JP2007215480A - Iron-fortified food composition - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide an iron-fortified food composition, excellent in flavor in a water-insoluble iron salt composition adjusted to minute particles, having secondary aggregation preventing effect in preservation and excellent in workability in production and redispersability in a water phase, in view of the fact that it starts to attach importance to the role of various kinds of minerals with respect to health maintenance and prevention of adult disease caused by mineral dietary intake shortage which is recently pointed out. <P>SOLUTION: This iron-fortified food composition contains water-insoluble iron salt and a chelating agent. The mixing ratio of the water-insoluble iron salt with the chelating agent is 0.05-20 pts.wt. of the chelating agent based on 100 pts.wt. of the water-insoluble iron salt, and the chelating agent is at least one kind selected from the group consisting of metaphosphate and citrate. <P>COPYRIGHT: (C)2007,JPO&INPIT

Description

  The present invention is a water-insoluble iron salt composition adjusted to fine particles, has an excellent flavor, has an effect of preventing secondary aggregation during storage, workability during production, and redispersibility in an aqueous phase The present invention relates to an excellent iron-reinforced food composition.

  In recent years, a shortage of mineral intake has been pointed out, and the role of various types of minerals has started to be emphasized with regard to prevention of adult diseases caused by the cause and maintenance of health.

  Among them, iron is known to exist in a state of being bound to hemoglobin, which is a protein in blood. When iron is deficient, it is supplemented by stored iron in tissues. The state of lack of stored iron is called latent anemia, and it is said that more than 60% of Japanese suffer from it. This tendency is particularly noticeable among high school girls and young adult women, and as a result, many women have iron deficiency anemia.

  The reason for this is thought to be the most derived from eating habits, but in the case of women, anemia due to iron deficiency such as physiological bleeding, increased iron demand due to pregnancy, and insufficient intake due to diet, etc. It is also a characteristic cause that it is in an easy environment.

  In order to eliminate this iron shortage, iron-enriched foods are being sold, and many products that are iron-enriched in milk, soft drinks, etc. are beginning to be sold. For example, in soft drinks for the purpose of strengthening iron, water-soluble iron such as iron lactate, ferrous gluconate and sodium iron citrate, and water-insoluble or poorly soluble iron such as ferric pyrophosphate Used in addition. However, water-soluble iron has a strong iron taste and has a problem in terms of sensuality, so that a large amount cannot be used at one time. In addition, since it is water-soluble, ionized iron has a high reactivity with the stomach wall, and when it is ingested excessively, it may cause ulcers. Moreover, the reactivity with the other component in a drink was also high, and there existed problems, such as precipitation, aggregation, and coloring by a reaction material. In addition, in water-insoluble or sparingly soluble iron, although the iron taste is improved, the specific gravity is as high as 2.75 or more, and when dispersed and added to a beverage, it precipitates in a short time, which is not preferable in terms of aesthetics as a food. was there.

  As a method for improving these, there is a method of mixing ferric pyrophosphate and gum arabic and pulverizing and / or dispersing by a chemical or physical method (for example, see Patent Document 1). Then, secondary agglomeration occurs over time, resulting in coarse particles on the order of microns, and when dispersed and added to beverages, there is a problem of precipitation in a short time. In these methods, when a high-concentration composition is prepared, the viscosity increases due to aggregation of particles, and handling becomes difficult.

Special Table 98/042210 (page 1-45)

  The present invention has been made for the purpose of developing a novel iron-reinforced food composition that does not have the above-mentioned problems.

  As a result of intensive studies to solve the above-mentioned problems, the inventors of the present invention have achieved a good flavor and high taste by adding a chelating agent to a water-insoluble iron salt in the production of an iron-reinforced food composition. It has been found that an iron-reinforced food composition having good dispersibility without cohesion even in concentration can be obtained, and the present invention has been completed. A feature of the present invention is that when a chelating agent is added to a water-insoluble iron salt, a very stable state of charge is formed, and secondary aggregation of particles is suppressed. The object is to produce an iron-reinforced food composition having good flavor and excellent dispersibility without cohesion.

  In addition, one or more selected from lysolecithin, polyglycerin fatty acid ester, soybean polysaccharide, pectin, carrageenan, CM cellulose, modified starch, galactomannan degradation product, gum arabic, and arabinogalactan may be used in combination. More preferred.

