CN113816410A - Method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash - Google Patents
Method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash Download PDFInfo
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- C01F7/00—Compounds of aluminium
- C01F7/02—Aluminium oxide; Aluminium hydroxide; Aluminates
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Abstract
The invention discloses a method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash, belonging to the field of hazardous solid waste disposal and utilization. The calcium aluminate which can be used in the fields of metallurgy, building materials and the like is obtained by mixing and uniformly mixing aluminum ash, waste incineration fly ash, fluorine fixing agent and denitrifying agent according to a certain proportion, heating for denitrogenation and dioxin degradation, and casting a melt. The aluminum ash comprises primary aluminum ash and secondary aluminum ash, an aluminum source is provided for preparing calcium aluminate, a calcium source is provided for waste incineration fly ash, the fluorine fixing agent realizes stable solidification of an element F in the mixture, and the nitrogen removing agent increases the contact probability of AlN and air. The method realizes the synergistic harmless treatment and high-value utilization of the hazardous waste aluminum ash and the waste incineration fly ash, and has the advantages of short flow, simple process, low cost and the like.
Description
Technical Field
The invention discloses a method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash, belonging to the field of hazardous solid waste disposal and utilization.
Background
Aluminous ash is a hazardous solid waste (HW48) generated during the process of electrolysis, processing and regeneration of aluminium, divided into primary aluminous ash and secondary aluminous ash. According to the official network of the State statistical office, the yield of electrolytic aluminum in China is 3708 ten thousand tons in 2020, and the aluminum ash production amount in the aluminum processing and regeneration process is estimated to generate aluminum ash (Al in the aluminum ash)2O3The content is generally more than 65 percent) is over 300 ten thousand tons. The waste incineration fly ash (hereinafter referred to as fly ash, the content of CaO in the fly ash is generally more than 40%) contains heavy metals, organic matters and other hazardous substances, and belongs to dangerous solid waste (HW18), and the generation and the stock of the fly ash in 2021 year exceed 1000 ten thousand tons. The traditional disposal methods of the aluminum ash and the fly ash are stockpiling and landfill, and the harmlessness and the resource of the aluminum ash and the fly ash cannot be realized.
The aluminum ash slag is rich in toxic and harmful substances such as fluoride, cyanide, aluminum carbide, aluminum nitride and the like, and the fly ash contains Cr, Zn, Pb and highly toxic dioxin, so that serious environmental pollution can be caused if the fly ash is not properly treated. Therefore, the harmless disposal and resource utilization of the aluminum ash and the waste incineration fly ash become bottleneck problems which hinder the green development of the economic society.
Chinese invention patent (CN 112794353A) discloses a method and a device for preparing polyaluminium chloride by recycling aluminium ash, wherein secondary aluminium ash is obtained by washing and drying, then waste hydrochloric acid is added to obtain aluminium chloride solution, and the aluminium chloride solution is aged, filtered and centrifuged to obtain the polyaluminium chloride, but the water consumption is large and a large amount of waste acid is generated.
The Chinese invention patent (CN 108275708B) discloses a secondary aluminum ash resource utilization method, which comprises the steps of grinding secondary aluminum ash into powder, then flushing the powder with steam under high pressure, recovering nitrogen and hydrogen fluoride, recovering chlorine salt through processes of suction filtration, evaporative crystallization and the like, roasting a filtered solid phase at 1300-1500 ℃ to recover fluoride, adding an alkali flux to carry out impurity removal smelting at 800-1100 ℃, then adding liquid to carry out solid-liquid separation, and finally calcining the leachate at more than 1000 ℃ to obtain alumina.
The Chinese invention patent (application No. 201910629363.4) discloses a method for harmlessly treating fly ash and bottom ash from waste incineration by low-temperature melting, which comprises the steps of carrying out magnetic separation and screening classification treatment on the bottom ash from waste incineration, respectively carrying out water washing, gravity separation and ore grinding pretreatment on the bottom ash with different particle sizes, granulating the obtained granules together with the washed fly ash, and drying and melting the obtained granules to provide partial production raw materials for nonferrous metallurgy.
