Preparation method of green zeolite

Abstract

The invention discloses a preparation method of green zeolite, which comprises the following steps: adding a silicon-aluminum source and a photocatalyst into a cesium-containing or sodium-containing solution, carrying out ultrasonic treatment for 1-10 hours, reacting for 1-3 days at normal temperature and normal pressure under an illumination condition, filtering, washing and drying to obtain cesium zeolite or natrolite; the silicon-aluminum source is fly ash or a silicon-aluminum-containing waste raw material; the composite photocatalyst is prepared by taking an organic framework material as a main body and adding a metal oxide and a magnetic substance and / or adding a biological porous material as a carrier. The zeolite is prepared from the fly ash and the silicon-aluminum-containing waste raw materials thereof, and the method is low in cost, safe and easy to operate.

Description

Technical Field

[0001] The present invention relates to the field of preparation of zeolites, and particularly to a method for preparing green zeolites. Background Art

[0002] Fly ash is the ash and slag produced by coal-fired power plants. Currently, it is mainly used for making bricks, etc. However, the large accumulation of fly ash not only occupies a large amount of land, but also causes serious pollution to the ecological environment such as water bodies, the atmosphere, and the soil. The content of the main active component, silicon-aluminum acid vitreous body, in fly ash is generally above 70%. The w(Si) / w(A1) range in natural zeolites is 1-6, and the w(Si) / w(A1) in the fly ash used in the reaction is within the range of 1-6, which meets the silicon-aluminum ratio required for synthesizing zeolites. Fly ash can be converted into zeolites under relatively mild conditions. Currently, there are dozens of synthesized fly ash zeolites. The zeolites reported in the literature to be synthesized from fly ash as the raw material by adding appropriate amounts of silicon and aluminum sources through hydrothermal synthesis mainly include A, X, Y, P, HS, ZSM, etc. Zeolite is a mineral with a wide range of uses, and its applications cover multiple fields, including industry, agriculture, environmental protection, and medicine. Currently, the synthesized fly ash zeolites are synthesized by high-temperature calcination and hydrothermal synthesis under high temperature and pressure, which consumes a large amount of energy, has a high cost, and has unstable factors such as high pressure, restricting industrial applications. Therefore, how to reduce energy and simplify the process is an important factor in the industrial application of fly ash zeolite.

[0003] Fission nuclides in high-level liquid waste (HLLW) 137 Cs has a high heat release rate and is easily leached. Compounds of cesium are very soluble in water and have strong physical and chemical mobility (extremely easy to dissolve and volatilize at high temperatures); cesium in high-level liquid waste mainly exists in the form of ions. 137 Cs is easily spread over a large area with surface water and groundwater and enters the biogeochemical cycle. 137 Cs has a half-life as long as 30 years and emits β and γ rays. Its radioactivity proportion in fission products increases with time. 137 Cs can enter the human body through food chains and other channels, causing damage to the human blood system and nervous system, leading to the occurrence of cancer, threatening the safety of animals and humans. 137 Cs is one of the most dangerous radioactive nuclides biologically. Therefore, how to safely and efficiently separate Cs(I) from HLLW has become one of the world-challenging topics in the field of nuclear waste treatment. Untreated nuclear wastewater contains radioactive cesium ( 137 Cs) up to 200 Bq / mL. If 137Cesium separation can, on the one hand, reduce the volume and storage life of the solidified body, simplify the geological disposal process and save costs; on the other hand, it can reduce the risks posed by cesium to organisms and the environment. Therefore, developing a simple separation technology for separating and enriching cesium from radioactive waste liquid will not only save geological disposal costs and enhance the safety of organisms, but also have great significance for nuclear waste treatment and environmental application prospects.

[0004] Nowadays, at home and abroad 137 The main treatment methods for cesium separation include solvent extraction, evaporation, foam separation, adsorption, membrane separation, precipitation, etc. Each method has its suitable environmental system, advantages and disadvantages. The main methods for cesium solidification treatment are: vitrification, ceramic solidification and glass-ceramic solidification. Ceramic solidified bodies have superior properties, but generally need to be treated under high temperature and pressure. The current synthesis of cesium zeolite in the existing technology mainly includes hydrothermal method, high-temperature melting method, hot pressing method and sol-gel method. It is usually synthesized by solid-state method at temperatures above 1000 °C or by hydrothermal synthesis at 200 °C - 300 °C. The solid-state method has high temperature and large energy consumption, and most of the high-temperature processes form a mixed solidified body mainly composed of cesium zeolite for geological disposal. The hydrothermal method is based on the formation of zeolite crystal nuclei by the solvation of solvent water under high temperature and high pressure, and relatively pure cesium zeolite can be obtained. The traditional hydrothermal method has a certain pressure, has unsafe factors, and the temperature is mostly 200 °C - 300 °C, with high energy consumption. Summary of the Invention

