Mite repellent and mite-repelling method

Abstract

To provide a mite repellent with high mite-repelling effect and high safety without easily producing dead mites.SOLUTION: A mite repellent contains an extract of a plant of the genus Catalpa in the family Bignoniaceae as an active ingredient. In one example, a mite-repelling method includes releasing the mite repellent into the air. In another example, the mite-repelling method includes application of the mite repellent to a textile product. In another example, the mite-repelling method includes bringing mites into contact with the mite repellent.SELECTED DRAWING: None

Description

[Technical field]

[0001] The present invention relates to a mite repellent and a method for repelling mites. [Background technology]

[0002] Since bedding such as futons, pillows, and sheets cannot be washed frequently at home, they can become breeding grounds for house dust mites such as Dermatophagoides farinae, Dermatophagoides pteronyssinus, and Tyrophagus putrescentiae. Proteins contained in the feces and molted shells of these mites are allergens that cause asthma and atopic dermatitis. Conventionally, synthetic products such as pyrethroid compounds have been widely used as repellents against mites, but the use of ingredients with higher safety or higher repellent effect has been investigated (for example, Patent Documents 1 to 10). [Prior art documents] [Patent documents]

[0003] [Patent Document 1] Japanese Patent Application Publication No. 6-239714 [Patent Document 2] Japanese Patent Application Publication No. Hei 1-193204 [Patent Document 3] JP 2017-39677 A [Patent Document 4] JP 2020-50636 A [Patent Document 5] JP 2020-100579 A [Patent Document 6] Patent Publication No. 2021-17430 [Patent Document 7] Patent Publication No. 2021-54740 [Patent Document 8] Patent Publication No. 2021-54741 [Patent Document 9] Patent Publication No. 2021-54742 [Patent Document 10] JP 2021-130638 A Summary of the Invention [Problem to be solved by the invention]

[0004] However, there is room for improvement in the performance of conventional mite repellents. In particular, the carcasses of mites that live indoors, such as house dust mites, can also cause allergies. Therefore, while the mite repellent effect is high, it is important not to kill the mites so that their carcasses do not appear.

[0005] To provide a mite repellent which has a high mite repellent effect, is highly safe, and hardly produces dead mites, and a method for repelling mites using the mite repellent. [Means for solving the problem]

[0006] In order to solve the above problems, the present inventors have conducted extensive research into the activity of natural ingredients against mites and have discovered that extracts from plants of the genus Catalpa in the family Bignoniaceae show excellent performance, thus completing the present invention.

[0007] The present invention has the following aspects. [1] A mite repellent containing an extract of a plant of the genus Catalpa in the family Bignoniaceae as the active ingredient. [2] The mite repellent according to [1], wherein the plant of the genus Catalpa in the family Bignoniaceae is Catalpa. [3] The mite repellent according to [1] or [2], wherein the extract of a plant of the genus Catalpa in the family Bignoniaceae is at least one extract selected from the group consisting of flowers, branches, fruits, seeds, leaves, stems, roots and bark. [4] The mite repellent according to any one of [1] to [3], wherein the extract of a plant of the genus Catalpa in the family Bignoniaceae is a methanol extract. [5] A method for repelling mites, comprising releasing the mite repellent according to any one of [1] to [4] into the air. [6] A method for repelling mites, comprising applying the mite repellent according to any one of [1] to [4] to a textile product. [7] A method for repelling mites, comprising contacting the mite repellent according to any one of [1] to [4] with mites. Effect of the Invention

[0008] The mite repellent of the present invention has a high mite repellent effect, is highly safe, and is less likely to produce dead mites. According to the method for repelling mites of the present invention, the repelling effect against mites is high, the safety is high, and moreover, the generation of dead mites is reduced. [Brief description of the drawings]

[0009] [Figure 1] FIG. 1 is a cross-sectional view that illustrates a test apparatus used in the examples. [Diagram 2] FIG. 2 is a plan view that illustrates a schematic diagram of a test apparatus used in the examples. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0010] In this specification, a numerical range expressed using "~" means a range including the numerical values ​​before and after "~" as the lower and upper limits. For example, "A~B%" means A% or more and B% or less.

