CN113144818A - Fly ash-based carbon dioxide absorption system and fly ash recycling method for absorbing carbon dioxide - Google Patents

Fly ash-based carbon dioxide absorption system and fly ash recycling method for absorbing carbon dioxide Download PDF

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CN113144818A
CN113144818A CN202110473359.0A CN202110473359A CN113144818A CN 113144818 A CN113144818 A CN 113144818A CN 202110473359 A CN202110473359 A CN 202110473359A CN 113144818 A CN113144818 A CN 113144818A
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carbon dioxide
molecular sieve
zeolite molecular
fly ash
sealing
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CN113144818B (en
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张峰
武全伟
孟庆宝
曲金星
尚宪猛
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Huadian Ningxia Lingwu Power Generation Co ltd
Huadian Electric Power Research Institute Co Ltd
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Huadian Ningxia Lingwu Power Generation Co ltd
Huadian Electric Power Research Institute Co Ltd
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    • B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
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    • B01D2259/00—Type of treatment
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  • Oil, Petroleum & Natural Gas (AREA)
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  • Silicates, Zeolites, And Molecular Sieves (AREA)
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Abstract

The invention provides a fly ash-based carbon dioxide absorption system, which comprises a carbon dioxide capturing device and a carbon dioxide sealing device; the carbon dioxide capture device comprises a hydrophobic zeolite molecular sieve absorption matrix obtained after fly ash treatment; the carbon dioxide sealing device comprises a filter residue sealing substrate obtained after fly ash treatment. According to the invention, through resource recycling in a power plant, the fly ash is taken as a matrix and is divided into two parts for comprehensive utilization, and meanwhile, a carbon dioxide capture device and a carbon dioxide sealing device are obtained and supplemented with each other for successive use, so that a set of complete fly ash-based carbon dioxide absorption system and a recycling method are formed. The invention realizes the preparation process of the hydrophobic zeolite molecular sieve high-strength material with the fly ash as the raw material; the disposal of the carbon dioxide is efficiently realized, the fly ash is simultaneously applied to the emission reduction and direct sealing of the carbon dioxide in the coal-fired power plant, and the problem of the stacking of the fly ash can be solved.

Description

Fly ash-based carbon dioxide absorption system and fly ash recycling method for absorbing carbon dioxide
Technical Field
The invention belongs to the technical field of carbon dioxide absorption by fly ash, relates to a fly ash-based carbon dioxide absorption system and a fly ash recycling method, and particularly relates to a fly ash-based carbon dioxide absorption system and a fly ash recycling method for absorbing carbon dioxide.
Background
Coal has an absolute leading role in national economic construction, and accounts for nearly 70% or even more of the total primary energy consumption of China for a long time. In China's coal consumption, 80% of coal is used as power coal and is directly used for combustion to generate heat energy and power. However, coal is a low-grade fossil fuel, and a large amount of pollutants such as sulfur oxides, nitrogen oxides and carbon dioxide exist in combustion flue gas of the coal. According to statistics, the CO and CO discharged by coal combustion in China2、SO2、 NOXAnd the proportion of dust to the total fuel combustion discharge amount is 71%, 85%, 90%, 70% and 70% in this order.
With the global warming becoming more serious, reducing the gas emission of the isothermal chamber such as carbon dioxide and protecting the environment become one of the global core problems to be solved at present. CO 22Is one of the main gases causing greenhouse effect and is a potential carbon resource, CO2It can be used as chemical raw material, refrigerant, oil field production increasing agent, inert medium, solvent and pressure source. Thus, various countries are working on reducing the carbon dioxide emissions from burning fossil fuels. The carbon dioxide emission reduction is realized through the processes of capture, transportation, sealing, application, conversion and the like, and the capture cost in the processes is about 75 percent or even higher. At present, most of CO from large emission sources2The concentration is less than 15%, however a small part (not)To 2%) CO from fossil fuel based industrial sources2Emission concentrations exceed 95%, so high concentration sources are potential targets for early implementation of carbon dioxide capture and sequestration technology (CCS). At present, the recovery of low concentration sources is also urgent, but the carbon dioxide capture material has the defects of poor recycling performance, toxicity, low capture efficiency, scarce raw materials and high energy consumption. Therefore, the development of a novel carbon capture material has become a focus of research.
The zeolite molecular sieve is natural or artificial crystalline aluminosilicate containing alkali metal or alkaline earth metal oxide, has strict structure and pores, and can separate substances with different molecular weights because the pore size is slightly changed due to the difference of the structure. The adsorption performance of zeolitic molecular sieve materials is largely dependent on two aspects: the porous structure and the large specific surface area of the porous structure can provide enough adsorption centers for adsorbates; secondly, the electrical property of the surface of the zeolite molecular sieve is that the zeolite molecular sieve formed by cations and a silicon-aluminum-oxygen framework with negative charges is a polar substance, and the surface of the zeolite molecular sieve has strong dispersion force and electrostatic force and shows strong affinity to polar (particularly water), unsaturated and easily polarized molecules. However, the adsorption of carbon dioxide by zeolites after absorbing water vapor is significantly reduced, which limits the use of zeolites for carbon dioxide capture. The gas discharged from the flue gas of coal-fired thermal power plant is mainly composed of about 5% -20% of water vapour and 10% -15% of carbon dioxide, so that the adsorption quantity of carbon dioxide is easily reduced by direct zeolite adsorption, and the conventional synthetic zeolite molecular sieve mainly utilizes Al (OH)3And the like, the price is high, and the scale production is not easy to form.
Therefore, how to obtain a hydrophobic zeolite with easy development and wide sources and provide a more economic and environmentally friendly recycling and absorption method has become a problem to be solved by many front-line researchers in the field.
Disclosure of Invention
In view of the above, the technical problem to be solved by the invention is to provide a fly ash-based carbon dioxide absorption system and a fly ash recycling method, the fly ash is used as a carbon dioxide absorption matrix in a power plant through resource recycling in the power plant, and capture and sealing of carbon dioxide can be realized, so that the fly ash-based carbon dioxide absorption system is applied to carbon dioxide emission reduction and direct sealing of carbon dioxide in the coal-fired power plant, the problem of stacking of fly ash can be solved, and the fly ash-based carbon dioxide absorption system is low in raw material price, simple in process and suitable for large-scale development and application.
