JP2003137537A - Method of manufacturing artificial zeolite - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a method of manufacturing artificial zeolite capable of effectively manufacturing it while reducing dispersion of its quality. SOLUTION: The artificial zeolite of high quality is efficiently manufactured as follows: a 1st hydrothermal reaction process is performed using a 1st raw material high in ingredient composition ratio of SiO2 /Al2 O3 * Al2 O3 * means an Al2 O3 component capable of hydrothermally reacting with an alkaline liquid among Al2 O3 equivalent contained plus both metal Al and Al nitride in terms of Al2 O3 ; after that a 2nd hydrothermal reaction process is performed by adding a 2nd raw material low in ingredient composition ratio of SiO2 /Al2 O3 *. Thereby a silicate ion of an aqueous solution of water glass generated in the 1st hydrothermal reaction process, reacts with an aluminate ion originated from the 2nd raw material.

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for producing artificial zeolite, and more particularly to a production technique suitable for producing artificial zeolite using waste as a raw material.

[0002]

2. Description of the Related Art Generally, zeolite is used in many fields because of its cation exchange function. Artificial zeolite manufactured artificially can be produced from wastes and unused resources as raw materials, and it is possible to produce useful substances from wastes and unused resources. Material that is suitable for the realization of a recycling and recycling society.

[0003]

However, when producing artificial zeolite from wastes or unused resources as a raw material as described above, it is extremely difficult to reduce the variation in raw material quality. There is a problem that it is extremely difficult to secure the quality and keep the quality constant.

In particular, the quality of artificial zeolite is included in the raw materials.
SiO_TwoAnd Al_TwoO_Three* (Contained Al_Two
O_ThreeAl, which reacts hydrothermally with alkaline solution_TwoO
_ThreeIngredients, metal Al and aluminum nitride Al_TwoO_ThreeExchange
Say the sum of the sums. Al that undergoes hydrothermal reaction with alkaline liquids
_TwoO_ThreeIngredients are aluminum hydroxide, Al in glass
_TwoO_ThreeMeans ingredients, etc. )) (Hereinafter, simply
Composition ratio SiO_Two/ Al_TwoO_Three* ”. )
To produce affected and high quality artificial zeolites,
Ingredient composition ratio SiO_Two/ Al_TwoO_Three* Is a molar ratio of 3.
It should be maintained within the range of 3 to 4.0. But Hara
Continuously using a single raw material of the same type and source
When manufacturing industrial zeolite, SiO in the raw material_TwoOr
Al_TwoO _ThreeSince the content of * varies, stable quality
The product cannot be manufactured.

Further, in order to maintain the component composition ratio of the raw material within the above range, an auxiliary raw material is added to the main raw material,
Alternatively, it is also possible to mix a plurality of raw materials, but in order to produce a high-quality artificial zeolite, it is necessary to cause a hydrothermal reaction under conditions suitable for the production of zeolite, so the treatment time is long. As a result, the production rate of zeolite decreases, and in order to shorten the treatment time, it is necessary to perform treatment under conditions different from the optimum conditions for improving the quality of zeolite, so the quality of zeolite may decrease. Therefore, there is a dilemma that it is not possible to achieve both improvement in zeolite quality and improvement in production efficiency.

Therefore, the present invention is to solve the above problems, and an object thereof is to provide a production method capable of efficiently producing an artificial zeolite while reducing the variation in the quality of the artificial zeolite. is there. Another object of the present invention is to provide a manufacturing method capable of simultaneously improving the quality of zeolite and the manufacturing efficiency. In particular, it is to provide a technique capable of producing a stable-quality artificial zeolite by using waste and unused resources.

[0007]

In order to solve the above-mentioned problems, the method for producing an artificial zeolite of the present invention comprises a component composition ratio S
_{iO 2 / Al 2 O 3 *} (Al 2 O 3 * , of the _Al 2 _{O 3} equivalent amount is contained, _Al 2 _{O 3} component to react an alkali solution and hydrothermal, as well as metallic Al and Al nitride Al
The first hydrothermal reaction step is carried out using a first raw material having a large sum of ₂ O ₃ conversion), and then the intermediate product produced in the first hydrothermal reaction step is treated with the first raw material from the first raw material. Is characterized in that the second hydrothermal reaction step is carried out by adding a second raw material having a small composition ratio SiO ₂ / Al ₂ O ₃ *.

