Fuel 117 (2014) 870–875

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Fuel
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Co-gasification of petroleum coke and biomass

Vera Nemanova ⇑, Araz Abedini, Truls Liliedahl, Klas Engvall
Department of Chemical Engineering and Technology, Chemical Technology, KTH Royal University of Technology, 100 44 Stockholm, Sweden

h i g h l i g h t s

 Co-gasification of biomass and petroleum coke in an atmospheric bubbling fluidised bed and thermogravimetric analyzer.
 Synergetic effect between biomass and petroleum coke was observed.
 The activation energy for pure petcoke is 121.5 kJ/mol, for the 50/50 blend it is 96.3, and for the 20/80 blend – 83.5 kJ/mol.
 Biomass ash has a catalytic effect on the reactivity of petcoke due to the alkali and alkaline earth metals present in ash.

a r t i c l e i n f o a b s t r a c t

Article history: Gasification may be an attractive alternative for converting heavy oil residue – petroleum coke into valu-
Received 4 July 2013 able synthetic gas. Due to the low reactivity of petroleum coke, it is maybe preferable to convert it in
Received in revised form 5 September 2013 combination with other fuels such as biomass. Co-gasification of petroleum coke and biomass was stud-
Accepted 17 September 2013
ied in an atmospheric bubbling fluidised bed reactor and a thermogravimetric analyser (TGA) at KTH
Available online 12 October 2013
Royal University of Technology. Biomass ash in the blends was found to have a catalytic effect on the
reactivity of petroleum coke during co-gasification. Furthermore, this synergetic effect between biomass
Keywords:
and petcoke was observed in the kinetics data. The activation energy Ea determined from the Arrhenius
Activation energy
Biomass
law for pure petcoke steam gasification in the TGA was 121.5 kJ/mol, whereas for the 50/50 mixture it
Co-gasification was 96.3, and for the 20/80 blend – 83.5 kJ/mol.
Fluidised bed Ó 2013 Elsevier Ltd. All rights reserved.
Petroleum coke

1. Introduction demand in aluminium and electrode industries. In 2005 more than

Currently, the world production of petroleum coke is steadily
expanding due to an increased consumption of oil and oil-related
products [1–3]. The low price, high calorific value, low ash content
and abundant availability of petcoke make it a very attractive fuel.
Petroleum coke (petcoke) is a by-product produced from heavy
crude oil residues by thermal cracking processes – delayed or fluid
coking (Fig. 1). Bayram et al. [4] reported that from 1 tonne of
crude oil approximately 31 kg of petcoke is produced. Petroleum
coke is a black solid material consisting of polycyclic aromatic
hydrocarbons with low hydrogen content. The typical elemental
composition of petcoke depends on the crude oil origin, but usually
it is composed of C: 91–99.5%, H: 0.035–4%, S: 0.5–8%, (N + O):
1.3–3.8% and the rest is metals [5].
The manufacture of carbon anodes for the aluminium smelting
industry, graphite electrodes for steel production and also nonfer-
rous industries are the main non-energy applications of petcoke
[5]. In Russia petcoke usage is higher than supply due to the
⇑ Corresponding author. Tel.: +46 768447559.
E-mail address: nemanova@kth.se (V. Nemanova).
650 thousand tonnes of petroleum coke were imported from China
(65%), Turkmenistan, Japan, Kazakhstan, England and the United
States [6].
According to Akpabio and Obot [7] around 75% of the world’s
petroleum coke is used in the energy sector (mostly in North
America). In the past, petroleum coke has often been burned as fuel
in boilers for heat and power production. However, the current
increasing use of natural gas, which is more convenient and clea-
ner to burn, has decreased the demand for petcoke [8]. Therefore,
new alternatives for utilisation of petroleum coke are of interest.
Gasification may be an effective option for converting petcoke into
syngas [9].
Gasification is a thermo-chemical process in which feedstock
undergoes partial oxidation reaction with an oxidising medium
(oxygen, air, carbon dioxide or steam) to produce permanent gases.
The process consists of several steps: drying, pyrolysis, gasification
and combustion, occurring simultaneously inside a gasifier. The
product composition, including solid, liquid and gas phases,
depends on feedstock (type of fuel, moisture, composition) and
gasification operating conditions (oxidising medium, gasifier type,
temperature, pressure etc.) [10].