The invention provides a fly ash-based carbon dioxide absorption system, which comprises a carbon dioxide capturing device and a carbon dioxide sealing device;
the carbon dioxide capture device comprises a hydrophobic zeolite molecular sieve absorption matrix obtained after fly ash treatment;
the carbon dioxide sealing device comprises a filter residue sealing substrate obtained after fly ash treatment.
Preferably, the hydrophobic zeolite molecular sieve absorption matrix comprises, by mass fraction of raw materials:
60-70 parts of a hydrophobically modified zeolite molecular sieve;
15-25 parts of Portland cement;
1-2 parts by weight of polyacrylamide;
water;
the mass ratio of the sum of the masses of the hydrophobically modified zeolite molecular sieve, the portland cement and the polyacrylamide to the water is 5: (1-2).
Preferably, the zeolite molecular sieve comprises one or more of 13X type zeolite molecular sieve, 10X type zeolite molecular sieve, Y type zeolite molecular sieve and A type zeolite molecular sieve;
the portland cement comprises type I portland cement and/or type I portland cement;
the filter residue sealing matrix contains metal oxide.
Preferably, the hydrophobically modified zeolite molecular sieve comprises SiO2A surface hydrophobically modified zeolite molecular sieve;
the metal oxide comprises CaO and Al2O3And MgO;
the filter residue sealing substrate is specifically a filter residue containing water.
Preferably, the zeolite molecular sieve and the filter residue are obtained synchronously after the fly ash is treated;
the specific process of the treatment is as follows:
and (3) performing iron removal pretreatment and alkali liquor treatment on the fly ash to obtain a filtrate and a solid mixture, crystallizing the filtrate to obtain the molecular sieve, wherein the solid mixture is filter residue.
Preferably, the fly ash-based carbon dioxide absorption system further comprises a carbon dioxide desorption device;
after the carbon dioxide is captured by the carbon dioxide capture device, the hydrophobic zeolite molecular sieve absorption matrix which captures the carbon dioxide is placed in a carbon dioxide desorption device, and the captured carbon dioxide is transferred to a carbon dioxide sequestration device.
The invention also provides a fly ash recycling method, which comprises the following steps:
1) performing iron removal pretreatment and alkali liquor treatment on the fly ash to obtain a filtrate and a solid mixture;
2) carrying out hydrothermal reaction crystallization on the mixture of the filtrate obtained in the step and aluminosilicate to obtain the zeolite molecular sieve, and then carrying out hydrothermal reaction on the zeolite molecular sieve and SiCl4Obtaining a hydrophobic modified zeolite molecular sieve after liquid phase deposition, and then solidifying the hydrophobic modified zeolite molecular sieve, portland cement, polyacrylamide and water to obtain a hydrophobic zeolite molecular sieve absorption matrix;
the solid mixture obtained in the step contains a certain amount of water, and the water is used as a filter residue sealing matrix;
3) placing the hydrophobic zeolite molecular sieve absorption matrix in a carbon dioxide capture device, and placing the filter residue sealing matrix in a carbon dioxide sealing device to respectively obtain the carbon dioxide capture device containing the hydrophobic zeolite molecular sieve absorption matrix and the carbon dioxide sealing device containing the filter residue sealing matrix;
4) and (2) capturing carbon dioxide in flue tail gas by the carbon dioxide capturing device containing the hydrophobic zeolite molecular sieve absorption matrix obtained in the step, then placing the hydrophobic zeolite molecular sieve absorption matrix capturing the carbon dioxide in a carbon dioxide desorption device, desorbing the captured carbon dioxide by hot steam, and then sending the carbon dioxide into a carbon dioxide sequestration device containing a filter residue sequestration matrix for sequestration.
Preferably, the iron removal pretreatment comprises magnetic separation iron removal and/or acid liquor iron removal;
the acid solution comprises one or more of hydrochloric acid solution, sulfuric acid solution and nitric acid solution;
the concentration of the acid liquor is 2-4 mol.L-1；
The temperature for removing iron in the acid liquor is 60-70 ℃;
the time for removing iron from the acid liquor is 5-6 hours;
the alkali liquor comprises a sodium hydroxide solution and/or a potassium hydroxide solution;
the alkali liquor treatment is a hydrothermal reaction;
the temperature of the alkali liquor treatment is 90-100 ℃;
the alkali liquor treatment time is 48-96 h.
Preferably, the aluminosilicates include soluble silicates and soluble aluminates;
the molar ratio of Si to Al in the mixture of the filtrate and the silicon-aluminum salt is 2.2-3.3;
the temperature of the hydrothermal reaction in the step 2) is 90-100 ℃;
the time of the hydrothermal reaction in the step 2) is 6-8 h;
the liquid phase deposition comprises the following specific steps:
zeolite molecular sieve and SiCl4Mixing with solvent, and roasting;
the zeolite molecular sieve and SiCl4The mass ratio of (1): (0.2 to 0.5);
the mass ratio of the zeolite molecular sieve to the solvent is 1: (3-5);
the mixing time is 5-6 h;
the roasting temperature is 400-500 ℃.
Preferably, the curing is normal-temperature curing;
the curing time is 12-24 h;
the flue comprises a flue of a coal-fired thermal power plant;
the desorption temperature is 30-50 ℃;
the desorption pressure is 300-400 MPa;
the sealing temperature is 40-80 ℃;
the partial pressure of the sealed carbon dioxide is 1-3 MPa;
and the liquid-solid ratio of the filter residue sealing matrix is 0.1-1.
The invention provides a fly ash-based carbon dioxide absorption system, which comprises a carbon dioxide capturing device and a carbon dioxide sealing device; the carbon dioxide capture device comprises a hydrophobic zeolite molecular sieve absorption matrix obtained after fly ash treatment; the carbon dioxide sealing device comprises a filter residue sealing substrate obtained after fly ash treatment. Compared with the prior art, the invention aims at the problem of the existing carbon dioxide absorption, the adsorption of the zeolite to the carbon dioxide is obviously reduced after the zeolite absorbs water vapor, and the application of the zeolite to the carbon dioxide capture in the flue gas of the coal-fired thermal power plant is further limited. The conventional synthetic zeolite molecular sieve is expensive and is not easy to form mass production and the like.