[0008] The present inventor has, on the basis of a large number of experiences of producing artificial zeolites using wastes and unused resources,
I have keenly realized how difficult it is to continuously realize artificial zeolite with stable quality. And
Based on numerous experiences and experiments, the inventor has found that the process of producing artificial zeolite is "water glass aqueous solution production reaction".
And that the two-stage reaction of "zeolite formation (precipitation) reaction" is involved. Both of these two-step reactions proceed in the hydrothermal reaction process, but the former "water glass aqueous solution formation reaction" and the latter "zeolite formation (deposition)"
"Reaction" means that the optimum reaction conditions are different from each other.
Higher temperature, higher pressure treatment is desirable in the "water glass aqueous solution formation reaction", while lower temperature, lower pressure treatment is desirable in the "zeolite formation (precipitation) reaction". For example, the latter "zeolite formation (precipitation) reaction" is 100 The reaction is likely to proceed at a temperature of about ℃
The production rate of useful zeolites such as site) and Faujasite is high, but when processed at higher temperature and pressure, other zeolites such as halonite (Analcime) are produced. As a result, the cation exchange capacity is lowered and the quality is lowered.

According to the present invention, a high component composition ratio SiO_Two
/ Al_TwoO_ThreeFirst hydrothermal reaction using the first raw material having *
Process, then low composition ratio SiO_Two/ Al
_TwoO _ThreeSecond hydrothermal reaction step by adding the second raw material having *
By carrying out
The lath can be efficiently generated, and the second hydrothermal reaction process can be performed.
In the course of adding the silicate ions of the water glass
As it reacts with the aluminate ion in the second raw material,
Zeolite can be produced efficiently. According to
Therefore, the overall zeolite production efficiency can be increased.
Wear. That is, the process can be completed in a short time or at a predetermined time.
Higher yields or higher cation exchange capacity between
Can be obtained. In addition, with the first hydrothermal reaction step
The second hydrothermal reaction process and reaction are set under different conditions.
Since it is possible to do so in the first hydrothermal reaction step
Process under conditions that give priority to the water glass aqueous solution generation reaction.
Produce the desired zeolite in the second hydrothermal reaction step
To give priority to the zeolite formation (precipitation) reaction
Artificial zeolite produced by processing according to conditions
Manufacturing more efficiently without degrading the quality of
Will be possible.

In the present invention, it is preferable that the composition ratio SiO ₂ / Al ₂ O ₃ * of the first raw material has a molar ratio of more than 4.0. According to the present invention, by setting the composition ratio SiO ₂ / Al ₂ O ₃ * of the first raw material to a value exceeding 4.0 in terms of molar ratio, a water glass aqueous solution is produced together with zeolite in the first hydrothermal reaction step. Therefore, by adding the second raw material in the second hydrothermal reaction step, the silicate ions and the second
Further zeolite can be efficiently produced by reacting with the aluminate ion of Al ₂ O ₃ * in the raw material.

In the present invention, it is preferable that the composition ratio SiO ₂ / Al ₂ O ₃ * of the second raw material has a molar ratio of less than 3.3. According to this invention, excess Al ₂ O ₃ * (aluminate ion) that can react with the aqueous solution of water glass generated in the first hydrothermal reaction step is present, and zeolite can be efficiently produced. .

In the present invention, the processing pressure or temperature in the first hydrothermal reaction step is preferably equal to or higher than the processing pressure or temperature in the second hydrothermal reaction step. According to this invention, the reaction can be efficiently advanced by prioritizing the water glass aqueous solution production reaction in the first hydrothermal reaction step, and the desired zeolite is efficiently produced in the second hydrothermal reaction step, A high-quality artificial zeolite (for example, a zeolite having a high cation exchange capacity) can be efficiently produced.

