CN109401794B

CN109401794B - Staged conversion combined fluidized bed reaction device and reaction method

Info

Publication number: CN109401794B
Application number: CN201710704543.5A
Authority: CN
Inventors: 徐俊; 钟思青; 霍威; 屠功毅
Original assignee: China Petroleum and Chemical Corp; Sinopec Shanghai Research Institute of Petrochemical Technology
Current assignee: China Petroleum and Chemical Corp; Sinopec Shanghai Research Institute of Petrochemical Technology
Priority date: 2017-08-17
Filing date: 2017-08-17
Publication date: 2021-02-09
Anticipated expiration: 2037-08-17
Also published as: CN109401794A

Abstract

The invention relates to a graded conversion combined fluidized bed reaction device and a reaction method, and mainly solves the problems of low carbon conversion rate and gasification intensity, low methane yield, low treatment capacity, difficult slag discharge and low pulverized coal utilization rate in the prior art. The invention relates to a graded conversion combined fluidized bed reaction device and a reaction method, wherein a catalyst-loaded carbon-containing raw material is pyrolyzed in a pyrolysis furnace, tar gas is collected after separation, semicoke particles loaded with a catalyst after pyrolysis, a gasifying agent and an oxidizing agent are subjected to partial combustion and gasification reaction in a fine reactor, then generated synthesis gas and carbon-containing particles which are not subjected to reaction are subjected to further gasification reaction in a coarse reactor, the reacted carbon-containing particles and part of the catalyst are continuously returned to the pyrolysis furnace, and slag is discharged from bottom ash in an intermittent graded slag discharging manner.

Description

Staged conversion combined fluidized bed reaction device and reaction method

Technical Field

The invention relates to a staged conversion combined fluidized bed reaction device and a reaction method.

Background

China is a large coal country, has rich coal resources, and with the rapid development of economy in China, the production and consumption of coal are increased in sections, and the coal yield in China in 2014 reaches 38.7 hundred million tons, which is close to one half of the world yield. China has become the largest world-wide coal producing and consuming countries. A large amount of pollutants are released in the direct combustion and utilization of coal, so that the haze is frequent in many areas of China, and the environmental problem is seriously influenced.

Coal gasification is a core technology for efficient and clean utilization of coal, and is the basis for developing the process industries such as coal-based chemical production, coal-based liquid fuel, Synthetic Natural Gas (SNG), IGCC power generation, hydrogen production, industrial gas and poly-generation systems. China is the largest coal gasification technology application market in the world. At present, various coal gasification technologies have been successfully applied to industrialization, and non-catalytic gasification technologies are adopted to increase the carbon conversion rate at the cost of high temperature and high pressure, which brings about the problems of large coal gas cooling strength, difficult gas purification, high energy consumption, strict requirements on equipment and the like. However, the catalytic gasification process of coal not only increases the gasification reaction rate, but also significantly reduces the gasification reaction temperature, enabling a mild gasification process of coal. Meanwhile, a plurality of synthesis processes can be carried out, and chemical raw materials such as methane, methanol, ammonia and the like can be synthesized while gasifying coal under the action of the catalyst, so that the process flow is shortened. Wherein, the method of coal catalytic gasification is used for directly preparing the synthesis gas rich in methane, which is an important research direction of coal catalytic gasification.

In the aspect of a reactor of a coal gasification technology, the method belongs to an entrained flow gasification technology. However, the technology needs to use high-quality coal with low ash melting point (< 1350 ℃) and low ash content (< 10-15%), and the method for solving the problem of high-ash melting point coal is usually to add 10-30% of fluxing agent, so that the ash content of the fed material is higher, and the operability and the economy of the high-ash melting point coal are influenced. At the same time, the excessive operating temperatures of entrained flow slag gasification technology increase the investment, maintenance and operating costs of the entrained flow. Research reports of the American Electric Power Research Institute (EPRI) indicate that the existing industrial entrained-flow gasifier is not suitable for the gasification of high-ash and high-ash fusion-point coal, and the world needs an industrialized fluidized bed gasification technology. The fluidized bed technology has the nature of adapting to high ash melting point and high ash coal types no matter combustion or gasification, and the evidence proves that the circulating fluidized bed boiler successfully combusts coal gangue.

Patent CN201010279560.7 discloses a multilayer fluidized bed catalytic gasification methane production process, which divides a gasification furnace into a synthesis gas generation section, a coal methanation section and a synthesis gas methanation section. The combustion, gasification, methanation and pyrolysis reactions are carried out in sections, and the reaction degree and temperature distribution of each section are controlled, so that the methane yield is improved. However, in the pyrolysis section above the gasification furnace, fine pulverized coal escapes from the gasification furnace without reaction, so that the carbon content of the fly ash is high, and the unreacted coal coke is back-mixed to the slag hole at the bottom of the gasification furnace and directly discharged from the gasification furnace, so that the carbon conversion rate in the reaction process is low. When the retention time of the coke particles in the gasification furnace is 2-3 h, the carbon conversion rate is basically maintained within the range of 60-90%.