0016-2361/$ - see front matter Ó 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.fuel.2013.09.050
 V. Nemanova et al. / Fuel 117 (2014) 870–875 871

Table 1
Ultimate and proximate analysis of pine pellets and petroleum coke.

Pine pellets Petroleum coke

Proximate analysis, as delivered
Moisture, wt% 4.5 0.5
Ash, wt% 0.5 1.4
Volatiles, wt% 76.5 6.0
Fixed carbon (by diff.), wt% 18.5 92.1
Lower heating value (MJ/kg) 19.2 36.2
Ultimate analysis, dry basis
Carbon, wt% 47.7 92.3
Hydrogen, wt% 6.3 3.4
Nitrogen, wt% 0.16 0.95
Oxygen (by diff.), wt% 45.3 0.7
Sulphur, wt% <0.012 1.168

At first glance petroleum coke seems to have better properties

compared to biomass, such as higher heating value and higher car-
bon content. However, petcoke also contains significantly more
sulphur. Pinto et al. [21] have examined the influence of different
catalytic materials on removal of sulphur and halogens compounds
Fig. 1. Schematic view of petroleum coke production from crude oil. during co-gasification of coals with different types of wastes, such
as pine, petcoke and polyethylene. They reported that the presence
of dolomite in the bubbling fluidised bed led to the highest sulphur
Due to the high fixed carbon content in petroleum coke, it may
reduction. However, this paper focuses on the gasification process
be complicated to gasify separately [11,12]; therefore it is, perhaps,
and does not touch upon sulphur contamination or the conse-
preferable to convert petcoke in combination with additional fuels
quences thereof.
such as coal or biomass.
Fermoso et al. [13–15] investigated gasification of a mixture of
coal, petcoke and biomass at atmospheric and high pressure in a 2.2. Gasification setup
fixed bed reactor. The results showed that binary (coal–biomass)
and ternary blends (coal–petcoke–biomass) have some synergetic Two series of experiments have been carried out: gasification
effects that enhance gas production. tests performed in 5 kW bubbling bed and thermogravimetric
Zhan et al. [12] used a thermogravimetric system, TherMax 500, analyses of different mixtures of petroleum coke and biomass in
to gasify Chinese petroleum coke and lignite with carbon dioxide. the thermogravimetric analyser (TGA).
They reported low reactivity of petcoke, due to its small BET sur- The atmospheric fluidised bed gasification system includes a
face area and carbon network structure similar to graphitic carbon. fuel feeder, a gas supply system, gas preheater, and a bubbling flu-
However, when petcoke was mixed with lignite the reactivity idised bed gasifier. A schematic view of the gasifier is shown in
increased. Fig. 2.
There are also other studies where petcoke is gasified using dif- The gasification reactor consists of a fluidised bed (an inner
ferent catalysts to increase its low reactivity. Zhou et al. [16] tested diameter of 0.05 m and a height of 0.30 m) and a freeboard (a
the catalytic activity of iron species for CO2 petcoke gasification.
They found that the gasification reactivity of petroleum coke was
enhanced with higher gasification temperature and increasing iron
species concentration.
Several researchers have carried through simulations and
modelling in regard to petcoke conversion into permanent gases
[17–19], and others have investigated co-gasification of petcoke
and coal [1,11,20] and the ternary mixture (petcoke–coal–biomass)
[13–15]. However, there are no studies on co-gasification of pet-
coke and biomass. The aim of the present work is to investigate
the effect of biomass on the reactivity of petroleum coke by
co-gasifying in a bubbling fluidised bed reactor. Several tests with
different petcoke contents mixed with biomass have been carried
out in the gasifier. The reactivities of petcoke, biomass and various
petcoke–biomass blends were also determined by thermogravi-
metric analysis.

