Composition containing natural pyrethrin and specific phosphorus-based antioxidant and use thereof

Abstract

The present invention relates to a composition containing natural pyrethrin and a phosphorus-based antioxidant selected from the group P. Group P: tetraphenyldipropylene glycol diphosphite, diisodecylphenylphosphite, diphenyl mono (2-ethylhexyl) phosphite, di-n-decylphenylphosphite, diphenylmono (tridecyl)phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'- methylenebis(4,6-di-tert-butylphenyl) 2-ethylhexylphosphite, hydrogenated bisphenol A pentaerythritol phosphite polymer, distearyl pentaerythritol diphosphite, tris(2,4-di-tert-butylphenyl) phosphite, and tris(tridecyl) phosphite.

Description

Composition Containing Natural Pyrethrin and Specific Phosphorus-Based Antioxidant and Its Use

[0001] The present invention relates to a composition containing natural pyrethrin and a specific phosphorus-based antioxidant and its use. This application claims priority based on Japanese Patent Application No. 2024-162211 filed in Japan on September 19, 2024, and incorporates its content herein by reference.

[0002] Due to the increasing natural orientation of consumers, natural pyrethrin has attracted attention (for example, Patent Document 1). Natural pyrethrin is suitably used for pest control, etc., but due to the instability of its chemical structure, the pest control effect may decrease over time or when exposed to high temperatures.

[0003] International Publication No. 2022 / 220294

[0004] An object of the present invention is to provide a new composition containing natural pyrethrin that has excellent pest control effect maintenance or thermal stability.

[0005] The inventors of the present invention conducted studies to provide a new composition containing natural pyrethrin. As a result, they found that a composition containing natural pyrethrin, a specific antioxidant, and a solid carrier has excellent effects, and completed the present invention.

[0006] The present invention includes, but is not limited to, the following embodiments. [1] A composition containing a natural pyrethrin and one or more phosphorus-based antioxidants selected from group P (hereinafter sometimes referred to as the present invention composition): Group P: A group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, hydrogenated bisphenol A / pentaerythritol phosphite polymer, distearyl pentaerythritol diphosphite, tris(2,4-di-tert-butylphenyl) phosphite, and tris(tridecyl) phosphite. [2] The composition according to [1], wherein group P consists of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, hydrogenated bisphenol A / pentaerythritol phosphite polymer, and distearyl pentaerythritol diphosphite. [3] The composition according to [1], wherein group P consists of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, and distearyl pentaerythritol diphosphite.[4] The composition according to [1], wherein group P is the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, and 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane. [5] The composition according to [1], wherein group P is the group consisting of tetraphenyldipropylene glycol diphosphite and diisodecylphenyl phosphite. [6] The composition according to any one of [1] to [5], wherein the mass ratio of natural pyrethrin to one or more phosphorus-based antioxidants selected from group P is in the range of 1:0.01 to 1:50. [7] The composition according to any one of [1] to [5], further comprising a phenolic antioxidant. [8] The composition according to [7], wherein the phenolic antioxidant comprises at least one selected from the group consisting of dibutylhydroxytoluene and butylhydroxyanisole. [9] A heat-dispersion insecticide containing the composition according to any one of [1] to [8].

[10] An insecticide mat containing the composition according to any one of [1] to [8].

[11] A method for controlling sanitary pests using the composition according to any one of [1] to [8].

[12] A method for controlling sanitary pests using the heat-dispersion insecticide according to [9].

[13] A method for controlling sanitary pests using the insecticide mat according to

[10] .

[0007] According to the present invention, it is possible to provide a novel composition containing natural pyrethrins that maintains pest control effectiveness or exhibits excellent thermal stability.

[0008] Figure 1 is a cross-sectional view of a heat vaporization type insecticide device using a liquid insecticide bottle. Figure 2 is a perspective view of a heat vaporization type insecticide device using an insect control mat.

[0009] <Natural Pyrethrins> The natural pyrethrins used in this invention contain six compounds as active ingredients: Pyrethrin I, Pyrethrin II, Cinerin I, Cinerin II, Jasmoline I, and Jasmoline II. Natural pyrethrins can typically be obtained as an extract or dried pyrethrin powder, obtained by extracting the active ingredients from a powder made by collecting, drying, and grinding only the calyx of the flower of chrysanthemum (Tanacetum cinerariifolium or Chrysanthemum cinerariaefolium) using a suitable solvent (also called a solvent), such as an organic solvent like methanol. In addition to the six compounds mentioned above, natural pyrethrins may also contain plant-derived impurities (such as fatty acids and flavonoids).In addition to the aforementioned Chrysanthemum cinerariaefolium, other plants from which natural pyrethrins can be obtained include Calendula officinalis, Chrysanthemum coccinum, Tagetes erecta, Tagetes minuta, Zinnia elegans, and Zinnia linnearis (References 1: Adnane. H. Alain, C. & Chantal, B. 2000. The Production of Pyrethrins by Plant Cell and Tissue Cultures of Chrysanthemum cinerariaefolium and Tagetes Species. Critical Reviews in Plant Sciences, 19(1):69-89; Reference 2: Kudakasseril, GJ and Staba, EJ 1988. Insecticidal phytochemicals. In: Cell Culture and Somatic Cell Genetics of Plants. pp. 537-552. Constabel, F. and Vasil, IK, Eds., Academic Press, New York, Reference 3: John E. Casida, Gary B. Quistad. 1995. PYRETHRUM FLOWERS, Production, Chemistry, Toxicology, and Uses. pp.123-125, Oxford University Press.).

[0010] The plant species and varieties that serve as the source of natural pyrethrins used in this invention are not limited to those mentioned above. The cultivation methods, cultivation conditions (weather, origin, soil type, etc.), harvest time, harvest part, harvesting method, washing method, extraction method, and purification method of the plants are not particularly limited. Natural pyrethrins used in this invention also include, for example, natural pyrethrins obtained using a vector into which a gene encoding a pyrethrin biosynthesis enzyme is incorporated.

[0011] The mass ratios of the six compounds used in the natural pyrethrins of the present invention—pyrethrin I, pyrethrin II, synerin I, synerin II, jasmolin I, and jasmolin II—are not particularly limited. Any mass ratio can be set for each compound in the range of 0.001 to 99% by mass relative to the total amount of natural pyrethrins. Typically, however, the natural pyrethrins are contained in the following mass ratios: pyrethrin I at 10 to 70% by mass, pyrethrin II at 10 to 70% by mass, synerin I at 1 to 20% by mass, synerin II at 1 to 20% by mass, jasmolin I at 1 to 20% by mass, and jasmolin II at 1 to 20% by mass, relative to the total amount of natural pyrethrins. As a specific example of a mixing ratio (mass ratio), [Pyrethrin I: Synerin I: Jasmolin I: Pyrethrin II: Synerin II: Jasmolin II] = 38.0:7.3:4.0:35.0:11.7:4.0 (Reference 3).

[0012] Examples of natural pyrethrins used in the present invention include pyrethrin I (total amount of pyrethrin I, synerin I, and jasmolin I) and pyrethrin II (total amount of pyrethrin II, synerin II, and jasmolin II), with pyrethrin I at 20 to 40% by mass and pyrethrin II at 12 to 31% by mass relative to the total amount of natural pyrethrin. The total amount of pyrethrin I and pyrethrin II in the natural pyrethrin is usually 10 to 99% by mass, preferably 15 to 90% by mass, and more preferably 20 to 85% by mass, relative to the total amount of natural pyrethrin.

[0013] <Phosphorus-based antioxidants> The phosphorus-based antioxidants used in this invention will now be described. As phosphorus-based antioxidants used in this specification, eleven phosphorus-based antioxidants listed in group P can be cited because they exhibit excellent effects in improving the thermal stability of natural pyrethrins, and one or more phosphorus-based antioxidants are selected and used from group P. The eleven phosphorus-based antioxidants listed in group P are all known compounds in themselves, and each can be manufactured or obtained by manufacturing according to or in accordance with a known method, or by obtaining a commercially available product. Furthermore, the phosphorus-based antioxidants may be indicated by different names depending on the nomenclature system of the compound or the language in which they are written, but if they are compounds with the same structure, they are all included in this specification. In other words, compounds registered under the same CAS registration number are all included in this specification as the same compound, even if the name is written differently.

[0014] The phosphorus-based antioxidants (1) to (11) that constitute group P are shown below. (1) Tetraphenyldipropylene glycol diphosphite (CAS registration number: 80584-85-6) is commercially available, for example, as JPP-100 (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.). (2) Diisodecylphenyl phosphite (CAS registration number: 25550-98-5) is commercially available from many suppliers (e.g., ADEKA). (3) Diphenyl mono(2-ethylhexyl) phosphite (CAS registration number: 15647-08-2) is commercially available, for example, as JPM-308 (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.). (4) Di-n-decylphenyl phosphite (CAS registration number: 1254-78-0) is commercially available from many suppliers (e.g., Shaanxi Dideu Medichem). (5) Diphenyl mono(tridecyl) phosphite (CAS registration number: 60628-17-3) is commercially available, for example, as JPM-313 (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.).

