CN114874815A - Device and method for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues - Google Patents
Device and method for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues Download PDFInfo
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- 230000015572 biosynthetic process Effects 0.000 title claims abstract description 35
- 238000003786 synthesis reaction Methods 0.000 title claims abstract description 35
- 238000000034 method Methods 0.000 title claims abstract description 23
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- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 94
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- 238000002309 gasification Methods 0.000 claims abstract description 23
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- 229910052742 iron Inorganic materials 0.000 claims description 16
- 238000000926 separation method Methods 0.000 claims description 13
- 238000000629 steam reforming Methods 0.000 claims description 12
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 11
- 239000012752 auxiliary agent Substances 0.000 claims description 10
- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims description 6
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- 229910010413 TiO 2 Inorganic materials 0.000 claims description 6
- 239000000969 carrier Substances 0.000 claims description 6
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- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 5
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- YDZQQRWRVYGNER-UHFFFAOYSA-N iron;titanium;trihydrate Chemical compound O.O.O.[Ti].[Fe] YDZQQRWRVYGNER-UHFFFAOYSA-N 0.000 description 1
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- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/46—Gasification of granular or pulverulent flues in suspension
- C10J3/54—Gasification of granular or pulverulent fuels by the Winkler technique, i.e. by fluidisation
- C10J3/56—Apparatus; Plants
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- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
- C01B3/40—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts characterised by the catalyst
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- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
- C01B3/42—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts using moving solid particles
- C01B3/44—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts using moving solid particles using the fluidised bed technique
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- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/02—Fixed-bed gasification of lump fuel
- C10J3/20—Apparatus; Plants
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- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/58—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels combined with pre-distillation of the fuel
- C10J3/60—Processes
- C10J3/64—Processes with decomposition of the distillation products
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- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/72—Other features
- C10J3/721—Multistage gasification, e.g. plural parallel or serial gasification stages
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- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/72—Other features
- C10J3/725—Redox processes
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- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/72—Other features
- C10J3/82—Gas withdrawal means
- C10J3/84—Gas withdrawal means with means for removing dust or tar from the gas
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- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
- C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
- C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
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- C01B2203/06—Integration with other chemical processes
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- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
- C01B2203/1047—Group VIII metal catalysts
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- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0913—Carbonaceous raw material
- C10J2300/0916—Biomass
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- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0983—Additives
- C10J2300/0986—Catalysts
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- C10J2300/00—Details of gasification processes
- C10J2300/16—Integration of gasification processes with another plant or parts within the plant
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- C10J2300/00—Details of gasification processes
- C10J2300/16—Integration of gasification processes with another plant or parts within the plant
- C10J2300/1603—Integration of gasification processes with another plant or parts within the plant with gas treatment
- C10J2300/1618—Modification of synthesis gas composition, e.g. to meet some criteria
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Abstract
The invention discloses a device and a method for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues, relates to the technical field of biomass fuel gasification and waste energy utilization, and solves the technical problems of low efficiency, serious resource waste and large secondary pollution of a traditional Chinese medicine residue disposal method. The process runs in a chemical chain circular reduction-oxidation mode, the oxygen carrier is recycled, and the high-moisture biomass dregs are directly used as raw materials to fully utilize the biomass components and moisture of the raw materials. The heat value and the quality of the synthesis gas are improved, the heat efficiency of the whole reaction system is also improved, and the method has the characteristics of high efficiency, low energy consumption and no pollution.
Description
Technical Field
The application relates to the technical field of biomass fuel gasification and waste energy utilization, in particular to a device and a method for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues.
Background
Chinese medicinal material resources are mainly divided into three main categories: mineral medicine, plant medicine and animal medicine, wherein the plant traditional Chinese medicine accounts for about 85%, but in the production of traditional Chinese medicine, the effective components extracted from the plant traditional Chinese medicine account for only 5% on average, and the left traditional Chinese medicine residue after extraction contains a large amount of resource components such as lignin, cellulose, moisture and the like, which can cause great resource waste if the traditional Chinese medicine residue is discarded without any use.
