CN118240583A - Method for preparing high-quality carbon material raw material by using coal - Google Patents
Method for preparing high-quality carbon material raw material by using coal Download PDFInfo
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- CN118240583A CN118240583A CN202410569054.3A CN202410569054A CN118240583A CN 118240583 A CN118240583 A CN 118240583A CN 202410569054 A CN202410569054 A CN 202410569054A CN 118240583 A CN118240583 A CN 118240583A
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- 239000003245 coal Substances 0.000 title claims abstract description 158
- 238000000034 method Methods 0.000 title claims abstract description 49
- 239000003575 carbonaceous material Substances 0.000 title claims abstract description 43
- 239000002994 raw material Substances 0.000 title claims abstract description 42
- 239000010426 asphalt Substances 0.000 claims abstract description 94
- 238000005984 hydrogenation reaction Methods 0.000 claims abstract description 45
- 239000003250 coal slurry Substances 0.000 claims abstract description 26
- 239000003921 oil Substances 0.000 claims description 74
- 238000000926 separation method Methods 0.000 claims description 71
- 239000000047 product Substances 0.000 claims description 68
- 239000007787 solid Substances 0.000 claims description 47
- 239000002904 solvent Substances 0.000 claims description 46
- 238000000197 pyrolysis Methods 0.000 claims description 39
- 239000006184 cosolvent Substances 0.000 claims description 30
- 238000004821 distillation Methods 0.000 claims description 30
- 239000003054 catalyst Substances 0.000 claims description 28
- 239000002002 slurry Substances 0.000 claims description 27
- 239000012265 solid product Substances 0.000 claims description 24
- 239000010742 number 1 fuel oil Substances 0.000 claims description 22
- 238000002360 preparation method Methods 0.000 claims description 21
- 239000012263 liquid product Substances 0.000 claims description 20
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 13
- 239000001257 hydrogen Substances 0.000 claims description 13
- 229910052739 hydrogen Inorganic materials 0.000 claims description 13
- 238000002156 mixing Methods 0.000 claims description 12
- 239000011280 coal tar Substances 0.000 claims description 11
- 239000000843 powder Substances 0.000 claims description 9
- 238000003763 carbonization Methods 0.000 claims description 7
- 239000004744 fabric Substances 0.000 claims description 7
- 239000011148 porous material Substances 0.000 claims description 7
- 239000010779 crude oil Substances 0.000 claims description 5
- NIFIFKQPDTWWGU-UHFFFAOYSA-N pyrite Chemical group [Fe+2].[S-][S-] NIFIFKQPDTWWGU-UHFFFAOYSA-N 0.000 claims description 4
- 229910052683 pyrite Inorganic materials 0.000 claims description 4
- 239000011028 pyrite Substances 0.000 claims description 4
- 238000001914 filtration Methods 0.000 claims description 3
- 238000006243 chemical reaction Methods 0.000 abstract description 27
- 238000006068 polycondensation reaction Methods 0.000 abstract description 15
- 238000004519 manufacturing process Methods 0.000 abstract description 14
- 238000005336 cracking Methods 0.000 abstract description 8
- 125000004432 carbon atom Chemical group C* 0.000 abstract description 4
- 238000003754 machining Methods 0.000 abstract description 2
- SMWDFEZZVXVKRB-UHFFFAOYSA-N Quinoline Chemical compound N1=CC=CC2=CC=CC=C21 SMWDFEZZVXVKRB-UHFFFAOYSA-N 0.000 description 18
- 239000003077 lignite Substances 0.000 description 18
- 230000008569 process Effects 0.000 description 16
- 239000002817 coal dust Substances 0.000 description 14
- 230000000694 effects Effects 0.000 description 11
- 239000011294 coal tar pitch Substances 0.000 description 10
- 239000002245 particle Substances 0.000 description 10
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 8
- 125000003118 aryl group Chemical group 0.000 description 8
- 239000011300 coal pitch Substances 0.000 description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 7
- 229910001868 water Inorganic materials 0.000 description 7
- 239000000203 mixture Substances 0.000 description 6
- 230000008901 benefit Effects 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 229910052757 nitrogen Inorganic materials 0.000 description 5
- 239000011295 pitch Substances 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 229910052717 sulfur Inorganic materials 0.000 description 5
- 238000005292 vacuum distillation Methods 0.000 description 5
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 4
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 4
- 239000003795 chemical substances by application Substances 0.000 description 4
- 238000004939 coking Methods 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 239000011593 sulfur Substances 0.000 description 4
- 239000003039 volatile agent Substances 0.000 description 4
- 238000004458 analytical method Methods 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 125000005842 heteroatom Chemical group 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 230000009257 reactivity Effects 0.000 description 3
- 239000010117 shenhua Substances 0.000 description 3
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 2
- 230000002411 adverse Effects 0.000 description 2
- 229910021529 ammonia Inorganic materials 0.000 description 2
- MWPLVEDNUUSJAV-UHFFFAOYSA-N anthracene Chemical compound C1=CC=CC2=CC3=CC=CC=C3C=C21 MWPLVEDNUUSJAV-UHFFFAOYSA-N 0.000 description 2
- 238000009835 boiling Methods 0.000 description 2
- 239000007795 chemical reaction product Substances 0.000 description 2
- 239000000571 coke Substances 0.000 description 2
- 238000000921 elemental analysis Methods 0.000 description 2
- 239000000284 extract Substances 0.000 description 2
- 125000000524 functional group Chemical group 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 2
- 239000007791 liquid phase Substances 0.000 description 2
- 239000011302 mesophase pitch Substances 0.000 description 2
- 239000011331 needle coke Substances 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 230000006641 stabilisation Effects 0.000 description 2
- 238000011105 stabilization Methods 0.000 description 2
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 230000018044 dehydration Effects 0.000 description 1
- 238000006297 dehydration reaction Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 238000002309 gasification Methods 0.000 description 1
- 238000005087 graphitization Methods 0.000 description 1
- 150000004678 hydrides Chemical class 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229920002521 macromolecule Polymers 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- -1 monocyclic aromatic hydrocarbon Chemical class 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 238000006116 polymerization reaction Methods 0.000 description 1
- 238000011112 process operation Methods 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 150000003254 radicals Chemical group 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10C—WORKING-UP PITCH, ASPHALT, BITUMEN, TAR; PYROLIGNEOUS ACID
- C10C3/00—Working-up pitch, asphalt, bitumen
- C10C3/02—Working-up pitch, asphalt, bitumen by chemical means reaction
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10C—WORKING-UP PITCH, ASPHALT, BITUMEN, TAR; PYROLIGNEOUS ACID
- C10C3/00—Working-up pitch, asphalt, bitumen
- C10C3/06—Working-up pitch, asphalt, bitumen by distillation
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- General Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Civil Engineering (AREA)
- Structural Engineering (AREA)
- Materials Engineering (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Organic Chemistry (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
Abstract
The invention provides a method for preparing high-quality carbon material raw materials by utilizing coal, which is characterized in that oil-coal slurry is hydrotreated under lower temperature and pressure conditions to avoid excessive cracking and polycondensation of raw material coal in the reaction process, so that higher asphalt product yield is obtained; meanwhile, the hydrogenation reaction can remove the foreign elements in the asphalt product, so that the quality of the coal-based asphalt product is greatly improved. The coal-based asphalt product can be used as a high-quality carbon material raw material, secondary finish machining is not needed, and the ordered growth of carbon atoms in the carbon material in the production process can be ensured, so that the high-quality carbon material product is prepared.
