CN112175655A - Enhanced reaction system and method for direct coal liquefaction - Google Patents
Enhanced reaction system and method for direct coal liquefaction Download PDFInfo
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- CN112175655A CN112175655A CN201910601025.XA CN201910601025A CN112175655A CN 112175655 A CN112175655 A CN 112175655A CN 201910601025 A CN201910601025 A CN 201910601025A CN 112175655 A CN112175655 A CN 112175655A
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Classifications
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
- C10G1/06—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal by destructive hydrogenation
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/18—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles
- B01J8/20—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles with liquid as a fluidising medium
- B01J8/22—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles with liquid as a fluidising medium gas being introduced into the liquid
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
- C10G1/08—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal with moving catalysts
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G7/00—Distillation of hydrocarbon oils
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/40—Characteristics of the process deviating from typical ways of processing
- C10G2300/4006—Temperature
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/40—Characteristics of the process deviating from typical ways of processing
- C10G2300/4012—Pressure
Abstract
The invention provides a reinforced reaction system and a method for direct coal liquefaction, which comprises the following steps: the feeding unit is used for preparing coal slurry and conveying the coal slurry and hydrogen; the liquefaction reaction unit is connected with the feeding unit and is used as a place for carrying out liquefaction reaction on the coal slurry and hydrogen, and the liquefaction reaction product is separated and rectified to obtain light fraction and distillate oil; the hydrogenation reaction unit is connected with the liquefaction reaction unit and is used for carrying out catalytic hydrogenation reaction on the light fraction and the distillate oil to obtain a hydrogen-donating solvent and product oil; and the micro-interface generator is respectively arranged between the liquefaction reaction unit and the hydrogenation reaction unit. The invention provides a reinforced reaction system and a method for direct coal liquefaction, which solve the problem of low reaction efficiency in the direct coal liquefaction process in the prior art because hydrogen cannot fully react with coal slurry.
Description
Technical Field
The invention relates to the technical field of direct coal liquefaction, in particular to a system and a method for a reinforced reaction of direct coal liquefaction.
Background
The direct coal liquefaction technology is a technological process for directly converting coal into a liquid product and a small amount of gas product through hydrogenation under the actions of high temperature, high pressure, hydrogen, a solvent and a catalyst. The direct coal liquefaction process typically includes four main sections: the method comprises the steps of oil coal slurry preparation, coal hydrogenation liquefaction reaction, solid-liquid separation and product quality improvement processing utilization. The coal is crushed, dried and ground into coal powder, the coal powder, a solvent and a catalyst are prepared into oil coal slurry suitable for conveying and heat transfer, the oil coal slurry is conveyed to a coal hydrogenation liquefaction reactor after being pressurized and preheated, coal is subjected to pyrolysis and hydrogenation reaction under the conditions of high temperature and high pressure to generate a liquid product, the liquefied oil generated by the reaction is separated from asphalt substances, unreacted coal, the catalyst and ash, the solvent is recovered to obtain coal liquefied crude oil, the coal liquefied crude oil is subjected to upgrading processing to produce a target product, and gasoline, diesel oil, aviation kerosene, special oil products, chemical raw materials and the like can be produced according to different schemes of the product.
The main influences of the current coal direct liquefaction for realizing industrialization include high construction investment cost, low coal liquefaction conversion rate and low oil yield, wherein the low oil yield is the most critical factor, and directly influences the economic benefit and market competitiveness of a coal direct liquefaction device. Because the coal direct liquefaction process conditions are relatively harsh, the coal liquefaction reaction temperature is high, the coal direct liquefaction reaction process mainly comprises pyrolysis and hydrogenation, secondary cracking of a target product cannot be avoided, the yield of the target product oil is reduced, the yield of byproduct gas is high, hydrogen consumption is increased, and the cost is increased; in addition, in the coal liquefaction reaction process, active components of coal are firstly converted, components which are difficult to convert need harsher conditions, while the direct coal liquefaction reaction process is a parallel-series reaction system, which also causes that in a second reactor or the latter half of the reaction, the hydrogen supply capacity of a circulating solvent is reduced, the hydrogen partial pressure is reduced, and the reaction severity is reduced on the contrary, which is not beneficial to improving the coal liquefaction conversion rate and the oil yield. At present, in most of direct coal liquefaction reaction processes, the direct coal liquefaction reaction process is a parallel series reaction system, so that the similar problems are all solved.
Disclosure of Invention
In view of the above, the invention provides a system and a method for a reinforced reaction of direct coal liquefaction, and aims to solve the problem that the reaction efficiency of coal liquefaction is reduced because hydrogen cannot fully react with coal slurry in the direct coal liquefaction process of the conventional emulsion bed reactor.
