CN115341064A - Zero-carbon fluidized reduction method for iron ore powder - Google Patents
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- C21B13/0073—Selection or treatment of the reducing gases
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Abstract
The invention belongs to the fields of chemical industry and metallurgy, and discloses a zero-carbon fluidized reduction method for iron ore powder. According to the method, iron ore powder fluidization reduction is coupled with the hydrogen production of the solid oxide electrolytic cell, high-temperature hydrogen generated by electrolysis is used as a reducing agent and fuel, and high-temperature water vapor generated by reduction is circularly used for the hydrogen production of the solid oxide electrolytic cell, so that the process matching of an electrolysis system and a reduction system is enhanced, and the process energy efficiency is improved; the iron ore powder is preheated by burning the reduction tail gas and hot oxygen gas which is a byproduct of high-temperature water vapor electrolysis, and meanwhile, partial hot hydrogen gas is introduced for combustion and heat supplement, so that the gas utilization rate and the system energy utilization rate are improved; the temperature of the hydrogen and water vapor mixed gas is stabilized by a high-temperature heat storage technology, and the service life of the solid oxide electrolytic cell is prolonged. The method has the advantages of strong process feasibility, environmental friendliness, high resource utilization rate, high energy utilization rate and high reaction efficiency, and has good economic and social benefits.
Description
Technical Field
The invention belongs to the field of chemical industry and metallurgy, and particularly relates to a zero-carbon fluidized reduction method for iron ore powder.
Background
As a typical gas-based reduction reactor, compared with a shaft furnace, the fluidized bed omits a pellet preparation link, can directly treat fine ore, has the advantages of high mass and heat transfer rate between gas and solid phases, high reduction efficiency and the like, and is an iron ore smelting technology with a good development prospect. The prior typical fluidized direct reduction ironmaking process comprises a FIOR/FINMET process, a Circored process, a Circofer process and the like.
In the FIOR/FINMET process (U.S. Pat. No. 5,5082251,5833734), iron ore fines having a particle size of less than 12.7mm are passed successively through 4 fluidized-bed reactors connected in series, counter-currently to the fluidized reducing gas. The temperature of the first-stage fluidized bed reactor is about 550 ℃, the temperature is gradually increased downwards, the temperature of the fourth-stage fluidized bed reactor is about 800 ℃, and the pressure is 1.1-1.4MPa. The metallization rate of the product at the outlet of the four-stage fluidized bed reaches 93 percent, and the content of C is about 0.5 to 3 percent. Conveying the reduced iron powder to a hot press, hot-pressing into blocks with the density of more than 5g/cm 3 It is more compact and can reduce the oxidation of products. The fluidized reducing gas consists of fresh gas obtained by steam reforming of natural gas and circulating gas, and is heated to 850 ℃ before entering the four-stage reactor. In the Circored process, the reduction system consists of a primary Circulating Fluidized Bed (CFB) and a secondary bubbling Fluidized Bed (FB) (US 5527379). The CFB reactor used in a plant with a production capacity of 50 ten thousand tons/year had an outer diameter of 5.2m and a height of 29.6m, an outer diameter of 5.5m for an external circulation cyclone, an outer diameter of 7.0m for an FB reactor, a total length of 17.5m, and four material chambers inside. Fluidizing the reducing gas to pure H 2 . The reduction temperature of the first-stage fast fluidized bed is 630-650 ℃, the reduction temperature of the second-stage bubbling fluidized bed is about 680 ℃, and the pressure is 0.4MPa. The obtained reduced iron powder can be hot pressed into briquettes or directly used for powder metallurgy. The Circofer process is similar to the Circored process, employing two stages of reduction: a first-stage fast fluidized bed and a second-stage bubbling fluidized bed. The difference is that the circumfer technology takes coal as main energy, the coal is partially oxidized in a heat generator outside the fast fluidized bed, not only can supply heat and fluidized reducing gas, but also can generate carbon powder, and can play a role of preventing bonding, thereby leading the iron ore powder to be reduced at higher temperature, and realizing the purpose of reducing the iron ore powderHigh efficiency production (US 5603748). The reduction temperature of the first-stage fast fluidized bed is 950 ℃, the metallization rate of the outlet product reaches 80 percent, the reduction temperature of the second-stage bubbling bed is 850 ℃, and the metallization rate of the outlet product reaches more than 93 percent.
