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Estimation of Carbon Dioxide Emissions in Rotary Hearth Furnace Using a


Thermodynamic Model

Article  in  Steel Research International · May 2017


DOI: 10.1002/srin.201600265

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FULL PAPER
Estimation of Carbon Dioxide Emissions in Rotary
Hearth Furnace Using a Thermodynamic Model
Binay Kumar, Srinibash Mishra, Gour Gopal Roy, and Prodip Kumar Sen

A thermodynamic model has been developed for the estimation of carbon dioxide (CO2)
emissions from rotary hearth furnace (RHF) using different reductant coals and external
fuel gases for the production of sponge iron. The model developed incorporates coal
pyrolysis and ore reduction. Output predictions including coal and fuel gas additions are
computed under no heat loss condition and the stoichiometric addition of the reductant
carbon. Validation with available data from literature has been carried out. The external
fuel gas quantity is determined by calculating adiabatic flame temperature (AFT) and heat
requirement in the reduction zone using software FactSage 6.4. Total iron present in the
sponge is variable depending on the reductant coal and sponge metallization. Combustion
products of producer gas and syn gas may be oxidizing to the metallic iron in the reduction
zone unless extra coal is added. The CO2 emission potential is computed based on complete
combustion of the exit gas from RHF. The emission is estimated to vary from 1.29 to 1.34
ton CO2/ton of sponge for a high VM and low ash coal, depending on external fuel. The
optimum post-combustion inside the reduction zone is found to be 20% under conditions of
stoichiometric coal rate.

1. Introduction loaded with thin stationary layers of prepared raw charge


on a flat, rotating refractory hearth.[1]
Presently, most of the iron is produced through blast Typically, the feed materials of the RHF process consists
furnace route, which requires metallurgical coke. The of composite pellets made from a mixture of iron ore fines
depletion of coking coal reserves and growing environ- and non-coking coal fines. The feed composite pellets are
mental concerns have motivated researchers to search for placed on the hearth one or two layers thick. Burners
coke-free iron ore reduction processes leading to alterna- located above the hearth provide the heat required to raise
tive routes of iron making. One class of methods is directed the composite pellets to reduction temperature and start
at the production of iron nuggets/sponge using iron ore the process. The burners are fired with fuel gases or oils like
fines and non-coking coal fines in the form of pellets. The natural gas, fuel oil, waste oil, etc. Most of the heat required
sponge/nuggets are then smelted separately. The other for maintaining the process is supplied by combustion of
class of methods directly produces molten iron. Several fuels. In this process, the temperature of the reduction
variants of RHF technologies aimed at sponge/nuggets zone is variable (1150–1400 8C).
production have evolved such as Inmetco, Fastmet, The composite pellets are fed and discharged continu-
Fastmelt, and ITmk3. It is claimed that these processes ously and stay on the hearth for only one revolution.
reduce CO2 emission, although specific data on cases are Reduction time of composite pellets is typically
lacking. 6–12 min,[2] depending on the reactivity of the composite
RHF process is a coal-based direct reduction process pellets and end product quality. The residence time varies
that uses iron ore fines and non-coking coal fines to with the properties of the iron oxide feed stocks. The
produce premium-quality sponge iron or iron nuggets. reduction of the iron oxides is achieved by the reaction of
From the operational angle, RHF is a modified tunnel kiln carbon contained in the reductant coal with the iron
oxides, generating in situ carbon monoxide (CO) gas. The
final products are in the form of sponge iron or iron
[] B. Kumar, S. Mishra, Prof. G. G. Roy, Prof. P. K. Sen nuggets depend on the degree of reduction. After
Department of Metallurgical and Materials Engineering, IIT Kharagpur, reduction, sponge iron or iron nuggets is discharged out
Kharagpur 721302, India
Email: prodipksen@outlook.com
of the RHF and recycled in a blast furnace (BF), basic
oxygen furnace (BOF), or electric arc furnace (EAF). The
DOI: 10.1002/srin.201600265 exit gas generated in RHF is treated at exit gas treatment