[0013] In the present invention, a plurality of kinds of raw materials, previously a large raw material group A component composition ratio _SiO 2 / _Al 2 _{O 3} *, in a small material group B of component composition ratio _SiO 2 / _Al 2 _{O 3} * Classified in advance, one raw material belonging to raw material group A or a mixture of a plurality of raw materials is the first raw material, and one raw material belonging to raw material group B or a mixture of a plurality of raw materials is the second raw material It is preferable to use. According to the present invention, by classifying a plurality of raw materials suitable as the first raw material and a plurality of raw materials suitable as the second raw material, the first raw material and the second raw material can be appropriately combined from them. Since and can be taken out and used, raw material management becomes easy, and stable production of artificial zeolite can be realized.

[0014]

BEST MODE FOR CARRYING OUT THE INVENTION Next, an embodiment of the method for producing an artificial zeolite according to the present invention will be described in detail with reference to the accompanying drawings. In the present embodiment, a plurality of types of raw materials for producing artificial zeolite are mixed with a component composition ratio SiO ₂ / A.
Raw material group A with high l ₂ O ₃ * and composition ratio SiO ₂ / A
The first hydrothermal reaction step is performed using one raw material belonging to the raw material group A or a mixture of a plurality of raw materials (first raw material), which is divided into a raw material group B having a low l ₂ O ₃ *, and thereafter. Then, one raw material belonging to raw material group B or a mixture of a plurality of raw materials (second raw material) was added, and the second hydrothermal reaction step was performed.

Raw material group A: As the material belonging to the raw material group A, the content of SiO ₂ is higher than that of Al ₂ O _3, and both zeolite and water glass aqueous solution can be produced by hydrothermal reaction. Is preferred. In particular, it is desirable that the component composition ratio SiO ₂ / Al ₂ O ₃ exceeds 4.0. More specifically, as wastes or unused resources, fly ash (coal ash captured by an electric dust collector, etc.), pearlite, volcanic ash, waste sand such as silica sand, waste caustic soil, waste Examples include foundry sand, waste activated clay, glass waste, water glass and cullet waste. When there are a plurality of raw materials belonging to the raw material group A, any one of these raw materials may be used as the above-mentioned first raw material, or two or more raw materials are mixed and the above-mentioned raw materials are mixed. You may use it as a 1st raw material.

Raw material group B: As a material belonging to the raw material group B, the Al ₂ O ₃ * content is higher than the SiO ₂ content and it reacts with a water glass aqueous solution under hydrothermal reaction to form zeolite. What is obtained is preferable. In particular, it is desirable that the composition ratio SiO ₂ / Al ₂ O ₃ * be less than 3.3. More specifically, as waste or unused resources, papermaking sludge ash, metakaolin, aluminum dross, aluminum hydroxide sludge, waste alkali aqueous solution containing aluminate ions (those discharged in the aluminum manufacturing process), Examples include quenched aluminum slag, waste aluminum alloy, blast furnace slag, and waste melting furnace slag. When there are a plurality of raw materials belonging to the raw material group B, any one of these raw materials may be used as the above-mentioned first raw material, or two or more raw materials are mixed and the above-mentioned raw materials are mixed. You may use it as a 1st raw material.

[0017] Incidentally, _Al 2 _{O 3} * is referred to herein, of the _Al 2 _{O 3} equivalent amount is contained, _Al 2 _{O 3} component to react an alkali solution and hydrothermal, and metal Al and Al nitride Is the sum of those converted into Al ₂ O ₃ .
The Al ₂ O ₃ component that hydrothermally reacts with the alkaline liquid means aluminum hydroxide, an Al ₂ O ₃ component in glass, and the like.

In the first hydrothermal reaction step, the first raw material is dispersed in an alkaline aqueous solution such as NaOH or preferably an alkaline aqueous solution containing SiO ₂ (silicate ions) to form a slurry solution, The slurry solution is heated. It is particularly preferable to heat under pressure. This step can be carried out, for example, as an autoclave treatment or a boiling treatment.