[0015] (6) 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane (CAS registration number: 64012-42-6) is commercially available, for example, as JPP-88 (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.). (7) 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite (CAS registration number: 126050-54-2) is commercially available, for example, as Adekastab HP-10 (trade name) (manufactured by ADEKA Corporation). (8) Hydrogenated bisphenol A / pentaerythritol phosphite polymer (CAS registration number: 101320-77-8) is commercially available, for example, as JPH-3800 (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.). (9) Distearyl pentaerythritol diphosphite (CAS registration number: 3806-34-6) is commercially available, for example, as Adekastab PEP-8 (trade name) (manufactured by ADEKA Corporation). (10) Tris(2,4-di-tert-butylphenyl) phosphite (CAS registration number: 31570-04-4) is commercially available, for example, as Irgafos168 (trade name) (manufactured by BASF Japan Ltd). (11) Tris(tridecyl) phosphite (CAS registration number: 77745-66-5) is commercially available, for example, as JP-333E (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.).

[0016] Of the phosphorus-based antioxidants (1) to (11) constituting group P, phosphorus-based antioxidants (1) to (9) are preferred, phosphorus-based antioxidants (1) to (6) are more preferred, and phosphorus-based antioxidants (1) and (2) are particularly preferred, from the viewpoint of maintaining the storage stability of natural pyrethrins.

[0017] In one embodiment of the present invention, the phosphorus-based antioxidant may be one or more phosphorus-based antioxidants selected from the group consisting of (1) tetraphenyldipropylene glycol diphosphite, (2) diisodecylphenyl phosphite, (3) diphenyl mono(2-ethylhexyl) phosphite, (4) di-n-decylphenyl phosphite, (5) diphenyl mono(tridecyl) phosphite, (6) 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, (7) 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, and (9) distearyl pentaerythritol diphosphite.

[0018] In one embodiment of the present invention, the composition of the present invention may further contain a phenolic antioxidant. Examples of such phenolic antioxidants include dibutylhydroxytoluene (hereinafter sometimes abbreviated as BHT), butylhydroxyanisole (hereinafter sometimes abbreviated as BHA), and 2,2'-methylenebis(6-tert-butyl-4-methylphenol), with BHT or BHA being preferred, and BHA being particularly preferred. In another embodiment, BHT can be suitably used as the phenolic antioxidant. BHT and BHA are commercially available, for example, from Kanto Chemical Co., Ltd. 2,2'-methylenebis(6-tert-butyl-4-methylphenol) is commercially available as Smirizer™ MDP-S. When the composition of the present invention contains a phenolic antioxidant, its content is preferably 0.01 to 10% by mass, more preferably 0.05 to 6% by mass, based on the total amount of the composition of the present invention. Furthermore, if the composition of the present invention contains a phenolic antioxidant, the mass ratio of natural pyrethrin to the phenolic antioxidant contained in the composition of the present invention is preferably 1:0.01 to 1:20, and more preferably 1:0.05 to 1:10.

[0019] In one embodiment of the present invention, the mass ratio of natural pyrethrin to one or more phosphorus-based antioxidants selected from group P is preferably 1:0.01 to 1:50, and more preferably 1:0.02 to 1:20. Specific examples of mass ratios of natural pyrethrin to one or more phosphorus-based antioxidants selected from group P include 1:0.01, 1:0.02, 1:0.03, 1:0.04, 1:0.05, 1:0.06, 1:0.07, 1:0.08, 1:0.09, 1:0.1, 1:0.2, 1:0.3, 1:04, 1:0.5, 1:0.6, 1:0.7, 1:0.8, 1:0.9, 1:1, 1:2, 1:3, 1:4, 1:5, 1:6, 1:7, 1:8, 1:9, 1:10, 1:15, 1:20, 1:25, 1:30, 1:35, 1:40, 1:45, and 1:50. In another embodiment of the present invention, the mass ratio of natural pyrethrin and one or more phosphorus-based antioxidants selected from group P to BHT and BHA is preferably 1:0.01:0:0 to 1:50:50:50, and more preferably 1:0.02:0.002:0.002 to 1:20:20:20.

[0020] The composition of the present invention can be applied to insect control agents for heat vaporization, insect control mats, and the like, as described later.

[0021] <Heat-Vaporized Insecticide Preparation> One embodiment of the present invention is a heat-vaporized insecticide preparation containing a natural pyrethrin and one or more phosphorus-based antioxidants selected from group P. The heat-vaporized insecticide preparation of one embodiment of the present invention is a preparation that can be used in a heat-vaporized insecticide device 100, for example, as shown in Figure 1. A solution 1 containing the heat-vaporized composition is filled into a liquid bottle 4. In this specification, a composition suitably used in a heat-vaporized insecticide preparation applied to a heat-vaporized insecticide device using a liquid bottle may be referred to as the heat-vaporized composition. A part of the liquid-absorbing wick 3 is immersed in the solution 1, and the liquid-absorbing wick is made to absorb the solution containing the heat-vaporized composition, and the upper part of the liquid-absorbing wick can be heated by a heating element 2. By indirectly heating the upper part of the liquid-absorbing wick to a temperature of about 60°C to about 150°C with the heating element 2, the heat-vaporized composition absorbed by the liquid-absorbing wick is vaporized into the atmosphere, thereby controlling insects. The heat vaporization insect control agent of one embodiment of the present invention is not limited to the apparatus shown in Figure 1, but can be applied to conventionally known heat vaporization insecticide devices and will exhibit excellent effects in all of them. Heat vaporization insecticide devices to which the heat vaporization insect control agent of the present invention can be applied are described, for example, in Japanese Patent Publication No. 52-12106, Japanese Utility Model Publication No. 58-45670, and Japanese Patent Publication No. 2012-176947.

[0022] In the heat-evaporative insecticide preparation of the present invention, a composition (also called the heat-evaporative composition) containing a natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is prepared in the form of a solution (solution 1) containing the composition and used. An oily solvent or an aqueous solvent is used as the solvent (also called the solvent) for preparing the heat-evaporative insecticide preparation. By dissolving the heat-evaporative composition in these solvents, a heat-evaporative insecticide preparation can be obtained. When an oily solvent is used, an oily solvent with a boiling point of 350°C or lower is usually used. Various organic solvents, mainly hydrocarbon solvents, can be used as such oily solvents, but aliphatic hydrocarbon solvents (paraffinic solvents or unsaturated aliphatic hydrocarbon solvents, or mixtures thereof) with a boiling point range of 150 to 350°C are particularly preferred. Examples of such solvents include paraffinic solvents such as n-paraffin and isoparaffin; deodorizing kerosene; and sewing machine oil (e.g., Sewing Lube (manufactured by ENEOS Corporation)), with paraffinic solvents being preferred. Specific examples of paraffinic solvents include Solvent No. 0 H (manufactured by ENEOS Corporation), Solvent No. 0 M (manufactured by ENEOS Corporation), Solvent No. 0 L (manufactured by ENEOS Corporation), IP Solvent 2028 (manufactured by Idemitsu Kosan Co., Ltd.), Norper 12 (manufactured by ExxonMobil Corporation), Norper 13 (manufactured by ExxonMobil Chemicals, Inc.), Norper 15 (manufactured by ExxonMobil Corporation), Isopar M (manufactured by ExxonMobil Corporation), Isopar L (manufactured by ExxonMobil Corporation), Isopar V (manufactured by ExxonMobil Corporation), and Isopar G (manufactured by ExxonMobil Corporation). Examples of organic solvents other than the hydrocarbon-based solvents mentioned above include glycerin, propylene glycol, methanol, acetone, xylene, chlorcene, isopropanol, and chloroform. When aqueous solvents are used, glycol ethers and water are usually used. Examples of such glycol ethers include ethylene glycol ethers, propylene glycol ethers, and dialkyl glycol ethers, with ethylene glycol ethers being preferred.Furthermore, among ethylene glycol ethers, ethylene glycol monobutyl ether, diethylene glycol monobutyl ether, propylene glycol monomethyl ether, propylene glycol monoethyl ether, and propylene glycol monopropyl ether are preferred. Note that one or a mixture of two or more glycol ethers may be used. The mass ratio of glycol ether to water is usually in the range of 1:0.4 to 1:8.5, preferably in the range of 1:1 to 1:8.5, and more preferably in the range of 1:1.4 to 1:3.6. The solvent may further contain an auxiliary solvent (also called an auxiliary solvent), and examples of auxiliary solvents include diisopropyl adipate, diisodecyl adipate, diisobutyl adipate, isopropyl myristate, isopropanol, benzyl acetate, ethanol, sucrose fatty acid ester, sorbitan fatty acid ester, propylene carbonate, 1,3-butylene glycol, and polyoxyethylene hydrogenated castor oil. A different solvent from the solvent used may be selected as the auxiliary solvent. For example, when a paraffinic solvent is used as the solvent, diisopropyl adipate or isopropyl myristate is preferred as the auxiliary solvent. The solvent content in the heat-vaporized insecticide is usually 65 to 99.99% by mass, preferably 80 to 99.8% by mass, based on the total amount of the heat-vaporized insecticide. If the heat-vaporized insecticide further contains an auxiliary solvent, the content of the auxiliary solvent is usually 5 to 30% by mass, preferably 10 to 25% by mass, based on the total amount of the heat-vaporized insecticide. The concentration of the composition (also called the heat-vaporized composition) containing natural pyrethrin and one or more phosphorus-based antioxidants selected from group P in the heat-vaporized insecticide is usually prepared to be about 1 to 50% by mass, preferably about 1 to 40% by mass, based on the total amount of the heat-vaporized insecticide. Here, the sum of the solvent content (percentage) and the concentration of the heat-evaporation composition shall not exceed 100% by mass. Furthermore, if an auxiliary solvent is included, the sum of the solvent content (percentage), the auxiliary solvent content, and the concentration of the heat-evaporation composition shall not exceed 100% by mass.The heat-evaporative insect control formulation of the present invention may also contain other components such as thickeners, surfactants, stabilizers, preservatives, or synergists.

