CN1752180A - Method with coke-oven gas dry coke quenching and coke desulfurating - Google Patents
Method with coke-oven gas dry coke quenching and coke desulfurating Download PDFInfo
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Abstract
The increase in demand of low sulfur coke, and the ability of the desulfurization of rich hydrogen coke-oven gas does not obtain utilizing in the process of coking.According to the characteristics of dry coke quenching technology, invented dry coke quenching process circulation coke-oven gas and realized the coke desulfurating method: the coke-oven gas that promptly circulates in the quenching stove of dry coke quenching auxiliary replaces round-robin rare gas element in the original technology (mainly being nitrogen).The endothermic pyrolysis reaction of the methane in the coal gas and coke-oven gas guarantee that with respect to the bigger heat transfer efficiency of nitrogen coal gas can more high efficiency quenching.The reaction of sulfide and organosulfur generates H in hydrogen in the coal gas and the coke
2S, thus reach the coke desulfurating purpose.Adopt this technology that the coke sulphur content is significantly reduced.
Description
Technical Field
The invention relates to a low-sulfur coke production technology and a dry quenching technology. The present invention belongs to the field of coal chemical industry and metallurgy.
Background
The largest consumer of coke is the iron industry. The sulfur content in the coke significantly affects the energy consumption and molten iron quality of blast furnace ironmaking. For every 0.1% increase in sulfur in the coke, the coke ratio needs to be increased by1.5%, while the capacity of the blast furnace is reduced by 2.5%. Most of the sulfur in the coke finally enters the molten iron, and the molten iron with high sulfur content increases the cost and time of the molten iron pretreatment.
China is a world large country for coke production. In recent decades, the total coke yield of China has doubled, and in recent years, the coke yield of the world is about 3.6 hundred million tons every year, wherein one third of the coke yield comes from China. The coke yield of China is the first in the world continuously, and the coke yield is about 1.2-1.3 hundred million tons every year. The coke has a special position in the development of national economy as an important raw material and fuel in the industries of metallurgy, machinery, chemical industry, nonferrous industry and the like. With the continuous development of economy in China, the demand of coke is continuously increased. According to statistics of the national statistical bureau, in recent years, 11000-12000 ten thousand tons of coke are consumed nationwide, and more than 1000 ten thousand tons of coke are exported. For the iron and steel industry, the blast furnace smelting is the main part of the iron and steel industry in the early 21 st century, and the total coke demand of the iron and steel industry in China is about 1 hundred million tons only.
At present, the quality of coke in China is below secondary coke. 1519 million tons of export coke in 2000 have an average price of 60.26 dollars/ton, which is 15-20 dollars/ton lower than the international normal price, and the national loss is about two hundred million and fifty million dollars. One of the important reasons is the high sulfur content of coke. This seriously affects the competitiveness of Chinese coke in the international market. The sulfur content of the coke is an important index for evaluating the quality of the coke, so that how to reduce the sulfur content of the coke is an urgent problem to be solved.
In order to overcome the adverse effect of sulfur in coke on smelting, the addition of sulfur-binding agent (CaO-base or CaCl) into coking coal has been adopted at home and abroad2Radical and BaCO3Radical sulfur-binding agents). The drawbacks of this process are reduced coke strength and increased coke ash. And thus has not been industrially applied. The sulfur in the coke finally enters the furnace slag and steel in the smelting process, and the resource of the sulfur cannot be realized. If the sulfur in the coke is transferred into the coal gas, the sulfur obtained after the coal gas is desulfurized can be recycled.
In the coke dry quenching process, cold inert gas is blown into the coke dry quenching furnace through a circulating fan to exchange heat with red hot coke, the coke is cooled, the inert gas absorbing the sensible heat of the red coke transfers the heat to a boiler to generate steam, and finally the cooled inert gas is blown into the coke dry quenching furnace through the fan to be recycled. Methane accounting for about 25-30% of coke oven gas is subjected to endothermic cracking reaction at a temperature above 800 ℃, and coke can be well cooled. And the coke oven gas has higher heat transfer efficiency than nitrogen. The quantity of circulating gas delivered is therefore reduced, with a corresponding reduction in energy consumption. The components of the recycle gas are mainly hydrogen, methane, and carbon monoxide, and therefore, coke is not oxidized. Therefore, the coke oven gas can replace inert gas to be circulated in the dry quenching process, and the purposes of recovering the sensible heat of the coke and desulfurizing the coke are achieved.
