JPH0764667B2 - Method for producing slow-acting granular organic fertilizer - Google Patents

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION The present invention relates to the production of a granular fertilizer containing an organic substance, which suppresses microbial decomposition and slows the fertilizer effect by granulating while adding a slurry-like mixture of urea and formaldehyde to an organic fertilizer. It is about the method.

[0002]

2. Description of the Related Art In recent years, there have been increasing demands for improving the safety and quality of agricultural products. Further, in cultivation of horticultural crops, prevention of continuous cropping failures such as soil diseases has become an important issue. For this reason, organic fertilizers have been reviewed, and the amount used has been increasing year by year. In addition, since organic fertilizers are slower than inorganic fertilizers, there are labor-saving effects on fertilization work, such as non-additional fertilizer cultivation and two consecutive crops with one fertilization. The improvement will reduce the runoff of fertilizer components and will have a positive impact on environmental issues. With the recent spread of mechanical fertilization and mulching cultivation, granular organic matter-containing fertilizers have been produced and put to practical use in order to prevent uneven seeding and to apply fertilizers efficiently.

[0003]

However, in the case of organic fertilizers, particularly in the case of vegetable oil dregs fertilizers, problems such as germination damage immediately after fertilization and growth failure such as poor survival are problematic. In addition, organic fertilizers are decomposed by microorganisms to be mineralized, but the mineralization generally reaches about 40% of the initial amount, and thereafter,
Continue gradual mineralization. Since the initial degradability is high, additional fertilization is required when the cultivation period is long. It is considered that the initial growth failure is caused by the generation of inhibitory substances such as the rapid decomposition of organic fertilizers and the organic acids generated during mineralization. Furthermore, since organic fertilizers alone have low components, the amount of fertilizer applied is large, and the amount of fertilizer application is increased.

In order to slow the fertilizer effect, a method has been developed for suppressing the elution of fertilizer components by coating the surface of the inorganic fertilizer with sulfur, other inorganic substance powder, thermoplastic resin, thermosetting resin or the like. Some of them have been put to practical use. But,
Fertilizers coated with powders of inorganic substances such as sulfur have problems in coating performance, and sufficient elution control is not performed.
In addition, fertilizers using a thermoplastic resin, a thermosetting resin, or the like as a covering material have a high cost and are difficult to use in general horticultural crops in terms of profit. In addition, since elution is suppressed in the early stage, the fertilizing effect at the time of initial growth is not sufficient, and in some cases, an inorganic fertilizer is also applied at the time of fertilizing to supplement the fertilizing effect. Further, since the coating resin has almost no decomposability, the shell of the resin may remain in the soil for a long period of time, or a harmful solvent such as tetrachloroethylene may be used during the production, which may adversely affect the environment. Further, in the cultivation of high-quality horticultural crops, it is necessary to use organic fertilizers in combination, resulting in poor work efficiency.

From these things, in addition to the safety possessed by organic fertilizers, the appearance of granular organic fertilizers having improved microbial degradability and being slowed down has been desired.

As a means for improving the quality of organic fertilizer, a method of adding a urea-formaldehyde mixture in the form of a slurry to an organic fertilizer, or a method of producing a compound fertilizer containing slow-release nitrogen, has been used at the time of mixing urea and formaldehyde. Several methods of mixing fertilizer raw materials have been proposed.
(Japanese Examined Patent Publication No. 63-288878, Japanese Patent Laid-Open No. 16068/1990)
5, Japanese Patent Publication No. 2-54315).

However, the above method is intended to prevent the decomposition of highly water-containing organic matter, and as a result, a fertilizer containing ureaform is produced. In this invention urea /
It has been specified that the molar ratio of formaldehyde is 1.33 or more. With such a large molar ratio, the amount of free urea not contained in the reaction system at the time of condensation increases, and the quality of ureaform as a slow-release fertilizer is poor.

In the above method, the purpose is to prevent the growth damage of the crop by applying the organic fertilizer, but the urea / formaldehyde molar ratio is suppressed to 1.32 or less, which is the opposite of the above method. A mixture of urea and formaldehyde having such a small molar ratio rapidly undergoes a condensation reaction unless the reaction conditions are controlled to highly resinify, and thus ureaform, which is hardly decomposable and has no fertilizing effect, is produced. Further, the stability as a slurry is poor, it is difficult to add the slurry, and there are problems in the storability of the slurry and the uniform dispersion during granulation of fertilizer, but a solution to such a problem has not been shown.