[0023] In the present invention, one embodiment of a composition (also called a heat-evaporation composition) containing natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a heat-evaporation composition containing natural pyrethrin and tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8 The composition contains one or more phosphorus-based antioxidants selected from the group consisting of 10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, hydrogenated bisphenol A / pentaerythritol phosphite polymer, distearyl pentaerythritol diphosphite, tris(2,4-di-tert-butylphenyl) phosphite, and tris(tridecyl) phosphite.

[0024] Another embodiment of the composition (also called a heat-evaporation composition) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition containing natural pyrethrin and one or more phosphorus-based antioxidants selected from the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, hydrogenated bisphenol A / pentaerythritol phosphite polymer, and distearyl pentaerythritol diphosphite.

[0025] Another embodiment of the composition (also called a heat-evaporation composition) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition containing natural pyrethrin and one or more phosphorus-based antioxidants selected from the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, and distearyl pentaerythritol diphosphite.

[0026] Another embodiment of the composition (also called a heat-evaporation composition) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition containing natural pyrethrin and one or more phosphorus-based antioxidants selected from the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, and 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane.

[0027] Another embodiment of the composition (also called a heat-evaporation composition) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition containing natural pyrethrin and one or more phosphorus-based antioxidants selected from the group consisting of tetraphenyldipropylene glycol diphosphite and diisodecylphenyl phosphite.

[0028] Another embodiment of the composition (also called a composition for heat evaporation) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition that further contains at least one phenolic antioxidant selected from the group consisting of BHT and BHA.

[0029] Another embodiment of the composition (also called a heat-evaporation composition) containing the natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition in which the mass ratio of the natural pyrethrin to one or more phosphorus-based antioxidants selected from group P is 1:0.01 to 1:50, and yet another embodiment is a composition in which the mass ratio of the natural pyrethrin to one or more phosphorus-based antioxidants selected from group P is 1:0.02 to 1:20.

[0030] Another embodiment of the composition (also called a heat-evaporation composition) containing the natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition in which the mass ratio of natural pyrethrin, one or more phosphorus-based antioxidants selected from group P, BHT, and BHA is 1:0.01:0:0 to 1:50:50:50, and yet another embodiment is a composition in which the mass ratio of natural pyrethrin, one or more phosphorus-based antioxidants selected from group P, BHT, and BHA is 1:0.02:0.002:0.002 to 1:20:20:20.

[0031] One embodiment of the heat-evaporation composition of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass, of one or more phosphorus-based antioxidants selected from group P, and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass, of a phenolic antioxidant such as BHT or BHA, per 200 parts by mass of natural pyrethrin; another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass, of a phenolic antioxidant such as BHT or BHA; and yet another embodiment is a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0032] Another embodiment of the heat-evaporation composition of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass, of tetraphenyldipropylene glycol diphosphite and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass, of a phenolic antioxidant such as BHT or BHA, per 200 parts by mass of natural pyrethrin; another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass, of a phenolic antioxidant such as BHT or BHA; and yet another embodiment is a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0033] Another embodiment of the heat-evaporation composition of the present invention is a composition comprising 200 parts by mass of natural pyrethrin, 140 to 160 parts by mass of tetraphenyldipropylene glycol diphosphite, and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0034] Another embodiment of the heat-evaporation composition of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass, of diisodecylphenyl phosphite and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass, of a phenolic antioxidant such as BHT or BHA, per 200 parts by mass of natural pyrethrin; another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass, of a phenolic antioxidant such as BHT or BHA; and yet another embodiment is a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0035] Another embodiment of the heat-evaporation composition of the present invention is a composition comprising 200 parts by mass of natural pyrethrin, 140 to 160 parts by mass of diisodecylphenyl phosphite, and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0036] Another embodiment of the heat-evaporation composition of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass, of diphenyl mono(2-ethylhexyl) phosphite and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass, of a phenolic antioxidant such as BHT or BHA, per 200 parts by mass of natural pyrethrin; another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass, of a phenolic antioxidant such as BHT or BHA; and yet another embodiment is a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0037] Another embodiment of the heat-evaporation composition of the present invention is a composition comprising 200 parts by mass of natural pyrethrin, 140 to 160 parts by mass of diphenyl mono(2-ethylhexyl) phosphite, and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0038] Another embodiment of the heat-evaporation composition of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass, of di-n-decylphenyl phosphite and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass, of a phenolic antioxidant such as BHT or BHA, per 200 parts by mass of natural pyrethrin; another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass, of a phenolic antioxidant such as BHT or BHA; and yet another embodiment is a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0039] Another embodiment of the heat-evaporation composition of the present invention is a composition comprising 200 parts by mass of natural pyrethrin, 140 to 160 parts by mass of di-n-decylphenyl phosphite, and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0040] Another embodiment of the composition for heat evaporation of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass of diphenylmono(tridecyl)phosphite and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass of a phenolic antioxidant such as BHT or BHA with respect to 200 parts by mass of natural pyrethrin. Another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass of a phenolic antioxidant such as BHT or BHA in the composition. Still another embodiment is a composition not containing a phenolic antioxidant such as BHT or BHA in the composition.

[0041] Another embodiment of the composition for heat evaporation of the present invention is a composition containing 140 to 160 parts by mass of diphenylmono(tridecyl)phosphite and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably not containing a phenolic antioxidant such as BHT or BHA with respect to 200 parts by mass of natural pyrethrin.

[0042] Another embodiment of the composition for heat evaporation of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass of 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass of a phenolic antioxidant such as BHT or BHA. Another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass of a phenolic antioxidant such as BHT or BHA in the composition. Still another embodiment is a composition not containing a phenolic antioxidant such as BHT or BHA in the composition.

[0043] Another embodiment of the heat-evaporation composition of the present invention is a composition comprising 200 parts by mass of natural pyrethrin, 140 to 160 parts by mass of 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0044] Another embodiment of the heat-evaporation composition of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass, of 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass, of a phenolic antioxidant such as BHT or BHA, per 200 parts by mass of natural pyrethrin; another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass, of a phenolic antioxidant such as BHT or BHA; and yet another embodiment is a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0045] Another embodiment of the heat-evaporation composition of the present invention is a composition comprising 200 parts by mass of natural pyrethrin, 140 to 160 parts by mass of 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0046] Another embodiment of the composition for heat evaporation of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass of a hydrogenated bisphenol A - pentaerythritol phosphite polymer and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass of a phenolic antioxidant such as BHT or BHA with respect to 200 parts by mass of natural pyrethrin. Another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass of a phenolic antioxidant such as BHT or BHA in the above composition. Still another embodiment is a composition not containing a phenolic antioxidant such as BHT or BHA in the above composition.

[0047] Another embodiment of the composition for heat evaporation of the present invention is a composition containing 140 to 160 parts by mass of a hydrogenated bisphenol A - pentaerythritol phosphite polymer and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably not containing a phenolic antioxidant such as BHT or BHA with respect to 200 parts by mass of natural pyrethrin.

[0048] Another embodiment of the composition for heat evaporation of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass of distearyl pentaerythritol diphosphite and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass of a phenolic antioxidant such as BHT or BHA with respect to 200 parts by mass of natural pyrethrin. Another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass of a phenolic antioxidant such as BHT or BHA in the above composition. Still another embodiment is a composition not containing a phenolic antioxidant such as BHT or BHA in the above composition.

