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UTILIZATION OF CO2 IN METALLURGICAL PROCESSES

Haijuan Wang1, *Nurni N. Viswanathan2 and Seshadri Seetharaman3
1

State Key Laboratory of Advanced Metallurgy and School of Metallurgical and Ecological Engineering,
University of Science and Technology Beijing,100083, Beijing, CHINA
2

Indian Institute of Technology Bombay, Powai, Mumbai-400 076, INDIA and Minerals and Metals
Research Laboratory, Lulea University of Technology, Lulea, SWEDEN
(*Corresponding author: vichuiitb@gmail.com)

Division of Materials Process Science , Royal Institute of Technology, SE-100 44, Stockholm, SWEDEN
ABSTRACT

The present work aims at some process modifications in specified metallurgical processes, wherein
CO2 can be used successfully as an oxidant for decarburization in steelmaking and applied in some nonferrous metals production processes. During the decarburization of Cr-containing high alloyed steels, the
present researchers investigated the possible use of CO2 instead of Ar-O2 mixture and could successfully
decarburize the steel melt without significant loss of alloyed Cr to the slag phase. A mathematical model was
developed based on the bubble formation accompanying the chemical reaction: C(molten steel)+ CO2(gas)= 2
CO(gas). The model predictions were tested by laboratory scale (1 kg) experiments carried out in an induction
furnace and very good agreement between the model predictions and experimental results were observed. A
national project has been sanctioned in China for the implementation of CO2 in decarburization of ferroalloys
as well enable the addition of pig iron in the electric arc furnace process when the scrap supply is limited.
New processes have been developed for the utilization of CO2 in the case of non-ferrous processes. A novel
method of treatment of Al dross by leaching with water and capturing the evolved NH3(formed by the
hydrolysis of AlN) has shown very promising results.
KEY WORDS
Carbon dioxide, decarburization, alloy steel, modeling, aluminum dross, Al oxidation.

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INTRODUCTION
The impact of carbon emissions on global environment, with special reference to global warming
is being discussed in many world forums since it was first discussed in the First Earth Summit held at
Stockholm in 1972. According to the National Oceanic and Atmospheric Administration (NOAA), USA,
carbon dioxide level in the atmosphere has increased rapidly from 340 ppm to 400 ppm in the last 35 years
(http://www.esrl.noaa.gov/gmd/ccgg/trends/). In the last 2014 UN meet on climate change, it was advocated
to have peak in greenhouse gas emission before 2020 and dramatically reduced emissions thereafter.
European Union countries have committed to a target of reducing emissions to 40 per cent below 1990 levels
by 2030. Prasad, Agarwal and Pande (2000) reported that metal industries contribute approximately 5% to
global CO2 emissions. Conscious efforts are being taken to reduce carbon emission by increasing process
efficiency as well as with usage of more and more hydrogen containing fuels(www.ulcos.org and
www.jisf.or.jp/course50/outline/index_en.htm). Efforts are also being made to capture and store CO2 in
underground
geological
formations
(http://www.ipcc.ch/pdf/specialreports/srccs/srccs_summaryforpolicymakers.pdf). In this context to a limited extent it may be also worth
to look at carbon dioxide (CO2) as a resource in metallurgical processes. For example CO2 can be used as a
string gas (Bruce, Weisang, Allibert, & Fruehan, 1987) to promote the chemical reactions, or a shielding
gas (Hara, Spence, & Eissenwasser, 1986; Katayama, & Abe, 1982) ) to protect the liquid steel from
contacting with air and absorbing nitrogen.
In this paper, two case studies exploring utilization of CO2 in metallurgical processes are presented.
1) Utilization of CO2 for decarburization of Cr containing alloy steels or ferrochrome and 2) leaching Aldross with CO2 saturated water to capture NH3 by converting to Ammonium carbonate by injecting CO2.
UTILIZATION OF CO2 IN STAINLESS STEEL AND FERROCHROME MAKING (Wang
Haijuan, 2010)
In stainless steel making process as well as medium and low carbon ferrochrome(M-LC FeCr)
production through converter process, the liquid steel or high carbon ferrochrome(HCFeCr) needs to be
decarburized by oxidizing carbon in preference to chromium. In order to achieve this, the activity of the
product of carbon oxidation, namely the carbon monoxide, is reduced by decreasing its partial pressure or in
other words oxygen partial pressure in the decarburizing gas is reduced. This principle has to lead to the
development of Vacuum Oxygen Decarburization (VOD) and Argon Oxygen Decarburization (AOD). On
the contrary, in stainless steel making using Electric Arc Furnace (EAF) process where pure oxygen injection
is practiced, the injection leads to significant Cr loss to the slag phase. Therefore in many plants EAF is used
as a simple melting unit followed by processing in AOD or VOD vessel to achieve lower carbon levels. In
EAFs, where oxygen is injected, the Cr lost to the slag is recovered by addition of Fe-Si. In place of oxygen,
Wang (2010) has explored the possibility of injecting CO2 to a stainless steel bath for exploring possibility
of reducing Cr oxidation. Investigations were carried out using laboratory scale experiments and followed
by analysis of experimental data using a mathematical model.
Experiments
Investigation on the effect of CO2 injection to a stainless steel bath was first carried out at KTH,
Stockholm(Wang, 2010) in a laboratory set-up as shown in Figure 1. As the focus of the investigation was
on Cr and C oxidation, Fe-Cr-C melts were used for conducting injection trials. Fe-Cr-C molten alloy was
kept at 1873K in an induction furnace. The steel and slag samples were placed in an Al2O3 crucible of 45mm
I.D. and 130mm height and positioned inside an outer graphite crucible, which in turn, was positioned inside
an induction furnace. The oxidant gas was injected into the liquid melt through an alumina lance of 3.5mm
I.D. The lance was immersed into the melt to a depth of 50 mm (total height of the bath was about 80mm)from