In the second hydrothermal reaction step, the second raw material is added to the slurry solution after the first hydrothermal reaction step is carried out to prepare a new slurry solution, which is heated in the same manner as above. Also in this step, it is particularly preferable to heat under pressure.
This step can also be performed, for example, as an autoclave treatment or a boiling treatment. In particular, the amount of the second raw material to be added in the second hydrothermal reaction step is determined in consideration of the composition ratio SiO ₂ / Al ₂ O ₃ * of the first raw material and the second raw material, and the first raw material (or the first raw material). The composition ratio SiO ₂ / Al ₂ O ₃ * of the total raw material of the water glass (silicate ion) obtained in the hydrothermal reaction step and the second raw material is 3.3 to 4.0 in molar ratio.
It is preferable to set it so as to fall within the range.

Here, the processing pressure or temperature of the first hydrothermal reaction step is preferably equal to or higher than the processing pressure or temperature of the second hydrothermal reaction step. For example, it is preferable to set the temperature of the first hydrothermal reaction step to 115 to 180 ° C. in order to promote the production of the water glass aqueous solution, and to set the temperature of the second hydrothermal reaction step to 90 to 110 ° C. Desirable to promote zeolite formation.

[0021]

EXAMPLES Next, the results of confirming the effects of the present invention by actually conducting a synthetic zeolite production test will be shown. However, the following conditions and results are examples of the present invention, and the present invention is
It is not limited to the following description.

[First Embodiment] First, a raw material belonging to the raw material group A and a raw material belonging to the raw material group B are selected, and these two kinds of raw materials (wastes) are mixed and used in one step. Hydrothermal treatment (hereinafter, simply referred to as “batch treatment”, which is a comparative example with respect to the present invention), and a first hydrothermal reaction step using raw materials belonging to the raw material group A,
After that, a comparison was made with the case where the second hydrothermal reaction step was carried out by adding the raw materials belonging to the raw material group B (hereinafter, simply referred to as “the case of tandem treatment”, which is an example of the present invention).

Fine powder of pearlite is selected as a raw material belonging to the raw material group A, and a waste alkaline aqueous solution containing aluminate ions is selected as a raw material belonging to the raw material group B. In the case of batch treatment, (A) in Table 1 below is selected. The mixture was mixed under the conditions of (C) to (C) to prepare a slurry solution, which was then autoclaved at 120 ° C. for 4 hours. In the case of tandem treatment, among those described in (A) to (C) of Table 1 below,
A fine pearlite powder and a sodium hydroxide aqueous solution were mixed to prepare a slurry solution, and the slurry solution was autoclaved at 120 ° C. for 2 hours, and then the slurry solution was once cooled to 100 ° C. The waste alkaline aqueous solution containing aluminate ion described in 1) was added and the mixture was kept at 100 ° C. for 2 hours.

[0024]

[Table 1]                 Pearlite fine powder 3.5N NaOH aqueous solution Waste alkali Aqueous solution   Condition (A) 100g 300ml 50ml   Condition (B) 100g 300ml 100ml   Condition (C) 100g 300ml 150ml   (Unit: ml is milliliter, waste alkaline aqueous solution contains aluminate ion Therefore, the amount of Na ions is 60 g / l (liter) and the amount of Al ions is 45 g / l)

Cation exchange capacity (CEC; base exchange capacity; unit meq / 100) of the artificial zeolite produced under the above conditions
g) was measured. The results are shown in Table 2.

[0026]

[Table 2]   Conditions (A) (B) (C)   For batch processing 240 230 175   For tandem processing 261 322 330

As shown in Table 2, in the case of batch processing,
While the cation exchange capacity tends to deteriorate as the amount of the waste alkali aqueous solution is increased, in the case of the tandem treatment, the cation exchange capacity is improved as the amount of the waste alkaline aqueous solution is increased. This indicates that the quality of the zeolite produced by the tandem treatment is improved and the zeolite production efficiency is increased. That is, as described above, even if the treatment time is the same (4 hours in each case), the tandem treatment promotes the production of zeolite more than the batch treatment, and a larger amount of the components derived from the waste alkali aqueous solution (aluminate ion). )
React to form a zeolite. In other words, the tandem process requires a shorter time than the batch process to obtain the same amount of zeolite or to achieve a similar cation exchange capacity.