In recent years, the Chinese medicine industry is developed rapidly, and the planting area and the production scale of Chinese medicines are greatly increased; meanwhile, the discharge amount of the traditional Chinese medicine residues tends to rise year by year. According to statistics, the annual discharge amount of the traditional Chinese medicine residues reaches 3000 ten thousand tons. Most of the traditional Chinese medicine dregs have extremely high initial water content, smell and easy decay and mildew, and have the risk of dregs returning to the market, the dregs need to be treated as dangerous solid waste, the treatment cost reaches 0.3 to 0.5 ten thousand yuan/ton, the cost is extremely high, and the administration enterprises cause huge economic burden. Although some traditional Chinese medicine enterprises process the traditional Chinese medicine residues to realize resource recycling, most of the traditional Chinese medicine residues are only treated as common wastes, and most of the traditional Chinese medicine residues are stacked, buried or burned, so that not only is serious resource waste caused, but also the surrounding environment is easily polluted, and the traditional Chinese medicine enterprises do not accord with the low-carbon and environment-friendly concepts advocated by the current state.
The resource utilization of the Chinese medicine residue mainly comprises three ways, including enrichment, extraction and utilization of effective components (namely, the effective components of the Chinese medicine residue are enriched and extracted through a chemical or fermentation conversion technology), ecological economic utilization (the biological organic matter components of the Chinese medicine residue are utilized to develop and produce organic fertilizer or be used for mushroom planting and the like) and high added value utilization (including diesel oil production through pyrolysis cracking, synthesis gas preparation through gasification and the like). The organic fertilizer prepared by using the Chinese medicine residues as raw materials can effectively improve the growth performance of plants. At present, the main preparation means of the traditional Chinese medicine residue organic fertilizer is a fermentation method, although the operation is simple, the fermentation period is long, a large amount of greenhouse gases such as methane, carbon dioxide and the like can be generated in the fermentation process, a large amount of waste water and waste liquid are generated, and thorough harmless treatment is difficult to realize. If the traditional Chinese medicine residues are used for planting mushrooms, the utilization rate of the traditional Chinese medicine residues can be improved, but the types of the traditional Chinese medicine residues which can be used for planting edible mushrooms are extremely limited due to the limitation of complexity of components of various traditional Chinese medicine residues. The traditional Chinese medicine residue can be used for producing fuel oil, coke and pyrolysis gas through catalytic pyrolysis. At present, due to the technical limit, the method has great environmental pollution, the fuel obtained by direct cracking has the defects of high oxygen content, low heat value and high cost of subsequent processing and upgrading, and the overall thermal efficiency is low. Aiming at the characteristics of the traditional Chinese medicine residues, a new way for realizing the resource and energy utilization of the traditional Chinese medicine residues becomes the current urgent need.
Disclosure of Invention
The application provides a device and a method for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues, and the technical purpose is to convert the traditional Chinese medicine residues into the high-quality synthesis gas and heat energy required by a traditional Chinese medicine factory on site, and realize a new way for harmless, reduced and resource comprehensive utilization of the traditional Chinese medicine residues.
The technical purpose of the application is realized by the following technical scheme:
a device for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues comprises a bubbling bed, an overflow pipe, a descending moving bed, a descending pipe, an ascending pipe, a gas-solid separation device, a biomass coke fixed bed, a high-temperature fan, a blower, an air preheater and a cyclone separator.
The descending moving bed comprises a descending moving bed upper end and a descending moving bed lower end which are connected with each other, and the descending moving bed is provided with a first input port, a second input port, a first output port and a second output port; high-water-content traditional Chinese medicine residues are input from a first input port at the upper end of the descending moving bed, a first output port of the descending moving bed is connected with an input port of the downcomer, and a second output port of the descending moving bed is connected with an input port of the biomass coke fixed bed; an output port of the biomass coke fixed bed is connected with an input port of the high-temperature fan, and an output port of the high-temperature fan is connected with a first input port of the air preheater; and a first output port of the air preheater is connected with a second input port of the bubbling bed, and a second output port of the air preheater is connected with a first input port of the ascending pipe.