[0011] The mite repellent of the present invention contains an extract of a plant of the genus Catalpa in the family Bignoniaceae as an active ingredient. Examples of plants of the genus Catalpa in the family Bignoniaceae include Catalpa japonica and Catalpa arvensis. Of these, Catalpa japonica is particularly preferred.

[0012] As the raw material for the mite repellent, the whole plant of the Bignoniaceae family Catalpa genus may be used, or a part of the plant may be used. For example, the flowers, branches, fruits, seeds, leaves, stems, roots, and bark may be used. Among them, the flowers and branches are preferably used because they are likely to produce a mite repellent with a high repellent effect. As the raw material for the mite repellent, the whole plant or a part of the plant of the genus Catalpa of the family Bignoniaceae may be used as is, but it is preferably used after being crushed or crushed by a crusher or crusher.

[0013] As the extraction method, a conventionally known method can be used. For example, extraction methods such as squeezing, steam distillation, atmospheric distillation, reduced pressure distillation, solvent extraction, etc. can be used. In one example of the steam distillation method, the leaves or fresh flowers of a plant of the genus Catalpa in the family Bignoniaceae are crushed and soaked in alcohol or hot water for several hours, and then steam distilled, and the distillate oil is collected to obtain an extract.

[0014] In one example of solvent extraction, the leaves or fresh flowers of a plant of the genus Catalpa in the family Bignoniaceae are crushed, heated in a solvent for several hours, and then filtered to obtain a filtrate, which is then concentrated to obtain an extract. The solvent used in the solvent extraction is preferably a polar solvent, such as water, alcohol-based solvents such as ethanol, methanol, butyl alcohol, ethylene glycol, propylene glycol, and glycerin, halogen-containing solvents such as chloroform, ether-based solvents such as dioxane, carbonyl-based solvents such as acetone and ethyl acetate, and mixtures thereof.

[0015] Among these, a methanol extract using methanol as a solvent extraction is preferred.

[0016] The mite repellent may contain only an extract of a plant of the genus Catalpa in the family Bignoniaceae as the active ingredient, or may further contain optional ingredients.

[0017] The mite repellent of the present invention may further contain other mite control ingredients known in the art, which may provide an even more excellent repellent effect.

[0018] Other mite control ingredients include, for example, pyrethroid compounds such as empenthrin, transfluthrin, allethrin, fenothrin, profluthrin, metofluthrin, eminence, pyrethrin I, pyrethrin II, cinerin I, cinerin II, jasmolin I, and jasmolin II; organophosphate agents such as dichlorvos, diazinon, fenitrothion, and malathion; N,N-diethyl-m-toluamide (DEET), dimethyl phthalate, dibutyl phthalate, 2-ethyl-1,3-hexanediol, and di-n-propyl isocinchomeronate. , p-Dichlorobenzene, Di-n-butyl succinate, Carane-3,4-diol, 1-Methylpropyl 2-(2-hydroxyethyl)-1-piperidinecarboxylate, Isopropyl myristate, Isobornyl thiocyanoacetate, Diphenyl, Diphenylmethane, Dibenzyl, Benzyl phenyl ether, Benzyl phenyl ethyl ether, Benzophenone, Benzyl phenyl ketone, Dibenzyl ketone, Benzalacetophenone, β-Phenylethyl benzoate, γ-Phenylpropyl benzoate, Phenylacetate, Benzyl phenyl acetate, β-phenylethyl phenyl acetate, phenyl cinnamate, benzyl cinnamate, β-phenylethyl cinnamate, β-phenylpropyl cinnamate, cinnamyl cinnamate, diphenyl carbinol, phenylbenzyl carbinol, dibenzyl carbinol, n-amyl benzoate, isoamyl benzoate, hexyl benzoate, heptyl benzoate, octyl benzoate, nonyl benzoate, cis-3-hexenyl benzoate, n-amyl salicylate, iso-amyl salicylate compounds such as ethyl ester, hexyl salicylate, cis-3-hexenyl salicylate, benzyl propionate, benzyl n-butyrate, benzoyl isobutyrate, benzyl n-valerate, benzyl isovalerate, benzyl caproate, benzyl heptanoate, benzyl caprylate, benzyl danylate, eugenol, methyl eugenol, and isoeugenol; terpene compounds such as α,β-phellandrene, α,β-pinene, α,β-terpinol, limonene, citronellal, linalool, citral, and menthol;Examples of such organic compounds include plant extracts such as natural pyrethrins, vetiver oil, patchouli oil, black pepper oil, clove leaf oil, shell ginger oil, and basil oil; isothiocyanate compounds such as methyl isothiocyanate, allyl isothiocyanate, phenyl isothiocyanate, ethyl isothiocyanate, vinyl isothiocyanate, propyl isothiocyanate, and isopropyl isothiocyanate; and aromatic ketone compounds such as acetophenone, propiophenone, and butyrophenone. The other mite control components may be used alone or in combination of two or more.