ß 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim steel research int. 87 (2016) No. 9999 1
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facilities. The heat of exit gas can be recovered at boiler and rate, exit gas composition, and volume for known
recuperator (heat exchanger). metallization of the end product. Before this, a base
There has been extensive work performed on the thermodynamic model is developed and validated with
reduction of iron ore–coal composite pellets and its available literature data. The effect of different external fuel
kinetics in RHF experimentally as well as mathematical gases like natural gas, coke-oven gas, syn gas, and producer
modeling.[3–13] But only few work has been reported on gas on exit gas composition and CO2 emissions has been
modeling of RHF for arriving at energy requirements and studied. Effect of reductant coal composition on coal rate
CO2 emission (kg-CO2/ton product iron) of RHF process is also investigated. Finally, the feasibility of post-
routes like Fastmelt and ITmk3. It is reported that energy combustion has been attempted for different external fuel
consumptions and emissions of CO2 from RHF are lower gases and their effect on CO2 emissions is examined to
than in the blast furnace route.[2] But the comparison make the system sustainable.
mentioned above may not give real picture because the
end products in the three cases are not same, viz. blast
furnace and Fastmelt products are in molten form, while
ITmk3 product is in solid form. In another comparison of 2. Thermodynamic Model for RHF Process
CO2 emission (kg-CO2) per ton of hot metal from Fastmelt
and ITmk3 process with a small blast furnace,[14] it is The RHF process is divided into three zones based on its
shown that ITmk3 reduces CO2 emissions by approxi- function as shown in Figure 1. Zone I  Preheating of the
mately 400 kg/THM compared to the small blast furnace. composite pellet from 25 to 400 8C and coal pyrolysis at
From the viewpoint of a life cycle analysis study, a 400 8C. Zone II  Heating of VM free composite pellet from
detailed study on CO2 emissions from ITmk3 process is 400 to 900 8C. Zone III  Reduction of the composite pellet
reported in the literature.[15] Comparison of CO2 emission at 900 8C and heating of sponge iron to 1250 8C. It is
from ITmk3 using natural gas as an external fuel was made assumed that like blast furnace processes, the commence-
with a conventional blast furnace. It was demonstrated ment of Boudouard reaction is at 900 8C, and thus the
that CO2 emission from ITmk3 is less compared with blast minimum reduction temperature is taken as 900 8C.
furnace per ton of pig iron. Also, CO2 emissions from Zone-I is conceptualized to signify preheating of
ITmk3-EAF are compared with those from BF-BOF. The composite pellets from 25 to 400 8C and pyrolysis of coal
comparison is made with and without scrap usage. Due to present in composite pellets at 400 8C. Since primary
the significant CO2 reduction by higher scrap usage ratio, pyrolysis of non-coking coal is starts at around 330–360 8C[18]
steelmaking by EAF takes significant advantage of CO2 and completed at around 500 8C, the pyrolysis temperature
emissions over BF-BOF. Gordon et al.[16] reported that CO2 in the present work is taken as 400 8C (close to the average of
emission per ton of product iron (either a liquid metal or these two temperatures). Zone-I enthalpy includes preheat-
solid DRI) from ITmk3 process is higher than gas-based ing of composite pellets up to 400 8C and decomposition of
DRI processes like Midrex and HYL, but lower than liquid coal and its subsequent transformation to products. The
metal processes such as Blast Furnace, Technored, cracking of coal hydrocarbon present in composite pellets in
Hismelt, Finex, and Rotary kiln with the smelter. It is the absence of air (oxygen) generates gases (major quantity
noted that the reported CO2 emission for ITmk3 is of CH4) and solid char. The generated gas from this zone is
considerably lower than the emission reported by previous the devolatized product gas. This pyrolysis gas is mixed with
work.[2,14,15] CO2 emission as mentioned above from RHF hot gases coming from zone-II. When two streams of hot
process is based on a calculation using natural gas as an gases (pyrolysis gas and hot gases from zone-II) mixed, they
external fuel for heat supply. Tsutsumi et al.[17] reported carry sufficient amount of sensible heat to supply the heat
one demonstration plant that used coke-oven gas as a required in zone-I before coming out from the furnace.
combustion fuel in RHF, but the RHF process performance Consequently, combustion of external fuel is not needed in
report was not provided. Information on the utilization of a zone-I. If the sensible heat of hot gases is not sufficient to
variety of fuel gases is scantily reported. fulfill the heat requirement in zone-I, post-combustion of
Development of a simple and efficient model for the hot gases coming from zone-II in zone-I may provide the
reduction of iron ore in RHF process using a variety of fuel required heat in this zone.
gases is necessary for estimation of CO2 emissions and also After preheating and coal pyrolysis in zone-I, the
to estimate the performance capability of the RHF process composite pellets consist of char and iron oxide only. In
such as fuel rate. zone-II, the VM free pellets are heated from 400 to 900 8C.
In the present study, a thermodynamic model for RHF Therefore, zone-II enthalpy includes preheating of com-
process has been developed which also includes a coal posite pellets (consisting of coal char and iron oxide only)
pyrolysis model. The coal pyrolysis model is used to up to 900 8C from 400 8C. Since in RHF, gases and solids
predict the quantity and composition of VM present in move in opposite direction, the heat required in zone-II
reductant coal based on proximate and ultimate analysis of may be recovered from the sensible heat of hot gases
coal. The model has been used to study the feed material moving from zone-III to zone-II. Zone-III hot gases consist
requirement, zone wise energy requirement, external fuel of gases generated from direct reduction of iron oxide at

2 steel research int. 87 (2016) No. 9999 ß 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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Figure 1. Schematic diagram of the thermodynamic model of RHF process.