The overflow pipe is arranged in the bubbling bed and is connected with a first output port of the bubbling bed, and an output port of the downcomer is connected with a first input port of the bubbling bed in the bubbling bed; and a first output port of the bubbling bed is connected with a second input port of the ascending pipe, and a second output port of the bubbling bed is connected with an input port of the cyclone separator.
The output port of the ascending pipe is connected with the input port of the gas-solid separation device, and the first output port of the gas-solid separation device is connected with the second input port of the descending moving bed.
The blower is connected with a second input port of the air preheater.
Furthermore, the diameter of the descending moving bed is larger than that of the descending pipe, so that the oxygen carrier and the traditional Chinese medicine residues are uniformly mixed, the conversion rate of the traditional Chinese medicine residues is improved, the diameter of the descending pipe is small, the pressure is balanced, oxygen carrier particles and unreacted coke can be smoothly discharged into a bubbling bed, nitrogen is prevented from being introduced, and the calorific value of synthesis gas is improved.
Furthermore, the air preheater adopts a dividing wall type gas-gas heat exchanger to recover heat of pyrolysis gas, and heats preheated air to 650-700 ℃ so as to reduce energy consumption of the system.
Furthermore, a second input port of the bubbling bed is provided with a plurality of air inlets, and the plurality of air inlets enable pyrolysis gas to be uniformly distributed in the bubbling bed so that the bed can reach above a critical fluidization speed and the steam reforming reaction is enhanced.
A method for preparing high-quality synthetic gas by gasifying high-water-content traditional Chinese medicine residues comprises the steps that the high-water-content traditional Chinese medicine residues are input from a first input port of a descending moving bed, the high-water-content traditional Chinese medicine residues are fully contacted with an oxidation state oxygen carrier and dried at the upper end of the descending moving bed, then the oxidation state oxygen carrier pyrolyzes the high-water-content traditional Chinese medicine residues at the lower end of the descending moving bed to generate coke and pyrolysis gas, and the coke enters a bubbling bed along with a reduction state oxygen carrier through a descending pipe; the pyrolysis gas at the upper end of the descending moving bed is mixed with water vapor to form high-moisture-content pyrolysis gas, the high-moisture-content pyrolysis gas is input into the biomass coke fixed bed to separate unreacted tar, is cooled by an air preheater and then enters a bubbling bed to be used as a fluidized medium and reforming gas, and carries out steam reforming reaction and coke gasification with a reduction-state oxygen carrier; the temperature in the bubbling bed is below 700 ℃, and the reduced oxygen carrier catalyzes coke gasification; and generating synthesis gas in the bubbling bed, separating fly ash by a cyclone separator, and finally generating and outputting high-quality synthesis gas.
The air preheater heats the air input by the blower to obtain preheated air, and the preheated air enters the ascending pipe; and part of the oxidation oxygen carrier after the steam reforming reaction in the bubbling bed is discharged out of the bubbling bed through an overflow pipe and enters an ascending pipe, the oxidation oxygen carrier and preheated air are subjected to strong exothermic reaction and are completely regenerated, and the regenerated oxidation state oxygen carrier is sent into a descending moving bed through a gas-solid separation device to start new circulation.
Further, the oxidation state oxygen carrier is an iron-based oxygen carrier, and the components of the iron-based oxygen carrier comprise a metal active component, an auxiliary agent and an inert carrier; the metal active component is Fe 2 O 3 35-50 wt% of the total weight; the auxiliary agent is CaO or Na 2 O, accounting for 0-25 wt% of the total weight; the inert carrier is Al 2 O 3 Or SiO 2 Or TiO 2 Or from Al 2 O 3 、SiO 2 、TiO 2 Any combination of (a) and (b).