The reason why the tandem treatment is more advantageous than the batch treatment is that in the tandem treatment, SiO ₂ is used in the first hydrothermal reaction step.
Water glass aqueous solution is efficiently generated by using the excess first raw material of Al ₂ O _{3 and} the excess _second glass of Al ₂ O ₃ is added in the _second hydrothermal reaction step.
The point is that the raw material can be added and reacted with water glass to efficiently produce (precipitate) zeolite.

That is, in the batch treatment, even if an aqueous solution of water glass is produced, since the aluminate ions coexist, the water glass is converted to zeolite as it is, and Na is consumed when the zeolite is produced. However, it becomes difficult to produce water glass more than that (reaction rate decreases). That is, the production reaction of water glass is a rate-determining reaction, which limits the production of zeolite.

On the other hand, in the tandem treatment, zeolite is produced together with water glass in the first hydrothermal reaction step.
Since the ingredient composition ratio SiO ₂ / Al ₂ O ₃ * of the raw materials is high, the amount of Na consumed due to the zeolite formation is relatively small, and accordingly, the decrease in the ability to generate the aqueous solution of water glass is suppressed, and the amount of water glass is reduced. The production rate becomes faster, and the amount of water glass finally obtained also increases. Then, in the second hydrothermal reaction step, the component composition ratio SiO ₂ / Al _{2 is} added to the water glass.
When the second raw material having a low O ₃ * is added, the reaction between water glass and aluminate ions is promoted, and zeolite is efficiently produced.

More specifically, in the case of the tandem treatment, the cation exchange capacity is improved as the amount of the waste alkali solution is increased. That is, a large amount of water glass is produced in the first hydrothermal reaction step. It can be said that it is because there is. On the other hand, in the case of batch treatment, the degree of suppression of water glass formation increases as the amount of waste alkali solution increases and the amount of aluminate ions increases, so that the deficiency of silicate ions necessary for the formation of zeolite increases. The ion exchange capacity is rather reduced. That is, in the tandem treatment, the water glass aqueous solution generation reaction and the zeolite generation (precipitation) reaction are performed in separate steps, so that the water glass aqueous solution generation reaction, which is a rate-determining reaction, can proceed more efficiently, As a result, the raw material components can be used more efficiently and a high-quality artificial zeolite can be produced.

The first hydrothermal reaction step and the second hydrothermal reaction step may be the same under the conditions of temperature, pressure and other external conditions. Even in this case, the two processes can be distinguished by the judgment criterion whether or not the second raw material is charged.

[Second Example] Next, an experiment for producing an artificial zeolite from various raw materials belonging to the raw material group B (papermaking sludge ash, refuse melting furnace slag, aluminum hydroxide sludge, aluminum dross) will be described. To do. In this experiment, the raw materials (wastes) belonging to the raw material group B and a plurality of alkaline aqueous solutions were mixed and heated to cause a hydrothermal reaction, and the cation exchange capacity of the resulting artificial zeolite was measured. . Papermaking sludge ash used here, refuse melting furnace slag, aluminum hydroxide sludge, aluminum
The composition of the dross is shown in Table 3 below.

[0034]

[Table 3]   Ingredient composition of papermaking sludge ash:   Ingredient CaO Al2O3 SiO2 MgO T-Fe Burning loss   wt% 3.5 54.2 26.4 5.2 3.8  0.1   Component composition of refuse melting furnace slag:   Ingredient CaO Al2O3 SiO2 MgO T-Fe Burning loss   wt% 28.3 17.3 35.5 2.2 3.7  0.1   Aluminum hydroxide sludge composition:   Ingredient CaO Al2O3 SiO2 MgO T-Fe   wt% 0.3 64.4 <1.0 <1.0 0.5   Composition of aluminum dross:   Ingredient CaO Al2O3 SiO2 MgO T-Fe   wt% <1.0 98.0 * <1.0 <1.0 <1.0   (Here, T-Fe represents the total amount of Fe. The ignition loss is the weight reduction amount when firing. Indicates. * Includes the converted amount of metallic aluminum. )