900 8C and gas generated due to the complete combustion For computing the quantity, composition, and tempera-
of external fuel gas. ture of the exit gases, the following procedure is followed.
In zone-III, direct reduction of iron oxide takes place at Once the amount of external fuel gas is known, the amount of
900 8C. This reduction reaction is highly endothermic in air required for complete combustion of external fuel gases
nature and to fulfill this heat requirement, combustion of and also the quantity and composition of zone-III gases
external fuel is needed. This zone consumes a majority generated that also includes the CO gas produced from
(more than 56%) of the total heat required in entire RHF. direct reduction of iron ore, are estimated. The hot gases
The enthalpy of zone-III include the heat of endothermic from zone-III proceed to zone-II. With known volume and
reduction of iron ore in the presence of carbon and heating temperature of waste gas from zone-III and an estimate of
of reaction product from 900 8C to an exit temperature of solid heat requirement in zone-II, the exit gas temperature
the final solid product (1250 8C for the present model). This from zone-II can then readily be calculated. Coal pyrolysis in
heat is supplied by combustion of external fuel gases like zone-I requires additional heat which is used to compute
natural gas, producer gas, syn gas, coke-oven gas, etc. solid heat requirement in zone-I including charge preheat-
All the thermodynamic data, for example, heat of ing. Using the volume, composition, and temperature of the
reaction, AFT, exit gas temperature, products of coal gas entering zone-I from zone-II, the gas composition and
pyrolysis, etc. used in this thermodynamic model has been temperature of the exit gas from RHF (V2, T3, Figure 2) are
estimated with the help of software FactSage 6.4.1 predicted. The total quantity of CO2 emitted from the RHF
including its downstream utilization as fuel is readily
estimated based on coal quantity (total carbon), fuel gas
2.1. Computation Approach requirement, and sponge analysis.

For known metallization of the final product (sponge iron or


iron nuggets), iron ore, and reductant carbon quantity is
initially estimated. Based on proximate analysis of coal, the 3. Model Validation
stoichiometric coal quantity required is worked out.
Subsequently, heat requirements in different zones (zone- 3.1. Coal Pyrolysis Model Validation for Zone-I
I, zone-II, and zone-III) of RHF have been estimated. Based
on the net heat demand in zone-III, the amount of external For assessing the contribution of coal pyrolysis toward total
fuel gas is determined once the AFT is calculated using emission, a coal model is developed which can predict the
FactSage 6.4. quantity and composition of VM present in reductant coal.
VM mainly contains CH4 and some CO, CO2, etc. which are
1
FactSage 6.4 is a trademark of Thermfact Ltd., and CRCT also the sources of CO2. Once the ultimate analysis and ash
(Montreal, Canada) and GTT-Technologies (Aachen, Germany). content of the reductant coal are known, with the help of

ß 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim steel research int. 87 (2016) No. 9999 3
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Figure 2. Schematic flow chart of the computational approach of the present model.

FactSage 6.4 software one can estimate the quantity and constituents as obtained from FactSage simulation is
composition of VM present in the reductant coal. readily obtained which provides the VM percentage in coal
The validation of composition and the volatile fraction as well as the FC. These are then compared with literature
is indirectly obtained from the prediction of proximate data.[19] This comparison is shown in Table 1. Based on a
analysis (dry ash basis) of the coal from ultimate analysis satisfactory match of computed FC and VM data with
and ash content. For purposes of validation, for given total literature data, the quantity of gases generated after
carbon (TC) from the ultimate analysis, fixed carbon (FC) pyrolysis is considered to be validated as no direct
and composition and quantity of VM on dry ash basis are measurements have been reported. Thus, for a given coal
computed using equilibrium module of FactSage 6.4 for sample, it is possible to predict both the quantity and
coal pyrolysis at 400 8C. The summation of the volatile composition of the pyrolysis gases once the ultimate

4 steel research int. 87 (2016) No. 9999 ß 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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Literature data WSA FactSage 6.4 results

