KR102484476B1 - O/W Stick-Type Clay Mask Cosmetic Composition Containing Water - Google Patents

Abstract

The present invention relates to an oil-in-water emulsified stick-type clay mask cosmetic composition, and more particularly, to an oil-in-water emulsion stick-type clay mask cosmetic composition having excellent product stability and low skin irritation.
The water-in-water emulsified stick-type clay mask cosmetic composition according to the present invention is an oil-in-water emulsion stick-type clay mask comprising sodium stearate, an oil phase hardness former, an aqueous phase hardness former, an emulsion stabilizer, a bulking agent, an oil phase part, a pH adjusting agent and an aqueous phase part. In the cosmetic composition, the oily hardness forming agent is polyethylene wax, paraffin and microcrystalline wax, and the emulsion stabilizer is characterized in that microcrystalline cellulose and cellulose gum.
The water-in-water emulsified stick-type clay mask cosmetic composition according to the present invention is obtained by adding a bulking agent, a specific component of an oil phase hardness forming agent, and an emulsion stabilizer in a specific ratio to a composition containing a sodium stearate solidifying agent, thereby forming the composition in water. By stabilizing by type, the stability against pH and moisture loss is excellent, and the spreadability and drying speed are also excellent.

Description

Oil-in-water emulsion stick type clay mask cosmetic composition {O/W Stick-Type Clay Mask Cosmetic Composition Containing Water}

The present invention relates to an oil-in-water emulsified stick-type clay mask cosmetic composition, and more particularly, to an oil-in-water emulsion stick-type clay mask cosmetic composition having excellent product stability and low skin irritation.

Since the skin covers the surface of the body, there are many opportunities for direct contact with stimuli from the outside or various pathogens, and is strongly influenced by the body. To easily maintain and improve skin health, massage or mask packs are used. Animal proteins such as eggs have been mainly used as cosmetic and massage packs in the past, but gel-type cosmetics in which skin nutrients are added to water-soluble polymers have been developed and are widely used. Natural packs using natural fruits and vegetables are also widely used. . In addition, recently, products using loess, clay, charcoal, elvan, and illite that generate far-infrared rays and negative ions have been developed and used in human life exposed to various pollution and environmental factors, and are used to prevent skin diseases and various attempts are being made to improve it.

In particular, research has been conducted on clay packs mainly made of clay/mud containing bentonite and germanium, which are used as raw materials for various minerals and cosmetics, and ocher packs mainly made of ocher, which has effects such as toxin removal and far-infrared radiation. and is also sold in the market.

Depending on the formulation and method of use, there are peel-off type packs that remove the dried film, wash-off type packs that remove the pack with water after applying the pack agent, tissue-off type packs that wipe off with a tissue, and sheet soaked in emulsion. It can be classified as a sheet type pack. Among them, the wash-off type pack is one of the most commonly used pack formulations because it is less irritating, convenient to use, and has excellent pore waste removal and dead skin care functions because the contents can be removed by washing the face after applying the pack agent and drying it. However, such a wash-off type pack has poor formulation stability, so there is a limit to the amount of ingredients exhibiting efficacy, or problems such as structural instability such as water generation at high or cold temperatures also occur.

Conventional clay (clay) / mud packs are mostly wash-off types that are applied to the skin and washed off when dry. More specifically, a certain amount is taken from a container and spread on the face and the like using hands. However, such a conventional clay pack has problems such as discomfort on the hand and irregular application.

Accordingly, Korean Patent Registration No. 2096009 discloses a stick type clay pack. However, it did not stick to the hand when used and had excellent sebum adsorption effect, but lacked moisturizing power because it did not contain oil, powder ingredients such as clay were not evenly dispersed, and there was a concern that water repellency could occur due to sodium stearate. .

Accordingly, the present inventors have made efforts to solve the above problems, and as a result, when a bulking agent, a specific component of an oil phase hardness former and an emulsion stabilizer are added in a specific ratio to a composition containing a sodium stearate solidifying agent, the composition By stabilizing with an oil-in-water type, it was confirmed that an oil-in-water emulsified stick-type clay mask cosmetic composition having excellent moisturizing power, storage hardness stability, spreadability, and drying speed could be prepared, and the present invention was completed.