Description
Technical Field
The invention relates to the technical field of coal chemical industry, in particular to a preparation method of a high-quality carbon material raw material.
Background
Carbon materials such as needle coke, carbon fiber, activated carbon and the like have higher application in the strategic emerging industry fields of new energy sources, automatic driving automobiles, energy storage, new generation information technology, high-end equipment manufacturing, energy conservation, environmental protection and the like. The coal resources in China are rich, the coal is utilized to prepare and produce the high-performance carbon material, the coal-based asphalt has the advantages of high carbon content, low molecular weight, high aromaticity, high polymerization degree and the like, and the prepared carbon material product has higher electric conductivity, heat conductivity, mechanical strength and graphitization performance and is a high-quality raw material for preparing the carbon material.
The existing preparation method of coal pitch mainly uses coal tar obtained after coal carbonization (the operation temperature is 500-1100 ℃) as a raw material, and pitch components in the coal tar are separated through separation methods such as distillation, extraction and the like. However, the preparation process of the coal tar pitch has the following technical problems:
Firstly, raw coal is subjected to severe cracking and polycondensation reaction at a very high temperature to generate a large amount of gas and coke products, so that the yield of coal-based asphalt is low (about 2% of the raw coal); meanwhile, asphalt products generated by coal pyrolysis are mutually polycondensed at high temperature to generate high-polycondensation organic matters, and the high-polycondensation organic matters can influence the ordered growth of carbon atoms in the carbon material generation process, so that the quality of the carbon material is seriously influenced, and when the coal asphalt prepared by the method is used for preparing the carbon material, the performance of the obtained carbon material is poor.
Secondly, in the carbonization process of coal, fine raw material coal dust and coke powder are mixed into coal tar along with reaction gas, so that coal-based asphalt products contain higher ash content; in addition, harmful elements such as oxygen, nitrogen, sulfur and the like in raw material coal cannot be effectively removed in the carbonization or coking process, and the harmful elements also enter coal tar and are further gathered in the coal-based asphalt product, so that the content of harmful miscellaneous elements in the coal-based asphalt product is very high; these ash and foreign elements can also severely affect the ordered growth of carbon atoms during the formation of the carbon material.
Therefore, the coal-based asphalt product cannot be directly used for producing high-grade carbon material products with high strength and high density, and secondary finishing is necessary, which can certainly increase equipment investment, operation cost, production period and the like of a carbon material production device, so that the production cost of the carbon material product is high, and the competitiveness of the product is seriously affected.
In addition, there is also a preparation method of coal-based asphalt, which is characterized in that the Shenhua group Limited liability company extracts the direct coal liquefaction residues and extracts asphalt products from the liquefaction residues. However, the reaction conditions adopted in the direct coal liquefaction process of Shenhua group Limited responsible company are very severe, and the reaction temperature of the process is 440-465 ℃ and the reaction pressure is 15-25MPa according to the patent CN108998068A filed by the process. The coal liquefaction process has the advantages that due to higher temperature and pressure, coal molecules are deeply cracked and hydrogenated in the reaction process to generate more oil products and gases, and the asphalt yield is lower. And asphalt generated by the process is mixed with unconverted coal, heavy liquefied oil and the like to form liquefied residues, and in order to obtain an asphalt product, the liquefied residues are required to be further processed, for example, asphalt substances are obtained by extracting the liquefied residues by adopting the technical scheme disclosed in patent CN101962560B, and then the asphalt substances are subjected to heat treatment to obtain a mesophase asphalt product with higher quality; according to the data disclosed in the examples of this patent, the yield of mesophase pitch was about 20% of the direct coal liquefaction residue, which generally accounts for about 30% of the feed coal, and it was further deduced that the yield of mesophase pitch was about 6% of the feed coal. The preparation method of the coal-based asphalt has very high equipment investment and operation cost due to very high pressure and temperature, and the yield of the mesophase asphalt is also low.
Along with the technical development of carbon materials, the demand of the market for high-quality coal-based asphalt is increasing, while the process route of the high-quality coal-based asphalt in the prior art is longer, the yield is lower, the market demand is difficult to meet, and a new technology of the high-quality coal-based asphalt with high yield and simple process route is urgently needed.