[0049] Another embodiment of the composition for heat evaporation of the present invention is a composition containing 140 to 160 parts by mass of distearyl pentaerythritol diphosphite and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably not containing a phenolic antioxidant such as BHT or BHA with respect to 200 parts by mass of natural pyrethrin.

[0050] Another embodiment of the heat-evaporation composition of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass, of tris(2,4-di-tert-butylphenyl) phosphite and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass, of a phenolic antioxidant such as BHT or BHA, per 200 parts by mass of natural pyrethrin; another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass, of a phenolic antioxidant such as BHT or BHA; and yet another embodiment is a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0051] Another embodiment of the heat-evaporation composition of the present invention is a composition comprising 200 parts by mass of natural pyrethrin, 140 to 160 parts by mass of tris(2,4-di-tert-butylphenyl) phosphite, and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0052] Another embodiment of the heat-evaporation composition of the present invention is a composition containing 100 to 200 parts by mass, preferably 120 to 180 parts by mass, more preferably 140 to 160 parts by mass, of tris(tridecyl)phosphite and 0 to 200 parts by mass, preferably 0 to 180 parts by mass, more preferably 0 to 160 parts by mass, of a phenolic antioxidant such as BHT or BHA, per 200 parts by mass of natural pyrethrin; another embodiment is a composition containing 0 to 10 parts by mass, preferably 0 to 5 parts by mass, of a phenolic antioxidant such as BHT or BHA; and yet another embodiment is a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0053] Another embodiment of the heat-evaporation composition of the present invention is a composition comprising 200 parts by mass of natural pyrethrin, 140 to 160 parts by mass of tris(tridecyl) phosphite, and 0 to 10 parts by mass of a phenolic antioxidant such as BHT or BHA, preferably a composition that does not contain a phenolic antioxidant such as BHT or BHA.

[0054] One embodiment of the heat-evaporative insect control formulation of the present invention is a heat-evaporative insect control formulation in which, based on the total amount of the heat-evaporative insect control formulation, the content of natural pyrethrin is 0.01 to 45% by mass, preferably 0.05 to 10% by mass, more preferably 0.1 to 1% by mass, the content of one or more phosphorus-based antioxidants selected from group P is 0.01 to 10% by mass, preferably 0.01 to 5% by mass, more preferably 0.1 to 1% by mass, the content of phenol-based antioxidants such as BHT or BHA is 0.01 to 10% by mass, preferably 0.01 to 5% by mass, more preferably 0.1 to 1% by mass, and the content of a solvent such as a paraffinic solvent is 35 to 99.97% by mass, preferably 85 to 99.9% by mass, more preferably 95 to 99% by mass. Here, the sum of the content of natural pyrethrins, phosphorus-based antioxidants, phenolic antioxidants such as BHT or BHA, and solvents such as paraffinic solvents shall not exceed 100% by mass.

[0055] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of tris(tridecyl) phosphite is 0.1 to 1% by mass, the content of BHT is 0.1 to 1% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 95 to 99% by mass. Here, the sum of the content of natural pyrethrin, tris(tridecyl) phosphite, BHT, and paraffinic solvent does not exceed 100% by mass.

[0056] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of tris(2,4-di-tert-butylphenyl) phosphite is 0.1 to 1% by mass, the content of BHT is 0.1 to 1% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 95 to 99% by mass. Here, the sum of the content of natural pyrethrin, tris(2,4-di-tert-butylphenyl) phosphite, BHT, and paraffinic solvent does not exceed 100% by mass.

[0057] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of diphenyl mono(tridecyl) phosphite is 0.1 to 5% by mass, the content of BHT is 0.01 to 10% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 64 to 89% by mass. Here, the sum of the content of natural pyrethrin, diphenyl mono(tridecyl) phosphite, BHT, diisopropyl adipate, and paraffinic solvent does not exceed 100% by mass.

[0058] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of diphenyl mono(tridecyl) phosphite is 0.1 to 5% by mass, the content of BHT is 0 to 1% by mass, the content of BHA is 0.01 to 7% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 66 to 89% by mass. Here, the sum of the content of natural pyrethrin, diphenyl mono(tridecyl) phosphite, BHT, BHA, diisopropyl adipate, and paraffinic solvent does not exceed 100% by mass.

[0059] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of di-n-decylphenyl phosphite is 0.1 to 5% by mass, the content of BHT is 0.01 to 10% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 64 to 89% by mass. Here, the sum of the content of natural pyrethrin, di-n-decylphenyl phosphite, BHT, diisopropyl adipate, and paraffinic solvent does not exceed 100% by mass.

[0060] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of tetraphenyldipropylene glycol diphosphite is 0.1 to 5% by mass, the content of BHT is 0.01 to 10% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 64 to 89% by mass. Here, the sum of the content of natural pyrethrin, tetraphenyldipropylene glycol diphosphite, BHT, diisopropyl adipate, and paraffinic solvent does not exceed 100% by mass.

[0061] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of tetraphenyldipropylene glycol diphosphite is 0.1 to 5% by mass, the content of BHT is 0 to 1% by mass, the content of BHA is 0.01 to 7% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 66 to 89% by mass. Here, the sum of the content of natural pyrethrin, tetraphenyldipropylene glycol diphosphite, BHT, BHA, diisopropyl adipate, and paraffinic solvent does not exceed 100% by mass.

[0062] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of diphenyl mono(2-ethylhexyl) phosphite is 0.1 to 5% by mass, the content of BHT is 0.01 to 10% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 64 to 89% by mass. Here, the sum of the content of natural pyrethrin, diphenyl mono(2-ethylhexyl) phosphite, BHT, diisopropyl adipate, and paraffinic solvent does not exceed 100% by mass.

[0063] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of diphenyl mono(2-ethylhexyl) phosphite is 0.1 to 5% by mass, the content of BHT is 0 to 1% by mass, the content of BHA is 0.01 to 7% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 66 to 89% by mass. Here, the sum of the content of natural pyrethrin, diphenyl mono(2-ethylhexyl) phosphite, BHT, BHA, diisopropyl adipate, and paraffinic solvent does not exceed 100% by mass.

[0064] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of diisodecylphenyl phosphite is 0.1 to 5% by mass, the content of BHT is 0.01 to 10% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 64 to 89% by mass. Here, the sum of the content of natural pyrethrin, diisodecylphenyl phosphite, BHT, diisopropyl adipate, and paraffinic solvent does not exceed 100% by mass.

[0065] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane is 0.1 to 5% by mass, the content of BHT is 0.01 to 10% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 64 to 89% by mass. Here, the sum of the content of natural pyrethrins, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, BHT, diisopropyl adipate, and paraffinic solvents does not exceed 100% by mass.

[0066] Another embodiment of the heat-vaporized insecticide preparation of the present invention is a heat-vaporized insecticide preparation in which, based on the total amount of the heat-vaporized insecticide preparation, the content of natural pyrethrin is 0.1 to 1% by mass, the content of 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane is 0.1 to 5% by mass, the content of BHT is 0 to 1% by mass, the content of BHA is 0.01 to 7% by mass, the content of diisopropyl adipate is 10 to 20% by mass, and the content of paraffinic solvent (e.g., Isopar M, Isopar L, or a mixture thereof) is 66 to 89% by mass. Here, the sum of the content of natural pyrethrins, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, BHT, BHA, diisopropyl adipate, and paraffinic solvents does not exceed 100% by mass.

[0067] Furthermore, while heating elements (heating element 2) that generate heat when electricity is applied are commonly used as heating elements in heat vaporization type insecticide devices, the device is not limited to these, and any known heating element, such as an air oxidation heating element or a heating element utilizing a platinum catalyst, can be used.

[0068] The liquid-absorbing core 3 is generally made of a porous material. As the porous material, for example, inorganic powders such as clay, talc, kaolin, silica, calcite, diatomaceous earth, gypsum, perlite, bentonite, acid clay, glass fiber, or asbestos are bonded and molded with an adhesive such as carboxymethylcellulose, starch, gum arabic, gelatin, or polyvinyl alcohol. Alternatively, inorganic substances such as clay, talc, bentonite, alumina, silica, or calcite are solidified into a core and fired, resin is molded into a core, or bundles of glass fibers are commonly used. The liquid-absorbing core may also contain dyes, preservatives, or antioxidants as appropriate, which can be added, for example, by mixing them during the bonding of the inorganic powder and the adhesive. Commercially available liquid-absorbing wicks can be used, and examples of such commercially available liquid-absorbing wicks include Fuji-Chem HK-100 (manufactured by Fuji Chemical Co., Ltd.) and Rauschert Steatite 45% (manufactured by Rauschert).

