KR101420660B1 - Method for synthesizing H2 and CO rich gas for the iron ore reduction using reforming process of Cokes Oven Gas - Google Patents
Method for synthesizing H2 and CO rich gas for the iron ore reduction using reforming process of Cokes Oven Gas Download PDFInfo
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Abstract
The present invention CO 2 to CH 4 of the coke oven gas (COG) as of a method of manufacturing a synthesis gas for reducing iron ores using a reforming reaction of CH 4, and more particularly, the coke oven gas (COG) under the Ni-containing catalyst Or CO 2 Wow H 2 O < / RTI > And a step of reacting with the reforming gas to obtain a reducing gas containing H 2 and CO.
According to the present invention, since a reducing gas suitable for use in reduction of iron ore can be obtained at a low cost, it is possible to lower the unit cost of producing iron, and it is possible to utilize the coke oven gas (COG) . Further, the reducing gas obtained by the present invention can be applied to the production of high value-added chemicals, and the like.
Description
The present invention relates to a method for obtaining the reducing gas used in the reduction process of iron ore and efficiently, and more particularly, the CO 2 or CO 2 with CH 4 of the coke oven gas (COG) H 2 O. The present invention relates to a method for producing iron ore reducing gas rich in hydrogen and carbon monoxide using a reforming reaction of a mixed gas of H 2 O and hydrogen.
The iron component is present in the form of oxides combined with oxygen, such as hematite (Fe 2 O 3 ) and magnetite (Fe 3 O 4 ), which are called iron ore. Therefore, a reduction process is essential to make iron from natural iron ores.
Syngas, which is composed of hydrogen and CO, is used as the reducing gas that can be used at this time. Generally, such reducing gas is used as a raw material in the petrochemical industry using natural gas, naphtha, It can be synthesized through an autothermal reforming reaction, or after a steam reforming reaction using water, performing a reverse water reaction in which H 2 is converted to CO, and then removing water and CO 2 from the synthesized gas.
On the other hand, in a steel mill, a reducing gas or a gas containing hydrogen as fuel is used, and a coke oven gas (COG) containing hydrogen is purified and used in a blast furnace or a flow furnace, or COG or natural gas gas has been steam reformed to obtain reducing gas, which is a major component of hydrogen, and has been blown into a blast furnace or a flow path.
However, when the coke oven gas (COG) is blown directly into the blast furnace or the flow path, the methane contained in the coke oven gas (COG) is converted into hydrogen and carbon monoxide by the endothermic reforming reaction , The temperature is lowered by the endothermic reaction, and therefore, it has to be prevented.
In addition, since the hydrogen obtained from the steam reforming of the conventional coke oven gas (COG) contains a large amount of water and carbon dioxide, it is necessary to further remove water and carbon dioxide, There was a problem that an additional calorie supply was required. On the other hand, since the reduction process of iron ores by hydrogen is an endothermic reaction, when the produced hydrogen is separated and blown into the blast furnace, the temperature in the furnace is lowered, so the amount of hydrogen used is limited.
Other methods for obtaining hydrogen from coke oven gas (COG) include decomposing tar contained in a high temperature coke oven gas (COG), which has recently been studied in Japan, And the partial oxidation at a high temperature of about 1200 ° C. or higher has been carried out to increase the amount of combustible gas components. However, due to the catalyst regeneration and high oxygen consumption There are problems of technical difficulties and low economic efficiency.
Accordingly, one aspect of the present invention provides a method for producing an iron ore reducing gas using a reforming reaction of coke oven gas (COG).
According to one aspect of the present invention, coke oven gas (COG) Ni catalyst CO 2 Or CO 2 and H 2 O to obtain a reducing gas containing H 2 and CO, comprising the steps of: reacting a reducing gas containing H 2 O with a reforming gas containing a mixed gas of H 2 O.
The coke oven gas (COG) of the coke oven gas (COG) of 1.2 times to 2.5 times, based on the volume of CH 4 gae nitriding gas (CO 2 And H 2 O).
The CO 2 Wow H 2 O, the volume ratio of CO 2 and H 2 O constituting the reforming gas is preferably 1: 0.3 to 1: 5.
The reaction is preferably carried out under a pressure of from 2 to 20 bar.