The Chinese invention patent (application No. 202011557600.X) discloses a harmless resource treatment improvement method of waste incineration fly ash, which removes heavy metals by taking polyvinyl chloride as a chlorinating agent in a heat treatment furnace through a chloride volatilization method. The fly ash and the polyvinyl chloride are kept at 900 ℃ for 2h, 100% of Pb and Zn and 50% of Cu and Mn can be removed, then the metal chloride is concentrated by using an aqueous solution in gas washing equipment, and acid gas is removed from gas flow.
The Chinese invention patent (application number: 202011500145.X) discloses a method for preparing a calcium aluminate steelmaking desulfurizer by melting high magnesium aluminum ash, which comprises the steps of carrying out wet ball milling on the high magnesium aluminum ash under the condition that the pH value is 12-13.5, hydrolyzing aluminum nitride and aluminum carbide, removing soluble salt, then carrying out dry grinding after mixing with steel slag and slaked lime, and finally roasting at 1350-1400 ℃ to obtain calcium aluminate; the invention discloses a method for preparing calcium aluminate by co-processing high magnesium aluminum ash and fly ash (application number: 202011500017.5). The process is similar to the method for preparing a calcium aluminate steelmaking desulfurizer by melting the high magnesium aluminum ash, a method of roasting after wet ball milling is adopted, the two invention patents are similar to the product of the invention, but the essence of wet ball milling is still to utilize alkaline solution to react with AlN, waste water is generated in the process, the ball milling energy consumption is high, and alkaline oxide is introduced in the alkaline environment to reduce the relative content of the calcium aluminate.
In conclusion, the existing harmless disposal and resource utilization of the aluminum ash and the fly ash have the problems of high cost, low utilization rate, heavy environmental burden and the like, and the research and development of a method for environment-friendly and efficient synergistic utilization of the aluminum ash and the fly ash are urgently needed.
Disclosure of Invention
The invention aims to fully utilize the component characteristics and detoxification mechanism of aluminum ash slag and fly ash and provide a method for preparing calcium aluminate by using aluminum ash slag and waste incineration fly ash, wherein the aluminum ash slag rich in alumina is used as an aluminum source of the calcium aluminate, the fly ash with a large amount of CaO is used as a calcium source of the calcium aluminate, the heat of heat treatment is utilized to promote the degradation of dioxin, reduce the toxicity equivalent, and simultaneously, chloride is volatilized, so that the harmlessness and the resource utilization of the aluminum ash slag and the fly ash are realized.
The invention is realized by the following technical scheme:
a method for preparing calcium aluminate by aluminum ash and waste incineration fly ash in cooperation with waste incineration fly ash comprises the steps of mixing and evenly mixing aluminum ash and waste incineration fly ash, a fluorine fixing agent and a denitrifying agent, heating in a heat treatment furnace to remove nitrogen, melting, and casting a melt to obtain calcium aluminate; the aluminum ash comprises primary aluminum ash and secondary aluminum ash, an aluminum source is provided for preparing calcium aluminate, a calcium source is provided for waste incineration fly ash, a fluorine fixing agent realizes stable solidification of an element F in a mixture, a denitrifying agent increases the contact probability of AlN and air, and the heat treatment furnace is any one of an electric arc furnace, a medium frequency furnace, a resistance furnace, a plasma furnace and a gas furnace;
further, the raw material ratio is 45-50 wt.% of aluminum ash residues, 40-50 wt.% of waste incineration fly ash, 5-15 wt.% of denitrifier, and 10-40 wt.% of fluorine fixing agent based on the total weight of the aluminum ash residues and the waste incineration fly ash.
Further, the fluorine-fixing agent is one or more of quicklime, calcium carbonate and calcium hydroxide.