In one aspect, the present invention provides an enhanced reaction system for direct coal liquefaction, comprising:
the feeding unit is used for preparing coal slurry and conveying the coal slurry and hydrogen;
the liquefaction reaction unit is connected with the feeding unit, converts the pressure energy of gas into the surface energy of hydrogen bubbles, enables the hydrogen bubbles to be broken into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm so as to increase the mass transfer area between the hydrogen and the coal slurry in the liquefaction reaction process, reduce the thickness of a liquid film and reduce the mass transfer resistance, is used as a place for the liquefaction reaction of the coal slurry and the hydrogen so as to enable the micron-sized bubbles to be blended into the coal slurry to form an emulsification system, and simultaneously separates and rectifies the liquefaction reaction products so as to obtain light fractions and distillate oil;
and the hydrogenation reaction unit is connected with the liquefaction reaction unit and is used for converting the pressure energy of the gas and/or the kinetic energy of the liquid in the mixed system of the light fraction, the distillate oil and the hydrogen into the surface of hydrogen bubbles so as to break the hydrogen into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm, so that the mass transfer area between the hydrogen and reactants in the mixed system in the catalytic hydrogenation process is increased, the thickness of a liquid film is reduced, the mass transfer resistance is reduced, and the micron-sized bubbles are used as the site of the hydrogenation reaction to perform catalytic hydrogenation on the light fraction and the distillate oil so as to obtain a hydrogen-supplying solvent and product oil.
Further, in the intensified reaction system for direct coal liquefaction, the liquefaction reaction unit includes: the system comprises a first micro-interface generator, a first reactor, a separator and a rectifying tower; wherein the content of the first and second substances,
the first micro-interface generator is arranged in the first reactor and used for converting the pressure energy of gas into the surface energy of hydrogen bubbles so that the hydrogen bubbles are broken into micron-sized bubbles, so that the mass transfer area between the hydrogen and the coal slurry in the liquefaction reaction process is increased, the thickness of a liquid film is reduced, and the mass transfer resistance is reduced;
the first reactor is connected with the feeding unit and is used as a place for carrying out liquefaction reaction on the coal slurry and the hydrogen so as to enable the micron-sized bubbles to be blended into the coal slurry to form an emulsifying system and carry out liquefaction reaction;
the separator is connected with the first reactor and is used for separating the products of the liquefaction reaction;
and the rectification liquid tower is connected with the separator and is used for rectifying the liquefied product separated by the separator to obtain light fraction and distillate oil.
Further, in the enhanced reaction system for direct coal liquefaction, the first micro-interface generator is a micro-pneumatic micro-interface generator.
Further, in the enhanced reaction system for direct coal liquefaction, the first reactor is a suspended bed, a fluidized bed or a fixed bed.
Further, in the intensified reaction system for direct coal liquefaction, the hydrogenation reaction unit includes: the second micro-interface generator, the second reactor, the gas-liquid separator and the fractionating tower; wherein the content of the first and second substances,
the second micro-interface generator is arranged between the liquefaction reaction unit and the second reactor and is used for converting pressure energy of gas and/or kinetic energy of liquid in a mixed system of the light fraction, the distillate oil and the hydrogen into the surface of hydrogen bubbles so that the hydrogen breaks the micron-sized bubbles, so that the mass transfer area between the hydrogen and reactants in the mixed system in the catalytic hydrogenation process is increased, the thickness of a liquid film is reduced, and the mass transfer resistance is reduced;
the second reactor is connected with the second micro-interface generator and is used as a place for the hydrogenation reaction to carry out catalytic hydrogenation on the light fraction and the distillate oil;
the gas-liquid separator is connected with the second reactor and is used for carrying out gas-liquid separation on the product of the hydrogenation reaction;
the fractionating tower is connected with the gas-liquid separator and is used for fractionating the liquid products separated by the gas-liquid separator.
Further, in the enhanced reaction system for direct coal liquefaction, the second micro-interface generator is selected from one of a pneumatic micro-interface generator, a hydraulic micro-interface generator and a gas-liquid linkage micro-interface generator.
Further, in the enhanced reaction system for direct coal liquefaction, the second reactor is a suspended bed, a fluidized bed or a fixed bed.
Further, in the enhanced reaction system for direct coal liquefaction, the temperature of the liquefaction reaction is 460-.