[0019] As described below, the mite repellent can be used by a method of transpiration, a method of contacting with mites to act, etc. There are active ingredient amounts suitable for various usage methods, but for example, the active ingredients are preferably blended in the mite repellent so as to be 0.001 to 99.99% by mass in total, more preferably 0.01 to 99.9% by mass, and particularly preferably 0.05 to 90% by mass.

[0020] The formulation of the mite repellent of the present invention is not particularly limited, and it may be in the form of a liquid, gel, solid, etc., and any appropriate ingredient may be used accordingly.

[0021] One of the formulations of the mite repellent of the present invention is a liquid formulation. When preparing the liquid formulation, a solvent is used. The solvent is not particularly limited. Although a conventionally known liquid medium can be used, it is preferable to use a liquid medium that is highly safe for the body.

[0022] Examples of the solvent include water such as deionized water and distilled water; hydrocarbon compounds such as hexane, paraffin, and isoparaffin; alkyl alcohols such as methanol, ethanol, 1-propanol, 2-propanol, 1-butanol, 2-butanol, 2-methyl-1-propanol, 2-methyl-2-propanol, pentanol, hexanol, heptanol, octanol, nonanol, and decanol; alkenyl alcohols such as allyl alcohol; aromatic ring-containing alcohols such as benzyl alcohol; phenols such as eugenol; halogenated hydrocarbon compounds such as chloroform; ether compounds such as diethyl ether and diethylene glycol diethyl ether; ketone compounds such as acetone; fatty acid compounds such as acetic acid and oleic acid; ester compounds such as acetate esters, propionate esters, and benzoate esters; glycol compounds such as ethylene glycol and propylene glycol; glycol ether compounds such as 2-phenoxyethanol and 3-methyl-3-methoxybutanol; vegetable oils such as dimethyl sulfoxide, sesame oil, linoleic oil, and salad oil. The solvent may be used alone or in combination of two or more kinds.

[0023] The amount of these solvents used in the repellent is preferably 0.1 to 99.99% by mass, more preferably 1 to 99.9% by mass, and even more preferably 10 to 99.5% by mass, based on the total mass of the repellent.

[0024] When preparing the liquid preparation, a surfactant may be used as necessary. Examples of the surfactant include conventionally known surfactants such as cationic surfactants, anionic surfactants, amphoteric surfactants, and nonionic surfactants. One type of surfactant may be used alone, or two or more types may be used in combination.

[0025] Other formulations of the mite repellent include solid or sheet-like agents obtained by impregnating and supporting the above-mentioned liquid agent on a suitable carrier. The carrier to be supported is not particularly limited, but examples thereof include wood, paper, woven fabric, nonwoven fabric, silica, talc, activated carbon, silica gel, zeolite, cellulose beads, ceramics, and resin pellets such as polypropylene.

[0026] As another formulation, a gelling agent can be mentioned, which is obtained by gelling the above-mentioned liquid agent with a gelling agent. The gelling agent may be any conventionally known agent. For example, carrageenan, gellan gum, agar, gelatin, guar gum, pectin, locust bean gum, xanthan gum, sodium alginate, cellulose derivatives, dibenzylidene-D-sorbitol, hydroxypropylated polysaccharides, inulin stearate, superabsorbent resins such as sodium acrylate, aluminum octylate, etc. The gelling agent may be used alone or in combination of two or more.

[0027] Hereinafter, some examples of the method of using the mite repellent of the present invention will be described, but the method of using the mite repellent of the present invention is not limited to the following descriptions.

[0028] In one example, a method for repelling mites includes releasing a mite repellent into the air. Examples of the method of releasing into the environment include a method of naturally evaporating the active ingredient from the mite repellent of the present invention, such as a liquid agent, a solid agent, or a gel agent, at room temperature, or a method of forced evaporation. Examples of the forced evaporation method include evaporation by heating, evaporation by blowing air, and evaporation by fumigation. In addition, a method of spraying or the like may be used as a method of releasing into the environment.