The reaction is preferably carried out at a temperature of 850 to 1000 ° C.
The reaction is preferably carried out at a reaction space velocity of 1,000 to 500,000 h < -1 & gt ;.
The total fraction of H 2 and CO in the reducing gas is preferably 70 to 100%.
The volume ratio of H 2 and CO (H 2 / CO) is preferably 1 to 4.
The conversion of CH 4 in the reaction is preferably 50 to 100%.
The CO 2 conversion rate of the reaction is preferably 50 to 100%.
The reducing gas containing H 2 and CO can be introduced into the flow path or the blast furnace.
According to the present invention, since a reducing gas suitable for use in reduction of iron ore can be obtained at a low cost, it is possible to lower the unit cost of producing iron, and it is possible to utilize the coke oven gas (COG) . Further, the reducing gas obtained by the present invention can be applied to the production of high value-added chemicals, and the like.
FIG. 1 shows an exemplary process conceptual diagram for producing a syngas for iron ore reduction using a reforming reaction of coke oven gas (COG) according to the present invention.
2 shows the thermodynamic equilibrium of the mixed reforming reaction depending on the volume ratio of CH 4 , CO 2 and H 2 O 2 (b) shows the conversion of CO 2 , FIG. 2 (c) shows the fraction of reducing gas, and FIG. 2 (d) shows the results of calculation using the aspen plus program. Is the ratio of H 2 / CO.
FIG. 3 shows the thermodynamic equilibrium of the reforming reaction when the ratio of the reforming gas containing H 2 O and CO 2 is 1: 1.6, based on the volume of CH 4 in the coke oven gas (COG) 3 (b) shows the conversion of CO 2 , FIG. 3 (c) shows the reducing gas fraction, and FIG. 3 (d) shows the results of calculation using the aspen plus program, Is the ratio of H 2 / CO.
4 is CH 4, CO 2, each 1 volume ratio of H 2 O: 0.4: 1.2 and 1: 0.8: illustrates the results of the 0.8 COG combined reforming, illustrating CH 4 conversion rates according to the reaction temperature .
Hereinafter, preferred embodiments of the present invention will be described with reference to the accompanying drawings. However, the embodiments of the present invention can be modified into various other forms, and the scope of the present invention is not limited to the embodiments described below.
According to the present invention, the coke oven gas (COG) Under the Ni-based catalyst, CO 2 Or CO 2 And H 2 O, to obtain a reducing gas containing H 2 and CO. The present invention also provides a method for producing an iron ore reducing gas, comprising the steps of: That is, the CH 4 in the coke oven gas of the present invention is CO 2 Or CO 2 < RTI ID = 0.0 > And H 2 O to produce a reducing gas comprising H 2 and CO.
The coke oven gas (COG) used in the present invention generally comprises constituents such as about 55% hydrogen, about 27% methane, about 9% carbon monoxide, about 2% C 2 H 4 , about 4% nitrogen, and about 3% Lt; / RTI >
1 shows an exemplary process conceptual diagram for producing a syngas for iron ore reduction using a reforming reaction of coke oven gas (COG) according to the present invention. Referring to FIG. 1, the coke oven gas (COG), CO 2 H 2 O is introduced into the reforming reactor to perform the reforming reaction, whereby the synthesis gas for reducing iron ore can be produced.
Although not shown in FIG. 1, the reforming reaction apparatus may include a metering gas supply device such as a blower to regulate the supply rate of coke oven gas (COG), CO 2 , and H 2 O. On the other hand, in the case of H 2 O, it may include a system for additionally controlling the supply amount of steam and the pressure after manufacturing water.
Further, an additional device may be included to control the specific reaction conditions of the reforming reaction. For example, a reaction pressure may be controlled by including a back-pressure regulator, etc., Alternatively, the reaction temperature may be controlled by an indirect heat supply method or the like, but the present invention is not limited thereto, and the reaction conditions can be controlled by various methods known in the art.
Although not shown in FIG. 1, it is preferable that the reforming reaction apparatus includes a catalyst. When the reaction gases are in contact with each other under the catalyst included in the reforming reaction apparatus, chemical reactions as shown in the following reaction formulas 1 to 4 occur.
CH 4 + CO 2 ↔ 2H 2 + 2 CO ... Reaction 1
CH 4 + H 2 O ↔ 3H 2 + CO ...
