla Combustione, Piazzale V. Tecchio 80, 80125 Napoli, Italy
*
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ABSTRACT: In the present study, a modified equilibrium model was developed by Aspen Plus to simulate the gasification of
biosolids (treated sewage sludge) in an atmospheric fluidized bed reactor (FBR) using air as a gasification agent. The model,
which is based on the Gibbs free energy minimization applying the restricted equilibrium method, was calibrated and validated
against a set of experimental data obtained in a pre-pilot-scale FBR. The comparison between the simulation results and the
experimental data showed satisfactory agreement, in particular, with respect to the content of combustible gases in the syngas
and the heating value. The main objective of the work was to assess the impact of different sludge pretreatment methods (i.e.,
torrefaction, anaerobic digestion, carbonization, hydrothermal treatment, and copelletization of sewage sludge with solid fuels)
and the key operating conditions (gasification temperature and equivalence ratio) on both the syngas quality (composition and
heating value) and the performance of the gasifier in terms of the carbon conversion efficiency (CCE), syngas yield (YG), and
cold gas efficiency (CGE) under the same operating conditions. Global sensitivity analysis was first performed by varying the
gasification temperature and the equivalence ratio (ER). Then, the impact of sludge pretreatments was evaluated by changing
the sludge composition in the model in line with experimental data from the pertinent literature. Results point out that the
torrefaction pretreatment in combination with gasification exhibits promising results in terms of gas quality (i.e., higher H2/CO
ratio and lower CO2/CO ratio) and LHV, even though the carbon conversion efficiency (CCE) slightly decreases presumably
because of the lower volatile content in the torrefied material with respect to the parent one.

1. INTRODUCTION sludge phase,2 thus making its disposal more complex and
A wastewater treatment plant typically produces two streams, expensive.
namely, the stream consisting of treated wastewater and the A biosolid is defined as a sewage sludge3 that has undergone
stream consisting of sludge separated from the wastewater. sufficient treatment for its stabilization and pathogen reduction
Both streams have requirements from authorities for discharge but still consists of a mixture of carbonaceous, phosphorus, and
or use for different purposes.1 Because of the growing nitrogenous compounds with heavy metals and (in its wet
awareness of climate change and other environmental state) microbial organisms. While phosphorus- and nitrogen-
concerns, requirements for wastewater discharge have been containing compounds make biosolids a potentially valuable
continuously strengthened in the past 30 years and more fertilizer,4 the presence of heavy metals, toxins, dioxins, and
efficient treatment processesphysical, chemical, biological, microbial contaminants makes them unsuitable for spreading
and otherhave been implemented across the globe.
The improved treatment efficiency also means that a higher Received: July 17, 2019
percentage of unwanted pollutants are transferred from the Revised: December 3, 2019
wastewater (such as heavy metals, polycyclic aromatic Accepted: December 6, 2019
hydrocarbons (PAHs), and organic micropollutants) into the Published: December 6, 2019

© 2019 American Chemical Society 299 DOI: 10.1021/acs.iecr.9b03902

Ind. Eng. Chem. Res. 2020, 59, 299−307
Industrial & Engineering Chemistry Research
on farmland because of the risk of contaminants entering the
food chain.5,6 Aside from land application, other uses for
sludge are available, including landfills and incineration.7,8
The Landfill Directive 99/31/EC9 prohibited the deposition
of both liquid and untreated wastes in landfills and indicated
some restrictions and quantitative targets for biodegradable
municipal solid wastes (such as sewage sludge) to dispose of in
landfills. Therefore, in most European countries depositing
sewage sludge in landfills is decreasing, whereas the most
common reuse option in EU-15 is recycling in agriculture.10 In
a lot of cases, the sludge or the ash from sludge combustion is
used in the production of cementitious building materials, in
particular, as an aggregate in cement, brick, and cement-based
mortar formulations.11,12
Because of the high carbon content, biosolids can also be
utilized as a renewable fuel. The study by Rulkens11 has
identified several sludge management options, among which
those involving the production of energy (heat, electricity, or
biofuel) seem to be the most promising ones. In more detail,
these include anaerobic digestion, codigestion, incineration in
combination with energy recovery, coincineration in coal-fired
power plants, coincineration in combination with organic
waste focused on energy recovery, use as an energy source in
the production of cement or building materials, pyrolysis,
gasification, supercritical (wet) oxidation, hydrolysis at high