  According to the present invention, in the production of a composition for iron-enhanced food, by adding a chelating agent to a water-insoluble iron salt, the iron has good flavor and good dispersibility without aggregation even at high concentrations. A fortified food composition can be provided.

  The iron-enriched food composition of the present invention is characterized by adding a chelating agent to a water-insoluble iron salt. In the present invention, the water-insoluble iron salt is not particularly limited. For example, ferric phosphate, ferrous phosphate, ferric pyrophosphate, ferrous pyrophosphate, ferric hydroxide, In order to provide an iron-reinforced food composition having good dispersibility without aggregation at a high concentration, ferric phosphate and ferric pyrophosphate are preferable. More preferably, it is ferric pyrophosphate. These may be blended singly or in combination of two or more.

  The insolubility of the water-insoluble iron salt used in the present invention is not particularly limited, but from the viewpoint of taste, gastrointestinal mucosal irritation and the like, the test method of the Japanese Seventh Edition Food Additives General Rules 29 In “very difficult to dissolve” (the amount of water required to dissolve 1 g of solute is 1,000 ml or more and less than 10,000 ml) or “almost insoluble” (the amount of water required to dissolve 1 g of solute is 10,000 ml or more) Applicable thing is said, Preferably, it corresponds to "almost insoluble".

The particle size of the water-insoluble iron salt used in the present invention is not particularly limited, but it is preferable to make it as fine as possible, preferably the average particle size is 0.8 μm or less, more preferably 0.6 μm or less, It is more preferable to make ultrafine particles up to 0.4 μm. As a method for forming fine particles, a physical crushing method or a neutral salt-forming method is preferable. As the physical crushing method, a wet pulverizer such as a dyno mill, a sand mill, and a coball mill, an emulsifying / dispersing device such as a nanomizer, a microfluidizer, and a homogenizer, and an ultrasonic disperser can be used. By making the particles fine, an iron-enriched food composition that is extremely stable even in water can be advantageously produced. The method for measuring the average particle size of the water-insoluble iron salt in the present invention is not particularly limited, and examples thereof include laser diffraction / scattering method, dynamic light scattering method, sedimentation method, image analysis method, and the like. From the viewpoint of simplicity, the laser diffraction / scattering method and the dynamic light scattering method are preferable.
In addition, the average particle diameter of the water-insoluble iron salt in the present invention is measured using the following equipment.
Measuring instrument: BECKMAN COULTER LS230 (Laser diffraction / scattering method)
Preliminary dispersion: TOMY ULTRASONIC DISUPTOR UD-200
OUT PUT Scale 5, 5 minutes

  The chelating agent in the present invention is not particularly limited as long as it has chelating ability, but organic acid salts such as citrate, malate, succinate, tartrate, gluconate, and metalin Examples include acid phosphates, condensed phosphates such as polyphosphates, and EDTA salts, which are used alone or in combination of two or more thereof. In order to provide a composition for use, metaphosphate and citrate are preferable, and metaphosphate is more preferable. Examples of the salt include alkali metal salts such as Na and K, ammonium salts, and the like.

  The addition amount of the chelating agent in the present invention is not particularly limited, but it is preferable to contain 0.05 to 20 parts by weight of the chelating agent with respect to 100 parts by weight of the water-insoluble iron salt. 10 to 10 parts by weight is more preferable, and 0.1 to 5 parts by weight is most preferable. When the addition amount of the chelating agent is below this range, secondary aggregation of the particles cannot be completely suppressed, and an iron-reinforced food composition having high dispersion stability may not be obtained. On the other hand, when the addition amount of the chelating agent is more than the range, dissolution of the water-insoluble iron salt occurs, and a metallic taste peculiar to iron is generated in the food to which the composition is added, which may lead to a decrease in flavor.

  The method for adding a chelating agent in the present invention is not particularly limited, but there are a method for dissolving a chelating agent in a dispersion of a water-insoluble iron salt, a method for dispersing a water-insoluble iron salt in an aqueous solution of a chelating agent, and the like. Used.