H 2 + CO 2 ↔ CO + H 2 O
CH 4 + 2H 2 O ↔ 4H 2 + CO 2 ...
Referring to equations (1) to ( 4 ) above, CH 4 and CO 2 in coke oven gas And / or H 2 O through the reaction mentioned above, the CO and H 2 are produced, with a H 2 and CO 2 reaction of the generated hydrogen or coke oven gas (COG), and CO is generated, such a reforming To finally obtain an iron ore reducing gas containing mainly H 2 and CO.
The catalyst for the reforming reaction of the present invention is preferably a nickel (Ni) -based reforming catalyst, and more specifically, a nickel-based reforming catalyst based on a support such as Al 2 O 3 , ZrO 2 , Ce-ZrO 2 or MgAl 2 O 4 A nickel-based reforming catalyst containing a promoter such as Ca, K, Mg, Ce, La, or a noble metal may be used.
In the present invention, thermodynamic equilibrium calculations were performed under various reaction conditions in order to find suitable reaction conditions for the synthesis of syngas for iron ore reduction.
The coke oven gas (COG) is a coke oven gas (COG) of 1.2 times to 2.5 times, based on the volume of CH 4 gae nitriding gas (CO 2 And H 2 O). That is, the volume of CH 4 in the coke oven gas (COG): total reforming gas (CO 2 And H 2 O) is preferably 1: 1.2 to 2.5, more preferably 1: 1.5 to 2.0.
The reforming gas (CO 2 And H 2 O) The case included a less than 1.2-fold based on the volume of CH 4 coke oven gas (COG), the CH 4 conversion and CO, so 2 conversion rate is lowered may cause problems of catalyst coking (coking) Iron Ore Reduction And when it is contained in an amount exceeding 2.5 times, the CH 4 conversion rate and the CO 2 conversion rate are increased but the unreacted reformed gas is increased, and the fraction of H 2 and CO in the finally obtained iron ore reducing gas There is a problem of lowering.
On the other hand, when the reforming gas of the present invention is CO 2 Wow H 2 O, the volume ratio of CO 2 and H 2 O constituting the reforming gas is preferably 1: 0.3 to 1: 5. When H 2 O exceeds the above range, the H 2 / CO ratio becomes higher than 4, which is not preferable as a synthesis gas for iron ore reduction. When H 2 O is contained in an amount less than the above range, there is a problem of catalyst caulking, which may cause problems in catalyst stability. The volume ratio of CO 2 and H 2 O is more preferably from 1: 1 to 1: 3.
The reforming reaction of the present invention is preferably carried out under a pressure of 2 to 20 bar, more preferably 4 to 10 bar. If the pressure at the reaction is less than 4 bar, When the pressure is higher than 10 bar, the methane conversion is lowered and the pressure is higher than that of the blast furnace / flow furnace, so that the reduced pressure There is a problem that an energy loss is generated.
The reforming reaction of the present invention is preferably carried out at a temperature of 850 to 1000 ° C, more preferably 900 to 950 ° C. When the reaction is carried out at a temperature lower than 850 ° C., the conversion of CH 4 or CO 2 is low. When the reaction is carried out at a temperature exceeding 1000 ° C., a reactor having a material which can be used stably for a long period at high temperature and high pressure is obtained There is a difficult problem.
The reforming reaction of the present invention is preferably performed at a reaction space velocity of 1,000 to 500,000 h -1 and more preferably at a reaction space velocity of 3,000 to 100,000 h -1 . The reaction space velocity is a value obtained by dividing the standard gas volume of the reactant flowing per hour by the volume of the catalyst. When the reaction space velocity is less than 1,000 h -1, the throughput of the reactant becomes small, There is a problem, and when it exceeds 500,000 h -1 , the conversion rate of methane and carbon dioxide is lowered due to the reaction rate problem.
Through the reforming reaction of the present invention, it is possible to finally obtain iron ores reducing gas containing mainly H 2 and CO. The total fraction of H 2 and CO in the gas is preferably 70 to 100%, more preferably 80 to 100%. When the total fraction of H 2 and CO in the syngas is less than 70%, there is a problem that iron ore reduction is not efficient when reducing the iron ore using such syngas.