Patent CN101942344A discloses a method and device for gasification of multi-stage staged conversion fluidized bed, which comprises coal preparation, gas supply, gasification, slag discharge, and fine powder transportation, wherein the multi-stage staged conversion fluidized bed gasification device comprises a melt aggregation ash separation unit, a multi-stage staged fluidized bed pyrolysis gasification reactor, and a semicoke fine powder circulating transportation unit, and has the characteristics of high gasification furnace volume utilization rate, large treatment capacity, and high total carbon utilization rate, and is suitable for a coal staged conversion integrated system, and can be used alone to produce coal gas suitable for large-scale coal-based methane synthesis and coal chemical industry. The pyrolysis-derived tar gas is not completely utilized in the staged gasification of the technology, and the tar gas with higher added value is not more efficiently utilized in the aspect of coal quality staged utilization; on the other hand, the technology adopts the slag-removing technology to selectively separate the fused ash and then dry-remove the slag, which has a qualitative breakthrough compared with the prior art and has higher stability, but because the position and the size of the slag can not be controlled in the process of slag formation in the reactor, and simultaneously, in the slag-removing process, because of the restriction of the structure, the semicoke and the slag can not be completely separated, the slag-removing efficiency is not high, the carbon content in the slag is not low, and the total carbon conversion rate is not high.

How to realize the localization of gasification raw materials and develop a gasification furnace suitable for different coal characteristics and downstream products is crucial to the development of coal chemical industry in China. The upgrading of the existing gasification technology realizes the graded conversion of coal, and the integration and optimization of different technologies is also an important trend in the development of the coal gasification technology. Meanwhile, it is also necessary to develop a gasification technology suitable for solid substances containing carbon other than coal, including biomass, liquefied residues, petroleum residues, solid wastes containing carbon, and the like.

In summary, in the coal catalytic gasification technology, because methanation reaction needs to be considered, the reaction temperature is low, so that the reaction rate and the carbon conversion rate are reduced, the direct discharge of the coarse slag at the bottom of the gasifier greatly affects the improvement of the carbon conversion rate, in terms of the energy utilization rate, the direct combustion gasification of tar causes great waste of energy and economy, and when the carbon conversion rate is low, the heat value of the carbon residue is not fully utilized. There is a need for a staged coal conversion process that can increase carbon conversion and increase gasification intensity, methane yield, and utilization of pulverized coal.

Disclosure of Invention

The invention mainly solves the technical problems of low carbon conversion rate and gasification strength, low methane yield, low treatment capacity, low slag discharge efficiency and low pulverized coal utilization rate in the prior art, and provides a novel catalytic gasification combined fluidized bed reaction device and a reaction method. The fluidized bed reactor in the method has the characteristics of high carbon conversion rate, high gasification strength, high methane yield, large treatment capacity, controllable slag discharge, stability and high efficiency, and the gasification furnace is stable in operation, so that the high efficiency and stability of the reaction are ensured.

The second technical problem to be solved by the present invention is to provide a reaction method corresponding to the first technical problem.

In order to solve one of the above technical problems, the technical scheme adopted by the invention is as follows: a graded conversion combined fluidized bed reaction device mainly comprises: the device comprises a fine reactor 4, a coarse reactor 5, a pyrolysis furnace 6 and a graded deslagging device 2, wherein the upper end of the fine reactor 4 is expanded and then communicated with the bottom of the coarse reactor 5, the coarse reactor 5 is communicated with the pyrolysis furnace 6, and the pyrolysis furnace 6 is communicated with the fine reactor 4 through a first material returning mechanism 9.

In the technical scheme, the height of the fine reactor 4 is 2-8 times of the height of the coarse reactor 5, and the diameter of the fine reactor 4 is 1.5-6 times of the diameter of the coarse reactor 5. The grading slag discharging device 2 is composed of an upper section of slag discharging device and a lower section of slag discharging device with different cylinder diameters, and the diameter of the upper section of slag discharging device is 2-10 times that of the lower section of slag discharging device. A grading baffle 3 is arranged in the grading slag discharging device 2, and the grading baffle is a porous baffle, an inclined baffle, a grating baffle or a ring core baffle. In the above technical solution, a preferable technical solution is that the classifying baffle is a ring core baffle. In the technical scheme, the diameter of the preferable upper-section slag discharging device is 7-10 times that of the lower-section slag discharging device.

The first material returning mechanism 9 and the second material returning mechanism 8 are non-mechanical material returning mechanisms, and the non-mechanical material returning mechanisms are U valves, J valves, L valves or W valves. The preferable non-mechanical material returning mechanism type in the technical scheme is a W valve. The W valve consists of a return pipe 12, a resistance pipe 13, an inclined pipe 14 and a vertical pipe 15; the bottom of the return pipe 12 is provided with a return pipe inflation air I; the bottom 13 of the resistance tube is provided with resistance tube inflation air H; the pipe diameters of the return pipe 12, the resistance pipe 13 and the inclined pipe 14 are 0.5-1 time of the pipe diameter of the vertical pipe; the material returning angle and the resistance angle of the W valve are 45-75 degrees, and the material returning angle is larger than or equal to the resistance angle. The material return angle and the resistance angle of the W valve which are optimized in the technical scheme are 60-75 degrees, and the pipe diameters of the resistance pipe 13 and the inclined pipe 14 are 0.7-1 times of the pipe diameter of the vertical pipe. In order to solve the second problem, the invention adopts the following technical scheme: a staged conversion combined fluidized bed reaction method comprises the following steps:

a. the carbon-containing raw material E loaded with the catalyst enters a pyrolysis furnace 6 for rapid pyrolysis, pyrolysis gas and semicoke after pyrolysis are separated in the pyrolysis furnace 6 and a cyclone separator 7, and coal tar D enters subsequent equipment for purification and separation;

b. the separated semicoke respectively flows through a first material returning mechanism 8 and a second material returning mechanism 9, and simultaneously enters the fine reactor 4 with a gasifying agent F to be mixed, combusted and gasified, the large granular slag after reaction and part of carbon-containing particles which are not completely reacted enter the graded slag discharging device 2 through valve control, the large granular slag is discharged from the bottom of the graded slag discharging device 2 after particle grading, and the carbon-containing particles flow into the upper end of the fine reactor 4 through the upper part of the graded slag discharging device 2 to continuously participate in the reaction;

c. the carbon-containing particles reacted in the fine reactor 4 enter a coarse reactor 5 for further gasification reaction through gas lift; and separating, purifying and collecting the reacted raw gas G, and feeding the separated carbon-containing particles and slag serving as heat carriers into a pyrolysis furnace 6 to provide heat for pyrolysis of the catalyst-loaded carbon-containing raw material E.

In the above technical solution, the raw material containing carbon is selected from at least one of coal, petroleum coke and biomass, and the gasifying agent is selected from at least one of oxygen, air, liquid water, steam, carbon dioxide or hydrogen. The catalyst is selected from at least one of alkali metal, alkaline earth metal and transition metal; the catalyst is loaded on the carbon-containing raw material in an impregnation method, a dry mixing method or an ion exchange method; the loading capacity of the catalyst accounts for 0.1-20% of the mass of the raw coal. The reaction conditions of the fine reactor 4 are: the reaction pressure is 0-6.5 MPa, the reaction temperature is 800-1300 ℃, the gas phase line speed is 2.0-15.0 m/s, and the flow state in the fine reactor 4 is fast fluidization; the reaction conditions of the crude reactor 5 are as follows: the reaction pressure is 0-6.5 MPa, the reaction temperature is 600-1000 ℃, the gas phase line speed is 0.1-1.0 m/s, and the flow state in the coarse reactor 5 is turbulent fluidization or bubbling fluidization; the operation temperature in the pyrolysis furnace 6 is lower than the temperature in the crude reactor by 100-300 ℃; the speed of the gas phase line in the lower section of the cylinder body in the grading slag discharging device 2 is 0.8-3 m/s, and the speed of the gas phase line in the upper section of the cylinder body is 0.1-0.3 m/s; the charging pressure of the return pipe charging air I at the bottom of the return pipe 12 in the W valve and the charging pressure of the resistance pipe charging air H at the bottom 13 of the resistance pipe are less than or equal to the pressure at the bottom in the vertical pipe 15.

In the invention, the semicoke and the gasifying agent after pyrolysis enter the fine reactor 4, and the reactor mainly comprises a combustion reaction and a gasification reaction, and also comprises a partial shift reaction and a methanation reaction. The fine reactor has high linear speed, high gas-solid ratio, high water-carbon ratio and high temperature controlled in the range of 800-1300 ℃, and is favorable for combustion and gasification reaction. Under the action of catalyst, the gas-solid two-phase flow state in the reactor is fast fluidized, so that the gas content is very high and the gas-solid contact efficiency is also very high, thus leading the combustion reaction rate and the gasification reaction rate to be faster and improving the carbon conversion rate and the utilization rate of carbon residue. The heat generated by the combustion reaction is used to provide heat removal and heat rejection in the gasification reaction zone and to provide the necessary heat and gasification agents for the gasification reaction.

In the present invention, the shift reaction, methanation reaction and partial gasification reaction are mainly performed in the raw reactor 5. CO and H in the gas component flowing from the fine reactor 4₂、CO₂、H₂O and CH₄Simultaneously, circulating synthesis gas is introduced into the bottom of the crude reactor 5, and the circulating synthesis gas is gas produced by the system, passes through a purification and separation system and then passes through CO₂Absorption apparatus for removing CO₂The synthesis gas after gas improves CO and H in the crude reactor 5₂In an amount of diluting CO₂Promoting shift reaction balance to move rightwards, increasing H₂The ratio of the gas phase to the CO is low, the gas-solid flow state is bubbling or turbulent flow, the gas-solid ratio is much lower than that in the fine reactor 4, and the temperature is controlled within the range of 600 plus one of 1000 ℃, so that the shift of the methanation reaction balance is promoted, and the outlet CH is improved₄Yield.