The coal direct liquefaction reinforced reaction system has the beneficial effects that the micro-interface generators are respectively arranged between the liquefaction reaction unit and the hydrogenation reaction unit. The micro-interface generator is used for crushing the hydrogen into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm in the micro-interface generator before the liquefaction reaction and the catalytic hydrogenation reaction so as to increase the phase boundary mass transfer area between the hydrogen and the corresponding reactant in the reaction process, reduce the thickness of a liquid film, reduce the mass transfer resistance and improve the mass transfer efficiency between reaction phases, thereby solving the problem of low reaction efficiency in the direct coal liquefaction process due to the fact that the hydrogen cannot fully react with coal slurry in the prior art. Meanwhile, the invention can flexibly adjust the range of the preset operation condition according to different raw material compositions, different product requirements or different catalysts so as to ensure the full and effective reaction, further ensure the reaction rate and achieve the purpose of strengthening the reaction.
Particularly, the liquefaction reaction unit is provided with a high-temperature separation tower, a low-temperature separator, an atmospheric distillation tower and a reduced-pressure distillation tower, and can separate and distill the products of the liquefaction reaction to generate light fraction, distillate oil and hydrogen and simultaneously remove waste and solid residues from the system, so that the reaction efficiency of the system is improved, and the utilization efficiency of resources is increased.
On the other hand, the invention also provides a reinforced reaction method for direct coal liquefaction, which comprises the following steps:
preparing raw material coal into coal slurry, directly feeding the coal slurry into a first reactor, introducing hydrogen into a first micro-interface generator arranged in the first reactor, converting pressure energy of gas and/or kinetic energy of liquid into hydrogen bubble surface energy through the first micro-interface generator, crushing the hydrogen bubbles into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm, and conveying the micron-sized bubbles into the first reactor to perform liquefaction reaction with the coal slurry;
carrying out gas-liquid separation on a liquefied reaction product in a separator, wherein a liquid phase part forms light fraction and distillate oil through a rectifying tower, the light fraction and distillate oil mixed solution and hydrogen are sent into a second micro-interface generator together, the pressure energy of the gas and/or the kinetic energy of the liquid are/is converted into the surface energy of hydrogen bubbles through the second micro-interface generator, the hydrogen bubbles are crushed into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm, the micron-sized bubbles are fused into the light fraction and distillate oil mixed solution to form a gas-liquid emulsification system, and the gas-liquid emulsification system is sent into the second reactor to carry out catalytic hydrogenation;
and separating the catalytic hydrogenation product into product oil and a hydrogen-supplying circulating solvent by a fractionating tower.
Further, in the method for the enhanced reaction of direct coal liquefaction, the temperature of the liquefaction reaction is 460-.
Compared with the prior art, the reinforced reaction method for direct coal liquefaction has the advantages that hydrogen is crushed into micron-sized bubbles in a micron scale by the first micro-interface generator and the second micro-interface generator, so that the phase boundary mass transfer areas of gas-phase reactants and liquid-phase reactants in a liquefaction reaction unit and a hydrogenation reaction unit in the direct coal liquefaction reaction process are effectively increased, the thickness of a liquid film is reduced, the mass transfer resistance is reduced, the mass transfer efficiency between the gas phase and the liquid phase is reinforced, and the problem of low reaction efficiency in the direct coal liquefaction process due to the fact that hydrogen cannot fully react with coal slurry in the prior art is solved. Meanwhile, the invention can flexibly adjust the range of the preset operation condition according to different raw material compositions, different product requirements or different catalysts so as to ensure the full and effective reaction, further ensure the reaction rate and achieve the purpose of strengthening the reaction.
Drawings
Various other advantages and benefits will become apparent to those of ordinary skill in the art upon reading the following detailed description of the preferred embodiments. The drawings are only for purposes of illustrating the preferred embodiments and are not to be construed as limiting the invention. Also, like reference numerals are used to refer to like parts throughout the drawings. In the drawings:
fig. 1 is a schematic structural diagram of an enhanced reaction system for direct coal liquefaction according to an embodiment of the present invention.
Detailed Description
Exemplary embodiments of the present invention will be described in more detail below with reference to the accompanying drawings. While exemplary embodiments of the invention are shown in the drawings, it should be understood that the invention can be embodied in various forms and should not be limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete, and will fully convey the scope of the invention to those skilled in the art. It should be noted that the embodiments and features of the embodiments may be combined with each other without conflict. The invention will be described in detail below with reference to the accompanying figure 1 in conjunction with an embodiment.