temperature, hydrogen production, acetone, butanol, or
ethanol and the direct generation of electrical energy by
means of specific microorganisms. Pyrolysis13−17 and gas-
ification18−20 were investigated by numerous researchers,
suggesting that biosolids have the potential to be used as a
clean energy source through these technologies. Additionally,
these conversion routes can reduce flue gas volumes and fix
heavy metals in the solid residues while producing valuable
products such as bio-oil and syngas; the gas flow coming from
a gasifier is significantly lower than the gas flow from an
incinerator having the same sludge-processing capacity.21 The
gasification of biosolids has been selected in the present study
because such a process (with a combined cycle) is, in general,
more efficient than the incineration or combustion of biosolids
for power generation11,22 and potentially provides environ-
mental benefits by reducing and preventing many emissions.
One reason for this is the possibility of removing compounds,
which would later form pollutants during the combustion
process, through simple cleaning and scrubbing.23
Gasification is a very complex process including numerous
chemical reactions that are partially unknown or unpredictable.
The main involved reactions include the combustion and
gasification ones, which are shown in Table S1.24
The primary product from the gasification process is a
combustible gas mixture, also called syngas, which mostly
consists of hydrogen, carbon monoxide, methane, carbon
dioxide, small amounts of nitrogen and light hydrocarbons, and
tars. The syngas produced can be utilized for electric power
generation, heat generation, chemical processes, and trans-
portation and in other industrial sectors. In addition, by
properly selecting the operating conditions and/or the catalyst,
a syngas rich in hydrogen can be obtained, which can be
converted to energy via hydrogen engines and fuel cell
technology without any greenhouse gas production.25
Table S2 summarizes past studies on sewage sludge
gasification with a particular emphasis on the selected
operating conditions (e.g., gasifying agents, reaction con-
ditions, and catalyst use) and the adopted reactor config-
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uration. The optimization of such parameters is required for
maximizing the gas yield, enhancing the gas quality, minimizing
the tar yield, and increasing the gasification efficiency.
Gasification modeling is an effective tool used to optimize
the design of a gasifier by studying the influence of the main
process variables, such as the gasifying agent type and
temperature, the feedstock type, pretreatments, and moisture
content on the process performance and efficiency.27 Depend-
ing on the adopted approach, biomass gasification models can
be divided into two main categories, namely, kinetic models
and equilibrium models.28 Kinetic models are useful in
predicting the progress and the product composition at
different positions along the reactor, whereas the equilibrium
models are typically used to assess the maximum achievable
yield of the desired product from a reacting system.29,30
When dealing with fluidized beds, the evolution of the
process at each point of the system can be hard to elaborate in
addition to the complex hydrodynamics and phase regimes
that add up to the calculations. For these reasons, equilibrium-
based modeling has recently gained more attention.31
Equilibrium modeling consists of two approaches: stoichio-
metric and nonstoichiometric.32 The stoichiometric model
requires a detailed specification of all the chemical reactions
and species involved.33 In contrast, nonstoichiometric models,
based on minimizing the total Gibbs free energy, need no
particular reaction mechanisms or species like the stoichio-
metric models. The only input needed is the elemental
composition of the feed that is known from the ultimate and
proximate analysis data.33 Thus, the nonstoichiometric method
is relatively easier to implement and has faster convergence.32
A common simulator used for model development is the
Aspen Plus chemical process software. It represents conversion
systems by dividing them into unit operation blocks, such as
reactors, separators, and heaters. These blocks are joined using
material and energy streams and, if possible, are configured
with appropriate correlations.33
For gasification, most studies have performed the
simulations through the minimization of the Gibbs free energy
of the system; this is the case for Nikoo et al.,34 who modeled
the gasification process in fluidized beds, and Ramzan et al.,35
who studied the influence of different kinds of fuels on biomass
gasification. Even though several simulation models for the
biomass gasification process have been developed so far by
using Aspen Plus, to the best of our knowledge very few studies
in the literature can be found on Aspen simulation models for
biosolid gasification, and none of them deal with different
sludge pretreatment methods.