Disclosure of Invention
The invention aims to solve the problems and the shortcomings, and provides a method for preparing high-quality carbon material raw materials by using coal, which is characterized in that compared with the existing preparation method of coal-based asphalt, coal oil slurry is hydrotreated under lower temperature and pressure conditions to avoid excessive cracking and polycondensation of raw material coal in the reaction process, so that higher asphalt product yield is obtained; meanwhile, the hydrogenation reaction can remove the foreign elements in the asphalt product, so that the quality of the coal-based asphalt product is greatly improved. The coal-based asphalt product can be used as a high-quality carbon material raw material, secondary finish machining is not needed, and the ordered growth of carbon atoms in the carbon material in the production process can be ensured, so that a high-grade carbon material product with high strength and high density is prepared.
The technical scheme of the invention is realized as follows: a method for preparing high-quality carbon material raw materials by utilizing coal comprises the steps of coal slurry preparation, pyrolysis hydrogenation and product separation; after pyrolysis hydrogenation of the coal oil slurry, separating the prepared cooked coal slurry to prepare a coal-based asphalt product serving as a high-quality carbon material raw material; the method is characterized in that: the weight ratio of the pulverized coal to the solvent oil in the coal oil slurry to the catalyst is 1:1.4-2:0.001-0.03; the catalyst is pyrite powder with granularity less than 200; the operation conditions of pyrolysis hydrogenation are as follows: the pressure is 4-8MPa, the temperature is 390-440 ℃, the residence time is 30-90 minutes, and the volume ratio of hydrogen to coal oil slurry is 300-600:1.
Further, the product separation comprises liquid-solid separation, the liquid-solid separation is pressurized hot filtration separation, and the liquid-solid separation comprises primary liquid-solid separation and secondary liquid-solid separation; firstly, mixing the cooked coal slurry with a cosolvent to perform primary liquid-solid separation to obtain a first liquid product and a first solid product, and then mixing the first solid product with the cosolvent to perform secondary liquid-solid separation to obtain a second liquid product and a second solid product; mixing the first liquid product with the second liquid product to produce a mixed liquid product; the cosolvent is light coal tar with a distillation range of less than 200 ℃.
Still further: the weight ratio of the cooked coal slurry to the cosolvent is 0.5-2:1, and the operation temperature of the primary liquid-solid separation is as follows: the pore diameter of the filter cloth is 200-800 meshes at 60-120 ℃ and the pressure is 0.1-0.8MPa.
Still further, the weight ratio of the first solid product to the co-solvent is 1:1.5-3, the operation temperature of the secondary liquid-solid separation is as follows: the temperature is 60-100deg.C, the pore diameter of the filter cloth is 200-800 meshes, and the pressure is 0.5-0.8MPa.
The invention has the beneficial effects that:
Firstly, under the actions of milder pressure, reaction temperature and catalyst, the invention enables coal molecules to be cracked and converted into asphaltene, enables the asphaltene to be dissolved in a solvent for the first time, and enables hydrogenation to be carried out for stabilization, thereby avoiding further cracking or polycondensation of the asphaltene, reducing the yield of low-molecular oil gas products or high-polycondensation organic matters, further obtaining higher yield of asphalt products, and enabling the generated asphalt products to retain the original aromatic ring structures in the coal molecules; meanwhile, when the oxygen, nitrogen and sulfur in the raw material coal are subjected to pyrolysis hydrogenation, the mixed elements are easily reacted with hydrogen to generate hydrides such as water, ammonia and hydrogen sulfide, so that the mixed elements and functional groups containing the mixed elements are effectively removed, the content of the mixed elements in the asphalt product can be greatly reduced, and the quality of the asphalt product is greatly improved; the coal-based asphalt product has the characteristics of compact and ordered arrangement of aromatic ring structures, high content of aromatic ring side chains and unsaturated rings, high reactivity, low content of quinoline insoluble substances and the like, and is a high-quality raw material for preparing various carbon materials.
Secondly, the pyrite powder with the granularity smaller than 200 meshes is used as the catalyst, so that on one hand, the catalyst is cheap and easy to obtain, the cost is lower, the catalyst recovery is not considered, and the economy and the operation convenience are higher; meanwhile, the catalyst particle diameter is smaller, so that the surface area of the catalyst particles is larger, the catalyst has very high dispersibility in the coal oil slurry, and the catalyst particles have higher reaction activity, thereby being more beneficial to promoting the cracking and hydrogenation processes of coal molecules.
In addition, the reaction temperature and the reaction pressure are low, and high-quality coal-based asphalt products can be directly produced, so that equipment with lower pressure and temperature grades can be adopted, the production process flow can be greatly simplified, the equipment investment and the operation cost can be greatly reduced, and higher economic benefits are realized.
Drawings
FIG. 1 is a block diagram of the process flow of the present invention.
Detailed Description
In order to make the technical solution of the present invention better understood by those skilled in the art, the technical solution of the present invention will be clearly and completely described below with reference to the accompanying drawings.
As shown in FIG. 1, the method for preparing high-quality carbon material raw materials by utilizing coal comprises an oil-coal slurry preparation device 1, a pyrolysis hydrogenation reactor 2, a liquid-solid separation device 3, a distillation separation device 4, a rotary carbonization device 5 and a solvent oil preparation device 6.