In order to meet the requirements of economic development and environmental protection and realize efficient and clean utilization of coal resources, clean coal utilization technologyhas been paid attention from all countries around the world. The coal hydrocracking is a coal conversion technology between gasification and liquefaction, and by utilizing the process, not only can coal gas with high calorific value be obtained, but also clean semicoke with low sulfur and low nitrogen can be obtained. Some research results also show that the process has the advantage of efficiently removing inorganic sulfur and organic sulfur in coal, and overcomes the defects of low desulfurization rate, high cost and narrow product application of the traditional physical and chemical desulfurization method. However, the traditional coal hydropyrolysis process takes expensive pure hydrogen as raw material, and the separation and recycling process of hydrogen is complex, and the investment accounts for 2/3 of the investment of the whole process. Therefore, foreign scholars propose a new process for co-pyrolysis of coal-coke oven gas in recent years, which greatly reduces the production cost and simplifies the production equipment. In addition to the features described above, a number of experimental results on this process indicate that: compared with the coal pyrolysis by using inert gas, the coal desulfurization rate is greatly improved by using coke oven gas to carry out the heating pyrolysis of the coal. The process shows that the coke oven gas has good desulfurization capability at the same time. However, these research and patented technologies are not directed to coke desulfurization, and the problem of coke desulfurization cannot be solved, because the aforementioned coal hydropyrolysis process generally uses a fluidized bed to heat and pyrolyze pulverized coal using hydrogen-rich gas as a carrier gas, the hydropyrolysis temperature generally does not exceed 700 ℃, the obtained product is low-sulfur particle semi-coke, and bulk coke cannot be obtained, and coking is that coal is heated to about 1000 ℃ in a fixed bed with air being isolated, and the product is bulk coke. So far, the research report andthe patent technology of coke desulfurization do not exist in countries all over the world.
Although the dry quenching process differs greatly between the cyclic coke oven gas desulfurization and the coal hydropyrolysis, the temperature of the coal hydropyrolysis is significantly lower than that of the red coke, and generally does not exceed 700 ℃, and the coal hydropyrolysis is generally carried out under pressure. However, previous work on the ability of coal to be hydropyrolyzed to produce low sulfur semi-coke has provided us with the suggestion that if coke oven gas is recycled during dry quenching, the coke can be desulfurized.
The closest Patent to this Patent is the METHOD OF OPERATING DRY Patent for apparatus for HOT COKE (United States Patent, Patent Number: 5,609,730). This patent is clearly distinguished from this patent. The difference is mainly in the composition of the gaseous medium cooling the heat exchange. The hydrogen-rich gas used in the method, such as coke oven crude gas, is different from the inert gas used in the traditional process, such as nitrogen and the like. The hydrogen-rich gas can not only quench coke, but also achieve the aim of coke desulfurization through the reaction of the hydrogen and organic sulfur and inorganic sulfur in the coke.
Disclosure of Invention
The invention aims to: the method adopts coke oven gas generated in the coking process as a raw material, and under the condition of not changing the prior process flow, the coke oven gas is circulated in a coke quenching furnace of a coke dry quenching device to replace inert gas (mainly nitrogen) circulated in the prior process. The endothermic cracking reaction of methane in the coal gas and the larger heat transfer efficiency of the coke oven gas relative to nitrogen ensure that the coke quenching of the coal gas can be carried out with higher efficiency. The hydrogen in the coal gas reduces sulfide and thiophenic sulfur in the coke and prevents the hydrogen sulfide in the coal gas from being converted into red coke to be thiophenic sulfur, thereby achieving the aim of coke desulfurization. The coal gas is not obviously consumed, and only needs to be circulated.