Further, the denitrifier is one or more of sodium carbonate, sodium hydroxide and borax.
Further, the specific method comprises the following steps:
(1) preparing materials: mixing aluminum ash, waste incineration fly ash, a fluorine fixing agent and a denitrifying agent according to a certain proportion and uniformly mixing;
(2) heating for nitrogen removal: pouring the mixture into a heat treatment furnace, converting AlN in the aluminum ash into Al by using high temperature and a denitrifier2O3；
(3) Melting: and (4) raising the temperature of the heat treatment furnace, preserving the heat for a period of time to obtain a melt, and casting to obtain the calcium aluminate.
Further, the heating and nitrogen removal temperature is 1000-1300 ℃, and the temperature is kept for 10-60 min.
Further, the melting temperature is 1400-1600 ℃, and the temperature is kept for 20-120 min.
The principle of the invention is as follows:
(1) AlN in the aluminous ash reacts with oxygen and bound water at the temperature of more than 800 ℃ to generate nitrogen (N) by oxidation reaction with Gibbs free energy of less than 02、NH3However, at this time, an alumina film is formed to cover AlN, so in the present invention, the produced alumina film can be destroyed by the denitrifying agent, the probability of AlN contacting with air is increased, and the AlN pollution problem is solved, and the AlN oxidation reaction equation is as follows:
2AlN+3H2O＝Al2O3+2NH3 (1)
4AlN+3O2＝2Al2O3+2N2 (2)
(2) the aluminum ash contains part of F elements, and is combined with CaO and fluorine fixing agent in the fly ash in a high-temperature melting stage to be stabilized in the aluminum tetrahedron.
(3) The dioxin can be effectively decomposed at the temperature of over 800 ℃, and the heat generated at high temperature can break the benzene ring of the dioxin to decompose the dioxin into CO2HCl and H2O and the like, and the temperature in the process of preparing the calcium aluminate is more than 1000 ℃, so that the aim of removing pollutants is achieved, and the organic decomposition of toxicity of dioxin and the like can be represented by the following chemical reaction formula:
CxHyClz+(x+(y-z)/4)O2＝xCO2+zHCl↑+(y-z)/2H2O↑ (3)
(4) the principle of calcium aluminate formation: when the temperature is higher than 1300 ℃, Al in the secondary aluminum ash2O3Increase in particle diffusion rate and diffusion coefficientThe diffusion degree of the calcium aluminate, CaO and fluorine fixing agent in the fly ash is deepened, and the equation of synthesizing the calcium aluminate by high-temperature melting is as follows:
12CaO+7Al2O3＝12CaO·7Al2O3
the invention has the beneficial technical effects that:
(1) the method adopts Al in the aluminum ash2O3AlN is used as an aluminum source, CaO in the fly ash is used as a calcium source, so that the consumption of raw materials is greatly reduced, and the full-component efficient utilization of the aluminum ash slag and the fly ash is realized;
(2) the method of the invention efficiently converts AlN in the aluminous ash into Al2O3While the dioxin in the fly ash is cracked into nontoxic CO under the condition of high temperature2HCl and H2O, realizing the synergistic harmless treatment of the hazardous waste aluminum ash and the fly ash;
(3) the method converts the fly ash into the calcium aluminate at high temperature, can realize high-efficiency volume reduction of the fly ash, saves a large amount of land compared with the traditional landfill and cement curing treatment method, and converts the fly ash into valuable products;
(4) the method has the advantages of simple process, low cost, no pollution and wide applicability, and is easy for industrialization.
Drawings
FIG. 1 is a schematic flow chart of a method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash in cooperation in an embodiment of the invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
On the contrary, the invention is intended to cover alternatives, modifications, equivalents and alternatives which may be included within the spirit and scope of the invention as defined by the appended claims. Furthermore, in the following detailed description of the present invention, certain specific details are set forth in order to provide a better understanding of the present invention. It will be apparent to one skilled in the art that the present invention may be practiced without these specific details.