In this context, the main objective of this work is to develop
a model for the gasification of biosolids in a fluidized bed
reactor to validate it against experimental data obtained
through a pilot-scale experimental campaign and utilize it to
examine the influence of the main operating parameters as well
as different sludge pretreatments (i.e., digestion, torrefaction,
carbonization, hydrothermal carbonization, and copelletiza-
tion) on both the performance of the gasifier and the syngas
quality. Specifically, an Aspen Plus model has been developed
to simulate the thermochemical transformation of biosolids to
high-value energy carriers through air gasification. The model
is based on Gibbs free energy minimization, and the restricted
equilibrium method by Gumz36 was used to calibrate it against
experimental data. In more detail, this was achieved by
specifying the temperature approach for a number of reactions
occurring in the gasification unit.
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Figure 1. Experimental setup.
2. MATERIALS AND METHODS
2.1. Fuel Properties and Characterization. The sewage
sludge sample was collected from a wastewater treatment plant
in northern Italy and then oven-dried and pelletized. The pellet
sample was kept in a sealed container to limit the moisture
uptake. The carbon, hydrogen, and nitrogen contents in the
sample have been determined using an elemental analyzer
(CHN 2000 LECO), with the balance being the oxygen
content. The moisture, volatiles, and fixed carbon and ash
contents have been obtained by thermogravimetric measure-
ments (TGA 701 LECO). The obtained results are reported in
Table S3.
The higher heating value (HHV, MJ/kg on a dry basis) of
the dried samples was measured using an oxygen bomb
calorimeter (Parr model 6200 calorimeter). The measurements
were repeated twice, and the average value was used for
subsequent calculation of the low calorie value (LHV),
according to the well-known correlation described by eq 1
LHVdry = HHVdry − 2.442(8.936Hdry × 100)
(1)
where Hdry represents the weight percent of hydrogen resulting
from elemental analysis and LHV and HHV are given in MJ/
kg.
2.2. Fluidized Bed Gasifier. The scheme of the
experimental setup used for the gasification tests is shown in
Figure 1. The pre-pilot-scale FBR is made from stainless-steel
tubes. The air preheater and electrical resistances allow the
reactor to reach the desired temperature (800−900 °C). In
particular, the air is heated to 600 °C (with a 6 kW heater) and
then flows through the gas distributor.
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The fuel is underbed fed into the reactor by a screw
conveyor, and its flow rate is regulated by a screw feeder. An
auxiliary nitrogen stream is used to insert the fuel feeding
devices and enters the gasifier with the fuel. For the gas
dedusting process, both cyclone and ceramic filters, with a
nominal aperture of 2 μm, are installed. To avoid tar
condensation, the cyclone and the transfer line are maintained
at 450 °C. A flare equipped with a methane pilot flame burns
the syngas coming from the gasifier upstream of the chimney.
The concentrations of CO, CO2, and CH4 gases are measured
online with an ABB continuous analyzer equipped with
infrared (IR) detectors, while the concentration of H2 is
measured with a thermal conductivity detector. Also, an off-
line gas chromatograph analysis is carried out for 3 L gaseous
samples with a thermal conductivity detector to determine the
major hydrocarbon species. When steady state is reached for
each test, the average gas composition is evaluated with an
error of less than 10% on the basis of the last 10 min of
analysis. Tar sampling is performed off-line with a gas
chromatograph equipped with a flame ionization detector
(FID) and according to protocol UNI CEN/TS 15.439
(2006).