As shown in fig. 1, the present invention includes the steps of:
1. Preparation of coal oil slurry
The raw material coal dust, the catalyst and the solvent oil from the solvent oil preparation device 6 are uniformly mixed in the coal slurry preparation device 1 according to a certain proportion to prepare coal oil slurry; in order to ensure the fluidity of the coal-oil slurry and the sufficient reaction of raw material coal dust, the granularity of the coal dust is preferably less than 200 meshes, so that coal dust particles have larger surface area, and can be fully contacted with solvent molecules, so that the solvent molecules can infiltrate into the coal dust particles, weaken and even break chemical bonds among coal macromolecules, so that the coal dust particles swell, the internal structure of the coal dust particles is looser and has larger volume, on one hand, the coal dust can be better suspended in solvent oil and is not easy to deposit, thereby being beneficial to the stability of the coal-oil slurry and being convenient for storage and transportation; on the other hand, the pyrolysis and hydrogenation of coal molecules are easier to occur, the pyrolysis hydrogenation reaction rate of the coal molecules is accelerated, and the conversion rate of coal is improved; in order to enable the catalyst particles to be more uniformly dispersed in the coal oil slurry and to have higher surface area, so that the catalyst particles have stronger reactivity, the catalyst particle size of the invention is also preferably less than 200 meshes; in addition, in order to reduce the adverse effect of moisture on the reaction and separation system of the invention and comprehensively consider the economic cost of dehydration, the moisture of the coal dust is less than 5 percent, and the moisture of the catalyst is less than or equal to 1 percent; the catalyst selected by the invention is low-cost and easily-obtained pyrite powder, so that the problem of catalyst recovery is not considered, and the operation procedure can be greatly simplified; in addition, in order to ensure that the coal oil slurry has better fluidity and can improve the processing capacity of the device, the ratio of coal powder to solvent oil in the coal oil slurry is 1:1.4-2, preferably 1:1.4-1.8; in order to ensure that the catalyst in the reaction system is enough to ensure the smooth running of the pyrolysis hydrogenation of the pulverized coal, and to control the cost of the catalyst and the adverse effect of the catalyst on the production device, the adding amount of the catalyst is 0.1-3 percent, preferably 0.3-0.5 percent, of the weight of the pulverized coal; the initial solvent oil used initially in the reaction is prepared from washing oil separated from low-temperature coal tar and anthracene oil according to a ratio of 1:1, the initial solvent oil is subjected to fixed bed unsaturated hydrogenation reaction to obtain hydrogenation mixed oil, the hydrogenation mixed oil is subjected to normal pressure distillation and cutting, and after light components before 180-200 ℃ are cut off, the rest distillate oil is the solvent oil used in the reaction; the aromatic carbon rate fa value of the solvent oil is between 0.45 and 0.50; the solvent oil has higher hydrogen supply capacity, and can provide high-activity hydrogen for free radical fragments produced by coal molecule pyrolysis so as to stabilize hydrogenation; after the continuous operation of the invention, the solvent oil fraction in the reaction product can be recycled, and the solvent oil does not need to be purchased additionally, thereby reducing the production cost of the invention.
2. Pyrolysis hydrogenation of coal oil slurry
The oil-coal-slurry is pressurized, mixed with pressurized hydrogen and enters a heating furnace to be heated (not shown in fig. 1), then enters a pyrolysis hydrogenation reactor 2, the oil-coal-slurry is subjected to pyrolysis hydrogenation treatment in a hydrogen atmosphere, and the obtained reaction product is cooled to obtain cooked coal-slurry; because the oil-coal-slurry pyrolysis hydrogenation reaction system is a gas-liquid-solid three-phase reaction system, the pyrolysis hydrogenation reactor 2 of the invention adopts a plug flow reactor, so that the materials in the reactor can keep continuous and stable flow, the residence time of the reaction materials in the reactor is easy to control, and the process operation conditions of the pyrolysis hydrogenation reactor 2 are as follows: the reaction pressure is 4-8MPa, the reaction temperature is 390-440 ℃, the gas-liquid ratio is 300-600:1, and the residence time is 30-90 minutes. The method can control the cracking depth of coal molecules under a milder condition, so that the coal molecules are cracked and converted into asphaltenes, the asphaltenes are dissolved in a solvent for the first time, hydrogenation is given for stabilization, further cracking or polycondensation of the asphaltenes is avoided, the productivity of low-molecular oil gas products or high-polycondensation coke products is reduced, higher yield of asphalt products is further obtained, and the generated asphalt products retain the original aromatic ring structures in the coal molecules; the oxygen, nitrogen and sulfur in the raw material coal are easy to react with hydrogen to generate water, ammonia and hydrogen sulfide when in pyrolysis hydrogenation, so that the hetero elements and functional groups containing the hetero elements are effectively removed, and the hetero elements in the asphalt product are greatly reduced, so that the coal-based asphalt product has the characteristics of compact and ordered aromatic ring structure arrangement, high content of aromatic ring side chains and unsaturated rings and high reactivity, and is a high-quality raw material for preparing various carbon materials; in addition, the pressure level of the equipment is reduced, and the equipment investment and the operation cost are further reduced.
3. Liquid-solid separation
The coal-based asphalt product serving as a high-quality carbon material raw material can be prepared by separating the cooked coal slurry. The product separation of the present invention includes liquid-solid separation and distillation separation.
Firstly, mixing the cooked coal slurry and the cosolvent according to a proportion, and then sending the mixture to a liquid-solid separation device 3 for separation to obtain a mixed liquid product and a second solid product. The liquid-solid separation device 3 of the present invention comprises a primary liquid-solid separation device 31 and a secondary liquid-solid separation device 32, wherein the primary liquid-solid separation device 31 and the secondary liquid-solid separation device 32 are preferably plate-frame type pressurized heat filtration devices.