Sl. No. Coals FC VM TC FC VM TC

1 Bituminous coal (Sample 1) 39.51 19.83 50.23 37.82 21.73 46.65


2 Bituminous coal (Sample 2) 32.46 17.48 41.14 31.22 18.13 39.55
3 Indonesian coal 56.23 28.28 70.36 53.84 29.81 65.99
4 Indian washed coal 43.50 18.67 52.87 42.59 19.05 55.71
5 Imported coal 54.16 39.39 74.24 52.35 40.40 71.70
6 Coal 7 (Jindal) 48.41 19.05 57.67 47.38 19.24 57.47
7 240 60.13 26.38 74.12 59.60 26.10 72.91
8 252 43.94 43.09 66.78 48.73 38.29 69.09
9 263 58.35 32.16 75.40 64.52 25.70 77.00
10 272 50.82 35.29 69.53 58.75 26.37 72.05
11 274 61.89 29.32 77.43 65.12 25.76 76.74
12 281 81.18 8.85 85.87 79.71 10.57 82.44
13 283 55.45 32.30 72.57 61.23 26.23 73.74
14 284 54.88 26.22 68.77 57.95 22.55 70.25
15 296 54.50 30.37 70.59 60.46 23.81 72.25
16 297 41.89 43.81 65.11 45.59 40.11 70.09
17 298 57.30 29.94 73.17 61.78 25.16 73.15
18 299 50.11 26.63 64.22 52.13 25.53 61.39
19 306 60.49 19.35 70.74 61.37 18.52 70.57
20 310 62.80 25.18 76.14 63.85 23.44 75.76

Table 1. Comparison of FC, VM, and TC (dry ash basis) from literature data[19] and FactSage 6.4 simulation.

analysis is known. Table 1 also compares TC (dry ash basis) According to WSA,[20]
computed using world steel association (WSA) ap-
proach[20] and FactSage 6.4. TC is the summation of FC Total Carbon ¼ 100  ½%Ash  0:47½%VM ð1Þ
and carbon present in VM, as obtained through model
predictions.
Equation for TC from regression analysis of literature
A regression equation (Equation 2) is developed
data,[19]
correlating TC with percentage ash and VM in coal and
compared with the formula for estimating TC given by
WSA (Equation 1). The correlation of TC developed from Total Carbon ¼ 100  0:97½%Ash  f0:43½%VMþ 2:59g;
data using FactSage 6.4 is given by Equation 2 with a
correlation coefficient of 0.97. The slight discrepancy R2 ¼ 97:32 ð2Þ
between these correlations may be attributed to a limited
number of coal samples studied in the present study.
Thus, the present correlation may be used to predict the
TC by knowing the proximate analysis of a coal sample. 3.2. Model Validation with ITmk3 Data
The TC value so obtained can be directly used to predict
the total CO2 emissions once fuel gas emissions are The data generated from the present thermodynamic
estimated. model are compared with data available for ITmk3 process

ß 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim steel research int. 87 (2016) No. 9999 5
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in the literature.[15] The present model has been tuned to reductant coals considered in the present study. From
an ITmk3 process for comparison. Table 3, it is clear that majority of the VM present in the coals
The major components of the hematite iron ore used are in the form of CH4. At lower temperature, CH4 and
in the present model are 65.3% Fe, 3.0% Al2O3, and 3.7% H2O are more stable than H2, CO2, and CO and on increasing
SiO2. The reductant coal taken for validating ITmk3 temperature, reforming of CH4 takes place (Equation 3 and
process has 22.9% VM and 8.8% ash in the dry base and 4) and CH4 and H2O converts into H2 and CO and/or CO2.
has 87.3% C, 4.89% H, 0.97% N, 6.23% O, and 0.60% S in Beyond 650 8C CO2 further, converts into CO (Equation 5)
dry ash-free base. Iron nuggets produced from the depending on CO/CO2 ratio.
ITmk3 process typically contain carbon of 2.5–3.0%. For
validating the present model, iron nuggets carbon is CH4 þ H2 O ¼ CO þ 3H2 ð3Þ
taken as 3.0%. In ITmk3 process, since the final product
(iron nugget) is obtained after reduction and melting
(iron and slag are separated), zone-III maximum CH4 þ 2H2 O ¼ CO2 þ 4H2 ð4Þ
temperature is taken as 1400 8C for validation only in
place of 1250 8C (present model exit temperature for
CO2 þ C ¼ 2CO ð5Þ
sponge process). The model predicted information such
as heat requirement in different zones, the amount of
external fuel gas requirements, as well as the compari-
son of model predicted results with literature data, are 4.1.2. Calculation of Heat of Decomposition (HOD) of
provided in Table 2. Additionally, gas temperature and Reductant Coal
volume at different zones, and calorific value (CV) and The HOD has been correlated with the CV of the coal on
composition of exit gas for the ITmk3 process are also the dry ash free (Qdaf) basis (kJ/100 g). Gyul’maliev et al.[21]
reported in Table 2. derived Equation 6 for calculating the CV of coals from the
For estimating CO2 emissions derived from reductant elemental composition on a dry ash-free (daf) basis of the
coal and natural gas, Fujita et al.[15] referred to unit heat organic matter of coals based on a large database. Using
value and carbon emission factor of fuels as a guideline to Equation 6, CV of coal-1, coal-2, and coal-3 are found to be
assess CO2 emissions. There is slight variation in data 34110, 33802, and 32781 kJ kg1, respectively.
available in literature and present model prediction. The
reason behind this may be the variation in the composition 4:184ð80:860C þ 239:548H  20:741O þ 15:225N  63:650SÞ
Qdaf ¼
of reductant coal and iron oxide. The validated model is 10
subsequently used for parametric study as discussed in the ð6Þ
following section.
where C, H, O, N, and S represent the percentages of
carbon, hydrogen, oxygen, nitrogen, and sulfur (daf basis)
present in coal.
4. Model Predictions (CO2 Emission) for With the help of Hess’s law, the enthalpy of formation of
Sponge Processes coals DH daf
298 (kJ/100 g) can be evaluated from the complete
combustion of 100 g of coal organic matter using the
No data points are available for validation from literature if Equation 7 and the HOD can be correlated to the enthalpy
the product is sponge iron. Since the ITmk3 process data is of formation from the Equation 8.
validated, it is assumed that the model can satisfactorily
X
predict input and output streams for a rotary hearth DH daf
298 ¼ DH C298 ðcombustion productsÞþQdaf ð7Þ
sponge process. However, in the sponge process, unlike in
ITmk3, no melting takes place. Suitable changes in the
model were made to account for the above changes HOD ¼ DH daf
298 ð8Þ
including different solid output temperature.
The HOD of reductant coals is estimated from the
calculated CV of coals. Estimated HOD of coal-1, coal-2,
4.1. Effect of Reductant Coal Type and coal-3 are 104, 1788, and 2509 kJ kg1, respectively.
These HOD values of reductant coals are used as an input
4.1.1. Prediction of VM Variations for heats required for pyrolysis of reductant coals during
For the present study, three different reductant coals have the heat requirements calculation in zone-I.
been considered. Coal-1 is low VM and low ash, coal-2 is high
VM and low ash, and coal-3 is high VM and high ash. Table 3 4.1.3. Char Rate Calculation
shows the ultimate and proximate analysis of reductant The carbon rate is initially calculated based on the reduction
coals, as well as the model predicted composition of VM in reaction provided in Figure 1. Coal rate and char rate per ton