The pyrolysis furnace 6 of the invention is a bubbling fluidized bed or a turbulent fluidized bed, the gas phase velocity in the bed is controlled at 0.1-1m/s, the heat source in the furnace is from the high-temperature solid heat carrier carbon-containing particles and ash brought from the coarse reactor 5 after gasification reaction, the temperature is controlled at 300 ℃ lower than the temperature in the coarse reactor 5 of the gasification reactor, the pyrolysis of the medium-high temperature carbon-containing raw material is carried out under the action of the catalyst, and the desired tar product and coal gas product can be obtained very easily. This part of tar is generally directly burned off in the gasification reactor in the prior art due to technical limitations; if the catalyst is not used, the particle heat of the heat carrier particles returned from the gasification furnace can not achieve the effect of high-temperature pyrolysis, and a large amount of tar is lost. In the gasification reaction taking lignite as raw material, the tar content of the lignite is notIf the tar is not extracted and is directly burnt, the economic impact is very large, so the invention extracts most of the tar as the product by firstly pyrolyzing the lignite at high temperature under the action of the catalyst. Under the action of the catalyst, the invention strengthens the pyrolysis condition that the carbon-containing raw material rapidly produces tar and coal gas and simultaneously generates semicoke under the medium-high temperature condition. The fluidized air in the bubbling fluidized bed pyrolysis furnace 6 mainly comes from CO in gasification reaction₂CO absorbed by the absorption device₂The product, the additional need for preparing CO is saved₂The cost of (2). And preferably, a bubbling fluidized bed or a turbulent fluidized bed is used as a pyrolysis device, the heat transfer efficiency is much higher than that of the traditional moving bed technology, and the agglomeration is not easy to block.

The pyrolysis furnace 6 in the present invention is preferably a new type of cyclone reactor, and like the cyclone separator, the cyclone reactor may have 1 to 4, preferably 2, inlets. The gas phase velocity at the inlet of the cyclone reactor is 15-30 m/s. The heat source in the furnace is brought by the high-temperature solid heat carrier M carbon-containing particles and ash slag from the crude reactor 5 after the gasification reaction, the temperature is controlled to be 100-300 ℃ lower than the temperature in the crude reactor 5 of the gasification reactor, and the pyrolysis of the medium-high temperature carbon-containing raw material is carried out under the action of the catalyst, so that the desired tar product and coal gas product can be obtained very easily. Under the action of the catalyst, the invention strengthens the pyrolysis condition that the carbon-containing raw material rapidly produces tar and coal gas and simultaneously generates semicoke under the medium-high temperature condition. The inlet of the cyclone reactor can be provided with an angle, so that the phenomenon that the gas enters the riser from the inlet through direct short circuit can be effectively reduced, the cyclone separation efficiency is improved, meanwhile, back mixing is avoided, the reaction sequence is carried out, the contact time is short, and the semicoke formation is facilitated to carry out the next gasification reaction.

The main reactor and the circulating system device in the invention are mature circulating fluidized bed systems, the internal temperature is easy to control, the gas-solid contact efficiency is high, and the mass transfer and heat transfer are strong. The first material returning mechanism 9 and the second material returning mechanism 8 are non-mechanical material returning mechanisms which are in the form of a U valve, a J valve, an L valve or a W valve and are not easy to leak and block. The whole structure is simple, the equipment is mature, and the abrasion and the leakage are not easy to occur.

In the invention, the first material returning mechanism 9 and the second material returning mechanism 8 are non-mechanical material returning mechanisms, and the type of the non-mechanical material returning mechanism is preferably a W valve. The particle circulation rate in the circulating fluidized bed system is a key parameter influencing the whole pulverized coal gasification throughput, and the semicoke particles passing through the material returning mechanism in unit area and unit time are directly related to the gasification strength and throughput, so that the sufficient amount of semicoke can be orderly supplemented under the pressurization condition except the amount of the gasification agent entering the reactor. The general non-mechanical valve is limited by the influence of pressure drop before and after the valve, and meanwhile, the gas is introduced too much, so that the gas is easy to be mixed with a vertical pipe and a cyclone separator at the top, and the operation threshold of the particle circulation rate is narrow. The W valve effectively improves the particle circulation rate, avoids gas reverse connection and can play a role in stabilizing high-flux circulation.

The grading deslagging device 2 has the function of discharging ash in the reactor in a controllable, orderly and high-efficiency manner. In the existing deslagging technology, because the position and the size of slagging can not be controlled in the slagging process in a reactor, and simultaneously, in the deslagging process, semicoke and ash can not be completely separated due to the restriction of a structure, the deslagging efficiency is not high, the carbon content in slag is not low, and the overall carbon conversion rate is not high. The grading slag discharging device 2 of the invention utilizes the difference of the fluidization characteristics of the carbon-containing particles and the ash slag, combines with the baffle plate and strengthens the segregation and grading of the particles. Meanwhile, the slag discharging port smoothly discharges ash slag with low carbon content by adopting a technology similar to a lock hopper according to a differential pressure principle.

CO originally present in the exhaust gas in the reaction apparatus system of the present invention₂The product is fully utilized, the energy of pyrolysis is also transferred from the gasification reaction, and the temperature of the whole system is in a lower level due to the addition of the catalyst, so that the invention is improved in the aspects of economy and safety compared with the prior art.

The reaction device and the method of the invention are not only used in the rich methane production process, but also can be used in processes of preparing fuel gas by using pulverized coal, preparing hydrogen by using pulverized coal and the like.

Compared with the prior art, the technical scheme of the invention has the characteristics of ordered slag discharge, high slag discharge efficiency, high particle circulation rate, large treatment capacity, high carbon conversion rate, high methane yield, high yield increase of tar and high pulverized coal utilization rate, reduces the carbon content in discharged ash slag by 2%, improves the particle circulation rate by 20%, ensures the high efficiency and stability of the reaction, and obtains better technical effect.

