Novel insect repellent composition

Abstract

The present invention relates to a physical and universally effective insect barrier, a particulate having an outer shell containing shellac or tree resin and an inner matrix containing beeswax and at least one insect and / or arachnid repellent, and a composition containing an adhesion promoter, to the use thereof for protecting plants or objects from insects and arachnids, and to a method for producing the particulate.

Description

Technical Field

[0001] The present invention relates to the field of insect or spider repellents for protecting organisms. The present invention also provides an insect / spider repellent composition that provides a physical barrier against biting insects such as ticks and spiders, as well as a method for producing the same.

Background Art

[0002] Insects, particularly ticks, mosquitoes, and flies, especially blood-sucking flies, are a year-round problem and are often considered pests for both animals and humans. Insects can transmit many different diseases, and when bitten, they can cause itching and / or discomfort to both animals and humans, and may also lead to infections in the bitten area. In addition, many humans and animals are allergic to being bitten by various insects or to insect infestations, and may have severe allergic reactions caused by insects, even resulting in death. Furthermore, with regard to livestock and pets, insects can cause serious economic problems.

[0003] As a result, compositions for repelling or killing insects are commonly used to keep insects away from animals and humans. However, many of the currently commercially available insecticides, including those available for human and / or household use, contain strong irritant chemicals that can be present at toxic concentrations for humans and animals. In addition, many common insecticide compositions are designed specifically for certain types of insects. Repellents are often selectively applied to certain insect species / spider species such as certain mosquito species or ticks, but are relatively ineffective against other insect species such as flies. Finally, the development of resistance to conventional repellents or toxins is being increasingly reported.

[0004] In particular, various undesirable side effects have been observed after the use of commercially available insecticides. These side effects include immediate or delayed neurotoxic reactions, asphyxiation, headache, and / or nausea. Furthermore, the strong irritant chemicals typically contained in currently available insecticides are known to cause significant skin irritation when applied directly to biological surfaces such as animal or human skin. In addition, most conventional insect repellents contain synthetic insecticides or essential oils. Synthetic repellents or contact insecticides generally have the drawback of having a certain degree of toxicity or, in some cases, a strong allergic effect when applied directly to the skin. The effects of conventional repellents last only for about a few hours. Some of the known insect repellents are harmful to the environment. In particular, they are toxic to aquatic organisms (the development of newt larvae) or act as contact poisons, but do not prevent the process of being stung very effectively, which is a major drawback in terms of disease transmission.

[0005] Currently, a wide variety of products are commercially available, and their raw material components have been known for a long time (e.g., N,N-diethyl-meta-toluamide (DEET) or para-menthane-3,8-diol (PMD), and chrysanthemum derivatives, i.e., extracts of the genus Chrysanthemum effective against mosquitoes, or icaridine / pecaridine against ticks). On the other hand, essential oils have also been increasingly used to supplement insect / tick repellents.

[0006] In any case, the effects of known products are limited to about 8 hours. None of the commercially available products are effective for more than one day against organisms, let alone economically feasible for livestock. Although heat-evaporative insect repellents are commercially available, they show spatially limited effectiveness, i.e., they are effective only "near the socket", are too selective and costly for application to livestock, and lack long-term effectiveness. Prolonging the adhesion of conventional insect repellents has been improved by formulating them as creams, but so far, further protection, i.e., physical protection, has not been considered or achieved by formulation, nor has the effect itself been enhanced, let alone the handling or reduction of toxic (side) effects.

[0007] Ogilvie-Battersby J.et al. reported the encapsulation of geraniol in gelatin / arabic gum, and in this case, microcapsules were obtained by using coacervation. This extended the release of geraniol, and the application of the above microcapsules as an insect repellent with long-term persistence was tested (Colloids and Surfaces A, 2022, vol.640).

[0008] US5221535 describes a micro-suspension system containing an insect repellent such as DEET together with a layer of phospholipid. The core of the liposphere is a solid insect repellent or an insect repellent dispersed in a solid vehicle such as wax.

[0009] Microcapsules containing a core with an active substance and a coating layer system with two layers of shellac and a pH adjusting substance are disclosed in WO2017 / 182350A1.

[0010] Amberkar Tejashree et al. reported on microcapsules with a beeswax core and a phenol-formaldehyde shell, and their processing (The 2 ndInternational Online Conference on Polymer Science - polymers and Nanotechnology for Industry 4.0, 2021, pp 1 - 5)

[0011] Da Silva Marcio R.M. et al. have reviewed and disclosed natural insect repellent formulations such as essential oils derived from geranium, eucalyptus, or lavender (Acta Tropica, 2020, vol.212).

[0012] Tavares M. et al. have provided an overview of insect repellent formulations (International Journal of Pharmaceutics, 2018, vol.539, no.1 - 2, pp.190 - 209).

[0013] In equestrian sports or horse breeding in general, there is a strong demand for effective and non - toxic insect repellents, especially considering the health and psychological burdens on animals and humans. Considering accompanying factors such as cost, compatibility, especially environmental compatibility, and effectiveness, there is no repellent that is effectively sustainable at an affordable price.

[0014] Therefore, there is an urgent need for improved long - lasting compositions for insect repellency that provide safer and more effective alternatives to existing chemical - based insecticides. Summary of the Invention Problems to be Solved by the Invention

[0015] Therefore, an object of the present invention is to provide a safe and long - lasting insect and / or spider repellent composition to which plants, humans, and animals show good tolerance. Means for Solving the Problems

[0016] This object is solved by the subject matter recited in the claims and further described herein. A physical and thus universally effective insect barrier is provided herein.

[0017] According to the present invention, i) - An outer shell comprising shellac or tree resin, and - An internal matrix comprising beeswax, and at least one insect and / or arachnid repellent, and having microparticles, and ii) An adhesion promoter selected from the group consisting of propolis, cetyl alcohol, cocoa butter, lysophosphatidylcholine, and magnesium silicate hydrate (talcum), A composition is provided that includes.

[0018] The composition of the present invention specifically prevents the beeswax of the outer shell and the internal matrix (core) containing shellac or tree resin from penetrating the biting means and proboscis of insects by following along with respect to the biting means and proboscis of insects.