In addition, many chinese patents also propose fluidized direct reduction ironmaking processes, such as CN103667571B, CN103725819B, CN106319126B, CN106467930B, etc. However, the existing fluidized ironmaking process is directly or indirectly dependent on fossil fuels, such as coal or natural gas combustion to provide heat, coal gasification or natural gas reforming to provide reducing gas (H) 2 CO) and the like, and the participation of fossil fuels can lead to the emission of a large amount of CO in fluidized iron making 2 Aggravate the greenhouse effect. For this reason, metallurgists began to explore iron making using clean energy. In Beijing in 1999, the 125 th Xiangshan science conference, xuandei academy proposed the concept of iron ore hydrogen reduction for the first time, and in the metallurgy strategy forum held by Shanghai university by the national science Foundation Committee in 2002, xuandei academy proposed the technical idea of hydrogen metallurgy again. Hydrogen energy is the cleanest energy in the world, has the advantages of high combustion heat value, rich sources and the like, and can be prepared in a large scale by water electrolysis besides fossil fuels. The hydrogen is used as a combustion product of fuel and a reduction product of a reducing agent only containing water in the iron-making industry, and is an important direction for sustainable development of the iron-making industry in the future.
The hydrogen production by water electrolysis is a mature technology for industrially producing hydrogen, and water molecules in an electrolytic cell are subjected to electrochemical reaction on an electrode by supplying energy through electric energy and are decomposed into hydrogen and oxygen. The water decomposition reaction mainly comprises the following steps: cathodic evolution reaction (HER) and anodic evolution reaction (OER). At present, water electrolysis hydrogen production technologies can be divided into three categories according to the difference of electrolytes, namely Alkaline Water Electrolysis (AWE), proton exchange membrane water electrolysis (PEM), and solid oxide water electrolysis (SOEC). Among them, the alkaline water electrolysis technology is the most mature and widely applied to industries such as energy storage, metallurgy, pharmacy, food and the like. The alkaline water electrolysis hydrogen production system has a simple structure, does not need to use a noble metal catalyst, and has the advantages of safe and reliable technology, low manufacturing cost, simple operation, long service life and the like, but the alkaline water electrolysis technology has the problems of low electrolysis efficiency, high energy consumption and the like. In addition, the alkaline water electrolysis technology works at room temperature, the process matching with high-temperature gas-based direct reduction iron making is poor, the heat loss of a room-temperature alkaline water electrolysis-high-temperature reduction iron making system is high, and the process energy efficiency is low. The proton exchange membrane technology has the advantages of no pollution in reaction, compact device structure, high conversion efficiency and the like, but the proton exchange membrane and the platinum electrode have higher catalytic cost, so that large-scale application of the proton exchange membrane and the platinum electrode is not realized. The solid oxide technology has the advantages of high efficiency, simplicity, flexibility, environmental friendliness and the like, the working temperature is as high as 600-1000 ℃, the theoretical decomposition voltage of water is reduced by high-temperature operation, namely, the reaction overpotential is effectively reduced, the energy consumption is reduced, and the hydrogen production efficiency of the solid oxide electrolytic cell is close to 100 percent.
In conclusion, through technological and technical innovation, on the premise of not using fossil fuel and introducing carbon-containing substances, hydrogen is efficiently produced by electrolyzing water, fluidized direct reduction iron making is carried out by taking hydrogen as a reducing agent and fuel, the technological matching performance of a hydrogen production system and a reduction system is enhanced, the process energy efficiency and stability are improved, the energy utilization rate is improved, the production cost is reduced, and the method is an important way for realizing high-energy-efficiency zero-carbon iron making.
Disclosure of Invention
Aiming at the problems in the prior art, the invention aims to provide a zero-carbon fluidized reduction method for iron ore powder. The method can realize zero carbon emission in the fluidized direct reduction iron making process, has strong process feasibility, is environment-friendly, has high resource utilization rate, energy utilization rate and reaction efficiency, and has good economic benefit and social benefit.
