Oxide complex for delivery of useful substances

Abstract

Provided are a system and a method for more efficiently applying a useful substance related to plant growth to a target plant.　The system and the method employ an oxide complex for delivering the useful substance into the plant, the oxide complex comprising an oxide aggregate and the useful substance.

Description

Oxide composites for delivering useful substances

[0001] The present invention relates to an oxide complex for delivering useful substances into a plant, a composition containing the oxide complex, and a method for delivering useful substances into a plant.

[0002] Pesticides have been used in the cultivation of useful plants such as grains, vegetables, fruits, and flowers. To ensure sufficient effectiveness on the target plants, many farms have resorted to large-scale pesticide application. However, this large-scale application is inefficient, as most of the active ingredients are either decomposed or leached into the soil, failing to exert their effects on the target plants. Furthermore, such large-scale application raises environmental concerns, such as residue in the soil. Therefore, there has been a need for technologies that allow for the efficient application of pesticide components to plants at lower doses.

[0003] As a technology for efficiently delivering the active ingredients of pesticides to plants, the use of pesticides with delivery systems using artificial nanoparticles has been proposed. Non-patent document 1 describes the application of gold nanoparticles coated with polyvinylpyrrolidone or citric acid as a foliar spray to wheat, and it has been confirmed that the gold nanoparticles and each substance were subsequently taken up by the plant. Non-patent document 2 reports that when chili pepper plants were grown in a culture medium containing plant hormones and a chitosan / zinc oxide nanoparticle complex, they showed significantly higher values ​​in stem length, leaf area, and fresh weight of leaves and roots compared to a control without nanoparticles.

[0004] Patent Document 1 reports that spraying a nano-biological insecticide, in which chitinase enzyme is immobilized on zinc oxide nanoparticles, onto corn effectively controlled the pest S. Zeamais. Patent Document 2 describes a nano-fertilizer having at least one plant nutrient coated on metal nanoparticles. It has been reported that administering metal nanoparticles coated with boron or a derivative thereof to plants could treat boron deficiency in plants.

[0005] International Publication No. 2023 / 018403, U.S. Patent Application Publication No. 2013-0219979

[0006] A. Avellan, et al., ACS Nano. Vol. 13, No. 5, pp. 5291-5305 (2019)G. Asgari-Targhi, et al., Int. J. Biol. Macromol., Vol.189, pp. 170-182 (2021)

[0007] The present invention aims to provide a system and method for more efficiently applying useful substances involved in plant growth to target plants.

[0008] As a result of diligent research, the inventors discovered that applying useful substances to plants as a composite with oxide aggregates enhances their effectiveness, leading to the completion of the present invention.

[0009] This specification provides the following inventions derived from the above findings: [1] An oxide complex for delivering a useful substance into a plant body, comprising an oxide aggregate and a useful substance. [2] The oxide complex according to [1], wherein the oxide complex is formed by bonding the oxide aggregate and the useful substance. [3] The oxide complex according to [2], wherein the bond is a covalent bond, a coordination bond, an ionic bond, or a hydrogen bond. [4] The oxide complex according to [2], wherein the bond is a covalent bond mediated by a hydroxyl group contained in the oxide aggregate and a hydroxyl group contained in the useful substance. [5] The oxide complex according to any one of [1] to [4], wherein the number-average particle diameter is 100 nm or more and 2000 nm or less. [6] The oxide complex according to any one of [1] to [5], wherein the oxide is a metal oxide and / or a nonmetal oxide. [7] The oxide complex according to [6], wherein the metal oxide comprises at least one selected from the group consisting of zinc (Zn) oxide, iron (Fe) oxide, potassium (K) oxide, calcium (Ca) oxide, magnesium (Mg) oxide, silver (Ag) oxide, manganese (Mn) oxide, molybdenum (Mo) oxide, copper (Cu) oxide, cobalt (Co) oxide, nickel (Ni) oxide, and aluminum (Al) oxide. [8] The oxide complex according to [6], wherein the nonmetallic oxide comprises at least one selected from the group consisting of silicon (Si) oxide, boron (B) oxide, and phosphorus (P) oxide. [9] The oxide complex according to any one of [1] to [8], wherein the useful substance is selected from a) herbicides; b) fertilizer components; c) amino acids, peptides, or proteins; d) sugars; e) biostimulants; f) plant growth regulators; g) fungicides; and h) insecticides.

[10] The herbicides include phenoxy acid herbicides, carbamate herbicides, acid amide herbicides, urea herbicides, sulfonium urea herbicides, pyrimidyloxybenzoic acid herbicides, triazine herbicides, dianodine herbicides, diazole herbicides, bipyridium herbicides, dinitroaniline herbicides, aromatic carboxylic acid herbicides, fatty acid herbicides, organophosphorus herbicides, amino acid herbicides, ioxynyl agents, biphenox agents, DBN agents, DCBN agents, cethoxidim agents, cretoxidim agents, teproxidim agents, ACN agents, and The oxide complex according to [9], comprising at least one selected from the group consisting of lorphthalim, flumioxazine, scinmethiline, carphetrazone ethyl, endotal disodium salt, benfresate, pentoxazone, pyraflufen ethyl, carbam, oxadiclomefone, indanophan, phentrazamide, benzobicyclon, butaphenacil, azaphenidine, pyrifthalide, fluthiaset-methyl, oxaziargyl, oxadiazone, and decyl alcohol.

[11] The oxide complex according to [9], wherein the fertilizer component comprises at least one selected from the group consisting of compounds comprising at least one of carbon (C), hydrogen (H), oxygen (O), nitrogen (N), phosphorus (P), potassium (K), calcium (Ca), magnesium (Mg), sulfur (S), boron (B), chlorine (Cl), zinc (Zn), copper (Cu), iron (Fe), manganese (Mn), molybdenum (Mo), nickel (Ni), sodium (Na), silicon (Si), selenium (Se), cobalt (Co), aluminum (Al), chromium (Cr), and cadmium (Cd).

[12] The oxide complex according to [9], wherein the amino acid, peptide, or protein is an amino acid, peptide, or protein that has a physiological function in the plant body.

[13] The oxide complex according to [9], wherein the sugar comprises at least one selected from the group consisting of monosaccharides, disaccharides, oligosaccharides, and polysaccharides.

[14] The oxide complex according to [9], wherein the biostimulant comprises at least one selected from the group consisting of peptides, amino acids, monosaccharides, disaccharides, oligosaccharides, polysaccharides, seaweed extracts, humic substances, organic acids, nucleic acids, plant extracts, food residues, and microbial metabolites.

[15] The oxide complex according to [9], wherein the plant growth regulator comprises at least one selected from the group consisting of ethylene agents, auxin agents, auxin antagonists, cytokinin agents, cytokinin antagonists, gibberellin agents, dwarfing agents, isoprothiolanes, oxin sulfate agents, cyanamide agents, choline agents, decyl alcohol agents, piperonyl butoxide agents, bendimetaline agents, MCPA agents, MCPB agents, NAC agents, quinoxaline-based / DEP agents, pyraflufen ethyl agents, prohydrojasmon agents, abscisic acid agents, brassinosteroid agents, jasmonic acid agents, florigen agents, chlorella extract agents, and shiitake mushroom mycelium extract agents.

[16] The bactericides include copper bactericides, organosulfur bactericides, organophosphorus bactericides, organochlorine agents, melanin biosynthesis inhibitors, benzimidazole bactericides, dicarboxyimide bactericides, acid amide bactericides, sterol biosynthesis inhibitors, methoxyacrylate bactericides, anilinopyrimidine bactericides, synthetic antibacterial agents, soil bactericides, antibiotic bactericides, natural bactericides, probenazole agents, isoprothiolane agents, ferrimzone agents, diclomazine agents, pencyclon agents, fluorimide agents, captan agents, and sulfenic acid agents. The oxide complex according to [9], comprising at least one selected from the group consisting of a dithianone agent, a quinoxaline agent, a diflumetrim agent, a fludioxonil agent, a bentazole agent, acibenzoral S-methyl agent, a triazine agent, a fluazinam agent, a diethofencarb agent, a cymoxanil agent, an iminoctadine acetate agent, an iminoclazine albesilate agent, a propamoclav hydrochloride agent, a dimethomorph agent, a diclocimet agent, a famoxadone agent, a cyazofamide agent, a cyflufenamide agent, and a thiadinil agent.

[17] The oxide complex according to [9], wherein the insecticide comprises at least one selected from the group consisting of organophosphate insecticides, carbamate insecticides, pyrethroid insecticides, nereistoxin insecticides, neonicotinoid insecticides, insect growth regulators, natural insecticides, acaricides, nematicides, pine wood nematode control agents, slug control agents, benzoepins, fibronils, chlorfenavirs, diafenthiurons, pyrometrozines, emamectin benzoic acid, sodium oleate, DBEDCs, indoxacarbs, and tolfenpyrads.

[18] An oxide complex according to any one of [1] to

[17] , wherein the plant is selected from the group consisting of monocots and dicots. [18-1] An oxide complex according to any one of [1] to

[17] , wherein the oxide aggregate is formed by the aggregation of oxide particles. [18-2] An oxide complex according to [18-1], wherein the oxide particles are nanoparticles. [18-3] An oxide complex according to [18-1] or [18-2], wherein the oxide particles have the property of being localized within the plant body.

[19] A composition for delivering a useful substance into a plant body, comprising the oxide complex according to any one of [1] to

[18] .

[20] A method for delivering a useful substance into a plant body, comprising applying the oxide complex according to any one of [1] to

[18] to a plant or soil, culture medium, or water surrounding the plant.

[21] A method for delivering a useful substance into a plant body, comprising the steps of: preparing an oxide complex by combining an oxide aggregate and a useful substance; and applying the oxide complex to a plant or soil, culture medium, or water surrounding the plant. This specification includes the disclosures of Japanese Patent Application No. 2025-013317, which forms the basis of the priority claim of this application.

[0010] According to the present invention, a system and method can be provided for more efficiently applying useful substances involved in plant growth to target plants.