2. Materials and methods

2.1. Materials

Pine pellets in the size range of 1.5–2 mm and ground and

sieved petroleum coke (1–1.5 mm) provided by Statoil, Norway
were used in the experiments. The results of ultimate and proxi-
mate analysis are listed in Table 1. Fig. 2. Schematic view of the KTH atmospheric fluidised bed reactor.
872 V. Nemanova et al. / Fuel 117 (2014) 870–875

diameter of 0.10 m and a height of 0.45 m). The total volume of the
reactor is 5.1 L. The reactor is heated with external heaters and the
maximum temperature is 950 °C. The bed material in the reactor is
350 g a-alumina with a particle size of 63–125 lm and density
3960 kg/m3. The fluidisation medium is nitrogen while the oxidis-
ing agent is pure oxygen. Before entering the reactor the fluidisa-
tion and oxidation media are pre-heated to 650 °C. When the
system is heated up to the desired temperature the fuel is fed, with
help of a screw feeder, directly into the fluidised bed near the gas
distribution plate at the bottom. The fuel hopper is provided with
nitrogen purge and a cooling system to prevent hot gases from
entering the hopper and making the fuel sticky.
After each experiment the remaining fuel and bed material
were weighed in order to calculate the unconverted fuel content
and as well as the feeding rate. The unconverted material was
sieved and the fractions of unconverted petcoke and biomass were
determined.
The cool, dry, clean gas composition was analysed with a gas
chromatograph (GC), equipped with a flame ionisation detector Fig. 3. Carbon mass balance for experiments.
(FID) and a thermal conductivity detector (TCD).
The tar sampling and analysis were accomplished using the
solid phase adsorption (SPA) method. In this method, a 100 ml For all gasification experiments the carbon mass balance was
gas sample is manually drawn through a solid phase extraction calculated based on fuel input (carbon content) and output (gas
(SPE) tube during 1 min. Later the SPE tube is eluted using two composition measured by GC, tar content and measured uncon-
different solvent mixtures to obtain an aromatic fraction and a verted char from biomass and petcoke) and the results are shown
phenolic fraction. The eluates are afterwards analysed by gas in Fig. 3.
chromatography. The details of the SPA method is described The found carbon mass balance is in the range of 92–98%. Light
elsewhere [22]. carbons CxHylight include CH4, C2H2, C2H4 and C2H6. Heavy carbons
Gas composition and tar samples were both taken every 10 min, CxHyheavy (tar) are hydrocarbons with a molecular mass higher than
after the system was in the steady-state condition. The data re- benzene. One interesting observation is that the amount of uncon-
ported is an average of the 12–15 gas and tar values. verted biomass in the different blends seems to be almost constant
in all experiments and does not depend on the gasification temper-
2.3. Thermogravimetric setup ature, oxygen concentration or petcoke content in the blend. Pet-
coke conversion in the blends increases with higher gasification
Thermogravimetric analysis was carried out using a Netzsch temperature (compare experiments II and IV) and higher oxygen
STA 449 F3 Jupiter apparatus, equipped with an electrical steam content in the input gas (experiments IV, V). It can also be observed
furnace with a maximum working temperature of 1250 °C. Steam that the more petcoke in the mixture, the higher the content of
was generated in a Bronkhorst High-Tech unit and led with a rate unconverted petcoke (experiments II and III).
of 86 ml/min together with nitrogen of high purity (99.99%) (a The main results, such as unconverted matter in the bed, prod-
rate: 67 ml/min) through a transfer line, heated up to 200 °C to uct gas composition, total tar concentration and benzene, fuel
avoid steam condensation. In the thermogravimetric analyser, conversion and product gas yield during co-gasification, are listed
the same nitrogen at a flow rate of 100 ml/min was used as protec- in Table 3. Conversion of biomass, petcoke and overall process is
tive gas. The original petcoke was milled and a 100 mg sample was calculated based on fuel input (Table 2) and output (Table 3),
heated to the desired 1200 °C at a rate of 10 °C/min, at total pres- respectively.
sure of 1 bar. The lowest overall conversion was found in the 50/50 petcoke/
All experiments were performed two or three times in order to biomass blend. Using a 20/80 mixture it may be possible to
examine the reliability of the test data. The results for the same enhance the overall conversion from 85.2% to 89.6% by increasing
tests showed a good reproducibility (<3%). gasification temperature from 800 to 900 °C; by raising oxygen
concentration in the fluidisation gas from 11% to 14% the overall
conversion may be increased further up to 90.8%. Petcoke conver-
3. Results and discussion
sion in a 20/80 mixture increases by 19% when the gasification
3.1. Gasification tests temperature is raised by 100 °C (experiments II and IV) and a
further 8.6% when the concentration of oxygen in the input gas is
The gasification conditions for the five experiments are summa- increased by 3%. Biomass conversion four of the experiments is
rised in Table 2. 94–95%, and only in the test with high petroleum coke content
(experiment III), the conversion decreases to around 90%.
Table 2
Gasification operating conditions. The product gas yield decreases with higher petcoke content in
the mixture due to a higher percentage of unconverted petcoke.
Gasification test I II III IV V
More gas is obtained at higher gasification temperature and oxy-
Petcoke concentration, % 0 20 50 20 20 gen content due to higher fuel and tar conversation (tests IV and
Petcoke fed, g 0 117 292 117 117
V). The gas composition at a gasification temperature of 800 °C
Biomass fed, g 569 467 292 467 467
Total gasification time, min 185 166 150 158 159 for different blends can be considered constant: the CO2 concentra-
Bed temperature, °C 800 800 800 900 900 tion is the range of 23–24%, H2 29–33%, CH4 8–9% and CO content
Nitrogen flow rate, L/min 8.45 8.45 8.45 7.90 7.64 in the range of 33–37%. At the higher temperature, 900 °C, the
Oxygen flow rate, L/min 1.08 1.08 1.08 1.00 1.24 main differences in the gas composition can be observed for CO2
Oxygen concentration, % 11 11 11 11 14
and CO (experiments II and IV): the CO2 concentration is strongly
 V. Nemanova et al. / Fuel 117 (2014) 870–875 873