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the top of the melt. Gases containing pure oxygen, pure carbon dioxide and their mixture of known
proportions were used for injection.
It is to be noted that for every molecule of O2 injected, two atoms of O is available for oxidizing
C. However, with every molecule of CO2 injected, only one atom of O is available for oxidizing C. Thus,
for the same flow rate of gas, CO2 would need a longer injection time. Additionally, the latter reaction being
endothermic, brings down the bath temperature which is not desirable in terms of energy. Therefore
experiments were also performed by gases containing both O2 and CO2 in varying proportions. The changes
of the concentrations of C as well as Cr in the metal phase were followed as functions of gas-blowing duration
by taking out samples periodically and analysing the same.

Figure1 - A schematic plot of the induction furnace experiments (Wang Haijuan, 2010 )
The composition of the Fe-Cr-C melts used for different experiments were with high carbon content
(C: 2.6-3.5 mass% and Cr: 11.8-15.1 mass%,) and with low carbon content (C: 0.26-0.29 mass% and Cr:
10.3-11.1 mass%). In all experiments, slag having CaO 40 mass%, MgO 10 mass %, SiO2 40 mass % and
Al2O3 10 mass % were used.
For the oxidation experiments, the alloy and the slag were melted under Ar atmosphere and the
oxidant gas was injected into the liquid metal at the targeted temperature. The temperature of the bath was
controlled by means of an EI Eurotherm controller at 187315K. Different gas flow rates were employed in
the experiments. Samples of the steel melt were taken at appropriate time intervals using quartz sampler
tubes of I.D. 6 mm and quenched in a water bath at room temperature. The chromium content of the samples
was analysed by X-ray fluorescence spectroscopy and the total carbon content by LECO combustion method.
Subsequent to the experiments at Stockholm, more experiments were carried out at the University
of Science and Technology, Beijing (Yu, Wang, Chu, Sun, & Lu, 2015) with high carbon ferrochrome. In
these experiments, the temperature of the bath was measured periodically.
Experimental Results(Wang Haijuan, 2010 and Yu Hongchao et al., 2015)
Figure 2(a) and 2(b) shows the variation of Cr with time for high carbon( around 3.0 mass%) and
low carbon( around 0.3 mass%) Fe-C-Cr melts with pure O2 and pure CO2 injection respectively. It is seen
in Figure 2(a) that in case of high carbon melts, CO2 injection for decarburization does not show any
significant Cr oxidation. Rather, it appears to show some Cr recovery suggesting some recovery from the
already oxidized Cr from the slag layer. On the other hand, for low carbon melts, shown in Figure 2(b),
significant Cr oxidation is seen for both O2 and CO2 injections. However, beyond 10 minutes of injection,

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Cr oxidation is significantly higher with O2 injection than with CO2 injection. This suggests that Cr oxidation
losses can be lowered with CO2 injection.