  In the present invention, the pH of the iron-enriched food composition forms an extremely stable charge state and is an important factor for suppressing secondary aggregation of particles. Specifically, in order to obtain an iron-reinforced food composition having high dispersion stability, the pH of the iron-reinforced food composition when the concentration of the water-insoluble iron salt is adjusted to 12% by weight is 2.8 to 4.2. It is preferable that it is 2.9-4.0, and it is more preferable that it is 3.0-3.8. If the pH of the iron-reinforced food composition is below this range, secondary aggregation of the particles is likely to be promoted, and a dispersion-stable composition may not be obtained. If the pH is above this range, the water-insoluble iron salt is likely to be dissolved, and a metallic taste peculiar to iron may be generated in the food to which the composition is added, leading to a decrease in flavor. The method for adjusting the concentration of the water-insoluble iron salt to 12% by weight is not particularly limited, but when the concentration of the water-insoluble iron salt is 12% by weight or more, it is diluted with ion-exchanged water. It is preferable to adjust to 12% by weight, and when it is 12% by weight or less, a method of concentrating by centrifugation or the like is preferable.

  The form of the iron-enriched food composition in the present invention is not particularly limited, but is preferably liquid or powder. Although it does not specifically limit as a liquid composition, From a viewpoint of handling, it is preferable that the viscosity in 25 degreeC is 20,000 mPa * s or less, and it is more preferable that it is 10,000 mPa * s. . Moreover, an iron reinforcement | strengthening powder composition can be prepared by dry-pulverizing the composition for iron reinforcement | strengthening foodstuffs of this invention as needed. Although there is no restriction | limiting in particular about the dryer used for drying, From a viewpoint of the quality-change prevention of a composition, it is preferable to carry out in a very short time, and it is desirable to use droplet spray type dryers, such as a spray dryer and a slurry dryer. Further, by granulating the powder composition, it is possible to prepare a granule composition having excellent solubility when added to food.

  The content concentration of the water-insoluble iron salt in the iron-reinforced food composition in the present invention is high from the viewpoints of transportation costs necessary for distribution, container costs, etc., and handling when added to foods. Concentrations are desired. The content concentration of the water-insoluble iron salt is preferably 1% by weight or more, more preferably 4% by weight or more, and further preferably 10% by weight or more. In the case of a liquid composition for iron-reinforced food, it is preferably 50% by weight or less from the viewpoint of viscosity and fluidity.

  The preferred concomitant substance in the present invention is not particularly limited. For example, lysolecithin, polyglycerin fatty acid ester, soybean polysaccharide, pectin, carrageenan, CM cellulose, modified starch, galactomannan degradation product, gum arabic, arabinogalactan By using one or more selected from among them, a role of further assisting dispersion stability can be given, and the features of the present invention are exhibited. Further, lysolecithin may be used in combination with one or more selected from polyglycerin fatty acid ester, soybean polysaccharide, pectin, carrageenan, CM cellulose, modified starch, galactomannan degradation product, gum arabic, and arabinogalactan. More preferred.

  Examples of the food containing the iron-enriched food composition in the present invention include secondary flour products represented by cookies, bread, noodles, etc., processed rice products such as white rice, red rice, porridge, cooked rice, livestock meat, fish meat, etc. Processed products and beverages such as soft drinks, dairy drinks, carbonated drinks, alcoholic drinks, etc. can be mentioned, and by adding water-insoluble iron salts to these, it is possible to easily carry out iron nutrition that tends to be insufficient Is possible. Especially in liquid foods, mainly beverages, the addition of water-insoluble iron salt has a very narrow range of application due to the sedimentation of iron components, but it is excellent in flavor and chemically stable according to the present invention. With this, iron can be strengthened.

Example 1
120 g of ferric pyrophosphate (manufactured by Tomita Pharmaceutical Co., Ltd.) and 0.3 g of sodium metaphosphate (manufactured by Yoneyama Chemical Co., Ltd.) were mixed and dispersed in 879.7 g of ion-exchanged water, and this dispersion was mixed with a wet mill Dinomill (WAB MULTI LAB). ) To obtain 1000 g of a 12 wt% ferric pyrophosphate composition. The obtained high-concentration composition had a viscosity as low as 600 mPa · s at 25 ° C., and the fluidity was good. The average particle size was 0.32 μm.