The temperature of the cooked coal slurry is 60-150 ℃, the cooked coal slurry and the cosolvent are mixed according to the weight ratio of 0.5-2:1, and the mixture is stirred uniformly and then enters a first-stage liquid-solid separation device 31, and the weight ratio of the cooked coal slurry and the cosolvent is preferably 1:1; in order to ensure that the mixture formed by mixing the coal-water slurry and the cosolvent has better fluidity and a filter screen meeting the requirements is easy to purchase, the operation temperature of the primary liquid-solid separation device 31 is 60-120 ℃, and the operation temperature can be adjusted by adjusting the temperature of the coal-water slurry; because the solid content in the material processed by the primary liquid-solid separation device 31 is relatively low, the operation pressure of the primary liquid-solid separation device 31 is relatively small and is 0.1-0.8MPa, preferably 0.3-0.5MPa, in order to achieve the aim of both production cost and production efficiency; the primary liquid-solid separation device 31 is used for separating to obtain a first liquid product and a first solid product; because more asphalt product still remains in the first solid product, in order to separate out the asphalt product, the invention mixes the first solid product with the cosolvent again, in order to ensure that the first solid product and the cosolvent can be fully and uniformly mixed, the asphalt product in the first solid product is dissolved in the cosolvent, the weight ratio of the first solid product to the cosolvent is 1:1.5-3, preferably 1:2, and the first solid product and the cosolvent are heated to 60-120 ℃ after being mixed, and at least stirred for 60 minutes, and then the mixture is sent to a secondary liquid-solid separation device 32 for separation; the operation pressure of the secondary liquid-solid separation device 32 is higher, preferably 0.5-0.8MPa, because the solid content in the secondary liquid-solid separation device 32 is higher and the viscosity of the liquid phase component is higher, and the secondary liquid-solid separation device 32 separates to obtain a second liquid product and a second solid product; the first liquid product and the second liquid product are mixed to obtain a mixed liquid product rich in coal-based asphalt. The filter cloth used for the primary liquid-solid separation device 31 and the secondary liquid-solid separation device 32 has a pore diameter of 200-800 meshes, preferably 200-400 meshes.
The cosolvent is light oil with the distillation range of less than 200 ℃ obtained by distilling coal tar, and because the cosolvent contains a large amount of monocyclic aromatic hydrocarbon components, the cosolvent has good solubility for coal-based asphalt which is also rich in aromatic ring structures, so that on one hand, the asphalt components can be prevented from being mutually polycondensed to generate high-polycondensation organic matters, the content of quinoline insoluble matters in an asphalt product is greatly reduced, and the yield and quality of the coal-based asphalt product are guaranteed; on the other hand, the cosolvent dissolves and dilutes the asphalt component in the coal-water slurry, and greatly weakens the cohesive force between the liquid phase and the solid phase in the coal-water slurry, thereby being capable of accelerating the separation speed during the liquid-solid separation, effectively avoiding the mixing of unreacted coal dust, catalyst and the like into the mixed liquid product, and greatly improving the quality of the asphalt product.
4. Distillation separation
And sending the mixed liquid product into a distillation separation device 4, sequentially carrying out first atmospheric distillation and reduced pressure distillation, recovering a cosolvent and solvent oil required by preparing coal slurry, and separating a coal-based asphalt product.
The distillation separation device 4 comprises a first atmospheric distillation tower 41 and a reduced pressure distillation tower 42, the mixed liquid product is firstly sent to the first atmospheric tower 41 for first atmospheric distillation, and the operation conditions of the first atmospheric tower 41 are as follows: the pressure at the top of the tower is 0.05-0.1MPa, and the temperature at the top of the tower is 180-220 ℃; so that the cosolvent with lower boiling point can be separated out from the top of the first atmospheric tower 41, and the cosolvent returns to the liquid-solid separation device for recycling; the heavy components at the bottom of the first atmospheric tower 41 are sent to a vacuum distillation tower 42, and the vacuum distillation tower 42 is operated under the following conditions: the pressure at the top of the tower is-0.1 Mpa, and the temperature at the bottom of the tower is 330-360 ℃; thus, the solvent distillate can be separated from the top of the vacuum distillation tower 42, and the coal-based asphalt product of the invention can be obtained after cooling and crushing the materials separated from the bottom of the vacuum distillation tower.
5. Rotary dry distillation
Because the second solid product also contains partial distillate oil and asphalt components, in order to continuously recycle solvent oil, the second solid product is sent into a rotary dry distillation device 5 for dry distillation treatment to obtain dry distillation crude oil and semicoke products; the rotary dry distillation device 5 is a low-temperature dry distillation device, and the operation temperature is as follows: operating at 500-550 ℃ under micro negative pressure; the obtained semicoke product has the advantages of low moisture, high volatile, low sulfur, low nitrogen and the like, is a very clean fuel, and can also be used for preparing coal water slurry for gasification hydrogen production and the like.
6. Solvent oil preparation
And mixing the dry distillation crude oil with solvent distillate oil, and then sending the mixture to a solvent oil preparation device 6 for hydrogenation and second normal pressure distillation in sequence to prepare the solvent oil with higher hydrogen supply capacity.
The solvent oil preparation device 6 comprises a solvent hydrogenation reactor 61 and a second atmospheric distillation tower 62; mixing the dry distillation crude oil with solvent distillate oil, then, firstly, feeding the mixture into a solvent hydrogenation reactor 61 for partial hydrogenation saturation to obtain hydrogenation mixed oil, feeding the hydrogenation mixed oil into a second atmospheric distillation tower 62 for distillation, obtaining a light oil product with the boiling point less than 180-200 ℃ at the top of the tower, wherein the bottom product is solvent oil, and returning the solvent oil to a coal slurry preparation device 1 for preparing coal slurry; the solvent hydrogenation reactor 61 is a fixed bed reactor, and the operation conditions are as follows: 330-390 ℃, airspeed of 1.0-1.5/h, hydrogen-oil ratio of 600-1000:1 and pressure of 9-12MPa; the catalyst used in the solvent hydrogenation reactor 61 is a catalyst disclosed in the application patent CN101370914a filed by the inventor in 2009 and named as a hydrogenation method of lignite liquefaction cycle solvent.
Example 1:
In the embodiment, lignite in Shenhua victory coal field is used as a raw material, and the raw material lignite is dried, crushed and sieved to prepare coal dust, wherein the coal dust has the following properties: moisture 4.67% (air dried basis), ash 9.64% (air dried basis), volatiles 42.36% (anhydrous ash free basis).
The operating parameters of each step in this embodiment are as follows:
preparing coal oil slurry: the weight ratio of the solvent oil to the pulverized coal is 1.8:1, and the adding amount of the catalyst is 0.5% of the amount of the pulverized coal; in this example, 96.34kg of hydrogenated solvent oil, 53.52kg of pulverized coal and 0.27kg of catalyst powder were taken and prepared into coal oil slurry in a coal slurry preparation apparatus 1.