[0005] In order to overcome the above-mentioned shortcomings and deficiencies of the existing technology, the purpose of the present invention is to provide a preparation method of green zeolite, which uses fly ash and its silicon-aluminum-containing waste raw materials to prepare zeolite, and can be low-cost, safe and easy to operate.

[0006] The purpose of the present invention is achieved through the following technical solutions:

[0007] The present invention provides a preparation method of green zeolite, including the following steps:

[0008] Add a silicon-aluminum source and a photocatalyst to an alkali solution containing cesium or sodium, ultrasonicate for 1 - 10 h, and then react for 1 - 3 days under normal temperature and pressure under light conditions. After filtration, washing and drying, cesium zeolite or sodium zeolite is obtained; the silicon-aluminum source is fly ash or other silicon-aluminum raw materials;

[0009] The photocatalyst is prepared by using an organic framework material as the main body and adding metal oxides and magnetic substances and / or adding biological porous materials as carriers to prepare a composite photocatalyst.

[0010] Preferably, the photocatalyst is g-C 3 N 4 / Fe 3 O 4 / M / BC or g-C3 N 4 / BC or g-C 3 N 4 / Fe 3 O 4 / M, where BC is pyrolytic biochar and M is semiconductor oxide.

[0011] Preferably, the preparation of the g-C 3 N 4 comprises the following steps:

[0012] Put dicyandiamide into a covered crucible and calcine it in a muffle furnace at a rate of 2 - 3 °C / min to 500 °C - 650 °C for 1 - 2 h to obtain a yellow solid; then grind this solid into powder, immerse it in 0.3 - 0.6 M acetic acid solution, ultrasonicate for 1 - 2 h and then stir for 4 - 5 h; finally, obtain a solid sample by centrifugation, wash it with water and ethanol, and dry it in a vacuum drying oven at 60 - 80 °C for 10 - 15 h to obtain g-C 3 N 4 .

[0013] Preferably, the preparation of the g-C 3 N 4 / Fe 3 O 4 / M comprises the following steps:

[0014] Mix g-C 3 N 4 with Fe 3 O 4 magnetic nanomaterials and oxide precursors, ultrasonically treat them, after hydrothermal reaction at 100 °C - 200 °C, centrifuge, filter and dry to obtain g-C 3 N 4 / Fe 3 O 4 / M; wherein, the molar ratio of g-C 3 N 4 , Fe 3 O 4 magnetic nanomaterials and oxide precursors is 1:0.1 - 0.5:0.05 - 0.6.

[0015] Preferably, the preparation of the pyrolytic biochar comprises the following steps:

[0016] Take dry biomass particles, dry them at a temperature of 100 °C - 120 °C, carry out pyrolysis in a tubular furnace under nitrogen protection, the nitrogen flow rate is 100 - 120 mL / min, the pyrolysis temperature is 750 - 800 °C, and the pyrolysis time is 100 min - 140 min to obtain the pyrolytic biochar.

[0017] Preferably, the g-C3 N 4 The preparation process of / BC is:

[0018] G C 3 N 4 The pyrolyzed biochar was immersed in a 0.3-0.6 M acetic acid solution, ultrasonicated for 2-3 h, and then stirred for 3-4 h. Finally, the solid sample was obtained by centrifugation, washed with water and ethanol, and dried in a vacuum oven at 60-80 °C for 10-15 h to obtain gC 3 N 4 / BC;

[0019] The gC 3 N 4 / Fe 3 O 4 The preparation process of / M / BC is as follows:

[0020] G C 3 N 4 / Fe 3 O 4 / M and pyrolyzed biochar were immersed in 0.3-0.6M acetic acid solution, ultrasonicated for 2-3h and then stirred for 3-4h; finally, solid samples were obtained by centrifugation, washed with water and ethanol, and dried in a vacuum drying oven at 60-80℃ for 10-15h to obtain gC 3 N 4 / Fe 3 O 4 / M / BC.