In order to achieve the purpose, the invention adopts the following technical scheme:
a zero-carbon fluidized reduction method for iron ore powder comprises a combustion preheating process 1, a fluidized reduction process 2, a purification and dust removal process 3, a heat storage process 4, a solid oxide electrolytic cell electrolysis process 5, a hydrogen pressurization process 6, an oxygen pressurization process 7 and a cooling process 8, and specifically comprises the following steps:
1) In the combustion preheating process 1, part of the purified tail gas from the purification and dust removal process 3 is combusted with part of hot hydrogen from the hydrogen pressurization process 6, hot oxygen from the oxygen pressurization process 7 and introduced supplementary air, and iron ore powder is preheated to obtain hot ore powder;
2) In the fluidized reduction process 2, the hot ore powder is subjected to hot hydrogen reduction from the hydrogen pressurization process 6 to obtain hot reduced ore and dust-containing tail gas;
3) In the purification and dust removal process 3, the dust-containing tail gas is subjected to purification and dust removal and water supplementation to obtain purified tail gas, part of the purified tail gas is sent to the combustion preheating process 1, and the rest of the purified tail gas is sent to the heat storage process 4;
4) In the solid oxide electrolytic cell electrolysis process 5, the hydrogen and water vapor mixed gas with stable temperature from the heat storage process 4 is electrolyzed by the solid oxide electrolytic cell under the action of electric energy to obtain hot hydrogen and hot oxygen, the hot hydrogen is sent to the hydrogen pressurization process 6, and the hot oxygen is sent to the oxygen pressurization process 7;
5) In the cooling step 8, the hot reduced ore from the fluidized reduction step 2 is cooled to obtain direct reduced iron.
The iron ore powder is iron ore concentrate, and the particle size of the iron ore powder is 0.1-5mm.
In the fluidized reduction process 2, the reduction temperature is 600-900 ℃, the reduction time is 0.5-2h, and the reduction pressure is 0.1-1MPa.
In the heat storage step 4, the heat storage technology is phase change heat storage, and the heat storage material is one or a combination of molten salts and metal alloys.
In the solid oxide electrolytic cell electrolysis step 5, the electrolyte material of the solid oxide electrolytic cell is Y 2 O 3 Stabilized ZrO 2 Based on electrolyte, the cathode material of the solid oxide electrolytic cell is Ni-doped Y 2 O 3 Stabilized ZrO 2 Cermet, solid oxide electrodeThe anode material of the electrolytic cell is perovskite type oxide-based material, and the electrolytic temperature is 600-900 ℃.
Preferably, the electrolyte material of the solid oxide electrolytic cell is 8mol% of Y 2 O 3 Stabilized ZrO 2 。
Preferably, the anode material of the solid oxide electrolytic cell is La 0.8 Sr 0.2 MnO 3-x -YSZ(Y 2 O 3 Stabilized ZrO 2 )、La 0.8 Sr 0.2 FeO 3-x -YSZ(Y 2 O 3 Stabilized ZrO 2 )、La 0.8 Sr 0.2 CoO 3-x -YSZ(Y 2 O 3 Stabilized ZrO 2 )、La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3-x -one of YSZ.
In the hydrogen pressurization step 6, the hot hydrogen outlet pressure is 0.11 to 1.1MPa.
In the oxygen pressurization step 7, the hot oxygen outlet pressure is 0.11 to 1.1MPa.
In the cooling step 8, the metallization rate of the directly reduced iron is not less than 92%.
Compared with the prior art, the invention has the following outstanding advantages:
(1) On the premise of not introducing carbon-containing substances, the iron ore powder fluidized reduction is coupled with the solid oxide electrolytic cell for electrolytic hydrogen production, hydrogen is used as a reducing agent for iron making and also used as fuel for heat supply, and high-temperature water vapor generated by reduction is circularly used for electrolytic hydrogen production in the solid oxide electrolytic cell, so that zero carbon emission in the direct reduction process of the iron ore powder is realized;
(2) In the invention, the high-temperature hydrogen generated by the electrolysis of the solid oxide electrolytic cell is used as the reducing gas of the fluidized reduction, the high-temperature water vapor generated by the fluidized reduction is used as the raw material of the solid oxide electrolytic cell, and the matching of the electrolysis hydrogen production system and the fluidized reduction iron making system is strong, thereby improving the energy efficiency of the whole process;
(2) According to the invention, the iron ore powder is preheated through the combustion of the hot oxygen generated by electrolyzing the reduction tail gas and the high-temperature water vapor, and part of hot hydrogen is introduced for combustion heat compensation, so that the gas utilization rate and the system energy utilization rate are improved;
(3) The invention stabilizes the temperature of the hydrogen-steam mixed gas by a high-temperature heat storage technology and prolongs the service life of the solid oxide electrolytic cell.
