CN111892963B - Gasification and reburning denitration method for waste cathode carbon block of electrolytic aluminum - Google Patents
Gasification and reburning denitration method for waste cathode carbon block of electrolytic aluminum Download PDFInfo
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- CN111892963B CN111892963B CN202010826514.8A CN202010826514A CN111892963B CN 111892963 B CN111892963 B CN 111892963B CN 202010826514 A CN202010826514 A CN 202010826514A CN 111892963 B CN111892963 B CN 111892963B
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L1/00—Liquid carbonaceous fuels
- C10L1/32—Liquid carbonaceous fuels consisting of coal-oil suspensions or aqueous emulsions or oil emulsions
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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
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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
- C10J3/72—Other features
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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
- 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
- C10J2300/0946—Waste, e.g. MSW, tires, glass, tar sand, peat, paper, lignite, oil shale
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Abstract
The invention discloses a method for gasifying and reburning denitration of waste cathode carbon blocks of electrolytic aluminum, which comprises the following steps: crushing waste cathode carbon of electrolytic aluminum, mixing with quicklime and water, and ball-milling to prepare carbon slurry; gasifying the carbon slurry at a temperature above the cryolite melting temperature and below 1500 ℃. The method realizes the recycling of alumina and fluoride of carbon block ash, the gasified gas is used as clean fuel or is used for reburning fuel of a coal-fired boiler, the carbon block disposal quantity is large, and the process is clean and efficient.
Description
Technical Field
The invention belongs to the technical field of electrolytic aluminum waste cathode carbon block treatment, and particularly relates to a method for gasifying and reburning denitration of an electrolytic aluminum waste cathode carbon block.
Background
The information in this background section is only for enhancement of understanding of the general background of the invention and is not necessarily to be construed as an admission or any form of suggestion that this information forms the prior art that is already known to a person of ordinary skill in the art.
The electrolytic aluminum process generates solid wastes including cathodes, side carbon blocks, impermeable materials, refractory bricks, cold ramming paste, insulating bricks, heat insulation plates and the like due to overhaul of an aluminum electrolytic cell. According to the service life of the electrolytic cell, namely the overhaul period of 4-6 years, 10-15 kg of waste cathodes and 10-20 kg of carbon slag are generated by smelting one ton of raw aluminum, so that a large amount of waste cathodes and carbon slag are generated. The waste cathode contains about 70% of carbon and 30% of electrolyte, and the carbon residue contains about 35% of carbon and 65% of electrolyte. The solid electrolyte contained in the two is a fluoride (cryolite 3 NaF. AlF is the main component)3) Has strong corrosiveness and contains trace cyanide [ Na ]4Fe(CN)6]. According to different parts, the mass content of fluorine element in the electrolytic aluminum waste cathode carbon block is 10-20%, and the fluorine element is a main harmful component in the electrolytic aluminum waste cathode carbon block. According to the classification of the national hazardous waste records, the waste cathode and carbon slag generated by the overhaul of the aluminum electrolysis cell belong to hazardous solid wastes.
At present, the existing treatment method of the waste cathode carbon block of the electrolytic aluminum comprises the following steps: mixing the treated electrolytic aluminum waste cathode carbon block with a calcium-based fluorine fixing agent in proportion, grinding the mixture into powder by a steel ball mill, and burning the powder in a furnace; during the combustion of waste cathode carbon block powder of electrolytic aluminum in a boiler, cyanide contained in the waste cathode carbon block powder is decomposed into CO at high temperature in the boiler2And N2The fluorine element is released as F in the furnace-Moiety F-Reacts with the added calcium-based fluorine fixing agent and calcium ions in the coal to generate insoluble calcium fluoride. However, calcium fluoride is easily decomposed at high temperature of 1200-1400 ℃ in a pulverized coal furnace, and the high-temperature fluorine-fixing rate of limestone, lime and other substances is very low. Therefore, the conversion of the fluorine element in ash solid phase is low, and a large amount of fluorine element can enter a wet desulphurization system along with flue gas in a gas phase form, so that unpredictable effects are brought, such as local scaling of the desulphurization system caused by excessive calcium fluoride, difficulty in treating fluorine ions in wastewater and the like.