[0019] The surprising effect of this composition is based in particular on the effective encapsulation of the insect / arachnid repellent. The adhesion promoter can in particular adhere to the body hair of animals and also act as a skin protectant in addition to the olfactory / chemical effect of the insect / arachnid repellent contained in the core of the microparticles.

[0020] In an alternative embodiment, the adhesion promoter adheres to surfaces, in particular to the cuticle or trichomes of plants. Thus, the composition of the present invention has physical strength, is water resistant, and is self-closing with respect to various biting insects and / or arachnids upon topical administration to a subject by body temperature that can lead to melting of the composition, and thus can further provide a long-term stable barrier.

[0021] Specifically, when applied to the surface of a plant, the composition of the present invention is advantageous because it also provides a long-term stable barrier that does not interfere with the exchange of gaseous components with the environment. In addition, the presence of beeswax and, optionally, propolis can also have a supporting effect on the treatment and healing of insect bites and other wounds caused by insects.

[0022] The compositions described herein have an effect that persists for a long time, particularly for more than two days, against stinging insects and spiders (mites). Since the repellent raw material component is stabilized by the core of fine particles, it is protected from being washed away by water. As a result, while the wax material forms a physical and skin-friendly barrier on the object to be treated, it is released into the surrounding air over a long period of time.

[0023] According to a specific embodiment, the adhesion promoter is propolis. In a further specific embodiment, the tree resin is pine resin or gum arabic. In one embodiment, the repellent is a natural and / or synthetic repellent, specifically, it is a lipophilic repellent.

[0024] Specifically, the synthetic repellents are selected from the group consisting of hydroxyethyl isobutyl piperidine carboxylate, permethrin, ethyl butyl acetylaminopropionate, diethyltoluamide (DEET), p-cymol, α-isomethyl ionone, and benzyl benzoate, acetamiprid, or any combination thereof. Specifically, the natural repellents are selected from the group consisting of Artemisia princeps, Artemisia princeps derivatives, extracts of the genus Chrysanthemum, borneol, lemon eucalyptus oil, thyme oil, tea tree oil, neem oil, Swiss stone pine oil, cumin oil, marjoram oil, sage oil, linalool, geraniol, cinnamyl alcohol, hydroxycitronellal, citronellol, coumarin, limonene, and eugenol, garlic extract, or any combination thereof.

[0025] In a specific embodiment, the outer shell of the microparticles described herein includes shellac and propolis. In a further embodiment, the composition described herein further contains alcohol, specifically ethanol and / or glycerol.

[0026] In a further embodiment, the internal matrix of the microparticles further includes an odorant and / or a sunscreen agent, specifically a sunscreen agent selected from titanium dioxide and zinc oxide.

[0027] Specifically, the microparticles described herein have an average particle size in the range of 20 to 500 μm. Furthermore, herein, a topical composition containing the composition of the present invention is provided, which is formulated as a balm, cream, powder, lotion, liquid, emulsion, gel, ointment, paste, pen, spray, or aerosol.

[0028] Specifically, the topical composition described herein contains microparticles containing beeswax in the range of 5 to 20%, shellac in the range of 1 to 10%, propolis in the range of 1 to 10%, an insect repellent in the range of 1 to 10%, and glycerin and / or oil in the range of 10 to 40%.

[0029] Furthermore, herein, a method for producing microparticles having an outer shell containing shellac or tree resin and an internal matrix containing beeswax and at least one insect and / or spider repellent, the following continuous steps i. a) molten beeswax, b) one or more insect and / or spider repellents, c) shellac or tree resin solubilized in alcohol, mixing and stirring; ii. constructing microparticles by performing an ultrasonic treatment step at a temperature in the range of 40 to 50 °C; is provided.

[0030] Specifically, the adhesion promoter is added in i. In a further embodiment of the method described herein, a carrier material, specifically glycerin or vegetable oil, is added to the microparticles, and optionally, a second sonication step is performed at a temperature within the range of 40 to 50 °C.

[0031] Also provided herein is the use of the composition of the present invention or the topical composition of the present invention as an insect and / or spider repellent. As another option, provided herein is the use of the composition of the present invention or the topical composition of the present invention for the treatment of plants or seedlings, humans or non-human animals, where the non-human animals are selected from domestic pets including canids and felids, equids such as horses, bovids, ovines, livestock including pigs or sheep, goats, monkeys, etc.

[0032] According to one embodiment, the plant may be, but is not limited to, a crop such as cereals, rice, wheat, rye, oats, barley, millet, maize, soybeans, or any kind of seeds.

[0033] Furthermore, provided herein is a method of protecting a plant, specifically a broadleaf plant or a coniferous plant, a seed or a seedling, or an animal from bites or stings by insects or spiders, the method comprising the step of topically administering the composition or topical composition described herein to the plant or animal.

[0034] The use of the composition of the present invention as an insect / spider defense is particularly effective against hairy animals or hairy regions of the above animals, specifically against horses. In the case of dogs and humans, the wax film formed after topical administration to the skin is not perceived as bothersome, so each composition can protect against insects. BRIEF DESCRIPTION OF THE DRAWINGS

[0035]

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Mode for Carrying Out the Invention

[0036] As used herein, the terms "comprise", "contain", "have", and "include" may be used synonymously and are to be understood as non-limiting definitions where additional members or parts or elements are possible. "Consisting" is considered the closest definition that does not include additional elements of the defining characteristics of consisting of. Thus, "comprising" has a broader meaning and includes the definition of "consisting".

[0037] As used herein, the term "about" means the same value or a value that differs by ±5% from the given value. As used in this specification and the claims, the singular forms, such as "a", "an", and "the", include the plural unless the context clearly indicates otherwise.

[0038] The terms "subject" or "animal" can be used interchangeably. The composition of the present invention contains fine particles. The above-mentioned fine particles are composed of an internal matrix or core encapsulated by an external shell or diaphragm.