[0021] Preferably, when the green zeolite is cesium zeolite, the molar ratio of silicon in the silicon-aluminum source, aluminum in the silicon-aluminum source, and cesium oxide in the cesium-containing solution is: silicon-aluminum source 1: 0.1-2: 0.1-2.

[0022] Preferably, the silicon-aluminum source is prepared by the following method: fly ash or waste raw materials containing silicon and aluminum are used as raw materials and subjected to alkali melting, calcination and activation treatment.

[0023] Preferably, the lighting condition is from ultraviolet light to visible light.

[0024] Preferably, the lighting condition is sunlight.

[0025] Preferably, the organic framework material is gC 3 N 4 ; The semiconductor oxide is TiO 2、 Bi 2 O 3 or WO 3 .

[0026] Compared with the prior art, the present invention has the following advantages and beneficial effects:

[0027] (1) The present invention is applied to the preparation of zeolite from waste containing silicon and aluminum sources such as fly ash, which can be achieved at normal temperature and pressure, with low cost, safe and simple operation, realizing resource utilization, and being green and environmentally friendly.

[0028] (2) The present invention is applied to the treatment of cesium in radioactive waste liquid, which can reduce the risk caused by cesium to organisms and the environment, save geological disposal costs, enhance the safety of organisms, and will have great significance for nuclear waste treatment and environmental application prospects. Description of the Drawings

[0029] Figure 1 SEM image of the photocatalyst prepared in Example 1 of the present invention.

[0030] Figure 2 XRD pattern of the cesium zeolite synthesized in Example 1 of the present invention and the standard sample.

[0031] Figure 3 SEM image of the cesium zeolite synthesized in Example 1 of the present invention.

[0032] Figure 4 SEM image of the photocatalyst prepared in Example 2 of the present invention.

[0033] Figure 5 XRD pattern of the Y zeolite synthesized in Example 2 of the present invention.

[0034] Figure 6 SEM image of the Y zeolite synthesized in Example 2 of the present invention. Detailed Description of the Invention

[0035] The present invention will be further described in detail below in conjunction with embodiments, but the embodiments of the present invention are not limited thereto.

[0036] Example 1

[0037] The preparation method of the green zeolite in this example is as follows:

[0038] (1) Preparation of photocatalyst (g-C 3 N 4 / Fe 3 O 4 / TiO 2 ):

[0039] Put 2 g of dicyandiamide into a covered crucible, heat it in a muffle furnace at a rate of 2 °C / min to 500 °C and calcine for 1 h to obtain a yellow solid. Then grind this solid into powder, immerse it in 20 mL of 0.3 M acetic acid solution, ultrasonicate for 2 h and then stir for 4 h. Finally, obtain a solid sample by centrifugation, wash it 3 times with water and ethanol, and dry it at 80 °C in a vacuum drying oven for 10 h. The obtained sample is labeled as g-C 3 N 4 。

[0040] Mix g-C 3 N 4 with Fe 3 O 4 magnetic nanomaterials and tetrabutyl titanate in a molar ratio of 1:0.2:0.3, ultrasonically treat, after hydrothermal reaction at 100 °C, centrifuge, filter and dry to obtain g-C 3 N 4 / Fe 3 O 4 / TiO 2 。The SEM image of the photocatalyst prepared in this example is as shown in Figure 1 and is in the shape of cotton floc.

[0041] (2) Preparation of silicon-aluminum source:

[0042] Using fly ash as raw material, perform alkali melting and calcination activation treatment:

[0043] Condition: fly ash: alkali = 1:1 (Wt / Wt), calcination temperature 500 °C, then the activated silicon-aluminum source is obtained;

[0044] (3) Preparation of cesium zeolite: Add the photocatalyst prepared in step (1) and the activated silicon-aluminum source prepared in step (2) into the radioactive waste liquid containing cesium, adjust the silicon-aluminum ratio according to the molar ratio of silicon-aluminum-cesium of 2:1:1.2, and ultrasonicate for 3 h; then irradiate with a 300 W xenon lamp light source, and under the action of the photocatalyst, react at normal temperature and pressure for 2 days to crystallize cesium in the nuclear waste liquid to form cesium zeolite, and after filtration, washing and drying, collect cesium zeolite.