Example 2
120 g of ferric phosphate (manufactured by Wako Pure Chemical Industries, Ltd.) and 0.07 g of sodium metaphosphate (manufactured by Yoneyama Chemical Industries) were mixed and dispersed in 879.93 g of ion-exchanged water. Wet pulverization was performed using MULTI LAB) to obtain 1000 g of a 12 wt% ferric phosphate composition. The obtained high-concentration composition had a sufficiently low viscosity at 25 ° C. of 1,810 mPa · s and good fluidity. The average particle size was 0.38 μm.

Example 3
120 g of ferric pyrophosphate (manufactured by Tomita Pharmaceutical) and 24 g of sodium citrate (manufactured by Tanabe Seiyaku) were mixed and dispersed in 856.0 g of ion-exchanged water, and this dispersion was used using a wet mill DYNOMILL (WAB MULTI LAB). Wet pulverization was performed to obtain 1000 g of a 12 wt% ferric pyrophosphate composition. The resulting high-concentration composition had a sufficiently low viscosity at 25 ° C. of 540 mPa · s and good fluidity. The average particle size was 0.24 μm.

Example 4
120 g of ferric phosphate (manufactured by Wako Pure Chemical Industries, Ltd.) and 6.0 g of sodium metaphosphate (manufactured by Yoneyama Chemical Co., Ltd.) were mixed and dispersed in 874.0 g of ion-exchanged water, and this dispersion was mixed with a wet mill dyno mill (WAB) Wet pulverization was performed using MULTI LAB) to obtain 1000 g of a 12 wt% ferric phosphate composition. The obtained high-concentration composition had a sufficiently low viscosity at 25 ° C. of 450 mPa · s and good fluidity. The average particle size was 0.34 μm.

Example 5
Ferrous pyrophosphate (produced by Tomita Pharmaceutical Co., Ltd.) 120 g, sodium metaphosphate (produced by Yoneyama Chemical Co., Ltd.) 1.0 g, lysolecithin (produced by Taiyo Chemical Co., Ltd.) 0.1 g are mixed and dispersed in ion-exchanged water 878.9 g, and the main dispersion is performed. The liquid was wet pulverized using a wet grinder Dynomill (WAB MULTI LAB) to obtain 1000 g of a 12 wt% ferric pyrophosphate composition. The obtained high-concentration composition had a sufficiently low viscosity at 25 ° C. of 320 mPa · s and good fluidity. The average particle size was 0.30 μm.

Example 6
Ion-exchanged water 899.0 g of ferric pyrophosphate (manufactured by Tomita Pharmaceutical), 0.5 g of sodium metaphosphate (manufactured by Yoneyama Chemical Co., Ltd.), 0.5 g of polyglycerin fatty acid ester (Sunsoft A-14E: manufactured by Taiyo Kagaku) The dispersion was wet pulverized using a wet grinder Dynomill (WAB MULTI LAB) to obtain 1000 g of a 12 wt% ferric pyrophosphate composition. The obtained high-concentration composition had a sufficiently low viscosity at 25 ° C. of 140 mPa · s and good fluidity. The average particle size was 0.28 μm.

Example 7
Ferric pyrophosphate (product of Tomita Pharmaceutical) 120 g, sodium citrate (product of Tanabe Seiyaku) 0.07 g, lysolecithin (product of Taiyo Kagaku) 0.1 g, gum arabic (manufactured by Sankyo Food Industry) 1 g of ion-exchanged water 878. The dispersion was mixed and dispersed in 83 g, and this dispersion was wet-ground using a wet grinder Dynomill (WAB MULTI LAB) to obtain 1000 g of a 12 wt% ferric pyrophosphate composition. The obtained high-concentration composition had a sufficiently low viscosity at 25 ° C. of 220 mPa · s and good fluidity. The average particle size was 0.34 μm.

Example 8
Ferric pyrophosphate (manufactured by Tomita Pharmaceutical) 360 g, sodium metaphosphate (manufactured by Yoneyama Chemical) 4.0 g, lysolecithin (manufactured by Taiyo Kagaku) 0.2 g, polyglycerin fatty acid ester (Sunsoft A-14E: manufactured by Taiyo Chemical) 0.5 g is mixed and dispersed in 635.3 g of ion-exchanged water, and this dispersion is subjected to wet grinding using a wet mill DYNOMILL (WAB MULTI LAB) to obtain 1000 g of a 36 wt% ferric pyrophosphate composition. Obtained. The obtained high-concentration composition had a sufficiently low viscosity at 1540 mPa · s at 25 ° C. and good fluidity. The average particle size was 0.38 μm.