Drawings
FIG. 1 is a flow chart of the zero-carbon fluidized reduction method of iron ore powder of the present invention.
Detailed Description
The invention is described in further detail below with reference to the figures and the detailed description.
Example 1
As shown in fig. 1, the method for zero-carbon fluidized reduction of iron ore powder comprises a combustion preheating process 1, a fluidized reduction process 2, a purification and dust removal process 3, a heat storage process 4, a solid oxide electrolytic cell electrolysis process 5, a hydrogen pressurization process 6, an oxygen pressurization process 7 and a cooling process 8, and specifically comprises the following steps:
1) In the combustion preheating process 1, part of the purified tail gas from the purification and dust removal process 3 is combusted with part of hot hydrogen from the hydrogen pressurization process 6, hot oxygen from the oxygen pressurization process 7 and introduced supplementary air, and iron ore powder is preheated to obtain hot ore powder;
2) In the fluidized reduction process 2, the hot ore powder is reduced by hot hydrogen from the hydrogen pressurization process 6 to obtain hot reduced ore and dust-containing tail gas;
3) In the purification and dust removal process 3, the dust-containing tail gas is subjected to purification and dust removal and water supplementation to obtain purified tail gas, part of the purified tail gas is sent to the combustion preheating process 1, and the rest of the purified tail gas is sent to the heat storage process 4;
4) In the solid oxide electrolytic cell electrolysis process 5, the hydrogen and water vapor mixed gas with stable temperature from the heat storage process 4 is electrolyzed by the solid oxide electrolytic cell under the action of electric energy to obtain hot hydrogen and hot oxygen, the hot hydrogen is sent to the hydrogen pressurization process 6, and the hot oxygen is sent to the oxygen pressurization process 7;
5) In the cooling step 8, the hot reduced ore from the fluidized reduction step 2 is cooled to obtain direct reduced iron.
Example 2
In this example, the method of zero-carbon fluidized reduction of iron ore powder described in example 1 was used. Firstly, iron ore powder (total iron content is about 50%) with the particle size of 0.1-5mm is preheated by combustion of reduction tail gas and partial hot hydrogen to obtain hot ore powder. Fluidizing and reducing the hot ore powder in hydrogen at 600 ℃ for 2h, wherein the reduction pressure is 1MPa, and obtaining hot reduced ore and reduction tail gas. Part of the reduced tail gas is used for combustion preheating after purification and dust removal, and the rest of the purified tail gas is sent into a solid oxide electrolytic cell after the temperature is stabilized by a heat storage technology, wherein a heat storage material is molten salt, and an electrolyte material of the solid oxide electrolytic cell is 8mol% of Y 2 O 3 Stabilized ZrO 2 The cathode material of the solid oxide electrolytic cell is Ni-doped Y 2 O 3 Stabilized ZrO 2 The anode material of the cermet and solid oxide electrolytic cell is La 0.8 Sr 0.2 MnO 3-x YSZ, electrolyzing at 600 ℃ to obtain hot hydrogen and hot oxygen, wherein part of the hot hydrogen is used for combustion preheating after being pressurized to 1.1MPa, the rest is used for fluidized reduction of iron ore powder, and the hot oxygen is used for combustion preheating after being pressurized to 1.1MPa. The direct reduced iron with the metallization rate higher than 92 percent can be obtained after the hot reduced ore is cooled.