[0039] The external shell or capsule contains shellac or tree resin. Shellac is a natural bioadhesive polymer and is an excretion product of a type of scale insect (Kerria Lacca) that creates so-called leaf varnish on special trees in a specific area. It is scraped directly from the tree and purified with ethanol. The melting point of shellac is about 75 °C. Shellac is soluble in alkaline solutions of ammonia, sodium borate, sodium carbonate, and sodium hydroxide, and also in various organic solvents. When dissolved in alcohol (e.g., ethanol) for application, a coating with excellent durability and hardness can be obtained. After gentle hydrolysis, shellac produces a complex mixture of aliphatic and alicyclic hydroxy acids and their polymers, and its exact composition varies depending on the source of the shellac and the harvesting season. The main component of the aliphatic component is aleuritic acid, while the main alicyclic component is shellolic acid. Shellac has UV resistance.

[0040] According to the present invention, using shellac, stable aggregates are formed in an ethanol-based solution together with beeswax liquefied by heating, and it further undergoes a homogenization process (ultrasonic treatment), specifically in the presence of propolis and oil. Shellac can form a gel-like shell on the surface of the beeswax aggregates to stabilize the colloid. After the evaporation of ethanol and in the presence of water, shellac crystallizes irreversibly, and it stabilizes the wax layer at the interface with air.

[0041] "Tree resin", specifically soft tree resin, is a hydrocarbon secretion of many plants, generally conifers such as cedar, acacia tree, Douglas fir, cypress, pine, and hemlock, but not limited to these. Most plant resins are composed of terpenes. Specific components are α-pinene, β-pinene, δ-3-carene, and sabinene, the monocyclic terpenes limonene and terpinolene, and small amounts of the tricyclic sesquiterpenes longifolene, caryophyllene, and δ-cadinene. There are also resins that contain a high proportion of resin acids.

[0042] "Gum arabic" is a natural gum also known as Sudan gum, acacia gum, gum Arabic, gum acacia, acacia, Senegal gum, and Indian gum. It originally consists of the solidified sap of two trees of the Acacia sensu lato species, Senegalia senegal and Vachellia seyal. The term "gum arabic" does not legally indicate a specific plant source. This gum is commercially collected from wild trees. Gum arabic is a complex mixture of glycoproteins and polysaccharides that are mainly polymers of arabinose and galactose. It is water-soluble.

[0043] "Matsuyani" is produced from oleoresin (turpentine) collected from various types of pine trees, and then boiling this to remove essential oils. "Beeswax", cera flava, is soluble in ethanol and insoluble in water. Beeswax is oxygen-permeable. The main components are long-chain hydrocarbons (myricin, or mainly myricyl palmitate) (weight ratio: approximately 65%), free cerotic acid, melissic acid, and similar acids (12%), saturated hydrocarbons (approximately 14%), alcohols (approximately 1%), and other, partly unknown substances such as aromatic substances specific to bee species (6%).

[0044] One of the important properties of beeswax is its microcidal property combined with skin compatibility, which cannot be achieved with other polymers such as paraffin or silicone. Therefore, when administered to the skin, the skin is protected but not "sealed", and at the same time, the formulation has durability against microbial / fungal parasitism.

[0045] Beeswax can form a water-stable layer, and when combined with shellac, also a natural product derived from lac insects, it is stable due to its colloidal properties, easy to apply, and enables the formation of a self-healing film that lasts for a long time, especially on the body hair of animals.

[0046] Beeswax is also very advantageous because it can be mixed with repellents added in oily, liquid, or particulate form. As used herein, "insect / spider repellent" means any substance that inhibits the approach or settlement of insects or spiders. The above repellents may be of natural origin or synthetic origin.

[0047] Common synthetic insect repellents include, but are not limited to, indalone, p-cymol, DEET (N,N-diethyl-m-toluamide), dimethylcarbate, dimethyl phthalate, ethyl butyl acetylaminopropionate (IR3535 or ethyl ester of 3-[N-butyl-N-acetyl]-aminopropionic acid), icaridin also known as picaridin, ethyl anthranilate, anthranilic acid-based insect repellents, metofluthrin, permethrin, SS220, tricyclodecenyl allyl ether, hydroxyethyl isobutyl piperidine carboxylate, α-isomethyl ionone, and benzyl benzoate.

[0048] Common natural insect repellents include, but are not limited to, chrysanthemum derivatives such as chrysanthemum, prallethrin, and allethrin, extracts of the genus Chrysanthemum, thyme oil, tea tree oil, neem oil, Swiss stone pine oil, cumin oil, black cumin oil, marjoram oil, sage oil, linalool, geraniol, cinnamyl alcohol, hydroxycitronellal, citronella oil, citronellol, coumarin, limonene, eugenol, the bark of cinnamon, Myrica Gale, nepetalactone, lemon eucalyptus oil (p-menthane-3,8-diol, PMD), lemongrass oil, cedarwood oil, cinnamon oil, clove oil, corn mint oil, garlic oil, geranium oil, peppermint oil, rosemary oil, spearmint oil, borneol, and tobacco.

[0049] Sage oil derived from the sage plant (Salvia officinalis) is a vegetable oil with a complex composition obtained by steam extraction. What it has in common with eucalyptus is the substance cineole, for which an insect repellent effect has been reported, but sage does not have as strong an irritation as eucalyptus oil.

[0050] Further natural insect / spider repellents can be α-terpinene, Andrographis paniculata extract, basil, sweet basil (Ocimum basilicum), breadfruit, Callicarpa americana (beautyberry) extract, camphor, carbaryl, castor oil, cedar oil, celery extract, clove oil, fennel oil (Foeniculum vulgare), hinokitiol, lavender, marigold, menthol, notecatone, oleic acid, pennyroyal mint, peppermint, rosemary, and yellow nitrite shade extract.

[0051] A composition containing fine particles and an adhesion promoter can specifically physically resist the stinging / biting means of insects. Even when the membrane is incompletely formed, the mixed repellent is released and becomes effective.

[0052] The composition maintains its effect over a period of 1 to 21 days, particularly 1 to 14 days, and especially 2 to 8 days. Specifically, the composition is effective for more than 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, or 21 days, particularly when essential oils are included. The long-lasting effect of the composition may be due to a self-healing effect, because the body temperature of the object to be protected causes continuous re-melting of the wax, and as a result, a strong protective barrier is repeatedly created from reservoirs in the integument and / or on the skin, which is particularly stably integrated due to the presence of adhesion promoters such as propolis. The composition of the present invention is thus maintained on the skin for several days and even up to several weeks.