[0069] The pests that can be controlled by the heat-evaporative insect control formulation of the present invention include various harmful insects and arthropods such as mites, and in particular harmful flying insects such as Culex pipiens, Culex tritaeniorhynchus, Culex zoonii, and Culex pipiens; Aedes mosquitoes such as Aedes aegypti and Aedes albopictus; Anopheles mosquitoes such as Anopheles sinensis; midges; houseflies such as Housefly, Housefly, and Housefly; blowflies, flesh flies, fruit flies, drain flies, phorid flies, horseflies, gnats, stable flies, and biting midges. Among these, mosquitoes such as Culex pipiens, Aedes mosquitoes, and Anopheles mosquitoes are particularly targeted pests. Furthermore, the heat-evaporative insecticide formulation of the present invention is also effective against mosquitoes, flies, fleas, bed bugs, house dust mites, indoor dust mites, cockroaches, ticks, and other sanitary pests that are classified as sanitary pests that transmit diseases and cause illness in humans, and these sanitary pests can also be listed as target pests for control.

[0070] One embodiment of the present invention is a method for controlling pests, including sanitary pests, comprising heating a heat-evaporative insecticide formulation to vaporize an effective amount of the heat-evaporative composition into the atmosphere. Another embodiment of the present invention is a method for controlling pests, including sanitary pests, wherein the heating of the heat-evaporative insecticide formulation is performed by having a liquid-absorbing wick absorb a solution containing the heat-evaporative composition, and then heating the upper part of the liquid-absorbing wick with a heating element. Yet another embodiment of the present invention is a method for controlling pests, including sanitary pests, wherein the heating of the upper part of the liquid-absorbing wick with a heating element is performed by indirectly heating the upper part of the liquid-absorbing wick to a temperature of about 60°C to about 150°C with a heating element. Yet another embodiment of the present invention is a method for exterminating sanitary pests, wherein the method for controlling pests is a method for exterminating sanitary pests. In this specification, "control" is a concept that includes extermination, repellent, and prevention. "Extermination" is a concept that includes killing, knocking down, driving away, or preventing the target pest from approaching, with killing or knocking down the target pest being preferable.

[0071] <Formulation for Pest Control Mats> One embodiment of the present invention is a formulation for pest control mats containing natural pyrethrin and one or more phosphorus-based antioxidants selected from group P. The aforementioned pest control mat may also be referred to as an electric mosquito trap mat. The formulation for pest control mats of one embodiment of the present invention is a formulation that can be applied to a pest control mat 11 used in a heat vaporization type insecticide device 200 as shown in Figure 2. In the heat vaporization type insecticide device 100 of Figure 2, a pest control mat 11 containing the formulation for pest control mats is placed on a hot plate 10, and by heating the hot plate to about 140 to 200°C, the natural pyrethrin contained in the pest control mat is vaporized into the atmosphere, thereby controlling pests. Furthermore, the formulation for pest control mats of one embodiment of the present invention is a formulation that can be applied to a pest control mat used in a heat vaporization type insecticide device described in Japanese Patent Publication No. 11-510055. In the heat vaporization type insecticide device described in Japanese Patent Publication No. 11-510055, pests can be controlled by burning a fuel such as butane gas to heat the pest control mat to approximately 120 to 200°C, thereby vaporizing the pest control mat composition held in the pest control mat into the atmosphere. That is, while the heat vaporization type insecticide device 200 shown in Figure 2 heats the hot plate 10 by electric heating, the heat vaporization type insecticide device described in Japanese Patent Publication No. 11-510055 heats the hot plate inside the device by burning a fuel such as butane gas. Although there are differences in the heat source and heating temperature between the two, the principle of vaporizing the natural pyrethrin held in the pest control mat into the atmosphere by heating is the same. In this specification, a composition suitably used in a pest control mat used in a heat vaporization type insecticide device that uses a pest control mat may be referred to as a pest control mat formulation. One embodiment of the present invention's insecticide mat formulation can be applied to conventionally known insecticide mats and is not limited to the apparatus shown in Figure 2. It can also be applied to a heat vaporization type insecticide apparatus using a conventionally known insecticide mat, and in both cases, it can produce excellent results.

[0072] Another embodiment of the present invention is an insect control mat in which an insect control mat formulation is held.

[0073] The aforementioned insect control mat is a fibrous carrier or a porous carrier on which an insect control mat formulation containing natural pyrethrin and an antioxidant is held. In one embodiment of the present invention, the insect control mat formulation usually contains 5 to 40% by mass of the total amount of the natural pyrethrin and one or more phosphorus-based antioxidants selected from group P, relative to the total amount of the insect control mat formulation, and may further contain a solvent (also called a solvent), a dye, a stabilizer, a fragrance, etc. as appropriate.

[0074] Examples of such solvents include ester-based solvents and hydrocarbon-based solvents. Specific examples of ester-based solvents include diisodecyl phthalate, di-2-ethylhexyl phthalate, diisopropyl adipate, diisobutyl adipate, diisodecyl adipate, di-n-octyl sebacate, diisononyl adipate, di-2-ethylhexyl sebacate, di-2-ethylhexyl azelate, di-n-hexyl azelate, di-2-ethylhexyl dodecanoate, dibutoxyethoxyethyl adipate, isopropyl palmitate, dioctyl adipate, di-n-butyl sebacate, acetyl tributyl citrate, di-2-ethylhexyl malate, isopropyl myristate, benzyl acetate, sucrose fatty acid esters, and sorbitan fatty acid esters. Examples of hydrocarbon-based solvents include n-paraffin-based solvents, isoparaffin-based solvents, and naphthenic solvents. Specifically, examples of n-paraffin solvents include dodecane, tridecane, tetradecane, pentadecane, Norper 13 (trade name, manufactured by ExxonMobil Chemicals Ltd.), Norper 15 (trade name, manufactured by ExxonMobil Chemicals Ltd.), n-paraffin grade M (trade name, manufactured by Nippon Oil Corporation), n-paraffin grade H (trade name, manufactured by Nippon Oil Corporation), and neothiozol (trade name, manufactured by Chuo Kasei Co., Ltd.). Examples of isoparaffin solvents include Isopar M (trade name, E Examples of suitable solvents include ExxonMobil (product name), Isopar V (product name, ExxonMobil), IP Solvent 2028 (product name, Exxon Kosan Co., Ltd.), IP Solvent 2835 (product name, Exxon Kosan Co., Ltd.), and Shellsol™ (product name, Shell Chemicals Japan Co., Ltd.). Examples of naphthenic solvents include Exol D80 (product name, ExxonMobil), Exol D110 (product name, ExxonMobil), and Exol D130 (product name, ExxonMobil). Kerosene can also be used. Other solvents include isopropanol, ethanol, propylene carbonate, 1,3-butylene glycol, and polyoxyethylene hydrogenated castor oil. Two or more of the above solvents may be used in combination, and solvents with different polarity and other properties can be combined.When using solvents with different properties in combination, one of them can be used as an auxiliary solvent. For example, when an n-paraffinic solvent, an isoparaffinic solvent, or a naphthenic solvent is used as the solvent, diisopropyl adipate or isopropyl myristate can be used as an auxiliary solvent.

[0075] The aforementioned insecticide mat formulation typically contains one or more of these solvents. The content is usually about 50 to 95% by mass of the total amount of the insecticide mat formulation. If the insecticide mat formulation further contains an auxiliary solvent, the content of the auxiliary solvent is usually 5 to 30% by mass, preferably 10 to 25% by mass, of the total amount of the insecticide mat formulation. The concentration of the composition (also called the insecticide mat composition) containing natural pyrethrin and one or more phosphorus-based antioxidants selected from group P in the insecticide mat formulation is usually prepared to be about 1 to 50% by mass, preferably about 1 to 40% by mass, and more preferably about 4 to 40% by mass, of the total amount of the insecticide mat formulation. Here, the sum of the solvent content (content rate) and the concentration of the insecticide mat composition does not exceed 100% by mass. Furthermore, if an auxiliary solvent is included, the sum of the content (percentage) of the solvent, the content of the auxiliary solvent, and the concentration of the insecticide mat composition shall not exceed 100% by mass.

[0076] Examples of dyes include anthraquinone-based blue dyes such as 1,4-dibutylaminoanthraquinone, 1,4-diisopropylaminoanthraquinone, 1,4-bis(2,6-diethyl-4-methylphenylamino)anthraquinone, 1-methylamino-4-orthotolylaminoanthraquinone, 1-methylamino-4-methatolylaminoanthraquinone, and 1-methylamino-4-paratolylaminoanthraquinone. These dyes may be used individually, in combination of two or more, or mixed with other dyes of different colors. Examples of stabilizers include ultraviolet absorbers such as benzotriazole-based ultraviolet absorbers and benzophenone-based ultraviolet absorbers.