Table 3
Results of gasification tests with biomass and petcoke-biomass blends.

Gasification test number I II III IV V

Unconverted material, g
Biomass 30 25 28 22 29
Petcoke – 61 161 39 25
Total 30 86 189 61 54
Conversion, %
Biomass 94.9 94.6 90.4 95.3 94.6
Petcoke – 47.6 44.8 66.7 75.3
Overall 94.9 85.2 67.6 89.6 90.8
Product gas yield, Nm3 dry/kg fuel 1.18 1.02 0.87 1.18 1.21
Fuel residue, g/kg fuel 52.7 140.6 346.2 107.2 77.3
Tar content, g/Nm3 dry (excluding benzene) 1.9 1.2 1.1 0.9 0.8
Benzene, g/Nm3 1.5 1.1 1.1 1.5 1.6
Gas composition, vol.% dry gas, N2
Free 24.1 23.2 23.3 7.3 7.2
CO2 29.3 29.5 31.4 30.8 28.4
H2 8.1 9.2 9.1 6.4 7.2
CH4 37.0 36.5 34.8 54.9 55.9
CO 1.5 1.6 1.4 0.6 0.8
C2H2 C2H4

reduced from 23% to 7% and the CO content is increased from 36%
to 55%.
This effect can be explained by water–gas shift reaction:
CO þ H2 O $ CO2 þ H2 þ 41 kJ=mol
The tar content in the product gas diminishes with higher
gasification temperature and higher oxygen concentration (exper-
iments IV and V); these factors that have been reported in the lit-
erature [23]. Tests I–III indicate that most of tar in the gasification
gas originates from the biomass: the less biomass in the mixture,
the lower total tar concentration in the product gas.
Normally, benzene is not classified as a tar component. How-
ever, it is a precursor for carbon deposition in downstream
catalytic processes. Benzene is also an important product and an
intermediate in the complex tar reaction network of cracking
heavier tars. As summarised in Table 3, benzene presence in the
product gas approximately equals the sum of the tar components.
In contrast to total tar content versus temperature dependence, the
concentration of benzene in the product gas increases with higher
gasification temperature and higher oxygen content in the fluidisa-
tion gas. This fact can be explained by thermal cracking of heavier
tars into smaller molecules including benzene [24]; the detailed tar
content is thus needed.
Fractions of the different tar components in the product gas
were measured and the concentration of each tar component in
the total tar was calculated, the results are given in Table 4. The
molecular mass of the chromatographically determined tar
compounds were in the range between 78 and 202 g/mol.
The higher the gasification temperature (experiment IV), the
amounts of toluene and indene are significantly lower compared
to the experiment conducted at 800 °C (test II).
According to Devi et al. [24] and Milne et al. [25], naphthalene is
the main and most stable component of the tar compounds. As
shown in Table 4 naphthalene concentration is in the range of
36–52% of the total tar content, independently of the gasification
temperature. Toluene, indene, acenaphthylene and phenanthrene
are present in the range of 23–39% of the total amount.
3.2. Thermogravimetric analysis (TGA)
In order to investigate the co-gasification of petcoke and bio-
mass in detail, thermogravimetric tests were performed.
Steam gasification of various blends of petcoke and biomass
was carried out in a thermobalance. The thermogravimetric curves
(the mass losses), obtained for biomass and petroleum coke, are
illustrated in Fig. 4.
As shown in Fig. 4, biomass gasification occurs in two steps: fast
pyrolysis (in the temperature range of 200–400 °C) and subsequent
slow gasification of the char remaining from biomass in the tem-
perature range of 400–900 °C.
Petroleum coke has very low reactivity due to its aromatic
nature and high heavy aromatic-to-aliphatic ratio [4]. It has previ-
ously been reported that aromatic carbon atoms are less reactive
than aliphatic carbons [26]. Gasification of petcoke commences