Pyrolysis hydrogenation of coal oil slurry: the operation condition of the pyrolysis hydrogenation reactor 2 is 8MPa, 420+/-5 ℃, the volume ratio of hydrogen to coal oil slurry is 600:1, and the residence time is 50 minutes; the pyrolysis hydrogenation of the coal oil slurry of this example was carried out on a pilot plant with a throughput of 120 kg/d.
Liquid-solid separation:
The operation temperature of the primary liquid-solid separation device 31 is 60-70 ℃, and the ratio of the cooked coal slurry to the cosolvent is 1:1; the operating pressure is 0.3MPa, and the pore diameter of the filter cloth is 300 meshes;
The operating temperature of the secondary liquid-solid separation device 32 is 60-70 ℃, and the ratio of the first solid product to the cosolvent is 1:2; the ratio of the first solid product to the cosolvent is 1:2, the operating pressure is 0.8MPa, and the pore diameter of the filter cloth is 300 meshes.
And (3) distilling and separating:
The operating conditions of the first atmospheric distillation column 41 are: the pressure at the top of the tower is 0.05-0.1MPa, and the temperature at the top of the tower is 180-220 ℃;
The operation conditions of the vacuum distillation column 42 are that the top pressure is-0.1 MPa, and the temperature of the column bottom is 330-360 ℃.
Rotary dry distillation: the operation conditions are as follows: operating at 500-550 ℃ under micro negative pressure;
Solvent oil preparation:
The solvent hydrogenation reactor 61 is a fixed bed reactor, and the operation conditions are as follows: 330-340 ℃, 1.0-1.2/h airspeed, 600-700:1 hydrogen-oil ratio and 9-10MPa pressure;
The operating conditions of the second atmospheric distillation column 62 are: the pressure at the top of the tower is 0.05-0.08MPa, and the temperature at the top of the tower is 180-210 ℃.
The yield of the coal-based asphalt of this example was 32.78% (anhydrous ashless basis), and the yield of the light oil was 27.56% (anhydrous ashless basis).
In the embodiment, the second solid product is analyzed, wherein the oil content is 55.93%, the asphalt content is 7.54%, and the residual asphalt content in the second solid product is lower through liquid-solid separation.
Example 2:
In this example, the operating temperature of the pyrolysis hydrogenation reactor 2 was adjusted to 410.+ -. 5 ℃ using the victory lignite used in example 1, and the other conditions were carried out in accordance with example 1. The yield of the coal-based asphalt of this example was 32.62% (anhydrous ashless basis), and the yield of the light oil was 22.57% (anhydrous ashless basis).
Example 3:
this example was continued using the victory lignite used in example 1, and the operation temperature of the pyrolysis hydrogenation reactor 2 was adjusted to 400.+ -. 5 ℃ and the other conditions were carried out in accordance with example 1. The yield of the coal-based asphalt of this example was 31.09% (anhydrous ashless basis), and the yield of the light oil was 17.07% (anhydrous ashless basis).
Example 4:
this example was continued using the victory lignite used in example 1, and the operation temperature of the pyrolysis hydrogenation reactor 2 was adjusted to 390.+ -. 5 ℃ and the other conditions were carried out in accordance with example 1. The yield of the coal-based asphalt of this example was 28.40% (anhydrous ashless basis), and the yield of the light oil was 7.71% (anhydrous ashless basis).
Examples 1-4 are the effects of different reaction temperatures on product yields, with the test conditions and test results shown in Table 1.
TABLE 1 comparison of temperature Condition implementation effects
| Examples | Coal type | Ratio of agent to coal | Temperature (DEG C) | Pressure MPa | Light oil yield% | Coal-based bitumen yield% |
| 1 | Lignite coal | 1.8:1 | 420 | 8 | 27.56％ | 32.78％ |
| 2 | Lignite coal | 1.8:1 | 410 | 8 | 22.57％ | 31.62％ |
| 3 | Lignite coal | 1.8:1 | 400 | 8 | 17.07％ | 31.09％ |
| 4 | Lignite coal | 1.8:1 | 390 | 8 | 7.71％ | 28.40％ |
As can be seen from Table 1, as the reaction temperature increases, the coal cracking depth increases, and the yields of light oil and coal-based pitch increase. In order to obtain a higher yield of coal-based asphalt products and a higher yield of light oil at the same time, the optimal reaction temperature of 420 ℃ can be optimized; if only for obtaining coal-based bitumen products, other reaction temperatures such as: 390 ℃, 400 ℃, 410 ℃.
Example 5:
In this example, the victory brown coal used in example 1 was continuously used, and the weight ratio of the solvent oil to the raw pulverized coal was adjusted to 1.6:1, the remaining conditions were as in example 1. The yield of the coal-based asphalt of this example was 30.65% (anhydrous ashless basis), and the yield of the light oil was 23.38% (anhydrous ashless basis).
Example 6:
in this example, the victory brown coal used in example 1 was continuously used, and the weight ratio of the solvent oil to the raw pulverized coal was adjusted to 1.4:1, the remaining conditions were as in example 1. The yield of the coal-based asphalt of this example was 28.37% (anhydrous ashless basis), and the yield of the light oil was 18.92% (anhydrous ashless basis).
Examples 1, 5 and 6 show the influence of different coal ratios (weight ratio of solvent oil to coal dust) on test results, and the test conditions and results of examples 1, 5 and 6 are shown in table 2.