An object of the present invention is to provide an oil-in-water emulsified stick-type clay mask cosmetic composition having excellent storage hardness stability, moisturizing power, spreadability and drying speed, and an oil-in-water emulsified stick for clay masks prepared therefrom.

In order to achieve the above object, the present invention is an oil-in-water emulsified stick-type clay mask cosmetic composition comprising sodium stearate, an oil phase hardness former, an aqueous phase hardness former, an emulsion stabilizer, a bulking agent, an oil phase part, a pH adjusting agent and an aqueous phase part. The oily hardness forming agent is polyethylene wax, paraffin and microcrystalline wax, and the emulsion stabilizer is microcrystalline cellulose and cellulose gum.

In the present invention, the water-in-water emulsified stick-type clay mask cosmetic composition contains 1 to 10% by weight of sodium stearate, 1 to 5% by weight of an oily hardness former, 0.1 to 10% by weight of an aqueous phase hardness former, and 0.3 to 5% by weight of an emulsion stabilizer. It is characterized in that it includes 0.1 to 30% by weight of bulking agent, 1 to 30% by weight of oil phase, 1 to 10% by weight of pH adjusting agent, and the remaining amount of water phase.

In the present invention, the mixing ratio (% by weight) of polyethylene wax, paraffin, and microcrystalline wax constituting the oily hardness former is 40 to 60:35 to 55:2 to 8.

In the present invention, the aqueous phase hardness forming agent is characterized in that disteaeth-100 IPDI (disteaeth-100 IPDI).

In the present invention, the mixing ratio (% by weight) of microcrystalline cellulose and cellulose gum constituting the emulsion stabilizer is characterized in that 10 to 20: 80 to 90.

In the present invention, the bulking agent is characterized in that at least one selected from the group consisting of kaolin, titanium dioxide, zinc, PVP and silica.

In the present invention, the oil phase part is characterized in that at least one selected from the group consisting of ester-based oils, hydrocarbon-based oils and vegetable oils.

In the present invention, the irritation reliever is characterized in that at least one selected from the group consisting of peony root extract, portulaca oleracea extract and centella asiatica extract.

In the present invention, the pH adjusting agent is characterized in that salicylic acid, sodium citrate and sodium chloride.

In the present invention, the water phase part is characterized in that at least one selected from the group consisting of purified water and moisturizing agents.

In the present invention, the oil-in-water emulsified stick-type clay mask cosmetic composition is one selected from the group consisting of irritation relievers, alcohols, skin conditioning agents, preservatives, coloring agents, flavoring agents, powders, sequestering agents, and cosmetic nutrients Characterized in that it further comprises at least one species.

The present invention also provides an oil-in-water emulsion stick for a clay mask prepared from the oil-in-water emulsion stick-type clay mask cosmetic composition.

The water-in-water emulsified stick-type clay mask cosmetic composition according to the present invention is obtained by adding a bulking agent, a specific component of an oil phase hardness forming agent, and an emulsion stabilizer in a specific ratio to a composition containing a sodium stearate solidifying agent, thereby forming the composition in water. By stabilizing by type, the stability to pH and moisture loss is excellent, and the spreadability and drying speed are also excellent.

In the present invention, (a) sodium stearate (sodium stearate); (b) an oily hardness former composed of polyethylene wax, paraffin and microcrystalline wax; (c) an aqueous phase hardness former; (d) an emulsion stabilizer composed of microcrystalline cellulose and cellulose gum; (e) bulking agents; (f) an oily portion; When (g) a pH adjusting agent and (h) an aqueous phase part are included in an oil-in-water emulsified stick-type clay mask cosmetic composition, it was confirmed that the pH of the formulation is stabilized and the durability (hardness, perspiration) of the formulation is also improved.

In the present invention, sodium stearate as a solidifying agent (sodium stearate); polyethylene wax, paraffin and microcrystalline wax as oily hardness formers; An oil-in-water emulsified stick-type clay mask cosmetic composition containing microcrystalline cellulose and cellulose gum as an emulsion stabilizer was prepared, and stability (perspiration), skin irritation, and texture of the formulation were evaluated. As a result, it was confirmed that the stability (perspiration), skin irritation, and texture of the formulation were excellent.