[0029] Among the methods for forced evaporation, the following method can be mentioned as an example of the evaporation method by heating. A method using a heating and evaporating device, as disclosed in Japanese Utility Model Application Laid-Open Publication No. 2-78077, in which the repellent stored in a liquid bottle is sucked up by a wick and the upper part of the wick is heated by a heater to evaporate the repellent. A method using a heating and evaporating device in which a mat-shaped impregnated body is impregnated with a repellent and the mat is placed on a heater to evaporate the repellent, as disclosed in Japanese Utility Model Laid-Open Publication No. 1-116072.

[0030] Evaporation by blowing air can be carried out, for example, by using a fan-type repellent device as disclosed in JP-A-11-308955, which is equipped with a drug holder and a blower, and releases the repellent from an outlet into the environment by bringing the drug holder into contact with the airflow generated by the blower.

[0031] Transpiration by fumigation can be carried out, for example, by using a fumigation device as disclosed in Japanese Utility Model Laid-Open Publication No. 54-148267, in which a storage chamber is formed in an open-topped container containing an organic foaming agent such as azo compound such as azodicarbonamide, a nitroso compound, or a hydrazide compound, and a repellent, and the bottom of the storage chamber is heated by a heating means to decompose the foaming agent and generate nitrogen gas, carbon dioxide gas, etc., which transpire the repellent.

[0032] Spraying can be carried out by using a sprayer to spray the liquid agent or by using an aerosol using a suitable propellant. When preparing a spray agent, the liquid agent may be combined with a spraying means such as a trigger spray or an atomizer. When preparing an aerosol agent, the liquid agent may be combined with an aerosol carrier such as LPG or isopentane and an aerosol spraying means such as an aerosol can.

[0033] In another example, a method of repelling mites includes contacting the mites with a mite repellent. The mite repellent may be in a liquid state, a solid state, or a gas state, as long as it is in a form that can contact mites. In this case, the repellent can exert a repellent effect by contacting the mites with the installed repellent. For example, it can be directly applied to bedding such as futons, pillows, and blankets, tatami mats, rugs, carpets, sofas, cushions, stuffed toys, clothes, and other places and objects where mites live. In addition, the mite repellent can be sprayed using a sprayer such as a pump spray or an aerosol.

[0034] In another example, a method for repelling dust mites includes applying a dust mite repellent to a textile. By placing and applying the mite repellent in a space such as a storage room, a chest of drawers, a closet, a wardrobe, a clothing case, a clothing storage bag, a futon storage bag, a living room, a bedroom, or the like, or in a space such as an entrance, the active ingredient is released into the above-mentioned environment, or by contacting the mites, the mites can be effectively repelled. The mite repellent of the present invention may also be applied by directly spraying, scattering, coating, etc., to objects including textile products such as tatami mats, rugs, carpets, floors, futons, pillows, sofas, and clothing where mites live.

[0035] (Mechanism of action) The mite repellent of the present invention described above can exert a repellent effect against pests of the order Acari, such as house dust mites such as Dermatophagoides farinae, Dermatophagoides pteronyssinus, and Tyrophagus putrescentiae, as well as mites, ixodid mites, house mites, cheyletid mites, and Cheyletid mites. Among these, the mite repellent of the present invention has a high repellent effect, but a low mite killing effect, and carcasses are unlikely to remain in the application area. Therefore, the mite repellent of the present invention is preferably used against house dust mites such as Dermatophagoides farinae, Dermatophagoides pteronyssinus, and Tyrophagus putrescentiae, which are allergens.

[0036] The mite repellent of the present invention exerts an excellent repellent effect for a long period of time against pests of the Arachnida class, such as house dust mites, Dermatophagoides farinae, and Tyrophagus putrescentiae. In addition, the extract of a plant of the Bignoniaceae family, Catalpa genus, is a natural product, and therefore is extremely safe. Therefore, the mite repellent of the present invention can be easily used in ordinary households, and can effectively prevent and remove damage caused by mites. Furthermore, since mites living indoors, such as Dermatophagoides farinae, can cause allergies even in their carcasses, it is important to have a high repellent effect but not to kill them so that the carcasses do not remain. The mite repellent of the present invention has an excellent repellent effect but a low mite killing effect, and therefore has an excellent allergen removal effect. The mite repellent of the present invention has an excellent repellent effect against pests of the order Acarina and is safe for humans, so that the mite repellent of the present invention can be easily used in ordinary households and is highly useful.