The beneficial effect of this application lies in:
(1) the catalytic pyrolysis-gasification of the high-water-content traditional Chinese medicine residues is coupled with a chemical chain technology, and the characteristic of chemical chain transfer of lattice oxygen is utilized, so that the high-energy-consumption gas separation process in conventional solid fuel gasification is avoided, and the efficiency of a reaction system is improved;
(2) fully utilizes resource components and water in the high-water-content Chinese medicine residue, and avoids introducing N 2 The heat value and the grade of the synthesis gas are improved, the fuel conversion rate is more than 95 percent theoretically, and the cold coal gas efficiency is more than 75 percent;
(3) the method has the advantages that the cheap natural iron-based ilmenite or red mud base material is used as a circulating oxygen transfer material, so that the functions of oxygen transfer, heat transfer and catalytic gasification are realized, the tar content and pollutant emission are greatly reduced, and the operation cost is reduced;
(4) the double reactors adopt an integrated structure of multi-stage step-by-step reaction, so that the thermal conversion reaction process and the heat and mass transfer process of the medicine residue waste are highly coupled and integrated, and the continuous and large-scale production is easy to realize.
Drawings
FIG. 1 is a schematic diagram of the structure of the apparatus of the present application;
FIG. 2 is a diagram of gasified gas products of the traditional Chinese medicine residues of the iron-based oxygen carrier under the same reaction conditions;
FIG. 3 is a graph of the carbon residue rate of the gasified product of the traditional Chinese medicine residues of the iron-based oxygen carrier provided by the application under the same reaction conditions;
in the figure: 1-2: a bubbling bed; 1-3: an overflow pipe; 1-4: the upper end of the descending moving bed; 1-5: the lower end of the descending moving bed; 1-6: a down pipe; 1-7: a riser pipe; 1-8: a gas-solid separation device; 1-9: a biomass coke fixed bed; 1-10: a high temperature fan; 1-11: a blower; 1-12: an air preheater; 1-13: a cyclone separator; 1-14: preheating air; 1-15: high-temperature flue gas; 1-16: high water content herb residue; 1-17: pyrolysis gas with high moisture content; 1-18: coke; 1-19: high quality syngas; 1-1-1: an oxidized form oxygen carrier; 1-1-2: a reduced oxygen carrier; 1-1-3: partially oxidizing the oxygen carrier.
Detailed Description
The technical solution of the present application will be described in detail below with reference to the accompanying drawings.
The device for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues, namely a chemical chain system, comprises 1-2 parts of a bubbling bed, 1-4 parts of the upper end of a descending moving bed, 1-5 parts of the lower end of the descending moving bed, 1-6 parts of a downcomer, 1-7 parts of an ascending pipe, 1-8 parts of a gas-solid separation device, 1-9 parts of a biomass coke fixed bed, 1-10 parts of a high-temperature fan, 1-11 parts of a blower, 1-12 parts of an air preheater, 1-13 parts of a cyclone separator and an auxiliary pipeline. The descending moving bed, the downcomer 1-6 and the bubbling bed 1-2 are connected in series to form a fuel reactor, the oxidation state oxygen carrier 1-1-1 gasifies the high-water-content traditional Chinese medicine residues 1-16, then the gasified high-water-content traditional Chinese medicine residues enter the bubbling bed 1-2 from the descending moving bed through pressure difference, and the gasified high-water-content traditional Chinese medicine residues and the reformed gas are subjected to steam reforming in the bubbling bed 1-2 to prepare high-quality synthesis gas 1-19. And (3) allowing the partial oxidation state oxygen carrier 1-1-3 to enter the ascending pipe 1-7 for reoxidation, and repeatedly performing oxidation-reduction reaction. The specific operation mode of the chemical chain system is as follows:
mixing the high-temperature oxidation state oxygen carrier 1-1 with the high-water-content traditional Chinese medicine residues 1-16 at the upper end of the descending moving bed, dehydrating and drying the high-temperature oxidation state oxygen carrier, pyrolyzing and gasifying the dried residues in the descending process, and discharging the incompletely reacted part of the residues and the reduction state oxygen carrier 1-1-2 into the bubbling bed 1-2 through pressure difference. The pressure difference is controlled and the oxygen carrier is prevented from sintering by adjusting the feeding speed of the traditional Chinese medicine dregs. In the bubbling bed 1-2, the reduced oxygen carrier 1-1-2 catalyzes and gasifies the incompletely reacted medicine dregs, tar and biomass coke under the action of a catalytic activity center, steam reforming reaction is carried out on pyrolysis gas, the reduced oxygen carrier is partially oxidized, then the reduced oxygen carrier enters an ascending pipe 1-7 and reacts with high-temperature air to be completely oxidized, and the regenerated high-temperature oxygen carrier is subjected to new circulation, so that the recycling and the continuous gasification of the medicine dregs are realized.