(a)

(b)

Figure 2 - The variation of chromium with time in (a) high carbon and (b) low carbon Fe-C-Cr melts
(Wang Haijuan, 2010 )
The effect of CO2 injection on C evolution in the steel bath is compared with that of O2 injection
for high and low carbon Fe-C-Cr melts as well, shown in Figure 3(a) and 3(b) respectively. As mentioned
before, the available O for oxidation from CO2 is half of that from O2. Hence for a fair comparison, amount
of oxygen available instead of time has been used to plot the C variation. As seen in Figure 3, at high carbon
contents decarburization is better with CO2 injection. However at low carbon contents, the difference
between two gases is not discernible. This indicated that, it would profit to introduce CO2 for quick carbon
removal at the early stage of decarburization as well as for Cr retention when the initial carbon content is
relatively high.

(a)

(b)

Figure 3 - The variation of C with injected reducible oxygen in (a) high carbon and (b) low carbon Fe-C-Cr
melts (Wang Haijuan, 2010)
Results of the experiments conducted with high carbon ferrochrome in China are shown in Figure
4(a) and (b), with the Cr content is around 60 mass% and the carbon content is around 8.0 mass%. The
authors try to use CO2 for decarburization of high carbon ferrochrome to produce medium and low carbon
ferrochrome through converter. The difficulty for Cr retention of this system is even higher that with Cr

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alloyed steel system. The figures show the variation of C, Cr and temperature with time. As seen in Figure
4(a), the decarburization rate with CO2 injection is distinctly higher than that with O2 while the Cr oxidation
is not obvious at both cases. That is because the carbon content in the melt is rarely high ( 8.0 mass %), Cr
is easy to be kept in the melt under high carbon situation during the decarburization process. One of the
issues with CO2 injection is that unlike that with O2, the decarburization reaction is highly endothermic.
Therefore, temperature was measured with CO2 injection in the present experiments. The melt temperature
decreasing with time is clearly seen in Figure 4(b). It is to be noted that, as these experiments were conducted
in induction furnace, there is constant source of power input which could compensate the endothermicity to
some extent. The experimental result predict that CO2 will have positive effect on decarburization and Cr
retention during medium and low carbon ferrochrome refining production in converter.

(a)

(b)

Figure 4 - (a)Variation of C and Cr (b) temperature with time for medium and low carbon ferrochrome
melts with O2 and CO2 injection (Yu Hongchao et al., 2015)
Analysis of the Results Using A Model(Wang , Viswanathan, Ballal, & Seetharaman, 2010)
Wang, Viswanathan, Ballal, and Seetharaman (2010) developed a model to understand the effect of
CO2 injection on oxidation of Cr and C in Fe-C-Cr melt. When gas is injected into a bath of liquid metal, the
rising bubbles through the metal bath form a plume region. Thus, the model captures phenomena primarily
at two scales 1) at the scale of a single bubble and 2) at the scale of plume or the reactor. For the laboratory
experiments, the whole reactor can be assumed to be in the plume region. However, in larger furnace, more
conceptual reactors can be constructed to simulate the mixing of the metal in the plume region with the rest.
As the bubbles rise through the bath, chemical reaction takes place at the gas-liquid interface
assisted by mass transfer of reactant species from bulk gas and liquid to the interface and vice versa of
product species. As the temperature involved is high, local equilibrium can be assumed at the gas/liquid
interface. These are illustrated using a schematic in Figure 5.

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Figure 5 - Schematic of equilibrium at the gas-liquid interface (Wang et al., 2010 )

The equations describing the mass transfer of C and Cr from the bulk metal to the bubble interface
are depicted in equations below.

=
nC

=
n Cr

=
n Cr

Ab kmC m
( wt %C B wt %C * )
100 M C

(1)

Ab kmCr m
( wt %Cr B wt %Cr * )
100 M Cr

(2)

Ab kmCr m
( wt %Cr B wt %Cr * )
100 M Cr

(3)

where, n i is the rate of transfer of species i; Ab is the surface area of the bubble; k is the mass
transfer coefficient; m is density of liquid steel; subscripts m and g refer to metal and gaseous phases
respectively; superscripts B and * refer to bulk and gas-liquid interfaces respectively.
In order to track the composition of the gas inside the bubble as it ascends, one needs to perform
mass balance for each species. If, for example, nC represents the number of moles of carbon inside the
bubble, and Ub represents the velocity of the bubble at any particular location l in the plume, one can
write a molar balance equation for the period during which the bubble travels a small distance dl :

d (U b nC )
= nC
dl

(4)

Similar equations can be written for the net oxygen removed from the bubble as well as for the
amount of Cr2O3 that can be formed at the bubble interface. The differential equations can be solved for a
given inlet gas composition and liquid metal composition.
Figure 6 shows the simulated variations of C and Cr contents in liquid steel. The figure also shows
the values obtained from the experiments. The agreement may be considered reasonable, especially
considering the scatter in data expected in these kinds of experiments.