Drawings

FIG. 1 is a schematic flow diagram of the process of the present invention;

FIG. 2 is a schematic structural view of a W-valve according to the present invention;

FIG. 3 is a schematic view of the ring core baffle of the present invention;

FIG. 4 is a schematic view of the angled baffle of the present invention;

FIG. 5 is a schematic view of a grille shutter according to the present invention;

FIG. 6 is a schematic view of a large orifice baffle according to the present invention.

In FIG. 1, 1 is a lock hopper; 2 is a grading deslagging device; 3 is a grading baffle; 4 is a fine reactor; 5 is a coarse reactor; 6 is a pyrolysis furnace; 7 is a cyclone separator; 8 is a first material returning mechanism; and 9 is a second material returning mechanism. A is ash residue; b is fluidized air of the grading deslagging device; c is circulating synthesis gas; d is coal tar; e is a carbon-containing raw material of a supported catalyst; f is gasifying agent selected from oxygen, air, liquid water, water vapor, carbon dioxide or hydrogen and their mixture; g is crude gas.

The carbon-containing raw material E loaded with the catalyst enters a pyrolysis furnace 6 for rapid pyrolysis, pyrolysis gas and semicoke after pyrolysis are separated in the pyrolysis furnace 6, and coal tar D enters subsequent equipment for purification and separation; the separated semicoke respectively flows through a first material returning mechanism 8 and a second material returning mechanism 9, and simultaneously enters the fine reactor 4 with a gasifying agent F to be mixed, combusted and gasified, the large granular slag after reaction and part of carbon-containing particles which are not completely reacted enter the graded slag discharging device 3 through valve control, the large granular slag is discharged from the bottom of the graded slag discharging device 3 after particle grading, and the carbon-containing particles flow into the upper end of the fine reactor 4 through the upper part of the graded slag discharging device 3 to continuously participate in the reaction; the carbon-containing particles reacted in the fine reactor 4 enter a coarse reactor 5 for further gasification reaction through gas lift; and separating, purifying and collecting the reacted raw gas G, and feeding the separated carbon-containing particles and slag serving as heat carriers into a pyrolysis furnace 6 to provide heat for pyrolysis of the catalyst-loaded carbon-containing raw material E.

In FIG. 2, 4 is a fine reactor; 12 is a return pipe; 13 is a resistance tube; 14 is an inclined tube; and 15 is a vertical pipe. In the figure, I is the air filled in the return pipe; h is the air filled by the resistance tube. Alpha is a return angle; beta is the drag angle.

The present invention will be further illustrated by the following examples, but is not limited to these examples.

Detailed Description

[ example 1 ]

The reaction process is as follows: the catalyst and the carbonaceous raw material enter a pyrolysis furnace through a feeding pipeline for pyrolysis, tar gas is collected after separation, semicoke particles loaded with the catalyst after pyrolysis, a gasifying agent and an oxidizing agent simultaneously perform partial combustion and gasification reaction in a fine reactor at a high linear speed and a low particle concentration, large granular slag after reaction and partial incompletely reacted carbonaceous particles enter a graded slag discharging device through valve control, the large granular slag is discharged from the bottom of the graded slag discharging device after particle grading, and the carbonaceous particles flow into the upper end of the fine reactor through the upper part of the graded slag discharging device to continuously participate in the reaction. And the carbon-containing particles reacted in the fine reactor enter the coarse reactor for further gasification reaction through gas lifting. And separating, purifying and collecting the reacted raw gas, and feeding the separated carbon-containing particles and slag serving as heat carriers into a pyrolysis furnace to provide heat for pyrolysis of the catalyst-loaded carbon-containing raw material.

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. Synthesis of circulating synthesis gas volume at outlet of gasification device20% of the total gas, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 1.1 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration was 20.8%, the conversion of outlet carbon reached 97.8%, the tar content was 6.7%, and the results are detailed in table 1.

[ example 2 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 300mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. GradingThe carbon content in the ash slag discharged from the bottom of the slag discharging device is 0.66 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 21.3%, the conversion rate of outlet carbon reaches 98.2%, and the tar content is 6.5%.

[ example 3 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 150mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.65 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 21 percent, the tar content is 6.5 percent, and the conversion rate of outlet carbon reaches 98.1 percent.

[ example 4 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the crude reactor had a diameter of 75mm and a height of 375 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 1.3 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 20.1 percent, the tar content is 6.6 percent, and the conversion rate of outlet carbon reaches 97.3 percent.

[ example 5 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1000 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.98 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 20.2 percent, the tar content is 6.6 percent, and the conversion rate of outlet carbon reaches 97.8 percent.

[ example 6 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height of the fine reactor is 3000mm, the linear speed is 15m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 1.2 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 23.4%, the conversion rate of outlet carbon reaches 97.6%, and the tar content is 6.3%.

[ example 7 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 7m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.6 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 22.5%, the conversion rate of outlet carbon reaches 98.5%, and the tar content is 6.6%.

[ example 8 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, and the reaction is carried outThe reaction temperature is 800 ℃, and the reaction pressure is 0.1 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 2.8 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 18.9%, the conversion rate of outlet carbon reaches 96.1%, and the tar content is 6.7%.

[ example 9 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 6.5 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. Pyrolysis furnace separationThe bubbling fluidized bed was selected, and the reaction temperature was 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 0.32 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration was 22.2%, the outlet carbon conversion reached 98.6%, the tar content 6.5%, and the results are detailed in table 2.