The method for burning and fixing fluorine in the waste cathode carbon block for electrolyzing aluminum comprises the following steps: (1) crushing waste cathode carbon blocks of electrolytic aluminum and grinding the crushed waste cathode carbon blocks into powder for later use; (2) spraying water-soluble calcium salt solution into the powder, stirring and simultaneously applying ultrasonic waves; (3) and (3) feeding the product obtained in the step (2) and raw coal into a fluidized bed boiler for combustion. The method not only has high fluorine fixing efficiency, but also converts fluorine into stable CaF2And fly ash and bottom ash are added after calcium fluoroaluminate and the like, so that the phenomenon that HF enters flue gas and affects denitration, desulfurization and wastewater treatment systems of a boiler system is reduced, and the content of fluorine finally discharged into the atmosphere is far less than the national discharge standard.
The process is based on the fact that waste cathode carbon blocks are mixed into a coal-fired boiler for combustion, the treatment capacity is small, and related fluorides are mainly mixed into coal-fired ash, desulfurization gypsum, desulfurization wastewater and the like. 32 to 47 percent of basic ash content received by the carbon block and 3NaF AlF in the carbon block3、NaF、CaF2Is subjected to high temperatureThe solid wastes such as coal ash and slag are transferred during combustion, and the high-value utilization is difficult.
Disclosure of Invention
Aiming at the technical problems in the prior art, the invention provides a method for gasifying and reburning denitration of waste cathode carbon blocks of electrolytic aluminum.
To solve the above technical problem, one or more of the following embodiments of the present invention provide the following technical solutions:
a gasification and reburning denitration method for waste cathode carbon blocks of electrolytic aluminum comprises the following steps:
crushing waste cathode carbon of electrolytic aluminum, mixing with quicklime and water, and ball-milling to prepare carbon slurry;
gasifying the carbon slurry at a temperature above the cryolite melting temperature and below 1500 ℃.
Compared with the prior art, one or more technical schemes of the invention have the following beneficial effects:
1) the characteristics of large ash content, difficult combustion, easy complete gasification of superfine gasification and water solubility of NaF of the waste cathode carbon of electrolytic aluminum are utilized to realize the wet grinding of NaF, calcium oxide and water together to prepare slurry and realize the in-situ generation of CaF2To avoid HF evolution and corrosion of the equipment.
2) The carbon slurry fuel prepared by ultra-fining waste cathode carbon realizes that calcium hydroxide is uniformly dispersed on the surface and the internal pores of carbon particles in the slurry gasification process, CaO generated by low-temperature decomposition of calcium hydroxide fully reacts with HF to generate calcium fluoride CaF in the processes of heated evaporation and pyrolysis of slurry droplets2And high temperature formation of stable calcium fluoroaluminate 11 CaO.7Al2O3·CaF2。
3) Solid fluoride contained in the prepared high-temperature gasified gas is separated by a cyclone separator, fine particles and gaseous fluoride are filtered by an alumina adsorbent, and the fluoride is greatly reduced to enter a subsequent boiler combustion system.
4) The gasified ash and the alumina adsorbent have high alumina and fluoride content, can be recycled as electrolytic aluminum raw materials, and realizes resource utilization.
5) The purified gasified gas is used as a boiler and a reburning denitration fuel, is clean and environment-friendly, does not bring negative effects to the boiler and environment-friendly facilities thereof, and has better environmental benefits.
6) The waste cathode carbon is prepared into the superfine carbon slurry fuel, the disposal amount of the carbon block and the scale selection range of the gasification furnace are large, the gasified gas is conveniently used for the boiler or the coal-fired boiler for blending combustion, the combustion system is slightly changed, the low-nitrogen combustion is conveniently realized, and the environment benefit and the social benefit are good.