[0011] This graph shows comparative data of zinc content in treated wheat plants (A), above-ground parts (B), and underground parts (C) of wheat treated with a ZnO suspension, compared to a control. Error bars in the graph indicate the standard deviation. "***" in the graph indicates a statistically significant difference at the 0.1% level compared to the control, as determined by Student's t-test. Fe ２ O ３This graph shows comparative data of iron content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of wheat plants treated with a suspension compared to a control. Error bars in the graph indicate the standard deviation. "*", "**", and "***" in the graph indicate statistically significant differences compared to the control at the 5%, 1%, and 0.1% levels, respectively, according to Student's t-test. This graph shows comparative data of magnesium content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of wheat plants treated with an MgO suspension compared to a control. Error bars in the graph indicate the standard deviation. "*" in the graph indicates statistically significant differences compared to the control at the 5% level, according to Student's t-test. This graph shows comparative data of zinc content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of soybean plants treated with a ZnO suspension compared to a control. Error bars in the graph indicate the standard deviation. The asterisk (*) in the figure indicates a statistically significant difference at the 5% level compared to the control, as determined by Student's t-test. Fe ２ O ３ This graph shows comparative data of iron content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of soybean plants treated with suspension and control. Error bars in the graph indicate the standard deviation. "***" in the graph indicates a statistically significant difference at the 0.1% level compared to the control, according to Student's t-test. This graph shows comparative data of magnesium content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of soybean plants treated with MgO suspension and control. Error bars in the graph indicate the standard deviation. "*" in the graph indicates a statistically significant difference at the 5% level compared to the control, according to Student's t-test. This graph shows comparative data of zinc content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of lettuce plants treated with ZnO suspension and control. Error bars in the graph indicate the standard deviation. "*" in the graph indicates a statistically significant difference at the 5% level compared to the control, according to Student's t-test. Fe ２ O ３This graph shows comparative data of iron content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of lettuce plants treated with a suspension compared to a control. Error bars in the graph indicate the standard deviation. "***" in the graph indicates a statistically significant difference at the 0.1% level compared to the control, as determined by Student's t-test. This graph shows comparative data of magnesium content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of lettuce plants treated with an MgO suspension compared to a control. Error bars in the graph indicate the standard deviation. "**" in the graph indicates a statistically significant difference at the 1% level compared to the control, as determined by Student's t-test. This graph shows the SPAD values ​​or mortality rates of various plants after application of ZnO-Glyp. Figure 10A shows the SPAD value of *Epipogium aquilinum* 13 days after application. Figure 10B shows the mortality rate of rice 20 days after application, and Figure 10C shows the mortality rate of wheat 8 days after application. Figure 10D shows the SPAD value of celosia 12 days after application. The numbers at the bottom of the graphs show the measured number-average particle size of various ZnO-Glyp. Error bars show the standard deviation. In the figures, "*" and "***" indicate a statistically significant difference from the control at the 5% and 0.1% levels, respectively, according to Dunnet's test. Different letters in the figures indicate a statistically significant difference at the 5% level according to Tukey's test. The tests were conducted with n=5 to 9 for *Epipogium aquilinum*, 3 replicates of 10 individuals each for rice and wheat, and n=3 for celosia. This is a continuation of Figure 10-1. This is a box plot showing the adhesion rate of ZnO-Glyp with number-average particle sizes of 60 nm and 1100 nm applied to leaves. In the figure, "***" indicates a statistically significant difference at the 0.1% level between the group with a number-average particle diameter of 60 nm and the group with a number-average particle diameter of 1100 nm, as determined by Student's t-test. Each test was conducted with n=8. Glyp and ZnO-Glyp １３ This graph shows the results of the 13C isotope incorporation tests. Error bars indicate the standard deviation. Different letters in the graph indicate a statistically significant difference at the 5% level according to the Tukey test. Each test was performed with n=3. SiO ２- A graph showing the SPAD values of Minato kamogusa after Glyp application. Error bars indicate the standard deviation. Different letters in the figure indicate significant differences at the 5% level by the Tukey test. The tests were each conducted with n = 5 - 10. SiO ２ - A micrograph showing the results of FE - SEM / EDS of - Glyp. Figure 14A shows the localization of P, and Figure 14B shows the localization of Si. SiO ２ - A micrograph showing the results of FE - SEM / EDS of - Glyp and the spectra of pixels of each element. Figure 15A is the micrograph, Figure 15B is the photo showing the localization of Si, Figure 15C is the photo showing the localization of P, and Figure 15D shows the spectrum obtained by integrating pixels on the image of each element. Fe ２ O ３ - Glyp, Fe ３ O ４ - A graph showing the SPAD values of Minato kamogusa after Glyp application. Error bars indicate the standard deviation. Different letters in the figure indicate significant differences at the 5% level by the Tukey test. The tests were each conducted with n = 5 - 9. A graph showing the SPAD values of Minato kamogusa after MgO - Glyp application. Error bars indicate the standard deviation. Different letters in the figure indicate significant differences at the 5% level by the Tukey test. The tests were each conducted with n = 5 - 10. Ag ２ - A graph showing the SPAD values of Minato kamogusa after AgO - Glyp application. Error bars indicate the standard deviation. Different letters in the figure indicate significant differences at the 5% level by the Tukey test. The tests were each conducted with n = 7 - 10. ZnO - Ca(H ２ PO ４ ) ２ - A box - and - whisker plot showing the fresh weight of the underground part of Komatsuna 21 days after the start of cultivation after ZnO - Ca(H ２ PO ４ ) ２This is a photograph of the appearance of komatsuna (Japanese mustard spinach) plants 21 days after application. The graph shows the stomatal conductance of cabbage after ZnO-CLE25 application. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Each experiment was conducted with n=4 to 6. SiO ２ - Graphs showing stomatal conductance of cabbage and soybeans after ABA application. Error bars indicate standard deviation. Figure 22A shows stomatal conductance of cabbage, and Figure 22B shows stomatal conductance of soybeans. Error bars indicate standard deviation. Different letters in the figures indicate a statistically significant difference at the 5% level according to Tukey's test. The experiment was conducted with n=3-4 for cabbage and n=4-5 for soybeans. Fe ２ O ３ -GA ３This is a box plot showing the height elongation of rice plants over 20 days after application. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Each experiment was conducted with n=13 to 17. This is a graph showing the SPAD values ​​of *Epipogium aureum* after application of a complex of various zinc compounds and Glyp. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Each experiment was conducted with n=8 to 10. This is a graph showing the SPAD values ​​of *Epipogium aureum* after application of a complex of various magnesium compounds and Glyp. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Each experiment was conducted with n=8 to 10. This is a box plot showing the height elongation of rice plants after application of a complex of magnesium oxide and ammonium sulfate. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. This is a box plot showing the boron content of soybeans after application of a complex of zinc oxide and boric acid. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. This is a box plot showing the molybdenum content of wheat after application of a complex of zinc oxide and disodium molybdate dihydrate. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. This is a box plot showing the SPAD value of wheat after application of a complex of zinc oxide and glucose. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. This is a box plot showing the fresh above-ground weight of wheat 13 days after application of a complex of zinc oxide and trehalose. In the figure, "*" indicates a statistically significant difference at the 5% level between the treatment intervals according to the t-test. This is a box plot showing the fresh above-ground weight of wheat 13 days after application of a complex of zinc oxide and D(+)-raffinose pentahydrate. Different letters in the figure indicate a statistically significant difference at the 5% level by Tukey's test. This is a box plot showing the fresh above-ground weight of barley 15 days after application of a complex of zinc oxide and alginate. In the figure, "*" and "**" indicate a statistically significant difference between the treatment groups at the 5% and 1% levels, respectively, by t-tests. This is a box plot showing the dry above-ground weight of wheat 14 days after application of a complex of zinc oxide and glycine betaine.Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. This is a box plot showing the dry weight of the underground part of wheat 14 days after application of a complex of zinc oxide and glutamic acid. In the figure, "*" indicates a statistically significant difference at the 5% level between the treatment groups according to the t-test. This is a box plot showing the dry weight of the underground part of wheat 13 days after application of a complex of zinc oxide and glutamine. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. This is a box plot showing the dry weight of the underground part of wheat 14 days after application of a complex of zinc oxide and arginine. In the figure, "*" indicates a statistically significant difference at the 5% level between the treatment groups according to the t-test. This is a box plot showing the mineral content of the above-ground part of wheat 12 days after application of a complex of zinc oxide and fulvic acid. Figure 37A shows the magnesium content, and Figure 37B shows the zinc content. In the figure, "**" and "***" indicate that there is a significant difference between the treatment intervals at the 1% and 0.1% levels, respectively, according to the t-test. Different letters in the figure indicate a significant difference at the 5% level, according to the Tukey test. This is a box plot showing the above-ground dry weight of soybeans 16 days after application of a complex of zinc oxide and fulvic acid. In the figure, "*" and "**" indicate that there is a significant difference between the treatment intervals at the 5% and 1% levels, respectively, according to the t-test. This is a graph showing the SPAD values ​​of *Echinops japonica* after application of a complex of zinc oxide and paraquat. Error bars indicate the standard deviation. Different letters in the figure indicate a significant difference at the 5% level, according to the Tukey test. This is a box plot showing the mortality rate of clover after application of a complex of zinc oxide and 2,4-dichlorophenoxyacetic acid. In the figure, "***" indicates that there is a significant difference compared to the control at the 0.1% level, according to the t-test. This is a box plot showing the mortality rate of clover after application of a zinc oxide and dicamba complex. In the figure, "***" indicates a statistically significant difference at the 0.1% level compared to the control, as determined by a t-test. This is a box plot showing the mortality rate of clover after application of a zinc oxide and DCMU wettable powder complex. In the figure, "***" indicates a statistically significant difference at the 0.1% level compared to the control, as determined by a t-test. This is a box plot showing the mortality rate of goosegrass after application of a zinc oxide and tepraloxidim complex. In the figure, "*" indicates a statistically significant difference at the 5% level compared to the control, as determined by a t-test.This is a box plot showing the mortality rate of goosegrass after application of a zinc oxide and alachlor complex. In the figure, "**" indicates a statistically significant difference at the 1% level compared to the control, as determined by a t-test. This is a box plot showing the mortality rate of goosegrass after application of a zinc oxide and oxadiclomefone complex. In the figure, "*" indicates a statistically significant difference at the 5% level compared to the control, as determined by a t-test. This is a box plot showing the mortality rate of clover after application of a zinc oxide and penoxulam complex. In the figure, "***" indicates a statistically significant difference at the 0.1% level compared to the control, as determined by a t-test. This is a box plot showing the mortality rate of clover after application of a zinc oxide and IPC complex. In the figure, "*" indicates a statistically significant difference at the 5% level compared to the control, as determined by a t-test. This is a box plot showing the mortality rate of clover after application of a zinc oxide and bendasone complex. In the figure, "*" indicates a statistically significant difference at the 5% level compared to the control, as determined by a t-test. This is a box plot showing the mortality rate of clover after application of a complex of zinc oxide and endotar. In the figure, "*" indicates a statistically significant difference at the 5% level compared to the control, as determined by a t-test. This is a box plot showing the mortality rate of clover after application of a complex of zinc oxide and mesotrione. In the figure, "*" indicates a statistically significant difference at the 5% level compared to the control, as determined by a t-test. This is a box plot showing the dry weight of soybean leaves after application of a complex of zinc oxide and acephate. Different letters in the figure indicate a statistically significant difference at the 5% level, as determined by Tukey's test. This is a box plot showing the dry weight of soybean leaves after application of a complex of zinc oxide and methomyl. Different letters in the figure indicate a statistically significant difference at the 5% level, as determined by Tukey's test. This is a box plot showing the dry weight of the above-ground parts of soybeans after application of a complex of zinc oxide and clothianidin. In the figure, "**" and "***" indicate statistically significant differences between the treatment intervals at the 1% and 0.1% levels, respectively, as determined by t-tests. This graph shows the disease lesion scores of wheat after application of a zinc oxide and kresoxime-methyl complex. Error bars indicate the standard deviation. Different letters in the graph indicate a statistically significant difference at the 5% level according to Tukey's test. This graph shows the disease lesion scores of wheat after application of a zinc oxide and pidflumetofen complex. Error bars indicate the standard deviation.Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. The graph shows the disease lesion scores of wheat after application of a zinc oxide and thiophanate-methyl complex. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test.

[0012] 1. Definitions and Composition In this specification, unless otherwise specified, "%" indicating concentration and content shall mean "weight %", i.e., weight / percentage of weight.

[0013] <Plants> In this specification, "plants" are not particularly limited and include all organisms classified as plants. In this specification, plants may be useful plants such as grains, vegetables, fruits, and flowers, or they may be harmful plants whose growth is to be suppressed, so-called weeds. In this specification, plants are preferably angiosperms and gymnosperms, and more preferably angiosperms. Angiosperms are classified into monocots and dicots, and both can be suitably used.

[0014] In this specification, monocotyledonous plants are not particularly limited to plants belonging to the class Monocotyledonous plants (Lilium class), and any of them can be used. Examples include plants belonging to the Amaryllidaceae, Araceae, Liliaceae, Asparagaceae, Hemerocaceae, Bromeliaceae, Iridaceae, Orchidaceae, and Grasses. Examples of plants in the Amaryllidaceae family are not limited, but include wild onion, wild garlic, chives, Crinum lily, red spider lily, daffodil, amaryllis, and rain lily. Examples of plants in the Araceae family are not limited, but include skunk cabbage, duckweed, konjac, taro, taro, taro, taro, water chestnut, lotus root, and dwarf vine. Examples of plants in the Liliaceae family are not limited, but include lilies, tulips, and dogtooth violets. Asparagaceae plants are not limited to this family, but examples include asparagus. Hemerocaceae plants are not limited to this family, but examples include aloe. Bromeliaceae plants are not limited to this family, but examples include pineapple. Iridaceae plants are not limited to this family, but examples include crocus, saffron, freesia, gladiolus, iris, Japanese iris, Japanese iris, and iris. Orchidaceae plants are not limited to this family, but examples include Cypripedium macranthos, Bletilla striata, Calanthe, Cymbidium goeringii, Cephalanthera falcata, and Cymbidium orchid. Grasses are not limited to this family, but examples include rice, wheat, barley, oats, rye, millet, foxtail millet, barnyard millet, corn, bamboo, sugarcane, adlay, Japanese pampas grass, and turfgrass.