[0053] Exemplarily, the skin temperature of a horse meets the melting point of the composition but not in the integument area (body hair). Since the fine particles in the integument reach the skin over time, in horses and other animals with fur, a depot effect (self-healing effect) is thus achieved.

[0054] Particularly in the ear and eye regions where chemical repellents cannot be used directly (due to proximity to mucous membranes, or irritating or allergy-inducing effects), the fine particles in liquid formulations such as lotions. The adhesion promoters propolis, cetyl alcohol, cocoa butter, lysophosphatidylcholine, and magnesium stearate monohydrate are non-toxic materials and can also act as emulsifiers or stabilizers.

[0055] In addition to the physical protective function, the fine particles contain insect / spider repellent active substances, which can also act as effective olfactory repellents against ticks and insects. According to one aspect of the present invention, the volatility of synthetic and natural repellents is reduced by the composition of the present invention, and in addition, the stability against the influence of water is enhanced by chemical and physical methods. Thereby, not only does the effectiveness due to the physical barrier effect increase, but also the chemical effect of the agent in the fine particles lasts longer by protecting against the influence of water / oxidation.

[0056] By selecting the corresponding insect / arachnid repellent, the composition can be adapted to the population of insects present in the area. For example, the addition of marjoram, thyme, and sage exhibits strong repellent properties against the biting fly Stomoxys calcitrans.

[0057] According to the present invention, the composition is used as an insect and / or arachnid repellent. Suction-feeding insects include mosquitoes (e.g., Aedes species, Culex species, and Anopheles species), butterflies (Phletotomen), midges (Culicoides species), black flies (Simulium species), biting flies (e.g., Stomoxys calcitrans), tsetse flies (Glossina species), horse flies (Tabanus species, Haematopota species, and Chrysops species), house flies (e.g., Musca domestica and Fannia canicularis), flesh flies (e.g., Sarcophaga carnaria), flies causing myiasis (e.g., Lucilia couprina, Chrysomyia chloropyga, Hypoderma bovis, Hypoderma lineatum, Dermatobia hominis, Oestrus ovis, Gasterophilus intestinalis, Cochliomyia hominovorax), bugs (e.g., Cimex lectularius, Rhodnius prolixus, Triatoma infestans), lice (e.g., Pediculus humanus, Haematipinus suis, Damalina ovis), louse flies (e.g., Melaphagus orinus), fleas (e.g., Pulex irritans, Cthenocephalides canis, Xenopsylla cheopsis), and chiggers (e.g., Dermatophilus penetrans).

[0058] Examples of biting insects include cockroaches (e.g., Blattela germanica, Periplaneta americana, Blatta orientalis, Supella supellectilium), beetles (e.g., Sitophilus granarius, Tenebrio molitor, Dermestes lardarius, Stegobium paniceum, Anobium puntactum, Hylotrupes bajulus), termites (e.g., Reticulitermes lucifugus), and ants (e.g., Lasius niger).

[0059] Examples of mites include ticks (e.g., Ornithodorus moubata, Ixodes ricinus, Boophilus microplus, Amblyomma hebreum) and mites in the narrow sense (e.g., Sarcoptes scabiei, Dermanyssus gallinae).

[0060] The composition of the present invention further comprises one or more adhesion promoters, specifically propolis, agar, cetyl alcohol, cocoa butter, lysophosphatidylcholine, and magnesium silicate hydrate (talcum), magnesium stearate, or any combination thereof. The adhesion promoter may be present free in the composition or may adhere to the outer shell.

[0061] As used herein, "propolis" or "bee glue" is a complex mixture that can vary from hive to hive, region to region, and season to season. It is usually dark brown, but green, red, black, and white hues may be seen depending on the resin source found in a particular hive area. The main constituents are water-insoluble flavonoids, phenolic acids, and many antioxidants. Propolis can act as a binder and emulsifier, has bactericidal properties, and is soluble in ethanol and ethanol / water mixtures.

[0062] North temperate propolis has approximately 50 types of constituents, mainly resin and vegetable balsam (50%), wax (30%), essential oils (10%), and pollen (5%). Propolis also contains a persistent lipophilic acaricide, a natural insecticide that inhibits mite parasitism. Overall, flavonoids, phenolic acids, and phenolic aldehydes are common constituents, while coumarins, stilbenes, and lignans are less common. Propolis can adhere beeswax to all kinds of materials (such as wood, stone). In this regard, propolis can be used for the adhesion of wax to skin / hair. Propolis also has a skin healing effect.

[0063] Particles containing beeswax and a repellent are coated with shellac and combined with an adhesion promoter to form a stable aggregate as a colloid, which can encapsulate a hydrophobic repellent and the repellent is slowly released after topical administration.

[0064] Cetyl alcohol, also known as hexadecane-1-ol and palmityl alcohol, is a C-16 fatty alcohol with the formula CH3(CH2) 15 OH. Cetyl alcohol takes the form of a waxy white solid or flakes at room temperature.

[0065] Cocoa butter, also called theobroma oil, is a pale yellow edible oil extracted from cocoa beans. Its melting point is 34 - 38 °C. Lysophosphatidylcholine, also known as lysophosphatidylcholine (LPC, lysoPC), is a type of chemical compound derived from phosphatidylcholine. Lysophosphatidylcholine has the following structure, where R is a variable fatty acid chain.

[0066]

Chemical formula

[0067] Talcum (talc) is a clay mineral with the chemical formula Mg3Si4O10 It is composed of magnesium silicate hydrate which is (OH)2. Specifically, the composition contains shellac, beeswax, and propolis together with an insect / spider repellent.

[0068] Magnesium stearate is a chemical compound of formula Mg2. This is a soap composed of a salt containing 2 equivalents of stearic acid and 1 equivalent of magnesium cation. Magnesium stearate is a white water-insoluble powder. Its uses utilize its softness, insolubility in many solvents, and low toxicity.