During the dry quenching process, hot red coke is transported from the coke oven to a quenching tower, lifted to the top end of the tower by a lifter, and discharged to a pre-storage chamber. Generally, the temperature of the coke at this time is 1050 ℃. The pre-chamber lid is only opened when the coke is discharged. The coke in the quenching furnace falls from the top by gravity and, after cooling, the temperature of the coke coming out of the bottom of the quenching furnace is about 180 ℃. The cooling of the coke is a result of the countercurrent heat exchange of the coke and the circulating inert gas. After the sensible heat of the coke is brought out of the coke quenching furnace by the inert gas, the heat is transferred to the steam by the steam generating device, and the steam with the temperature of about 350 ℃ and the pressure of 2.06MPa can be generated. The cooled gas from the steam generating device is returned to the quenching furnace. The components of the recycle gas are mainly hydrogen, carbon monoxide, methane, and therefore, coke is not oxidized.
The coke oven gas is a coking byproduct and usually contains 50-55% of H225 to 30% of CH4The rest is small amount of CO and CO2，CnHmEtc. H2The S content is generally about 0.7%. The sulfur in the coke is derived from coking coal. Most of the sulfur in coal exists in the form of pyrite sulfur, one part of sulfur exists in the form of organic sulfur, and the content of sulfate sulfur generally does not exceed 0.2% and is close to a constant. Organic sulfur is generally divided into aliphatic sulfur and aromatic sulfur, and mainly includes sulfides such as mercaptan and thioether. During coking, sulfur is present in coal at about 60% of the solids and 40% of the volatiles. There is both inorganic sulfur and organic sulfur attached to carbon groups in the coal in the coke. In the pre-coking stage (the colloidal stage), the sulfur in the gas is mainly derived from sulfur in aliphatic sulfur-containing compounds in the coal; in the later stage of coking, the sulfur in the coal gas mainly comes from two parts of pyrite sulfur and thiophene organic sulfur. In the later stage of coking, because the gas generation rate is greatly reduced and the coking chamber is lack of active hydrogen, the sulfur in the semicoke rarely enters the gas, and most of the sulfur in the coal is remained in the coke before the coke is discharged from the furnace. During the red hot coke cooling process, inorganic and organic sulfur in the coke is converted to thiophenic sulfur, which is difficult to remove once formed. If coke oven gas with hydrogen-rich atmosphere is used as the medium for heat exchange in the process of dry quenching, the conversion of inorganic sulfur and organic sulfur into thiophenic sulfur can be weakened, and partial sulfur in the coke can be converted into H2S enters the coal gas, so that the sulfur in the coke is further removed. Generally, coke oven gas of a coking byproduct is used as civil gas or chemical raw materials after being subjected to desulfurization and purification treatment, and gas for dry quenching can also enter a coke oven gas purification treatment system after passing through a heat exchanger and then enter a gas pipe network after being subjected to desulfurization treatment.
The technology of the invention is to purify and desulfurize the low-sulfur gas, or hydrogen, or natural gas, or water vapor generated by the coke oven in the process of dry quenchingGas, or a mixture thereof, is introduced into the dry quenching furnace as shown in FIG. 1. On one hand, sensible heat in the coke is transferred to a steam boiler by utilizing higher heat transfer efficiency of the coke oven gas to save energy and generate electricity, the flow of circulating gas can be reduced, and thus the power energy consumed by wind power transmission is saved. On the other hand, iron sulfide and thiophenic sulfur in the coke react with the introduced hydrogen or hydrogen product at high temperature to generate H2S enters into coal gas, thereby achieving the purpose of coke desulfurization. The main chemical reaction is as follows:
hydrogen generation reaction:
and (3) coke desulfurization reaction:
as can be seen from the above reaction, any gas containing hydrogen or gases that can react to form hydrogen in dry quenching can be used in the present invention. Preferably low sulfur coke oven gas, or hydrogen, or natural gas, or steam, or a mixture thereof. The gas can be desulfurized and rapidly dry-quenched by only containing hydrogen, but for better effect, the content of hydrogen is preferably 10 to 100% by weight, more preferably 20 to 100% by weight,and most preferably 50 to 100% by weight. Introducing low-sulfur coke oven gas, or hydrogen, or natural gas, or water vapor, or a mixture of the coke oven gas and the water vapor in the dry quenching process, not only reducing the sulfur content of the coke, but also recovering the sensible heat of the coke and increasing the gas content to convert the sensible heat of the coke into the chemical energy of the gas,due to CH4Or H2The O-cleavage is an endothermic reaction. Because the reaction absorbs heat, the heat exchange efficiency can be improved, and the heat exchange time is reduced.