The high-water-content traditional Chinese medicine residues 1-16 are directly added into the upper end 1-4 of the descending moving bed, are directly mixed with the oxygen carrier, are dried through high-efficiency contact heat transfer, and are continuously pyrolyzed and gasified at the lower end 1-5 of the descending moving bed. The pyrolysis gas at the upper end 1-4 of the descending moving bed is mixed with water vapor to form high-moisture-content pyrolysis gas, the high-moisture-content pyrolysis gas is input into a biomass coke fixed bed 1-9 to separate unreacted tar, is cooled by an air preheater 1-12 and then enters a bubbling bed 1-2 to be used as a fluidizing medium and reforming gas, and is subjected to steam reforming reaction and coke gasification with a reduced oxygen carrier 1-1-2; the temperature in the bubbling bed is 700 ℃, and the coke is gasified by the reduced oxygen carrier 1-1-2; the synthesis gas generated in the bubbling bed is separated by the cyclone separators 1-13 to be discharged out of the system, and finally the high-quality synthesis gas is output for pharmaceutical enterprises to use.
The method adopts the dividing wall type gas-gas heat exchanger as the air preheater 1-12 to recover the process heat, and uses the pyrolysis gas to heat the preheated air 1-14 to 650-700 ℃, thereby avoiding the waste of the process heat and reducing the energy consumption.
The diameter of the descending moving bed and the descending pipe 1-6 is changed, the diameter of the descending moving bed is larger, the oxygen carrier and the traditional Chinese medicine residues are uniformly mixed, efficient heat and mass transfer is guaranteed, the conversion rate of the traditional Chinese medicine residues is improved, and the diameter of the descending pipe is reduced to balance pressure, so that the oxygen carrier and the pyrolysis products of the traditional Chinese medicine residues can be smoothly discharged into the bubbling bed.
The working principle is as follows: the application provides a method for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues based on a chemical chain mode, an iron-based oxygen carrier has the functions of heat transfer, oxygen transfer and catalytic activity centers, the rapid dehydration and gasification, tar precipitation and in-situ cracking and biomass coke catalytic gasification of the traditional Chinese medicine residues are sequentially realized at the side of a fuel reactor, and the high-water-content pyrolysis gas is upgraded and converted into the high-quality synthesis gas. Based on the principle, a chemical chain system is constructed and operates in a circulating oxidation-reduction mode, so that the water-containing traditional Chinese medicine residues are efficiently gasified, and the high-quality synthesis gas is prepared.
The oxygen carrier is the core of the method for preparing high-quality synthesis gas, and the iron-based oxygen carrier has good oxygen carrying capacity, heat transfer capacity, carbon deposition resistance, cyclic reaction stability and sufficient mechanical strength, and is low in price. The oxygen carrier consists of an active component, an auxiliary agent and an inert carrier; the active component is Fe 2 O 3 The catalyst is used for providing active oxygen and a catalytic active center, and the total weight ratio is 35 wt% -50 wt%. The auxiliary agent is CaO and Na 2 O, accounting for 0-25 wt% of the total weight, is used for accelerating the oxygen ion migration rate of the metal active component, improving the gasification conversion rate of the traditional Chinese medicine residue, promoting the pyrolysis of tar, promoting the water gas reaction in the steam reforming process and improving H 2 And the yield of CO is increased, and the quality of the synthesis gas is improved. The inert carrier is Al 2 O 3 、SiO 2 、TiO 2 The composite material formed by random combination is used for improving the stability and the anti-carbon deposition capability of the carrier.
Example 1:
as shown in fig. 1, the apparatus for preparing high quality synthesis gas by gasifying herb residue with high water content described in the present application is realized by a chemical chain system composed of a descending moving bed, a downcomer, a bubbling bed, an ascending tube and auxiliary devices thereof connected in series, and the system comprises: 1-2 parts of bubbling bed, 1-3 parts of overflow pipe, 1-4 parts of upper end of descending moving bed, 1-5 parts of lower end of descending moving bed, 1-6 parts of downcomer, 1-7 parts of riser, 1-8 parts of gas-solid separation device, 1-9 parts of biomass coke fixed bed, 1-10 parts of high-temperature fan, 1-11 parts of blower, 1-12 parts of air preheater, 1-13 parts of cyclone separator and auxiliary pipeline.