6 steel research int. 87 (2016) No. 9999 ß 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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Model predicted information
Zone-I, 4H1 1.6
Heat requirements (GJ) Zone-II, 4H2 1.1
Zone-III, 4H3 4.8
Preheat air 1.5
Amount of natural gas required for 4H3 (Nm ) 3
167.7
Zone-III entry temperature of hot combustion product gases (8C) 2496.0
Zone-III, T1 1000.0
Exit gas temperature (8C) Zone-II, T2 674.4
RHF, T3 313.2
Zone-III, V1 2347.16
Exit gas volume (Nm3) Zone-II, V2 2347.16
RHF, V3 2491.90
–3
CV of exit gas (kJ Nm ) 4320.11
CO2 7.01
Exit gas composition (%) H2O 14.90
N2 50.93
CO 23.36
CH4 3.80
Comparison of the model predicted results with literature data
Literature data[15] Model prediction
Coal (kg) 500 501a)
Energy balance
Input (GJ)
Reductant coal 13.34 14.48
External fuel 4.60 4.83
Preheat air 4.37 1.47
Power 0.69
Total 23.00 20.78b)
Output (GJ)
Offgas (Total) 10.58c) 10.75
Ironmaking process 10.12 10.03
Total 20.70 20.78
Total CO2 emission (kg) 1627 1672
a)
Based on char composition and quantity.
b)
Power not included.
c)
Including losses.

Table 2. Model predicted information and comparison of the model predicted results with literature data per ton iron nugget for the
ITmk3 process.

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Coal-1 Coal-2 Coal-3

Ultimate analysis
C 94.93 87.30 82.40
H 2.17 4.89 5.83
N 1.08 0.97 0.99
O 1.29 6.23 10.39
S 0.52 0.60 0.39
Proximate analysis
FC 81.18 68.30 50.11
VM 8.85 22.90 26.63
Ash 9.97 8.80 23.26
Predicted VM composition (wt%)
CH4 80.07 58.95 59.63
CO2 0.91 11.97 19.23
CO 0.06 0.16 0.56
N2 5.37 3.90 2.85
H2O 13.59 25.02 17.72

Table 3. Ultimate analysis, proximate analysis, and predicted VM in reductant coals.

of sponge (based on proximate analysis of coal) for a Sponge iron product grades, as well as coal and char rate per
different degree of metallization with reductant coals are ton of sponge, are estimated and reported in Table 4. It may
estimated based on the stoichiometric carbon rate be noted that higher char rate leads to a lower grade of
(257–283 kg, depending on the degree of metallization). sponge. In composite pellets, gangue associated with coal