Table 2, comparative table of the effect of the implementation of the ratio of the agent to the coal
| Examples | Coal type | Ratio of agent to coal | Temperature (DEG C) | Pressure MPa | Light oil yield% | Coal-based bitumen yield% |
| 1 | Lignite coal | 1.8:1 | 420 | 8 | 27.56％ | 32.78％ |
| 5 | Lignite coal | 1.6:1 | 420 | 8 | 23.38％ | 30.65％ |
| 6 | Lignite coal | 1.4:1 | 420 | 8 | 18.92％ | 28.37％ |
As can be seen from Table 2, the yields of coal-based asphalt and light oil are significantly reduced with the reduction of the agent-coal ratio, which indicates that the solvent oil of the present invention has higher hydrogen supply capacity, and in order to obtain more target product-coal-based asphalt, the agent-coal ratio is preferably 1.8:1. Other agent-coal ratios can be selected as the optimal agent-coal ratio under the condition of comprehensively considering economic benefits.
Example 7:
This example was continued using the victory brown coal used in example 1, and the operation pressure of the pyrolysis hydrogenation reactor 2 was adjusted to 6MPa, and the other conditions were carried out in accordance with example 1. The yield of the coal-based asphalt of this example was 30.97% (anhydrous ashless basis), and the yield of the light oil was 23.39% (anhydrous ashless basis).
Example 8:
This example was continued using the victory brown coal used in example 1, and the operation pressure of the pyrolysis hydrogenation reactor 2 was adjusted to 7MPa, and the other conditions were carried out in accordance with example 1. The yield of the coal-based asphalt of this example was 31.52% (anhydrous ashless basis), and the light oil yield was 25.37% (anhydrous ashless basis).
The effects of different pressures on test results are shown in examples 1, 7 and 8, and the test conditions and results of examples 1, 7 and 8 are shown in Table 3.
TABLE 3 comparison of the effects of different reaction pressures
As can be seen from Table 3, the increase in pressure is advantageous for the increase in yield of light oil and coal-based asphalt, but if the pressure is too high, the investment cost for equipment and the operation cost are greatly increased, so that the reaction pressure of the present invention is preferably 8MPa; other pressures may also be selected as the optimal operating pressures with a combination of economic considerations.
Example 9:
In the embodiment, long flame coal in the Erdos area is used as a raw material, and the properties of the coal powder prepared by drying the long flame coal are as follows: moisture 3.98% (air dried basis), ash 10.57% ((air dried basis)), volatiles 34.10% (anhydrous ash free basis); the process conditions used in this example were the same as in example 1. The yield of the coal-based asphalt of this example was 30.76% (anhydrous ashless basis), and the yield of the light oil was 11.92% (anhydrous ashless basis).
Example 10:
In the embodiment, the air coal in northeast is used as the raw material, and the coal powder prepared by drying the air coal has the following properties: moisture 3.84% (air dried basis), ash 8.85% (air dried basis), volatiles 46.44% (anhydrous ash free basis); the process conditions used in this example were the same as in example 1. The yield of the coal-based asphalt of this example was 39.41% (anhydrous ashless basis), and the yield of the light oil was 34.18% (anhydrous ashless basis).
Example 11:
In the embodiment, 1/3 coking coal is used as a raw material, and the coal powder prepared by drying the 1/3 coking coal has the following properties: moisture 3.68% (air dried basis), ash 11.76% (air dried basis), volatiles 35.29% (anhydrous ashless basis); the process conditions used in this example were the same as in example 1. The yield of the coal-based asphalt of this example was 45.72% (anhydrous ashless basis), and the yield of the light oil was 15.40% (anhydrous ashless basis).
The influence of different coal types on the test results is shown in examples 1, 9, 10 and 11, and the test conditions and results of examples 1, 9, 10 and 11 are shown in table 4.
Table 4, comparison Table of the implementation effects of different coal types
| Examples | Coal type | Ratio of agent to coal | Temperature (DEG C) | Pressure MPa | Light oil yield% | Coal-based bitumen yield% |
| 1 | Lignite coal | 1.8:1 | 420 | 8 | 27.56％ | 32.78％ |
| 9 | Long flame coal | 1.8:1 | 420 | 8 | 11.92％ | 30.76％ |
| 10 | Gas coal | 1.8:1 | 420 | 8 | 34.18％ | 39.41％ |
| 11 | 1/3 Coking coal | 1.8:1 | 420 | 8 | 15.40％ | 45.72％ |
As can be seen from table 4, the present invention can obtain coal-based asphalt yields of 30% or more for a plurality of coal types; in the existing coal tar pitch preparation process, the yield of coal-based pitch relative to raw material coal is only 2% -6%; therefore, the yield of the coal-based asphalt is far higher than that of the prior art, the applicability of coal types is wide, and the coal-based asphalt can be popularized in a plurality of coal producing areas.
The coal-based pitches obtained in example 1, example 9, and example 10 (sample 1, test 9, and test 10) and the coal tar pitch in the elm zone were subjected to ash, quinoline insolubles, and elemental analysis, respectively, and the analysis results are shown in table 5. Analysis results show that compared with coal tar pitch, the pitch raw material prepared by the process of the invention has quinoline insoluble content and ash content of about 0.1 percent; the quinoline insoluble content in the coal tar pitch is 10.73% and the ash content is 0.28%, so that the quality of the coal-based pitch prepared by the method is far higher than that of the existing coal tar pitch, and the index of quinoline insoluble matters is lower than that of the coal tar pitch by two orders of magnitude. This is because in the course of coal tar production, pitch produced by coal pyrolysis and asphaltene are mutually polycondensed into high polycondensation organic matters, so that quinoline insoluble matters in the pitch product are very high; the process can effectively avoid the secondary polycondensation of asphalt and asphaltene, so that the high polycondensation organic matters in the product are very few, and further, the quinoline insoluble matters in the asphalt product are very low. Elemental analysis also shows that compared with coal tar pitch, the coal-based pitch obtained by the invention has obviously improved hydrogen content, relatively higher H/C atomic ratio and relatively lower S, N, O content; because the coal-based asphalt product has the characteristics, the coal-based asphalt product can be directly used for preparing high-grade carbon materials such as needle coke, mesophase asphalt, super activated carbon, porous carbon and the like without pretreatment, and the economic value of the coal-based asphalt product is far higher than that of the existing coal tar asphalt product.