2.3. Experimental Conditions. The operating conditions
of the performed gasification tests are listed in Table S4. In
more detail, the bed temperature (T), the unexpanded bed
height (H), and the air flow rate have been kept constant,
whereas the equivalence ratio (ER, i.e., the actual air−fuel
ratio/the air−fuel ratio for complete combustion) has been
changed from 0.15 to 0.30 by varying the fuel flow rate from
7.0 to 3.5 kg/h.
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Figure 2. Aspen Plus system flowsheet.
3. NUMERICAL MODELING
The following assumptions have been made in the present
study to model the air gasification of a biosolid in a fluidized
bed reactor:
• Steady-state, isothermal process,
• Zero-dimensional, kinetic-free model,
• Instantaneous devolatilization of a biosolid,
• Syngas consisting of a mixture of H2, CO, CO2, CH4,
and H2O,
• Reacting system at atmospheric pressure,
• Tar formation is not modeled.
The simulation model was set up using Aspen Plus
commercial software with external Fortran modules. The
development of an Aspen Plus model typically involves the
following steps: (1) specification of the stream class, (2)
selection of the property method, (3) specification of the
system components from a database and identification of the
conventional and nonconventional ones, and (4) setup of the
process flow sheet using the unit operation blocks and the
mass and energy streams. Then, the feed streams and the unit
operation blocks are detailed.
In the present work, the MIXCINC stream class was chosen
for the simulation because the process includes conventional
gas and liquid phases as well as conventional and nonconven-
tional solid phases (i.e., solid carbon and biosolid). In more
detail, the biosolid was defined as a nonconventional
component by entering its ultimate and proximate composition
under the component attributes of the feed stream (Table S1).
Ashes were also defined as a nonconventional component with
an ash content set to 100%.
The thermodynamic properties of conventional components
were estimated using the Boston−Matthias-modified Peng−
Robinson equation of state, which is suitable for nonpolar or
mildly polar mixtures such as hydrocarbons and light gases.37
Enthalpy model HCOALGEN and density model DCOA-
LIGT were instead selected to calculate the enthalpy and
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density of unconventional components, which use the data
from proximate, ultimate, and sulfur analyses. 35 The
HCOALGEN model includes a number of different
correlations that can be selected by the user to set different
option codes. In the present study, the option code was set to
6-1-1-1, which returns a correlation requiring a user-input
value for the heat of combustion (HCOMB). For the biosolid,
the low calorific value (LHV) listed in Table S3 was taken as
HCOMB.
3.1. Flowsheet Development. In Aspen Plus, there is no
specific block to represent the gasification reactor. Therefore,
to model the fluidized-bed gasification of biosolids, it used a
combination of more blocks (Figure 2), which represent,
respectively, the feedstock decomposition, the reaction
between the decomposition products and the gasification
agent (gasification process), and the separation of the inert
matter and the unreacted char in the feedstock (ashes) from
the gasification products.
3.2. Blocks and Streams Description. 3.2.1. Decom-
position. First, the stream FEED consisting of sludge pellets
with a 14% moisture content enters the DECOMP block used
to decompose, at ambient temperature and pressure, the
nonconventional material into its constituent elements (C, O2,
N2, and H2), water, and ash. Specifically, the RYIELD reactor
is used for the DECOMP block because the stoichiometry and
kinetics are unknown, but a yield distribution is known. The
mass yields of the RYIELD reactor (DECOMP) are
determined and set starting from the data of ultimate and
proximate analyses (Table S3) by using a Calculator block (i.e.,
a user subroutine written in FORTRAN) termed FEEDDEC.
The outlet stream (DECFEED) from the DECOMP block
enters the S-CHAR separator to remove unconverted cold char
(C-CHAR) from the main stream just before the gasification
reactor. Regarding the amount of unconverted char from FB
gasifiers, it has been set on the basis of the results from the
experimental tests described in sections 2.2 and 2.3 (Table S5).