7) Compared with the existing method for treating the dangerous waste of the electrolytic aluminum waste cathode carbon block, the method has the advantages that the main equipment used by the method is a wet ball mill, a gasification furnace and alumina high-temperature purification equipment, the method is easy to realize, the gasification gas blending combustion transformation can be carried out by combining a coal-fired boiler, and the comprehensive utilization benefit of the waste is high.
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The accompanying drawings, which are incorporated in and constitute a part of this specification, are included to provide a further understanding of the invention, and are incorporated in and constitute a part of this specification, illustrate exemplary embodiments of the invention and together with the description serve to explain the invention and not to limit the invention.
FIG. 1 is a process flow diagram of an embodiment of the invention.
Detailed Description
It is to be understood that the following detailed description is exemplary and is intended to provide further explanation of the invention as claimed. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.
It is noted that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of exemplary embodiments according to the invention. As used herein, the singular forms "a", "an" and "the" are intended to include the plural forms as well, and it should be understood that when the terms "comprises" and/or "comprising" are used in this specification, they specify the presence of stated features, steps, operations, devices, components, and/or combinations thereof, unless the context clearly indicates otherwise.
A gasification and reburning denitration method for waste cathode carbon blocks of electrolytic aluminum comprises the following steps:
crushing waste cathode carbon of electrolytic aluminum, mixing with quicklime and water, and ball-milling to prepare carbon slurry;
gasifying the carbon slurry at a temperature above the cryolite melting temperature and below 1500 ℃. Below this temperature range, cryolite is stable, the amount of volatilization above the melting temperature is large, and the degree of conversion of fluorine into calcium fluoride is limited; in addition, the gasification rate of the charcoal is very low, generally above 1200 ℃, and the coke, graphite electrode and H are mixed2O and CO2The reaction is violent, and the gasification efficiency can be ensured. Too high a gasification temperature leads to destruction of the refractory and melting of the ash.
In some embodiments, the amount of quicklime added is such that the molar ratio of calcium in the quicklime to fluorine in the carbon block is 1: 1.5-2.5.
Furthermore, the solid content in the carbon slurry is 50-70%.
Furthermore, the mass of the particles with the particle diameter smaller than 45 μm in the solid particles in the carbon slurry accounts for more than 90 percent of the total mass of the solid. The actual corresponding industry sieve mesh number is 325 meshes. The cathode carbon block is coke special for the electrode, the graphitization degree is high, high-temperature reaction is needed in the combustion gasification reaction, solid particles are too large to be completely gasified, and the carbon conversion rate is low.
In some embodiments, the method further comprises the step of subjecting the gasification gas to gas-solid separation.
Further, the method also comprises the step of carrying out fluoride adsorption on the gasified gas by using an alumina adsorbent.
Firstly, removing fly ash by gas-solid separation, then removing fluoride by adsorption of alumina, and reacting the alumina with HF to generate AlF3。
Further, the method also comprises a step of introducing the purified gasified gas into a boiler for combustion, or a step of using the purified gasified gas as the boiler reburning gas.
Furthermore, when gasification gas is used as boiler reburn gas, the heat input of the gasification gas is 10% to 30% of the heat input of the boiler.
Further, the method also comprises the step of recycling the ash residue after gas-solid separation and the invalid alumina adsorbent as the electrolytic aluminum raw material.
Example 1
A method for gasifying and reburning denitration of waste cathode carbon blocks of electrolytic aluminum comprises the following steps:
(1) crushing the waste cathode carbon blocks of the electrolytic aluminum into crushed materials with the granularity less than or equal to 30mm by a hammer crusher, doping quicklime powder (the granularity is less than or equal to 30mm) according to the calcium-fluorine molar ratio of 1:2, and performing ball milling to prepare carbon slurry fuel, wherein the water addition amount and the solid material ratio are 60: 100;
(2) the accumulated mass of particles with the solid particle size of less than 45 mu m in the prepared carbon slurry fuel accounts for 90 percent of the total mass of the solid particles;
(3) adopting a Texaco (Texaco) pressure gasification furnace, wherein the gasification pressure is 6.5MPa, and the gasification temperature is 1350 ℃; the carbon conversion rate can reach 99% at most, and the effective gas (CO + H) in the gasified gas2) The volume content reaches 83 percent.