Accordingly, in one aspect, the present invention provides an oil-in-water emulsified stick-type clay mask cosmetic composition comprising sodium stearate, an oil phase hardness former, an aqueous phase hardness former, an emulsion stabilizer, a bulking agent, an oil phase part, a pH adjuster and an aqueous phase part, The oil-in-water emulsified stick-type clay mask cosmetic composition is characterized in that the oily hardness forming agents are polyethylene wax, paraffin, and microcrystalline wax, and the emulsion stabilizer is microcrystalline cellulose and cellulose gum.

In the present invention, the sodium stearate is for solidifying the formulation, and may be used in an amount of 1 to 10% by weight, preferably 2 to 5% by weight, based on the total composition. If the content of sodium stearate is less than 1% by weight, the solidification effect is insignificant, and if it exceeds 10% by weight, the hardness is too hard, resulting in poor usability or high PH, resulting in low product stability and high skin irritation. safety is also low.

In the present invention, the hardness forming agent is to maintain the hardness of the formulation and prevent sweating, and the aqueous phase hardness forming agent is characterized in that disteaeth-100 IPDI (disteaeth-100 IPDI), oily hardness Forming agents are characterized by polyethylene wax, paraffin and microcrystalline wax.

Of the total composition, the aqueous phase hardness forming agent may be used in an amount of 0.1 to 10% by weight, preferably 0.5 to 3% by weight, and if it is out of this range, the application property may be significantly reduced or the stick-type formulation itself may not be formed.

The mixing ratio (% by weight) of polyethylene wax, paraffin, and microcrystalline wax constituting the oily hardness former is preferably 40 to 60:35 to 55:2 to 8. When the mixing ratio is out of the range, the hardness is increased and the application property is remarkably deteriorated, and there is a problem that the sweating phenomenon may be noticeable.

Of the total composition, the oily hardness former may be used in an amount of 1 to 5% by weight, preferably 1 to 4% by weight, and if it is out of this range, the spreadability may be significantly reduced or the stick-type formulation itself may not be formed.

The emulsion stabilizer in the total composition may be used in an amount of 0.3 to 5% by weight, preferably 0.5 to 3% by weight. If the emulsion stabilizer is less than 0.3% by weight, the dispersion stability is not good and the sweating phenomenon may be intensified, and if it exceeds 5% by weight, the feeling of use and spreadability are significantly reduced, and rather, powder aggregation and viscosity at high temperatures There is a difficult problem when charging by rising. The mixing ratio (wt%) of microcrystalline cellulose and cellulose gum constituting the emulsion stabilizer is preferably 10-20: 80-90.

In the present invention, the bulking agent is for skin protection, skin soothing and sebum management effects, and kaolin, titanium dioxide, zinc, PVP, silica, etc. may be exemplified, but are not limited thereto.

Of the total composition, the bulking agent may be used in an amount of 0.1 to 30% by weight, preferably 10 to 18% by weight. If the bulking agent is less than 0.1% by weight, there is a problem in that moisture evaporation is intensified and the drying rate is significantly reduced during use, and if it exceeds 30% by weight, it is difficult to disperse, the feeling of use and spreadability are not good, and the viscosity is high during filling, so the formulation There is a problem with formation.

In the present invention, the oil phase part may be exemplified by ester oils, hydrocarbon oils, vegetable oils and the like.

Examples of the ester-based oil include Cetyl Ethylhexanoate, Isocetyl Ethylhexanoate, Isocetyl Myristate, Isopropyl Myristate, and Neopentyl Glycol Dicaprate (Neopentyl glycol dicaprate), Hexyl laurate, Triethylhexanoin, Pentaerythrityl tetraoctanonate, Ethylhexyl palmitate, Isononyl isononanoate (Isononyl isononanoate) and the like can be exemplified, and the hydrocarbon-based oils include petroleum-based oils such as liquid paraffin, vaseline and isoparaffins, synthetic oils such as hydrogenated polydecene, synthetic squalane and polybutene, vegetable squalene, etc. Plant-based oils of can be exemplified. The vegetable oils include olive oil, meadowfoam oil, rosehip oil, avocado oil, camellia oil, macademia nut oil, pima Caster oil, jojoba oil, coconut oil, palm oil, and compounds separated from them, such as caprylic/capric triglyceride, can be exemplified. It is not limited to this.