[0015] In this specification, dicotyledonous plants are not particularly limited to plants belonging to the class Dicotyledons, and any of them can be used. Examples include plants belonging to the Asteraceae, Brassicaceae, Cucurbitaceae, Fabaceae, Gentianaceae, Rosaceae, Rutaceae, Solanaceae, etc. Examples of plants in the Asteraceae family are not limited to burdock, mugwort, aster, daisy, calendula, safflower, garland chrysanthemum, marguerite, chrysanthemum, chicory, artichoke, sunflower, lettuce, chamomile, butterbur, stevia, etc. Examples of plants in the Brassicaceae family are not limited to horseradish, mustard greens, cabbage, broccoli, bok choy, mizuna, turnip, radish, wasabi, etc. Examples of plants in the Cucurbitaceae family are not limited to cucumber, watermelon, pumpkin, zucchini, gourd, loofah, winter melon, bottle gourd, melon, etc. Examples of leguminous plants include peanuts, chickpeas, rooibos, quince, peas, sweet peas, broad beans, sword beans, soybeans, kidney beans, kudzu, and adzuki beans. Examples of gentianaceae plants include gentians and swertia. Examples of roseaceae plants include roses, Japanese roses, almonds, apricots, plums, cherries, Japanese apricots, peaches, Japanese kerria, loquats, apples, and hawthorn. Examples of citrus plants include Satsuma mandarins, yuzu, and lemons. Examples of nightshade plants include tomatoes, eggplants, potatoes, peppers, tobacco, Chinese lanterns, petunias, and goji berries.

[0016] <Oxide Aggregates> In this specification, "oxide aggregates" refer to aggregates of oxide particles, preferably oxide nanoparticles. In this specification, "nanoparticles" refer to particles having a number-average particle diameter of 1 to 100 nm. In this specification, "number-average particle diameter" refers to the average particle diameter when the number of particles is measured as the number of particles, such as when there are n particles of particle diameter D, and refers to the number-average particle diameter measured using a dynamic light scattering (DLS) analyzer. Unless otherwise specified, "particle diameter" in this specification refers to "number-average particle diameter".

[0017] The material constituting the oxide particles is not particularly limited, but it is preferable to use a material that facilitates particle formation with a uniform particle size. The material constituting the oxide particles may be a single material or a mixture of multiple materials. The material constituting the oxide particles, i.e., the oxide, is preferably an oxide containing essential elements of the target plant in order to promote introduction into the plant body. The oxide may be a metal oxide, a nonmetal oxide, or a mixture thereof. The metal oxide is not particularly limited and includes oxides of all metals, but may include at least one selected from the group consisting of zinc (Zn) oxide, iron (Fe) oxide, potassium (K) oxide, calcium (Ca) oxide, magnesium (Mg) oxide, silver (Ag) oxide, manganese (Mn) oxide, molybdenum (Mo) oxide, copper (Cu) oxide, cobalt (Co) oxide, nickel (Ni) oxide, and aluminum (Al) oxide. The nonmetal oxide may include at least one selected from the group consisting of silicon (Si) oxide, boron (B) oxide, and phosphorus (P) oxide. Suitable oxides include zinc oxide (ZnO) and iron oxide (Fe ２ O ３ ), magnesium oxide (MgO), silicon dioxide (SiO ２ ) can be used.

[0018] Known methods for producing oxide particles include solid-phase methods, which involve mechanically or chemically crushing a solid phase (lump) to form particles; liquid-phase methods, which involve obtaining a substance dissolved in a solution as particulate solids; and gas-phase methods, which involve heating a substance in a vacuum, evaporating it, and then cooling it. In this specification, oxide particles may be particles produced by any of these methods.

[0019] Oxide aggregates are formed by agglomerating the oxide particles. Oxide aggregates may be prepared simultaneously with the preparation of oxide particles, or they may be prepared by agglomerating only the oxide particles. Alternatively, oxide particles may be agglomerated simultaneously when forming a composite by mixing oxide particles with the useful substances described later. For example, oxide aggregates can be obtained by agglomerating oxide particles by suspending them in an aqueous solution of a predetermined pH. The particle size of the aggregates can be adjusted by adjusting the pH of the aqueous solution. The pH of the aqueous solution can be appropriately set according to the oxide particles to be agglomerated. In addition to, or instead of, adjusting the pH, oxide aggregates can also be obtained by physical means such as centrifugation.

[0020] In this specification, the elements constituting the oxide particles may have the property of being localized within the plant body. More specifically, it is preferable that the elements exhibit a higher abundance in a particular part or organ than in other parts or organs. The parts or organs to which the elements are localized will vary depending on the type of plant being introduced. The elements constituting the oxide particles may be localized in any part of the plant body, but may be localized in at least one selected from the roots, leaves, stems, seeds, flowers, tubers, and rhizomes of the plant.

[0021] The localization of the aforementioned elements within a plant may be confirmed or predicted for the target plant based on known knowledge, for example. For instance, it has been reported that when ZnO was sprayed on the leaves of wheat, the zinc content in the wheat grain increased (T. Zhang, et al., J. Agric. Food Chem. Vol. 66, No. 1, pp. 2572-2579 (2018)). According to this report, when monocotyledonous plants such as wheat or grasses are introduced, ZnO can be said to be localized to the fruiting body. On the other hand, it has been reported that in cabbage, the zinc content in the underground part (roots) increased with increasing amounts of Zn applied to the soil (P. Pongrac, et al., Plant and Soil, Vol. 434, pp. 141-165 (2019)). According to this report, in dicotyledonous plants such as cabbage, zinc is localized in the roots, so if dicotyledonous plants such as cabbage are introduced, it can be inferred that ZnO will also be localized in the roots. In cabbage cultivation, it has been reported that the silicon content of sprouts increased as a result of applying silicon to calcium-deficient or sufficiently calcium-rich soil (DL Silva, et al., Scientific Reports, Vol. 11, No. 1770 (2021)). According to this report, in dicotyledonous plants such as cabbage, silicon is localized in the sprouts, so if dicotyledonous plants such as cabbage are introduced, SiO ２ It can be inferred that it has localization to buds. Thus, the localization of oxide particles can be confirmed or predicted based on known knowledge, etc., based on the target plant and the elements that make up the oxide particles used.

[0022] In the examples described below, it was confirmed that ZnO particles were localized in the above-ground parts other than the treated leaves and in the roots of monocotyledonous plants (wheat), and in the leaves of dicotyledonous plants (soybeans, lettuce). ２ O ３It was confirmed that the particles localized in the leaves of monocots (wheat) and in the leaves of dicots (soybeans, lettuce). It was confirmed that the MgO particles localized in the above-ground parts other than the treated leaves of monocots (wheat) and dicots (soybeans), and in the leaves of dicots (lettuce).

[0023] <Useful Substances> In this specification, "useful substance" refers to a substance other than water that can have a desired effect on plant growth, either directly or indirectly. Examples of useful substances that can be used include a) herbicides; b) fertilizer components; c) amino acids, peptides, or proteins; d) sugars; e) biostimulants; f) plant growth regulators; g) fungicides; and h) insecticides, etc.

[0024] <Oxide Composites> In this specification, "oxide composite" refers to a composite containing a useful substance and an oxide aggregate. Here, "containing" a useful substance and an oxide aggregate includes not only oxide composites in which the useful substance and the oxide aggregate are bonded, but also oxide composites in which the useful substance and the oxide aggregate are simply in physical proximity. An example of an oxide composite in which the useful substance and the oxide aggregate are simply in physical proximity is the zinc oxide-paraquat composite. In Example 28, analysis of the zinc oxide-paraquat composite by FT-IR showed that chemical bonding between ZnO and paraquat could not be confirmed, but the zinc oxide-paraquat composite demonstrated the effects of the present invention. In this specification, it is preferable that "oxide composite" is a composite in which a useful substance and an oxide aggregate are bonded. The means for bonding the useful substance and the oxide aggregate are not particularly limited as long as the useful substance can be fixed to the surface of the oxide aggregate, and can be appropriately selected depending on the type of useful substance and the type of oxide. For example, if the useful substance is a polysaccharide (e.g., chitosan) and the oxide is a metal oxide (e.g., ZnO), a method can be employed in which the useful substance and the oxide aggregate are brought together under alkaline conditions and heated. For example, a crosslinking agent (e.g., a carbodiimide crosslinking agent, a silane coupling agent, etc.) can be used to bond the useful substance and the oxide aggregate.

[0025] In oxide composites, the "bonding" preferably refers to a chemical bond between the useful substance and the oxide aggregate. Here, "chemical bonding" can be either covalent or non-covalent. More specifically, "chemical bonding" can be any intermolecular bond, such as covalent bonding, coordination bonding, ionic bonding, or hydrogen bonding. "Coordination bonding" may refer to a coordination bond formed between a metal atom present on the surface of the oxide aggregate or oxide particles and a functional group of the useful substance. In an aggregate of oxide composites, the chemical bonds between the useful substance and the oxide aggregate may all be of the same type, or multiple types of chemical bonds may be present. Chemical bonding is not particularly limited, but it can be a bond between the hydroxyl groups (-OH) of the oxide aggregate or oxide particles and the functional groups of the useful substance. In particular, it can be a bond between the hydroxyl groups (-OH) of the oxide aggregate or oxide particles and the functional groups containing hydroxyl groups of the useful substance. In this case, the bond may be covalent (dehydration condensation) or non-covalent (hydrogen bonding), but it is preferable to use covalent bonding for a stronger bond. The functional group containing a hydroxyl group in a useful substance is not particularly limited, but it can also include a sulfonic acid group (-SO ３ H), enol group (CH ２ =C(OH)-), carboxyl group (-COOH), phosphate group (H ２ PO ４ － Examples include the following. When a crosslinking agent is used, the useful substance and the oxide aggregate can be bonded together by covalent bonds (e.g., amide bonds).

[0026] Whether or not the useful substance and the oxide aggregate are chemically bonded is not particularly limited, but can be confirmed by the following methods, for example: 1) Obtain the infrared absorption spectrum of the washed oxide composite particles and check for the presence or absence of characteristic absorption peaks of both the useful substance and the oxide; 2) Coat the oxide composite particles with a carbon sample stage or the like, and perform elemental analysis using a field emission scanning electron microscope (FE-SEM) and an energy dispersive X-ray spectrometer (EDS) to confirm whether the localization agreement rate (probability of existing in the same position) of elements derived from the useful substance and elements derived from the oxide is, for example, 50% or more, more preferably 60% or more or 70% or more.

[0027] 2. Oxide Composite for Delivering Useful Substances into Plants The first embodiment of the present invention is an oxide composite for delivering useful substances into plants. The oxide composite of this embodiment is characterized by comprising an oxide aggregate and a useful substance, and / or by the oxide aggregate and the useful substance being bonded together. By using the oxide composite of this embodiment, the adhesion of the oxide composite to plants can be improved, thereby enabling plants to take in more of the useful substance alone, the oxide composite, and / or the composite of oxide particles (preferably oxide nanoparticles) separated from the aggregate and the useful substance into the plant. According to the oxide composite of this embodiment, the amount of useful substance used in plants can be reduced from known amounts.

[0028] The number-average particle size of the oxide composite in this embodiment is preferably 100 nm to 2000 nm, and more preferably 300 nm to 1500 nm. By setting the particle size of the oxide composite within the above range, the adhesion of the oxide composite to the plant body can be enhanced, and the oxide composite is retained in the plant body with high adhesion, allowing more of the useful substance to be taken up into the plant body. Here, only the useful substance may be taken up into the plant body, but it may also be a composite of an oxide aggregate, or oxide particles (preferably oxide nanoparticles) separated from the oxide aggregate, and the useful substance. In particular, when a composite of the useful substance and oxide particles is taken up, it becomes possible to deliver the useful substance to a desired location in the plant body by utilizing the localization of the oxide particles, thereby further reducing the amount of useful substance used.

