Human repellent

Abstract

The present invention provides a human repellent that maintains the water resistance of the formed film sprayed or applied to the skin surface even when sweating due to water work, water play, or outdoor exercise, and that allows the active ingredient to remain in the formed film while ensuring the evaporation of the active ingredient from the formed film for a long period of time. [Means for solving the problem] A human insect repellent that repels pests, comprising at least one active ingredient selected from N,N-diethyl-m-toluamide, picaridin, 3-[N-acetyl-N-butyl]-aminopropionate ethyl ester, and p-menthanediol compounds, along with a film-forming agent and an emulsifier.

Description

[Technical Field]

[0001] The present invention relates to a human repellent that, when applied directly to the skin of the human body, repels pests from approaching the human body. [Background technology]

[0002] Traditionally, there are known human repellents that are applied to the skin to prevent pests such as mosquitoes, gnats, horseflies, and ticks, especially mosquitoes, from approaching.

[0003] These human-use repellents contain active ingredients such as N,N-diethyl-m-toluamide (DEET), picaridin, and p-menthanediol compounds. Because they can easily repel insects by being sprayed or applied to the surface of the skin, they have become widely used.

[0004] However, conventional human repellents have the problem that the active ingredients applied to the skin surface are washed away by water-related activities such as washing dishes, playing in water, or sweating, resulting in poor persistence of the repellent effect and low residual effect.

[0005] In response to this problem, Patent Document 1 describes a water-resistant repellent containing active ingredients such as DEET and picaridin, a cellulose derivative, silicone oil, and alcohol. This conventional water-resistant repellent is said to be able to effectively repel pests regardless of water-related work, water play, or sweating. [Prior art documents] [Patent Documents]

[0006] [Patent Document 1] Japanese Patent Publication No. 2019-94319 [Overview of the project] [Problems that the invention aims to solve]

[0007] However, even with these conventional water-resistant repellents, sufficient water resistance was not always achieved, and further improvements were needed.

[0008] Incidentally, in order to further impart water resistance to human repellents, it is conceivable to further incorporate a water-resistant film-forming agent in addition to the active ingredients, apply this to the skin surface, and form a film layer on the skin surface. This allows the active ingredients to remain inside the film layer formed on the skin surface, thereby imparting water resistance to the active ingredients.

[0009] However, as will be discussed later, in order for the active ingredient to neutralize the sensory perception of pests, it is necessary for the active ingredient to evaporate sufficiently from the inside to the outside of the film layer, that is, to ensure evaporative efficiency so that the active ingredient can reach the pests. In particular, when sweating occurs due to outdoor exercise, sweat in the human body is produced from inside the skin, not from the outside, and it is preferable to evaporate this moisture from sweating as quickly as possible, as it may damage the formed film layer.

[0010] Thus, when forming a film layer on the skin surface, a new problem arises: the film layer must maintain its water resistance, retain the active ingredients within it, and ensure sufficient evaporation for the remaining active ingredients to evaporate to the outside of the film layer over a long period of time.

[0011] The object of the present invention is to provide a human repellent that, when applied to the surface of human skin, maintains its water resistance and allows the active ingredient to remain inside the film layer formed on the skin surface, while also ensuring long-term evaporation of the remaining active ingredient to the outside of the film layer. [Means for solving the problem]

[0012] The present invention, for achieving the above objective, is a human repellent that, when applied directly to the skin of a person, repels pests from approaching the person, and is characterized in that it contains at least an active ingredient, a film-forming agent, and a volatile solvent, wherein the active ingredient is at least one or more selected from N,N-diethyl-m-toluamide, picaridin, 3-[N-acetyl-N-butyl]-aminopropionate ethyl ester, and p-mentanediol compounds.

[0013] The human repellent according to the present invention, which achieves the above objective, is characterized in that the film-forming agent is a combination of two or more silicones having different chemical structures.

[0014] To achieve the above objective, the present invention provides a human repellent that further contains an emulsifier, characterized in that the emulsifier is a silicone-based emulsifier.

[0015] The human repellent according to the present invention, which achieves the above objective, is characterized in that the film-forming agent is a combination of an acrylic polymer having a silicone structure and a silicone network resin.

[0016] The human repellent according to the present invention for achieving the above objective is characterized in that the film-forming agent is a combination of alkyl acrylate copolymer methylpolysiloxane ester and trimethylsiloxysilicate.

[0017] To achieve the above objective, the present invention provides a human body repellent in which the film-forming agent comprises a polymer having a main chain having acrylic acid [-CH2CH(R)COO-] or methacrylic acid [-CH2C(CH3)(COOH)-] as repeating units and side chains having dimethylsiloxane [-(CH3)2Si-O-] as repeating units, and [(CH3)3SiO 0.5 It is characterized by a combination of a silicone mesh resin having repeating units of [SiO2] and [[SiO2]] units.

[0018] The repellent for human use according to the present invention for achieving the above object is characterized in that the volatile solvent contains a combination of linear silicone oil and cyclic silicone oil.

[0019] The repellent for human use according to the present invention for achieving the above object is characterized in that the repellent for human use is an emulsion product enclosed in a container.