The research of the invention proves that the fly ash can not only provide a large amount of SiO for the artificial synthetic zeolite material2And Al2O3The source can also provide CaO and MgO for the mineralization and sealing of the carbon dioxide, so that the fly ash waste is recycled comprehensively to obtain a high value-added product, and the strategic requirements of the development of the circular economy can be met. The invention creatively obtains a fly ash-based carbon dioxide absorption system, utilizes the resource recycling in a power plant, takes fly ash as a matrix, divides the fly ash into two parts for comprehensive utilization, and simultaneously obtains a carbon dioxide capture device and a carbon dioxide sealing device which are complementary and are used in succession, thereby forming a set of complete fly ash-based carbon dioxide absorption system and recycling method. The invention realizes the preparation process of the hydrophobic zeolite molecular sieve high-strength material with the fly ash as the raw material; and effectively realizes the disposal of carbon dioxide step by step and the disposal of fly ashThe method is applied to the emission reduction of carbon dioxide and the direct sealing of carbon dioxide in coal-fired power plants, and can also solve the problem of the stacking of fly ash. The invention utilizes the solid waste to prepare the energy storage material for energy recovery, realizes the recovery and utilization of resources and energy, has cheap raw materials, simple process and mild conditions, and is suitable for the development and application of industrial scale.
Experimental results show that the hydrophobic zeolite molecular sieve in the carbon dioxide capture device provided by the invention has good CO2The adsorption capacity can be 2.0-4.0 mmol/g, carbon dioxide can be sealed in filter residue obtained by alkali infiltration and separation of fly ash, the carbonation efficiency can be 40-80%, and CO can be obtained2The sealing capacity is 100-300 g/kg.
Drawings
FIG. 1 is a schematic flow chart of a fly ash recycling method provided by the invention.
Detailed Description
For a further understanding of the invention, preferred embodiments of the invention are described below in conjunction with the examples, but it should be understood that these descriptions are included merely to further illustrate the features and advantages of the invention and are not intended to limit the invention to the claims.
All of the starting materials of the present invention, without particular limitation as to their source, may be purchased commercially or prepared according to conventional methods well known to those skilled in the art.
All the raw materials of the present invention are not particularly limited in purity, and the present invention preferably employs analytically pure or purity conventional in the art of carbon dioxide absorbing material preparation.
The invention provides a fly ash-based carbon dioxide absorption system, which comprises a carbon dioxide capturing device and a carbon dioxide sealing device;
the carbon dioxide capture device comprises a hydrophobic zeolite molecular sieve absorption matrix obtained after fly ash treatment;
the carbon dioxide sealing device comprises a filter residue sealing substrate obtained after fly ash treatment.
The carbon dioxide capture device comprises a hydrophobic zeolite molecular sieve absorption matrix obtained after fly ash treatment.
The invention is not particularly limited to the specific composition of the hydrophobic zeolite molecular sieve absorption matrix in principle, and a person skilled in the art can select and adjust the matrix according to the actual application situation, the raw material situation and the product requirement, in order to better realize the capture and the sealing of carbon dioxide, improve the capture and the sealing effects and realize the recycling of resources and energy, the hydrophobic zeolite molecular sieve absorption matrix preferably comprises the following components in percentage by mass:
60-70 parts of a hydrophobically modified zeolite molecular sieve;
15-25 parts of Portland cement;
1-2 parts by weight of polyacrylamide;
water;
the mass ratio of the sum of the masses of the hydrophobically modified zeolite molecular sieve, the portland cement and the polyacrylamide to the water is 5: (1-2).
More specifically, the amount of the hydrophobically modified zeolite molecular sieve is preferably 60 to 70 parts by weight, more preferably 62 to 68 parts by weight, and even more preferably 64 to 66 parts by weight. The amount of the portland cement is preferably 15 to 25 parts by weight, more preferably 17 to 23 parts by weight, and still more preferably 19 to 21 parts by weight. The amount of the polyacrylamide is preferably 1 to 2 parts by weight, more preferably 1.2 to 1.8 parts by weight, and still more preferably 1.4 to 1.6 parts by weight. The mass ratio of the sum of the masses of the hydrophobically modified zeolite molecular sieve, the portland cement and the polyacrylamide to the water is preferably 5: (1-2), more preferably 5: (1.2 to 1.8), more preferably 5: (1.4-1.6).
The specific selection of the zeolite molecular sieve is not particularly limited in principle, and can be selected and adjusted by those skilled in the art according to the actual application situation, the raw material situation and the product requirement, and in order to better achieve the capture and sequestration of carbon dioxide, improve the capture and sequestration effects and achieve the recycling of resources and energy, the zeolite molecular sieve preferably comprises one or more of 13X type zeolite molecular sieve, 10X type zeolite molecular sieve, Y type zeolite molecular sieve and a type zeolite molecular sieve, and more preferably 13X type zeolite molecular sieve, 10X type zeolite molecular sieve, Y type zeolite molecular sieve or a type zeolite molecular sieve.
The concrete selection of the portland cement is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application situation, the raw material situation and the product requirement.
According to the invention, polyacrylamide is added into the hydrophobic zeolite molecular sieve absorption matrix, so that the strength, compression and fracture resistance of the matrix material can be enhanced, and the matrix material can be used as a matrix reinforcing agent.
The specific selection of the hydrophobically modified zeolite molecular sieve is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application condition, the raw material condition and the product requirement2A surface hydrophobically modified zeolite molecular sieve.
The carbon dioxide sealing device comprises a filter residue sealing substrate obtained after fly ash treatment.
The invention has no special limitation on the components in the filter residue obtained after the fly ash is treated in principle, and a person skilled in the art can select and adjust the components according to the actual application condition, the raw material condition and the product requirement2O3And one of MgOOr more, more preferably CaO or Al2O3And MgO.
The shape of the filter residue in the filter residue sealing matrix is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application condition, the raw material condition and the product requirement.
The water content of the filter residue in the filter residue sealing matrix is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements.
The invention has no special limitation on how to obtain the hydrophobic zeolite molecular sieve absorption matrix and the filter residue sealing matrix in principle, namely, the treatment mode of how to obtain the zeolite molecular sieve and the filter residue is not particularly limited, and a person skilled in the art can select and adjust the treatment mode according to the actual application condition, the raw material condition and the product requirement.
The specific process of the treatment is preferably as follows:
and (3) performing iron removal pretreatment and alkali liquor treatment on the fly ash to obtain a filtrate and a solid mixture, crystallizing the filtrate to obtain the molecular sieve, wherein the solid mixture is filter residue.