Reductant coal

Coal-1 Coal-2 Coal-3

Coal rate Char rate Coal rate Char rate Coal rate Char rate
(kg) (kg) (kg) (kg) (kg) (kg)

Degree of 100% 348 317 413 318 515 378


metallization
95% 332 303 394 304 494 362
90% 317 289 377 291 474 348

Fe(M) Fe(O) Fe(T) Fe(M) Fe(O) Fe(T) Fe(M) Fe(O) Fe(T)


(kg) (kg) (kg) (kg) (kg) (kg) (kg) (kg) (kg)
Degree of 100% 877.0 0.0 877.0 875.0 0.0 875.0 801.5 0.0 801.5
metallization
95% 823.2 43.3 866.5 821.8 43.3 865.0 755.7 39.8 795.5
90% 771.3 85.7 857.0 770.4 85.6 856.0 711.0 79.0 790.0
Fe(M)-Metallic iron; Fe(O)-Iron in residual iron oxides; Fe(T)-Total iron.

Table 4. Coal and char rate, and metallic iron, iron in residual iron oxides and total iron per ton of sponge for different degree of
metallization, and reductant coals.

8 steel research int. 87 (2016) No. 9999 ß 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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remain in the sponge iron after reduction, therefore, total of metallization and reductant coals.
iron is less in high ash coal composite pellets (coal-3).
Therefore, for premium-quality sponge product high ash Fex Oy þ yCO ¼ xFe þ yCO2 ð9Þ
content reductant coal is not suitable.

C þ CO2 ¼ 2CO ð10Þ


4.2. Estimation of Heat Requirement in Different Zones
Figure 3a clearly indicates that heat requirement per ton
As mentioned earlier, RHF is divided into three zones. In of sponge in zone-I is minimum in coal-1 and maximum in
zone-I, feed materials are heated up to 400 8C from 25 8C, coal-3 because HOD as well as coal rate for coal-1 is
and coal pyrolysis takes place at 400 8C. Since the feed minimum whereas, in the case of coal-3, HOD and coal
materials (iron ore and coal) quantity and composition are rate both are high (Section 4.1.2 and Table 4). With the
known, the heat requirement in zone-I is predicted using decrease in the degree of metallization, heat requirement
FactSage 6.4 software. In zone-II, devolatized composite in zone-I is slightly reduced because there is a minor
pellets consist of iron ore and char only because coal reduction in coal and ore rate. In zone-II, devolatized coal
volatilizationhad taken place in zone-I. Therefore, heat (char) and iron ore are heated from 400 to 900 8C only.
requirement in zone-II is calculated from sensible heat Since this zone only involves sensible heat and no other
required to heat the coal char and iron ore from 400 to heat of reactions is involved, heat requirement in zone-II is
900 8C. Reduction reaction[4,9–11,13,22–24] (Equation 9 and almost equal in all the reductant coals and negligible
10) at 900 8C carried out in zone-III, which is highly reduction with a decrease in the degree of metallization.
endothermic in nature and after reduction the reaction Heat requirement in zone-II are shown in Figure 3b.
product consist of metallic iron, iron in combined form, Figure 3c represents the heat demand in zone-III per
and gangue. Finally, the reaction product is heated to solid ton of sponge. For coal-1 and 2, char rate and metallic
exit temperature (1250 8C for the present study) from iron both are almost equal; therefore, heat requirement is
900 8C. Heat requirement in zone-II and zone-III was also also same. But in the case of coal-3, char rate is high and
estimated using FactSage 6.4 software. Figure 3 shows the metallic iron is less per ton of the sponge (Table 4), that is,
heat requirement in the three zones for a different degree lesser amount of iron ore to be reduced; therefore, the heat

Figure 3. Heat requirement in a) Zone-I, b) Zone-II, c) Zone-III, and d) total heat requirement per ton of sponge.

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External fuel gases

Producer gas Coke-oven gas Syn gas Natural gas

Composition (%)
CO 22.00 5.50 46.31 0.00
CO2 13.00 2.00 16.22 0.00
H2 21.00 51.90 33.44 0.00
CH4 3.00 32.00 2.17 100.00
N2 41.00 4.80 1.86 0.00
–1
Model predicted CV (kJ mol ) 137.76 412.33 231.28 802.37
Model predicted AFT (8C) 2211 2511 2525 2496

Table 5. Composition, model predicted CV, and AFT of external fuel gases.