Example 3
In this example, the iron ore powder zero-carbon fluidized reduction method described in example 1 was adopted. Firstly, iron ore powder (the total iron content is about 62%) with the particle size of 0.1-5mm is preheated by combustion of reduction tail gas and part of hot hydrogen gas, and hot ore powder is obtained. Fluidizing and reducing the hot ore powder in hydrogen at 900 ℃ for 0.5h under the reduction pressure of 0.1MPa to obtain hot reduced ore and reduced tail gas. Part of the reduced tail gas is used for combustion preheating after purification and dust removal, and the rest of the purified tail gas is sent into a solid oxide electrolytic cell after the temperature is stabilized by a heat storage technology, wherein the heat storage material is metal alloy, and the electrolyte material of the solid oxide electrolytic cell is 8mol percent of Y 2 O 3 Stabilized ZrO 2 The cathode material of the solid oxide electrolytic cell is Ni-doped Y 2 O 3 Stabilized ZrO 2 Anode material of cermet and solid oxide electrolytic cell is La 0.8 Sr 0.2 FeO 3-x -YSZ, electrolysis at 900 ℃ to obtain hot hydrogen and oxygen, hot hydrogenAfter the pressure of the gas is increased to 0.11MPa, part of the gas is used for combustion preheating, the rest of the gas is used for fluidized reduction of iron ore powder, and after the pressure of the hot oxygen is increased to 0.11MPa, the hot oxygen is used for combustion preheating. The direct reduced iron with the metallization rate higher than 92 percent can be obtained after the hot reduced ore is cooled.
Example 4
In this example, the iron ore powder zero-carbon fluidized reduction method described in example 1 was adopted. Firstly, iron ore powder (total iron content is about 70%) with the particle size of 0.1-5mm is preheated by combustion of reduction tail gas and part of hot hydrogen gas to obtain hot ore powder. Fluidizing and reducing the hot ore powder in hydrogen at 800 ℃ for 0.7h under the reduction pressure of 0.5MPa to obtain hot reduced ore and reduced tail gas. Part of the reduced tail gas is used for combustion preheating after purification and dust removal, and the rest of the purified tail gas is sent into a solid oxide electrolytic cell after the temperature is stabilized by a heat storage technology, wherein the heat storage material is molten salt, and the electrolyte material of the solid oxide electrolytic cell is 8mol percent of Y 2 O 3 Stabilized ZrO 2 The cathode material of the solid oxide electrolytic cell is Ni-doped Y 2 O 3 Stabilized ZrO 2 The anode material of the cermet and solid oxide electrolytic cell is La 0.8 Sr 0.2 CoO 3-x -YSZ, electrolyzing at 700 ℃ to obtain hot hydrogen and hot oxygen, wherein part of the hot hydrogen is used for combustion preheating after the hot hydrogen is pressurized to 0.7MPa, the rest is used for fluidized reduction of iron ore powder, and the hot oxygen is used for combustion preheating after the hot oxygen is pressurized to 0.2 MPa. The direct reduced iron with the metallization rate higher than 92 percent can be obtained after the hot reduced ore is cooled.
Example 5
In this example, the iron ore powder zero-carbon fluidized reduction method described in example 1 was adopted. Firstly, iron ore powder (the total iron content is about 55 percent) with the particle size of 0.1-5mm is preheated by burning reduction tail gas and partial hot hydrogen to obtain hot ore powder. Fluidizing and reducing the hot ore powder in hydrogen at 750 deg.c for 1 hr under the reducing pressure of 0.3MPa to obtain hot reduced ore and reduced tail gas. Part of the reduced tail gas is used for combustion preheating after purification and dust removal, and the rest of the purified tail gas is sent into a solid oxide electrolytic cell after the temperature is stabilized by a heat storage technology, wherein the heat storage material is metal alloy, and the electrolyte material of the solid oxide electrolytic cell is 8mol percent of Y 2 O 3 StabilizedZrO 2 The cathode material of the solid oxide electrolytic cell is Ni-doped Y 2 O 3 Stabilized ZrO 2 The anode material of the cermet and solid oxide electrolytic cell is La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3-x And (3) electrolyzing at 850 ℃ to obtain hot hydrogen and hot oxygen, wherein part of the hot hydrogen is used for combustion preheating after the hot hydrogen is pressurized to 0.4MPa, the rest of the hot hydrogen is used for fluidized reduction of iron ore powder, and the hot oxygen is used for combustion preheating after the hot oxygen is pressurized to 0.15 MPa. The direct reduced iron with the metallization rate higher than 92 percent can be obtained after the hot reduced ore is cooled.