[0069] The composition may further contain an alcohol, specifically ethanol or glycerol, or a combination thereof, specifically up to 20% by weight / volume at most. A sunscreen protectant may be further contained in the internal matrix, or in an alternative embodiment, added to the composition as an additional raw material component.

[0070] A sunscreen protective agent is, for example, an organic substance (light protection filter) that is liquid or crystalline at room temperature, absorbs ultraviolet light, and can release the absorbed energy in the form of radiation of a longer wavelength, such as heat. The UVB filter may be oil-soluble or water-soluble. Oil-soluble substances include, for example, 3-benzylidenecamphor or 3-benzylidenenorcamphor and its derivatives, such as 3-(4-methylbenzylidene)camphor; 4-aminobenzoic acid derivatives, preferably 2-ethylhexyl 4-(dimethylamino)benzoate, 2-octyl 4-(dimethylamino)benzoate, and amyl 4-(dimethylamino)benzoate; esters of cinnamic acid, specifically 2-ethylhexyl 4-methoxycinnamate, propyl 4-methoxycinnamate, isoamyl 4-methoxycinnamate, 2-ethylhexyl 2-cyano-3,3-diphenylcinnamate (octocrylene); esters of salicylic acid, specifically 2-ethylhexyl salicylate, 4-isopropylbenzyl salicylate, monomethyl salicylate; derivatives of benzophenone, specifically 2-hydroxy-4-methoxybenzophenone, 2-hydroxy-4-methoxy-4-methylbenzophenone, 2,2-dihydroxy-4-methoxybenzophenone; esters of benzylmalonic acid, specifically di-2-ethylhexyl 4-methoxybenzylmalonate; triazine derivatives, such as 2,4,6-trianilino-(p-carbo-2-ethyl-1-hexyloxy)-1,3,5-triazine and octyltriazone, or dioctylbutamidotriazine; propane-1,3-dione, 1-(4-tert-butylphenyl)-3-(4-methoxyphenyl)propane-1,3-dione, etc.; and ketotricyclo(5.2.1.0)decane derivatives.

[0071] Suitable water-soluble substances are 2-phenylbenzimidazole-5-sulfonic acid and its alkali, alkaline earth, ammonium, and alkylammonium salts; sulfonic acid derivatives of benzophenone, specifically 2-hydroxy-4-methoxybenzophenone-5-sulfonic acid and its salts; sulfonic acid derivatives of 3-benzylidenecamphor, such as 4-(2-oxo-3-bornylidene-methyl)benzenesulfonic acid and 2-methyl-5-(2-oxo-3-bornylidene)sulfonic acid and their salts, etc. In particular, derivatives of benzoylmethane, 1-(4'-tert-butyl-phenyl)-3-(4'-methoxyphenyl)propane-1,3-dione, 4-tert-butyl-4'-methoxydibenzoyl-methane, 1-phenyl-3-(4-isopropylphenyl)-propane-1,3-dione, etc., and furthermore enamine compounds and colloidal lignin are suitable as typical UV-A filters.

[0072] UV-A and UV-B filters may of course be used in combination. In addition, insoluble light-protective pigments, i.e., finely dispersed metal oxides or salts, are also suitable for this purpose. Examples of suitable metal oxides are, in particular, zinc oxide and titanium dioxide, and oxides of iron, zirconium, silicon, manganese, aluminum, and cerium, and mixtures thereof. Silicate (talc), barium sulfate, or zinc stearate may be used as the salt. The particles may have an average particle size of less than 100 nm, preferably 5 - 50 nm, particularly 15 - 30 nm. The pigments may also be surface-treated, i.e., hydrophilized or hydrophobized. A typical example is coated titanium dioxide. Silicone, particularly trialkoxyoctylsilane or simethicone, may be used as a hydrophobic coating agent. In sunscreens, so-called micro-pigments or nano-pigments are particularly used as encapsulated active ingredient components. Preferably, micronized zinc oxide may be used.

[0073] The repellent substance may be contained in the internal matrix or, in addition, added to the composition as a further raw material component. Natural flavors can be extracts of flowers (lily, lavender, rose, jasmine, neroli, ylang-ylang), stems and leaves (geranium, patchouli, petitgrain), fruits (anise, coriander, cumin, juniper), fruit peels (bergamot, lemon, orange), roots (mace, angelica, celery, cardamom, costus, iris, calamus), woods (pine, sandalwood, guaiac, cedar, rosewood), herbs and grasses (tarragon, lemongrass, sage, thyme), needles and twigs (fir, spruce, pine, mountain pine), resins and balsams (galbanum, elemi, benzoin, myrrh, olibanum, opopanax). Animal-derived raw materials such as civet and castoreum may also be used. Typical synthetic flavor compounds are products of the ester, ether, aldehyde, ketone, alcohol, and hydrocarbon types. Examples of ester-type flavor compounds include benzyl acetate, phenoxyethyl isobutyrate, p-tert-butylcyclohexyl acetate, linalyl acetate, dimethylbenzylcarbinyl acetate, phenylethyl acetate, linalyl benzoate, benzyl formate, ethylmethylphenylglycinate, allylcyclohexyl propionate, styrallyl propionate, and benzyl salicylate. Examples of ethers include benzyl ethyl ether, and examples of aldehydes include straight-chain alkanals having 8 to 18 carbon atoms, citral, citronellal, citronellyloxyacetaldehyde, cyclamen aldehyde, hydroxycitronellal, lilial, and bourgeonal. Examples of ketones and alcohols include anethole, citronellol, eugenol, isoeugenol, geraniol, linalool, phenylethyl alcohol, and terpineol, and examples of hydrocarbons mainly include terpenes and balsams. However, preferably, a mixture of different flavors that together create an attractive scent is used.Volatile essential oils with lower volatility, which are mainly used as aroma components, are also suitable as perfume oils. For example, sage oil, chamomile oil, clove oil, Melissa oil, mint oil, cinnamon leaf oil, lime blossom oil, juniper berry oil, vetiver oil, oliban oil, galbanum oil, labolanum oil, and lavandin oil. Preferably, bergamot oil, dihydromyrcenol, linalool, linalyl acetate, citronellol, phenylethyl alcohol, α-hexylcinnamaldehyde, geraniol, benzylacetone, cyclamen aldehyde, linalool, ambroxan, indole, hedione, sandelice (sandalbutenol), lemon oil, mandarin oil, orange oil, allylamyl glycolate, cyclovertal, lavandin oil, muscat sage oil, β-damascenone, geranium oil, bourbon, cyclohexyl salicylate, Vertofix Coeur, Iso-E-Super, Fixolide, Evernyl, Iraldein (registered trademark) gamma, phenylacetic acid, geranyl acetate, benzyl acetate, rose oxide, irotyl, and floramate are used alone or as a mixture.