Drawings
FIG. 1 is a schematic diagram of a process for removing sulfur in coke by circulating coke oven gas in a dry quenching process. In the figure: 1. coke quenching furnace 2, blower 3, heat exchange boiler 4, desulfurizing device 5, purifying and dedusting device
Carrying out the step
A branch is added in front of the blower 2 for adding fresh coke oven gas for gas circulation. The coke oven raw gas generated by the coking chamber is mainly composed of H2、CH4、CO、H2S and tar composition, and the coke oven crude gas is purified to remove dust, tar and H2And entering a circulation process after S. The purified coke oven crude gas and the circulating coke oven gas enter the coke quenching furnace 1 together to exchange heat with hot coke, and the sulfur in the coke is removed to form H2And S. CH in fresh coke oven gas4The heat exchange efficiency can be well improved. And the air quantity in the coke dry quenching process can be controlled by adjusting the ratio of the coke oven gas flow to the circulating gas flow. After the coke oven gas comes out of the coke quenching furnace, the coke oven gas flows through a purification device 5 to remove dust, and then enters a heat exchange boiler 3 to heat water vapor. Most of the cooled coal gas is recycled by the blower 2, and a small part of the cooled coal gas is subjected to H removal by the desulfurization device2And S, leaving the system. The circulation ratio is the effect of adjusting heat transfer and the conveying amount of gas. A branch is added on a pipeline between the heat exchange boiler 3 and the blower 2 and used for taking part of the coke oven gas out of the circulating gas path. The coke oven gas can be continuously utilized after passing through a desulphurization device 4. Can also be directly used for producing coal gas. Other implementation steps are the same as those of the common dry quenching method.
Examples
Example 1
5kg of coke of a certain factory is loaded in a small vertical straight pipe quenching chamber reactor, the sulfur content of the coke is 0.71 percent, the reactor is heated, heating is stopped when the temperature reaches the actual coke discharging temperature of the coke oven of 1000 ℃, and simulated coke oven gas at normal temperature (about 25 ℃) is fed from the bottom of the reactor to cool red hot coke, wherein the components of the coke oven gas (all gas components in the example are in volume percentage) are about 55 percent H2-25 percent CH4-15 percent CO-5 percent N2, the gas supply speed is 50L/min, and gas supply is stopped until the temperature of the furnace is reduced to 200 ℃. The test cooling process takes 160 minutes, and the average sulfur content of the coke after the test is 0.45 percent. And nitrogen is introduced under the same conditions for experimental comparison, the cooling process takes about 190 minutes, and the average sulfur content of the coke is 0.70%. After the coal gas is introduced, the sulfur content of the coke is reduced to 0.45 percent from the original 0.71 percent, the desulfurization rate reaches 37 percent, and the cooling time is reduced by 16 percent.
Example 2
Simulated coke oven gas blown in as in example 1 was 55% H2-25％CH4-15％CO-5％N2The experiment of example one was repeated with natural gas instead. The natural gas comprises the following main components: 93.38% CH4-2.68％N2-1.86％CO2-1.67％C2H6. The test cooling time is 110min, and the average sulfur content of the coke obtained by analysis after the test is 0.50%. Compared with a blank test in which nitrogen is introduced under the same condition, the sulfur content of the coke is reduced by 30% and the cooling time is reduced by 42% after the coal gas is introduced.