On the other hand, the volume ratio (H 2 / CO) of H 2 and CO in the iron ore reducing gas is preferably 1 to 4, more specifically, the iron ore reducing gas containing an H 2 / An iron ore reduction gas suitable for a common blast furnace and having a H 2 / CO ratio of about 3 is suitable for the flow furnace.
Iron ore volume ratio of reduction in H 2 and CO gas (H 2 / CO) is the case of less than 1 is relatively lowered, the volume ratio of H 2 and CO than the reduction rate of iron ore using a gas with a large amount of hydrogen comprising (H 2 / CO) is more than 4 and contains a large amount of hydrogen, a reduction reaction of iron ores occurs by hydrogen, and this reaction is a considerable endothermic reaction, so that there is a problem that additional heat energy must be supplied from the outside.
In view of this, it is most preferable to use H 2 / CO mixed gas within the mixing ratio range of the present invention for the reduction of iron ore. Further, the reducing power of the synthesis gas having an H 2 / CO ratio of 2 or more is 100% The use of such a mixed gas can increase the production of iron ore, thereby achieving CO 2 reduction ultimately.
The CH 4 conversion and the CO 2 conversion rate of the reforming reaction of the present invention are preferably 50 to 100%, and when the CH 4 conversion rate and the CO 2 conversion rate are less than the above ranges, the reducing gas fraction in the generated gas is low, There is a problem.
On the other hand, the reducing gas containing H 2 and CO obtained from the reforming reaction of the present invention may be blown into a flow path or a blast furnace and used as a reducing gas for iron ores. However, the present invention is not limited thereto and can be widely applied to a process for reducing iron ores.
Hereinafter, the present invention will be described more specifically by way of specific examples. The following examples are provided to aid understanding of the present invention, and the scope of the present invention is not limited thereto.
Example
One.
CH
4
,
CO
2
And
H
2
O
of
At a volume ratio
Calculation of the characteristics of the mixed reforming reaction
The composition of the product gas of the thermodynamic equilibrium reaction was calculated by using a program (aspen plus) to confirm the characteristics of the mixed reforming reaction according to the volume ratio of CH 4 , CO 2 and H 2 O.
Example One
The production gas composition of the thermodynamic equilibrium reaction was set at a reaction pressure of 5 bar by setting the volume ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) to 1.0: 0.4: 0.8 at a reaction temperature of 750 to 950 ° C. Program (aspen plus).
Example 2
The production gas composition of the thermodynamic equilibrium reaction was measured in the same manner as in Example 1, except that the volume ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set to 1.0: 0.4: 1.2. Program (aspen plus).
Example 3
The production gas composition of the thermodynamic equilibrium reaction was determined in the same manner as in Example 1, except that the ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set at 1.0: 0.4: 1.6. Program (aspen plus).
Example 4
The production gas composition of the thermodynamic equilibrium reaction was determined in the same manner as in Example 1, except that the volume ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set to 1.0: 0.4: 2.0. Program (aspen plus).
Example 5
The production gas composition of the thermodynamic equilibrium reaction was measured in the same manner as in Example 1, except that the volume ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set at 1.0: 0.8: 0.8. Program (aspen plus).
The results of Examples 1 to 5 are shown in Fig. 2, wherein Fig. 2 (a) shows methane conversion, Fig. 2 (b) shows CO 2 conversion, Fig. 2 (c) shows fraction of reducing gas, ) Represents the H 2 / CO ratio, respectively.
2, when the method for producing iron ore reducing gas of the present invention is used, the ratio of H 2 / CO of the reducing gas generated at a reaction temperature of 850 ° C. or higher is included within the range of 1 to 5, The conversion of methane and the conversion of CO 2 were all above 50%, so it was confirmed that it could be used as a reducing gas for iron ore.
2.
COG
of mine
CH
4
of
By volume
H
2
O
And
CO
2
Containing
Reform
Calculation of the nature of the reforming reaction when the gas ratio is 1: 1.6
If the ratio of the reforming gas containing H 2 O and CO 2 is 1: 1.6 based on the volume of CH 4 in the COG, the production gas composition of the thermodynamic equilibrium reaction is programmed as aspen plus The results of the reforming reaction were calculated using the ratio of the mixed gas containing H 2 O and CO 2 of 1: 1.6 based on the volume of CH 4 in the COG.