Comparative Example 1
120 g of ferric pyrophosphate (manufactured by Tomita Pharmaceutical) was mixed with 880 g of ion-exchanged water, and this dispersion was wet-ground using a wet grinder Dynomill (WAB MULTI LAB), and 12 wt% ferric pyrophosphate. 1000 g of composition was obtained. The resulting high-concentration composition had a very high viscosity of 25,000 mPa · s at 25 ° C. due to the influence of particle aggregation and was difficult to handle. The average particle size was 1.1 μm.

Comparative Example 2
120 g ferric pyrophosphate (manufactured by Tomita Pharmaceutical Co., Ltd.) and 0.01 g sodium citrate (manufactured by Tanabe Seiyaku Co., Ltd.) were mixed with 8799.99 g of ion-exchanged water, and this dispersion was used with a wet mill DYNOMILL (WAB MULTI LAB). Wet pulverization was performed to obtain 1000 g of a 12 wt% ferric pyrophosphate composition. The resulting high-concentration composition had a very high viscosity of 22,000 mPa · s at 25 ° C. due to the influence of particle aggregation, and was difficult to handle. The average particle size was 1.2 μm.

Comparative Example 3
120 g of ferric pyrophosphate (manufactured by Tomita Pharmaceutical) and 36 g of sodium citrate (manufactured by Tanabe Seiyaku) were mixed with 844 g of ion-exchanged water, and this dispersion was subjected to wet grinding using a wet mill DYNOMILL (WAB MULTI LAB). And 1000 g of 12 wt% ferric pyrophosphate composition was obtained. The obtained high-concentration composition had a sufficiently low viscosity at 25 ° C. of 340 mPa · s and good fluidity, but the whole liquid was colored yellow due to dissolution of ferric pyrophosphate. The average particle size was 0.37 μm.
Table 1 shows the amount of the chelating agent added to 100 parts by weight of the water-insoluble iron salt.

Test example 1
The pH of the water-insoluble iron salt compositions obtained in Examples 1 to 8 and Comparative Examples 1 to 3 was measured under the following conditions.
pH: pH of the iron-enriched food composition when the concentration of the water-insoluble iron salt is adjusted to 12% by weight

Test example 2
The water-insoluble iron salt compositions obtained in Examples 1 to 8 and Comparative Examples 1 to 3 were diluted with ion-exchanged water so that the iron concentration became 50 ppm, and a sensory test was performed with 10 panelists.
Evaluation point Does not taste iron. 0
There is almost no iron taste. 1
Slightly iron taste. 2
It tastes iron. 3
Strengthen iron. 4

Test example 3
The water-insoluble iron salt compositions obtained in Examples 1 to 8 and Comparative Examples 1 to 3 were diluted with ion-exchanged water so that the iron concentration became 50 ppm, and allowed to stand at room temperature for 3 days and 7 days for dispersion. Stability was examined.
Evaluation points were set as follows and evaluated.
Evaluation point Good dispersion state. 0
Some precipitation is seen. 1
The upper layer begins to become transparent and precipitation is observed. 2
The upper layer becomes transparent and a precipitate layer is seen. 3
The upper and middle layers are transparent and there are many precipitated layers. 4
It completely settles and the liquid becomes clear. 5

  As shown in Table 2, the iron-fortified food composition containing 0.05 to 20 parts by weight of the chelating agent with respect to 100 parts by weight of the water-insoluble iron salt has less unpleasant taste peculiar to iron, and It was confirmed that the dispersion stability was high. On the other hand, when no chelating agent is added, and when the addition amount of the chelating agent is 0.05 parts by weight or less or 20 parts by weight or more with respect to 100 parts by weight of the water-insoluble iron salt, flavor or dispersion stability This resulted in problems with sex.

Measurement of serum iron by administration of various iron preparations Test Example 4
10 g of each 12% ferric pyrophosphate composition obtained in Example 1 and Comparative Example 1 was taken and dissolved in 170 g of distilled water to prepare a test solution (Fe: 2 mg / g).