[0037] Although several embodiments have been described above, each embodiment is presented as an example and does not limit the scope of the present invention. Each embodiment described in this specification can be modified in various ways within the scope of the effects of the invention, and can be combined with features described in other embodiments within the scope of feasibility. EXAMPLES

[0038] The present invention will be described in more detail below using examples, but the present invention is not limited to the description of the following examples.

[0039] <Example 1> A non-aqueous solvent extract 1 was obtained from Catalpa flowers as follows. First, 5 g of Catalpa flowers and 50 mL of methanol were placed in a 100 mL eggplant-shaped flask, and then refluxed at 85° C. for 5 hours. Next, the contents of the flask were filtered, and the filtrate was concentrated. This concentration was performed under reduced pressure using an evaporator at room temperature. In this manner, a non-aqueous solvent extract 1 was obtained. Thereafter, the non-aqueous solvent extract 1 was dissolved in dimethyl sulfoxide and filtered, and a dimethyl sulfoxide solution 1 having a concentration of the non-aqueous solvent extract 1 of 4 mass % was obtained as a test sample.

[0040] <Example 2> Non-aqueous solvent extract 2 was obtained from Catalpa twigs as follows. First, 5 g of Catalpa twigs and 50 mL of methanol were placed in a 100 mL eggplant-shaped flask, and then refluxed at 85° C. for 5 hours. Next, the contents of the flask were filtered, and the filtrate was concentrated. This concentration was performed under reduced pressure using an evaporator at room temperature. In this manner, non-aqueous solvent extract 2 was obtained. Thereafter, the non-aqueous solvent extract 2 was dissolved in dimethyl sulfoxide and filtered to obtain a dimethyl sulfoxide solution 2 having a concentration of 4 mass% of the non-aqueous solvent extract 2. The dimethyl sulfoxide solution 2 was used as a test sample.

[0041] <Comparative Example 1> Morimura Shoji Co., Ltd.'s product "Geranium Oil" was prepared as a test sample.

[0042] <Comparative Example 2> The test sample was prepared by steam distillation of essential oil from the leaves of Cymbopogon citrarus (East Indian lemongrass).

[0043] <Repellency test> In accordance with JIS L 1920 "Testing method for anti-mite performance of textile products," mites were raised and their population density was adjusted. Repellency tests were conducted using the test equipment shown in Figures 1 and 2. The test sample of each example was diluted in advance with ethanol to a final concentration of 0.1% by mass. 60 mg of each sample was applied to a cotton cloth having a diameter of 40 mm to obtain a test piece. As shown in Figures 1 and 2, a test specimen 23 was placed in a small glass petri dish 22 with a diameter of 45 mm and a height of 17 mm, and 0.05 g of attractant feed 24 was placed in the center. Then, mite medium 21 containing approximately 10,000 live Dermatophagoides farinae was evenly spread on a large plastic petri dish 20 with a diameter of 90 mm and a height of 14 mm, and the small glass petri dish 22 was placed in the center. The mite medium 21 was a mixture of powdered feed for rearing medium and dry yeast in a mass ratio of 1:1. Thereafter, the large plastic petri dish 20 was placed in a plastic container 25 containing saturated saline solution 26 to adjust humidity. The plastic container 25 was then covered and sealed, and placed in a room at a temperature of 25°C ± 1°C. After being left for 20 hours after placement, the total number of mites on the test piece 23 and on the attractant feed 24 was counted. This test was repeated three times, using cotton cloth that had not been treated with any drug as a blank. The total number of counts from the three tests was calculated, and the repellency rate and mortality rate were calculated using the following formulas. The results are shown in Table 1.