Referring to fig. 1, an enhanced reaction system for direct coal liquefaction according to an embodiment of the present invention includes: a feeding unit 1, a liquefaction reaction unit 2 and a hydrogenation reaction unit 3; the feeding unit 1 is used for preparing coal slurry and conveying the coal slurry and hydrogen; the liquefaction reaction unit 2 is connected with the feeding unit, and converts the pressure energy of the gas into the surface energy of the hydrogen bubbles to break the hydrogen bubbles into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm so as to increase the mass transfer area between the hydrogen and the coal slurry in the liquefaction reaction process, reduce the thickness of a liquid film and reduce the mass transfer resistance, and is used as a place for the liquefaction reaction of the coal slurry and the hydrogen so as to enable the micron-sized bubbles to be blended into the coal slurry to form an emulsification system, and simultaneously, the liquefaction reaction product is separated and rectified so as to obtain light fraction and distillate oil; the hydrogenation reaction unit 3 is connected with the liquefaction reaction unit, and is used for converting pressure energy of gas and/or kinetic energy of liquid in a mixed system of the light fraction, the distillate oil and the hydrogen into the surface of hydrogen bubbles so as to break the hydrogen into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm, so as to increase the mass transfer area between the hydrogen and reactants in the mixed system in the catalytic hydrogenation process, reduce the thickness of a liquid film and reduce the mass transfer resistance, and is used as a place of the hydrogenation reaction to perform catalytic hydrogenation on the light fraction and the distillate oil to obtain a hydrogen-supplying solvent and product oil.
Specifically, the feed unit 1 includes: a hydrogen feeding pipeline 11, a coal pretreatment device 12, a catalyst preparation device 13, a coal slurry preparation device 14 and a coal slurry pump 15. One end of the hydrogen feeding pipeline 11 is externally connected with a hydrogen source, and the other end of the hydrogen feeding pipeline is respectively connected with the liquefaction reaction unit 2 and the hydrogenation reaction unit 3 for hydrogen transportation; the coal pre-processor is connected with the inlet end of the coal slurry preparation device 14 and is used for preparing raw material coal powder; the catalyst preparation device 13 is connected with the inlet end of the coal slurry preparation device 14 and is used for preparing catalyst raw materials into ultrafine-particle catalyst powder; the outlet end of the coal slurry preparation device 14 is connected with the inlet of the coal slurry pump 15 and is used for receiving the raw material coal powder and the catalyst powder, and injecting a hydrogen-supplying solvent into the coal slurry preparation device 14, and mixing the raw material coal powder, the catalyst powder and the hydrogen-supplying solvent to form coal slurry; the outlet end of the coal slurry pump 15 is connected with the liquefaction reaction unit 2, and is used for conveying the coal slurry prepared by the coal slurry preparation device 14 to the liquefaction reaction unit 2 for liquefaction reaction.
When the system is in operation, the liquefied raw coal is dried and pulverized by the coal pretreatment device 12 to produce pulverized coal of a certain particle size. The catalyst raw material is made into the catalyst of ultrafine particles by the catalyst preparation device 13. The coal powder and the catalyst are mixed with the hydrogen-donating solvent in the coal slurry preparation device 14 to prepare coal slurry, the coal slurry enters the liquefaction reaction unit 2 after being prepared, and meanwhile, the hydrogen conveying pipeline conveys the hydrogen to the liquefaction reaction unit 2.
Specifically, the liquefaction reaction unit 2 includes: a first micro-interface generator 21, a first reactor 22, a high-temperature separator 23, a low-temperature separator 24, an atmospheric distillation tower 25 and a vacuum distillation tower 26; the first micro-interface generator 21 is located inside the first reactor 22, is connected to the hydrogen feeding pipe 11, and is configured to convert pressure energy of the gas into surface energy of hydrogen bubbles, so that the hydrogen bubbles are broken into micron-sized bubbles with a diameter of 1 μm or more and less than 1mm, so as to increase a mass transfer area between the hydrogen and the coal slurry in the liquefaction reaction process, reduce a liquid film thickness, reduce mass transfer resistance, and convey the micron-sized bubbles into the first reactor 22, so as to enhance mass transfer efficiency and reaction efficiency in the liquefaction reaction process within a preset operating condition range; the inlet end of the first reactor 22 is connected with the coal slurry pump 15 and the hydrogenation reaction unit 3 respectively, the outlet end of the first reactor is connected with the inlet of the high-temperature separator 23, and the first reactor is used for receiving coal slurry and hydrogen micron-sized bubbles and serving as a reaction chamber for liquefaction reaction of the coal slurry and the hydrogen micron-sized bubbles so that the micron-sized bubbles are blended into the coal slurry to form an emulsification system and carry out liquefaction reaction; the outlet end of the high-temperature separator 23 is respectively connected with the inlet ends of the low-temperature separator 24 and the normal-pressure rectifying tower 25, and is used for carrying out gas-liquid separation on the liquefied reaction product to obtain a gas-phase product which enters the low-temperature separator 24 and a liquid-phase product which enters the normal-pressure rectifying tower 25; the outlet end of the low-temperature separation tower is respectively connected with a hydrogen feeding pipeline 11 and an atmospheric distillation tower 25, and is used for receiving the gas-phase product separated from the high-temperature separator 23 and further carrying out gas-liquid separation on the gas-phase product, the generated gas-phase product enters the hydrogen feeding pipeline 11 to be mixed with hydrogen for recycling, a waste gas part is discharged from the system, and the generated liquid-phase product enters the atmospheric distillation tower; the outlet end of the atmospheric fractionating tower is respectively connected with the second micro-interface separator and the vacuum rectification tower 26, and is used for fractionating the liquid-phase products generated by the high-temperature separator 23 and the low-temperature separator 24 to obtain light fractions, the light fractions enter the hydrogenation unit 3, and the tower bottom materials enter the vacuum rectification tower 26; the outlet end of the vacuum rectifying tower 26 is connected with the inlet end of the hydrogenation reaction unit 3, and is used for removing asphalt and solid from the tower bottom material generated by the atmospheric rectifying tower 25 to obtain distillate oil which enters the hydrogenation reaction unit 3, and a liquefied residue removal system. In this embodiment, the first micro-interface generator is a pneumatic micro-interface generator using gas as driving force; the first reactor may be any one of a suspended bed, an emulsified bed or an ebullated bed.