[0077] In the present invention, one embodiment of a composition (also called a composition for insect control mats) containing natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition containing natural pyrethrin and tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8 The composition contains one or more phosphorus-based antioxidants selected from the group consisting of 10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, hydrogenated bisphenol A / pentaerythritol phosphite polymer, distearyl pentaerythritol diphosphite, tris(2,4-di-tert-butylphenyl) phosphite, and tris(tridecyl) phosphite.

[0078] Another embodiment of the composition (also called a composition for insect control mats) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition containing natural pyrethrin and one or more phosphorus-based antioxidants selected from the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, hydrogenated bisphenol A / pentaerythritol phosphite polymer, and distearyl pentaerythritol diphosphite.

[0079] Another embodiment of the composition (also called a composition for insect control mats) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition containing natural pyrethrin and one or more phosphorus-based antioxidants selected from the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, and distearyl pentaerythritol diphosphite.

[0080] Another embodiment of the composition (also called a composition for insect control mats) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition containing natural pyrethrin and one or more phosphorus-based antioxidants selected from the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, and 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane.

[0081] Another embodiment of the composition (also known as the composition for insect control mats) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition containing natural pyrethrin and one or more phosphorus-based antioxidants selected from the group consisting of tetraphenyldipropylene glycol diphosphite and diisodecylphenyl phosphite.

[0082] Another embodiment of the composition (also known as the composition for insect control mats) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition that further contains at least one phenolic antioxidant selected from the group consisting of BHT and BHA.

[0083] Another embodiment of the composition (also called a composition for insect control mats) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition in which the mass ratio of natural pyrethrin to one or more phosphorus-based antioxidants selected from group P is 1:0.01 to 1:50, and yet another embodiment is a composition in which the mass ratio of natural pyrethrin to one or more phosphorus-based antioxidants selected from group P is 1:0.02 to 1:20.

[0084] Another embodiment of the composition (also called a composition for insect control mats) containing the aforementioned natural pyrethrin and one or more phosphorus-based antioxidants selected from group P is a composition in which the mass ratio of natural pyrethrin, one or more phosphorus-based antioxidants selected from group P, BHT, and BHA is 1:0.01:0:0 to 1:50:50:50, and yet another embodiment is a composition in which the mass ratio of natural pyrethrin, one or more phosphorus-based antioxidants selected from group P, BHT, and BHA is 1:0.02:0.002:0.002 to 1:20:20:20.

[0085] One embodiment of the insecticide mat composition of the present invention is a composition containing, with respect to 13.3 parts by mass of natural pyrethrin, 1 to 30 parts by mass, preferably 1 to 20 parts by mass, more preferably 8 to 12 parts by mass, of one or more phosphorus-based antioxidants selected from group P, and 0 to 20 parts by mass, preferably 0.01 to 20 parts by mass, more preferably 0.1 to 10 parts by mass, of a phenolic antioxidant such as BHT or BHA.

[0086] Another embodiment of the insecticide mat composition of the present invention is a composition containing 8 to 12 parts by mass of tris(tridecyl)phosphite and 0 to 5 parts by mass of BHT, with respect to 13.3 parts by mass of natural pyrethrin.

[0087] Another embodiment of the insecticide mat composition of the present invention is a composition containing 8 to 12 parts by mass of tris(tridecyl)phosphite and 1 to 5 parts by mass of BHT, with respect to 13.3 parts by mass of natural pyrethrin.

[0088] Another embodiment of the insecticide mat composition of the present invention is a composition containing 8 to 12 parts by mass of 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite and 0 to 5 parts by mass of BHT, with respect to 13.3 parts by mass of natural pyrethrin.

[0089] Another embodiment of the insecticide mat composition of the present invention is a composition containing 8 to 12 parts by mass of 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite and 1 to 5 parts by mass of BHT, with respect to 13.3 parts by mass of natural pyrethrin.

[0090] Another embodiment of the insecticide mat composition of the present invention is a composition containing 8 to 12 parts by mass of distearyl pentaerythritol diphosphite and 0 to 5 parts by mass of BHT, with respect to 13.3 parts by mass of natural pyrethrin.

[0091] Another embodiment of the insecticide mat composition of the present invention is a composition containing 8 to 12 parts by mass of distearyl pentaerythritol diphosphite and 1 to 5 parts by mass of BHT, with respect to 13.3 parts by mass of natural pyrethrin.

[0092] One embodiment of the insecticide mat formulation of the present invention is a formulation in which, with respect to the volume of the insecticide mat formulation, the mass-to-volume ratio concentration of natural pyrethrin is 1 to 40 w / v%, preferably 5 to 20 w / v%, more preferably 10 to 15 w / v%, the mass-to-volume ratio concentration of one or more phosphorus-based antioxidants selected from group P is 1 to 30 w / v%, preferably 1 to 20 w / v%, more preferably 8 to 12 w / v%, the mass-to-volume ratio concentration of a phenolic antioxidant such as BHT or BHA is 0 to 20 w / v%, preferably 1 to 10 w / v%, more preferably 1 to 5 w / v%, and the content of a solvent such as a paraffinic solvent is an amount adjusted to the above concentrations. Here, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, phosphorus-based antioxidants, phenolic antioxidants such as BHT or BHA, and solvents such as paraffinic solvents does not exceed 100 w / v%. Another embodiment of the insecticide mat formulation of the present invention may further contain an auxiliary solvent such as isopropyl myristate. When an auxiliary solvent is included, the mass-to-volume ratio concentration of the auxiliary solvent is 1 to 30 w / v%, preferably 10 to 30 w / v%, and more preferably 15 to 25 w / v%, and the amount of the solvent, such as a paraffinic solvent, is the amount used to adjust the concentration. Furthermore, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, phosphorus-based antioxidant, phenolic antioxidant such as BHT or BHA, auxiliary solvent, and solvent such as a paraffinic solvent does not exceed 100 w / v%.

[0093] Another embodiment of the insecticide mat formulation of the present invention is such that, relative to the volume of the insecticide mat formulation, the mass-to-volume ratio concentration of natural pyrethrin is 10 to 15 w / v%, the mass-to-volume ratio concentration of tris(tridecyl) phosphite is 8 to 12 w / v%, the mass-to-volume ratio concentration of BHT is 0 to 5 w / v%, and the content of a solvent such as a paraffinic solvent is adjusted to the aforementioned concentrations. Here, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, tris(tridecyl) phosphite, BHT, and the solvent such as a paraffinic solvent does not exceed 100 w / v%.

[0094] Another embodiment of the insecticide mat formulation of the present invention is such that, relative to the volume of the insecticide mat formulation, the mass-to-volume ratio concentration of natural pyrethrin is 10 to 15 w / v%, the mass-to-volume ratio concentration of tris(tridecyl) phosphite is 8 to 12 w / v%, the mass-to-volume ratio concentration of BHT is 1 to 5 w / v%, and the content of a solvent such as a paraffinic solvent is adjusted to the aforementioned concentrations. Here, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, tris(tridecyl) phosphite, BHT, and the solvent such as a paraffinic solvent does not exceed 100 w / v%.

[0095] Another embodiment of the insecticide mat formulation of the present invention may further contain an auxiliary solvent such as isopropyl myristate. When an auxiliary solvent is included, the mass-to-volume ratio concentration of the auxiliary solvent is 15 to 25 w / v%, and the amount of the solvent, such as a paraffinic solvent, is adjusted to the aforementioned concentration. Furthermore, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, tris(tridecyl) phosphite, BHT, the auxiliary solvent, and the paraffinic solvent does not exceed 100 w / v%.

[0096] Another embodiment of the insecticide mat formulation of the present invention is such that, relative to the volume of the insecticide mat formulation, the mass-to-volume ratio concentration of natural pyrethrin is 10 to 15 w / v%, the mass-to-volume ratio concentration of 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite is 8 to 12 w / v%, the mass-to-volume ratio concentration of BHT is 0 to 5 w / v%, and the content of a solvent such as a paraffinic solvent is adjusted to the aforementioned concentrations. Here, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, BHT, and the solvent such as a paraffinic solvent does not exceed 100 w / v%.

[0097] Another embodiment of the insecticide mat formulation of the present invention is such that, relative to the volume of the insecticide mat formulation, the mass-to-volume ratio concentration of natural pyrethrin is 10 to 15 w / v%, the mass-to-volume ratio concentration of 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite is 8 to 12 w / v%, the mass-to-volume ratio concentration of BHT is 1 to 5 w / v%, and the content of a solvent such as a paraffinic solvent is adjusted to the aforementioned concentrations. Here, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, BHT, and the solvent such as a paraffinic solvent does not exceed 100 w / v%.

[0098] Another embodiment of the insecticide mat formulation of the present invention may further contain an auxiliary solvent such as isopropyl myristate, and when an auxiliary solvent is included, the mass-to-volume ratio concentration of the auxiliary solvent is 15 to 25 w / v%, and the amount of the solvent such as a paraffinic solvent is adjusted to the above concentration. Furthermore, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, BHT, the auxiliary solvent, and the paraffinic solvent does not exceed 100 w / v%.