The oil phase part may be used in an amount of 1 to 30% by weight, preferably 1 to 10% by weight, based on the total composition. If the content of the oily phase is less than 1% by weight, it is difficult to play a role as a solvent, and there is a problem in that the water retention effect is lowered when using the product. There is a problem that skin trouble may occur due to the oil content more than necessary.

Since sodium stearate, a solidifying agent used in the present invention, has a high pH, it is necessary to adjust the pH of the composition to 7.0 to 9.0 using a pH adjusting agent in order to stabilize the formulation. Therefore, the present invention is characterized in that a mixture of salicylic acid, sodium citrate and sodium chloride is used as a pH adjusting agent. The pH adjusting agent may be used in an amount of 1 to 10% by weight, preferably 3 to 6% by weight, based on the total composition. If the content of the pH adjusting agent is less than 1% by weight or exceeds 10% by weight, the solid formulation collapses, resulting in product stability problems or increased skin irritation, resulting in product safety problems as well as too high hardness. Applicability can be significantly deteriorated.

In addition, the mixing ratio (wt%) of salicylic acid, sodium citrate and sodium chloride constituting the pH adjusting agent is characterized in that 6.0 to 7.2: 4.5 to 5.4: 89.5 to 87.4. If even one of the three components constituting the pH adjusting agent is missing or out of the mixing ratio, there is a problem in that the formulation collapses at high temperatures, sweating phenomenon, or skin irritation occurs.

In the present invention, the aqueous phase part may include purified water and a moisturizer. Moisturizers can be used in an amount of 0.1% to 30% by weight of the total composition, and purified water is used according to the content of sodium stearate, oil phase hardness former, aqueous phase hardness former, emulsion stabilizer, bulking agent, oil phase, and pH adjusting agent. It can be freely used within the range of being 100% by weight.

Examples of the humectant include methyl propanediol, butylene glycol, glycerin, propylene glycol, ethylhexyl glycerin, 1,2-hexanediol, sorbitol, dipropylene glycol, and hyaluronic acid. It is not limited.

In addition, the water-in-water emulsified stick-type clay mask cosmetic composition according to the present invention may contain additives such as irritation relievers, alcohols, skin conditioning agents, preservatives, coloring agents, flavoring agents, powders, sequestering agents, and cosmetic nutrients as needed. can be further included.

Niacinamide as the skin conditioning agent, disodium EDTA as the sequestering agent, peony root extract, portulaca oleracea extract, centella asiatica extract as the stimulant, and adenosine, vitamin C derivatives, etc. as the cosmetic nutrient. It can be exemplified, but is not limited thereto.

In another aspect, the present invention relates to an oil-in-water emulsion stick for a clay mask made of an oil-in-water emulsion stick-type clay mask cosmetic composition.

The oil-in-water emulsified stick for clay masks of the present invention has the advantages of high storage hardness and stability, excellent spreadability, moisturizing power, and skin stability.

[Example]

Hereinafter, the present invention will be described in more detail through examples. These examples are only for illustrating the present invention, and it will be apparent to those skilled in the art that the scope of the present invention is not to be construed as being limited by these examples.

Examples 1 to 3 and Comparative Examples 1 to 6: Preparation of moisture stick-type sunscreen cosmetics

According to the components and compositions shown in Table 1 below, microcrystalline cellulose, cellulose gum, and PVP were added to purified water heated to 70 ° C. in an aqueous beaker, homomixed for 10 minutes, and uniformly dispersed, and then returned to the aqueous beaker. was heated to 90° C., and sodium stearate, salicylic acid, sodium citrate, and sodium chloride were added, and dissolved and mixed using a paddle mixer slowly at 100 rpm. After completely dissolving, mix with a mixer while adding methyl propanediol, butylene glycol, 1,2-hexanediol, disodium EDTA, peony root extract (manufacturer: radiant), disteares-100 IPDI and purified water. It was stirred at 100 rpm. Caprylic/capric triglyceride, polyethylene, paraffin, and microcrystalline wax were added to an oil phase beaker and heated to 90° C. to completely dissolve them. Next, while gradually introducing the contents of the oil phase beaker into the contents of the water phase beaker, they were uniformly mixed by homomixing at 100 rpm or more for 5 minutes. Thereafter, kaolin, diisostearyl maleate, thio2, and silica were added, and homomixing was performed at 100 rpm or more for 5 minutes. After confirming that the mixture was completely dissolved and dispersed, it was cooled to room temperature to prepare a solidified clay mask cosmetic.