Table 4
GC-detectable tar components in the product gas (% of total tar, excluding benzene).

I II III IV V
Toluene 18.4 12.9 12.1 2.3 2.8
m/p-Xylene 1.1 2.1 4.5 5.1 5.6
Indan 5.4 1.4 2.3 3.1 3.0
Indene 10.4 10.0 10.9 5.1 5.6
Naphthalene 44.7 42.3 36.4 44.2 51.3
1-Methylnaphthalene 1.3 1.0 2.3 2.2 2.2
Acenaphthylene 8.3 8.6 9.2 14.0 9.8
Fluorene 2.0 3.2 3.2 0.9 0.9
Phenanthrene 4.4 8.6 9.0 9.9 7.2
Anthracene 1.2 2.7 2.5 1.2 0.7
Fluorantene 1.4 3.6 4.0 5.9 5.2
Pyrene 1.3 3.5 3.7 6.1 5.9
Fig. 4. Steam gasification of petcoke and biomass using TGA.
874 V. Nemanova et al. / Fuel 117 (2014) 870–875

at temperatures above 800 °C (Fig. 4), when the biomass is almost

gasified. In other words, co-gasification of petroleum coke and bio-
mass in the thermobalance does not occur simultaneously, but
sequentially. Therefore, from the curves obtained during single
component gasification, it is possible to calculate new numerical
data for different petcoke–biomass blends based on their relative
proportions in the mixtures using the following equation:

mm ¼ mp x þ mb y ð1Þ

where mm is the mass losses for a given mixture (%), mb, mp is mass
losses for biomass and petcoke at the same temperature, respec-
tively, obtained experimentally (%), x, y is the petcoke and biomass
concentrations in the given mixture (–).
Using the previously mentioned equation new theoretical plots
have been calculated for the mixtures 50/50 (x = 0.5, y = 0.5) and
20/80 (x = 0.2, y = 0.8). Steam co-gasification tests were performed
in the TG for the same blends, and the calculated and experimental
plots are shown in Fig. 5.
Fig. 5A illustrates an excellent correlation between calculated
and experimental data for the mixtures (50/50, 20/80) up to
900 °C (90 min). After 90 min a difference between the theoretical
and experimental values may be noticed (Fig. 6B): gasification of
the 50/50 blend ends 6 min earlier than calculated, for the 20/80
mixture the difference between experimental and theoretical gas-
ification completion is 13 min. In Fig. 5 this is summarised, the
more biomass in the mixture, the higher the difference between
calculated and experimental values, the less time/lower tempera-
ture needed to complete the co-gasification process.
Fig. 6. Relation between reaction rate ln r (min1) and temperature 1000/T (K1).
In accordance with the results obtained during co-gasification,
it can be concluded that there is a synergetic effect between pet-
coke and biomass in high-temperature steam co-gasification due
to biomass residue – ash. In other words, the more biomass ash
in the mixture with petcoke, the faster complete gasification is
achieved. Biomass ash has early been found to have a good cata-
lytic effect on tar reduction [27].
Detailed ash analysis is presented in Table 5. Biomass ash has
more than 65% of alkali and alkaline earth metals (CaO, K2O,
MgO and Na2O) that play a catalytic role in gasification process
[28], whereas petcoke ash has a higher content of nickel and vana-
dium (55%).
The synergetic effect between petcoke and biomass may be
proven by kinetic calculations. The carbon conversion fraction (x)
and the gasification reaction rate (r) were determined using the
following equations:
x ¼ mm0 m
o m
ð2Þ
ash