Hydrogen enters a first micro-interface generator 21, is crushed into micron-sized bubbles and then enters a first reactor 22, and is subjected to liquefaction reaction with coal slurry entering the first reactor 22, a liquefaction reaction product generated by the first reactor 22 enters a high-temperature separator 23 for gas-liquid separation, a gas-phase product obtained by separation of the high-temperature separator 23 enters a low-temperature separator 24 for further gas-liquid separation, the gas-phase product obtained by the low-temperature separator 24 is mixed with the hydrogen for recycling, and a waste gas part is discharged out of the system. Liquid phase products of the high-temperature separator 23 and the low-temperature separator 24 enter an atmospheric distillation tower 25 to separate light fraction, materials at the bottom of the atmospheric distillation tower 25 enter a vacuum distillation tower 26 to remove asphalt and solids, the materials at the bottom of the vacuum distillation tower 26 are liquefied residues, and the liquefied residues are discharged out of the system. In order to ensure that the residue can be removed smoothly at a certain temperature, the solids content of the residue is generally controlled to 50-55 wt.%. The light fractions and distillate oil generated by the atmospheric distillation tower 25 and the vacuum distillation tower 26 are mixed with hydrogen and enter the hydrogenation reaction unit 3.
Specifically, the hydrogenation reaction unit 3 includes: a second micro-interface generator 31, a second reactor 32, a gas-liquid separator 33, and a product fractionation column 34; the second micro-interface generator 31 is arranged between the liquefaction reaction unit and the second reactor 31, and is used for converting pressure energy of gas and/or kinetic energy of liquid in a mixed system of the light fraction, the distillate oil and the hydrogen into hydrogen bubble surface, so that the hydrogen is broken into micron-sized bubbles with the diameter of more than or equal to 1 μm and less than 1mm, the mass transfer area between the hydrogen and reactants in the mixed system in the catalytic hydrogenation process is increased, the thickness of a liquid film is reduced, and the mass transfer resistance is reduced, so that the mass transfer efficiency and the reaction efficiency in the hydrogenation reaction process are enhanced within a preset operation condition range; the inlet end of the second reactor 32 is connected with the outlet end of the second micro-interface generator 31, and the outlet end of the second reactor is connected with the inlet end of the gas-liquid separator 33, so as to receive the gas-liquid emulsion generated by the second micro-interface generator 31 and serve as a catalytic hydrogenation reaction chamber of the gas-liquid emulsion; the outlet end of the gas-liquid separator 33 is respectively connected with the product fractionating tower 34 and the hydrogen feeding pipeline 11, so that gas-liquid separation is performed on the catalytic hydrogenation product, the obtained gas-phase product and hydrogen are mixed and recycled, the waste part is removed from the system, and the obtained liquid-phase product enters the product fractionating tower 34; the product fractionating tower 34 is further connected to the first reactor 22, and is configured to fractionate the liquid-phase product produced by the gas-liquid separator 33 to obtain a product oil and a circulating solvent, and the circulating solvent is circulated to the first reactor 22 to perform a secondary liquefaction reaction. In this embodiment, the second micro-interface generator 31 is selected from one of a pneumatic micro-interface generator, a hydraulic micro-interface generator, and a gas-liquid linkage micro-interface generator, wherein the pneumatic micro-interface generator is driven by gas, and the input gas amount is much larger than the liquid amount; the hydraulic micro-interface generator is driven by liquid, and the input air quantity is generally smaller than the liquid quantity; the gas-liquid linkage type micro-interface generator is driven by gas and liquid at the same time, and the input gas amount is close to the liquid amount; the second reactor may be any one of a suspended bed, an emulsified bed or an ebullated bed.