The descending moving beds (1-4 and 1-5) and the descending pipes 1-6 are connected with the bubbling bed 1-1 in series to realize the rapid dehydration of the traditional Chinese medicine residues, the separation and in-situ cracking of tar, the catalytic gasification of biomass coke and the quality improvement of synthesis gas in sequence at the side of the fuel reactor.
The diameter of the descending moving bed is larger, the high-temperature oxidation state oxygen carrier 1-1-1 is uniformly mixed with the high-water-content traditional Chinese medicine residue 1-16, and high-efficiency heat transfer and mass transfer are achieved. The diameter of the downcomer 1-6 is relatively small, so that the pressure is balanced, and part of the un-gasified traditional Chinese medicine residues and the oxygen carrier are sent into the bubbling bed, so that nitrogen is prevented from being introduced, and the quality of pyrolysis gas is improved.
The bubbling bed 1-2 provides an environment for the reaction of the oxygen carrier, the biomass coke and the tar, adopts bubbling fluidization, adjusts the mixed flow between the gasification product and the oxygen carrier, and controls the reaction and the quality of the synthesis gas by regulating and controlling the temperature and the flow rate of the reforming steam.
The ascending pipe 1-7 is a place for realizing oxidation regeneration of the partial oxidation oxygen carrier 1-1-3, and the oxidation oxygen carrier is conveyed to the upper end of the ascending pipe and enters a descending moving bed by adopting fast fluidization.
The ascending pipe 1-7 is internally subjected to strong exothermic reaction, part of generated heat is absorbed by flue gas, the heat is discharged by a heat exchanger for enterprises to use, and the rest heat is carried into the descending moving bed by the oxidation state oxygen carrier 1-1-1 in a sensible heat manner to provide required heat and lattice oxygen for the gasification of the traditional Chinese medicine residues.
The air preheaters 1-12 adopt a dividing wall type heat exchanger form, preheat air to 650-700 ℃ by recovering heat of high-temperature pyrolysis gas, reduce energy consumption and reduce the temperature of the pyrolysis gas at the same time.
The chemical chain system described above operates as follows:
the oxygen carrier is oxidized at high temperature in the ascending pipe 1-7 to reach the high temperature of 900-. The pyrolysis gas at the upper end 1-4 of the descending moving bed is mixed with water vapor to form high-moisture-content pyrolysis gas, the high-moisture-content pyrolysis gas is input into a biomass coke fixed bed 1-9 to separate unreacted tar, is cooled by an air preheater 1-12 and then enters a bubbling bed 1-2 to be used as a fluidizing medium and reforming gas, and is subjected to steam reforming reaction and coke gasification with a reduced oxygen carrier 1-1-2; the temperature in the bubbling bed is 700 ℃, and the coke is gasified by the reduced oxygen carrier 1-1-2; the synthesis gas generated in the bubbling bed is separated by the cyclone separators 1-13 to be discharged out of the system, and finally the high-quality synthesis gas is output for pharmaceutical enterprises to use.
The oxygen carrier is continuously and repeatedly used for a plurality of times in the descending moving beds (1-4 and 1-5), the bubbling bed 1-2 and the ascending pipe 1-7. The oxygen carrier in the descending moving bed pyrolyzes and gasifies the Chinese medicine dregs, and the Chinese medicine dregs lose oxygen to become a reduction state oxygen carrier. The tar and the biomass coke are catalyzed and gasified by a reduction oxygen carrier in the bubbling bed 1-2, the reduction oxygen carrier and pyrolysis gas are subjected to steam reforming reaction to improve the quality of the synthesis gas, the oxygen carrier is partially oxidized during the reaction process, and then the synthesis gas enters an ascending pipe 1-7 for complete oxidation and regeneration. The reaction belongs to a strong exothermic reaction, and is regulated and controlled by adjusting the air flow, so that local temperature runaway and oxygen carrier sintering caused by too fast reaction are prevented. The high-temperature flue gas after the reaction is discharged with heat for the enterprise heat supply of system through the heat exchanger.