[0029] 2-1. Herbicide-Oxide Complex The first embodiment of the oxide complex of this embodiment is one in which a herbicide is used as the useful substance. The plants to which the oxide complex of this embodiment is applied are preferably not useful plants, but harmful plants whose growth is to be suppressed, so-called weeds. Examples of such plants include monocots belonging to the genera Apocynum, Atractylodes, Picea, Oats, Brachiaria, Brachyaria, Goosegrass, Echinocloa, Goosegrass, Platypus, Laurium, Panicum, Phragmites, Strawberry, Leucobryum, and Setaria, as well as dicots belonging to the genera Digitalia, Anthemis, Amaranthus, Ragweed, Capsella, Cornflower, Cenopodium, Conisza, Desclionia, Galium, Kochia, Chrysanthemum, Poppy, Ragweed, White Mustard, Arabis, Chickweed, and Shepherd's Purse.

[0030] In this embodiment, the herbicide is not particularly limited, but examples include phenoxy acid herbicides (2,4-PA, MCPA, MCPB, MCPP, triclopyr, clomeprop, naproanilide, cyhalofop-butyl, fluazifop, quizalofop-ethyl, fluazifop-P), carbamate herbicides (IPC, fenmedifam, desmedifam, benthiocarb, orisobencarb, esprocarb, molinate, dimepiperate, pyributicarb), and acid amide herbicides (DCPA, alachlor). , butachlor, pretilachlor, metrachlor, dimethylnamide, tenylchlor, bromobutide, etobenzanide, diflufenican, mefenacet, napropamide, cafenstrol, propizamide, isoxaben, asharam), urea herbicides (DCMU, linuron, siduron, dimuron, methyl dimuron, cumylon, carbyrate, isouron, tebuthiuron), sulfonium urea herbicides (bensulfuron methyl, ethoxysulfuron, pyrasulfuron ethyl, Azimsulfuron, halosulfuron-methyl, flazasulfuron, cinosulfuron, nicosulfuron, limsulfuron, thifensulfuron-methyl, imazosulfuron, metosulfuron-methyl, cyclosulfamuron, floraslam, trifloxysulfuron sodium salt), pyrimidyloxybenzoic acid herbicides (pyriminobac-methyl, bispyribac sodium salt), triazine herbicides (CAT, atrazine, simetryn, ametrine, promethrine, dimethametryn, cyanazine, triaziflam) , metrivudine, metmitron), dianodine herbicides (Terbasil, flumasil, renacil, PAC, bentazon, tazomet), diazole herbicides (pyrazolate, pyrazoxifen, benzofenap), bipyridium herbicides (paraquat, diquat), dinitroaniline herbicides (trifluralin, veslodin, prodiamine, pendimethalin, oryzalin), aromatic carboxylic acid herbicides (MDBA, imazapyr, imazakine, imazakine ammonium salt, dithiopyr, TCTP,Imazamox ammonium salt), fatty acid herbicides (DPA, tetrapion), organophosphate herbicides (amiprophos-methyl, butamiphos, SAP, anirophos), amino acid herbicides (glyphosate, bialaphos, glufosinate), others (ioxynil, bifenox, DBN, DCBN, cethoxidim, cretoxidim, tepraloxidim, ACN, chlorphthalim, flumioxazine) Herbicides such as scinmethiline, carphetrazone ethyl, endotal disodium salt, benfresate, pentoxazone, pyraflufen ethyl, carbam, oxadiclomefone, indanophan, fentrazamide, benzobicyclon, butaphenacil, azaphenidine, pyriftalide, fluthiaset-methyl, oxaziargyl, oxadiazone, and decyl alcohol can be used. For example, they may contain glyphosate, glufosinate, 2,4-D, dicamba, paraquat, diquat, atrazine, mesotrione, florpyrauxifenbenzyl, epiriphenacil, icaphorin, or mesotrione. Herbicides are usually used to suppress the growth of unwanted plants in agricultural land, etc.

[0031] The oxides used in the oxide composite of this embodiment can be appropriately selected according to the type of plant to be weeded and the part to which the herbicide is to be delivered. As the oxide, for example, an oxide that is localized to the roots can be used. For example, if the target plant is a monocotyledonous plant, ZnO can be used.

[0032] The application method of the oxide complex according to this embodiment is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or coating on leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0033] 2-2. Fertilizer Component-Oxide Complex The second embodiment of the oxide complex of this embodiment is an embodiment in which a fertilizer component is used as the useful substance. The plants to which the oxide complex of this embodiment is applied are preferably useful plants such as grains, vegetables, fruits, and flowers.

[0034] In this embodiment, the fertilizer components are not particularly limited, but compounds containing at least one of the following can be used: carbon (C), hydrogen (H), oxygen (O), nitrogen (N), phosphorus (P), potassium (K), calcium (Ca), magnesium (Mg), sulfur (S), boron (B), chlorine (Cl), zinc (Zn), copper (Cu), iron (Fe), manganese (Mn), molybdenum (Mo), nickel (Ni), sodium (Na), silicon (Si), selenium (Se), cobalt (Co), aluminum (Al), chromium (Cr), and cadmium (Cd). The fertilizer components are not limited, but for example, ammonium chloride, urea, potassium chloride, superphosphate, ammonium nitrate, potassium nitrate, calcium cyanamide, boric acid, potassium sulfate, phosphoric acid, diammonium phosphate, calcium dihydrogen phosphate, ammonium sulfate, etc. can all be used.

[0035] The materials constituting the oxide used in the oxide composite of this embodiment can be appropriately selected according to the type of useful plant to be applied and the part to which the fertilizer components are to be delivered. Furthermore, although not limited to these, oxide aggregates containing elements different from the fertilizer components used can be used. As the oxide, for example, an oxide that is localized to the seeds of the target plant can be used. For example, if the target plant is a monocotyledonous plant, ZnO can be used.

[0036] The application method of the oxide complex according to this embodiment is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or coating on leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0037] 2-3. Amino Acid / Peptide / Protein-Oxide Complex A third embodiment of the oxide complex of this embodiment is an embodiment in which amino acids, peptides, or proteins are used as useful substances. The plants to which the oxide complex of this embodiment is applied are preferably useful plants such as grains, vegetables, fruits, and flowers. The amino acids, peptides, or proteins used in this embodiment may be those that have physiological functions in the plant body. The amino acids, peptides, or proteins used in this embodiment are not limited to, but can be, for example, 5-aminolevulinic acid, glycine betaine, methionine, CLE peptide, florigen, amino acid polymers, physiologically active proteins, etc.

[0038] The substances constituting the oxide used in the oxide composite of this embodiment can be appropriately selected according to the type of useful plant to be applied and the part to which amino acids, peptides, or proteins are to be delivered. For example, as the oxide, an oxide that is localized to the leaves of the target plant can be used. For example, if the target plant is a monocotyledonous plant, ZnO, Fe ２ O ３ MgO can be used.

[0039] The application method of the oxide complex according to this embodiment is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or coating on leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0040] 2-4. Sugars A fourth aspect of the oxide complex of this embodiment is one in which sugars are used as the useful substance. The plants to which the oxide complex of this embodiment is applied are preferably useful plants such as grains, vegetables, fruits, and flowers. The sugars used in this embodiment may be those that have physiological functions in the plant body. The sugars used in this embodiment can be at least one selected from the group consisting of monosaccharides, disaccharides, oligosaccharides, and polysaccharides. The sugars are not particularly limited, but for example, they can be glucose, trehalose, raffinose, alginic acid, chitosan, etc.

[0041] The substances constituting the oxide used in the oxide composite of this embodiment can be appropriately selected according to the type of useful plant to be applied and the part to which the sugars are to be delivered. For example, as the oxide, an oxide that is localized to the leaves of the target plant can be used. For example, if the target plant is a monocotyledonous plant, ZnO, Fe ２ O ３ MgO can be used.

[0042] The application method of the oxide complex according to this embodiment is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or coating on leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0043] 2-5. Biostimulant-Oxide Complex The fifth aspect of the oxide complex of this embodiment is an aspect in which a biostimulant is used as the useful substance. The plants to which the oxide complex of this embodiment is applied are preferably useful plants such as grains, vegetables, fruits, and flowers. In this disclosure, "biostimulant" refers to a substance that enhances resistance to abiotic stress and consequently achieves increased yield and improved quality. More specifically, it refers to a component that has functions that affect plant growth, such as regulating reactive oxygen species, improving the photosynthetic capacity of plants, promoting flowering and fruit setting, controlling transpiration, regulating osmotic pressure, improving the rhizosphere environment, increasing root mass, and promoting establishment.

[0044] Biostimulants that can be used include peptides (e.g., CLE peptide), amino acids (e.g., 5-aminolevulinic acid, glycine betaine, methionine), sugars (monosaccharides, oligosaccharides (e.g., raffinose), disaccharides (e.g., trehalose), polysaccharides (e.g., alginic acid), etc.), seaweed extracts, humic substances, organic acids, nucleic acids, plant extracts, food residues, microbial metabolites, etc. Biostimulants are typically used in the cultivation of crops, etc., to increase yields, etc. For example, they may contain CLE peptide or 5-aminolevulinic acid.

[0045] The materials constituting the oxide used in the oxide composite of this embodiment can be appropriately selected according to the type of useful plant to be applied and the part to which the biostimulant is to be delivered. For example, as the oxide, an oxide that is localized to the leaves of the target plant can be used. For example, if the target plant is a monocotyledonous plant, ZnO, Fe ２ O ３ MgO can be used.

[0046] The application method of the oxide complex according to this embodiment is not particularly limited, but may include application to above-ground parts (e.g., spraying or coating on leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0047] 2-6. Plant Growth Regulator - Oxide Complex The sixth aspect of the oxide complex of this embodiment is an aspect in which a plant growth regulator is used as the useful substance. The plants to which the oxide complex of this embodiment is applied are preferably useful plants such as grains, vegetables, fruits, and flowers. In this specification, "plant growth regulator" refers to a chemical used to control the growth and development of useful plants in order to achieve effects such as improved quality, increased yield, stable yield under unfavorable conditions, and reduced labor in production.

[0048] In this embodiment, the plant growth regulator is not particularly limited, but examples include ethylene agents, auxin agents (indolebutyrate, eticlozate, cloxifonac, dichlorprop, 1-naphthylacetamide, 4-CPA), auxin antagonists (maleic acid hydrazide), cytokinin agents (benzylaminopurine, forflorfenuron), cytokinin antagonists (PI-55), gibberellins, dwarfing agents (inabenfide, uriconazole P, chlormecoat, paclobutrazol, flurprimidol, me Plant growth regulators can be used, such as picotet chloride, prohexadione calcium salt, trinexapac ethyl, daminozide, imazapyr, and others (isoprothiolane, oxine sulfate, cyanamide, choline, decyl alcohol, piperonyl butoxide, bendimetaline, brassinosteroids, jasmonic acid, florigen, MCPA, MCPB, NAC, quinoxaline / DEP, pyraflufen ethyl, prohydrojasmonic acid, abscisic acid, chlorella extract, shiitake mushroom mycelium extract). For example, they may contain gibberellin or abscisic acid. Plant growth regulators are usually used in the cultivation of crops, etc., to increase yields.

[0049] The substances constituting the oxide used in the oxide composite of this embodiment can be appropriately selected according to the type of useful plant to be applied and the part to which the plant growth regulator is to be delivered. For example, as the oxide, an oxide that is localized to the leaves of the target plant can be used. For example, if the target plant is a monocotyledonous plant, ZnO, Fe ２ O ３ MgO can be used.

[0050] The application method of the oxide complex according to this embodiment is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or coating on leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0051] 2-7. Fungicide-Oxide Complex The seventh embodiment of the oxide complex of this embodiment is an embodiment in which a fungicide is used as the useful substance. The plants to which the oxide complex of this embodiment is applied are preferably useful plants such as grains, vegetables, fruits, and flowers.