[0020] The repellent for human use according to the present invention for achieving the above object is characterized in that the repellent for human use is a spray product enclosed in a container equipped with a sprayer. Effects of the Invention

[0021] According to the present invention, when applied to the skin surface of the human body, it is possible to provide a repellent for human use that can maintain the water resistance of the coating layer formed on the skin surface, allow the active ingredient to remain inside the coating, and at the same time ensure the transpiration property that allows the residual active ingredient to transpire out of the coating layer for a long time.

[0022] Further, according to the present invention, water resistance can be maintained and transpiration property can also be ensured regardless of perspiration caused by, for example, washing work, playing in water, and particularly long-time exercise outdoors. Mode for Carrying Out the Invention

[0023] Hereinafter, the repellent for human use according to the present invention will be described in detail.

[0024] The repellent for human use according to the present invention, when applied directly to the skin of the human body, is for repelling pests from approaching the human body. The means for applying the repellent for human use is not particularly limited, and for example, a method of spraying in the form of a mist is preferable.

[0025] The human body repellent according to the present invention is obtained by mixing an active ingredient, a film-forming agent, a volatile solvent, an emulsifier, and other components, dissolving or dispersing them in a volatile solvent to form a liquid or emulsion, and applying this to the surface of the human body by means of spraying or other means to form a film layer on the skin surface. (Applicable pests) Pests to which the repellent effect of the human repellent according to the present invention can be applied include insects that physically or mentally harm humans, such as mosquitoes, black flies, horseflies, ticks, house dust mites, bed bugs, fleas, midges, and leeches. (Active ingredients in human repellents) The active ingredient of the present invention is an effective ingredient for repelling pests from approaching the human body, and preferably at least one or more selected from, for example, N,N-diethyl-m-toluamide, picaridin, 3-[N-acetyl-N-butyl]-aminopropionate ethyl ester, and p-menthanediol compounds, of which picaridin is particularly preferred.

[0026] The N,N-diethyl-m-toluamide of this invention is an organic compound also known as DEET. It has been used in Japan for over 50 years and is the most widely used insect repellent ingredient worldwide because it maintains its repellent effect with just one application. It has repellent effects against major pests such as mosquitoes and ticks, as well as many other pests such as leeches, bed bugs, horseflies, and gnats, making it usable as an insect repellent in a variety of situations.

[0027] The Icaridin of this invention is an organic compound that is either 1-(1-methylpropoxycarbonyl)-2-2-hydroxyethyl)piperidine or 1-methylpropyl ester of 2-(2-hydroxyethyl)-1-piperidinecarboxylic acid. Since each of these organic compounds has two chiral carbon atoms in its structure, there are a total of four optical isomers. In other words, "Icaridin" is a general term that encompasses each of these isomers or one or more combinations selected from them. Icaridin is an insect repellent ingredient approved in Japan in 2015, and has the advantage of being reapplied as many times as needed whenever pests are a concern, as there are no age restrictions or restrictions on the number of applications.

[0028] The ethyl 3-[N-acetyl-N-butyl]-aminopropionate of the present invention can repel harmful insects such as mosquitoes and horseflies from the skin of the body.

[0029] Examples of p-menthanediol compounds used in the present invention include α-pinene, geraniol, citronellal, linalool, spearmint (containing components: limonene, carvone, etc.), nutmeg (containing components: geraniol, linalool, eugenol, safrole, pinene, etc.), peppermint (containing components: menthol, jasmone, carvacrol, limonene, etc.), cinnamon (containing components: cinnamic aldehyde, eugenol, safrole, cymene, dipentene, phellandrene, pinene, etc.), clove (containing components: furflor, eugenol, caryophyllene, pinene, etc.), eucalyptus (containing components: caffeine, fenkene, phellandrene, pinene, citronellal, cineole, etc.), garlic (containing components: diallyl disulfide, etc.), and p-menthane-3,8-diol.

[0030] The active ingredient contained in the human repellent of the present invention, for example, picaridin, acts on receptors present on the sensory receptors of insect antennae, promoting the production of secondary neurotransmitters and transmitting a certain response to the brain. As a result, in insects that receive picaridin, the original response generated by attractants from blood-feeding sources such as humans is overwhelmed by the response generated by picaridin, and the recognition of the blood-feeding source is inhibited. It is believed that picaridin exerts its repellent effect through this mechanism.

[0031] The proportion of the active ingredients in the present invention depends on the type of active ingredient, but when the total amount of the human repellent is considered to be 100% by mass, it is, for example, 2.5 to 40.0% by mass, preferably 3.0 to 30.0% by mass, and more preferably 5.0 to 20.0% by mass. (Film-forming agent) The film-forming agent of the present invention is mixed with an active ingredient, a volatile solvent, an emulsifier, and other components, dissolved or dispersed in the volatile solvent to form a liquid or emulsion, and after being applied to the surface of human skin by means of spraying or other means, a film layer is formed on the skin surface as the volatile solvent evaporates. The film layer formed on the skin surface must have both water resistance to keep the active ingredient inside the film layer regardless of contact with moisture, and evaporability to allow the active ingredient to exert a repellent effect, that is, the property of being able to evaporate the active ingredient to the outside of the skin layer by utilizing the gas permeability of the film layer.