[0045] The XRD patterns of the cesium zeolite synthesized in this example and the standard sample are as shown in Figure 2 and are consistent with the standard cesium waste liquid phase structure. The SEM image of the cesium zeolite synthesized in this example is as shown in Figure 3 and the zeolite is spherical granular. The Cs 2 O content in the zeolite is 23.5%-45%, and cesium exists in a crystalline state with good migration stability.

[0046] Example 2

[0047] (1) Preparation of photocatalyst (g-C 3 N 4 / BC):

[0048] Put 5 g of dicyandiamide into a covered crucible and calcine it in a muffle furnace at a rate of 2 °C / min to 650 °C for 2 h to obtain a yellow solid. Then grind this solid into powder, immerse it in 50 mL of 0.6 M acetic acid solution, sonicate for 2 h and then stir for 4 h. Finally, obtain a solid sample by centrifugation, wash it 3 times with water and ethanol, and dry it at 80 °C in a vacuum drying oven for 15 h. The obtained sample is labeled as g-C 3 N 4 (A).

[0049] Take the dried biomass particles, dry them at 100 °C, and pyrolyze them in a tube furnace under nitrogen protection. The nitrogen flow rate is 100 mL / min, the pyrolysis temperature is 750 °C, and the pyrolysis time is 120 min. The obtained pyrolytic biochar is labeled as BC.

[0050] According to the mass percentage of BC / A being 1 - 10% (Wt / Wt), immerse A and BC in 30 mL of 0.5 M acetic acid solution, sonicate for 2 h and then stir for 4 h. Finally, obtain a solid sample by centrifugation, wash it 3 times with water and ethanol, and dry it at 80 °C in a vacuum drying oven for 12 h. The obtained sample is labeled as g-C 3 N 4 / BC. The SEM image of the photocatalyst prepared in this example is as Figure 4 shown, and the catalyst is circular particles.

[0051] (2) Preparation of silicon-aluminum source:

[0052] Using silicon-aluminum-containing waste raw materials as raw materials, perform alkali fusion calcination activation treatment:

[0053] Condition: silicon-aluminum-containing waste raw materials: alkali = 1:2 (Wt / Wt), calcination temperature 700 °C, then the activated silicon-aluminum source is obtained;

[0054] (3) Preparation of Y zeolite: Add the photocatalyst prepared in step (1) and the silicon-aluminum source prepared in step (2) to the NaOH solution (3 mol / L), use a 300 W xenon lamp light source, and under the action of the photocatalyst, react at normal temperature and pressure for 2 days to form Y zeolite. After filtration, washing, and drying, collect the Y zeolite.

[0055] The XRD patterns of the Y zeolite synthesized in this example and the standard sample are as Figure 5 shown, which is consistent with the crystal phase structure of the standard Y zeolite. The SEM image of the Y zeolite synthesized in this example is as Figure 6 shown, which is a tetrahedral structure.

[0056] Example 3

[0057] (1) Preparation of photocatalyst (g-C 3N 4 / Fe 3 O 4 / Bi 2 O 3 ):

[0058] Put 5 g of dicyandiamide into a covered crucible, heat it in a muffle furnace at a rate of 2 °C / min to 600 °C and calcine for 1.5 h to obtain a yellow solid. Then grind this solid into powder, immerse it in 30 mL of 0.5 M acetic acid solution, ultrasonicate for 2 h and then stir for 4 h. Finally, obtain a solid sample by centrifugation, wash it 3 times with water and ethanol, and dry it in a vacuum drying oven at 80 °C for 12 h. The obtained sample is labeled as g-C 3 N 4 。

[0059] Mix g-C 3 N 4 with Fe 3 O 4 magnetic nanomaterials and Bi(NO 3 ) 3 and ultrasonically treat them according to a molar ratio of 1:0.5:0.6. After hydrothermal reaction at 200 °C, centrifuge, filter and dry to obtain g-C 3 N 4 / Fe 3 O 4 / Bi 2 O 3 。

[0060] (2) Preparation of silicon-aluminum source:

[0061] Use fly ash as raw material and carry out alkali melting and calcination activation treatment:

[0062] Condition: fly ash: alkali = 1:1.5 (Wt / Wt), calcination temperature 600 °C, then the activated silicon-aluminum source can be obtained;

[0063] (3) Preparation of cesium zeolite: Add 0.3 g of the photocatalyst prepared in step (1) and the activated silicon-aluminum source prepared in step (2) (adjusted to a silicon-aluminum molar ratio of 2:1, 0.8 g of silicon dioxide, and the silicon-aluminum adjustment can be achieved by adding reagent silicon-aluminum source or using the silicon-aluminum raw material leached from fly ash) into the cesium solution (using a simulated cesium hydroxide concentration of 0.04 g / ml, 25 ml), ultrasonicate for 5 h; then irradiate with a 300 W xenon lamp light source, and under the action of the photocatalyst, react at normal temperature and pressure for 3 days to crystallize cesium in the nuclear waste liquid to form cesium zeolite. After filtration, washing and drying, collect the cesium zeolite.