[0074] As used herein, fine particles are particles having a particle size of 0.1 to 1000 μm, preferably, the average particle size is in the range of 10 to 700 μm, specifically 20 to 500 μm, more specifically 50 to 250 μm.

[0075] The compositions described herein may be in any form suitable for topical application to the skin, specifically to hair or fur. Non-limiting examples thereof are balsams, creams, powders, lotions, liquids, emulsions, gels, ointments, pastes, pens, sprays, shampoos, or aerosols. Emulsifiers, fillers such as polymers such as cellulose derivatives, PEG, oil / fatty acid mixtures, petrolatum, lanolin, and hydrogels may be added to the composition, and non-limiting examples thereof are Nivea®, Bepanthen®, or some soap, etc.

[0076] In a specific embodiment, the microparticles include beeswax in the range of 5 to 20% by weight / volume, specifically in the range of 5 to 10% by weight / volume; shellac in the range of 1 to 20% by weight / volume, specifically in the range of 5 to 10% by weight / volume; propolis in the range of 1 to 10% by weight / volume, specifically in the range of 1 to 5% by weight / volume; an insect repellent in the range of 1 to 10% by weight / volume, and optionally, glycerin and / or oil in the range of 10 to 50% by weight / volume. The adhesion promoter may be present in an amount of at least 5% by weight / volume, specifically in the range of 5 to 60% by weight / volume, specifically in the range of 5 to 50% by weight / volume, 5 to 40% by weight / volume, 5 to 30% by weight / volume, or 5 to 20% by weight / volume.

[0077] A further aspect of the present invention is the production of the microparticles of the composition described herein. The method includes a step of mixing and stirring molten beeswax carefully heated to the melting point, i.e., molten beeswax heated to a temperature of about 62 to 65°C. One or more insect and / or spider repellents and shellac or tree resin solubilized in alcohol, specifically ethanol, are added, and microparticles are formed by performing an ultrasonic treatment step at a temperature in the range of 40 to 50°C. Optionally, an adhesive is added before the ultrasonic treatment, specifically, it is propolis dissolved in ethanol, and in this case, the whole composition may have the gel-like properties of balsam.

[0078] The composition thus obtained can be used as a stock or base preparation, which can later be formulated into a cream, lotion, gel, or spray by adding specific substances.

[0079] The above composition formulated with additional excipients to provide the corresponding state of aggregation as desired is preferably stored at room temperature, protected from light. The composition of the present invention is stable for at least 6 months, specifically 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18 months or more.

[0080] A carrier material, specifically glycerin or vegetable oil, may be added to the microparticles, and if desired, a second ultrasonic treatment step is performed at a temperature within the range of 40 to 50 °C. Such a carrier material may be glycerin, oil, or a commercially available skin care cream, in which case a cream is produced. When the composition is emulsified in an aqueous solution, a lotion can be produced. When mixed with a powder such as talcum (magnesium stearate hydrate), a coarse powder suitable for treating long body hair is obtained.

[0081] Some examples of methods in which the composition according to the present invention can be used are shown below. Use as a balm for horses and the legs of animals and other livestock: When the formulation is applied to the area to be protected above the hoof using a sponge / cloth / towel, a wax film is formed by the composition, which provides a strong physical barrier and, depending on the type of repellent, produces an odor effect with a depot effect, which is stably maintained for several days and weeks even when exposed to water.

[0082] Use as a cream agent for horses and other animals and livestock: In addition, by adding a carrier substance (cream) to the composition of the present invention, specifically, since the ear canal may be blocked, in particular, in sensitive areas (such as the ear) where a spray agent is not suitable and a thick layer of substance is not desirable, targeted application can be enabled. Non-limiting examples of cream agents are Nivea®, Beiersdorf, Hamburg, Germany, and Bepanthen®, Bayer, Austria GmbH.

[0083] Application to the neck region of horses and other animals, specifically livestock: The composition may be emulsified in an aqueous solution by further ultrasonic treatment, thereby obtaining a lotion that can be applied over a wide area by rubbing or by a spray agent. If the spray process is perceived as a noise that stimulates, the head region of the animal cannot be treated very much, and also, the eyes / mucosa should not be treated with a spray agent.

[0084] Application to dogs, for example, as a balm / powder: The composition formulated as a lotion can be applied to short-haired animals, especially for tick repellent, or as a balm, to the short-haired or hairless abdominal region. In the case of long fur, a coarse powder formulation containing the composition of the present invention is suitable. For example, by adding repellents such as cumin and neem oil, a repellent effect is achieved, and furthermore, a depot effect is obtained by the storage characteristics of the composition, whereby the repellent characteristics against insects and spiders have an effect that lasts for a long time. By administering this substance to the skin, a systemic effect can also be expected.

[0085] Application to humans: As an insect / tick repellent, application to humans is also possible, and the composition can be applied to the skin without causing the irritating / allergic effects of the essential oil that may be present in the fine particles as desired.

[0086] The composition can be used for the treatment of human or non-human animals. Specifically, the non-human animals can include domestic pets such as canids like male dogs, female dogs, or puppies, felids like male cats, female cats, or kittens, equids such as horses like gelded horses, mares, foals, fillies, or stallions, bovids such as male cows, female cows, heifers, steers, or calves, ovines like male sheep, female sheep, or lambs, suids such as female pigs, male pigs, pre-pubertal castrated pigs, post-pubertal castrated pigs, piglets, or piglets, etc. Insect / arachnid repellents that are generally known to harm each animal are not included in the composition.