[0052] The fungicides are not particularly limited, but examples include copper fungicides (organocopper agents, nonylphenolsulfonate copper agents, DBEDC agents), organosulfur fungicides (zineb agents, maneb agents, manzeb agents, ambam agents, polycarbamate agents, propineb agents, dilam agents, thiram agents, thiadiazine agents), organophosphorus fungicides (IBP agents, EDDP agents, triflofosmethyl agents, fosetyl agents), organochlorine agents (TPN agents), melanin biosynthesis inhibitors (fusalide agents, tricyclazole agents, pyroquilon agents, carpropamide agents), and benzimidazole fungicides (thiophanate methyl agents, benomide agents). (L-type fungicides, thiabenzol-type fungicides), dicarboxyimide-type fungicides (iprodione-type fungicides, procymidone-type fungicides), acid amide-type fungicides (mepronil-type fungicides, flutolanil-type fungicides, flametopyr-type fungicides, tifluzamide-type fungicides, metalaxyl-type fungicides, oxadixyl-type fungicides, fenhexamide-type fungicides, phenoxanil-type fungicides), sterol biosynthesis inhibitors (triadimefone-type fungicides, vitertanol-type fungicides, mycrobutanil-type fungicides, hexaconazole-type fungicides, tebuconazole-type fungicides, propiconazole-type fungicides, difenoconazole-type fungicides, ibuconazole-type fungicides, imibenconazole-type fungicides, cyproconazole-type fungicides, triflumizole-type fungicides, prochloraz-type fungicides, peph Razoates, phenalimol, pyrifenox, triforin, tetraconazole, oxpoconazole fumarate, fenbuconazole, simeconazole), methoxyacrylate fungicides (azoxystrobin, kresoximmethyl, metminostrobin, trifloxystrobin, famoxadone), anilinopyrimidine fungicides (mepanipyrim, cyprodinil, pyrimethanil), synthetic antibacterial agents (tecrophthalam, oxolinic acid), soil fungicides (fursulfamide, hydroxyisoxazole, eclomethamyl). Zole preparations, dazomet preparations, chloreneb preparations, metasulfocarb preparations, methyl isothiocyanate preparations, D-D preparations, methyl bromide, chloropicrin preparations, carbams, sodium carbams), antibiotic fungicides (streptomycin preparations, oxytetracycline preparations, blastosidine S preparations, kasugamycin preparations, polyoxin preparations, validamycin preparations, mildiomycin preparations), natural fungicides (machine oil preparations, rapeseed oil preparations), probenazole preparations, isoprothiolan preparations, ferimzone preparations, diclomazine preparations, pencyclon preparations, fluorimide preparations, captan preparations, sulfenate preparations,Dithianone, quinoxaline, diflumetrim, fludioxonil, bentazole, acibenzolar S-methyl, triazine, fluazinam, diethofencarb, cymoxanil, iminoctadine acetate, iminoclazine albesilate, propamocarb hydrochloride, dimethomorph, diclocimet, famoxadone, cyazofamide, cyflufenamide, thiadinil, etc. can be used. For example, it may contain fluxapiroxad, ametoctrazine, oxathiapiproline, sulfoxaflor, pidflumetofen, metalaxyl M, oxathiapiproline, or mandipropamide. Fungicides are used for the purpose of preventing infection of crops and / or suppressing the growth of infected pathogens.

[0053] 2-8. Insecticide-Oxide Complex The eighth aspect of the oxide complex of this embodiment is an aspect in which an insecticide is used as the useful substance. The plants to which the oxide complex of this embodiment is applied are preferably useful plants such as grains, vegetables, fruits, and flowers.

[0054] Examples of insecticides include organophosphate insecticides (CYAP, MPP, MEP, ECP, pyrimiphos-methyl, dianodine, quinalphos, isoxathion, pyridafenthion, chlorpyrifos-methyl, chlorpyrifos, malathion, PAP, dimethoate, ethylthiometon, fosalon, PMP, DMPT, prothiophos, sulprophos, profenophos, pyraclophos, DDVP, monoclotophos, BRP, CVMP, dimethylvinphos, CVP, propaphos, acephate, isofen Phosphates, DEPs, EPNs, Ethiones), Carbamate insecticides (NACs, MIPCs, BPMCs, PHCs, XMCs, Ethiofencarbs, Carbosulfan, Benfuracarbs, Frathiocarbs, Methomyls, Oxamyls, Thiodicarbs, Alanicarbs), Pyrethroid insecticides (Allethrins, Resmethrins, Permethrins, Cypermethrins, Cyfluthrins, Cyhalothrins, Tralomethrins, Fenpropathrins, Bifenthrins, Fenvalerates, Esfenvalerates, Flucitrinates, F Luvalinate, acrinatrin, cycloprothrin, etofenprox, silafluofen, tefluthrin), nereistoxin insecticides (cartap, thiocyclam, bensultap), neonicotinoid insecticides (imidacloprid, acetamiprid, nitenpyram, thiacloprid, thiamethoxam, dinotefuran, clothianidin), insect growth regulators (buprofezin, isoprothiolane, diflubenzuron, tiflubenzuron, hexaflumuron, lufenuron, flufenoxuron, Chlorfluazurone, tebufenozide, chromafenozide, cyromazine, methoxyfenozide, pyriproxyfen), natural insecticides (pyrrhizum, deris, nicotine sulfate, machine oil, rapeseed oil, starch, fatty acid glycerides, diatomaceous earth), acaricides (Kelthane, phenisobromolate, tetradiphon, BPPS, quinoxaline, amitraz, phenothiocarb, hexythiazox, fenbutatin oxide, dienochlor, fenpyroximate, tebufenpyrad, fluazinam, pyridaben,Pyrimidife, clofendecine, etoxazole, halfenprox, milbemectin, bialaphos, acekinosyl, bifenazate, propylene glycol monofatty acid ester, fluacrypyrim, spirofuclofen, chlorfenapyr), nematicides (D-D, DCIP, methylisothiocyanate, dazomet, benomyl, fostiazate, oxamyl, pyraclophos, carbam, carbam sodium salt, kazusaphos), pine wood nematode control agents (pinene oil, carbam, carbam sodium You can use sluice salts, MEP agents, MPP agents, pyridafenthion agents, prothiophos agents, malathion agents, NAC agents, acetamiprid agents, thiacloprid agents, mesulfenphos agents, morantel tartrate agents, levamisole hydrochloride agents, nemadectin agents, emamectin benzoic acid, milbemectin agents), slug control agents (metaldehyde agents), benzoepin agents, fibronil agents, chlorfenavir agents, diafenthiuron agents, pymetrozine agents, emamectin benzoic acid, sodium oleate agents, DBEDC agents, indoxacarb agents, tolfenpyrad agents, etc. For example, it may contain spirotetramat, ethiprole, zimphropyridaz, fluxapyroxad, chlorfenapyr, afidopiropene, fipronil, spinosad, sulfoxaflor, triflumezopyrim, or cyantraniliprole. Insecticides are used to prevent and / or control pest damage to crops and other agricultural products.

[0055] 3. Composition for delivering useful substances into plant tissue A second embodiment of the present invention is a composition for delivering useful substances into plant tissue. The composition of this embodiment is characterized by containing any of the oxide complexes described in section 2, "Oxide complexes for delivering useful substances into plant tissue." The "composition" referred to herein may be a liquid composition or a solid composition.

[0056] The composition of this embodiment may include, in addition to the oxide complex, at least one of a carrier, dispersant, stabilizer, pH adjuster, anti-solidification agent, and defoamer. For liquid compositions, a liquid carrier can be used; for solid compositions, a solid carrier can be used. For the former, water can be used, for example. For the latter, cellulose, talc, bentonite, etc., can be used. The dispersant is an agent used to uniformly disperse the oxide complex in the liquid; for example, a surfactant can be used. It is preferable to use a biodegradable compound as the surfactant, and biosurfactants such as rhamnolipid are known as such surfactants. The stabilizer is an agent used to suppress the decomposition, denaturation, etc., of the useful substance. The stabilizer can be appropriately selected depending on the type of useful substance used. For example, if the useful substance is a peptide, glycerol, amino acids, etc., can be used. For the carrier, dispersant, stabilizer, pH adjuster, anti-solidification agent, defoamer, etc., it is preferable to use substances known to have no adverse effects on the environment or agents approved by the authorities as pesticide additives, depending on the purpose.

[0057] The content of the oxide complex in the composition of this embodiment is not particularly limited and can be adjusted as appropriate according to the intended use. For example, in the case of a liquid composition, the content of the oxide complex can be 0.001 to 1.0%, particularly 0.005 to 0.5% or 0.01 to 0.2%.

[0058] 3-1. Herbicide Composition The first aspect of this embodiment is a herbicide composition. Specifically, the herbicide composition of this embodiment includes the oxide complex described in section "2-1. Herbicide-Oxide Complex". The method of application of the herbicide composition is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or applying to leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0059] 3-2. Fertilizer Composition The second aspect of this embodiment is a fertilizer composition. Specifically, the fertilizer composition of this embodiment includes the oxide complex described in section "2-2. Fertilizer Components - Oxide Complexes". The application method of the fertilizer composition is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or applying to leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0060] 3-3. Amino Acid / Peptide / Protein Composition The third aspect of this embodiment is an amino acid / peptide / protein composition. Specifically, the amino acid / peptide / protein composition of this embodiment includes the oxide complex described in section "2-3. Amino Acid / Peptide / Protein-Oxide Complex". The application method of the amino acid / peptide / protein composition is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or coating on leaves), mixing into soil, mixing into a culture medium or water (in the case of hydroponics).

[0061] 3-4. Biostimulant Composition The fourth aspect of this embodiment is a biostimulant composition. Specifically, the biostimulant composition of this embodiment includes the oxide complex described in section "2-4. Biostimulant-Oxide Complex". The method of application of the biostimulant composition is not particularly limited, but may include application to above-ground parts (e.g., spraying or coating on leaves), mixing into soil, mixing into a growing medium or water (in the case of hydroponics), etc.

[0062] 3-5. Plant Growth Regulating Composition The fifth aspect of this embodiment is a plant growth regulating composition. Specifically, the plant growth regulating composition of this embodiment includes the oxide complex described in section "2-5. Plant Growth Regulating Agents - Oxide Complexes". The method of application of the plant growth regulating composition is not particularly limited, but may include application to above-ground parts (e.g., spraying or applying to leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0063] 3-6. Fungicide Composition The sixth aspect of this embodiment is a fungicide composition. Specifically, the fungicide composition of this embodiment includes the oxide complex described in section "2-6. Fungicide-Oxide Complex". The method of application of the fungicide composition is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or applying to leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0064] 3-7. Insecticide Composition The seventh aspect of this embodiment is an insecticide composition. Specifically, the insecticide composition of this embodiment includes the oxide complex described in section "2-7. Insecticide-Oxide Complex". The method of application of the insecticide composition is not particularly limited, but may include, for example, application to above-ground parts (e.g., spraying or coating on leaves), mixing into soil, or mixing into a growing medium or water (in the case of hydroponics).

[0065] 4. Method for delivering useful substances into a plant (I) A third embodiment of the present invention is a method for delivering useful substances into a plant, characterized by applying any oxide complex described in section "2. Oxide complexes for delivering useful substances into a plant" to a plant or the soil, culture medium, or water surrounding the plant. The method of this embodiment may also include applying a composition described in section "3. Compositions for delivering useful substances into a plant" to a plant or the soil, culture medium, or water surrounding the plant, that is, applying any oxide complex described in section "2. Oxide complexes for delivering useful substances into a plant" in the form of a composition.

[0066] Methods for directly applying the oxide complex to plants include spraying or coating the above-ground parts of the plants, particularly applying it to the upper or lower surfaces of the leaves. In soil cultivation, the oxide complex can be mixed into the soil near the plants. In hydroponic cultivation, the oxide complex can be suspended in the growing medium or water near the plants. The application rate can be adjusted as appropriate according to the desired effect, but it is preferable that the amount of the useful substance applied is less than the known effective amount of that useful substance. For example, it can be 1% to 90%, 5% to 80%, or 10% to 50% of the known effective amount.