Example 3
Simulated coke oven gas blown in as in example 1 was 55% H2-25％CH4-15％CO-5％N2Is changed into H2The test of example one was repeated, and after the test the average sulfur content of the coke analyzed was 0.41% and the cooling time was 205 min. Compared with the corresponding blank test, after the coal gas is introduced, the sulfur content of the coke is reduced by 42 percent, and the cooling time is increased by 8 percent.
Example 4
The gas supply speed in example 1 was changed to 80L/min, the test of example one was repeated, and after the test, the average sulfur content of the coke analyzed was 0.39%, and the cooling time was about 105 min. The average sulfur content of the coke in the corresponding blank test is 0.70 percent, and the temperature reduction time is 122 min. After the coal gas is introduced, the sulfur content of the coke is reduced by 45 percent, and the cooling time isreduced by 14 percent.
Example 5
The coke from example 1 was heated to 1100 c and the test of example one was repeated, after which the average sulfur content of the resulting coke was analyzed to be 0.40% and the time to cool was 190 min. The average sulfur content of the coke in the corresponding blank test is 0.70 percent, and the cooling time is 212 min. After the coal gas is introduced, the sulfur content of the coke is reduced by 44%, and the cooling time is reduced by 10%.
Example 6
A gas circulation apparatus was constructed on the basis of example 1, the gas circulation was forced by an oil-free vacuum pump, and the circulating gas was cooled by condensed water. Circulating coke oven gas in the pipeline, the main component is 55% H2-25％CH4-15％CO-5％N2. The gas flow entering the furnace tube is controlled to be 50L/min. The ratio of the flow of the circulating gas to the flow of the newly added coke oven gas is 10: 1. The procedure of example 1 was repeated to cool 5Kg of coke from 1000 ℃ to 200 ℃. The cooling time was 175min, and the sulfur content in the coke after the test was 0.48%. Compared with a blank test in which nitrogen is introduced under the same condition, the average sulfur content of the coke is 0.70 percent. The cooling process took 201 minutes. After the coal gas is introduced, the sulfur content of the coke is reduced by 32 percent, and the cooling time is reduced by 13 percent.
Example 7
The experiment of example 6 was repeated, the ratio of the circulation gas flow to the flow of freshly added coke oven gas being changed to 8: 1. The cooling time was 164min, and the sulfur content in the coke after the test was 0.46%. Compared with the blank test, the sulfur content of the coke is reduced by 35%, and the cooling time is reduced by 18%.
Example 8
The experiment of example 6 was repeated, the ratio of the circulation gas flow to the flow of freshly added coke oven gas being changed to 4: 1. The cooling time was 155min, and the sulfur content in the coke after the test was 0.41%. The sulfur content of the coke was reduced by 42% and the cooling time by 22% compared to the blank test.
Claims (4)
1. A method suitable for rapid dry quenching and coke desulfurization is characterized in that: the coke quenching heat exchange medium is hydrogen-rich component gas.
2. The heat exchange medium hydrogen-rich component gas of claim 1, wherein: the hydrogen-rich component gas is low-sulfur coke oven gas, or hydrogen, or natural gas, or a mixture of the low-sulfur coke oven gas and the hydrogen.
3. The heat exchange medium hydrogen-rich component gas of claim 2, wherein: the content of a hydrogen component or a methane component in the hydrogen-rich component gas is 10-100%.
4. Apparatus for the rapid dry quenching method as claimed in claim 1, 2 or 3 comprising: a pipeline is arranged in front of an air blower at the air inlet section of a circulating pipeline of the dry quenching device and is connected with compressed hydrogen-rich component gas, and a pipeline is arranged on a pipeline of the circulating gas leaving a heat exchange boiler and is connected with a desulfurizing device to produce clean coal gas.
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| CN108704435A (en) * | 2018-06-01 | 2018-10-26 | 中国环境科学研究院 | A kind of coal chemical enterprise exhaust gas/pollutant energy-saving and emission-reduction method and device |
| CN108704435B (en) * | 2018-06-01 | 2020-10-02 | 中国环境科学研究院 | Energy-saving and emission-reducing method and device for waste gas/pollutants of coking enterprise |
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