[0087] The use for protecting plants and seedlings from pests and diseases includes protection through the composition against nano / microbiological invaders such as fungi and unwanted bacterial / viral species. On a larger scale, plants and seedlings are protected from arthropods and nematodes, for example, weevils, aphids, thrips, leaf beetles, whiteflies, spider mites, caterpillars, moths, and wireworms, earwigs, spiders, pill bugs, Colorado potato beetles, etc. Compositions formulated with each repellent may also have the potential to protect seeds and seedlings from mice and birds.

Examples

[0088] The examples described herein are illustrative of the present invention and are not intended to be limiting of the present invention. Different embodiments of the present invention have been described in accordance with the present invention. Many modifications and changes may be made to the techniques described and shown herein without departing from the scope of the present invention. Therefore, it should be understood that the examples are merely illustrative and do not limit the scope of the present invention.

[0089] Example 1: Raw materials for the "proof of principle" formulation: Basic formulation

[0090]

Table 1

[0091] Added selected repellent substances: - thyme oil - marjoram oil - tea tree oil - Swiss stone pine oil - neem oil (especially to obtain acaricidal effect) - black cumin / cumin oil - sage oil The repellent substances were added to the base formulation before ultrasonic treatment (about 2 ml per 100 ml of base formulation).

[0092] Treatment of horses: legs The suitability for horses was widely tested. On the legs, especially in the type with moderately hairy front legs (Arabian), the slow release of the repellent and its slow disappearance due to the balm formulation made it possible to efficiently reduce being bitten by insects over several days to several weeks. In this example, it was shown that the physical barrier function of the composition of the present invention effectively avoided being bitten by insects. At the same time, no ticks were seen in the treated area.

[0093] Ears It was shown that the cream formulation containing the composition of the present invention is very suitable for treating the outer ears to avoid being bitten or bothered by insects in the head region. In this regard, since the ears are sensitive to occlusion and the spray sound is generally difficult to tolerate, especially in the head region, thick balm or spray formulations containing the composition are not very preferred formulations.

[0094] Alternative addition of known repellents: - Autan® - “Anti-Brumm”® Before ultrasonic treatment, it was added to the basic formulation at a ratio of 1:10.

[0095] The ultrasonic treatment was carried out for approximately 15 minutes. In a 50 ml Falcon (placed in a beaker filled with water at 20 °C), ultrasonic treatment was performed with an output of W (watts) at 70% amplitude (at approximately 2-minute intervals). After the treatment, the sample was warmed to approximately 40 °C.

[0096] The stability of the basic formulation was shown to be at least 6 months at room temperature (under light protection). The presence of microorganisms / fungi was not detected, and the integrity of the particles was fully confirmed by optical microscope images.

[0097] Preparation of the spray formulation: Before use, the composition was diluted 1:10 with ethanol (30%), 20 wt / vol% of deionized water was added, and the spray bottle was filled. As another option, the composition may be added to a basic emulsion (neutral lipid) as a carrier material.

[0098] Preparation of the ear ointment formulation (varies depending on the desired final consistency): - Agar, derived from red algae - To give the final product a gel-like property - Other emulsifiers (except propolis) - Cetyl alcohol and lysophosphatidylcholine - A very soft, yellowish-white cream was obtained. - Cocoa / Shea butter - A cream is obtained, but at a higher concentration (20 - 40 wt / wt%) and a harder consistency like that of a deodorant stick.

[0099] Preparation of the powder formulation: Magnesium stearate powder or natural hydrated magnesium silicate was mixed with the prepared basic formulation (see above) as a filler, (-emulsification was added-), and a coarse powder that can be dispersed on the coat of long-haired dogs was formed.

[0100] Example 2 Basic formulation

[0101]

Table 2

[0102] Ultrasonic treatment: The basic formulation was subjected to ultrasonic treatment (at approximately 2-minute intervals) in a 50 ml Falcon at amplitudes of 70% for approximately 15 minutes within a range not exceeding 50 °C (before and after adding glycerin / vegetable oil / carrier material).

[0103] Preparation of spray formulations: The composition was diluted 1:10 with ethanol and 20% in deionized water before use and filled into a spray bottle. As an alternative, the composition was added to a basic emulsion (neutral lipid) as a carrier material.

[0104] Preparation of powder formulations: (In the case of a long hair coat) 50 wt / wt% of the basic formulation was mixed with magnesium stearate powder (or alternatively magnesium silicate hydrate) or silicon dioxide (particle size less than 45 μm) and applied to the coat.

[0105] Preparation of ointment formulations: The basic formulation (see above) was stirred in a carrier substance at a ratio of 1:2. The carrier substances were as follows. - Nivea® - Bepanthen® - Soap (for shampoo) Polyethylene glycol or similar inert carrier materials are also envisaged (a mixture of panthenol as a skin protectant or a sunscreen material such as TiO₂ or some other light filter substance is conceivable).

[0106] Addition of repellents / odoriferous substances: - Thyme oil - Marjoram oil - Sage oil - Cumin / black cumin - (Neem oil - due to its strong acaricidal effect) Added to the base formulation before ultrasonic treatment (approximately 1 - 2 ml per 100 ml of base formulation).

[0107] Alternative: Addition of conventional chemical repellents: - Autan (Registered Trademark) - 「Anti - Brumm」(Registered Trademark) Before ultrasonic treatment, it was added to the basic formulation at a ratio of 1:10.

[0108] The stability of the base formulation was tested over 12 months at room temperature (under light protection), and there was no visible deterioration, such as a change in odor quality or the presence of microorganisms (microscopic analysis).

[0109] Example 3: Proof of Particle Formation The composition was prepared as described above, and a lipid - stainable fluorescent dye (BODIPY (trademark)) was added. This emits green light after appropriate excitation.

[0110] In Figure 1, large shellac particles can be seen in this optical microscope image on the left, but they are not visible in the fluorescence excitation image (right side), and only the free accumulation of wax indicated by the arrow is visible in the transmission image. From this result, it is confirmed that the shellac coating effectively encapsulates the wax particles (without defects).

[0111] The above results (the presence of an intact protective shellac shell) were confirmed by the following experiment. The above microparticles were incubated in an organic strong solvent (dimethyl sulfoxide, DMSO). Then, the penetration of the fluorescent dye into the wax core of the particles was observed. (The scale bar in all images corresponds to 20 μm and was measured in phosphate - buffered solution). The results are shown in Figure 2.