[0032] Since the film-forming agent of the present invention is applied directly to the skin surface, it is preferable that it not only be highly safe but also highly water-resistant and evaporative. Among materials with such properties, silicone is highly safe, highly water-resistant during film formation, and also highly evaporative due to its high gas permeability. The reason why silicone has excellent gas permeability lies in its molecular structure, which is derived from the molecular structure of silicone in which an oxygen atom and a methyl group are bonded to a silicon atom. In silicone, silicon and oxygen are bonded in a bent manner, so the methyl groups of the side chains can easily rotate freely around this bent silicon-oxygen bond as an axis, and these methyl groups of the side chains suppress the interaction between molecular chains, so it can be said that it is a polymer with many gaps at the micro level. Therefore, it is a material with high gas permeability and, consequently, excellent evaporative properties.

[0033] Examples of such silicones include silicone-modified polynorvonene, silicone-modified pullulan, silicone network resins, fluorine-modified alkylsiloxysilicate, phenyl-modified alkylsiloxysilicate, and acrylic polymers containing a silicone structure (hereinafter sometimes referred to as "(Acrelites / Dimethicone) copolymer"). (Acrylic polymer containing film-forming agent / silicone structure) The acrylic polymer containing a silicone structure in this invention forms a film upon evaporation of the solvent in which it is dissolved or dispersed, and is a component that imparts water resistance, sebum resistance, and water repellency to the active ingredient.

[0034] Acrylic polymers containing a silicone structure are preferably polymers having a main chain having acrylic acid [-CH2CH(R)COO-] or methacrylic acid [-CH2C(CH3)(COOH)-] as repeating units, and side chains having siloxane [-R2Si-O-] (wherein R represents the same or different monovalent organic group) as repeating units.

[0035] The main chain having acrylic acid or methacrylic acid as repeating units is preferably a main chain having one or both of acrylic acid or methacrylic acid and one or both of alkyl acrylate [-CH2CH(R)COO-] or alkyl methacrylate [-CH2C(CH3)RCOO-] as repeating units. For example, a main chain having methacrylic acid, 2-ethylhexyl acrylate, methyl methacrylate, and butyl methacrylate as repeating units is an example.

[0036] Side chains having siloxane as a repeating unit are preferably those in which all R groups are alkyl groups, i.e., side chains having dialkylsiloxane as a repeating unit, and more preferably those in which all R groups are methyl groups, i.e., side chains having dimethylsiloxane [-(CH3)2Si-O-] as a repeating unit.

[0037] Hereinafter, a polymer having a main chain with acrylic acid or methacrylic acid as repeating units and side chains with dimethylsiloxane as repeating units may be referred to as "(Acrylates / Dimethicone) Copolymer" (also called "Alkyl Acrylate Copolymer Methyl Polysiloxane Ester" according to the notation in the Quasi-Drug Raw Material Standards).

[0038] Among the (Acreitz / Dimethicone) copolymers, particularly preferred ones include, for example, Shin-Etsu Chemical Co., Ltd.'s "KP-543" ((Acreitz / Dimethicone) copolymer butyl acetate solution), "KP-545" ((Acreitz / Dimethicone) copolymer cyclopentasiloxane (also called "decamethylcyclopentasiloxane" according to the notation in the Quasi-Drug Raw Material Standards; the same applies hereinafter) solution), and "KP-549" These include "(Acre-Lite / Dimethicone) Copolymer Methyl Trimethicone Solution", "KP-550" ((Acre-Lite / Dimethicone) Copolymer Isododecane Solution), and "KP-545L" ((Acre-Lite / Dimethicone) Copolymer Dimethicone Solution (also called "Dimethylpolysiloxane," and according to the notation in the Quasi-Drug Raw Material Standards, also called "Methylpolysiloxane"; the same applies hereinafter)).

[0039] Acrylic polymers containing a silicone structure can be produced, for example, by graft polymerization, in which an acrylic polymer is used as the main chain and a dialkylpolysiloxane, preferably dimethylpolysiloxane, is introduced as a side chain to this main chain. Graft polymerization can be carried out by substituting a portion of the carboxyl group (-COOH) of the acrylic acid or methacrylic acid in the repeating units constituting the main chain with a hydroxyl group or a hydroxyalkyl group of the dialkylpolysiloxane, preferably dimethylpolysiloxane, and then ester bonding. In other words, a graft polymer consisting of an acrylic polymer and dimethylpolysiloxane can be obtained. (Film-forming agent / Silicone mesh resin) The silicone mesh resin in this invention forms a film upon evaporation of the solvent in which it was dissolved, and is a component that imparts water resistance, sebum resistance, and water repellency to the active ingredients.

[0040] Silicone mesh resins include, for example, [R3SiO 0.5 A resin having repeating units of [M] units (M units; R in the formula represents the same or different monovalent organic groups) and [SiO2] units (Q units) (hereinafter sometimes referred to as "MQ resin") is preferred.