(4) The gasified gas passes through a cyclone separator and an alumina adsorbent layer in sequence to remove ash and fluoride in the gasified gas;
(5) the combustion flue gas of the gasified gas after the boiler is combusted and purified meets the emission standard of a natural gas boiler.
Example 2
A method for gasifying and reburning denitration of waste cathode carbon blocks of electrolytic aluminum comprises the following steps:
(1) crushing the waste cathode carbon blocks of the electrolytic aluminum to crushed materials with the granularity less than or equal to 30mm by a hammer crusher, adding quicklime powder (the granularity is less than or equal to 30mm) according to the calcium-fluorine molar ratio of 1:1.5, adding water and solid materials in a ratio of 65:100, and performing ball milling to prepare carbon slurry fuel;
(2) the accumulated mass of the solid particles with the particle size of less than 45 mu m in the prepared carbon slurry fuel accounts for 95 percent of the total mass of the solid particles;
(3) adopting a Texaco pressurized gasification furnace, wherein the gasification pressure is 6.5MPa, and the gasification temperature is 1400 ℃; the carbon conversion rate can reach 99.3 percent, and the effective gas (CO + H)2) The volume content reaches 83.5 percent.
(4) The low-nitrogen combustion transformation of the coal-fired boiler is combined, the gasified gas is mixed with the coal-fired boiler, the input heat accounts for 15%, the concentration of nitrogen oxides at the inlet of a boiler flue gas denitration facility is reduced by 12%, the SCR denitration operation cost is reduced, and the problems of other environment-friendly facilities of the coal-fired boiler are not caused.
Example 3
A method for gasifying and reburning denitration of waste cathode carbon blocks of electrolytic aluminum comprises the following steps:
(1) crushing the waste cathode carbon block of the electrolytic aluminum to crushed materials with the granularity less than or equal to 30mm by a hammer crusher, adding quicklime (the granularity is less than or equal to 30mm) according to the molar ratio of calcium to fluorine of 1:2, and adding water in a proportion of 65:100 to the solid materials.
(2) The particle size of solid particles in the prepared carbon slurry fuel is less than 45 mu m, and the accumulated mass of particles with the particle size of less than 45 mu m accounts for 95 percent of the total mass of the solid particles;
(3) adopting a Texaco pressurized gasification furnace, wherein the gasification pressure is 6.5MPa, and the gasification temperature is 1400 ℃; the carbon conversion rate can reach 99.3 percent, and the effective gas (CO + H)2) The volume content is up to 83.5 percent.
(4) The low-nitrogen combustion transformation of the coal-fired boiler is combined, the gasified gas is mixed with the coal-fired boiler, the input heat accounts for 30%, the concentration of nitrogen oxides at the inlet of a boiler flue gas denitration facility is reduced by 26%, the SCR denitration operation cost is reduced, and the problems of other environment-friendly facilities of the coal-fired boiler are not caused.
Example 4
(1) Crushing the waste cathode carbon blocks of the electrolytic aluminum by a hammer crusher to crushed materials with the granularity less than or equal to 30mm, mixing quicklime powder (the granularity less than or equal to 30mm) according to the calcium-fluorine molar ratio of 1:2, and adding water and solid materials according to the ratio of 60: 100.