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Figure 6 - Simulated variations of C and Cr in the liquid steel along with the corresponding
experimental data (Wang et al., 2010)
Simultaneous oxidation of C and Cr in the melt can be best understood by plotting the evolving C
against the Cr content. In order to aid the discussions, C and Cr contents in the melt in equilibrium with
carbon monoxide at one atmospheric pressure and solid Cr2O3 are also depicted in Figure 7. Based on this
equilibrium consideration, one can clearly see from the figure that Cr can be protected without being oxidized
till the carbon content in the melt reduces to 0.77 wt%. However, in the actual oxidation process, oxidation
of Cr starts much above this carbon content of 0.77 wt %. It should be noted that as per the present model,
equilibrium prevails at the gas-melt interface. Therefore, the C and Cr concentrations in the bulk are much
above the equilibrium values because of mass transfer resistances.

Figure 7 - Carbon and chromium composition evolution in a Fe-1.20C-22Cr melt injected with gases
containing 100%O2, 50%O2-50%CO2 and 100%CO2 separately (Wang et al., 2010)

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It can be clearly seen from Figure 7 that the increase in CO2 content in the injected gas leads to bulk
metal compositions moving closer to the equilibrium line. In other words, with increasing CO2 content in the
injected gas, higher amount of Cr is protected from oxidation. This clearly demonstrates that the loss of
chromium by oxidation can be lowered by injecting CO2 especially during the initial stages of blowing where
in the carbon contents are high.
Energy estimates for replacing some fraction O2 with CO2 injection during stainless making were
made by performing material and heat balances (Wang Haijuan, 2010). These estimates show that, by adding
20% CO2 in the system, the electric energy will increase by 17 kWh/tons. However, if one can retain 0.3
mass% Cr in the melt, the cost saving will then be more than the energy consumption. Energy consumption
resulting from the introduction CO2 can be compensated by introducing more hot metal. For pure O2 injected
to 40% hot metal + 60% scrap, the energy consumption is the same as that for 60% hot metal+ 40% scrap
blowing 50%O2+50%CO2. The energy consumption decreases with hot metal ratio increase in EAF. The
tap-to-tap time could possibly be shortened by introducing CO2. This shows a possibility to use high ratio
hot metal in EAF process if the scrap is limited.
The micro-model developed to capture reaction rates at the vicinity of single bubble in a melt is
being considered for incorporation in a process model for AOD process that would enable the use of CO2O2-Ar mixtures for effective decarburization. A national project has been sanctioned in China for the
implementation of CO2 injection in decarburization of ferroalloys as well enable the addition of pig iron in
the electric arc furnace process when the scrap supply is limited.
CO2 ASSISTED LEACHING OF SALT CAKE FROM ALUMINUM MELTING(Li, Guo, Zhang ,
Teng, & Seetharaman, 2012)
Salt cake is the dross formed during Al melting. Though specially designed salts are added to
prevent oxidation of Al melting, some Al do react with air to form products such Al2O3, AlN etc. In addition
to this, significant amount metallic Al gets trapped inside the pasty dross or salt cake. The Al from the salt
cake, is recovered by leaching out the salts from the dross and separating the metal. The wastes generated
from this process are usually land filled and has large impact on environment.
During the leaching of salt cake, the AlN in the cake results in generation of NH3gas, which is
environmentally undesirable. In addition to this, minor amounts of CH4 as well as PH3 are also generated
from Al4C3 and AlP by hydrolysis. The product formed during leaching of salt cake influenced significantly
by pH of water. Ammonia being alkaline, changes the pH beyond 9. This results in loss of metallic Al from
the salt cake, as alkaline environment is more favourable for Al hydrolysis to form Aluminium hydroxide.
Yerushalmi (1992) recommends keeping the pH value in the range of 5-8 to minimize Al loss during
leaching. One of the suggested methods is to add magnesium chloride which would decrease the pH by
releasing HCl. As an alternative, leaching with CO2-saturated water was explored by Li et al.(2012). Unlike
HCl, carbonic acid is a weak acid and hence has moderate effect on pH. It is also beneficial as it would
enable fixation of carbon by form ammonium carbonate or bicarbonate.
Experiments(Li et al, 2012)
Experiments were performed using Al dross supplied Stena Aluminum AB, Sweden. A schematic
of the experimental apparatus is shown in Figure 8. The ammonia released would first dissolve in the
leachant itself and any remaining would escape to be absorbed in Boric acid Leaching tests were conducted
with both pure water as well as CO2 saturated water for different solid-to-liquid ratios. The pH was
monitored continuously. The chemical analysis of salt cake as well as residue after leaching were carried
out using XRF. The leach solution was analysed for NH4+.