[0067] 5. Method for delivering useful substances into a plant (II) A fourth embodiment of the present invention is a method for delivering useful substances into a plant, comprising the steps of: preparing an oxide complex by combining an oxide aggregate and a useful substance; and applying the oxide complex to the plant or the soil, culture medium, or water surrounding the plant. According to the method of this embodiment, a suitable oxide complex can be prepared and applied to the plant according to the target plant, the type of useful substance, and the desired effect.

[0068] 5-1. Oxide Composite Preparation Step The method of this embodiment includes a step of preparing an oxide composite. The useful substance and the substances constituting the oxide in the oxide composite to be prepared can be appropriately selected according to the target plant and the desired effect. For example, if the target plant is cabbage, as described above, it is known that zinc is localized in the roots and silica in the buds, so for example, if you want to deliver the useful substance to the roots, use ZnO, and if you want to deliver it to the buds, use SiO ２ For example, if you want to promote the growth of cabbage sprouts, you can select calcium dihydrogen phosphate, a fertilizer component, as a useful substance. If the localization of elements in the target plant is unknown, you may introduce various oxide (nano) particles or elements into the plant beforehand and measure the elemental content in different parts of the plant to determine the localization.

[0069] This process involves bonding a selected useful substance with an oxide aggregate. The method for bonding the useful substance and the oxide aggregate is not particularly limited as long as the useful substance can be fixed to the surface of the oxide aggregate, and can be appropriately selected depending on the type of useful substance and the elements constituting the oxide aggregate. However, it is particularly preferable to use a method that allows for chemical bonding between the useful substance and the oxide. For example, if the useful substance is a polysaccharide (e.g., chitosan) and the oxide aggregate is a metal oxide aggregate (e.g., ZnO), a method can be used in which the useful substance and the oxide aggregate are brought together under alkaline conditions and heated. Reaction conditions such as pH, temperature, and time can be appropriately set according to the type of useful substance and oxide aggregate used.

[0070] This process may, if necessary, include incorporating the prepared oxide complex into the composition. Unless otherwise specified, and unless otherwise contradictory, the constituent materials, content, and preparation method of the composition referred to herein are the same as those described in section 3, "Compositions for delivering useful substances into plant tissue."

[0071] 5-2. Application Process The method of this embodiment includes the step of applying the prepared oxide complex to plants, the soil surrounding the plants, the growing medium, and water. Unless otherwise specified and unless otherwise contradicted, the application method in this step is the same as the application method described in "4. Method for delivering useful substances into plant tissue (I)".

[0072] 6. Other Embodiments In addition to the embodiments described above, the present invention also encompasses any embodiment comprising a composite of a useful substance and an oxide aggregate. For example, it also encompasses plants grown by applying the oxide composite, and seeds, tubers, fruits, etc., obtained from said plants.

[0073] The following describes embodiments of the present invention, but the present invention is not limited in any way to these embodiments.

[0074] [Example 1] Localization of various oxide particles in wheat plants (1-1) Preparation of oxide particle suspensions Zinc oxide particles (ZnO), iron oxide particles (Fe ２ O ３ A suspension of magnesium oxide particles (MgO) was prepared, along with ZnO (particle size 50 nm, DLS measurement), and Fe. ２ O ３ (Particle size 40 nm, DLS measurement) and MgO (Particle size 875 nm, DLS measurement) were synthesized by the liquid-phase method. The various oxide particles were suspended in distilled water.

[0075] (1-2) Application to wheat plants: Seeds of wheat (variety: white wheat) were sown in plastic pots filled with black granular soil and cultivated for 10 days to grow the plants. One leaf of each plant was coated with the various oxide particle suspensions prepared in (1-1), and cultivation was continued for 5 days. As a control, the same test was performed on plants coated with water instead of the oxide particle suspension.

[0076] (1-3) Wheat plants were collected after analytical treatment and separated into treated leaves, non-treated above-ground parts, and underground parts, and each was thoroughly dried in an oven. After drying, each sample was crushed, placed in a test tube, and dissolved in nitric acid solution while heating. The supernatant after dissolution was subjected to atomic absorption spectrophotometer to measure the content of each element.

[0077] Figure 1 shows comparative data of zinc content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of wheat plants treated with ZnO suspension compared to a control. Zinc content is expressed as zinc per 1 mg of dry matter weight. Error bars in the figure indicate the standard deviation. "***" in the figure indicates a statistically significant difference at the 0.1% level compared to the control, as determined by Student's t-test. While no difference was observed in treated leaves compared to the control, the zinc content was significantly higher in the above-ground parts other than treated leaves and in the underground parts of plants treated with ZnO suspension. From these results, it was considered that ZnO has localization in the above-ground parts and roots of wheat.

[0078] Figure 2 shows Fe ２ O ３ This figure shows comparative data of iron content in treated wheat plants (A), above-ground parts (B), and underground parts (C) compared to a control group. Iron content is expressed as iron per 1 mg of dry matter weight. Error bars in the figure indicate the standard deviation. "*", "**", and "***" in the figure indicate statistically significant differences from the control group at the 5%, 1%, and 0.1% levels, respectively, as determined by Student's t-test. In the treated leaves, Fe... ２ O ３ The iron content was significantly higher in plants treated with the suspension compared to the control. On the other hand, in the above-ground parts other than the treated leaves and in the underground parts, Fe ２ O ３ It was confirmed that the iron content was significantly lower in plants treated with the suspension. From these results, it was found that in wheat, Fe ２ O ３ It was thought to have localization to the leaves.

[0079] Figure 3 shows comparative data of magnesium content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of wheat plants treated with MgO suspension compared to a control. Magnesium content is expressed as magnesium per 1 mg of dry matter weight. Error bars in the figure indicate the standard deviation. An asterisk (*) in the figure indicates a statistically significant difference at the 5% level compared to the control, as determined by Student's t-test. In the above-ground parts other than treated leaves, the magnesium content was significantly higher in plants treated with MgO suspension compared to the control. On the other hand, no significant difference was observed in the treated leaves or underground parts compared to the control. From these results, it was considered that MgO is localized to the above-ground parts in wheat.

[0080] [Example 2] Localization of various oxide particles in soybean plants (2-1) Preparation of oxide particle suspensions Various oxide particle suspensions were prepared in the same manner as in (1-1) above.

[0081] (2-2) Application to soybean plants: Soybean seeds (variety: Fukuyutaka) were sown in plastic pots filled with black granular soil and cultivated for 18 to 30 days to grow the plants. One leaf of each plant was coated with the various oxide particle suspensions prepared in (2-1), and cultivation was continued for 5 days. As a control, the same test was performed on plants coated with water instead of the oxide particle suspension.

[0082] (2-3) After the analysis treatment of soybean plants, the plants were collected and separated into treated leaves, above-ground parts other than treated leaves, and underground parts, and each was thoroughly dried in an oven. After drying, each sample was crushed and placed in a test tube, and then dissolved in nitric acid solution while heating. The supernatant after dissolution was subjected to atomic absorption spectrophotometer to measure the content of each element.

[0083] Figure 4 shows comparative data of zinc content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of soybean plants treated with ZnO suspension compared to a control. Zinc content is expressed as zinc per 1 mg of dry matter weight. Error bars in the figure indicate the standard deviation. An asterisk (*) in the figure indicates a statistically significant difference at the 5% level compared to the control, as determined by Student's t-test. It was confirmed that the zinc content was significantly higher in plants treated with ZnO suspension in the treated leaves. On the other hand, no significant difference was observed in above-ground parts other than treated leaves or in underground parts compared to the control. From these results, it was considered that ZnO is localized to the leaves in soybeans.

[0084] Figure 5 shows Fe ２ O ３ This figure shows comparative data of iron content in soybean plants treated with a suspension, and in the treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of the control. Iron content is expressed as iron per 1 mg of dry matter weight. Error bars in the figure indicate the standard deviation. "***" in the figure indicates a statistically significant difference at the 0.1% level compared to the control, as determined by Student's t-test. In the treated leaves, Fe... ２ O ３ The iron content was significantly higher in plants treated with the suspension compared to the control. On the other hand, no significant difference was observed in the above-ground parts other than the treated leaves and in the underground parts compared to the control. From these results, it can be concluded that in soybeans, Fe ２ O ３ It was thought to have localization to the leaves.

[0085] Figure 6 shows comparative data of magnesium content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of soybean plants treated with MgO suspension compared to a control. Magnesium content is expressed as magnesium per 1 mg of dry matter weight. Error bars in the figure indicate the standard deviation. An asterisk (*) in the figure indicates a statistically significant difference at the 5% level compared to the control, as determined by Student's t-test. In the above-ground parts other than treated leaves, the magnesium content was significantly higher in plants treated with MgO suspension compared to the control. On the other hand, no significant difference was observed in the treated leaves or underground parts compared to the control. From these results, it was considered that MgO is localized to the above-ground parts of soybeans.

[0086] [Example 3] Localization of various oxide particles in lettuce plants (3-1) Preparation of oxide particle suspensions Various oxide particle suspensions were prepared in the same manner as in (1-1) above.

[0087] (3-2) Application to Lettuce Plants Lettuce (variety: Chima Sangchu) seeds were sown in plastic pots filled with black granular soil and cultivated for 25 to 40 days to grow the plants. One leaf of each plant was coated with the various oxide particle suspensions prepared in (3-1) and cultivation was continued for 5 days. As a control, the same test was performed on plants coated with water instead of the oxide particle suspension.

[0088] (3-3) Analytical samples of lettuce plants were collected after treatment and separated into treated leaves, non-treated above-ground parts, and underground parts, and each was thoroughly dried in an oven. After drying, each sample was crushed and placed in a test tube, then dissolved in nitric acid solution while heating. The supernatant after dissolution was subjected to atomic absorption spectrophotometer to measure the content of each element.

[0089] Figure 7 shows comparative data of zinc content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of lettuce plants treated with ZnO suspension and a control. Zinc content is expressed as zinc per 1 mg of dry matter weight. Error bars in the figure indicate the standard deviation. An asterisk (*) in the figure indicates a statistically significant difference at the 5% level compared to the control, as determined by Student's t-test. It was confirmed that the zinc content was significantly higher in plants treated with ZnO suspension in the treated leaves. On the other hand, no significant difference was observed in above-ground parts other than treated leaves or in underground parts compared to the control. From these results, it was considered that ZnO is localized to the leaves in lettuce.

[0090] Figure 8 shows Fe ２ O ３ This figure shows comparative data of iron content in treated lettuce plants (A), above-ground parts (B), and underground parts (C) compared to a control group. Iron content is expressed as iron per 1 mg of dry matter weight. Error bars in the figure indicate the standard deviation. "***" in the figure indicates a statistically significant difference at the 0.1% level compared to the control, as determined by Student's t-test. In the treated leaves, Fe... ２ O ３ The iron content was significantly higher in plants treated with the suspension compared to the control. On the other hand, no significant difference was observed in the above-ground parts other than the treated leaves and in the underground parts compared to the control. From these results, it can be concluded that in lettuce, Fe... ２ O ３ It was thought to have localization to the leaves.

[0091] Figure 9 shows comparative data of magnesium content in treated leaves (A), above-ground parts other than treated leaves (B), and underground parts (C) of lettuce plants treated with MgO suspension compared to a control. Magnesium content is expressed as magnesium per 1 mg of dry matter weight. Error bars in the figure indicate the standard deviation. "**" in the figure indicates a statistically significant difference at the 1% level compared to the control, as determined by Student's t-test. In treated leaves, the magnesium content was significantly higher in plants treated with MgO suspension compared to the control. On the other hand, no significant difference was observed in above-ground parts other than treated leaves or in underground parts compared to the control. From these results, it was considered that MgO is localized to the leaves in lettuce.

[0092] Table 1 summarizes the localization of various oxide particles based on their behavior within wheat, soybean, and lettuce plants. In the table, "○" indicates areas where localization was observed, and "×" indicates areas where localization was not observed.