[0044] Repellency rate (%) = {(A1-A2) / A1} x 100 Mortality rate (%)=(A3 / A2)×100 A1: Number of mites on blank cotton cloth and on bait 24 A2: Number of mites on test pieces 23 and on attractant feed 24 after pesticide treatment A3: Number of dead mites on test pieces 23 and on bait for attracting 24 when treated with pesticides

[0045] [Table 1]

[0046] Both Examples 1 and 2 showed a high repellent effect against Dermatophagoides farinae. Moreover, since the mortality rate was low, it was expected that an excellent allergen prevention effect would be exhibited. In Comparative Example 1, a sufficient repellent effect was not obtained. In Comparative Example 2, the repellent effect was high, but the mortality rate was also high, so there was a concern that the corpses that could become allergens would remain in the application area.

[0047] <Gel> An ethanol solution containing 0.1% natural pyrethrin and 1% non-aqueous solvent extract 1 was prepared. 10 g of this ethanol solution was mixed with 85 g of isoparaffin, and 5 g of aluminum octylate was added, heated to 60°C, and stirred. This was filled into a container measuring 35 mm in length, 35 mm in width, and 75 mm in height, and left to stand at room temperature for 3 hours to obtain a gel-like mite repellent.

[0048] <Aerosol agent> An aerosol formulation was prepared by filling a commercially available 200 ml aerosol can with the composition having the formulation shown below. Active ingredient: Natural pyrethrin 0.4ml Active ingredient: Non-aqueous solvent extract 1 1.0ml Solvent: Ethanol 38.6ml Propellant: LPG 30.0ml Propellant: Isopentane 30.0ml

[0049] After spraying an aerosol mite repellent evenly onto the carpet, the carpet remained free of mites for about a month.

[0050] <Spray> The composition having the following composition was placed in a commercially available 150 ml Trig container to prepare a spray. Active ingredient: Natural pyrethrin 0.1g Active ingredient: Non-aqueous solvent extract 2 0.1g Solvent: Ethanol 10g Fragrance 0.05g Surfactant 0.1g Ion exchange water 88.75g

[0051] When this spray was sprayed evenly onto clothing, the clothes remained free of mites for about a week.

[0052] <Fumigants> 10 g of an ethanol solution containing 10% non-aqueous solvent extract 1, 55 g of azodicarbonamide, and 35 g of talc were kneaded together, granulated in a conventional manner, and dried to prepare a fumigant.

[0053] <Heat evaporation agent> A pulp mat measuring 3 cm x 3 cm was impregnated with 100 mg of an ethanol solution containing 10% of the non-aqueous solvent extract 2 to obtain a heat-transmitting agent. This heat-transmitting agent evaporates the active ingredients using a heater.

[0054] <Granular formulation> 50 g of pulp granular impregnated material (average particle size 5 mm) was impregnated with 50 mL of an ethanol solution containing 10% non-aqueous solvent extract 1, air-dried, and then placed in a breathable nonwoven bag to obtain a granular repellent.

[0055] From the above results, it was confirmed that a mite repellent that has a high mite repellent effect and does not produce many dead mites was provided. Because Catalpa is a natural ingredient, it is expected to be highly safe. [Industrial Applicability]

[0056] The mite repellent of the present invention has a high mite repellent effect, is highly safe, and is less likely to produce dead mites. According to the method for repelling mites of the present invention, the repelling effect against mites is high, the safety is high, and moreover, the generation of dead mites is reduced. [Explanation of symbols]

[0057] 20 Large Petri Dish 21 Mite medium 22 Small Petri Dish 23 Specimen 24 Attraction feed 25 Plastic containers 26 Saturated Salt Water

Claims

1. A mite repellent containing an extract of a plant of the genus Catalpa in the family Bignoniaceae as an active ingredient.

2. 2. The mite repellent according to claim 1, wherein the plant of the genus Catalpa in the family Bignoniaceae is Catalpa.

3. 2. The mite repellent according to claim 1, wherein the extract of a plant of the genus Catalpa in the family Bignoniaceae is at least one extract selected from the group consisting of flowers, branches, fruits, seeds, leaves, stems, roots and bark.

4. 2. The mite repellent according to claim 1, wherein the extract of a plant of the genus Catalpa in the family Bignoniaceae is a methanol extract.

5. A method for repelling mites, comprising releasing the mite repellent according to any one of claims 1 to 4 into the air.

6. A method for repelling mites, comprising applying the mite repellent according to any one of claims 1 to 4 to a textile product.

7. A method for repelling mites, comprising contacting the mite repellent according to any one of claims 1 to 4 with mites.

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