[ example 10 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 1500 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 0.14 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 28.9%, the conversion rate of outlet carbon reaches 99%, and the tar content is 6.3%.

[ example 11 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 4.5. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 3.8 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 27.7%, the conversion rate of outlet carbon reaches 95.1%, and the tar content is 6.8%.

[ example 12 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 2. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 2.5 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 24.2%, the conversion rate of outlet carbon reaches 96.5%, and the tar content is 6.6%.

[ example 13 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 700 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 0.71 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 21.1%, the conversion rate of outlet carbon reaches 98.1%, and the tar content is 6.3%.

[ example 14 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 500 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 1.2 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 20.3%, the conversion rate of outlet carbon reaches 97.6%, and the tar content is 6.6%.

[ example 15 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 10% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 0.37 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 19.9%, the conversion rate of outlet carbon reaches 98.5%, and the tar content is 6.6%.

[ example 16 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the diameter of the coarse reactor is 75mm, and the height of the coarse reactor isIs 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 45% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a bubbling fluidized bed, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 3.4 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 24.2%, the conversion rate of outlet carbon reaches 95.4%, and the tar content is 6.7%.

[ example 17 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, the reaction temperature is 600 DEG C. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 0.53 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration was 21.8%, the outlet carbon conversion reached 98.3%, the tar content was 6.8%, and the results are detailed in table 3.

[ example 18 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a grid baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.7 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 21.7%, the conversion rate of outlet carbon reaches 98.2%, and the tar content is 6.8%.

[ example 19 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and an inclined baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.65 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 21.7%, the conversion rate of outlet carbon reaches 98.2%, and the tar content is 6.8%.

[ example 20 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in ash slag discharged from the bottom of the grading slag discharging device is 0.91 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 21.8%, the conversion rate of outlet carbon reaches 97.9%, and the tar content is 6.5%.

[ example 21 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 2, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.8 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 21.8%, the conversion rate of outlet carbon reaches 98%, and the tar content is 6.8%.

[ example 22 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 10, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 0.55 percent, and the particle circulation rate is 32kg/m²S, outlet CH₄The concentration is 21.8%, the conversion rate of outlet carbon reaches 98.3%, and the tar content is 6.8%.

[ example 23 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a W valve, the ratio of the pipe diameters of a material returning pipe, a resistance pipe and an inclined pipe of the W valve to the pipe diameter of a vertical pipe is 1, the angle between the material returning angle and the resistance angle is 60 degrees, and the ratio of the inflation pressure of the inflation air of the material returning pipe and the resistance pipe to the pressure of the inner bottom of the vertical pipe is less than 1. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 0.55 percent, and the particle circulation rate is 39kg/m²S, outlet CH₄The concentration was 22.6%, the outlet carbon conversion reached 98.7%, the tar content was 7%, and the results are detailed in table 4.

[ example 24 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a W valve, the ratio of the pipe diameters of a material returning pipe, a resistance pipe and an inclined pipe of the W valve to the pipe diameter of a vertical pipe is 0.7, the angle between a material returning angle and the resistance angle is 60 degrees, and the ratio of the inflation pressure of the inflation air of the material returning pipe and the resistance pipe to the pressure of the inner bottom of the vertical pipe is less than 1. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.55 percent, and the particle circulation rate is 38kg/m²S, outlet CH₄The concentration is 22.4%, the conversion rate of outlet carbon reaches 98.6%, and the tar content is 7%.

[ example 25 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a W valve, the ratio of the pipe diameters of a material returning pipe, a resistance pipe and an inclined pipe of the W valve to the pipe diameter of a vertical pipe is 0.5, the angle between a material returning angle and the resistance angle is 60 degrees, and the ratio of the inflation pressure of the inflation air of the material returning pipe and the resistance pipe to the pressure of the inner bottom of the vertical pipe is less than 1. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 0.55 percent, and the particle circulation rate is 36kg/m²S, outlet CH₄The concentration is 22.3%, the conversion rate of outlet carbon reaches 98.5%, and the tar content is 7%.

[ example 26 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a W valve, the ratio of the pipe diameters of a material returning pipe, a resistance pipe and an inclined pipe of the W valve to the pipe diameter of a vertical pipe is 1, the angle between the material returning angle and the resistance angle is 75 degrees, and the ratio of the inflation pressure of the inflation air of the material returning pipe and the resistance pipe to the pressure of the inner bottom of the vertical pipe is less than 1. The carbon content in the ash slag discharged from the bottom of the grading and deslagging device is 0.55 percent, and the particle circulation rate is 36kg/m²S, outlet CH₄The concentration is 22.3%, the conversion rate of outlet carbon reaches 98.5%, and the tar content is 7%.

[ example 27 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a W valve, the ratio of the pipe diameters of a material returning pipe, a resistance pipe and an inclined pipe of the W valve to the pipe diameter of a vertical pipe is 1, the angle between the material returning angle and the resistance angle is 45 degrees, and the ratio of the inflation pressure of the inflation air of the material returning pipe and the resistance pipe to the pressure of the inner bottom of the vertical pipe is less than 1. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.55 percent, and the particle circulation rate is 35kg/m²S, outlet CH₄The concentration is 22.1%, the conversion rate of outlet carbon reaches 98.5%, and the tar content is 7%.