[0093]

[0094] [Example 4] Herbicidal Efficacy Test of Zinc Oxide-Glyphosate Complex (ZnO-Glyp) (4-1) Preparation of ZnO-Glyp ZnO reagent (particle size 20 nm) was supplied by Fujifilm Wako Pure Chemical Industries, Ltd., and glyphosate was supplied by LGC Standards, Inc. The particle size (degree of aggregation) was adjusted by adjusting the amount of ZnO reagent and pH. The binding reaction of ZnO and glyphosate was carried out by mixing in solution. In this section, the following tests using ZnO-Glyp were carried out under conditions of a glyphosate concentration of 0.1%, unless otherwise specified.

[0095] Analysis of the prepared ZnO-Glyp using Fourier transform infrared spectroscopy (FT-IR) (Cary 670 (Agilent Corporation)) revealed infrared absorption at the same wavelength as both ZnO and glyphosate, as well as absorption originating from the P-O bond. This confirmed that ZnO and Glyp were chemically bonded, forming a complex. The number-average particle size of ZnO-Glyp was measured using a DLS analyzer (DLS-8000 or ELSZ-2000 (Otsuka Electronics Co., Ltd.)). The particle sizes of the prepared ZnO-Glyp were approximately 100 nm, 200 nm, 400 nm, 500 nm, 700 nm, 800 nm, 1000 nm, 1100 nm, 1300 nm, and 1400 nm.

[0096] (4-2) Application of ZnO-Glyp to various plants ZnO-Glyp application tests were conducted on plants of Adenophora triphylla, rice, wheat, and celosia. Water (control), a 0.1% glyphosate aqueous solution (Glyp), and an aqueous suspension of ZnO-Glyp of various particle sizes equivalent to 0.1% glyphosate were applied to the above-ground parts of each plant. At the time of application, the above-ground height of each plant was 8-13 cm for Adenophora triphylla, 22-23 cm for rice, 15-20 cm for wheat, and 17-23 cm for celosia. SPAD values ​​or individual plant mortality rates were measured 8, 12, 13, or 20 days after application. For Adenophora triphylla and celosia, SPAD values ​​were measured using a chlorophyll meter (SPAD-502plus (Konica Minolta)). For rice and wheat, the mortality rate was measured. For rice, the criterion for death was the cessation of new leaf development, and for wheat, it was the yellowing of all leaves. The experiment was conducted with n=5-9 for *Epipogium aparine*, 3 replications of 10 individuals each for rice and wheat, and n=3 for *Celosia argentea*.

[0097] Figure 10 shows the SPAD values ​​or mortality rates of various plants after application of ZnO-Glyp. Figure 10A shows the SPAD value of *Epipogium aureum* 13 days after application. Figure 10B shows the mortality rate of rice 20 days after application, and Figure 10C shows the mortality rate of wheat 8 days after application. Figure 10D shows the SPAD value of celosia 'Celosia' 12 days after application. The numbers at the bottom of the graphs indicate the particle size measurements of each type of ZnO-Glyp. In the figures, "*" and "***" indicate a statistically significant difference from the control at the 5% and 0.1% levels, respectively, according to Dunnet's test. Error bars indicate the standard deviation. Different letters in the figures indicate a statistically significant difference at the 5% level according to Tukey's test. The SPAD value of *Epipogium aureum* was lower when ZnO-Glyp with a particle size of 400 nm or larger was applied. The mortality rate of rice plants was higher with increasing particle size of ZnO-Glyp applied, and was significantly higher with ZnO-Glyp with a particle size of 1100 nm. The mortality rate of wheat plants was high with ZnO-Glyp with a particle size of over 1000 nm. The SPAD value of celosia plants was significantly lower with ZnO-Glyp with a particle size of 1300 nm. In all plants, a stronger herbicidal effect was observed when ZnO-Glyp was applied compared to when glyphosate was applied alone.

[0098] (4-3) Adhesion of ZnO-Glyp to the leaves of *Epipogium aquilinum* ZnO-Glyp with particle sizes of 62.9 ± 17.0 nm (hereinafter referred to as "60 nm") and 1079 ± 237.6 nm (hereinafter referred to as "1100 nm") was applied to the entire surface of both sides of the leaves of *Epipogium aquilinum*. The amount of zinc on the leaf surface after application was measured and the adhesion rate to the leaf was calculated by dividing it by the amount of zinc applied.

[0099] Figure 11 shows the adhesion rates of various ZnO-Glyp particles. In the figure, "***" indicates a statistically significant difference at the 0.1% level compared to the control, as determined by a t-test. It was confirmed that the adhesion rate was significantly higher when ZnO-Glyp with a particle size of 1100 nm was applied compared to when ZnO-Glyp with a particle size of 60 nm was applied. This suggests that the high weed control efficiency observed when applying ZnO-Glyp with a larger particle size is due to the high adhesion rate of the composite with that particle size, which allows the herbicide effect to be sustained.

[0100] (4-4) Glyp uptake efficiency of *Echinococcus mutabilis* when ZnO-Glyp is applied. １３ Glyp( １３ Prepare C-Glyp) １３ C-ZnO-Glyp was prepared. １３ The particle size of C-ZnO-Glyp was 1141.5 ± 317.9 nm. Similar to (1-2), water (control), １３ C-Glyp, １３ C-ZnO-Glyp was applied to *Epipogium aquilinum*. Leaves were collected 12 days after application and thoroughly dried in an oven. After drying, each sample was ground and analyzed using a stable isotope ratio mass spectrometer (ANCA-GSL / Hydra2022, Sercon). １３ The relative abundance (%) of element C was calculated. The experiment was conducted with n=3.

[0101] Figure 12 shows the conditions for each of the following １３ This shows the proportion of element C. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. １３ When applying C-ZnO-Glyp, １３ Compared to when C-Glyp is applied, １３ The significantly higher uptake of C indicates that the use of the ZnO complex promoted the uptake of Glyp in *Epipogium aquilinum*.

[0102] [Example 5] Silicon dioxide-glyphosate composite (SiO ２ - Herbicide efficacy test using Glyp (5-1) SiO ２ - Preparation of Glyp SiO ２ The reagents used were AEROSIL (manufactured by Nippon Aerosil Co., Ltd., particle size 200 nm (DLS measurement)) and glyphosate (manufactured by LGC Standards). ２ By adjusting the amount of reagents, pH, etc., the particle size (degree of aggregation) is controlled, and two types of SiO with different particle sizes are produced. ２ -Glyp was prepared. SiO ２ The glyphosate binding reaction was carried out by mixing in solution. Unless otherwise specified, the following tests were performed under conditions of a glyphosate concentration of 0.1%.

[0103] Two types of prepared SiO ２ - Glyp were each analyzed by FT-IR. As a result, a shift in the wavelength of the spectrum derived from the Si-O bond was confirmed in both, and from this, it was speculated that SiO ２ and Glyp were chemically bonded to form a complex. Using a DLS analyzer, the number-average particle diameter of each SiO ２ - Glyp was measured. The particle diameters of the prepared SiO ２ - Glyp were 978.2 ± 219.5 nm and 1280.5 ± 258.8 nm. Hereafter, the former is referred to as "SiO ２ - Glyp (1000 nm)", and the latter is referred to as "SiO ２ - Glyp (1300 nm)".

[0104] (5-2) Application of SiO ２ - Glyp to Minato-kamogusa An application test of SiO ２ - Glyp was carried out on the plant body of Minato-kamogusa. On the above-ground parts of various plants with an above-ground height of 7 to 11 cm, water (control), 0.1% glyphosate aqueous solution (Glyp), SiO ２ - Glyp (1000 nm) aqueous suspension, and SiO ２ - Glyp (1300 nm) aqueous suspension were applied so as to be 150 μL / plant body. The SPAD value 5 days after spraying was measured. The test was carried out with n = 5 to 10 for each.

[0105] Fig. 13 shows the SPAD values of Minato-kamogusa under each condition. The error bars indicate the standard deviation. Different alphabet letters in the figure indicate a significant difference at the 5% level by the Tukey test. It was confirmed that the SPAD value of Minato-kamogusa after the application of SiO ２ - Glyp was significantly decreased compared with the control and Glyp.

[0106] (5-3) Localization coincidence rate of SiO ２ and Glyp The SiO ２ - Glyp prepared in (5-1) was applied to a carbon sample stage and dried, and elemental analysis was performed using a field emission scanning electron microscope (FE-SEM) and an energy dispersive X-ray analyzer (EDS).

[0107] Figure 14 shows the FE-SEM / EDS results. Figure 14A shows the localization of phosphorus (P), and Figure 14B shows the localization of silicon (Si). The localization agreement rate between P and Si was 71.8%. Figure 15 shows the FE-SEM / EDS results. Figure 15A shows the electron microscope image, Figure 15B shows the localization of Si, Figure 15C shows the localization of P, and Figure 15D shows the spectrum of the elements accumulated from the pixels on the image. As shown in Figure 15D, the elemental abundances of Si and P on the image were 50%:50%. From these results, SiO ２ - In Glyp, SiO ２ The presence of Glyp at the same location and in nearly equal amounts suggested that they are bound together at a high rate.

[0108] [Example 6] Iron oxide-glyphosate complex (Fe ２ O ３ - Glyp, Fe ３ O ４ - Glyp) Herbicide efficacy test (6-1) Fe ２ O ３ - Glyp, Fe ３ O ４ - Preparation of Glyp Fe ２ O ３ The reagent (particle size 20-40 nm) is manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. ３ O ４ The reagents (particle size 50-100 nm) were supplied by Sigma-Aldrich Japan, and the glyphosate was supplied by LGC Standards. The binding reaction of iron oxide and glyphosate was carried out by mixing in solution. Unless otherwise specified, the following tests were performed under conditions of a glyphosate concentration of 0.1%.

[0109] Prepared Fe ２ O ３ - Analysis of Glyp using FT-IR revealed that Fe ２ O ３ We confirmed that Fe exhibits the same absorption as glyphosate, as well as absorption originating from the P-O bond. ２ O ３ It was confirmed that the compound and Glyp are chemically bonded and form a complex. Using a DLS analyzer, Fe ２ O ３ - Glyp, Fe ３ O４ - The number-average particle size of Glyp was measured. ２ O ３ - Glyp, Fe ３ O ４ The particle sizes of -Glyp were 775.8 ± 126.5 nm and 1166.9 ± 256.0 nm, respectively.

[0110] (6-2) Fe ２ O ３ - Glyp, Fe ３ O ４ - Application of Glyp to *Lysimachia japonica* Fe to the plant body of *Lysimachia japonica* ２ O ３ - Glyp, Fe ３ O ４ - A Glyp application test was conducted. Various plants with above-ground parts 6-10 cm tall were treated with water (control), a 0.1% glyphosate aqueous solution (Glyp), and an amount of Fe equivalent to 0.1% glyphosate. ２ O ３ - Glyp aqueous suspension, Fe equivalent to 0.1% glyphosate ３ O ４ -Glyp aqueous suspension was applied to each plant at a rate of 100 μL / plant. The SPAD value was measured 14 days after application. Each test was conducted with n=5 to 9 participants.

[0111] Figure 16 shows the SPAD values ​​of *Corydalis ambigua* under each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Compared to the control and Glyp, Fe ２ O ３ - Glyp, Fe ３ O ４ - It was confirmed that the SPAD value of *Epipactis thunbergii* decreased significantly after Glyp application.

[0112] [Example 7] Herbicidal efficacy test using magnesium oxide-glyphosate complex (MgO-Glyp) (7-1) Preparation of MgO-Glyp MgO reagent (particle size 50 nm) was supplied by Fujifilm Wako Pure Chemical Industries, and glyphosate was supplied by LGC Standards. The binding reaction of MgO and glyphosate was carried out by mixing in solution. Unless otherwise specified, the following tests were conducted under conditions of a glyphosate concentration of 0.1%.