[0099] Another embodiment of the insecticide mat formulation of the present invention is such that, relative to the volume of the insecticide mat formulation, the mass-to-volume ratio concentration of natural pyrethrin is 10 to 15 w / v%, the mass-to-volume ratio concentration of distearyl pentaerythritol diphosphite is 8 to 12 w / v%, the mass-to-volume ratio concentration of BHT is 0 to 5 w / v%, and the content of a solvent such as a paraffinic solvent is adjusted to the aforementioned concentrations. Here, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, distearyl pentaerythritol diphosphite, BHT, and the solvent such as a paraffinic solvent does not exceed 100 w / v%.

[0100] Another embodiment of the insecticide mat formulation of the present invention is such that, relative to the volume of the insecticide mat formulation, the mass-to-volume ratio concentration of natural pyrethrin is 10 to 15 w / v%, the mass-to-volume ratio concentration of distearyl pentaerythritol diphosphite is 8 to 12 w / v%, the mass-to-volume ratio concentration of BHT is 1 to 5 w / v%, and the content of a solvent such as a paraffinic solvent is adjusted to the aforementioned concentrations. Here, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, distearyl pentaerythritol diphosphite, BHT, and the solvent such as a paraffinic solvent does not exceed 100 w / v%.

[0101] Another embodiment of the insecticide mat formulation of the present invention may further contain an auxiliary solvent such as isopropyl myristate, and when an auxiliary solvent is included, the mass-to-volume ratio concentration of the auxiliary solvent is 15 to 25 w / v%, and the amount of the solvent such as a paraffinic solvent is adjusted to the above concentration. Furthermore, the sum of the mass-to-volume ratio concentrations of natural pyrethrin, distearyl pentaerythritol diphosphite, BHT, the auxiliary solvent, and the solvent such as a paraffinic solvent does not exceed 100 w / v%.

[0102] An insect control mat according to one embodiment of the present invention can usually be manufactured by impregnating a fibrous carrier or porous carrier with the insect control mat formulation according to one embodiment of the present invention. Examples of fibrous carriers include natural fibers such as pulp, cellulose, and cotton, synthetic fibers such as polyester and acrylic, and inorganic fibers such as glass fibers and asbestos. Examples of porous carriers include porous inorganic materials such as diatomaceous earth, porous magnetic materials such as unglazed pottery, and porous resins such as foamed urethane and foamed polypropylene. The size of the fibrous carrier or porous carrier used in the present invention is usually 2.0 to 4.0 cm² in apparent volume before holding the insect control mat formulation. ３ (For example, 2.2 cm x 3.5 cm x 0.28 cm (approximately 2.2 cm) ３ ), 3.8cm x 4.8cm x 0.20cm (approximately 3.6cm ３ The range is approximately ), and the pest control mat of one embodiment of the present invention is a fibrous carrier or porous carrier 2.2 cm ３Each mat typically contains 20 to 1600 mg of the insect control mat formulation. In one embodiment of the present invention, the insect control mat formulation can appropriately contain other insect control active compounds, repellents, etc., which is expected to further improve its efficacy.

[0103] A pest control mat according to one embodiment of the present invention can also be manufactured by molding and processing a composition containing the aforementioned natural pyrethrin, one or more phosphorus-based antioxidants selected from group P, other components selected optionally, and a solid carrier into a desired shape using a known method. For example, such a pest control mat can be manufactured in a similar manner to the substrate used in the air treatment apparatus described in Japanese Patent Publication No. 2009-526056. Japanese Patent Publication No. 2009-526056 discloses a substrate having a pore network structure formed by adhering granular particles, in which air treatment chemicals such as natural pyrethrin can be supported within the pores. Such a substrate can be attached to the air treatment apparatus described in Japanese Patent Publication No. 2009-526056 and heated to release air treatment chemicals such as natural pyrethrin from the substrate. In other words, similar to the substrate of Japanese Patent Publication No. 2009-526056, a pest control mat can be manufactured by solidifying a composition containing the aforementioned natural pyrethrin, one or more phosphorus-based antioxidants selected from group P, other components selected optionally, and a solid carrier, and molding it into a predetermined shape.

[0104] One embodiment of the present invention provides a pest control mat formulation that is effective against the same pests as those to which the above-described heat-evaporative pest control formulation is applied. In particular, mosquitoes such as Culex mosquitoes, Aedes mosquitoes, and Anopheles mosquitoes are examples of pests that can be controlled, and it may also be effective against sanitary pests such as mosquitoes, flies, fleas, bed bugs, house dust mites, indoor dust mites, cockroaches, and ticks. One embodiment of the present invention is a method for controlling pests, including sanitary pests, which includes heating a pest control mat that holds the pest control mat formulation to evaporate an effective amount of the pest control mat composition into the atmosphere. Another embodiment of the present invention is a method for controlling pests, including sanitary pests, in which the heating of the pest control mat is performed by placing the pest control mat on a hot plate and heating the pest control mat with the heated hot plate. Another embodiment of the present invention is a method for controlling pests, including sanitary pests, wherein heating the hot plate is done by heating the hot plate to a temperature of about 140 to 200°C by electric heating. Another embodiment of the present invention is a method for controlling pests, including sanitary pests, wherein heating the hot plate is done by heating the hot plate to a temperature of about 120 to 200°C by burning fuel. Another embodiment of the present invention is a method for exterminating sanitary pests, wherein the method for controlling the target pests is a method for exterminating sanitary pests. In this specification, "control" is a concept that includes extermination, repellent, and prevention. "Extermination" is a concept that includes killing, knocking down, driving away, or keeping away the target pests, and it is preferable to kill or knock down the target pests.

[0105] The present invention will be described in more detail below with reference to examples and comparative examples, but the present invention is not limited to these examples. In the examples and comparative examples, the following natural pyrethrins, antioxidants, solvents, auxiliary solvents, and liquid-absorbing wicks were used. Natural pyrethrin 1: OMRI product manufactured by MGK; Natural pyrethrin 2: 50% natural pyrethrin (containing BHT) manufactured by BRA; Antioxidant 1: 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite (ADEKA Stab HP-10 (product name) (manufactured by ADEKA Corporation)); Antioxidant 2: Diphenyl mono(2-ethylhexyl) phosphite (JPM-308 (product name) (manufactured by Johoku Chemical Industry Co., Ltd.)); Antioxidant 3: Di-n-decylphenyl phosphite (manufactured by Johoku Chemical Industry Co., Ltd.); Antioxidant 4: Tetraphenyldipropylene glycol diphosphite (JPP-100 (product name) (manufactured by Johoku Chemical Industry Co., Ltd.)); Antioxidant 5: Diphenyl mono(tridecyl) phosphite (JPM-313 (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.));

[0106] Antioxidant 6: Hydrogenated bisphenol A / pentaerythritol phosphite polymer (JPH-3800 (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.)); Antioxidant 7: Tris(2,4-di-tert-butylphenyl) phosphite (Irgafos 168 (trade name) (manufactured by BASF Japan Ltd.)); Antioxidant 8: Distearyl pentaerythritol diphosphite (ADEKA Stab PEP-8 (trade name) (manufactured by ADEKA Corporation)); Antioxidant 9: Tris(tridecyl) phosphite (JP-333E (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.)); Antioxidant 10: Diisodecylphenyl phosphite (manufactured by Johoku Chemical Industry Co., Ltd.); Antioxidant 11: A mixture of 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane and 3,9-bis(isotridecyloxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane (JPP-88 (trade name) (manufactured by Johoku Chemical Industry Co., Ltd.));

[0107] Solvent 1: A mixed solvent of Isopar M and Isopar L in a 4:6 (mass ratio) ratio (Isopar M (trade name) and Isopar L (trade name) are both isoparaffinic solvents manufactured by ExxonMobil); Solvent 2: Isopar M (trade name) (manufactured by ExxonMobil, isoparaffinic solvent); Auxiliary solvent 1: Diisopropyl adipate; Auxiliary solvent 2: Isopropyl myristate; Liquid absorbent wick 1: Fuji-Chem HK-100 (manufactured by Fuji Chemical Co., Ltd., ceramic, φ7 mm, length 73 mm); Liquid absorbent wick 2: Rauschert Steatite 45% (manufactured by Rauschert, ceramic, φ7 mm, length 73 mm)

[0108] Examples 1-11, Comparative Examples 1 and 2 (Stability Test of Natural Pyrethrin with Antioxidants) Natural pyrethrin 1, antioxidant, and BHT were mixed on an aluminum dish (circular, 3.8 cm in diameter) to the composition shown in Table 1. After heating on a 180°C heater for 1 hour, the weight-average molecular weight Mw of the resulting natural pyrethrin polymer was analyzed by gel permeation chromatography (GPC). The above procedure was repeated three times, and the average values ​​of the analysis results are shown in Table 1. Note that the weight-average molecular weight Mw of the natural pyrethrin polymer is shown as a polystyrene equivalent. The polymer analysis conditions for the gel permeation chromatography (GPC) are shown below. [Polymer Analysis Conditions 1] Gel Permeation Chromatography (GPC) Pump: Shimadzu LC-20AD Detector: Shimadzu SPD-M20A Photodiode Array Detector Detection Wavelength: 254 nm Columns: Shimadzu Shim-pack GPC-803 (8.0 mm ID × 300 mm), Shimadzu Shim-pack GPC-804 (8.0 mm ID × 300 mm) (in series) Guard Column: Shimadzu GPC-800P (4.6 × 10 mm) Column Temperature: 40°C Eluent: Tetrahydrofuran Flow Rate: 1 mL / min

[0109]

[0110] When the weight-average molecular weight Mw of the generated natural pyrethrin polymer increases, it becomes less volatile, and its efficacy decreases. The phosphorus-based oxidizing agent according to the present invention shows superior efficacy in suppressing the polymerization of natural pyrethrin due to heating compared to the antioxidant BHT, and is suggested to show superior efficacy in maintaining the pest control effect of natural pyrethrin and improving its thermal stability.