The second micro-interface generator 31 breaks the hydrogen into micron-sized bubbles and mixes the micron-sized bubbles with the light fraction and the distillate oil to form a gas-liquid emulsion, the gas-liquid emulsion is conveyed to the inside of the second reactor 32, the second reactor 32 is subjected to catalytic hydrogenation for the purpose of improving the hydrogen supply performance of the gas-liquid emulsion, the material at the outlet of the second reactor 32 enters the gas-liquid separator 33 for gas-liquid separation, the gas-phase product generated by the gas-liquid separator 33 is mixed with the hydrogen for recycling, and the waste gas is partially discharged out of the system. The liquid phase material generated by the gas-liquid separator 33 enters a product fractionating tower 34, and the product oil and the circulating solvent are fractionated. Wherein the circulating solvent is circulated to the first reactor 22 for secondary liquefaction reaction, and the product oil is all gasoline and diesel oil fractions.
In the enhanced reaction system for direct coal liquefaction in this embodiment, the first micro-interface generator 21 is arranged inside the first reactor 22, and the second micro-interface generator 31 is arranged at the inlet end of the second reactor 32, so that hydrogen is broken into micron-sized bubbles with a diameter of micron level in the corresponding micro-interface generator before liquefaction reaction and catalytic hydrogenation reaction, the phase boundary mass transfer area between reactants such as hydrogen and coal slurry in the reaction process is effectively increased, the mass transfer efficiency between reaction phases is improved, and the problem of low reaction efficiency in the direct coal liquefaction process due to insufficient reaction of hydrogen and coal slurry in the prior art is solved.
The following describes the specific method and effect of the system according to the present invention with reference to specific embodiments.
An enhanced reaction method for direct coal liquefaction comprises the following steps:
preparing raw material coal into coal slurry, feeding the coal slurry into a first reactor, and introducing hydrogen into a first micro-interface generator at the same time;
the first micro-interface generator enables hydrogen to be crushed to form micron-sized bubbles with the diameter being more than or equal to 1 mu m and less than 1mm so as to improve the mass transfer area between the coal slurry and the hydrogen, simultaneously reduces the thickness of a liquid film and reduces the mass transfer resistance, the micron-sized bubbles are conveyed to the inside of the first reactor after being crushed and mixed with the coal slurry to form a gas-liquid emulsion, and a liquefaction reaction is carried out, so that the mass transfer efficiency and the reaction efficiency of the micron-sized bubbles in the liquefaction reaction process are enhanced within a preset operating condition range;
carrying out gas-liquid separation on the liquefied reaction product in a separator, wherein a liquid phase part forms a light fraction and a distillate oil through a rectifying tower, and the light fraction and the distillate oil are mixed and then are sent to the interior of the second micro-interface generator together with hydrogen;
the second micro-interface generator enables hydrogen to be crushed to form micron-sized bubbles with the diameter being more than or equal to 1 mu m and less than 1mm so as to improve the mass transfer area between the coal slurry and the hydrogen, simultaneously reduces the thickness of a liquid film and reduces the mass transfer resistance, and the micron-sized bubbles are conveyed into the second reactor after being crushed to be mixed with the mixture of the light fraction and the distillate oil to form a gas-liquid emulsion, and are subjected to catalytic hydrogenation reaction so as to strengthen the mass transfer efficiency and the reaction efficiency in the catalytic hydrogenation reaction process within the range of preset operating conditions;
and separating the catalytic hydrogenation product into product oil and other hydrogen-donating solvents by a fractionating tower.
In this example, the reaction temperature of the liquefaction reactionThe temperature is 400-460 ℃, the pressure is 2-14MPa, the gas-liquid ratio is 100-2000, and the space velocity is 0.7-1.2h-1。
In the embodiment, the reaction temperature of the catalytic hydrogenation reaction is 200-380 ℃, the pressure is 4-11MPa, the gas-liquid ratio is 300-800, and the space velocity is 0.6-1.8h-1。
It can be understood that the range of the preset operation conditions can be flexibly adjusted according to different raw material compositions, different product requirements or different catalysts, so as to ensure the full and effective reaction, further ensure the reaction rate and achieve the purpose of strengthening the reaction. Meanwhile, in the present embodiment, the kind of the catalyst is not particularly limited, and may be one or a combination of several of an iron-based catalyst, a molybdenum-based catalyst, a nickel-based catalyst, a cobalt-based catalyst, and a tungsten-based catalyst, as long as the strengthening reaction can be smoothly performed.
