Citation
Ogakwu, Omale Sunday
(2020)
Carbon dioxide sequestration by mineral carbonation using electric arc furnace slag.
Doctoral thesis, Universiti Putra Malaysia.
Abstract
Fossil fuel usage is the primary source of anthropogenic air pollution, where carbon
dioxide (CO2) is the most prominent agent that contributes to global climate change.
The iron and steel industries are major contributors to gaseous CO2 emission. These
industries also produce solid wastes in the form of slags during operations.
Steelmaking in electric arc furnace (EAF) generates between 10-15% slag wastes per
ton of steel production, which can be used in mineral carbonation to capture and store
CO2. In this study, the EAF slag from an iron and steelmaking factory in Klang,
Malaysia, was utilized for the CO2 sequestration through both direct aqueous and
indirect mineral carbonation method in a batch reactor. The direct aqueous
carbonation investigation was at room temperature, and different solid/liquid ratio,
pressure, and time. The indirect carbonation was performed, after the extraction of
essential metallic ions from the EAF slag at a different temperature, solvent
concentration, and solid/liquid ratio. The direct aqueous mineral sequestration capacity was 58.36±5.84g CO2/kg of slag
under room temperature after 3 hr, solid/liquid ratio of 1:5, and using < 63 μm particle
size. The sequestration efficiency was 28.11 %, and the degree of carbonation was
23.30 % at the pressure of 5 bars. The shrinking core model shows that the direct
aqueous carbonation was by the ash layer product phase-controlled, with the
regression coefficient (R2) of 0.97. In the dissolution of essential metallic ions like Ca, Mg, and Fe, the slag from EAF
was the source. The dissolution efficiency was affected by temperature, solvent
concentration, solid/liquid ratio, and reaction time. At the temperature of 75 oC, Ca
ion was extracted from the slag with 86.46 % efficiency and Mg ion of 30.13 % after
1 hr of using 0.22 M HCl. However, the dissolution in the solid/liquid ratio of 10 g/l was higher than 20 g/l and 30 g/l. The dissolution of Ca ion was 80.27 %, 61.33 %,
and 50.53 %, and that of Mg ion was 26.63 %, 24.20 %, and 22.16 %, respectively,
after 1 hr in 0.22 M HCl. The acid concentration of 0.44 M extracts more Ca, Mg and
Fe ions than 0.33 M and 0.22 M. The efficiency after 1 hr.; at 35℃ from 20 g/l was
68.84 %, 65.63 %, 61.33 % for Ca, and 27.52 %, 26.40 %, 24.20 % of Mg, while that of Fe from 20 g/l was 10.09 %, 8.76 %, and 5.18 % respectively.
Meanwhile, in the indirect carbonation, the dissolved Ca ion was used for the
formation of calcium carbonate through CO2 sequestration. The formed precipitate
calcium carbonate (PCC) of 98.61 ± 1 % purity, and the sequestration capacity of
0.4105 ± 0.195 kg of CO2/kg of CaCO3 within 1 hr was achieved. This shows that
at moderate conditions (0.22 M HCl, 35℃, and 1 hr), both CO2 sequestration
and calcium carbonate of high purity were realized. In a reaction of a heterogeneous solid-liquid mixture, the modified shrinking core
model was appropriate. The modified shrinking core model best interpreted the
kinetics behavior for all the parameters studied in the dissolution of Ca ion from the
EAF slag. From the regression coefficient (R2), the dissolution was controlled by the
product layer phase. The order of reaction for acid concentration and S/L ratio was 0.31419 and -1.02459
respectively. The activation energy of the process over the temperature range was,
calculated to be Ea = 3.881KJ/mol From the results of the two sequestration
methods, the indirect route was better with a higher sequestration capacity and calcium
carbonate of high purity. The EAF slag demonstrated the potential and available
material for both CO2 sequestration and economic purposes, instead of being
landfilled.
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