The inventor finds that the reaction activity is better when the coal-based asphalt product is used for producing the mesophase asphalt, and compared with coal tar asphalt, the polycondensation temperature of the mesophase asphalt can be reduced by about 10 ℃ and the polycondensation time can be reduced by 30-40 minutes.
TABLE 5 comparison of asphalt analysis for different coal bases
| Asphalt type | C％ | H％ | O％ | N％ | S％ | Softening point of | Ash content | Quinoline insolubles |
| Sample 1 | 90.6 | 5.9 | 1.9 | 1.4 | 0.2 | 105℃ | 0.06％ | 0.08％ |
| Sample 9 | 90.5 | 5.7 | 2.1 | 1.3 | 0.4 | 117℃ | 0.10％ | 0.13％ |
| Sample 10 | 90.6 | 5.8 | 1.8 | 1.5 | 0.3 | 115℃ | 0.09％ | 0.12％ |
| Coal tar pitch | 90.9 | 4.2 | 2.8 | 1.6 | 0.5 | 93℃ | 0.28％ | 10.73％ |
In summary, compared with the existing coal tar pitch production technology, the invention can obtain higher high-quality coal-based pitch yield at lower temperature and pressure, thereby greatly increasing the yield of the high-quality coal-based pitch, solving the technical problem of insufficient raw materials of the current high-quality carbon materials, and having outstanding substantive characteristics and remarkable progress.
Claims (10)
1. A method for preparing high-quality carbon material raw materials by using coal comprises the following steps of: preparing coal oil slurry, carrying out pyrolysis hydrogenation and separating products; the coal slurry is subjected to pyrolysis hydrogenation to obtain the needed cooked coal slurry, and the cooked coal slurry is subjected to product separation to obtain a coal-based asphalt product serving as a high-quality carbon material raw material; the method is characterized in that: the weight ratio of the pulverized coal to the solvent oil in the coal oil slurry to the catalyst is 1:1.4-2:0.001-0.03; the catalyst is pyrite powder with granularity less than 200; the operation conditions of pyrolysis hydrogenation are as follows: the pressure is 4-8MPa, the temperature is 390-440 ℃, the residence time is 30-90 minutes, and the volume ratio of hydrogen to coal oil slurry is 300-600:1.
2. The method for preparing high-quality carbon material raw materials by coal according to claim 1, wherein the method comprises the following steps: the product separation comprises liquid-solid separation, wherein the liquid-solid separation is pressurized hot filtration separation, and the liquid-solid separation comprises primary liquid-solid separation and secondary liquid-solid separation; firstly, mixing the cooked coal slurry with a cosolvent to perform primary liquid-solid separation to obtain a first liquid product and a first solid product, and then mixing the first solid product with the cosolvent to perform secondary liquid-solid separation to obtain a second liquid product and a second solid product; mixing the first liquid product with the second liquid product to produce a mixed liquid product; the cosolvent is light coal tar with a distillation range of less than 200 ℃.
3. The method for preparing high-quality carbon material raw materials by coal according to claim 2, wherein the method comprises the following steps: the weight ratio of the cooked coal slurry to the cosolvent is 0.5-2:1, and the operation temperature of the primary liquid-solid separation is as follows: the pore diameter of the filter cloth is 200-800 meshes at 60-120 ℃ and the pressure is 0.1-0.8MPa.
4. The method for preparing high-quality carbon material raw materials by coal according to claim 2, wherein the method comprises the following steps: the weight ratio of the first solid product to the cosolvent is 1:1.5-3, the operation temperature of the secondary liquid-solid separation is as follows: the temperature is 60-120 ℃, the pore diameter of the filter cloth is 200-800 meshes, and the pressure is 0.5-0.8MPa.
5. The method for preparing high-quality carbon material raw materials by coal according to claim 2, wherein the method comprises the following steps: the product separation also includes distillation separation; the distillation separation comprises first normal pressure distillation separation and reduced pressure distillation separation; the mixed liquid product is subjected to first normal pressure distillation and separation to obtain recovered cosolvent and heavy components; and then carrying out reduced pressure distillation separation on the heavy components to obtain solvent distillate oil and coal-based asphalt products.
6. The method for preparing high-quality carbon material raw materials by using coal according to claim 5, wherein the method comprises the following steps: the first atmospheric distillation separation operating conditions are: the pressure at the top of the tower is 0.05 to 0.1MPa, and the temperature at the top of the tower is 180-220 ℃.
7. The method for preparing high-quality carbon material raw materials by using coal according to claim 5, wherein the method comprises the following steps: the operation conditions of the reduced pressure distillation separation are as follows: the pressure at the top of the tower is-0.05 to-0.1 MPa, and the temperature at the bottom of the tower is 330-360 ℃.
8. The method for preparing high-quality carbon material raw materials by using coal according to claim 5, wherein the method comprises the following steps: the method also comprises the steps of low-temperature carbonization: carrying out low-temperature carbonization on the second solid product to obtain carbonized crude oil and semicoke products; the operation temperature of the low-temperature carbonization is 500-550 ℃.
9. The method for preparing high-quality carbon material raw materials from coal according to claim 8, wherein the method comprises the following steps: the preparation method also comprises the steps of solvent oil preparation: mixing the dry distillation crude oil with solvent distillate oil, and then carrying out hydrotreatment to obtain hydrogenated mixed oil; carrying out second normal pressure distillation separation on the hydrogenated mixed oil to obtain solvent oil and light oil products; the operating conditions of the hydrotreatment are as follows: 330-390 ℃, airspeed of 1.0-1.5/h, hydrogen-oil ratio of 600-1000:1 and pressure of 9-12MPa.
10. The method for preparing high-quality carbon material raw materials by coal according to claim 1, wherein the method comprises the following steps: the granularity of the pulverized coal in the coal oil slurry is smaller than 200 meshes.
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