The stream C-CHAR is then heated to the gasifier temper-
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Industrial & Engineering Chemistry Research
ature, which is accomplished by using the block entitled C-
HEAT coupled with the TCHAR subroutine written in
FORTRAN and finally mixed with the gas stream leaving the
gasifier by means of the block MIXER.
3.2.2. Gasification. It is well known that the gasification
process does not straightforwardly reach the chemical
equilibrium state because of the short residence time of
gases in the reactor. Accordingly, significant deviations are
typically found between the predicted and the experimental
values of the syngas composition, when equilibrium modeling
approaches (stoichiometric and nonstoichiometric models) are
applied.33
Therefore, to better simulate the nonequilibrium conditions
of real gasifiers, a modified equilibrium model for biosolid
gasification was set in the present work by using the Aspen
Plus RGibbs block with the restricted chemical equilibrium.36
In more details, the restricted equilibrium was established by
selecting the calculation option “Restricted chemical equili-
brium−specify the temperature approach or reactions” in the
RGibbs block. Such an option allows the specification of a set
of chemical reactions with an associated value of the
temperature approach (ΔTapproach), which represents the
difference between the chemical equilibrium temperature and
the real reactor temperature. In more details, this means that,
by specifying a zero-temperature approach value for each
reaction, RGibbs returns the equilibrium gas composition at
the reactor temperature. On the other hand, the possibility to
set an equilibrium temperature different from that of the
reactor (ΔTapproach ≠ 0) allows us to move the reaction
equilibrium versus the reagents or products depending on the
case and hence to modify the composition of the syngas at the
outlet of the RGibbs reactor so as to better simulate the
nonequilibrium conditions of the real gasifier.
The chemical reactions listed in Table S1 are the ones
considered in this work for the gasification process. The
chemistry of the gasifier was calibrated to fit the experimental
data obtained in the pre-pilot-scale FBR by using the “Data
Fit” in the model analysis tools; in particular, this was achieved
by varying the ΔTapproach values for reactions R1 and R3−R5 as
well as the char split fraction in the S-CHAR block, which
allows the model predictions on the gas composition to
converge to the experimental data from Test II shown in Table
S4. The outlet stream from the gasifier is expressed as RAW-
SYNG.
It is worth noting that, in order to simplify the system, the
simulations were carried out under the condition that all of the
energy required for the gasification process comes from the
heat streams (EXTRAQ1 and EXTRAQ2), as shown in Figure
2. Accordingly, because the enthalpy of the DEC-FEED stream
was not equal to the enthalpy of the FEED stream as a result of
the breakup of the chemical bonds, heat stream QDECOMP
was connected between the DECOMP unit and the GASIFIER
to replenish the difference in enthalpy.
3.2.3. Separation. Outlet stream MIXFLOW from the
MIXER block goes to the separation block, CYCLONE, which
separates the unreacted char (fixed carbon) and ash as a stream
(ASH) and the remaining components (H2, N2, H2O, CO,
CO2, and CH4) as the stream (SYNGAS) by using the split
fractionation of the components.
4. RESULTS AND DISCUSSION
4.1. Experimental Results. The two sets of experimental
data on the air gasification of a biosolid in a fluidized bed
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reactor at atmospheric pressure were obtained in a pre-pilot-
scale facility available at the IRC-CNR Institute in Naples
(Figure 1). Table S5 shows the average composition of the
syngas arising from the treatment of biosolid under the
operating conditions listed in Table S4 for both Tests I and II
along with the gas yield (YG), tar concentration, carbon
conversion efficiency (CCE), and cold gas efficiency (CGE).
The ER value exerts a major influence on the promotion of
the oxidation reactions and can express two extreme
conditions. At very low ER (<0.2), the amount of oxygen in
the system is low, leading to incomplete gasification (i.e., high
char content in the ashes) and more tar formation, whereas at
high ER (>0.5), a high flow of air enters the system, thus
promoting complete combustion of the fuel in addition to tar
and char, thereby generating more CO2, H2O, and heat energy
at the expense of the synthesis gas quality and the process
efficiency.38−40
It can be seen that the production of hydrogen, carbon
monoxide, and methane decrease as ER increases while the
total gas yield increases, as a result of full oxidation of the
biomass to CO2. Moreover, the tar produced, carbon
conversion efficiency, and CGE decrease with ER.