[0041] The MQ resin is preferably one in which all R groups in the formula constituting the M unit are alkyl groups, i.e., trialkylsiloxysilicate, and preferably one in which all R groups in the formula constituting the M unit are methyl groups [CH3], i.e., trimethylsiloxysilicate.

[0042] Among trimethylsiloxysilicates, particularly preferred ones include, for example, Shin-Etsu Chemical Co., Ltd.'s "KF-7312J" (cyclopentasiloxane solution of trimethylsiloxysilicate), "KF-7312K" (dimethicone (non-volatile) solution of trimethylsiloxysilicate), "KF-7312L" (dimethicone solution of trimethylsiloxysilicate), "KF-7312T" (methyltrimethicone solution of trimethylsiloxysilicate), and "X-21-5595" (trimethylsiloxy These can be obtained from the following products: isododecane solution of silicic acid, X-21-5249 (cyclopentasiloxane solution of trimethylsiloxysilicate), X-21-5250 (cyclopentasiloxane solution of trimethylsiloxysilicate), X-21-5616 (isododecane solution of trimethylsiloxysilicate), KF-9021 (cyclopentasiloxane solution of trimethylsiloxysilicate), and KF-9021-1D (isododecane solution of trimethylsiloxysilicate).

[0043] The process by which the human repellent of the present invention forms a film is as follows: The active ingredient, film-forming agent, emulsifier, volatile solvent, and other components are blended and mixed to form a liquid or emulsion, which is then directly applied to the surface of the human body, such as by spraying. When the volatile solvent evaporates and dries in the human repellent applied to the skin surface, the active ingredient is retained on the skin. This can be inferred in more detail as follows.

[0044] First, immediately after applying a human repellent to the surface of human skin, the active ingredient and film-forming agent dissolve or disperse in the volatile solvent, remaining in a liquid or emulsion state on the skin surface.

[0045] Next, as the volatile solvent evaporates and drying progresses, the film-forming agent and other non-volatile solvent components remain on the skin surface, forming a film layer. In this film layer, the portion derived from the film-forming agent constitutes the outer layer, while the portion derived from the active ingredient constitutes the inner layer between the outer layer and the skin surface. In other words, the inner layer containing the active ingredient exists between the outer layer, which consists of the film-forming agent, and the skin surface.

[0046] In this manner, the active ingredients are retained within the coating layer.

[0047] As mentioned above, in the human repellent of the present invention, the film layer formed on the skin surface must have water resistance in order to retain the active ingredient inside the film layer, and also have evaporative properties, that is, the property that allows the active ingredient to evaporate from the inside to the outside of the film layer in order to exert a repellent effect on the active ingredient.

[0048] Furthermore, for a coating layer to be evaporative, it must also be gas-permeable. However, when considering the water resistance and gas permeability of the silicones that make up the coating agent, each type has its advantages and disadvantages, and using only one type of silicone does not necessarily fully satisfy both water resistance and gas permeability. This is because, as will be explained later, water resistance and gas permeability are sometimes conflicting requirements.

[0049] Therefore, in order to further achieve both water resistance and evaporative properties, the present invention may use a combination of two or more silicones with different chemical structures to achieve both water resistance and evaporative properties.

[0050] In particular, when considering sweating caused by outdoor exercise, this sweat is expelled from within the body, and it is desirable to evaporate not only the active ingredients but also the water produced by this sweat as quickly as possible, as this can damage the formed film layer.

[0051] On the other hand, prioritizing only evaporative properties leads to a decrease in film strength and thus reduced water resistance, while prioritizing only water resistance leads to a decrease in gas permeability and thus reduced evaporative properties.

[0052] Therefore, as described above, the present invention may use a combination of two or more silicones with different chemical structures to further achieve both water resistance and evaporative properties, and may be able to maintain its repellent effect for a long period of time, even when sweating occurs due to outdoor exercise, etc.

[0053] The blending ratio of the film-forming agent of the present invention is, for example, 0.1 to 15.0% by mass, preferably 0.2 to 10.0% by mass, and more preferably 0.3 to 0.5% by mass, when the total amount of the human body repellent is considered to be 100% by mass. When two types of silicone are used, the blending ratio is preferably 1 to 4 to 4 to 1. When three or more types of silicone are used, the blending ratio can be evenly divided by the number of silicones, and the upper and lower limits can be adjusted based on that blending ratio. (Film-forming agent / combination) When using two types of silicone as film-forming agents in the present invention, a combination of, for example, an acrylic polymer containing a silicone structure (hereinafter referred to as "component A") and trialkylsiloxysilicate (hereinafter referred to as "component B") is preferred. More preferably, a combination of an acrylic polymer containing a silicone structure having a main chain made of a copolymer obtained by copolymerizing one or both of acrylic acid or methacrylic acid with one or both of alkyl acrylate or alkyl methacrylate and a side chain made of dimethylpolysiloxane, and trimethylsiloxysilicate as component B is preferred. A combination of the above-mentioned "KP-543", "KP-545", "KP-549", "KP-550", and "KP-545L" as component A and the above-mentioned "KF-7312J", "KF-7312K", "KF-7312L", "KF-7312T", "X-21-5595", "X-21-5249", "X-21-5250", "X-21-5616", "KF-9021", and "KF-9021-1D" as component B is particularly preferred.