The invention is a complete and refined integral recycling method, better realizes the capture and sealing of carbon dioxide, improves the capture and sealing effects, realizes the recycling of resources and energy, and preferably adopts a carbon dioxide desorption device;
more specifically, after the carbon dioxide is captured by the carbon dioxide capturing device, the hydrophobic zeolite molecular sieve absorbing matrix in which the carbon dioxide is captured is placed in a carbon dioxide desorption device, and the captured carbon dioxide is transferred to a carbon dioxide sequestration device.
The invention also provides a fly ash recycling method, which comprises the following steps:
1) performing iron removal pretreatment and alkali liquor treatment on the fly ash to obtain a filtrate and a solid mixture;
2) carrying out hydrothermal reaction crystallization on the mixture of the filtrate obtained in the step and aluminosilicate to obtain the zeolite molecular sieve, and then carrying out hydrothermal reaction on the zeolite molecular sieve and SiCl4Obtaining a hydrophobic modified zeolite molecular sieve after liquid phase deposition, and then solidifying the hydrophobic modified zeolite molecular sieve, portland cement, polyacrylamide and water to obtain a hydrophobic zeolite molecular sieve absorption matrix;
the solid mixture obtained in the step contains a certain amount of water, and the water is used as a filter residue sealing matrix;
3) placing the hydrophobic zeolite molecular sieve absorption matrix in a carbon dioxide capture device, and placing the filter residue sealing matrix in a carbon dioxide sealing device to respectively obtain the carbon dioxide capture device containing the hydrophobic zeolite molecular sieve absorption matrix and the carbon dioxide sealing device containing the filter residue sealing matrix;
4) and (2) capturing carbon dioxide in flue tail gas by the carbon dioxide capturing device containing the hydrophobic zeolite molecular sieve absorption matrix obtained in the step, then placing the hydrophobic zeolite molecular sieve absorption matrix capturing the carbon dioxide in a carbon dioxide desorption device, desorbing the captured carbon dioxide by hot steam, and then sending the carbon dioxide into a carbon dioxide sequestration device containing a filter residue sequestration matrix for sequestration.
In the method for recycling fly ash, the selection of materials, the parameter range and the corresponding preferred principle, if not specifically noted, may correspond to the selection of materials, the parameter range and the corresponding preferred principle for the fly ash-based carbon dioxide absorption system, and are not described in detail herein.
Firstly, the fly ash is subjected to iron removal pretreatment and alkali liquor treatment to obtain a filtrate and solid mixture.
The specific process of the iron removal pretreatment is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application situation, the raw material situation and the product requirement.
The specific selection of the acid solution is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application situation, the raw material situation and the product requirement.
The concentration of the acid liquor is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, in order to better capture and seal carbon dioxide, improve the capture and seal effects and recycle resources and energy, the concentration of the acid liquor is preferably 2-4 mol · L-1More preferably 2.4 to 3.6 mol.L-1More preferably 2.8 to 3.2 mol.L-1。
The temperature for removing iron from the acid liquor is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, so that the method can better capture and seal carbon dioxide, improve the capture and seal effects and recycle resources and energy, and the temperature for removing iron from the acid liquor is preferably 60-70 ℃, more preferably 62-68 ℃, and more preferably 64-66 ℃.
The time for removing iron from the acid liquor is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application condition, the raw material condition and the product requirement, in order to better capture and seal carbon dioxide, improve the capture and seal effects and recycle resources and energy, the time for removing iron from the acid liquor is preferably 5-6 hours, more preferably 5.2-5.8 hours, and more preferably 5.4-5.6 hours.
The invention is a complete and refined integral recycling process, better realizes the capture and the sealing of carbon dioxide at the same time, improves the capture and the sealing effects, realizes the recycling of resources and energy, and the concrete step of the iron removal pretreatment can be as follows:
firstly, carrying out magnetic separation and iron removal on fly ash in a power plant, and then mixing the fly ash with 2-4 mol.L-1The mass volume ratio of the hydrochloric acid aqueous solution is 1: (3-4) (more preferably 1 (3.2-3.8), more preferably 1 (3.4-3.6)) and reacting at 60-70 ℃ for 5-6 h to remove active metal impurities.
The specific selection of the alkali liquor is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application situation, the raw material situation and the product requirement.
The specific process of the alkali liquor treatment is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application condition, the raw material condition and the product requirement.
The temperature of the alkali liquor treatment is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, the carbon dioxide is captured and sequestered at the same time, the capturing and sequestering effects are improved, and the recycling of resources and energy sources is realized, wherein the temperature of the alkali liquor treatment is preferably 90-100 ℃, more preferably 92-98 ℃, and more preferably 94-96 ℃.
The time for treating the alkali liquor is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application situation, the raw material situation and the product requirement, in order to better capture and seal carbon dioxide, improve the capture and seal effects and recycle resources and energy, the time for treating the alkali liquor is preferably 48-96 hours, more preferably 58-86 hours, and more preferably 68-76 hours.
The invention then carries out hydrothermal reaction crystallization on the mixture of the filtrate obtained in the step and aluminosilicate to obtain the zeolite molecular sieve, and then carries out hydrothermal reaction on the zeolite molecular sieve and SiCl4Obtaining a hydrophobic modified zeolite molecular sieve after liquid phase deposition, and then solidifying the hydrophobic modified zeolite molecular sieve, portland cement, polyacrylamide and water to obtain a hydrophobic zeolite molecular sieve absorption matrix;
the solid mixture obtained in the above step contains a certain amount of water, and is used as a filter residue sealing matrix.
The specific components of the aluminosilicate are not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application situation, the raw material situation and the product requirement.
The invention has no particular limitation on the molar ratio of Si to Al in the mixture of the filtrate and the sodium aluminum salt in principle, and a person skilled in the art can select and adjust the molar ratio according to the actual application situation, the raw material situation and the product requirement, in order to better realize the capture and the sealing of carbon dioxide, improve the effects of the capture and the sealing and realize the recycling of resources and energy, the molar ratio of Si to Al in the mixture of the filtrate and the silicon aluminum salt is preferably 2.2-3.3, more preferably 2.4-3.1, and more preferably 2.6-2.9.
The temperature of the hydrothermal reaction in the step 2) is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, in order to better realize the capture and the sealing of carbon dioxide, improve the capture and the sealing effects and realize the recycling of resources and energy, the temperature of the hydrothermal reaction in the step 2) is preferably 90-100 ℃, more preferably 92-98 ℃, and more preferably 94-96 ℃.