Example 1
Mixing 45 wt.% of aluminous ash, 45 wt.% of fly ash, 15 wt.% of sodium carbonate and 20% of CaO (the weight ratio of the aluminous ash to the waste incineration fly ash), adding the mixture into an intermediate frequency furnace, heating the mixture to 1200 ℃, preserving the temperature for 10 minutes, then heating the mixture to 1500 ℃, preserving the temperature for 30 minutes, pouring out the melt in the intermediate frequency furnace, and casting to obtain the calcium aluminate.
Example 2
Mixing 45 wt.% aluminum ash, 45 wt.% fly ash, 10 wt.% sodium hydroxide and 25% CaCO3Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into a resistance furnace, heating to 1250 ℃, preserving the heat for 15 minutes, heating to 1450 ℃, preserving the heat for 90 minutes, pouring out the melt in the resistance furnace, and casting to obtain the calcium aluminate.
Example 3
47 wt.% aluminum ash, 43 wt.% fly ash, 5 wt.% sodium hydroxide, 5 wt.% sodium carbonate and 20% CaO, 4% CaCO3Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into an intermediate frequency furnace, heating to 1000 ℃, preserving heat for 60 minutes, heating to 1480 ℃, preserving heat for 85 minutes, pouring out the melt in the intermediate frequency furnace, and casting to obtain the calcium aluminate.
Example 4
Mixing 46 wt.% of aluminous ash, 43 wt.% of fly ash, 11 wt.% of sodium carbonate and 10% of CaO (the weight ratio of the aluminous ash to the waste incineration fly ash), adding the mixture into a plasma furnace, heating the mixture to 1300 ℃ and preserving the temperature for 30 minutes, then heating the mixture to 1600 ℃ and preserving the temperature for 25 minutes, pouring out the melt in the plasma furnace and casting to obtain the calcium aluminate.
Example 5
Mixing 48 wt.% of aluminous ash, 44 wt.% of fly ash, 8 wt.% of borax and 13% of Ca (OH)2Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into a gas furnace, heating to 1180 ℃, preserving heat for 50 minutes, heating to 1490 ℃, preserving heat for 110 minutes, pouring out the melt in the gas furnace, and casting to obtain the calcium aluminate.
Example 6
Mixing 47 wt.% of aluminous ash, 44 wt.% of fly ash, 9 wt.% of sodium carbonate and 12% of CaO (the weight ratio of the aluminous ash to the waste incineration fly ash), adding the mixture into a gas furnace, heating to 1170 ℃, preserving heat for 45 minutes, heating to 1420 ℃, preserving heat for 80 minutes, pouring out the melt in the gas furnace, and casting to obtain the calcium aluminate.
Example 7
Mixing 46 wt.% of aluminum ash, 48 wt.% of fly ash, 3 wt.% of borax, 3 wt.% of sodium hydroxide and 11 wt.% of CaO (the weight ratio of the aluminum ash to the fly ash from the garbage incineration), adding the mixture into a gas furnace, heating to 1160 ℃, preserving heat for 48 minutes, heating to 1440 ℃, preserving heat for 105 minutes, pouring out the melt in the gas furnace, and casting to obtain the calcium aluminate.
Example 8
Mixing 46 wt.% of aluminum ash, 46 wt.% of fly ash, 2 wt.% of sodium carbonate, 3 wt.% of borax, 3 wt.% of sodium hydroxide and 11% of CaO (the weight ratio of the aluminum ash to the fly ash from refuse incineration), adding the mixture into an intermediate frequency furnace, heating to 1160 ℃, preserving heat for 48 minutes, heating to 1440 ℃, preserving heat for 105 minutes, pouring out the melt in the intermediate frequency furnace, and casting to obtain the calcium aluminate.