[0054] When the sum of the masses of component A and component B is taken as 100, the proportion of component B's mass to the sum is preferably 30% to 95%, more preferably 50% to 90%, and particularly preferably 70% to 85%. If the above proportion is less than 30% or greater than 95%, sufficient water resistance can be obtained, but sufficient transpiration may not be obtained. On the other hand, if the above proportion is between 30% and 95%, sufficient water resistance and sufficient transpiration can be obtained.

[0055] The film layer formed by the film-forming agent described above, being made of silicone, exhibits the following effects.

[0056] In other words, the active ingredient, such as picaridin, gradually volatilizes as a gas and reaches the pests, thereby exerting its repellent effect. Even when retained inside the coating layer, as described above, it passes through the microscopic gaps present in the coating layer, evaporates to the outside of the coating layer, reaches the pests, and exerts its repellent effect. Thus, the coating layer of the present invention does not inhibit the evaporation of the active ingredient. (Volatile solvent) In this invention, the volatile solvent is a component that dissolves or disperses the active ingredient, film-forming agent, etc., to facilitate direct application by means of spraying or other methods. The volatile solvent evaporates after application, and as a result, the film-forming agent forms a film layer.

[0057] The blending ratio of the volatile solvent of the present invention is preferably 70 to 90% by mass in total, and more preferably 80 to 85%.

[0058] As volatile solvents, for example, alcohol, water, silicone oil, as well as isododecane and butyl acetate can be used.

[0059] As for the alcohol, methanol, ethanol, and isopropyl alcohol are preferred, with ethanol being more preferred. As for the water, purified water is preferred. (Volatile solvents / Volatile silicone oils) The human repellent in the present invention preferably contains volatile silicone oil. The reason for this is as follows: When not in use, it dissolves the film-forming agent, allowing the human repellent to be stored stably for a long period of time in a usable state, and when in use, it volatilizes to ensure that the dissolved film-forming agent reliably forms a film layer.

[0060] Furthermore, volatile solvents only need to be substantially volatile; it is not necessarily required that all of them volatilize. In other words, even if some of the components constituting the volatile solvent do not volatilize, for example, due to their large molecular weight, those components may help, rather than hinder, the formation of the coating layer as part of the coating layer.

[0061] The volatile silicone oil is preferably composed of trisiloxane, dimethylpolysiloxane (also called "dimethicone," and also "methylpolysiloxane" according to the notation in the Quasi-Drug Raw Material Standards; the same applies hereinafter), ethylmethicone (in which one of the two methyl groups in the repeating unit portion of dimethylpolysiloxane is substituted with an ethyl group), or methyltrimethicone, and more preferably composed of dimethylpolysiloxane.

[0062] The blending ratio of the volatile silicone in the present invention is preferably 0.5 to 6.0% by mass, and more preferably 1.0 to 3.0% by mass, when the total amount of the human body repellent is considered to be 100% by mass.

[0063] In order to ensure that the volatile silicone oil has a volatility that does not hinder the formation of the film layer by the film-forming agent, it is preferable that its kinematic viscosity is low. Here, in the case of a linear volatile silicone oil, the kinematic viscosity at 25°C is, for example, 0.5 to 4.5 mm. 2 Preferably, it is 1.0 to 3.5 mm in length / s. 2 A value of / s is more preferable, and 1.5 to 2.5 mm 2 In particular, those with a viscosity of / s are preferred. Furthermore, in the case of cyclic volatile silicone oils, the kinematic viscosity at 25°C is, for example, 3.5 to 4.5 mm. 2 A value of / s is preferred. There is a certain correlation between kinematic viscosity and molecular weight; if the kinematic viscosity is high, the molecular weight is also high, and if the kinematic viscosity is low, the molecular weight is also low. Furthermore, if the molecular weight is low, it is volatile, and if the molecular weight is high, it is not volatile.

[0064] Among dimethylpolysiloxanes, linear examples include "KF-96L-1.5cs" manufactured by Shin-Etsu Chemical Co., Ltd. (viscosity of 1.5 mm at 25°C 2 / s), and "KF-96L-2cs" manufactured by the same company (kinematic viscosity of 2.0 mm at 25°C 2 / s) are preferable, and those obtained from the above-mentioned "KF-96L-2cs" are more preferable.

[0065] In addition to these, dimethylpolysiloxane, which is a volatile silicone oil, may be derived from the solvent that dissolves the film-forming agent. For example, it may be derived from the above-mentioned "KF-96L-2cs" contained as a solvent in each of the above-mentioned "KP-545L" and the above-mentioned "KF-7312L".

[0066] Among dimethylpolysiloxanes, as cyclic ones, for example, cyclopentasiloxane is preferable, decamethylcyclopentasiloxane is more preferable, and "KF-995" manufactured by Shin-Etsu Chemical Co., Ltd. (viscosity of 4.0 mm at 25°C 2 / s) is particularly preferable.