Comparative Example One
The production gas composition of the thermodynamic equilibrium reaction was measured in the same manner as in Example 1, except that the volume ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set at 1.0: 0.0: 1.6. Program (aspen plus).
Example 6
Except that the volume ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set to 1.0: 0.4: 1.2, the production gas composition of the thermodynamic equilibrium reaction Program (aspen plus).
Example 7
The production gas composition of the thermodynamic equilibrium reaction was measured in the same manner as in Example 1, except that the volume ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set at 1.0: 0.8: 0.8. Program (aspen plus).
Example 8
Except that the volume ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set at 1.0: 1.2: 0.4, the production gas composition of the thermodynamic equilibrium reaction Program (aspen plus).
Example 9
The production gas composition of the thermodynamic equilibrium reaction was measured in the same manner as in Example 1, except that the volume ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set at 1.0: 1.6: 0.0 Program (aspen plus).
In Examples 6 to 9, when the ratio of the reforming gas containing H 2 O and CO 2 based on the volume of CH 4 in the coke oven gas (COG) was 1: 1.6, the characteristics of the reforming reaction were predicted The results of the thermodynamic equilibrium calculations are shown in Fig. FIG. 3 (a) shows the methane conversion, FIG. 3 (b) shows the CO 2 conversion, FIG. 3 (c) shows the reducing gas fraction, and FIG. 3 (d) shows the H 2 / CO ratio.
As can be seen from Examples 6 to 9 and Comparative Example 1, in Examples 6 to 9 of the present invention, the ratio of H 2 / CO was less than all 4, but when only H 2 O was used as a reforming agent, H 2 / CO It is not suitable to directly use the reducing agent for iron manufacturing because the ratio exceeds 4, and it can be confirmed that the H 2 / CO ratio needs to be adjusted to 4 or less through additional supply of CO.
3.
CH
4
,
CO
2
And
H
2
O
of
At a volume ratio
Characterization of Mixed Reforming Reaction
Example 10
Experiments were carried out to confirm the characteristics of COG mixed reforming reaction using PseudoChem commercial reformed Ni catalysts. For this purpose, general fixed bed reactivity evaluation apparatus was used to measure the reaction temperatures of 800, 850, 900, in CH 4 at 950 ℃ coke oven gas (COG): CO 2: H 2 O volume ratio of 1.0: 0.4: set to 1.2 and the reaction was carried out at 5bar.
Example 11
The mixed reforming reaction of coke oven gas (COG) was performed in the same manner as in Example 11, except that the ratio of CH 4 : CO 2 : H 2 O in the coke oven gas (COG) was set at 1.0: 0.8: 0.8. Respectively.
FIG. 4 shows the results of mixed reforming according to the volume ratios of CH 4 , CO 2 and H 2 O in Examples 10 and 11, wherein the conversion of CH 4 .
As can be seen from Examples 10 and 11, it was confirmed that the CH 4 conversion rate can be 50% at 850 ° C or higher in actual catalyst experiments. In this case, H 2 / CO ratio is 3 or less, H 2 + CO reduction gas fraction was more than 70%.
While the present invention has been particularly shown and described with reference to exemplary embodiments thereof, it is to be understood that the invention is not limited to the disclosed exemplary embodiments, but, on the contrary, It will be obvious to those of ordinary skill in the art.
Claims (11)
In the reaction, the coke oven gas (COG) is reacted with 1.2 to 2.5 times of reforming gas (CO 2 and H 2 O) based on the volume of CH 4 in the coke oven gas (COG) Way.
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| JP2007056159A (en) | 2005-08-25 | 2007-03-08 | Nippon Steel Corp | Method for producing high calorie gas |
| KR20110084772A (en) * | 2010-01-18 | 2011-07-26 | 주식회사 포스코 | Apparatus for manufacturing molten irons that is capable of reducing carbon dioxide emissions |
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| JP2007056159A (en) | 2005-08-25 | 2007-03-08 | Nippon Steel Corp | Method for producing high calorie gas |
| KR20110084772A (en) * | 2010-01-18 | 2011-07-26 | 주식회사 포스코 | Apparatus for manufacturing molten irons that is capable of reducing carbon dioxide emissions |
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