division main ingredient Example 1 Example 2 Example 3 Comparative Example 1 Comparative Example 2 Comparative Example 3 Comparative Example 4 Comparative Example 5 Comparative Example 6 solidifying agent sodium stearate 2.8 2.8 2.8 2.8 2.8 2.8 2.8 2.8 2.8 PH regulator salicylic acid 0.28 0.28 0.28 0.28 0.28 0.28 0.28 0.28 0.28 sodium citrate 0.21 0.21 0.21 0.21 0.21 0.21 0.21 0.21 0.21 sodium chloride 3.71 3.71 3.71 3.71 3.71 3.71 3.71 3.71 3.71 bulking agent kaoline 16 16 16 16 16 16 16 16 16 Diisostearyl Maleate 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 Tio2 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 silica One One One One One One One One One Pvp 2 2 2 2 2 2 2 2 2 pay-per-view Caprylic/Capric Triglyceride 2 2 2 2 2 2 2 2 2 aqueous hardness former Dice Steareth-100 ipedi.i 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 Oily hardness former polyethylene One 1.2 2.9 One One 5 - - 5 paraffin 0.9 1.5 1.8 0.9 0.9 0.9 - 0.9 2.7 microcrystalline wax 0.1 0.1 0.3 0.1 0.1 0.1 - 0.1 0.3 Prime Minister Purified water to 100 to 100 to 100 to 100 to 100 to 100 to 100 to 100 to 100 Methyl Propanediol 6 6 6 6 6 6 6 6 6 Butylene Glycol 3 3 3 3 3 3 3 3 3 1,2-Hexanediol 2 2 2 2 2 2 2 2 2 additive Disodium EDT 0.02 0.02 0.02 0.02 0.02 0.02 0.02 0.02 0.02 Peony Root Extract 0.01 0.01 0.01 0.01 0.01 0.01 0.01 0.01 0.01 oil paint
stabilizator microcrystalline cellulose 0.065 0.26 0.39 - 0.78 0.78 - 0.26 0.26 cellulose gum 0.435 1.74 2.61 - 5.22 5.22 - 1.74 1.74

Test Example 1: Hardness test

The results of measuring the surface hardness of the cosmetic compositions of Examples 1 to 3 and Comparative Examples 1 to 3 and 6 through a rheometer are shown in Table 2 below. Hardness measurement was performed after storage at 25 ° C. for one day after manufacture, and was measured at a depth of 1 cm at a speed of 5 cm / min using a 15 mm diameter adapter.

Example 1 Example 2 Example 3 Comparative Example 1 Comparative Example 2 Comparative Example 3 Comparative Example 6 relative hardness 1008 1052 1015 992 1102 1836 1512 Cutting strength (g/f) 68 95 85 82 96 200 150

Test Example 2: Stability evaluation

Stability evaluation was carried out at room temperature, 35 ° C, 45 ° C for a short period of 2 days, 5 days, 10 days, 20 days and for a long period of up to 3 months, and then the state of the product was observed to evaluate the stability of the product. Based on the evaluation criteria below, perspiration on the surface of the stick formulation sample was visually observed to evaluate stability, and the results are shown in Table 3. Very good condition was marked with ◎, good condition with ○, normal condition with △, and poor condition with X.

Example 1 Example 2 Example 3 Comparative Example 1 Comparative Example 2 Comparative Example 3 Comparative Example 6 sweating room temperature ◎ ◎ ◎ ○ △ ○ ◎ 35°C ○ ◎ ◎ X X ○ ◎ 45°C

○ ◎ ◎ X X ○ ◎

As shown in Table 3, the cosmetic composition prepared by mixing the emulsion stabilizer in an appropriate amount showed very good results in terms of stability.

Test Example 3: Evaluation of the texture of the formulation

After manufacturing products using the cosmetics prepared in Examples and Comparative Examples, a panel of 100 women aged 20-50 judged the degree of moisture, feeling of use, and cleansing power of the O / W moisture mud stick formulation through sensory evaluation. At this time, the usability evaluation score was indicated as 5 points for very good, 3 points for excellent, 0 points for normal, -3 points for bad, and -5 points for very bad. For each individual's evaluation score, the score was calculated by the formula shown below, and the final results are shown in Table 4 below.