[0064] Example 4

[0065] The preparation method of the green zeolite in this example is as follows:

[0066] (1) Preparation of photocatalyst (g-C 3 N 4 / Fe 3 O 4 / TiO 2 / BC):

[0067] (1-1) Preparation

[0068] Put 2 g of dicyandiamide into a covered crucible, heat it in a muffle furnace at a rate of 2 °C / min to 500 °C and calcine for 1 h to obtain a yellow solid. Then grind this solid into powder, immerse it in 20 mL of 0.3 M acetic acid solution, ultrasonicate for 2 h and then stir for 4 h. Finally, obtain a solid sample by centrifugation, wash it 3 times with water and ethanol, and dry it at 80 °C in a vacuum drying oven for 10 h. The obtained sample is labeled as g-C 3 N 4 .

[0069] Mix g-C 3 N 4 with Fe 3 O 4 magnetic nanomaterials and tetrabutyl titanate in a molar ratio of 1:0.2:0.3, ultrasonically treat, after hydrothermal reaction at 100 °C, centrifuge, filter and dry to obtain g-C 3 N 4 / Fe 3 O 4 / TiO 2 ;

[0070] Put 5 g of dicyandiamide into a covered crucible, heat it in a muffle furnace at a rate of 2 °C / min to 650 °C and calcine for 2 h to obtain a yellow solid. Then grind this solid into powder, immerse it in 50 mL of 0.6 M acetic acid solution, ultrasonicate for 2 h and then stir for 4 h. Finally, obtain a solid sample by centrifugation, wash it 3 times with water and ethanol, and dry it at 80 °C in a vacuum drying oven for 15 h. The obtained sample is labeled as g-C 3 N 4 (A).

[0071] (1-2) Preparation of BC:

[0072] Take the dried biomass particles, dry them at 100 °C, pyrolyze them in a tube furnace under nitrogen protection, with a nitrogen flow rate of 100 mL / min, a pyrolysis temperature of 750 °C, and a pyrolysis time of 120 min. The obtained pyrolyzed biochar is labeled as BC;

[0073] (1-3) Preparation of g-C 3 N 4 / Fe 3 O 4 / TiO 2 / BC:

[0074] The g-C 3 N 4 / Fe 3 O 4 / TiO 2 / BC and BC were immersed in 30 mL of 0.5 M acetic acid solution, sonicated for 2 h and then stirred for 4 h. Finally, the solid sample was obtained by centrifugation, washed three times with water and ethanol, and dried at 80 °C for 12 h in a vacuum drying oven. The obtained sample was labeled as g-C 3 N 4 / BC.

[0075] (2) Preparation of the silicon-aluminum source:

[0076] Using fly ash as raw material, it was activated by alkali fusion and calcination:

[0077] Condition: fly ash: alkali = 1:1 (Wt / Wt), calcination temperature 550 °C, thus obtaining the activated silicon-aluminum source;

[0078] (3) Preparation of cesium zeolite: The photocatalyst prepared in step (1) and the activated silicon-aluminum source prepared in step (2) were added to the radioactive waste liquid containing cesium. According to the molar ratio of silicon:aluminum:cesium of 2:1:1.2, the silicon-aluminum ratio was adjusted and sonicated for 3 h; then irradiated with a 300 W xenon lamp light source. Under the action of the photocatalyst, the reaction occurred at normal temperature and pressure for 2 days to crystallize cesium in the nuclear waste liquid to form cesium zeolite. After filtration, washing and drying, the cesium zeolite was collected.

[0079] The above embodiments are preferred embodiments of the present invention, but the embodiments of the present invention are not limited by the described embodiments. Any other changes, modifications, substitutions, combinations, and simplifications made without departing from the spirit and principle of the present invention shall be equivalent replacement methods and are all included in the protection scope of the present invention.