100 g of papermaking sludge ash having the above composition was added with 300 m of the alkaline solution of (a) to (d) shown in Table 4 below.
1 was mixed with 1 to prepare a slurry solution. And these slurry solutions were heated at 100 degreeC for 2 hours, and the artificial zeolite was produced by the hydrothermal reaction. The cation exchange capacity is shown in Table 5 (1). Further, 100 g of the melting furnace slag was mixed with 300 ml of the alkaline solutions (a) to (d) shown in Table 4 above to prepare a slurry solution. Then, these slurry solutions are added to 120
The mixture was heated at 0 ° C. for 2 hours to generate an artificial zeolite by hydrothermal reaction. The cation exchange capacity is shown in Table 5 (2). Furthermore, aluminum hydroxide sludge 30g
Is an alkaline solution 3 of (a) to (d) shown in Table 4 above.
Each was mixed with 00 ml to prepare a slurry solution.
And these slurry solutions were heated at 120 degreeC for 4 hours, and the artificial zeolite was produced by the hydrothermal reaction. The cation exchange capacity is shown in Table 5 (3). Also,
10 g of aluminum dross is shown in Table 4 (a)-
A slurry solution was prepared by mixing with 300 ml of the alkaline solution of (d). And these slurry solutions were heated at 120 degreeC for 4 hours, and the artificial zeolite was produced by the hydrothermal reaction. The cation exchange capacity is shown in Table 5.
It shows in (4).

[0036]

[Table 4] (a) 3.5N NaOH aqueous solution (effective composition:
Na ₂ O) (b) 3.5N sodium orthosilicate solution (effective composition:
2Na ₂ O.SiO ₂ ) (c) 3.5N sodium metasilicate aqueous solution (effective composition: N
a ₂ O.SiO ₂ ) (d) 3.5N No. 2 water glass aqueous solution (effective composition: Na
₂ O ・ 2SiO ₂ )

[0037]

[Table 5]   Alkaline solution (a) (b) (c) (d)   (1) 160 210 280 330   (2) 150 180 240 290   (3) 23 133 270 380   (4) 15 158 290 410   (Cation exchange capacity is meq / 100g)

Of the above alkaline solutions, all of (b) to (d) other than (a) belong to the aqueous solution of water glass. By using these aqueous solution of water glass, the artificial zeolite produced is The cation exchange capacity was higher than that using sodium hydroxide. In addition, among the water glasses, a cation exchange capacity higher is obtained by using (c) having a larger amount of silicate ions than that of (b), and further by using (d) having a larger amount of silicate ions than (c). A high cation exchange capacity is obtained.

From these experiments, it was confirmed that a higher cation exchange capacity can be obtained by mixing the second raw material belonging to the raw material group B with the aqueous solution of water glass. Also,
It was also confirmed that the higher the concentration of silicate ions in the water glass aqueous solution, the higher the cation exchange capacity obtained. Therefore, in the case of producing an artificial zeolite using a raw material belonging to the raw material group B, when water glass is previously produced from the raw material belonging to the raw material group A in the tandem treatment, the artificial zeolite is produced as the amount of produced water glass increases. Will improve the quality of.

[Third Embodiment] Next, 100 g of the raw materials belonging to the raw material group A and an aqueous solution of 3.5 N sodium hydroxide 30
0 ml was mixed and the first hydrothermal reaction step was carried out at 160 ° C. for 4 hours, after which metakaolin (composition shown in Table 6) as a raw material belonging to the raw material group B was appropriately added, and the second hydrothermal reaction step was performed.
It was kept at 100 ° C. for 2 hours as a hydrothermal reaction step. Here, the amount of metakaolin added is the SiO ₂ concentration (silicate ion concentration) in the slurry solution after the first hydrothermal reaction step.
In consideration of the above, by adding metakaolin, the component composition ratio Si
The O ₂ / Al ₂ O ₃ * was determined so that the molar ratio was 4.0. SiO _{2 in} the slurry solution after the first hydrothermal reaction step
Table 7 shows the concentration (silicate ion concentration), the amount of metakaolin added, and the cation exchange capacity of the finally produced artificial zeolite.