Example 2:
the iron-based oxygen carrier provided by the application is Fe 2 O 3 CaO and Na as active components 2 O is a composite oxygen carrier with a catalytic function formed by an auxiliary agent and an inert carrier, and the oxidation-reduction process is repeated in a descending moving bed, a descending pipe, a bubbling bed and an ascending pipe.
The above metal active component Fe 2 O 3 For providing active oxygen and catalytic active center, the total weight ratio is controlled in the range of 35 wt% to 50 wt%, and the loading amount depends on the inert carrier structure and the specific surface area. Fe 2 O 3 Is prepared from Chinese medicinal residueGasification oxygen supply, and the reduced Fe simple substance or FeO as a catalytic active center improves the conversion rate of tar and the H of pyrolysis gas 2 And CO yield.
The iron-based oxygen carrier provided by the application is added with CaO and Na 2 O as an auxiliary agent for increasing Fe 2 O 3 Oxygen ion migration capacity is used for improving the gasification conversion rate of the traditional Chinese medicine residues, simultaneously, the water gas reaction is promoted in the bubbling bed, the quality of the synthesis gas is improved, and the total weight ratio is controlled within the range of 0-25 wt%.
The application provides an iron-based oxygen carrier, which is prepared from Al 2 O 3 、SiO 2 、TiO 2 One or the composite material combined by the inert carrier is used for increasing active component Fe 2 O 3 The reactivity, the cycling stability and the carbon deposition resistance of the catalyst.
Three iron-based oxygen carriers were prepared and tested for their performance. As shown in fig. 2, the product distribution of the traditional Chinese medicine slag synthesis gas of the three iron-based oxygen carriers under the same reaction conditions is shown. Compared with the method using quartz stone (Sands) as the bed material, the synthesis gas has higher CO under three oxidation state iron-based oxygen carriers (Fe-O, RM-O, AI-O) 2 After the steam reforming of reduced oxygen carriers (Fe-Re, RM-Re, AI-Re) and low-temperature pyrolysis gas, the CO yield is greatly reduced, and H 2 The yield is improved, and the RM (red mud) oxygen carrier contains CaO and Na 2 O as an auxiliary agent and having a lower CH 4 The yield is expected to obtain higher-quality synthesis gas by regulating and controlling the proportion of the auxiliary agent.
As shown in FIG. 3, the gasification residual carbon content of the dregs of the above iron-based oxygen carrier under the same reaction conditions is shown. Compared with pure pyrolysis (Sands) of the traditional Chinese medicine residues, the iron-based oxygen carrier reduces the amount of residual carbon in the traditional Chinese medicine residue gasification product. The reduced oxygen carrier and the oxidized oxygen carrier have no obvious influence on the residual carbon content in the gasification product of the Chinese medicine residue, and both the reduced oxygen carrier and the oxidized oxygen carrier are about 5 wt%.
The foregoing is an exemplary embodiment of the present application, and the scope of the present application is defined by the claims and their equivalents.