In order to further verify the processing method provided by the invention, the beneficial effects of the invention are further illustrated by combining the examples and the comparative examples.
The following is the liquefaction result of direct liquefaction of an enhanced coal under three different reaction conditions using the preferred embodiment of the present invention.
The first embodiment is as follows:
the type of reactor: a first reactor emulsifying bed and a second reactor suspending bed.
The reactor temperature: the first reactor is 400 ℃, and the second reactor is 330 ℃.
Reaction pressure: the first reactor is 2MPa, and the second reactor is 4 MPa.
Hydrogen-oil ratio: a first emulsion bed reactor 100 and a second emulsion bed reactor 250.
Coal slurry concentration: 40/50 (dry coal/solvent, mass ratio).
The addition amount of the catalyst is as follows: liquefaction catalysis aid: 1.0wt% (iron/dry coal).
The addition amount of sulfur: S/Fe =2 (molar ratio).
In this example, the conversion of coal was 80.23%, the oil yield in the product was 50.10%, and the hydrogen consumption was 9.18%.
Example two:
the type of reactor: a first reactor suspended bed and a second reactor boiling bed.
The reactor temperature: the first reactor is 430 ℃ and the second reactor is 290 ℃.
Reaction pressure: the first reactor is 8MPa, and the second reactor is 7 MPa.
Hydrogen-oil ratio: a first emulsion bed reactor 1000, a second emulsion bed reactor 500.
Coal slurry concentration: 40/50 (dry coal/solvent, mass ratio).
The addition amount of the catalyst is as follows: liquefaction catalysis aid: 1.0wt% (iron/dry coal).
The addition amount of sulfur: S/Fe =2 (molar ratio).
In this example, the conversion of coal was 82.24%, the oil yield in the product was 54.97%, and the hydrogen consumption was 8.03%.
Example three:
the type of reactor: the first reactor is a boiling bed, and the second reactor is an emulsifying bed.
The reactor temperature: 460 ℃ in the first reactor and 200 ℃ in the second reactor.
Reaction pressure: the first reactor is 14MPa, and the second reactor is 4 MPa.
Hydrogen-oil ratio: a first emulsion bed reactor 2000, a second emulsion bed reactor 700.
Coal slurry concentration: 40/50 (dry coal/solvent, mass ratio).
The addition amount of the catalyst is as follows: liquefaction catalysis aid: 1.0wt% (iron/dry coal).
The addition amount of sulfur: S/Fe =2 (molar ratio).
In this example, the conversion of coal was 87.36%, the oil yield in the product was 60.56%, and the hydrogen consumption was 7.76%.
In view of the above, the invention provides a system and a method for enhancing reaction of direct coal liquefaction, which solve the problem of low reaction efficiency in the direct coal liquefaction process in the prior art because hydrogen cannot fully react with coal slurry.
It will be apparent to those skilled in the art that various changes and modifications may be made in the present invention without departing from the spirit and scope of the invention. It is intended that the present invention cover the modifications and variations of this invention provided they come within the scope of the appended claims and their equivalents.
Claims (10)
1. An enhanced reaction system for direct coal liquefaction, comprising:
the feeding unit is used for preparing coal slurry and conveying the coal slurry and hydrogen;
the liquefaction reaction unit is connected with the feeding unit, converts the pressure energy of gas into the surface energy of hydrogen bubbles, enables the hydrogen bubbles to be broken into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm so as to increase the mass transfer area between the hydrogen and the coal slurry in the liquefaction reaction process, reduce the thickness of a liquid film and reduce the mass transfer resistance, is used as a place for the liquefaction reaction of the coal slurry and the hydrogen so as to enable the micron-sized bubbles to be blended into the coal slurry to form an emulsification system, and simultaneously separates and rectifies the liquefaction reaction products so as to obtain light fractions and distillate oil;
and the hydrogenation reaction unit is connected with the liquefaction reaction unit and is used for converting the pressure energy of the gas and/or the kinetic energy of the liquid in the mixed system of the light fraction, the distillate oil and the hydrogen into the surface of hydrogen bubbles so as to break the hydrogen into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm, so that the mass transfer area between the hydrogen and reactants in the mixed system in the catalytic hydrogenation process is increased, the thickness of a liquid film is reduced, the mass transfer resistance is reduced, and the micron-sized bubbles are used as the site of the hydrogenation reaction to perform catalytic hydrogenation on the light fraction and the distillate oil so as to obtain a hydrogen-supplying solvent and product oil.