[0067] In addition to these, decamethylcyclopentasiloxane, which is a volatile silicone oil, may be derived from the solvent that dissolves the film-forming agent. For example, it may be derived from the above-mentioned "KF-995" contained as a solvent in each of the above-mentioned "KP-545", the above-mentioned "KF-7312J", the above-mentioned "X-21-5249", the above-mentioned "X-21-5250" and the above-mentioned "KF-9021". (Volatile solvent / Combination) As the volatile solvent in the present invention, one type or a combination of two or more selected from alcohols, water, and silicone oils is preferable, and a combination of all three types is more preferable.

[0068] When using two types of silicone oil as the volatile solvent of the present invention, a combination of a linear component (hereinafter referred to as "component C") and a cyclic component (hereinafter referred to as "component D") is preferred, and a combination of dimethylpolysiloxane as component C and cyclopentanesiloxane as component D is preferred.

[0069] When the sum of the mass of component C and the mass of component D is taken as 100, the proportion of the mass of component C to this sum is preferably 40% to 90%, more preferably 40% to 80%, and particularly preferably 60% to 70%. (emulsifier) The human repellent of the present invention preferably further contains an emulsifier, in order to ensure excellent applicability to the skin by good dispersion or dissolution of each component, and to ensure long-term storage stability of the repellent components.

[0070] Suitable emulsifiers include, for example, silicone-based emulsifiers, polyether-modified silicones, and polyglycerin-modified silicones, with polyether-modified silicones being more preferred.

[0071] Such polyether-modified silicones may have either linear or branched silicone chains. Examples include linear polyoxyethylene-methylpolysiloxane copolymers, linear poly(oxyethylene-oxypropylene)methylpolysiloxane copolymers, branched silicone chain polyoxyethylene-methylpolysiloxane copolymers, and alkyl-silicone-chain branched polyoxyethylene-methylpolysiloxane copolymers.

[0072] Among these, one or more selected from the group consisting of linear polyoxyethylene-methylpolysiloxane copolymers, linear poly(oxyethylene-oxypropylene)methylpolysiloxane copolymers, and modified versions thereof are preferred in terms of improving emulsification stability.

[0073] Linear poly(oxyethylene-oxypropylene)methylpolysiloxane copolymers are particularly preferred if they are obtained from, for example, Shin-Etsu Chemical Co., Ltd.'s "KF-6012".

[0074] The blending ratio of the emulsifier of the present invention is preferably, for example, 0.1 to 0.5% by mass, and more preferably 0.2 to 0.4% by mass. (Other ingredients) The human repellent of the present invention may optionally contain wetting agents, UV blocking agents, thickeners, preservatives, colorants, moisturizers, fragrances, pH adjusters, etc. However, the human repellent of the present invention does not need to contain other components. (Human repellent in a spray bottle) The human repellent of the present invention may be sealed in a container with a spray nozzle, for example, and used by spraying it from the nozzle and applying it directly to the skin of the human body. By using it in this embodiment, a repellent effect can be easily obtained. [Examples]

[0075] The present invention will be specifically described below with reference to examples, but the present invention is not limited to the following description. (Water resistance test evaluation) As test examples of the human repellent of the present invention, each component was prepared according to the respective mixing ratios shown in [Table 1] below, yielding Examples 1 to 3 and Comparative Examples 1 to 3. Here, the mixing ratio of each component is expressed in mass%, and the total of all components is considered to be 100% by mass. The same applies to [Table 2] below.

[0076] For each test example, we tested and evaluated its water resistance, that is, whether the mosquito repellent effect remained even after immersion in water. The test results and their evaluations are shown in [Table 1] below.

[0077] [Table 1]

[0078] The manufacturers, product names, and product numbers for the components listed in [Table 1] are listed below. • Active ingredient: Icaridin: Made by Saltigo • Solvent: Methylpolysiloxane: "KF-96L-2cs" manufactured by Shin-Etsu Chemical Co., Ltd. • Solvent: Decamethylcyclopentasiloxane: "KF-995" manufactured by Shin-Etsu Chemical Co., Ltd. • Emulsifier: Poly(oxyethylene-oxypropylene)methylpolysiloxane copolymer: "KF-6012" manufactured by Shin-Etsu Chemical Co., Ltd. • Film-forming agent 1: Mixture of alkyl acrylate copolymer methylpolysiloxane ester and decamethylcyclopentanesiloxane: "KP-545" manufactured by Shin-Etsu Chemical Co., Ltd. • Film-forming agent 2: Mixture of trimethylsiloxysilicate and methylpolysiloxane: "KF-7312L" manufactured by Shin-Etsu Chemical Co., Ltd. Note that while film-forming agents 1 and 2 are commercially available mixed and dissolved in a solvent, we used a commercially available product consisting only of a solvent without solute to adjust the composition to the components shown in [Table 1]. The same applies to [Table 2] described below. (Water resistance evaluation test / test method) 1 mL / 600 cm² of Example 1 was applied to one forearm of the subject. 2 The sample was applied in this manner, and after the solvent evaporated, one forearm coated with Example 1 was immersed in water for 4 minutes, then the immersion was removed and it was allowed to stand. After confirming that the moisture had naturally dried, this was designated as the "chemical treatment area".