Further, in the above method, it is pointed out that it is difficult to mix urea and formaldehyde and stabilize them in the form of a slurry for a long period of time, but a specific solution to them is not shown. In addition, specific examples of land fertilizers are inorganic fertilizers, and the optimum granulation water content is relatively low. For this reason,
If a high-moisture slurry-like urea-formaldehyde mixture is used, the water content becomes excessive and granulation becomes difficult, so the usage ratio is greatly limited.

In view of the above situation, the inventors of the present invention have conducted extensive studies in order to suppress the microbial decomposition and mineralization of organic fertilizers to give the organic fertilizer a slower effect.
To the organic fertilizer, slurry urea mixed in a specific molar ratio condition, a condensation reaction during granulation and drying of fertilizer particles under strictly controlled conditions while adding a mixture of formaldehyde, and by urea formation, It was found that the fertilizer particles were uniformly filled with ureaform, which has a high slow release effect, the invasion of microorganisms was controlled, and the fertilizer effect could be moderately slowed down. The invention was completed.

[0011]

According to the present invention, urea and formaldehyde are mixed at a urea / formaldehyde molar ratio of 1.0.
~ 1.4 and add an alkaline substance
Then, the slurry obtained by mixing under conditions of pH 6.7 to 7.3 is added to the organic fertilizer, and then the pH in the granulation step from the start of granulation to at least immediately before the end of granulation is maintained at 5 to 6 And, a method for producing a slow-acting granular organic fertilizer characterized by performing granulation and drying at a temperature of 40 to 80 ° C. during granulation and 80 to 90 ° C. during drying, more preferably in the granulation step. Immediately before the end of granulation, raise the pH to 6.7 to 7.3,
This is a method of performing the subsequent granulation and drying steps within this pH range. Here, just before the end of granulation, counting from the end of granulation,
It refers to the time point up to 10% before the entire granulation step period.

The organic fertilizer used in the present invention includes bone meal, skin meal, rapeseed meal, soybean meal, dried microbial fertilizer,
There are no particular restrictions on the fish residue. Inorganic fertilizer,
For example, lime superphosphate and the like are sticky, and when granulated with a slurry-like mixture of urea and formaldehyde, they become large particles. On the other hand, it has been difficult to granulate an organic fertilizer by itself because of its low specific gravity and low cohesive strength, but it can be granulated easily by utilizing the adhesiveness of the condensate after the methyleneation reaction. In addition, the physical buffering action of the organic fertilizer facilitates the control of water content during granulation, and also has the effect of alleviating the tackiness of the condensate after the methyleneation reaction, preventing solidification and obtaining good granules. As described above, the present invention exerts a special effect by granulating while adding a slurry-like mixture of urea and formaldehyde in the presence of an organic fertilizer, and is a method particularly suitable for granulating an organic fertilizer. However, such organic fertilizer may be mixed with an appropriate amount of inorganic fertilizer. The inorganic fertilizer to be mixed is not particularly limited, such as urea, ammonia sulfate, ammonium phosphate, lime superphosphate, potassium sulfate, and potassium chloride. In the case of mixed fertilizer, the content of organic fertilizer in the total fertilizer is appropriately 20% by weight to 100% by weight, but in order to produce a stable slow-release granular organic fertilizer, The content is preferably 50% by weight to 100% by weight.

The slurry-form urea-formaldehyde mixture in the present invention has a molar ratio of urea to formaldehyde of 1.0 to 1.4, preferably 1.2 to 1.3. The water content is preferably 35% by weight to 45% by weight.

The pH at the time of forming the slurry is adjusted to the range of 6.7 to 7.3. This is necessary to secure the stability of the slurry, the storability, the fluidity during pipe transportation, and the dispersibility when mixed with other fertilizer raw materials. When urea and formaldehyde are mixed in the above molar ratio, the acidity is strong and the condensation reaction immediately proceeds to solidify and the slurry state cannot be maintained.
The pH should be adjusted with ammonia water, alkali such as MgO, KOH, etc.
It is possible to adjust to a desired range by adding a resinous substance .