[0112] The layer - forming characteristics were also visually confirmed by SEM (scanning electron microscope observation) after air - drying and gold sputtering. The results are shown in Figure 3.

[0113] Example 4: A microscope slide is used as a substrate, and a droplet of the formulation is applied and sealed with a coverslip. A standard optical microscope is used to visualize the structure of the sample. A reference slide with a scale bar is used to identify the average particle size of the spherical particles. The temperature is raised by a fan and measured with a non-contact infrared thermometer.

[0114] The results are shown in Figures 4 to 7. Figure 4: After further heating (above approximately 40 °C): Formation of the front of the melted wax from top right to bottom left, and in the bottom left, an area of non-melted material is still visible.

[0115] Figure 5: After in situ heating to approximately 40 °C with warm air (infrared measurement on the coverslip), a film visible just above the (glass - slide) surface is formed, and at the same time, oil / wax / shellac particles are preserved (related to the depot effect).

[0116] Figure 6: Sequential images: In situ crack repair. The layer on the slide surface was "damaged" with a needle, and the "repair" was recorded by raising the temperature from an initial temperature of approximately 30 °C. (The time elapsed from top to bottom is approximately 2 minutes)

[0117] Figure 7: After application and evaporation of ethanol, the formation of layers and the aggregation of particles (wax / shellac aggregates) become visible under an optical microscope. These aggregated aggregates act as a reservoir for repellents and at the same time as a source of wax, thus causing the depot / self - repair effect. From there, the essential oils or repellents contained are sequentially released into the surrounding air.

[0118] Example 5: In the growth experiment using treated corn, typical germination behavior of corn was obtained, and the occurrence of mold was reduced compared to untreated corn.

[0119] Figure 8 shows a corn seedling with a protective layer made from the composition. Figure 8A shows the edge part of the corn under a micrograph (40×). A wax layer that appears white is visible, which is the result of treatment with the composition. In Figure 8B, as a result of the wax layer, light is reflected from the surface treated with the composition.

Claims

1. i) - An external shell containing shellac or tree resin, - Beeswax, and an internal matrix containing at least one insect and / or spider repellent, Particles having, and ii) An adhesion promoter selected from the group consisting of propolis, cetyl alcohol, cocoa butter, lysophosphatidylcholine, and magnesium silicate hydrate (talcum). A composition comprising.

2. The composition according to claim 1, wherein the adhesion promoter is propolis.

3. The composition according to claim 1 or 2, wherein the tree resin is pineyani or gum arabic.

4. The repellent is a natural repellent or a synthetic repellent. Specifically, the repellent is a lipophilic repellent. Specifically, the synthetic repellent is selected from the group consisting of hydroxyethyl isobutyl piperidine carboxylate, permethrin, ethyl butyl acetylaminopropionate, diethyltoluamide (DEET), p-cymol, α-isomethyl ionone, and benzyl benzoate. Specifically, the natural repellent is selected from the group consisting of Artemisia princeps, extracts of the genus Chrysanthemum, borneol, lemon eucalyptus oil, thyme oil, tea tree oil, neem oil, Swiss stone pine oil, cumin oil, marjoram oil, sage oil, linalool, geraniol, cinnamyl alcohol, hydroxycitronellal, citronellol, coumarin, limonene, and eugenol, or any combination thereof. The composition according to any one of claims 1 to 3.

5. The composition according to any one of claims 1 to 4, wherein the external shell contains shellac and propolis.

6. The composition according to any one of claims 1 to 5, further comprising an alcohol, specifically ethanol and / or glycerol.

7. The composition according to any one of claims 1 to 6, wherein the internal matrix further comprises an odorant and / or a sunscreen agent, specifically a sunscreen agent selected from titanium dioxide and zinc oxide.

8. The composition according to any one of claims 1 to 7, wherein the particles have an average particle size in the range of 20 to 500 μm.

9. A topical composition comprising the composition according to any one of claims 1 to 8 and being a balm, cream, powder, lotion, liquid, emulsion, gel, ointment, paste, pen, spray, or aerosol.

10. The topical composition according to claim 9, comprising beeswax within the range of 5 to 20%, shellac within the range of 1 to 20%, propolis within the range of 1 to 10%, and an insect repellent within the range of 1 to 10%, at least 5% of an adhesion promoter, and, optionally, glycerin and / or oil within the range of 10 to 40% in the form of microparticles.

11. A method for producing microparticles having an outer shell containing shellac or a tree resin, beeswax, and an inner matrix containing at least one insect and / or spider repellent, the method comprising the following sequential steps: i. a) molten beeswax, b) one or more insect and / or spider repellents, c) shellac or a tree resin solubilized in alcohol, mixing and stirring; ii. constructing microparticles by performing an ultrasonic treatment step at a temperature within the range of 40 to 50°C. A method comprising the above steps.

12. The method according to claim 11, wherein the adhesion promoter is added in step i.

13. The method according to claim 11 or 12, wherein a carrier material, specifically glycerin or a vegetable oil, is added to the microparticles, and, optionally, a second ultrasonic treatment step is performed at a temperature within the range of 40 to 50°C.

14. The composition according to any one of claims 1 to 8, or the topical composition according to claim 9 or 10, for use in the treatment of humans or non-human animals.

15. The composition for use according to claim 14, wherein the non-human animal is selected from domestic pets including canids and felids, equids such as horses, bovids, ovines, livestock including pigs or sheep, goats, monkeys, etc.

16. Use of the composition according to any one of claims 1 to 8, or the topical composition according to claim 9 or 10, for the treatment of plants, specifically broad-leaved plants, coniferous plants, seeds, or seedlings.

17. Use of the composition according to claim 16, wherein the plant is selected from the group consisting of rice, wheat, rye, oats, barley, millet, maize, and soybeans.

18. A method for protecting a plant or an animal from bites or stings by insects or spiders, the method comprising the step of topically administering to the animal the composition according to any one of claims 1 to 8, or the topical composition according to claim 9 or 10.

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