dx 1
r¼  ð3Þ
dt 1  x
where m0 is the initial mass of the sample (mg), m is instantaneous
sample mass at reaction time t (mg), mash is the ash mass (mg).
The gasification conversion (x) and the gasification reaction rate
(r) for experiments with petroleum coke and the blends (50/50 and
20/80) were calculated using Eqs. (1) and (2), respectively. The
logarithmic reaction rate ln r (min1) versus the reciprocal
gasification temperature 1000/T (K1) for the experiments with
petcoke are shown in Fig. 6.

Table 5
Biomass and petroleum coke ash analysis.

Biomass Petcoke
SiO2 12.8 12.8
Al2O3 1.0 15.4
CaO 33.0 1.5
Fe2O3 1.7 2.9
K2O 23.2 0.6
MgO 5.4 0.6
MnO 3.7 0.0
Na2O 1.7 1.9
P2O5 5.3 0.4
Ba 2.5 2.4
Cu 0.5 1.2
Ni 0.0 27.5
Fig. 5. Experimental and calculated data for 50/50 and 20/80 petcoke/biomass V 0.0 28.4
mixtures. (A) Temperature range 20–1200 °C. (B) Temperature range 900–1200 °C.
 V. Nemanova et al. / Fuel 117 (2014) 870–875
Table 6
Activation energy Ea and pre-exponential factor estimated from r at 850–950 °C.
Ea, kJ/mol A0, min1
100% Petcoke 121.5 3856
50% Petcoke + 50% biomass, experimental 96.3 597
20% Petcoke + 80% biomass, experimental 83.5 299
As can be seen in Fig. 6 the logarithmic gasification reaction rate
ln r exhibits a linear relationship with the temperature, 1/T, the
same dependence was found in the literature [2,16,29–31]. Apply-
ing the Arrhenius Eq. (4), the activation energy Ea and the pre-
exponential factor A0 were calculated; the results are presented
in Table 5.
 
Ea
r ¼ A0 exp
RT
According to the kinetic data listed in Table 6 there is a signifi-
cant synergetic effect between petroleum coke and biomass during
co-gasification: petroleum coke with high biomass ash content has
remarkably higher reactivity with steam than pure petcoke. The
catalytic effect of mineral content in the carbonaceous material
on the petroleum coke reactivity has also been noticed in the work
by Harris and Smith [31].
4. Conclusions
Co-gasification testes of petroleum coke and biomass were con-
ducted at KTH Royal University of Technology. The first part of this
study was performed in the 5 kW atmospheric fluidised bed reac-
tor. Operating temperature in the bed was 800 and 900 °C, oxygen
was used as oxidising medium. Petroleum coke/biomass blends
were used in the proportions of 0/100, 20/80 and 50/50. Higher
gasification temperature (900 °C and above) and higher oxygen
concentration in the fluidising gas are favourable for high petcoke
conversion. By raising temperature in the reactor by 100 °C and
oxygen concentration by 3% it is possible to increase the petcoke
conversion in a 20/80 mixture from 47.6% to 75.3% and the total
conversion from 85.2% to 90.8%. Moreover, the tar concentration
in the product gas decreases from 1.2 to 0.8 g/Nm3.
The second part of the present work was dedicated to non-iso-
thermal steam gasification tests in a thermogravimetric analyser.
The same petroleum coke/biomass blends were heated up to
1200 °C at a rate of 10 °C/min, with a total pressure of 1 bar. Higher
biomass content in the mixture leads to shorter gasification finish-
ing time than calculated (6 min difference for the 50/50 mixture
and 13 min for the 20/80). Alkali and alkaline earth metals from
biomass ash increase the reactivity of petroleum coke during co-
gasification. This synergetic effect between biomass and petcoke
was proven by kinetics data. The activation energy Ea, determined
from the Arrhenius law, was 121.5 kJ/mol for pure petcoke steam
gasification, whereas for the 50/50 mixture it was 96.3 and for
the 20/80 blend – 83.5 kJ/mol.
Acknowledgment
The research is supported by the Swedish Energy Agency
(Energimyndigheten).
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