[0079] The other forearm of each subject was immersed in water for 4 minutes without applying any repellent, and then the immersion was removed and the area was left to stand. After confirming that the water had naturally dried, this area was designated as the "untreated group."

[0080] A container was placed containing 50 or more female Aedes albopictus mosquitoes. One forearm coated with Example 1 was placed inside the container, and the number of Aedes albopictus mosquitoes that tethered to this forearm was measured. This was defined as the "number of tethered mosquitoes in the pesticide-treated area."

[0081] Similarly, the other forearm, which had not been treated with any repellent, was placed in a container containing more than 50 female Aedes albopictus mosquitoes. The number of Aedes albopictus mosquitoes that were attached to this forearm was counted and defined as the "number of mosquitoes attached to the untreated area."

[0082] The repellency rate in Example 1 was calculated based on the number of tethered fish in the chemical-treated area and the number of tethered fish in the untreated area, according to the following formula (Equation 1).

[0083] (Formula 1) Repellency rate (%) = (1 - number of tethered fish in the chemically treated area ÷ number of tethered fish in the untreated area) × 100 Furthermore, similar to Example 1, the repellency rates were also determined for Examples 2 and 3, and Comparative Examples 1 to 3.

[0084] Based on this, the repellency rate of each test example was used as an indicator of the water resistance it possessed. (Water resistance evaluation test / evaluation method) Based on the above test results, regarding water resistance, i.e., the repellency rate after immersion in water, test cases with a water resistance of 90% or more and 100% or less were evaluated as "good" (hereinafter referred to as "○"), test cases with a water resistance of 50% or more and less than 90% were evaluated as "neither good nor bad" (hereinafter referred to as "△"), and test cases with a water resistance of less than 50% were evaluated as "bad" (hereinafter referred to as "×"). (Water resistance evaluation test / summary) First, we will compare Comparative Example 1 with Examples 1-3 and Comparative Examples 2 and 3.

[0085] Comparative Example 1 received a failing grade, indicating that it did not exhibit water resistance. This was because immersion in water washed away the active ingredient from the skin surface, resulting in the complete loss of its repellent effect.

[0086] In contrast, Examples 1-3 received a "○" rating, demonstrating a high degree of water resistance. Comparative Examples 2 and 3 also received a "△" rating, indicating inferiority compared to Examples 1-3, but still demonstrating a considerable degree of water resistance.

[0087] The reason for this is that, despite immersion in water, the active ingredients remained on the skin surface, resulting in the entire repellent effect persisting in Examples 1-3, while only a portion of the repellent effect persisted in Comparative Examples 2 and 3.

[0088] Next, comparing Examples 1-3 with Comparative Examples 2 and 3, Examples 1-3 received a "○" rating, while Comparative Examples 2 and 3 received a "△" rating. This indicates that using a combination of two film-forming agents resulted in superior water resistance compared to using only one film-forming agent.

[0089] Furthermore, Examples 1 to 3 will be examined in detail. Example 1 had 100% water resistance, Example 2 had 95% water resistance, and Example 3 had 93% water resistance. In all cases, a combination of an acrylic polymer containing a silicone structure (alkyl acrylate copolymer methylpolysiloxane ester) (component A) and a silicone network resin (trimethylsiloxysilicate) (component B) was used as a film-forming agent.

[0090] Here, assuming that the sum of the masses of component A and component B is 100, the proportion of the mass of component B relative to this sum was 83% for Example 1, 63% for Example 2, and 36% for Example 3.

[0091] From the above, it can be seen that the greater the proportion of component B relative to the proportion of component A, the better the water resistance. However, in comparison with Comparative Example 2, it can be reasonably inferred that there is an upper limit to the numerical range with critical significance when the proportion of component B is 83% or close to it, as this does not necessarily mean that the water resistance is excellent, and in fact the water resistance decreases. (Sweat resistance evaluation test) As further test examples of the human repellent of the present invention, each component was prepared in the respective proportions shown in [Table 2] below to obtain Comparative Example 1 and Example 4. Comparative Example 1 is the same as "Comparative Example 1" in the water resistance evaluation test. (Sweat resistance evaluation test / test method) For each test example, sweat resistance, i.e., whether or not the active ingredient remains after sweating, was tested and evaluated. The test results and their evaluations are shown in [Table 2] below.

[0092] [Table 2]

[0093] 1 mL / 600 cm² of Example 4 was applied to the forearms and feet of the subjects. 2 The substance was applied to the subject's forehead, and after the solvent evaporated, the subject was made to exercise until sweat was dripping from their forehead. After the subject had sweated, the treated area was wiped with cotton wool, and the amount of the active ingredient (icaridin) adhering to the cotton wool was quantified to determine the remaining amount, which was defined as the "amount remaining after sweating."