required is less compared to coal-1 and -2. With the process. The total emission has been estimated using the
decrease in the degree of metallization, heat requirements exit gas quantity and composition analysis for different
per ton of sponge for all three reductant coals are reductant coals and external fuel gases. In actual practice,
decreased. As shown in Figure 3d, total heat requirement it is very difficult to produce 100% metallized sponge iron;
per ton of sponge for the RHF process is maximum for therefore, results based on 90% metallization are reported
coal-3 with minimum metallic iron and minimum for coal- in this section and next section. Figure 4a shows the
1 with maximum metallic iron. predicted direct emissions from the RHF as well as
downstream CO2 emissions from different external fuel
gases and reductant coals for 90% metallization. CV of
4.3. Prediction of External Fuel Gas Requirement natural gas is maximum compared to other fuel gases but
the direct CO2 emission for coke-oven gas is minimum
Table 5 represents the composition, and the model because combustion of coke-oven gas primarily produces
predicted CV and AFT (external fuel gas and air enters water vapor since it contains around 50% H2. Similarly, CV
at 600 8C) of external fuel gases. The requirement of natural of syn gas is almost double of producer gas but, both
gas, coke-oven gas, producer gas, and syn gas as an produces approximately identical direct CO2 emission.
external fuel per ton of sponge are 173, 273, 842, and Therefore, it cannot be pre-assumed that the higher caloric
490 Nm3, respectively for 100% metallization with coal-1. It fuel gives lower emission. The emission value depends not
is found that the amount of external fuel gas requirement only on the CV but also on the constituents of the fuel gas.
decreases with a decrease in the degree of metallization The downstream CO2 emission does not depend on the
and is related to the CV of the external fuel gases. The external fuel gas because it is completely combusted. It is
higher the CV of the external fuel gas, the lower is the related to the CO generated during the reduction of iron
requirements and vice versa. Since the primary objective of ore and coal pyrolysis gases. Figure 4b illustrates a typical
the external fuel is to supply the heat demand of zone-III calculation methodology for estimating the total emis-
only and the endothermic reduction reaction heat demand sions. Figure 4a also indicates that with an increase in VM
(>90% of zone-III heat requirements) is independent of in reductant coal, the downstream CO2 emission will
reductant coal. Therefore, the effect of reductant coal is increase (coal-2 and 3) since higher VM in reductant coal
found to be very less in the requirement of external fuel results in more carbon bearing pyrolysis gases. Thus, to
gases, especially for external fuel with high CV. minimize the total CO2 emission from RHF process, high
VM reductant coals are not beneficial.
The composition, volume, temperature, and CV of exit
4.4. Prediction of CO2 Emission gas for different external fuel gases and coal-2 with 90%
metallization are computed and reported in Table 6,
Direct emission (CO2 generated inside the RHF on considering no post-combustion. Exit gas volume per ton
combustion of external fuel as well as post-combustion of sponge varies from 1818 to 2209 Nm3 depending on
of gases in the kiln) and downstream emission (CO2 external fuel. Lower gas volume results in lower exit gas
produced when exit gas is combusted completely outside temperature but, higher heat content since CO generated
the RHF) constitute the total CO2 emission from RHF from the iron ore reduction in zone-III and VM of the

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Figure 4. a) Predicted direct and downstream CO2 emission from different fuel gases and reductant coals, and b) typical model prediction
of CO2 emission in RHF for 90% metallization of iron ore (coal-2).

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Per ton of product sponge

Producer gas Coke-oven gas Syn gas Natural gas


3
Exit gas volume (Nm ) 2209 1910 1818 1915
Exit gas composition (vol%)
CO2 13.56 5.66 16.65 6.86
H2O 10.68 17.17 10.90 14.58
N2 50.85 48.37 42.88 49.84
CO 21.68 25.07 26.34 25.01
CH4 3.22 3.73 3.23 3.71
Exit gas temperature (8C) 352 222 208 221
Predicted CV of exit gases 3910 4521 4753 4510
(kJ Nm–3)

Table 6. The composition, volume, temperature, and model predicted CV of exit gas for different external fuel gases and coal-2 with 90%
metallization considering no post-combustion.

reductant coal is independent of external fuel. CV of exit coke-oven gas and natural gas per ton of sponge and even
gases varies from 3910 to 4753 kJ Nm3 and chemical more than BF emission. With the decrease in the degree of
energy associated with the exit gas is around 8.63 GJ per metallization, emissions values also decrease since CO
ton of sponge which can be further utilized in drying of generation in reduction zone, and external fuel require-
pellets, preheating of air, and power generation. Figure 5 ment is reduced because a lesser amount of iron ore to be
represents the comparison of predicted total CO2 emission reduced.
per ton of sponge from different external fuels and The total CO2 emission value from BF route is around 1.8
reductant coal with a degree of metallization considering ton tcs1.[25] For coke-oven gas and natural gas as an external
no post-combustion inside RHF. Coal containing high VM fuel in RHF, the total CO2 emission values vary from 1.29 to
leads to higher emission values. Total CO2 emissions from 1.34 ton per ton sponge considering 90% metallization
producer and syn gas are around 350–400 kg more than (1.70 t-CO2/tcs) and further melting of sponge iron in an

Figure 5. Predicted total CO2 emission (kg ton1 of sponge) with different degree of metallization and reductant coals; a) coke-oven gas,
b) natural gas, c) producer gas, and d) syn gas.