[0111] Examples 12, 13, Comparative Examples 3 and 4 (Heat Stability Test of Natural Pyrethrin in Heat-Dispersing Insecticide Formulations) 34 g of a mixture obtained by mixing natural pyrethrin 2, an antioxidant, BHT, and a solvent to the composition shown in Table 2 was filled into 45 mL liquid mosquito repellent bottles. A stopper with an absorbent wick 1 inserted was attached, and the device was energized for 10 days (total 160 hours) by repeating the ON / OFF cycle twice a day for 8 hours each time. After this, the weight-average molecular weight Mw (polystyrene equivalent) of the natural pyrethrin polymer generated in the heated portion of the absorbent wick was analyzed by gel permeation chromatography (GPC). The above procedure was repeated twice, and the average values ​​of the analysis results are shown in Table 2. The polymer analysis conditions for the gel permeation chromatography (GPC) were the same as those for [Polymer Analysis Conditions 1] described above.

[0112] The BHT amounts in the table represent the total amount of BHT contained in natural pyrethrin 2 and the amount added from external sources.

[0113] When the weight-average molecular weight Mw of the generated natural pyrethrin polymer increases, it becomes less volatile, and its efficacy decreases. The phosphorus-based oxidizing agent according to the present invention showed superior efficacy in suppressing the generation of natural pyrethrin polymer in the heated portion of the liquid-absorbing wick compared to the antioxidant BHT. Therefore, it was suggested that in heat-evaporative insecticide formulations, the increase in molecular weight of natural pyrethrin due to heating is suppressed, and the insecticide effect of natural pyrethrin is maintained.

[0114] Examples 14-24 and Comparative Example 5 (Volatility of Natural Pyrethrin in Heat-Vaporized Insecticide Formulations) Each component was mixed to achieve the composition shown in Table 3. 34 g of the resulting mixture was filled into 45 mL liquid mosquito repellent bottles, and a stopper with an absorbent wick 1 or 2 (φ7 mm, length 73 mm) inserted was attached. The bottles were powered on for a total of 34 days, with "8 hours of power on - 4 hours of power off" considered equivalent to one day of use. On days 0, 6, 14, 20, 28, and 34 of the total usage period, the amount of natural pyrethrin volatilized in one hour during the 4-5 hour period after the start of power on each day was analyzed (μg / hr). The amount of natural pyrethrin volatilized (μg / hr) was determined by collecting the volatilized vapor at predetermined intervals using a urethane foam-packed column for a predetermined time, extracting it with acetone, and quantitatively analyzing the extract by high-performance liquid chromatography. The results are shown in Table 4.

[0115] The BHT amounts in the table represent the total amount of BHT contained in natural pyrethrin 2 and the amount added from external sources.

[0116] Compared to the antioxidants BHT and BHA, the phosphorus-based oxidizing agent according to the present invention did not show a decrease in the amount of natural pyrethrin volatilized during 34 days of use, regardless of the type of wick used. As a result, it was suggested that the phosphorus-based oxidizing agent according to the present invention is highly effective in maintaining the pest control effect of natural pyrethrin in heat-evaporation pest control formulations.

[0117] Examples 25-27, Comparative Examples 6 and 7 (Evaluation of pest control mats) The pest control mat formulations prepared by mixing each component to have the composition shown in Table 5 were spread at a rate of 0.75 mL per blank mat material (made of pulp and cotton linter, 0.21 cm thick, 3.5 cm long side, 2.2 cm short side, mass 695 mg) to obtain pest control mats that held 100 mg of natural pyrethrin as the active ingredient per mat. Two of the obtained pest control mats (Examples 25-27, Comparative Example 7: total amount of natural pyrethrin active ingredient 200 mg / treatment group, Comparative Example 6: total amount of natural pyrethrin active ingredient 400 mg / treatment group) were heated on a ceramic heater at 180°C, and the amount of natural pyrethrin volatilized in one hour during the first 3-4 hours after the start of heating and the amount of natural pyrethrin remaining after 4 hours of heating were analyzed. The amount of natural pyrethrin volatilized (mg / hr) was determined by collecting the volatilized vapor at predetermined intervals using a urethane foam-packed column for a predetermined time, extracting it with acetone, and quantitatively analyzing the extract by high-performance liquid chromatography. The amount of natural pyrethrin remaining (mg) was determined by extracting it with acetone from the heated mat, and quantitatively analyzing the extract by high-performance liquid chromatography. The results are shown in Table 6.

[0118] The BHT amounts in the table represent the total amount of BHT contained in natural pyrethrin 2 and the amount added from external sources.

[0119] In the table, N.D. indicates that data is unavailable. The pest control mats of Examples 25-27, by containing a specific amount of the phosphorus-based antioxidant according to the present invention, exhibit superior volatilization of natural pyrethrin during the 1-hour period between 3-4 hours after the start of heating compared to Comparative Examples 6 and 7. Furthermore, they also exhibit superior residual amount of natural pyrethrin after 4 hours of heating compared to Comparative Example 7. These results suggest that using the phosphorus-based antioxidant according to the present invention in formulations for pest control mats suppresses the polymerization of natural pyrethrin and exhibits excellent effects in maintaining pest control efficacy even in applications involving heating.

[0120] According to the present invention, it is possible to provide a novel composition containing natural pyrethrins that maintains pest control effectiveness or exhibits excellent thermal stability.

[0121] 1. Solution containing a composition for heating and vaporization 2. Heating element 3. Liquid absorption wick 4. Liquid solution bottle 10. Hot plate 11. Pest control mat 12. Power switch 13. Housing

Claims

1. A composition containing natural pyrethrins and one or more phosphorus-based antioxidants selected from group P: Group P: A group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, hydrogenated bisphenol A / pentaerythritol phosphite polymer, distearyl pentaerythritol diphosphite, tris(2,4-di-tert-butylphenyl) phosphite, and tris(tridecyl) phosphite.

2. The composition according to claim 1, wherein group P is the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, hydrogenated bisphenol A / pentaerythritol phosphite polymer, and distearyl pentaerythritol diphosphite.

3. The composition according to claim 1, wherein group P is the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane, 2,2'-methylenebis(4,6-di-tert-butylphenyl)2-ethylhexyl phosphite, and distearyl pentaerythritol diphosphite.

4. The composition according to claim 1, wherein group P is the group consisting of tetraphenyldipropylene glycol diphosphite, diisodecylphenyl phosphite, diphenyl mono(2-ethylhexyl) phosphite, di-n-decylphenyl phosphite, diphenyl mono(tridecyl) phosphite, and 3,9-bis(nonylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5.5]undecane.

5. The composition according to claim 1, wherein group P is the group consisting of tetraphenyldipropylene glycol diphosphite and diisodecylphenyl phosphite.

6. The composition according to any one of claims 1 to 5, wherein the mass ratio of natural pyrethrin to one or more phosphorus-based antioxidants selected from group P is in the range of 1:0.01 to 1:

50.

7. The composition according to any one of claims 1 to 5, further comprising a phenolic antioxidant.

8. The composition according to claim 7, wherein the phenolic antioxidant comprises at least one selected from the group consisting of dibutylhydroxytoluene and butylhydroxyanisole.

9. A heat-dispersed insecticide containing the composition described in any one of claims 1 to 5.

10. A pest control mat containing the composition described in any one of claims 1 to 5.

11. A method for controlling sanitary pests using the composition described in any one of claims 1 to 5.

12. A method for controlling sanitary pests using the heat-evaporative insecticide described in claim 9.

13. A method for controlling sanitary pests using the pest control mat described in claim 10.

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