2. The enhanced reaction system for direct coal liquefaction according to claim 1, wherein the liquefaction reaction unit comprises: the system comprises a first micro-interface generator, a first reactor, a separator and a rectifying tower; wherein the content of the first and second substances,
the first micro-interface generator is arranged in the first reactor and used for converting the pressure energy of gas into the surface energy of hydrogen bubbles so that the hydrogen bubbles are broken into micron-sized bubbles with the diameter of micron level, thereby increasing the mass transfer area between hydrogen and coal slurry in the liquefaction reaction process, reducing the thickness of a liquid film and reducing the mass transfer resistance;
the first reactor is connected with the feeding unit and is used as a place for carrying out liquefaction reaction on the coal slurry and the hydrogen so as to enable the micron-sized bubbles to be blended into the coal slurry to form an emulsifying system and carry out liquefaction reaction;
the separator is connected with the first reactor and is used for separating the products of the liquefaction reaction;
and the rectification liquid tower is connected with the separator and is used for rectifying the liquefied product separated by the separator to obtain light fraction and distillate oil.
3. The enhanced reaction system for direct coal liquefaction according to claim 2, wherein the first micro-interface generator is a micro-pneumatic micro-interface generator.
4. The enhanced reaction system for direct coal liquefaction according to claim 3, wherein the first reactor is a suspended bed, an emulsified bed or an ebullated bed.
5. The enhanced reaction system for direct coal liquefaction according to claim 1, wherein the hydrogenation reaction unit comprises: the second micro-interface generator, the second reactor, the gas-liquid separator and the fractionating tower; wherein the content of the first and second substances,
the second micro-interface generator is arranged between the liquefaction reaction unit and the second reactor and is used for converting pressure energy of gas and/or kinetic energy of liquid in a mixed system of the light fraction, the distillate oil and the hydrogen into hydrogen bubble surface so that the hydrogen is crushed into micron-sized bubbles with the diameter of micron grade, thereby increasing the mass transfer area between the hydrogen and reactants in the mixed system in the catalytic hydrogenation process, reducing the thickness of a liquid film and reducing the mass transfer resistance;
the second reactor is connected with the second micro-interface generator and is used as a place for the hydrogenation reaction to carry out catalytic hydrogenation on the light fraction and the distillate oil;
the gas-liquid separator is connected with the second reactor and is used for carrying out gas-liquid separation on the product of the hydrogenation reaction;
the fractionating tower is connected with the gas-liquid separator and is used for fractionating the liquid products separated by the gas-liquid separator.
6. The enhanced reaction system for direct coal liquefaction according to claim 4, wherein the second micro-interface generator is selected from one of a pneumatic micro-interface generator, a hydraulic micro-interface generator and a gas-liquid linkage micro-interface generator.
7. The enhanced reaction system for direct coal liquefaction according to claim 6, wherein the second reactor is a suspended bed, an emulsified bed or an ebullated bed.
8. The enhanced reaction system for direct coal liquefaction as claimed in claim 1, wherein the temperature of the liquefaction reaction is 460 ℃, the pressure is 2-14MPa, and the hydrogen-oil ratio is 100-2000, the temperature of the catalytic hydrogenation reaction is 330-380 ℃, the pressure is 4-11MPa, and the hydrogen-oil ratio is 250-700.
9. An enhanced reaction method for direct coal liquefaction is characterized by comprising the following steps:
preparing raw material coal into coal slurry, directly feeding the coal slurry into a first reactor, introducing hydrogen into a first micro-interface generator arranged in the first reactor, converting pressure energy of gas and/or kinetic energy of liquid into hydrogen bubble surface energy through the first micro-interface generator, crushing the hydrogen bubbles into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm, and conveying the micron-sized bubbles into the first reactor to perform liquefaction reaction with the coal slurry;
carrying out gas-liquid separation on a liquefied reaction product in a separator, wherein a liquid phase part forms light fraction and distillate oil through a rectifying tower, the light fraction and distillate oil mixed solution and hydrogen are sent into a second micro-interface generator together, the pressure energy of the gas and/or the kinetic energy of the liquid are/is converted into the surface energy of hydrogen bubbles through the second micro-interface generator, the hydrogen bubbles are crushed into micron-sized bubbles with the diameter of more than or equal to 1 mu m and less than 1mm, the micron-sized bubbles are fused into the light fraction and distillate oil mixed solution to form a gas-liquid emulsification system, and the gas-liquid emulsification system is sent into the second reactor to carry out catalytic hydrogenation;
and separating the catalytic hydrogenation product into product oil and a hydrogen-donating solvent through a fractionating tower.
10. The enhanced reaction method as claimed in claim 9, wherein the temperature of the liquefaction reaction is 460 ℃, the pressure is 2-14MPa, and the hydrogen-oil ratio is 100-2000, the temperature of the catalytic hydrogenation reaction is 330-380 ℃, the pressure is 4-11MPa, and the hydrogen-oil ratio is 250-700.
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