The temperature at which the slurry is generated can be room temperature. It is usually stored at 30 ° C or lower with stirring.

The slurry-like urea / formaldehyde mixture slurry produced under such conditions is added to the organic fertilizer, and granulated and dried to produce ureaform having a high slowing effect due to the condensation reaction, and the granular organic fertilizer is produced. can get. The conditions at the start of granulation are pH 5 to 6 and temperature 40 to 80 ° C.
Done in. The pH can be adjusted with a sulfuric acid aqueous solution, a phosphoric acid aqueous solution, or the like. In the present invention, the pH buffering action of the organic fertilizer allows the pH of the mixture to be adjusted slowly and the methyleneation to proceed slowly.

The pH may be kept at 5 to 6 until the final stage of granulation and until the subsequent drying step, but in a more preferred embodiment, most of the granulation step is pH.
After granulating while keeping at 5-6, pH immediately before the end of granulation
The pH is raised to 6.7 to 7.3, and the final step of granulation and the drying step are performed within the above pH range. By thus adjusting the pH stepwise, it is possible to promote the resinification in the initial stage and suppress the resinification thereafter, so that a granular fertilizer having an excellent slowing effect can be obtained, which is more preferable.

The granulation and drying temperature is 40 to 80 ° C. during granulation,
The temperature is set to 80 to 90 ° C during drying. Granulation temperature 40 to 80 ° C
By keeping the value at 1, the condensation reaction is promoted, and the condensation reaction can be performed in a short time. However, if it is carried out at a temperature higher than this range, resinification will proceed too much and high-quality slow-release fertilizer cannot be obtained.

In the drying process, the condensation reaction is terminated by evaporating the water content while continuing the condensation. Drying temperature is 8
When the temperature is 0 ° C or lower, sufficient drying is not performed, but when the temperature is higher than 90 ° C, it is highly resinified and ureaform having no fertilizing effect is produced, which is not preferable.

The reaction time is 20-40 both during granulation and during drying.
It is preferable to carry out in minutes. Since the condensation reaction does not proceed too much, it is necessary to complete the reaction in a relatively short time.

In the condensation reaction, 1 is used as an acid catalyst if necessary.
% Phosphoric acid aqueous solution, 1% sulfuric acid aqueous solution and the like may be used, but the use of a catalyst is not essential.

The amount of the slurry-like urea and formaldehyde mixture added when granulating the organic fertilizer varies depending on the ratio of the organic fertilizer, the type and the ratio of the organic fertilizer to be mixed, and the type, but it is usually 10 to the fertilizer. % To 60% by weight. However, in order to produce a stable slow-moving granular organic fertilizer, the amount of the slurry-like urea-formaldehyde mixture used is preferably 40 to 60% by weight based on the fertilizer.

The granulating apparatus can be arbitrarily selected from the commonly used rotary cylinder type granulator, pellet type granulator, briquette type granulator and the like. Further, as the drying device, an appropriate model may be selected from a rotary cylinder type drier, a fluidized bed type drier, a band type drier and the like.

[0024]

EFFECTS OF THE INVENTION The present invention has the following effects by granulating while adding a slurry urea-formaldehyde mixture to powder manure under the above-mentioned specific production conditions.

(1) A relatively low urea / formaldehyde molar ratio reduces the proportion of free urea.

(2) However, if the above-mentioned molar ratio is simply lowered, there is a risk of highly condensing into ureaform having no fertilizing effect, but in the present invention, pH and temperature are strictly controlled, and slurry form is obtained. Stability and storability are given to the mixture of urea and formaldehyde, and the reaction is terminated in a short time, and the pH is buffered by the organic fertilizer.
Is slowly adjusted and the methyleneation proceeds slowly, so that ureaform having a high proportion of the slow-release nitrogen portion can be uniformly dispersed in the fertilizer grains.

(3) Due to the physical buffering action of the organic fertilizer, the permissible range of water content of the granulated product is increased, and the control of water content during granulation becomes easy. In addition, due to the viscosity-reducing effect of the organic fertilizer during granulation, the adhesion of the condensate of the condensate after the methyleneation reaction is alleviated in the device and between the granules is reduced. In addition, a special device is not required for drying, the drying energy can be reduced, and the productivity can be improved and the production cost can be reduced.