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Figure 6. a) Percentage decrease in external fuel requirement, b) percentage decrease in total CO2 emission, and c) decrease in CO/CO2
ratio with post-combustion (coal-2 with 90% metallization).

electric arc furnace is estimated to produce around 0.15 ton post-combustion of the CO generated from reduction
additional CO2/tcs. Therefore, net total CO2 emission reaction in zone-III itself is not beneficial. Again excess
through RHF route may be estimated to 1.85 ton tcs1 for heat from zone-III that moves to zone-I and -II, become
coke-oven gas and natural gas which is almost similar to the superfluous as the heat requirements in these zones are
blast furnace route steel making. For syn gas and producer meager. Besides, generation of excess heat will lead to heat
gas, total CO2 emission values are estimated to more than 2.2 loss and less energy efficient system. On the other hand, if
ton tcs1 because of lower calorific values. Also for reduction such CO laden gas is combusted outside at proper useful
of iron ore in reduction zone, CO/CO2 ratio should be greater sink, overall energy efficiency is expected to be better.
than two to avoid reoxidation.[26] In the case of natural gas But partial post-combustion of CO might lead to a
and coke-oven gas, CO/CO2 ratio in the reduction zone is reduction in external fuel gas requirement which finally
3.80 and 4.65, respectively which is much more than two results in a decrease in CO2 emission. The typical effects of
whereas for producer gas and syn gas this ratio is 1.63 and partial post-combustion in reduction zone (coal-2 with
1.61, respectively. Therefore, producer and syn gas may not 90% metallization) on fuel gas requirement, total CO2
be suitable for external heat supply as well as CO2 emission emission, and CO/CO2 ratio in the reduction zone is
control unless extra coal is added to maintain a reducing represented in Figure 6.
atmosphere over the bed. The emission values computed It is evident that the introduction of partial post-
earlier for these fuels would accordingly increase. combustion in the reduction zone provides additional heat
in this zone, thus reducing external fuel gas requirement as
well as total CO2 emission. The percentage decrease in
4.5. Effect of Post-Combustion in Reduction Zone external fuel requirement with post-combustion is same
for all external fuels. However, external fuel having least
In RHF, solids and gases moves in opposite direction CO2 emission on no post-combustion (coke-oven gas)
and majority of the heat required in RHF process is have the least percentage decrease in CO2 emission on the
utilized in reduction zone (zone-III); therefore, complete introduction of the same degree of post-combustion as

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compared to other external fuels having higher CO2 is outside the major scope of this paper dealing with
emission on no post-combustion. But CO/CO2 ratio emissions.
also decreases with post-combustion, and beyond 20% 9. Regarding gas phase compositions, oxidation of the gas
post-combustion, this ratio becomes less than two even for phase constituents has been considered as being
natural gas and coke-oven gas. Therefore, more than 20% governed by reaction stoichiometry. The possible effects
post-combustion might not be beneficial as atmosphere of departure from equilibrium in the gas phase at various
no longer remains reducing to sponge. reaction zone temperatures are not considered since the
space velocity of the gas phase is considerable, and there
is insufficient time to attain equilibrium.
10. Thermodynamic calculations made in this work for
5. Conclusions predicting heats of reaction, adiabatic flame tempera-
ture estimate, and coal pyrolysis are likely to provide a
1. A thermodynamic model for a sponge iron producing foundation for emission calculations for different
unit based on RHF has been developed. The model has degrees of metallization signifying the departure from
been validated based on limited literature data and is equilibrium.
capable of predicting exit gas volume and composition
including CO2 emission per ton of sponge for a
specified metallization and fuel gas. Received: July 20, 2016; Revised: October 5, 2016
2. For a specific coal composition (VM-8.85 and FC-
81.18) lowest achievable coal rate (stoichiometric) for
100% metallization of the sponge is 348 kg per ton of Keywords: Rotary hearth furnace; External fuel; CO2
sponge iron. emission; Reductant coal; Degree of metallization
3. CO2 emissions have been estimated for some operat-
ing cases using different coal and fuel gases. Coke-
oven gas generates lowest CO2 (1.2 ton per ton of
sponge) when compared with natural gas, syn gas, and References
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ß 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim steel research int. 87 (2016) No. 9999 15

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