[0094] Similarly, 1 mL / 600 cm² of Example 4 was applied to the forearms and feet of the subjects. 2 The drug was applied to the area, and after the solvent evaporated, the treated area was wiped with cotton wool without the subject moving. The amount of active ingredient (icaridin) adhering to the cotton wool was quantified, and the remaining amount was determined, which was defined as the "amount remaining before sweating."

[0095] The ratio of the amount remaining after sweating to the amount remaining before sweating, that is, the remaining rate of the active ingredient (icaridin) after sweating, was calculated based on the following (Equation 2).

[0096] (Formula 2) Remaining rate (%) = Amount remaining after sweating ÷ Amount remaining before sweating × 100 Furthermore, similar to Example 4, the survival rate was also determined for Comparative Example 1.

[0097] Based on this, the survival rate of each test sample was used as an indicator of its sweat resistance. (Sweat resistance evaluation test / evaluation method) Based on the above test results, regarding sweat resistance, i.e., the retention rate after sweating, in the forearm, test cases with a retention rate of 50% to 100% were evaluated as "good" (hereinafter referred to as "○"), test cases with a retention rate of 40% to less than 50% were evaluated as "neither good nor bad" (hereinafter referred to as "△"), and test cases with a retention rate of less than 40% were evaluated as "bad" (hereinafter referred to as "×"). Similarly, in the foot, test cases with a retention rate of 90% to 100% were evaluated as "good" (hereinafter referred to as "○"), test cases with a retention rate of 80% to less than 90% were evaluated as "neither good nor bad" (hereinafter referred to as "△"), and test cases with a retention rate of less than 80% were evaluated as "bad" (hereinafter referred to as "×"). Even after sweating, test cases with a retention rate of ○ (evaluated) were judged to be good. (Sweat resistance evaluation test / summary) Comparative Example 1 and Example 4 are compared. In Comparative Example 1, the sweat resistance evaluation on the forearm was negative (×), while in Example 4, the sweat resistance evaluation on the forearm was positive (○). Similarly, in Comparative Example 1, the sweat resistance evaluation on the foot was negative (×), while in Example 4, the sweat resistance evaluation on the foot was positive (○). From these results, it can be seen that in Example 4, which used a film-forming agent, the washing away of the active ingredient due to sweating was suppressed compared to Comparative Example 1, which did not use a film-forming agent.

[0098] Let's examine this in more detail. Looking at the retention rate of the active ingredient in the arm after sweating, Comparative Example 1 had a retention rate of 36%, while Example 4 had a retention rate of 51%, showing approximately 1.4 times higher retention than Comparative Example 1. Furthermore, looking at the retention rate of the active ingredient in the foot after sweating, Comparative Example 1 had a retention rate of 73%, while Example 4 had a retention rate of 97%, showing approximately 1.3 times higher retention than Comparative Example 1. As described above, in both the arm and leg areas, Example 4 showed a higher retention rate compared to Comparative Example 1.

[0099] As described above, the human repellent according to the present invention contains an active ingredient having a repellent effect, a film-forming agent that forms a film layer, and a volatile solvent. More preferably, it contains two or more types of film-forming agents with different chemical structures, and even more preferably, a combination of two or more types of silicones, thereby achieving and maintaining both water resistance and evaporative properties. For this reason, it can maintain a repellent effect against pests for a long period of time, even against sweat generated from within the body, especially dripping sweat during outdoor exercise.

Claims

1. A human repellent that is applied directly to the skin of the human body to deter pests from approaching the human body, It contains at least an active ingredient, a film-forming agent, and a volatile solvent, A human repellent characterized in that the active ingredient is at least one or more selected from N,N-diethyl-m-toluamide, picaridin, 3-[N-acetyl-N-butyl]-aminopropionate ethyl ester, and p-menthanediol compounds.

2. The human repellent according to claim 1, characterized in that the film-forming agent is a combination of two or more silicones having different chemical structures.

3. A human repellent further containing an emulsifier, characterized in that the emulsifier is a silicone-based emulsifier, as described in claim 1.

4. The human repellent according to claim 1, characterized in that the film-forming agent is a combination of an acrylic polymer having a silicone structure and a silicone network resin.

5. The human repellent according to claim 1, characterized in that the film-forming agent is a combination of alkyl acrylate copolymer methylpolysiloxane ester and trimethylsiloxysilicate.

6. The film-forming agent is acrylic acid [-CH ２ CH(R)COO-] or methacrylic acid [-CH ２ C(CH ３ )(COOH)-] as a repeating unit in the main chain, and dimethylsiloxane [-(CH ３ ) ２ Si-O-] as a repeating unit in the side chain; and a silicone network resin having [(CH ３ ) ３ SiO ０．５ units and [SiO ２ units as repeating units, wherein the repellent for human body according to claim 1 is characterized in that the film-forming agent is a combination of the polymer and the silicone network resin.

7. The repellent for human use according to claim 1, characterized in that the volatile solvent contains a combination of linear silicone oil and cyclic silicone oil.

8. The human repellent according to claim 1, characterized in that the aforementioned human repellent is an emulsion product sealed in a container.

9. The human repellent according to claim 1, characterized in that the aforementioned human repellent is a spray product sealed in a container with a spray nozzle.

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