Example 9
Mixing 48 wt.% aluminous clinker, 47 wt.% fly ash, 5 wt.% sodium carbonate and 10% CaO, 2% Ca (OH)2，2％CaCO3Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into an intermediate frequency furnace, heating to 1090 ℃ for heat preservation for 52 minutes, heating to 1400 ℃ for heat preservation for 120 minutes, pouring out the melt in the intermediate frequency furnace, and casting to obtain the calcium aluminate.
Example 10
49 wt.% of aluminous clinker, 40 wt.% of fly ash, 5 wt.% of sodium carbonate, 6 wt.% of borax, 20% of CaO, 5% of CaCO3Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into an intermediate frequency furnace, heating to 1080 ℃, preserving heat for 55 minutes, heating to 1550 ℃, preserving heat for 50 minutes, pouring out the melt in the intermediate frequency furnace, and casting to obtain the calcium aluminate.
Example 11
Mixing 50 wt.% of aluminous ash, 42 wt.% of fly ash, 8 wt.% of sodium carbonate and 30% of CaO (the weight ratio of the aluminous ash to the waste incineration fly ash), adding the mixture into an intermediate frequency furnace, heating to 1050 ℃ and preserving the temperature for 40 minutes, then heating to 1460 ℃ and preserving the temperature for 100 minutes, pouring out the melt in the intermediate frequency furnace, and casting to obtain the calcium aluminate.
Example 12
50 wt.% of aluminous ash, 41 wt.% of fly ash, 9 wt.% of sodium carbonate and 30% of CaO, 10% of CaCO3Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into an electric arc furnace, heating to 1100 ℃, preserving the heat for 35 minutes, heating to 1530 ℃, preserving the heat for 35 minutes, pouring out the melt in the electric arc furnace, and casting to obtain the calcium aluminate.
Example 13
Mixing 49 wt.% of aluminous ash, 46 wt.% of fly ash, 5 wt.% of sodium carbonate and 15% of CaO (the weight ratio of the aluminous ash to the waste incineration fly ash), adding the mixture into an intermediate frequency furnace, heating to 1150 ℃ and preserving heat for 20 minutes, then heating to 1540 ℃ and preserving heat for 40 minutes, pouring out the melt in the intermediate frequency furnace, and casting to obtain the calcium aluminate.
Example 14
50 wt.% of aluminum ash, 41 wt.% of fly ash, 9 wt.% of sodium carbonate and 35% of CaCO3Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into an intermediate frequency furnace, heating to 1270 ℃, preserving heat for 25 minutes, heating to 1560 ℃, preserving heat for 20 minutes, pouring out the melt in the intermediate frequency furnace, and casting to obtain the calcium aluminate.
Example 15
50 wt.% aluminum ash, 42 wt.% fly ash, 8 wt.% sodium carbonate and 30% CaCO3，7％Ca(OH)2Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into an intermediate frequency furnace, heating to 1260 ℃, preserving the temperature for 18 minutes, heating to 1470 ℃, preserving the temperature for 70 minutes, pouring out the melt in the intermediate frequency furnace, and casting to obtain the calcium aluminate.
Example 16
Mixing 45 wt.% aluminum ash, 50 wt.% fly ash, 5 wt.% sodium carbonate, 20% CaO, 10% CaCO3，6％Ca(OH)2(the weight ratio of the aluminum ash to the waste incineration fly ash) is mixed and then added into a plasma furnace, and thenAnd raising the temperature to 1280 ℃, preserving the heat for 22 minutes, then heating to 1520 ℃, preserving the heat for 60 minutes, pouring out the melt in the plasma furnace, and casting to obtain the calcium aluminate.
Example 17
Mixing 45 wt.% aluminous clinker, 46 wt.% fly ash, 9 wt.% sodium carbonate and 20% CaO, 14% Ca (OH)2Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into a plasma furnace, heating to 1240 ℃, preserving heat for 23 minutes, heating to 1590 ℃, preserving heat for 22 minutes, pouring out the melt in the plasma furnace, and casting to obtain the calcium aluminate.