Claims (5)
1. A device for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues is characterized by comprising a bubbling bed (1-2), an overflow pipe (1-3), a descending moving bed, a downcomer (1-6), an ascending pipe (1-7), a gas-solid separation device (1-8), a biomass coke fixed bed (1-9), a high-temperature fan (1-10), a blower (1-11), an air preheater (1-12) and a cyclone separator (1-13);
the descending moving bed comprises a descending moving bed upper end (1-4) and a descending moving bed lower end (1-5) which are connected with each other, and the descending moving bed is provided with a first input port, a second input port, a first output port and a second output port; high-water-content traditional Chinese medicine residues (1-16) are input from a first input port at the upper end (1-4) of the descending moving bed, a first output port of the descending moving bed is connected with an input port of the downcomer (1-6), and a second output port of the descending moving bed is connected with an input port of the biomass coke fixed bed (1-9); the output port of the biomass coke fixed bed (1-9) is connected with the input port of the high-temperature fan (1-10), and the output port of the high-temperature fan (1-10) is connected with the first input port of the air preheater (1-12); a first output port of the air preheater (1-12) is connected with a second input port of the bubbling bed (1-2), and a second output port is connected with a first input port of the ascending pipe (1-7);
the overflow pipe (1-3) is arranged in the bubbling bed (1-2) and is connected with a first output port of the bubbling bed (1-2), and an output port of the downcomer (1-6) is connected with a first input port of the bubbling bed (1-2) in the bubbling bed (1-2); a first output port of the bubbling bed (1-2) is connected with a second input port of the ascending pipe (1-7), and a second output port of the bubbling bed (1-2) is connected with an input port of the cyclone separator (1-13);
the output port of the ascending pipe (1-7) is connected with the input port of the gas-solid separation device (1-8), and the first output port of the gas-solid separation device (1-8) is connected with the second input port of the descending moving bed;
the blower (1-11) is connected with a second input port of the air preheater (1-12);
the diameter of the descending moving bed is larger than that of the downcomer (1-6).
2. The apparatus of claim 1, wherein the air preheater (1-12) recovers pyrolysis gas heat using a dividing wall gas-gas heat exchanger and heats the preheated air (1-14) to a temperature of 650 ℃ to 700 ℃.
3. The apparatus according to claim 1, wherein the second inlet of the bubbling bed (1-2) is provided with at least two inlets.
4. A method for preparing high-quality synthesis gas by gasifying high-water-content traditional Chinese medicine residues is characterized in that the high-water-content traditional Chinese medicine residues (1-16) are input from a first input port of a descending moving bed, the high-water-content traditional Chinese medicine residues (1-16) are fully contacted and dried with an oxidation state oxygen carrier (1-1-1) at the upper end (1-4) of the descending moving bed, then the traditional Chinese medicine residues are pyrolyzed and gasified by the oxidation state oxygen carrier (1-1-1) at the lower end (1-5) of the descending moving bed, and the oxidation state oxygen carrier loses oxygen to become a reduction state oxygen carrier (1-1-2);
the pyrolysis gas at the upper end (1-4) of the descending moving bed is mixed with water vapor to form high-moisture-content pyrolysis gas, the high-moisture-content pyrolysis gas is input into a biomass coke fixed bed (1-9) to separate unreacted tar, is cooled by an air preheater (1-12), enters a bubbling bed (1-2) to serve as a fluidized medium and reformed steam, and performs steam reforming reaction and coke gasification with a reduced oxygen carrier (1-1-2); the temperature in the bubbling bed is 700 ℃, and the reduced oxygen carrier (1-1-2) catalyzes coke gasification; synthetic gas is generated in the bubbling bed (1-2), fly ash is separated by a cyclone separator (1-13) and discharged out of the system, and finally high-quality synthetic gas (1-19) is output;
the air preheater (1-12) heats air input by the blower (1-11) to obtain preheated air (1-14), and the preheated air (1-14) enters the ascending pipe (1-7); and partial oxidation oxygen carriers (1-1-3) after steam reforming reaction in the bubbling bed (1-2) are discharged from the bubbling bed through an overflow pipe (1-2) and enter an ascending pipe (1-7) to be subjected to strong exothermic reaction with preheated air (1-14) for complete regeneration, the regenerated oxidation state oxygen carriers (1-1-1) are sent into a descending moving bed through a gas-solid separation device (1-8) to start new circulation, and the separated high-temperature flue gas (1-15) is discharged from a system and used for heat supply of enterprises.
5. The method according to claim 4, characterized in that the oxygen carrier in an oxidized state (1-1-1) is an iron-based oxygen carrier, the composition of which comprises a metal active component, an auxiliary agent and an inert carrier; the metal active component is Fe 2 O 3 35-50 wt% of the total weight; the auxiliary agent is CaO or Na 2 O, accounting for 0-25 wt% of the total weight; the inert carrier is Al 2 O 3 Or SiO 2 Or TiO 2 Or from Al 2 O 3 、SiO 2 、TiO 2 Any combination of (a) and (b).
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