[0041]

[Table 6]   Metakaolin composition:   Ingredient CaO Al2O3 SiO2 MgO T-Fe   wt% 0.3 45.0 52.9 0.1 0.2

[0042]

Table 7 after the first raw material first hydrothermal reaction SiO ₂ concentration metakaolin amount CEC Fly ash 75 g / L 42 g 250 Ash 120 g / L 69 g 385 silica sand washing waste soil 40 g / L 23 g 195 waste Keso soil 150 g / L 87 g 392 Waste casting sand 50g / L 29g 203 Waste activated clay 170g / L 98g 403 Glass scrap 250g / L 144g 420 (Cation exchange capacity (CEC) is unit meq / 100g)

As shown in Table 7 above, the larger the amount of water glass (silicate ions) produced in the first hydrothermal reaction step, the larger the cation exchange capacity of the manufactured artificial zeolite. Therefore, in the second hydrothermal reaction step, it is understood that the water glass produced in the first hydrothermal reaction step reacts with the added second raw material to efficiently produce the artificial zeolite. Generally, (B) of Table 4
Although the water glass shown in (D) is expensive, in the present invention, water glass is produced from the first raw material in the first hydrothermal reaction step, and the artificial glass is produced using this, so it is inexpensive and efficient. A high-quality artificial zeolite can be obtained. In addition, by producing the artificial zeolite in two steps as described above, the degree of production of water glass is less likely to change, and a stable quality artificial zeolite can be obtained.

[0044]

As described above, according to the present invention,
The artificial zeolite can be efficiently manufactured with stable quality. Further, it is possible to continuously and stably produce zeolite by using waste and unused resources.

   ─────────────────────────────────────────────────── ─── Continued front page    (72) Inventor Junsuke Haruna             2-17-3 Nakanoike, Tokai City, Aichi Prefecture (72) Inventor Akio Itami             645-20 Kuruzumicho, Matsuyama City, Ehime Prefecture (72) Inventor Akiko Hayashi             6781-10 Ryuue, Iida City, Nagano Prefecture F term (reference) 4G073 CB06 FB28 FB45 FC01 FE10

Claims (5)

[Claims] 1. A compositional ratio of SiO ₂ / Al ₂ O ₃ * (A
l ₂ O ₃ * is the sum of the Al ₂ O ₃ equivalent amount contained, that is, the Al ₂ O ₃ component that hydrothermally reacts with the alkaline liquid, and the metal Al and the nitrided Al converted into Al ₂ O ₃ ) The first hydrothermal reaction step is performed using a first raw material having a large composition ratio, and then the intermediate product produced in the first hydrothermal reaction step is added to the first raw material with a composition ratio SiO ₂ / A higher than that of the first raw material.
A method for producing an artificial zeolite, characterized in that the second hydrothermal reaction step is carried out by adding a second raw material having a small l ₂ O ₃ *. 2. The composition ratio of the first raw material SiO ₂ / A
The method for producing an artificial zeolite according to claim 1, wherein l ₂ O ₃ * has a molar ratio of more than 4.0. 3. The composition ratio of the second raw material SiO ₂ / A
The method for producing an artificial zeolite according to claim 1 or 2, wherein l ₂ O ₃ * has a molar ratio of less than 3.3. 4. The processing pressure or temperature of the first hydrothermal reaction step is equal to or higher than the processing pressure or temperature of the second hydrothermal reaction step. The method for producing an artificial zeolite according to the item. 5. A plurality of kinds of raw materials are mixed in a composition ratio SiO ₂
/ Al ₂ O ₃ * with a large raw material group A and the composition ratio SiO
₂ / Al ₂ O ₃ * having a small raw material group B, and one raw material belonging to raw material group A or a mixture of a plurality of raw materials is used as the first raw material, and one belonging to raw material group B A method for producing an artificial zeolite, characterized in that a raw material or a mixture of a plurality of raw materials is used as the second raw material.