The time of the hydrothermal reaction in the step 2) is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application situation, the raw material situation and the product requirement, in order to better realize the capture and the sealing of carbon dioxide, improve the capture and the sealing effects and realize the recycling of resources and energy, the time of the hydrothermal reaction in the step 2) is preferably 6-8 hours, more preferably 6.4-7.6 hours, and more preferably 6.8-7.2 hours.
The invention is a complete and refined integral recycling method, better realizes the capture and the sealing of carbon dioxide at the same time, improves the capture and the sealing effects, realizes the recycling of resources and energy, and the specific steps of the liquid phase deposition are preferably as follows:
zeolite molecular sieve and SiCl4Mixing with solvent, and calcining.
More preferably: cyclohexane is used as a solvent, SiCl is added4Liquid, zeolite molecular sieve weight: SiCl4Weight: cyclohexane weight 1: (0.2-0.5): (3-5), capping, oscillating for 5-6 h, drying, and 40Roasting at 0-500 deg.c to the original zeolite state.
The invention is in principle directed to said zeolitic molecular sieves and SiCl4The mass ratio of the zeolite molecular sieve and SiCl is not particularly limited, and can be selected and adjusted by a person skilled in the art according to the actual application condition, the raw material condition and the product requirement4Is preferably 1: (0.2 to 0.5), more preferably 1: (0.25 to 0.45), more preferably 1: (0.3-0.4).
In the invention, the mass ratio of the zeolite molecular sieve to the solvent is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to the actual application situation, the raw material situation and the product requirement, in order to better realize the capture and the sequestration of carbon dioxide, improve the capture and the sequestration effects and realize the recycling of resources and energy, the mass ratio of the zeolite molecular sieve to the solvent is preferably 1: (3-5), more preferably 1: (3.4 to 4.6), more preferably 1: (3.8-4.2).
The mixing time is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, in order to better capture and seal carbon dioxide, improve the capture and seal effects and recycle resources and energy, the mixing time is preferably 5-6 hours, more preferably 5.2-5.8 hours, and more preferably 5.4-5.6 hours.
The roasting temperature is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, the carbon dioxide is better captured and sealed, the capturing and sealing effects are improved, and the recycling of resources and energy sources is realized, wherein the roasting temperature is preferably 400-500 ℃, more preferably 420-480 ℃, and more preferably 440-460 ℃.
The curing process is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, so that the carbon dioxide can be captured and sealed better, the capturing and sealing effects are improved, and the recycling of resources and energy sources is realized, wherein the curing is preferably normal-temperature curing, and can be 5-40 ℃, or 10-35 ℃, or 15-30 ℃, or 20-25 ℃.
The curing time is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, the carbon dioxide capture and sequestration are better realized, the capture and sequestration effects are improved, the recycling of resources and energy sources is realized, the curing time is preferably 12-24 hours, more preferably 14-22 hours, and more preferably 16-20 hours
In the invention, the solid mixture contains a certain amount of water and is used as a filter residue sealing matrix. That is, the inside also contains alkali, and the alkali is soaked. The invention has no special limitation on the source and proportion of water in the filter residue sealing matrix (solid mixture) in principle, and a person skilled in the art can select and adjust the water according to the actual application condition, the raw material condition and the product requirement. The liquid-solid ratio of the filter residue sealing matrix, namely a certain amount of water contained in the solid mixture, is preferably 0.1-1, more preferably 0.3-0.8, and more preferably 0.5-0.7.
According to the invention, the hydrophobic zeolite molecular sieve absorption matrix is placed in a carbon dioxide capture device, and the filter residue sealing matrix is placed in a carbon dioxide sealing device, so that the carbon dioxide capture device containing the hydrophobic zeolite molecular sieve absorption matrix and the carbon dioxide sealing device containing the filter residue sealing matrix are respectively obtained.
Finally, the carbon dioxide capturing device containing the hydrophobic zeolite molecular sieve absorption matrix obtained in the step captures carbon dioxide in flue tail gas, then the hydrophobic zeolite molecular sieve absorption matrix capturing the carbon dioxide is placed in a carbon dioxide desorption device, and the captured carbon dioxide is desorbed through hot steam and then sent into a carbon dioxide sealing device containing a filter residue sealing matrix for sealing.
The invention is not particularly limited to the specific selection of the flue in principle, and the skilled person can select and adjust the flue according to the actual application situation, the raw material situation and the product requirement.
The desorption temperature is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, the carbon dioxide is better captured and sequestered, the capturing and sequestering effects are improved, and the recycling of resources and energy sources is realized, wherein the desorption temperature is preferably 30-50 ℃, more preferably 34-46 ℃, and more preferably 38-42 ℃.
The desorption pressure is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, the carbon dioxide is better captured and sequestered, the capturing and sequestering effects are improved, the recycling of resources and energy is realized, and the desorption pressure is preferably 300-400 MPa, more preferably 320-380 MPa, and more preferably 340-360 MPa.
The temperature for sealing is not particularly limited in principle, and can be selected and adjusted by a person skilled in the art according to actual application conditions, raw material conditions and product requirements, the carbon dioxide is captured and sealed better, the capturing and sealing effects are improved, and the recycling of resources and energy sources is realized, wherein the temperature for sealing is preferably 40-80 ℃, more preferably 45-75 ℃, more preferably 50-70 ℃, and more preferably 55-65 ℃.
The invention has no particular limitation on the pressure of the partial pressure of the sequestered carbon dioxide in principle, and a person skilled in the art can select and adjust the partial pressure according to the actual application condition, the raw material condition and the product requirement, in order to better realize the capture and sequestration of the carbon dioxide at the same time, improve the effects of the capture and sequestration and realize the recycling of resources and energy, the partial pressure of the sequestered carbon dioxide is preferably 1-3 MPa, more preferably 1.4-2.6 MPa, and more preferably 1.8-2.2 MPa.
The invention is a complete and refined integral recycling method, which better realizes the capture and sealing of carbon dioxide at the same time, improves the capture and sealing effects, and realizes the recycling of resources and energy, and the specific steps of the fly ash recycling method can be as follows:
firstly, carrying out iron removal pretreatment on the fly ash to remove iron oxide components in the fly ash, then mixing the fly ash and a NaOH solution according to a certain proportion, carrying out hydrothermal reaction for a period of time, and filtering and separating reactants to obtain a filtrate and solid mixture.