(4) Further, by utilizing the adhesiveness of the condensate obtained after the methyleneation reaction of the organic fertilizer, which is generally difficult to granulate, the granulating property is improved and low moisture granulation becomes possible. It reduces the drying energy.

(5) By thus uniformly filling the granular fertilizer with ureaform, contact between the organic fertilizer in the granular fertilizer and the microorganisms in the soil is limited, and microbial decomposition is suppressed. Ureaform is gradually degraded by microorganisms,
Since the contact area between the organic fertilizer and the soil gradually expands, fertilization effect appears. As described above, fertilizer has an ideal slow release effect due to the dual effect of slowing down ureaform and suppressing microbial degradation by limiting contact between organic fertilizer and soil.

(6) Since all the raw materials are ordinary fertilizer raw materials, the resin shell does not remain in the soil unlike the resin-coated fertilizer.

(7) Due to these effects, it becomes possible to produce granular organic fertilizer having a high slow release rate, which is suitable for cultivation of high quality crops.

[0032]

EXAMPLES The present invention will be specifically described with reference to the following examples. First, in Example 1 and Comparative Examples 1 to 3, the influence of the production conditions of the urea / formaldehyde condensate on the physical properties of the condensate was investigated.

Example 1 150 g of urea and a concentration of 37 were added so that the molar ratio of urea / formaldehyde was 1.25.
162 g of a wt% aqueous formaldehyde solution was mixed and placed in warm water at a temperature of 30 ° C. with stirring.

The pH was adjusted to 7.2 by adding magnesium oxide.
And adjusted to 30 ° C. for 60 minutes. A 40 wt% aqueous citric acid solution was added to adjust the pH to 6.0, and the mixture was allowed to stand at 40 ° C. for 36 minutes. Add magnesium oxide and p
The H was adjusted to 7.2, a condensation reaction was carried out at 40 ° C. for 4 minutes, and then dried at 90 ° C. to obtain a product.

The total amount of nitrogen in the obtained product, ammonia nitrogen, urea nitrogen, cold water insoluble nitrogen (nitrogen insoluble in water at 25 ± 2 ° C.), thermal buffer insoluble nitrogen (pH 7.5 ± 0.2)
(Insoluble nitrogen in the boiling phosphate buffer solution) was measured, and the activity coefficient was calculated by the following calculation method. The results are shown in Table 1.

Comparative Example 1 150 g of urea and 101 g of an aqueous formaldehyde solution having a concentration of 37% by weight were mixed so that the urea / formaldehyde molar ratio was 2.0, and the mixture was placed in hot water at a temperature of 30 ° C. with stirring. In the following procedure, the condensation reaction was performed in the same manner as in Example 1 to obtain a product. The same measurement as in Example 1 was performed on the obtained product. The results are shown in Table 1.
Are also shown.

[Comparative Example 2] Urea and an aqueous formaldehyde solution having a concentration of 37% by weight were mixed in the same amount and operation as in Example 1, and the mixture was stirred as it was without adjusting the pH as in Example 1. The product was left for 60 minutes at 30 ° C., then for 40 minutes at 40 ° C., and then dried at 90 ° C. to obtain a product. The pH during the condensation reaction was 4.2. For the obtained product, the total amount of nitrogen, cold water-insoluble nitrogen, and heat buffer solution-insoluble nitrogen were measured in the same manner as in Example 1 to calculate the activity coefficient. The results are also shown in Table 1.

Comparative Example 3 The same operation as in Example 1 was carried out except that the condensation reaction temperature and the drying temperature were 100 ° C.
Got the product. The total amount of nitrogen in the product, cold water insoluble nitrogen, and thermal buffer solution insoluble nitrogen were measured, and the activity coefficient was calculated. The results are also shown in Table 1.

[0039]

[Table 1]

As shown in Table 1, in Example 1 of the present invention, by reducing the urea / formaldehyde molar ratio, the product obtained was contained in the reaction system as compared with the product obtained in Comparative Example 1. There is a small proportion of free urea and a large proportion of nitrogen that is soluble in the thermal buffer. In addition, by controlling the pH and the reaction temperature, Comparative Examples 2-3
It was confirmed that the activity coefficient was higher than that of the product obtained in 1.