Claims

1. A method for preparing green zeolite, characterized in that: The following steps are involved: Adding a silicon-aluminum source and a photocatalyst to a cesium- or sodium-containing solution, subjecting the solution to ultrasonic treatment for 1-10 hours, and then reacting the solution under light conditions at room temperature and pressure for 1-3 days, filtering, washing, and drying the solution to obtain a cesium zeolite or a sodium zeolite; the silicon-aluminum source is fly ash or other silicon-aluminum raw materials; The photocatalyst is based on an organic framework material, and metal oxides and magnetic substances and / or biological porous materials are added as carriers to prepare a composite photocatalyst.

2. The method for preparing green zeolite according to claim 1, characterized in that: The photocatalyst is g-C3N4 / Fe3O4 / M / BC or g-C3N4 / BC or g-C3N4 / Fe3O4 / M, wherein BC is pyrolyzed biochar and M is a semiconductor oxide.

3. The method for preparing green zeolite according to claim 2, characterized in that: The preparation of g-C3N4 comprises the following steps: Put dicyandiamide into a covered pan, heat it to 500°C-650°C in a muffle furnace at a rate of 2-3°C / min and calcine it for 1-2 hours to obtain a yellow solid; then grind the solid into powder, immerse it in a 0.3-0.6M acetic acid solution, ultrasonicate it for 1-2 hours and then stir it for 4-5 hours; finally, obtain a solid sample by centrifugation, wash it with water and ethanol, and dry it at 60-80°C in a vacuum drying oven for 10-15 hours to obtain g-C3N4.

4. The method for preparing green zeolite according to claim 3, characterized in that: The preparation of g-C3N4 / Fe3O4 / M comprises the following steps: The g-C3N4 is mixed with Fe3O4 magnetic nanomaterials and oxide precursors, subjected to ultrasonic treatment, and subjected to hydrothermal reaction at 100°C to 200°C, followed by centrifugation, filtration and drying to obtain g-C3N4 / Fe3O4 / M; wherein the molar ratio of g-C3N4, Fe3O4 magnetic nanomaterials and oxide precursors is 1:0.1-0.5:0.05-0.

6.

5. The method for preparing green zeolite according to claim 3, characterized in that: The preparation of the pyrolysis biochar comprises the following steps: The dried biomass particles are dried at a temperature of 100°C to 120°C, and pyrolyzed in a tubular furnace under nitrogen protection, with a nitrogen flow rate of 100 to 120 mL / min, a pyrolysis temperature of 750 to 800°C, and a pyrolysis time of 100 min to 140 min to obtain pyrolysis biochar.

6. The method for preparing green zeolite according to claim 3, characterized in that: The preparation process of g-C3N4 / BC is as follows: g-C3N4 and pyrolyzed biochar were immersed in 0.3-0.6M acetic acid solution, ultrasonicated for 2-3h and then stirred for 3-4h; finally, a solid sample was obtained by centrifugation, washed with water and ethanol, and dried in a vacuum drying oven at 60-80°C for 10-15h to obtain g-C3N4 / BC; The preparation process of g-C3N4 / Fe3O4 / M / BC is as follows: The g-C3N4 / Fe3O4 / M and pyrolyzed biochar were immersed in a 0.3-0.6 M acetic acid solution, ultrasonicated for 2-3 h and then stirred for 3-4 h; finally, the solid sample was obtained by centrifugation, washed with water and ethanol, and dried in a vacuum drying oven at 60-80°C for 10-15 h to obtain g-C3N4 / Fe3O4 / M / BC.

7. The method for preparing green zeolite according to claim 1, characterized in that: When the green zeolite is cesium zeolite, the molar ratio of silicon in the silicon-aluminum source, aluminum in the silicon-aluminum source, and cesium oxide in the cesium-containing solution is 1:0.1-2:0.1-2.

8. The method for preparing green zeolite according to claim 1, characterized in that: The silicon-aluminum source is prepared by the following method: fly ash or waste raw materials containing silicon and aluminum are used as raw materials and subjected to alkali melting, calcining and activation treatment.

9. The method for preparing green zeolite according to claim 1, characterized in that: The illumination conditions are from ultraviolet light to visible light.

10. The method for preparing green zeolite according to claim 1, characterized in that: The lighting condition is sunlight.

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