Example 18
Mixing 46 wt.% of aluminous clinker, 44 wt.% of fly ash, 10 wt.% of sodium carbonate and 19% of CaO, 14% of Ca (OH)2Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into a plasma furnace, heating to 1300 ℃ and preserving heat for 10 minutes, then heating to 1580 ℃ and preserving heat for 24 minutes, pouring out the melt in the plasma furnace and casting to obtain the calcium aluminate.
Example 19
49 wt.% aluminous clinker, 45 wt.% fly ash, 6 wt.% sodium carbonate and 20% CaO, 20% Ca (OH)2Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into a plasma furnace, heating to 1200 ℃, keeping the temperature for 44 minutes, heating to 1570 ℃, keeping the temperature for 27 minutes, pouring out the melt in the plasma furnace, and casting to obtain the calcium aluminate.
Example 20
Mixing 47 wt.% aluminous ash, 47 wt.% fly ash, 6 wt.% sodium carbonate and 15% CaO, 20% Ca (OH)2Mixing the materials (the weight ratio of the aluminum ash to the waste incineration fly ash), adding the mixture into a plasma furnace, heating to 1240 ℃, preserving heat for 26 minutes, then heating to 1530 ℃, preserving heat for 41 minutes, pouring out the melt in the plasma furnace, and casting to obtain the calcium aluminate.
While several embodiments of the present invention have been illustrated and described herein, it will be appreciated by those skilled in the art that changes can be made to the embodiments described herein without departing from the spirit of the invention. The above examples are merely illustrative and should not be taken as limiting the scope of the invention.
Claims (7)
1. A method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash in cooperation is characterized in that the aluminum ash, the waste incineration fly ash, a fluorine fixing agent and a denitrifier are mixed and uniformly mixed, and the mixture is heated in a heat treatment furnace for denitrogenation, melting and melt casting to obtain calcium aluminate; the aluminum ash comprises primary aluminum ash and secondary aluminum ash, an aluminum source is provided for preparing calcium aluminate, a calcium source is provided for waste incineration fly ash, a fluorine fixing agent realizes stable solidification of an element F in a mixture, a denitrifying agent increases the contact probability of AlN and air, and the heat treatment furnace is any one of an electric arc furnace, a medium frequency furnace, a resistance furnace and a gas furnace.
2. The method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash as raw materials according to claim 1, wherein the raw materials comprise 45-50 wt% of aluminum ash, 40-50 wt% of waste incineration fly ash, 5-15 wt% of denitrifier, and fluorine fixing agent which is 10-40% of the total weight of the aluminum ash and the waste incineration fly ash.
3. The method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash as claimed in claim 1, wherein the fluorine-fixing agent is one or more of quicklime, calcium carbonate and calcium hydroxide.
4. The method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash as claimed in claim 1, wherein the denitrifier is one or more of sodium carbonate, sodium hydroxide and borax.
5. The method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash as claimed in claim 1, wherein the specific method comprises:
s1, batching: mixing aluminum ash, waste incineration fly ash, a fluorine fixing agent and a denitrifying agent according to a certain proportion and uniformly mixing;
s2, heating for nitrogen removal: pouring the mixture into a heat treatment furnace, and utilizing high temperatureAnd the denitrifier converts AlN in the aluminous ash into Al2O3；
S3, melting: and (4) raising the temperature of the heat treatment furnace, preserving the heat for a period of time to obtain a melt, and casting to obtain the calcium aluminate.
6. The method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash as claimed in claim 5, wherein the heating and nitrogen removal temperature is 1000-1300 ℃ and the temperature is kept for 10-60 min.
7. The method for preparing calcium aluminate by using aluminum ash and waste incineration fly ash as claimed in claim 5, wherein the melting temperature is 1400-1600 ℃ and the temperature is kept for 20-120 min.
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