The filtrate is a silicon-rich solution, which is used as a raw material of the carbon dioxide capture material. Testing Si in solution with spectrophotometer4+And (3) adding sodium aluminum salt into the mixture according to the concentration, adjusting the amount ratio of Si/Al substances to be 2.2-3.3, continuing hydrothermal reaction and crystallization, and filtering, washing and drying after the hydrothermal reaction is finished to obtain the 13X-type zeolite molecular sieve. By SiCl4Chemical liquid deposition of SiCl4Enters the zeolite pore canal and reacts with the hydroxyl on the inner surface to generate SiO2The coating covers Al-OH, Si-OH and other hydrophilic centers on the surface of the zeolite, so that the surface of the zeolite is hydrophobized. Then the zeolite molecular sieve, Portland cement, polyacrylamide and water are placed in a mould, and solidified to obtain the high-strength hydrophobic zeolite solid block which is placed in a capturing device.
And the solid mixture is used as a raw material for directly mineralizing and storing the carbon dioxide. Soaking the solid mixture in water, and placing in a sealing device as filler.
Referring to fig. 1, fig. 1 is a schematic flow chart of a fly ash recycling method provided by the invention.
The fly ash-based carbon dioxide absorption system and the fly ash recycling method for absorbing carbon dioxide are provided by the steps of the invention, the fly ash is taken as a matrix and is divided into two parts for comprehensive utilization through resource recycling in a power plant, and the carbon dioxide capture device and the carbon dioxide sequestration device are obtained and supplemented with each other for successive use, so that a set of complete fly ash-based carbon dioxide absorption system and recycling method are formed.
The preparation method takes the fly ash as a matrix, and realizes the preparation process of the hydrophobic zeolite molecular sieve high-strength material taking the fly ash as a raw material; the disposal of the carbon dioxide is realized step by step and efficiently, the coal ash is simultaneously applied to the emission reduction of the carbon dioxide in a coal-fired power plant and the direct sealing of the carbon dioxide, and the problem of the stacking of the coal ash can be solved. When the high-strength zeolite solid block absorbs carbon dioxide in a flue of a coal-fired thermal power plant, the waste heat of the electric power plant is used for desorbing the capture material in the desorption device, and then the capture material enters the sealing device for sealing, so that the processes of transportation and storage between the two steps of capture and sealing are saved, and the high utilization of resources and energy is realized. The invention utilizes the solid waste to prepare the energy storage material for energy recovery, realizes the recovery and utilization of resources and energy, has cheap raw materials, simple process and mild conditions, and is suitable for the development and application of industrial scale.
Experimental results show that the hydrophobic zeolite molecular sieve in the carbon dioxide capture device provided by the invention has good CO2The adsorption capacity can be 2.0-4.0 mmol/g, carbon dioxide can be sealed in filter residue obtained by alkali infiltration and separation of fly ash, the carbonation efficiency can be 40-80%, and CO can be obtained2The sealing capacity is 100-300 g/kg.
To further illustrate the present invention, a fly ash-based carbon dioxide absorbing system and a fly ash recycling method according to the present invention are described in detail with reference to the following examples, but it should be understood that the examples are implemented on the premise of the technical solution of the present invention, and the detailed embodiments and specific operation procedures are given only for further illustrating the features and advantages of the present invention, not for limiting the claims of the present invention, and the scope of the present invention is not limited to the following examples.
Example 1
Firstly, the fly ash of a power plant is subjected to iron removal pretreatment, and the fly ash and 2 mol.L are mixed-1The mass volume ratio of the hydrochloric acid aqueous solution is 1: 3.2, mixing, reacting for 6 hours at the temperature of 60-70 ℃, and removing active metal impurities. Then mixing the fly ash with 2mol/L NaOH solution, reacting for 6h at 90 ℃, and filtering and separating the reactant to obtain a filtrate and solid mixture. The filtrate is a silicon-rich solution which is used as a raw material of the zeolite molecular sieve. Testing Si in solution with spectrophotometer4+Adding sodium aluminosilicate into the mixture, adjusting the amount ratio of Si/Al substances to 2.8, continuing hydrothermal reaction and crystallization at the crystallization temperature of 90 ℃ for 2d, filtering, washing and drying to obtain the 13X-type zeolite molecular sieve. Cyclohexane is used as a solvent, SiCl is added4Liquid, zeolite molecular sieve weight: SiCl4Weight: cyclohexane weight 1: 0.5: and 5, covering the cover, oscillating for 6 hours, drying, and roasting at 400 ℃ until the zeolite is originally the same. Then 60 parts by weight of zeolite molecular sieve, 20 parts by weight of Portland cement, 1 part by weight of polyacrylamide and water accounting for 0.35 part by weight of the solid materials are mixed and placed in a mold, and the mixture is cured for 24 hours at room temperature. Preparing the hydrophobic 13X type zeolite molecular sieve.
The performance test of the hydrophobic 13X-type zeolite molecular sieve prepared in the embodiment 1 of the invention shows that CO is available2The adsorption capacity may be 2.4 mmol/g.
And (3) measuring the liquid-solid ratio of the solid mixture obtained in the step to be 0.2, and taking the solid mixture as a filter residue sealing matrix to a carbon dioxide sealing device.
And (3) taking the hydrophobic 13X-type zeolite molecular sieve obtained in the step as a hydrophobic zeolite molecular sieve absorption matrix, and taking the hydrophobic 13X-type zeolite molecular sieve as a solid filler to be placed in an absorption tower to a carbon dioxide capture device.
Flue gas of a coal-fired thermal power plant containing high-concentration carbon dioxide enters an absorption tower, the carbon dioxide is absorbed by a carbon dioxide capturing device, and the rest tail gas is discharged or enters a tail gas treatment device. And (5) operating for a period of time, and saturating the carbon dioxide concentration of the packing in the absorption tower. And transferring the carbon dioxide adsorbed solid filler into a desorption tower, and desorbing under the working condition of 300MPa by using hot steam at 50 ℃. And introducing the desorbed gas into a carbon dioxide sealing device containing a filter residue sealing matrix, and sealing at 40 ℃ under the partial pressure of 1MPa of carbon dioxide.
The performance of the capturing, desorbing and sealing processes of the invention is tested.
The results show that the filter residue obtained by the alkali infiltration and separation of the fly ash can store carbon dioxide, the carbonation efficiency can be 50 percent, and the CO content can be increased2The sealing capacity was 180 g/kg.