  After 8 groups of 10 10-week-old male SD rats were fasted for 18 hours, the test solution was forcibly orally administered to the rats using a sonde at a rate of Fe: 2 mg / kg per rat. In addition, as a blank, only water was orally administered to rats as described above. After administration, blood was collected from the tail vein after 0, 0.5, 1, 2, 4 or 8 hours, and serum was promptly separated, followed by iron (serum) in serum according to the standard method of International Committe for Standardization in Hematology. The iron) concentration was measured.

  The amount of iron absorbed was determined based on the area under the serum iron curve [(μg / dl) · Hour] 0 to 8 hours after administration of the test solution and the area under the serum iron curve [(μg / dl) · Hour 0 to 8 hours after administration of the blank. ] Difference. The results are shown in Table 4.

  According to this result, compared with the ferric pyrophosphate composition obtained in Comparative Example 1, the ferric pyrophosphate composition containing the chelating agent obtained in Example 1 had iron in serum. The concentration was increased up to about twice, and it was revealed that the iron-enriched food composition of the present invention has an improved bioavailability.

Example 9
The 12 wt% ferric pyrophosphate composition obtained in Example 1 was pulverized with a spray dryer to obtain a 50 wt% ferric pyrophosphate powder composition.

Example 10
1.0 g of the 12 wt% ferric pyrophosphate composition obtained in Example 1 was added to 1 L of apple juice drink and pasteurized by heating to obtain an iron-enriched apple juice drink. (Fe: 3.6 mg / 100 ml)
The obtained beverage was satisfactory in both color and flavor.

Example 11
1.0 L of the 12 wt% ferric pyrophosphate composition obtained in Example 1 was added to 1 L of milk, and heat sterilized to obtain iron-enriched milk. (Fe: 3.6 mg / 100 ml)
The obtained milk had no problems in color and flavor.

Example 12
1.0 L of 12 wt% ferric pyrophosphate composition obtained in Example 1 was added to 1 L of sour milk beverage, and heat sterilized to obtain an iron-fortified sour milk beverage. (Fe: 3.6 mg / 100 ml)
The obtained beverage was satisfactory in both color and flavor.

Example 13
1.0 L of the 12 wt% ferric pyrophosphate composition obtained in Example 1 was added to 1 L of soft drink, and heat sterilized to obtain an iron-reinforced soft drink. (Fe: 3.6 mg / 100 ml)
The obtained drinking water was satisfactory both in color and flavor.

Example 14
To 500 g of tablet powder, 3.3 g of the 50 wt% ferric pyrophosphate powder composition obtained in Example 9 was added, and tableting was performed to obtain an iron-reinforced tablet. (Fe: 1.0 mg / grain)
The obtained tablet was satisfactory in both color and flavor.

  The iron-enriched food composition of the present invention has a good flavor and excellent dispersibility without agglomeration, and is therefore useful as an iron-enriched food composition for foods, and its industrial use The value is great.

Claims (11)

An iron-enriched food composition comprising a water-insoluble iron salt and a chelating agent. The iron-enriched food composition according to claim 1, wherein the mixing ratio of the water-insoluble iron salt and the chelating agent is 0.05 to 20 parts by weight of the chelating agent with respect to 100 parts by weight of the water-insoluble iron salt. . The chelating agent is one or more selected from the group consisting of a metaphosphate and a citrate, and the iron-enriched food composition according to claim 1 or 2. The composition for iron-enriched food according to any one of claims 1 to 3, wherein lysolecithin is used in combination. It is characterized in that one or more selected from the group of polyglycerin fatty acid ester, soybean polysaccharide, pectin, carrageenan, CM cellulose, modified starch, galactomannan degradation product, gum arabic, and arabinogalactan are used in combination. The iron-reinforced food composition according to any one of claims 1 to 4. The iron-enriched food composition according to any one of claims 1 to 5, wherein the water-insoluble iron salt is fine particles having an average particle size of 0.8 µm or less. The iron fortification according to any one of claims 1 to 6, wherein the pH of the iron-fortified food composition when the concentration of the water-insoluble iron salt is adjusted to 12% by weight is 2.8 to 4.2. Composition for food. The iron-enriched food composition according to any one of claims 1 to 7, wherein the form is liquid. The iron-enriched food composition according to any one of claims 1 to 7, wherein the form is powdery. The iron-enriched food composition according to claim 1, wherein the bioavailability of iron is improved. A food comprising the iron-enriched food composition according to claim 1.