[Example 2] 1350 g of rapeseed oil residue, 510 g of deboned bone powder, 450 g of steamed hair powder, dried cell fertilizer 2
10 g were mixed, and the mixture had a urea / formaldehyde molar ratio of 1.25 and had a pH of 7.2 with magnesium oxide.
The mixture was allowed to stand for 30 minutes at 30 ° C. for 60 minutes, and 1050 g of a slurry-like mixture of urea and formaldehyde was added, and granulation was performed with a plate-type granulator while adding water. At that time, the granulation operation was performed while adding a 70 wt% sulfuric acid aqueous solution so that the pH of the granulated product was 6.0.

After the granulation operation, the granulated product was placed in a thermostat box dryer at 80 ° C. and dried. The obtained dried granules were sieved with a sieve of 2 mm and 4 mm, the granules of 2 to 4 mm were used as product granule fertilizers, and the weight% of the product granule fertilizers to the total dry granules was used as the product yield. Further, 20 grains were arbitrarily taken out from the product granular fertilizer, the hardness was measured with a Kiya type hardness meter, and the average grain hardness was determined. These results are shown in Table 2.
Shown in. Further, while adding water to 200 g of the above-mentioned compounding ratio at any time, the change of the rotational resistance value was measured by a Yamazaki type rotational torque meter. The results are shown in Fig. 1.

[Comparative Example 4] Instead of the organic fertilizer mixture of rapeseed meal, deboning powder, steamed hair powder and dried bacterial cell fertilizer used in Example 2, 804 g of diammonium phosphate, 684 g of ammonium sulfate and 750 g of potassium chloride. Was mixed with the mixture of urea and formaldehyde used in Example 2, and no water was added, and 40% by weight citric acid aqueous solution was used instead of 70% by weight sulfuric acid aqueous solution. The product granular fertilizer was produced in the same manner as in 2, and the same measurement as in Example 2 was performed. The results are also shown in Table 2 and FIG.

[Comparative Example 5] 1350 g of rapeseed meal, 510 g of debris powder, 450 g of steamed hair powder, dried cell fertilizer 2
While mixing 10 g and adding water without adding a mixture of urea and formaldehyde, a product granular fertilizer was manufactured in the same manner as in Example 2 and the same measurement was performed. The results are also shown in Table 2 and FIG.

[0045]

[Table 2]

As shown in Table 2, in Example 2 of the present invention, a granular product fertilizer having a good product yield and a good product hardness after drying was obtained, but in Comparative Example 4, the total amount was 4 mm or more, and a large grain was obtained. No product granular fertilizer was obtained. In addition, the product of Comparative Example 5 in which only the organic fertilizer was granulated was inferior in product yield and product hardness as compared with Example 2.

Further, as is clear from FIG. 1, in Comparative Example 4 in which the inorganic fertilizer was used, the amount of water exceeded the peak of the rotation resistance value when the raw materials were mixed. This allows
It was confirmed that the physical buffering effect of the inorganic fertilizer was not sufficient to produce granular fertilizer using the urea-formaldehyde mixture in slurry form.

The rotational resistance value measured in Example 2 is
A peak was obtained when the water content was lower than the rotational resistance value measured in Comparative Example 5 in which only the organic fertilizer was granulated. From this, it was confirmed that when granulating an organic fertilizer using a slurry-like urea-formaldehyde mixture, it is possible to granulate with a lower water content than when granulating an organic fertilizer without using this. .

[Example 3] 650 g of deboned powder, 450 g of steamed leather powder, 450 g of rapeseed meal, castor oil meal 3
10 g were mixed, and the mixture had a urea / formaldehyde molar ratio of 1.25 and had a pH of 7.2 with magnesium oxide.
Urea in the form of slurry, which was adjusted to
384 g of formaldehyde mixture was added, and granulation operation was performed for 40 minutes at 40 ° C. with a dish-type granulator while adding water.
At that time, 70% by weight sulfuric acid aqueous solution was added at the same time as the start of the granulation so that the pH of the granulated product became 6.0, and the pH of the granulated product was adjusted to 7.2 4 minutes before the end of the granulation. Magnesium oxide was added.

The granulated product after the granulation operation was placed in a thermostat box dryer at 80 ° C. and dried. The obtained dried granules were sieved to 2 mm and 4 mm, and the granules of 2 to 4 mm were subjected to the mineralization test as product granular fertilizers. The mineralization rate was measured by the following method. The results are shown in Table 3.