(2) The particle size of solid particles in the prepared carbon slurry fuel is less than 45 mu m, and the accumulated mass of particles with the particle size of less than 45 mu m accounts for 90 percent of the total mass of the solid particles;
(3) adopting a Texaco (Texaco) pressure gasification furnace, wherein the gasification pressure is 6.5MPa, and the gasification temperature is 1350 ℃; the carbon conversion rate can reach 99 percent, and the effective gas (CO + H)2) The volume content is up to 83 percent.
(4) Analysis of gasifier Ash, where Al2O3The mass percentage of (B) is 26%.
Example 5
(1) Crushing the waste cathode carbon blocks of the electrolytic aluminum to crushed materials with the granularity less than or equal to 30mm by a hammer crusher, adding quicklime powder (the granularity is less than or equal to 30mm) according to the calcium-fluorine molar ratio of 1:2.5, and adding water and solid materials according to the ratio of 60: 100.
(2) The particle size of solid particles in the prepared carbon slurry fuel is less than 45 mu m, and the accumulated mass of particles with the particle size of less than 45 mu m accounts for 90 percent of the total mass of the solid particles;
(3) adopting a Texaco (Texaco) pressurized gasification furnace, wherein the gasification pressure is 6.5MPa, and the gasification temperature is 1150 ℃; the carbon conversion rate can reach 94%, and the effective gas (CO + H)2) The volume content is up to 78 percent.
(4) Analysis of gasifier Ash, where Al2O3The mass percentage of (B) is 25%.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (6)
1. A method for gasifying and reburning denitration of waste cathode carbon blocks of electrolytic aluminum is characterized by comprising the following steps: the method comprises the following steps:
crushing waste cathode carbon of electrolytic aluminum, mixing with quicklime and water, and ball-milling to prepare carbon slurry;
gasifying the carbon slurry at a temperature above the melting temperature of cryolite and below 1500 ℃;
carrying out gas-solid separation on the gasified gas, and carrying out fluoride adsorption on the gasified gas by using an alumina adsorbent;
the cleaned gasification gas is used as boiler reburning gas.
2. The method for gasifying, reburning and denitrating the waste cathode carbon block of electrolytic aluminum according to claim 1, wherein the method comprises the following steps: the addition amount of the quicklime enables the molar ratio of calcium in the quicklime to fluorine in the carbon block to be 1: 1.5-2.5.
3. The method for gasifying, reburning and denitrating the waste cathode carbon block of electrolytic aluminum according to claim 2, wherein the method comprises the following steps: the solid content in the carbon slurry is 50-70%.
4. The method for gasifying, reburning and denitrating the waste cathode carbon block of electrolytic aluminum according to claim 3, wherein the method comprises the following steps: the mass of the particles with the particle diameter smaller than 45 μm in the solid particles in the carbon slurry accounts for more than 90 percent of the total mass of the solid.
5. The method for gasifying, reburning and denitrating the waste cathode carbon block of electrolytic aluminum according to claim 1, wherein the method comprises the following steps: when the gasification gas is used as the boiler reburning gas, the input heat of the gasification gas accounts for 10% -30% of the input heat of the boiler.
6. The method for gasifying, reburning and denitrating the waste cathode carbon block of electrolytic aluminum according to claim 1, wherein the method comprises the following steps: also comprises the step of recycling the ash residue after gas-solid separation and the invalid alumina adsorbent as electrolytic aluminum raw materials.
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| CN111250515A (en) * | 2020-01-21 | 2020-06-09 | 山东大学 | Method for burning and fixing fluorine of waste cathode carbon block of electrolytic aluminum and application thereof |
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| CN103415596A (en) * | 2011-02-23 | 2013-11-27 | 西格里碳素欧洲公司 | Method for processing used cathode material containing carbon |
| CN102161049A (en) * | 2011-04-01 | 2011-08-24 | 陈俊贤 | Comprehensive utilization method of waste and old cathode carbon blocks of aluminium electrolytic bath |
| CN107720723A (en) * | 2017-11-09 | 2018-02-23 | 北京科技大学 | A kind of method of overall treatment aluminium electrolytic tank |
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