[ example 28 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a W valve, the ratio of the pipe diameters of a material returning pipe, a resistance pipe and an inclined pipe of the W valve to the pipe diameter of a vertical pipe is 1, the material returning angle is 60 degrees, the resistance angle is 75 degrees, and the ratio of the inflation pressure of the inflation air of the material returning pipe and the resistance pipe to the pressure of the inner bottom of the vertical pipe is less than 1. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.55 percent, and the particle circulation rate is 33kg/m²S, outlet CH₄The concentration is 21.8%, the conversion rate of outlet carbon reaches 98.3%, and the tar content is 7%.

[ example 29 ]

Experiment selectionCrushing the inner Mongolia lignite into powder with the particle size of less than 2mm to obtain the powder, and mixing the powder with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. The ratio of the diameter of the upper section to the diameter of the lower section of the grading deslagging device is 7, and a ring core baffle is arranged in the grading deslagging device. The material returning mechanism adopts a W valve, the ratio of the pipe diameters of a material returning pipe, a resistance pipe and an inclined pipe of the W valve to the pipe diameter of a vertical pipe is 1, the angle between the material returning angle and the resistance angle is 60 degrees, and the ratio of the inflation pressure of the inflation air of the material returning pipe and the resistance pipe to the pressure of the inner bottom of the vertical pipe is equal to 1. The carbon content in the ash slag discharged from the bottom of the grading slag discharging device is 0.55 percent, and the particle circulation rate is 33kg/m²S, outlet CH₄The concentration is 21.9%, the conversion rate of outlet carbon reaches 98.3%, and the tar content is 7%.

[ COMPARATIVE EXAMPLE 1 ]

The reaction process is as follows: the catalyst and the carbon-containing raw material enter a pyrolysis furnace through a feeding pipeline for pyrolysis, the tar gas is collected after separation, and after pyrolysis, the semicoke particles loaded with the catalyst, the gasifying agent and the oxidant simultaneously perform partial combustion and gasification reaction in a fine reactor at a high linear speed and a low particle concentration. And the carbon-containing particles reacted in the fine reactor enter the coarse reactor for further gasification reaction through gas lifting. And separating, purifying and collecting the reacted raw gas, and feeding the separated carbon-containing particles and slag serving as heat carriers into a pyrolysis furnace to provide heat for pyrolysis of the catalyst-loaded carbon-containing raw material.

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading capacity of the catalyst accounts for 5 percent of the mass of the raw coal. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. Slag is discharged by adopting an ash fusion technology. The material returning mechanism adopts a U valve. The carbon content in the ash slag discharged from the bottom of ash fusion is 2.7 percent, and the particle circulation rate is 30kg/m²S, outlet CH₄The concentration was 20.5%, the outlet carbon conversion reached 93.2%, the tar content was 6.8%, and the results are detailed in table 5.

[ COMPARATIVE EXAMPLE 2 ]

The experiment selects inner Mongolia lignite, the inner Mongolia lignite is crushed to be less than 2mm to obtain pulverized coal, and the pulverized coal is mixed with 5% of potassium carbonate catalyst. The diameter of the fine reactor is 50mm, the height is 3000mm, the linear speed is 2m/s, the water-carbon ratio is 1mol/mol, the reaction temperature is 800 ℃, and the reaction pressure is 2 MPa; the coarse reactor had a diameter of 75mm and a height of 1500 mm. The loading of the catalyst accounts for 5% of the raw coal mass. The amount of the circulating synthesis gas accounts for 20% of the total amount of the synthesis gas at the outlet of the gasification device, and the ratio of hydrogen to carbon monoxide in the circulating synthesis gas is 1. The pyrolysis furnace selects a cyclone reactor with 1 inlet, the inlet angle is 5 degrees, and the reaction temperature is 600 ℃. Adopts a dry-type solid slag-discharging technology of a boiler to discharge slag. The material returning mechanism adopts a U valve. The carbon content in the bottom-discharged ash was 7.8%, and the particle circulation rate was 32kg/m²S, outlet CH₄The concentration is 21.1%, the conversion rate of outlet carbon reaches 89.7%, and the tar content is 6.8%.

[ COMPARATIVE EXAMPLE 3 ]

By using existing meansIn the technology, a gasification reaction device in the process of preparing the methane-rich gas by catalytic gasification of a multilayer fluidized bed selects inner Mongolia lignite with the grain diameter of less than 1mm, a catalyst of 15 percent of potassium carbonate, the operating pressure of 2.5MPa, the operating temperature of 700 ℃ and the gas phase line speed of 1.2 m/s. CO + H in outlet gas component obtained by experiment₂The content is 60.2%, the methane content is 7.9%, and the carbon conversion rate is 55%.

[ COMPARATIVE EXAMPLE 4 ]

The method adopts a Lurgi furnace in the prior art as a coal gasification reaction device in the process of preparing methane from coal, selects inner Mongolia lignite with the grain diameter smaller than 1mm, uses 15 percent of potassium carbonate as a catalyst, and has the operation pressure of 2.5MPa, the operation temperature of 700 ℃ and the gas phase line speed of 1.2 m/s. CO + H in outlet gas component obtained by experiment₂The content of 64 percent, the methane content of 14.1 percent and the carbon conversion rate of 91.7 percent.