Mineralization Test Method Air-dried soil of upland field soil (Kamikawa alluvial soil) was sieved with a 2 mm sieve and tested under a sieve. 50 g of dry soil (N50 mg / 100 g dry soil) is mixed with an equivalent amount of the above-mentioned granular fertilizer, and the mixture is put into a 200 ml polybin, and the maximum water capacity is 5
Water is added to 0%, the lid is closed, and the mixture is allowed to stand at 30 ° C. After a predetermined period of time, the soil containing the sample is transferred to a total volume of 1 liter of polybin, and 500 ml of 10% KCl aqueous solution is added,
Shake for 30 minutes, and analyze 50 ml of the filtrate for ammonia nitrogen (AN) and nitrate nitrogen (NN) by a steam distillation method. From this, the mineralization rate is calculated by the following formula.

Comparative Example 6 225 g of urea and a concentration of 37 were added so that the molar ratio of urea / formaldehyde was 1.25.
243 g of a weight% formaldehyde aqueous solution was mixed and placed in warm water of 30 ° C. with stirring. The pH was adjusted to 7.2 by adding magnesium oxide, and the mixture was left at 30 ° C. for 60 minutes. The pH was adjusted to 6.0 by adding 40% by weight aqueous citric acid solution and left at 40 ° C. for 36 minutes. Magnesium oxide was added to adjust the pH to 7.2, a condensation reaction was carried out at 40 ° C. for 4 minutes and then dried at 80 ° C. to obtain ureaform.

228 g of the above-mentioned ureaform and demolition powder 6
50g, steamed leather powder 450g, rapeseed oil residue 450g,
310 g of castor oil cake was mixed and granulated with a dish granulator for 40 minutes at 40 ° C. while adding water. After the granulation operation, put the granulated product in a thermostat box dryer at 80 ° C,
Dried. The obtained dried granules were sieved in the same manner as in Example 3, and the granules of 2 to 4 mm were used as product granule fertilizers for the mineralization test. The results are also shown in Table 3.

[0054]

[Table 3]

As shown in Table 3, the product obtained by the method of the present invention in which the slurry-like mixture of urea and formaldehyde was added to the organic fertilizer and granulated was the organic fertilizer after the ureaform of Comparative Example 6 was condensed. Compared to the product obtained by mixing, the mineralization rate is slower and the fertilizing effect is slower.

[Brief description of drawings]

FIG. 1 is a diagram showing a relationship between a water content and a rotation resistance value of an organic fertilizer granule according to the method of the present invention and a granule according to another method.

[Explanation of Codes] Organic Fertilizer Granules of the Present Invention (Example 2) Inorganic Fertilizer Granules (Comparative Example 4) Organic Fertilizer Granules Granulated without Using a Urea / Formaldehyde Mixture (Comparative Example 5)

─────────────────────────────────────────────────── ─── Continuation of the front page (51) Int.Cl. ⁶ Identification number Reference number within the agency FI Technical indication C05F 1:00 5:00 11:08) (72) Inventor Tomotaka Asano 3-chome, Higashiikebukuro, Toshima-ku, Tokyo No. 1-1, Asahi Industry Co., Ltd. (72) Inventor Yoshihiko Kubo, 1-1-1, Higashiikebukuro, Toshima-ku, Tokyo Asahi Industry Co., Ltd. (56) Reference JP-A-2-160685 (JP, A) Flat 2-54315 (JP, A)

Claims (2)

[Claims] 1. Urea and formaldehyde are mixed with urea / formaldehyde.
So that the molar ratio of mualdehyde is 1.0 to 1.4
And adding an alkaline substance to obtain a pH of 6.7 to 7.3.
The slurry obtained by mixing under the conditions of is added to the organic fertilizer, and then the pH in the granulation step from the start of granulation to at least immediately before the end of granulation is kept at 5 to 6 and at the time of granulation 40 to
A method for producing a slow-acting granular organic fertilizer, which comprises performing granulation and drying at a temperature of 80 ° C and a temperature of 80 to 90 ° C during drying. 2. The pH of the granulation step immediately before the end of granulation is 5
~ 6, pH in the subsequent granulation and drying process
Is maintained at 6.7 to 7.3, The method for producing a slow-acting granular organic fertilizer according to claim 1, characterized in that.