The high concentration of nitrogen in the syngas was due to
the use of air as a gasification/fluidization agent. This means
that, although the process is cheaper than with pure oxygen,
the quality of the produced gas is lower.
4.2. Modeling Results. 4.2.1. Model Validation. The
restricted chemical equilibrium model (RCEM) developed in
this work comes from setting the temperature approach for
reactions R1 and R3−R5 (Table S1) equal to −286.52,
−325.80, 282.81, and 71.08 °C, respectively, which are the
values obtained by calibrating the gasifier chemistry to fit the
experimental data from Test II (section 3.2.2). The developed
model has been validated against the experimental data from
Test I (gasification temperature 780 °C and ER 0.15), as
shown in Table S6. Simulation results from the simpler
chemical equilibrium model (CEM with no restricted
equilibrium approach) are also shown in Table S6 for
comparison.
Satisfactory agreement between the RCEM simulation
results and the experimental data emerges. For example, H2,
CO, and CO2 data are predicted with an average error of
within 15% and are significantly lower than those associated
with CEM simulations (from 60 to 95%). These findings are
consistent with those obtained by Marcantonio et al.,41 who
recently modeled the gasification of “lignocellulosic residues”
in a fluidized bed reactor. On the other hand, a greater error
resulted in the simulation of the syngas lower heating value,
which can be mostly ascribed to the overprediction of CH4.
The under- or overprediction of CH4 is a common problem for
gasification modelers; one example is the steady-state model of
a biomass fluidized bed gasifier reported by Doherty et al.,42
where CH4 was overpredicted by a substantial amount
(CH4,exp = 3.4% vs CH4,model = 7.7%, leading to a relative
error of about 125%). Furthermore, Prins et al.43 stated that
the product gas from fluidized bed gasifiers generally contains
much more CH4 than predicted.
4.2.2. Sensitivity Analyses. Sensitivity analyses were
performed with the aim of investigating the influence of
various parameters on the biosolid gasification in a fluidized
bed reactor. In particular, the present study focuses on the
influence of the gasification temperature, the equivalence ratio
(ER), and sludge pretreatments (i.e., digestion, carbonization,
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torrefaction, and copelletization with solid fuels and hydro-

thermal treatment) on both the syngas quality (composition
and LHV) and the efficiency (CGE) of the gasifier.
4.2.2.1. Effect of Gasification Temperature. In the model,
the gasification temperature depends on the temperature of the
gasification agent (air) entering the gasifier; namely, it is
controlled by changing the heat stream to the air preheating
unit in the flowsheet shown in Figure 2. In particular, in the
present work, the heating stream was set so as to ensure a
gasification temperature (i.e., a product gas temperature) of
between 600 and 900 °C at a given constant equivalence ratio
(ER = 0.3). The influence of the gasification temperature on
the product gas composition is illustrated in Figure 3. It can be

Figure 4. Effect of gasification temperature on the LHVgas and CGE.

Figure 3. Effect of gasification temperature on syngas composition.

observed that the concentration of hydrogen and carbon

monoxide increases with the increase in temperature, whereas
the concentration of methane slightly decreases with gas- Figure 5. Effect of equivalence ratio on syngas composition.
ification temperature. These observations can be justified by
the fact that the water−gas reaction raises the production of
carbon monoxide and hydrogen.39 Also, the reverse methana-
tion reaction is thermodynamically promoted at higher
temperatures.