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Figure 8 - Experimental apparatus used for leaching of salt-cake using CO2 saturated water (Li Peng et al.,
2012) 1. Carbon dioxide 2. Gas Buffer 3. Manometer 4. Reaction Bottle 5. Thermostat with magnetic
stirrer 6. Gas Valve 7. Absorption Bottle with Boric Acid 8. Computer 9. pH measurement
Experimental Results(Li et al.)
Figure 9 shows the variation of pH with time at 291 K for leaching with deionized water and that
with CO2 saturated water. In case of water, the value of pH rose suddenly from 6.5 to 8.75. This might
have been caused by NH3 being released from the moist air reacting with AlN before leaching. Further the
pH value increased steady to a value of 9.0. In case of CO2-saturated water, the pH value increased slowly
from 4.5 to 5.5 even after 100 minutes.

Figure 9 - pH vs. time for Al salt cake in deionized water and CO2-saturated water at 291 K
(Li et al., 2012)
Figure 10 shows the amount of ammonia remained in the reaction bottle and that escaped to be
absorbed in the absorption bottle. The amount of ammonia present in the reaction bottle when leaching was
with CO2-saturated solution is significantly less compared that with deionized water. The leaching time also
do not show any effect on the amount of ammonia in the reaction bottle when leaching was with CO2saturated water. This indicates that, because of carbonic ions the leaching of AlN has already ceased within
an hour. The ammonia that escaped to the absorption bottle when the leaching was CO2-saturated water is

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almost negligible compared to that with de-ionized water. This suggests that leaching with carbonated water
would be extremely environmental friendly.

Ammonia in Reaction Bottle

Ammonia in the Absorption Bottle

Figure 10 - Mass of ammonia in the reaction bottle and in the absorption bottle after leaching process with
and without CO2 bubbling(Li et al., 2012)
An alternate procedure was suggested by Li P., Zhang M., Teng L.D. and Seetharaman S. (2013)
by leaching the salt cake with water and capturing the ammonia evolved downstream by carbonic acid. This
resulted in near-total recovery of the ammonia as NH4HCO3 solution that can be directly used as a fertilizer.
The leach residue could be used for producing the highly value-added Mg-SiAlON ceramic material from
extremely low-cost waste material.
SUMMARY
Along with reducing CO2 emissions and sequestration of CO2, possibilities of utilizing CO2 in
metallurgical processes also need to be further explored. In alloy steel making, decarburization with O2-CO2
mixtures instead of pure O2 show a promise in terms of carbon oxidation in preference to alloying elements
such as Cr. Experimentation at the larger scale with appropriate estimation of process energetics is the way
forward. CO2 utilization in leaching of Al dross to produce useful ammonium carbonates is also being
demonstrated.
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Hara, R. D. O., Spence, A. G. R. & Eissenwasser, J. D. (1986). Carbon dioxide shrouding and purging at
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Katayama, H., & Abe, Y. (1982). Production of low nitrogen steels, International Symposium on the
Physical Chemistry of Iron and Steelmaking, Toronto, Canada, 32-37.
Li, P., Guo, M., Zhang, M., Teng, L. D., & Seetharaman, S.(2012). Leaching process investigation of
secondary Aluminum dross: The effect of CO2 on leaching process of salt cake from Aluminum
remelting process, Metallurgical and Materials Transactions B, 43, 1220-1230.

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Li, P., Zhang, M., Teng, L. D., & Seetharaman, S. (2013). Recycling of Al salt cake: utilization of evolved
ammonia, Metallurgical and Materials Transactions-B, 44, 16-19.
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Wang, Haijuan (2010). Investigations on the oxidation of iron-chromium and iron-vanadium molten
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Wang, H. J., Viswanathan, N. N., Ballal, N. B., & Seetharaman, S. (2010). Modelling of physico-chemical
phneomena between gas inside a bubble and liquid metal during injection of oxidant gas, International
Journal of Chemical Reaction Engineering, 8, Article No. 33.
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Yerushalmi, D. (1992). US Patent 5, 102, 453.

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