TABLE 1

TABLE 2

TABLE 3

TABLE 4

TABLE 5

Claims

1. A graded conversion combined fluidized bed reaction device mainly comprises: the device comprises a fine reactor (4), a coarse reactor (5), a pyrolysis furnace (6) and a grading slag discharging device (2), wherein the grading slag discharging device (2) consists of an upper slag discharging device and a lower slag discharging device which have different cylinder diameters, and the diameter of the upper slag discharging device is 2-10 times that of the lower slag discharging device;

a grading baffle (3) is arranged in the grading slag discharging device (2), and the grading baffle (3) is in the form of a ring-core baffle;

the upper end of the fine reactor (4) is expanded and then communicated with the bottom of the coarse reactor (5), the coarse reactor (5) is communicated with the pyrolysis furnace (6), and the pyrolysis furnace (6) is communicated with the fine reactor (4) through a first material returning mechanism (9);

the first material returning mechanism (9) is a non-mechanical material returning mechanism, and the non-mechanical material returning mechanism is in a W valve type; the W valve consists of a material return pipe (12), a resistance pipe (13), an inclined pipe (14) and a vertical pipe (15); the bottom of the return pipe (12) is provided with a return pipe inflation air (I); the bottom of the resistance tube (13) is provided with a resistance tube inflation air (H); the pipe diameters of the return pipe (12), the resistance pipe (13) and the inclined pipe (14) are 0.5-1 time of the pipe diameter of the vertical pipe; the return angle and the resistance angle of the W valve are 45-75 degrees, and the return angle is larger than or equal to the resistance angle;

the pyrolysis furnace (6) is a cyclone reactor, 1-4 inlets of the cyclone reactor are provided, and the inlets are provided with angles.

2. The staged conversion combined fluidized bed reactor according to claim 1, wherein the height of the fine reactor (4) is 2 to 8 times the height of the coarse reactor (5), and the diameter of the coarse reactor (5) is 1.5 to 6 times the diameter of the fine reactor (4).

3. The staged conversion combined fluidized bed reactor according to claim 1, wherein the staged baffle (3) is in the form of a perforated baffle, an inclined baffle or a grid baffle.

4. A graded conversion combined fluidized bed reaction method, which adopts any one of the graded conversion combined fluidized bed reaction devices in claims 1-3, and comprises the following steps:

(a) the carbon-containing raw material (E) loaded with the catalyst enters a pyrolysis furnace (6) for rapid pyrolysis, pyrolysis gas and semicoke after pyrolysis are separated in the pyrolysis furnace (6) and a cyclone separator (7), and coal tar (D) enters subsequent equipment for purification and separation;

(b) the separated semicoke respectively flows through a first material returning mechanism (9) and a second material returning mechanism (8) and simultaneously enters a fine reactor (4) with a gasifying agent (F) for mixing, combustion and gasification reaction, the reacted large-particle slag and part of incompletely reacted carbon-containing particles enter a graded slag discharging device (2) through valve control, the large-particle slag is discharged from the bottom of the graded slag discharging device (2) after particle grading, and the carbon-containing particles flow into the upper end of the fine reactor (4) through the upper part of the graded slag discharging device (2) to continuously participate in the reaction;

(c) after reaction in the fine reactor (4), the carbon-containing particles enter a coarse reactor (5) through gas lifting for further gasification reaction; and separating, purifying and collecting the reacted raw gas (G), and feeding the separated carbon-containing particles and slag serving as heat carriers into a pyrolysis furnace (6) to provide heat for pyrolysis of the catalyst-loaded carbon-containing raw material (E).

5. The staged conversion combined fluidized bed reaction method according to claim 4, wherein the carbonaceous feedstock is selected from at least one of coal, petroleum coke, and biomass, and the gasifying agent is selected from at least one of oxygen, air, liquid water, steam, carbon dioxide, and hydrogen.

6. The staged conversion combined fluidized bed reaction method according to claim 4, wherein the catalyst is selected from at least one of alkali metals, alkaline earth metals, transition metals; the catalyst is loaded on the carbon-containing raw material in an impregnation method, a dry mixing method or an ion exchange method; the loading capacity of the catalyst accounts for 0.1-20% of the mass of the raw coal.

7. The staged conversion combined fluidized bed reaction method according to claim 4, characterized in that the reaction conditions of the fine reactor (4) are: the reaction pressure is 0-6.5 MPa, the reaction temperature is 800-1300 ℃, the gas phase line speed is 2.0-15.0 m/s, and the flow state in the fine reactor (4) is fast fluidization; the reaction conditions of the crude reactor (5) are as follows: the reaction pressure is 0-6.5 MPa, the reaction temperature is 600-1000 ℃, the gas phase line speed is 0.1-1.0 m/s, and the flow state in the coarse reactor (5) is turbulent fluidization or bubbling fluidization; the operation temperature in the pyrolysis furnace (6) is lower than the temperature in the crude reactor by 100-300 ℃; the gas phase line speed in the lower section of the cylinder body in the grading slag discharging device (2) is 0.8-3 m/s, and the gas phase line speed in the upper section of the cylinder body is 0.1-0.3 m/s; the inflation pressure of the return pipe inflation air (I) at the bottom of the return pipe (12) in the W valve and the inflation pressure of the resistance pipe inflation air (H) at the bottom of the resistance pipe (13) are less than or equal to the pressure at the bottom in the vertical pipe (15).