As a result, the LHV of syngas produced and CGE increases
with temperature as illustrated in Figure 4. With regard to the
influence of the gasification temperature on the process
performances, this finding agrees with other published
work.26,39,44
4.2.2.2. Effect of Equivalence Ratio. The equivalence ratio
is an important gasifier design parameter. It is the ratio of the
actual air−fuel ratio to the stoichiometric air−fuel ratio.
Because the complete oxidation of the fuel has to be avoided in
gasification processes, the amount of air entering the reactor is
typically set much lower (ER = 0.2−0.5) than the
stoichiometric conditions required for complete combustion. Figure 6. Effect of equivalence ratio on the LHVgas and CGE.
Figures 5 and 6 show the effect of varying the equivalence
ratio (within the 0.1−0.5 range) on both the syngas quality
(composition and heating value) and the process efficiency literature.34,45 The influence of ER on LHV and CGE is shown
(CGE) at a fixed syngas temperature (780 °C). in Figure 6. Results show that while the LHV gradually
Simulation results show that the production of carbon decreases with increasing ER, a different trend was observed
monoxide and light hydrocarbons (i.e., methane and ethane) for the CGE, which can be ascribed to the different impact of
decreases gradually as ER increases, whereas the hydrogen ER on the syngas flow rate (kg/h).
content exhibits a slight increase only for ER values from 0.1 to 4.2.2.3. Effect of Different Sludge Pretreatments. The
0.3, remaining virtually unchanged for higher values (Figure 5). impact of several sludge pretreatments, namely, digestion,
The trend in syngas quality follows the same trend as in the torrefaction, hydrothermal treating (HTC), carbonization and
304 DOI: 10.1021/acs.iecr.9b03902
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copelletization with solid fuels, was considered by changing the
sludge composition in the model in line with experimental data
from the pertinent literature. In more detail, the composition
of treated sludges was borrowed from studies by Isemin et al.46
for the digestion and torrefaction at 200 and 300 °C, by
Merzari47 for sludge hydrothermal carbonization, by Draper48
for sludge carbonization, and by Constantinescu et al.49 for the
copelletization of sludge with beech sawdust (S+BS) and
lignite (S+L) in a 50:50 ratio by mass.
Table S7 shows the proximate and the ultimate composi-
tions of pretreated sludges, which are next gasified with air at
780 °C and ER 0.2 by assuming the same moisture content for
each of them (i.e., 10%). The elemental analysis data relative to
the investigated sludge samples are also shown in Figure 7 as
Figure 7. Van Krevelen diagram for the investigated fresh and
pretreated sludge samples.
expressed in terms of O/C and H/C elemental ratios on a dry
ash-free (daf) basis (Van Krevelen diagram) to better highlight
the difference in the composition as induced by the
investigated sludge pretreatments.
It is worth noting that because of the lack of experimental
data on the proximate composition of the raw S1 sludge
subjected to digestion and torrefaction treatments by Isemin et
al.46 as well as the similarity of the S1-sludge elemental
composition50 to that of the sludge used in Tests I and II, the
latter was assumed to be the raw feedstock for digestion and
torrefaction experiments. Because the feedstock moisture
content is well known to affect the syngas composition,51 the
same value (i.e., 10% moisture) was assumed for all of the
investigated raw and pretreated sludges during their air
gasification.