Example 1 Example 2 Example 3 Comparative Example 1 Comparative Example 2 Comparative Example 3 Comparative Example 6 moisture 4.1 4 3.4 3.6 1.9 2.2 2.2 spreadability 4 3.2 3.9 3.3 3.2 0.5 -2.2 cleansing power 3.9 4 3.3 2.8 2.4 3.5 3 sebum adsorption 3.9 4.2 4 2.9 3.2 1.2 1.1

As shown in Table 4, Examples 1 to 3 were evaluated as excellent in all items, and specifically, when the dispersion of kaolin and other powder raw materials was better, it was found that the sebum adsorption effect and detergency were improved. This tendency showed a great difference depending on the content or presence of emulsion stabilizers, oil phase components and oil phase hardness formers. In the case of Comparative Example 1, since the emulsion stabilizer was not included, it was evaluated that the dispersion stability was lowered and the spreadability or sebum adsorption ability was lowered. It also received bad reviews. In Comparative Example 3, the hardness was too hard due to the excessive amount of the oily hardness former, and the spreadability was remarkably poor. In the case of Comparative Example 4, the hardness was not formed because the oily hardness former was not included, so it was not evaluated because it could not be made into a stick formulation, Even in the case of Comparative Example 5, the content of the oily hardness forming agent was insufficient, so it was impossible to implement it as a stick formulation. In Comparative Example 6, when the content of paraffin was high and the content of polyethylene was low in the oily hardness former, all of the items such as moisture, spreadability, and sebum adsorption ability received remarkably low scores due to the sticky feeling and high hardness.

Having described specific parts of the present invention in detail above, it will be clear to those skilled in the art that these specific descriptions are only preferred embodiments, and the scope of the present invention is not limited thereby. will be. Accordingly, the substantial scope of the invention will be defined by the appended claims and their equivalents.

Claims (11)

1 to 10% by weight of sodium stearate, 1 to 5% by weight of oil phase hardness former, 0.1 to 10% by weight of aqueous phase hardness former, 0.3 to 5% by weight of emulsion stabilizer, 0.1 to 30% by weight of bulking agent, 1 to 30% by weight of oil phase In the oil-in-water emulsified stick-type clay mask cosmetic composition containing 1 to 10% by weight of a pH modifier and the remaining amount of the water phase, the oil hardness former comprises polyethylene wax, paraffin and microcrystalline wax in a range of 40 to 60:35 55: 2 to 8% by weight, and the emulsion stabilizer is mixed with microcrystalline cellulose and cellulose gum in a ratio of 10 to 20: 80 to 90% by weight. cosmetic composition.
delete delete The oil-in-water emulsified stick-type clay mask cosmetic composition according to claim 1, wherein the aqueous phase hardness forming agent is disteaeth-100 IPDI.
delete The oil-in-water emulsified stick-type clay mask cosmetic composition according to claim 1, wherein the bulking agent is at least one selected from the group consisting of kaolin, titanium dioxide, zinc, PVP, and silica.
The oil-in-water emulsified stick-type clay mask cosmetic composition according to claim 1, wherein the oil phase part is at least one selected from the group consisting of ester-based oils, hydrocarbon-based oils, and vegetable oils.
The oil-in-water emulsified stick-type clay mask cosmetic composition according to claim 1, wherein the pH adjusting agent is salicylic acid, sodium citrate and sodium chloride.
The oil-in-water emulsified stick-type clay mask cosmetic composition according to claim 1, wherein the water phase part is at least one selected from the group consisting of purified water and a moisturizer.
The method of claim 1, wherein the oil-in-water emulsified stick-type clay mask cosmetic composition is selected from the group consisting of irritation relievers, alcohols, skin conditioning agents, preservatives, coloring agents, flavoring agents, powders, sequestering agents, and cosmetic nutrients An oil-in-water emulsified stick-type clay mask cosmetic composition, characterized in that it further comprises at least one.
An oil-in-water emulsion stick for a clay mask made of the oil-in-water emulsion stick-type clay mask cosmetic composition according to any one of claims 1, 4, and 6 to 10.