In the present invention,% is not specified, and is a mass percentage content.
The method can be realized by upper and lower limit values and interval values of intervals of process parameters (such as temperature, time and the like), and embodiments are not listed.
Conventional technical knowledge in the art can be used for the details which are not described in the present invention.
Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and are not limited. Although the present invention has been described in detail with reference to the embodiments, it will be understood by those skilled in the art that various changes may be made and equivalents may be substituted without departing from the spirit and scope of the invention as defined in the appended claims.
Claims (8)
1. The method for zero-carbon fluidized reduction of iron ore powder comprises a combustion preheating process (1), a fluidized reduction process (2), a purification and dust removal process (3), a heat storage process (4), a solid oxide electrolytic cell electrolysis process (5), a hydrogen pressurization process (6), an oxygen pressurization process (7) and a cooling process (8), and specifically comprises the following steps:
1) In the combustion preheating process (1), part of purified tail gas from the purification and dust removal process (3) is combusted with part of hot hydrogen from the hydrogen pressurization process (6), hot oxygen from the oxygen pressurization process (7) and introduced supplementary air, and iron ore powder with the thickness of 0.1-5mm is preheated to obtain hot ore powder;
2) In the fluidized reduction process (2), reducing the hot ore powder by hot hydrogen from the hydrogen pressurization process (6) at 600-900 ℃ to obtain hot reduced ore and dust-containing tail gas;
3) In the dust-removing purification process (3), the dust-containing tail gas is purified and dedusted, water is supplemented to obtain purified tail gas, part of the purified tail gas is sent to the combustion preheating process (1), and the rest of the purified tail gas is sent to the heat storage process (4);
4) In the solid oxide electrolytic cell electrolysis process (5), the hydrogen and water vapor mixed gas with stable temperature from the heat storage process (4) is electrolyzed by the solid oxide electrolytic cell under the action of electric energy at the temperature of 600-900 ℃ to obtain hot hydrogen and hot oxygen, the hot hydrogen is sent to the hydrogen pressurization process (6), and the hot oxygen is sent to the oxygen pressurization process (7);
5) In the cooling step (8), the hot reduced ore from the fluidized reduction step (2) is cooled to obtain direct reduced iron.
2. The method of zero-carbon fluidized reduction of iron ore powder according to claim 1, wherein the iron ore powder is iron ore concentrate.
3. The method for zero-carbon fluidized reduction of iron ore powder according to claim 1 or 2, wherein in the fluidized reduction process (2), the reduction time is 0.5-2h, and the reduction pressure is 0.1-1MPa.
4. The method for zero-carbon fluidization reduction of iron ore powder according to any one of claims 1 to 3, wherein in the heat storage step (4), the heat storage technology is phase change heat storage, and the heat storage material is one or a combination of a molten salt and a metal alloy.
5. The method for zero-carbon fluidized reduction of iron ore powder according to any one of claims 1 to 4, wherein in the solid oxide electrolytic cell electrolysis process (5), the electrolyte material of the solid oxide electrolytic cell is Y 2 O 3 Stabilized ZrO 2 Based on electrolyte, the cathode material of the solid oxide electrolytic cell is Ni-doped Y 2 O 3 Stabilized ZrO 2 The anode material of the metal ceramic and solid oxide electrolytic cell is a perovskite type oxide-based material.
6. The method for zero-carbon fluidized reduction of iron ore powder according to any one of claims 1 to 5, wherein in the hydrogen pressurization process (6), the hot hydrogen outlet pressure is 0.11 to 1.1MPa.
7. The method for zero-carbon fluidized reduction of iron ore powder according to any one of claims 1 to 6, wherein in the oxygen pressurization process (7), the hot oxygen outlet pressure is 0.11 to 1.1MPa.
8. The method for zero-carbon fluidized reduction of iron ore powder according to any one of claims 1 to 7, wherein the metallization rate of the directly reduced iron in the cooling process (8) is not less than 92%.
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