Example 2
Firstly, the fly ash of a power plant is subjected to iron removal pretreatment, and the fly ash and 4 mol.L are mixed-1The mass volume ratio of the hydrochloric acid aqueous solution is 1: 3.2, mixing, reacting for 6 hours at the temperature of 60-70 ℃, and removing active metal impurities. Then mixing the fly ash with 2mol/L NaOH solution, reacting for 10h at 90 ℃, and filtering and separating the reactant to obtain a filtrate and solid mixture. The filtrate is a silicon-rich solution which is used as a raw material of the zeolite molecular sieve. Testing Si in solution with spectrophotometer4+Adding sodium aluminum salt into the mixture, adjusting the amount ratio of Si/Al substances to 3.0, continuing hydrothermal reaction and crystallization at the crystallization temperature of 100 ℃ for 2d, filtering, washing and drying to obtain the 13X-type zeolite molecular sieve. Cyclohexane is used as a solvent, SiCl is added4Liquid, zeolite molecular sieve weight: SiCl4Weight: cyclohexane weight 1: 0.5: and 5, covering the cover, oscillating for 6 hours, drying, and roasting at 500 ℃ until the zeolite is originally the same. Then 60 parts by weight of zeolite molecular sieve, 20 parts by weight of Portland cement, 2 parts by weight of polyacrylamide and water accounting for 0.35 part by weight of the solid materials are mixed and placed in a mold for solidification. Preparing the hydrophobic Y-type zeolite molecular sieve.
The performance test of the hydrophobic Y-type zeolite molecular sieve prepared in the embodiment 2 of the invention shows that CO has high molecular weight and high molecular weight2The adsorption capacity may be 2.2 mmol/g.
And (3) measuring the liquid-solid ratio of the solid mixture obtained in the step to be 0.1, and taking the solid mixture as a filter residue sealing matrix to a carbon dioxide sealing device.
And (3) taking the hydrophobic 13X-type zeolite molecular sieve obtained in the step as a hydrophobic zeolite molecular sieve absorption matrix and as a solid filler to be placed in an absorption tower to obtain the carbon dioxide capture device.
Flue gas of a coal-fired thermal power plant containing high-concentration carbon dioxide enters an absorption tower, the carbon dioxide is absorbed by a carbon dioxide capturing device, and the rest tail gas is discharged or enters a tail gas treatment device. And (5) operating for a period of time, and saturating the carbon dioxide concentration of the packing in the absorption tower. And transferring the carbon dioxide adsorbed solid filler into a desorption tower, and desorbing under the working condition of 300MPa by using hot steam at 50 ℃. And introducing the desorbed gas into a carbon dioxide sealing device containing a filter residue sealing matrix, and sealing at 40 ℃ under the partial pressure of 1MPa of carbon dioxide.
The performance of the capturing, desorbing and sealing processes of the invention is tested.
The results show that the filter residue obtained by the alkali infiltration and separation of the fly ash can store carbon dioxide, the carbonation efficiency can be 62 percent, and the CO content can be increased2The sealing capacity was 210 g/kg.
Example 3
Firstly, the fly ash of a power plant is subjected to iron removal pretreatment, and the fly ash and 3 mol.L are mixed-1The mass volume ratio of the hydrochloric acid aqueous solution is 1: 3.2, mixing, reacting for 6 hours at the temperature of 60-70 ℃, and removing active metal impurities. Then mixing the fly ash with 2mol/L NaOH solution, reacting for 9h at the hydrothermal reaction temperature of 90 ℃, and filtering and separating the reactant to obtain a filtrate and solid mixture. The filtrate is a silicon-rich solution which is used as a raw material of the zeolite molecular sieve. Testing Si in solution with spectrophotometer4+Adding sodium aluminum salt into the mixture, adjusting the amount ratio of Si/Al substances to 3.0, continuing hydrothermal reaction and crystallization at the crystallization temperature of 100 ℃ for 2d, filtering, washing and drying to obtain the 13X-type zeolite molecular sieve. Cyclohexane is used as a solvent, SiCl is added4Liquid, zeolite molecular sieve weight: SiCl4Weight: cyclohexane weight 1: 0.5: and 5, covering the cover, oscillating for 6 hours, drying, and roasting at 500 ℃ until the zeolite is originally the same. Then 60 parts by weight of zeolite molecular sieve, 20 parts by weight of Portland cement, 1 part of polyacrylamide, andmixing water accounting for 0.35 mass of the solid material, filling the mixture into a mold, and curing. Preparing the hydrophobic Y-type zeolite molecular sieve.
The performance test of the hydrophobic Y-type zeolite molecular sieve prepared in the embodiment 3 of the invention shows that CO has high molecular weight and high molecular weight2The adsorption capacity may be 2.6 mmol/g.
And (3) measuring the liquid-solid ratio of the solid mixture obtained in the step to be 0.2, and taking the solid mixture as a filter residue sealing matrix to a carbon dioxide sealing device.
And (3) taking the hydrophobic 13X-type zeolite molecular sieve obtained in the step as a hydrophobic zeolite molecular sieve absorption matrix and as a solid filler to be placed in an absorption tower to obtain the carbon dioxide capture device.
Flue gas of a coal-fired thermal power plant containing high-concentration carbon dioxide enters an absorption tower, the carbon dioxide is absorbed by a carbon dioxide capturing device, and the rest tail gas is discharged or enters a tail gas treatment device. And (5) operating for a period of time, and saturating the carbon dioxide concentration of the packing in the absorption tower. And transferring the carbon dioxide adsorbed solid filler into a desorption tower, and desorbing under the working condition of 300MPa by using hot steam at 50 ℃. And introducing the desorbed gas into a carbon dioxide sealing device containing a filter residue sealing matrix, and sealing at 40 ℃ under the partial pressure of 1MPa of carbon dioxide.
The performance of the capturing, desorbing and sealing processes of the invention is tested.
The results show that the filter residue obtained by the alkali infiltration and separation of the fly ash can store carbon dioxide, the carbonation efficiency can be 68 percent, and the CO content can be increased2The sealing capacity was 250 g/kg.