The obtained simulation results are shown in Table S8. In
line with experimental results by Xie et al.,51 the anaerobic
digestion process of sludge slightly reduces the gas quality, as
evidenced by the decrease in the H2/CO ratio and the rise in
the CO2/CO ratio. Moreover, the content of combustible
gases from the digested feedstock (DG-S1) is lower than that
of the untreated one (Raw-S1), thus resulting in a lower LHV
and CGE. Similar but even worse results were obtained
following the sludge treatment via carbonization, hydro-
thermal, and copelletization processes. However, it is worth
noting that the decrease observed in the syngas quality (cf. the
H2/CO, CO2/CO and LHV values) and the gasification
process performance (CCE and CGE) for DG-S1, Hydrochar-
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S2, Char-S3, S4+BS, and S4+L samples I is mostly due to
different kinds of changes in the sludge composition as clearly
emerges from the Van Krevelen diagrams shown in Figure 7. In
particular, while an undesired increase in the O/C ratio
occurred for sludges subjected to anaerobic digestion (DG-S1)
and copelletization (S4+BS and S4+L), also associated with a
marked decrease in H/C in this latter case, a remarkable
decrease in the carbon and hydrogen content was observed
following the carbonization treatment, which also led to a
significant increase in the sludge ash content. Again, data show
that the quality of syngas arising from the air gasification of
torrefied T220-DG-S1 and T300-DG-S1 sludge is higher than
that of the parent feedstock (DG-S1) and increases with the
increase in the severity of the torrefaction treatment, namely,
the increase in the torrefaction temperature. In more details, it
results that the torrefied feedstocks produced more H2 and CO
and less CO2 than the parent one, thus resulting in a higher
LHV. This result is consistent with what was observed by
Brachi et al.29 and Anukam et al.,52 who investigated the
influence of torrefaction on the gasification processes of
tomato peels and sugar cane bagasse, respectively. The major
drawback associated with such a treatment is that the particle
conversion efficiency (CCE) is lower for torrefied materials
presumably because of the lower volatile content.53 The lower
CGE associated with T220-DG-S1 and T300-DG-S1 feed-
stocks is probably due to the fact that the LHV of torrefied
sludges increases to a greater extent than that of the associated
syngas.
This confirms that torrefaction is the most suitable feedstock
pretreatment for sludge gasification among the investigated
ones.
5. CONCLUSIONS
A computer simulation model of the thermochemical trans-
formation of biosolids to chemical energy through air
gasification was developed using Aspen Plus. The aims of
this work, which were to develop a model for the biosolids
gasification process in a fluidized bed reactor, to validate it
against actual pilot-scale plant data, and utilize it to examine
the influence of the main operating parameters on gasifier
performance, were achieved. The model is based on the
chemical reactions of methanation, the water gas shift, water
gas, hydrogen, ethene, and carbon combustion and on the
setting of the temperature approach for these. Model validation
was carried out through a comparison with experimental data.
Good agreement between the experimental data and the
properties of the syngas, predicted by the model, was found.
This means that the developed model is capable of predicting
gasifier performance accurately over a wide range of operating
conditions and biosolid properties. The influence of some
sludge pretreatments (i.e., digestion, torrefaction, hydro-
thermal treatments, carbonization and copelletization with
biomass) on the gas composition, heating value, syngas yield,
carbon conversion efficiency and cold gas efficiency was also
investigated. The results suggest torrefaction combined with
gasification as a suitable technology for biosolids valorization.
Further studies will be conducted to investigate the
feasibility of this potential source for the production of energy
via combined heat and power (CHP) applications.
DOI: 10.1021/acs.iecr.9b03902
Ind. Eng. Chem. Res. 2020, 59, 299−307
Industrial & Engineering Chemistry Research
■
*
ASSOCIATED CONTENT
S Supporting Information
The Supporting Information is available free of charge at
https://pubs.acs.org/doi/10.1021/acs.iecr.9b03902.
List of reactions, summary of key research on the
gasification of sewage sludge; biosolid composition and
heating values; overview of operating conditions used for
the gasification tests; average concentration of syngas,
tar produced, gas yield, carbon conversion efficiency,
and CGE in each test; comparison of model results with
experimental data; characteristics of the different
modeled sludges; and comparison of the model results
for the four raw and pretreated sludge samples (PDF)
■
AUTHOR INFORMATION
Corresponding Author
*Phone: +39 3401718890. E-mail: ashraf.abdelkhalig@
uniparthenope.it.
ORCID
Ashraf Abdelrahim: 0000-0001-5255-5049
Paola Brachi: 0000-0003-2584-1394
Notes
The authors declare no competing financial interest.
■
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307 DOI: 10.1021/acs.iecr.9b03902

Ind. Eng. Chem. Res. 2020, 59, 299−307