While the present invention has been described in detail with respect to a fly ash-based carbon dioxide absorption system and a fly ash recycling method for absorbing carbon dioxide, the principles and embodiments of the present invention are described herein using specific examples, which are set forth only to facilitate an understanding of the methods and their core concepts, including the best mode, and to enable any person skilled in the art to practice the invention, including making and using any devices or systems and performing any incorporated methods. It should be noted that, for those skilled in the art, it is possible to make various improvements and modifications to the present invention without departing from the principle of the present invention, and those improvements and modifications also fall within the scope of the claims of the present invention. The scope of the invention is defined by the claims and may include other embodiments that occur to those skilled in the art. Such other embodiments are intended to be within the scope of the claims if they have structural elements that do not differ from the literal language of the claims, or if they include equivalent structural elements with insubstantial differences from the literal languages of the claims.

Claims (10)

1. A fly ash-based carbon dioxide absorption system is characterized by comprising a carbon dioxide capture device and a carbon dioxide sequestration device;
the carbon dioxide capture device comprises a hydrophobic zeolite molecular sieve absorption matrix obtained after fly ash treatment;
the carbon dioxide sealing device comprises a filter residue sealing substrate obtained after fly ash treatment.
2. The fly ash-based carbon dioxide absorption system according to claim 1, wherein the hydrophobic zeolite molecular sieve absorption matrix comprises, in terms of raw material mass fraction:
60-70 parts of a hydrophobically modified zeolite molecular sieve;
15-25 parts of Portland cement;
1-2 parts by weight of polyacrylamide;
water;
the mass ratio of the sum of the masses of the hydrophobically modified zeolite molecular sieve, the portland cement and the polyacrylamide to the water is 5: (1-2).
3. The fly ash-based carbon dioxide absorption system of claim 2, wherein the zeolite molecular sieve comprises one or more of a 13X type zeolite molecular sieve, a 10X type zeolite molecular sieve, a Y type zeolite molecular sieve, and an a type zeolite molecular sieve;
the portland cement comprises type I portland cement and/or type I portland cement;
the filter residue sealing matrix contains metal oxide.
4. The fly ash-based carbon dioxide absorbing system of claim 3, wherein the hydrophobically modified zeolite molecular sieve comprises SiO2A surface hydrophobically modified zeolite molecular sieve;
the metal oxide comprises CaO and Al2O3And MgO;
the filter residue sealing substrate is specifically a filter residue containing water.
5. The fly ash-based carbon dioxide absorption system according to claim 2, wherein the zeolite molecular sieve and the filter residue are obtained by treating fly ash and then synchronously;
the specific process of the treatment is as follows:
and (3) performing iron removal pretreatment and alkali liquor treatment on the fly ash to obtain a filtrate and a solid mixture, crystallizing the filtrate to obtain the molecular sieve, wherein the solid mixture is filter residue.
6. The fly ash-based carbon dioxide absorption system according to any one of claims 1 to 5, further comprising a carbon dioxide desorption device;
after the carbon dioxide is captured by the carbon dioxide capture device, the hydrophobic zeolite molecular sieve absorption matrix which captures the carbon dioxide is placed in a carbon dioxide desorption device, and the captured carbon dioxide is transferred to a carbon dioxide sequestration device.
7. A fly ash recycling method is characterized by comprising the following steps:
1) performing iron removal pretreatment and alkali liquor treatment on the fly ash to obtain a filtrate and a solid mixture;
2) obtained by the stepsThe mixture of the filtrate and aluminosilicate is crystallized by hydrothermal reaction to obtain zeolite molecular sieve, and then the zeolite molecular sieve and SiCl are added4Obtaining a hydrophobic modified zeolite molecular sieve after liquid phase deposition, and then solidifying the hydrophobic modified zeolite molecular sieve, portland cement, polyacrylamide and water to obtain a hydrophobic zeolite molecular sieve absorption matrix;
the solid mixture obtained in the step contains a certain amount of water, and the water is used as a filter residue sealing matrix;
3) placing the hydrophobic zeolite molecular sieve absorption matrix in a carbon dioxide capture device, and placing the filter residue sealing matrix in a carbon dioxide sealing device to respectively obtain the carbon dioxide capture device containing the hydrophobic zeolite molecular sieve absorption matrix and the carbon dioxide sealing device containing the filter residue sealing matrix;
4) and (2) capturing carbon dioxide in flue tail gas by the carbon dioxide capturing device containing the hydrophobic zeolite molecular sieve absorption matrix obtained in the step, then placing the hydrophobic zeolite molecular sieve absorption matrix capturing the carbon dioxide in a carbon dioxide desorption device, desorbing the captured carbon dioxide by hot steam, and then sending the carbon dioxide into a carbon dioxide sequestration device containing a filter residue sequestration matrix for sequestration.
8. The fly ash recycling method of claim 7, wherein the iron removal pretreatment comprises magnetic iron removal and/or acid liquor iron removal;
the acid solution comprises one or more of hydrochloric acid solution, sulfuric acid solution and nitric acid solution;
the concentration of the acid liquor is 2-4 mol.L-1；
The temperature for removing iron in the acid liquor is 60-70 ℃;
the time for removing iron from the acid liquor is 5-6 hours;
the alkali liquor comprises a sodium hydroxide solution and/or a potassium hydroxide solution;
the alkali liquor treatment is a hydrothermal reaction;
the temperature of the alkali liquor treatment is 90-100 ℃;
the alkali liquor treatment time is 48-96 h.
9. The fly ash recycling method of claim 7, wherein the aluminosilicates include soluble silicates and soluble aluminates;
the molar ratio of Si to Al in the mixture of the filtrate and the silicon-aluminum salt is 2.2-3.3;
the temperature of the hydrothermal reaction in the step 2) is 90-100 ℃;
the time of the hydrothermal reaction in the step 2) is 6-8 h;
the liquid phase deposition comprises the following specific steps:
zeolite molecular sieve and SiCl4Mixing with solvent, and roasting;
the zeolite molecular sieve and SiCl4The mass ratio of (1): (0.2 to 0.5);
the mass ratio of the zeolite molecular sieve to the solvent is 1: (3-5);
the mixing time is 5-6 h;
the roasting temperature is 400-500 ℃.
10. The fly ash recycling method of claim 7, wherein the curing is normal temperature curing;
the curing time is 12-24 h;
the flue comprises a flue of a coal-fired thermal power plant;
the desorption temperature is 30-50 ℃;
the desorption pressure is 300-400 MPa;
the sealing temperature is 40-80 ℃;
the partial pressure of the sealed carbon dioxide is 1-3 MPa;
and the liquid-solid ratio of the filter residue sealing matrix is 0.1-1.
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