[0113] Analysis of the prepared MgO-Glyp by FT-IR revealed that it exhibited the same absorption as both MgO and glyphosate, as well as absorption originating from the P-O bond. This confirmed that MgO and Glyp were chemically bonded, forming a complex. The number-average particle size of MgO-Glyp was measured using a DLS analyzer. The particle size of the prepared MgO-Glyp was 773.1 ± 187.9 nm.

[0114] (7-2) Application of MgO-Glyp to Lathyrus chinensis An application test of MgO-Glyp was conducted on Lathyrus chinensis plants. Water (control), 0.1% glyphosate aqueous solution (Glyp), and an aqueous suspension of MgO-Glyp equivalent to 0.1% glyphosate were applied to the above-ground parts of various plants with a height of 6-10 cm, at a rate of 100 μL / plant. The SPAD value was measured 6 days after application. Each test was conducted with n=5-10.

[0115] Figure 17 shows the SPAD values ​​of *Lindernia procumbens* under each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. It was confirmed that the SPAD values ​​of *Lindernia procumbens* after MgO-Glyp application were significantly lower compared to the control and Glyp.

[0116] [Example 8] Silver oxide-glyphosate complex (Ag ２ Herbicide efficacy test using O-Glyp (8-1) Ag ２ Preparation of O-Glyp Ag ２ The reagent used was from Fujifilm Wako Pure Chemical Industries (particle size 80 nm (DLS measurement)), and the glyphosate used was from LGC Standards. ２O. The binding reaction of glyphosate was carried out by mixing in solution. Unless otherwise specified, the following tests were performed under conditions of a glyphosate concentration of 0.1%.

[0117] Prepared Ag ２ Analysis of O-Glyp using FT-IR revealed that Ag ２ We confirmed that both oxygen and glyphosate exhibited the same absorption, as well as absorption originating from the P-O bond. This indicates that Ag ２ It was confirmed that O and Glyp are chemically bonded and form a complex. Using a DLS analyzer, Ag ２ The number-average particle size of O-Glyp was measured. ２ The particle size of O-Glyp was 141.1 ± 46.7 nm.

[0118] (8-2) Ag ２ Application of O-Glyp to *Lysimachia japonica*: Ag applied to the plant body of *Lysimachia japonica*. ２ An O-Glyp application test was conducted. Various plants with above-ground heights of 7-11 cm were treated with water (control), a 0.1% glyphosate aqueous solution (Glyp), and an amount of Ag equivalent to 0.1% glyphosate. ２ O-Glyp aqueous suspension was applied to each plant at a rate of 150 μL / plant. The SPAD value was measured 4 days after application. Each test was conducted with n=7 to 10 participants.

[0119] Figure 18 shows the SPAD values ​​of *Cypripedium macranthos* under each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Compared to the control and Glyp, Ag ２ A significant decrease in the SPAD value of *Epipogium aureum* after application of O-Glyp was confirmed.

[0120] [Example 9] Zinc oxide-calcium dihydrogen phosphate complex (ZnO-Ca(H ２ PO ４ ) ２ Growth promotion effect test by (9-1) ZnO-Ca(H ２ PO ４ ) ２A complex of calcium dihydrogen phosphate and ZnO, which are components of the prepared fertilizer, was prepared using the following procedure. ZnO was prepared by the liquid-phase method (particle size approximately 30 nm (DLS measurement)), and calcium dihydrogen phosphate manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. was used. The particle size (degree of aggregation) was adjusted by adjusting the amount of ZnO and pH. The bonding reaction of ZnO and calcium dihydrogen phosphate was carried out by mixing in solution. Unless otherwise specified, the following tests were conducted under conditions of a calcium dihydrogen phosphate concentration of 1.0%. Prepared ZnO-Ca(H) ２ PO ４ ) ２ Analysis using FT-IR revealed that both ZnO and calcium dihydrogen phosphate exhibited the same absorption, as well as absorption originating from the P-O bond. This indicates that ZnO and Ca(H) ２ PO ４ ) ２ It was confirmed that the two chemically bond and form a complex. Using a DLS analyzer, it was determined that ZnO-Ca(H ２ PO ４ ) ２ The number-average particle size was measured. ２ PO ４ ) ２ The particle size was 753.0 ± 138.0 nm.

[0121] (9-2) ZnO-Ca(H ２ PO ４ ) ２ For the application to komatsuna, seeds of komatsuna (variety: Natsurakuten) were sown in cell trays filled with sand (no fertilizer) and cultivated for 21 days. Water (control) and Ca(H) were applied to the above-ground parts of each plant. ２ PO ４ ) ２ Aqueous solution, ZnO-Ca(H ２ PO ４ ) ２ Each plant was sprayed with 2 mL of the aqueous suspension, and cultivation was continued for 21 days. Each plant was collected, and the fresh weight (FW) of the underground part was measured. The experiment was conducted with n=25.

[0122] Figure 19 shows the fresh underground weight of komatsuna under each condition 21 days after application. Error bars in the figure indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Figure 20 shows photographs of the external appearance of each plant 21 days after application. ZnO-Ca(H ２ PO ４ ) ２ In plants treated with this method, the growth of the underground parts was significantly promoted.

[0123] [Example 10] Test of the stomatal closure effect of zinc oxide-CLE25 peptide complex (ZnO-CLE25) on cabbage (10-1) Preparation of ZnO-CLE25 CLE25 peptide was obtained from Fujifilm Wako Pure Chemical Industries, Ltd. ZnO reagent (particle size 20 nm) was supplied by Fujifilm Wako Pure Chemical Industries, and CLE25 peptide was supplied by Peptide Research Institute Co., Ltd. The particle size (degree of aggregation) was adjusted by adjusting the amount of ZnO reagent and pH. The binding reaction of ZnO and CLE25 peptide was carried out by mixing in solution. Considering the stability of the CLE25 peptide, the above reaction was carried out under low temperature and light-shielded conditions. The following tests were carried out under conditions of glyphosate concentration 0.1%, unless otherwise specified. Analysis of the prepared ZnO-CLE25 by FT-IR confirmed that both ZnO and CLE25 peptide had the same absorption, as well as absorption originating from the C=O bond. This confirmed that ZnO and CLE25 were chemically bonded, forming a complex. The number-average particle size of ZnO-CLE25 was measured using a DLS analyzer. The particle size of the prepared ZnO-CLE25 was 96.5 ± 22.4 nm.

[0124] (10-2) Application of ZnO-CLE25 to cabbage 42 days after sowing, the leaves of cabbage (variety: Harunami) were sprayed with water (control), a 100 μM CLE25 peptide aqueous solution, and an aqueous suspension of ZnO-CLE25 equivalent to 100 μM CLE25 peptide, each at a rate of 2 mL / plant.

[0125] (10-3) Measurement of Stomatal Conductance For each leaf after application, stomatal conductance was measured 4 hours after application using a porometer (SC-Leaf Porometer (METER)) to check the stomatal opening and closing state. The results are shown in Figure 21. It was confirmed that stomatal conductance was significantly reduced when ZnO-CLE25 was used compared to when CLE25 was applied alone.

[0126] [Example 11] Silicon dioxide-abscisic acid complex (SiO ２ - Stomatal closure effect test using ABA (11-1) SiO ２ - Preparation of ABA: Abscisic acid (ABA), a plant hormone, and silicon dioxide (SiO2) ２ A complex was prepared with SiO. ２ The mixture was prepared by a liquid-phase method (particle size approximately 60 nm), and abscisic acid manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. was used. ２ The particle size (degree of aggregation) was adjusted by adjusting the quantity, pH, etc. SiO ２ The abscisic acid binding reaction was carried out by mixing in solution. Considering the stability of abscisic acid, the above reaction was carried out under low temperature and light-shielded conditions. In the following tests, the abscisic acid concentration was changed depending on the plant species.

[0127] Prepared SiO ２ Analysis of ABA using FT-IR confirmed absorption originating from the C-H bond in ABA. ２ It was confirmed that ABA and SiO2 chemically bonded together, forming a complex. ２ - The particle size of ABA was 374.3 ± 55.9 nm for the composite applied to cabbage and 314.9 ± 69.9 nm for the composite applied to soybeans.

[0128] (11-2) SiO to cabbage ２ - Leaves of ABA-treated cabbage (variety: Harunami) 37 days after sowing were treated with water (control), 30 μM ABA, and SiO2 equivalent to 30 μM ABA. ２- An aqueous suspension of ABA was sprayed at a rate of 2 mL per plant. The experiment was conducted with n=3-4 plants. To check the stomatal open / closed state of each leaf after application, stomatal conductance was measured using a porometer 5 hours after application.

[0129] (11-3) SiO to soybeans ２ - Leaves of ABA-treated soybeans (variety: Fukuyutaka) 34 days after sowing were treated with water (control), 10 μM ABA peptide aqueous solution, and SiO2 equivalent to 10 μM ABA peptide. ２ - An aqueous suspension of ABA was sprayed at a rate of 5 mL per plant. The experiment was conducted with n=4-5 plants. To check the stomatal open / closed state of each leaf after application, stomatal conductance was measured using a porometer 2 hours after application.

[0130] The results are shown in Figure 22. Figure 22A shows the results of the stomatal closure test on cabbage, and Figure 22B shows the results of the stomatal closure test on soybeans. In both plants, applying SiO2 was more effective than applying ABA alone. ２ - It was confirmed that using ABA resulted in significantly lower stomatal conductance.

[0131] [Example 12] Iron oxide-gibberellate complex (Fe ２ O ３ -GA ３ ) Test on the effect of elongation of grass height (12-1) Fe ２ O ３ -GA ３ Preparation of Fe ２ O ３ The reagents are Fujifilm Wako Pure Chemical Industries (particle size 20-40 nm), gibberellic acid (GA ３ The reagents used were manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. Fe ２ O ３ The binding reaction of gibberellic acid was carried out by mixing in solution. Unless otherwise specified, the following tests were performed using GA. ３ The test was conducted under conditions of a concentration of 5.0 μM.

[0132] Prepared Fe ２ O ３ -GA ３ The results of the FT-IR analysis showed that GA ３We confirmed unique absorption, as well as absorption originating from C-O and C-H bonds. ２ O ３ and GA ３ It was confirmed that the two elements are chemically bonded and form a complex. Fe ２ O ３ -GA ３ The particle size was 413.2 ± 85.9 nm.

[0133] (12-2) Fe ２ O ３ -GA ３ Rice seeds (variety: Nipponbare) were sown in cell trays filled with black granular growing medium and cultivated for 20 days to grow the plants. 5.0 μM GA ３ solution, 5.0 μM GA ３ A considerable amount of Fe ２ O ３ -GA ３ The complex suspension was applied to the above-ground parts of the plant at a rate of 100 μL per plant. GA ３ Rice plants that were not treated were used as a control. The experiment was conducted with n=13 to 17. After application, the rice plants were grown for 20 days, and the height elongation of the rice plants before and after growth was measured.

[0134] The results are shown in Figure 23. Error bars in the figure indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to the Tukey test. 5.0 μM GA ３ Fe did not show a significant effect on the elongation of rice plants, but Fe ２ O ３ -GA ３ It was confirmed that this significantly increased the height of the plants.

[0135] [Example 13] Test of herbicidal effect of zinc compound-Glyp complex (13-1) Preparation of various zinc compound-Glyp complexes Zinc oxide-Glyp complex (ZnO-Glyp) was prepared in the same manner as in Example 1. Zinc fluoride (ZnF) was used instead of zinc oxide. ２ (Manufactured by Tokyo Chemical Industry Co., Ltd.), zinc phosphate tetrahydrate (Zn ３ (PO ４ ) ２ 4H ２ O, manufactured by Fujifilm Wako Pure Chemical Industries, Ltd., zinc sulfate heptahydrate (ZnSO4)４ 7H ２ Using O (manufactured by Nacalai Tesque), the zinc oxide was reacted with Glyp in the same way as with (ZnF ２ - Glyp, Zn ３ (PO ４ ) ２ -Glyp, ZnSO ４ -Glyp). ZnF ２ - Glyp, Zn ３ (PO ４ ) ２ -Glyp, ZnSO ４ Regarding Glyp, no chemical bond between the zinc compound and Glyp could be confirmed.

[0136] (13-2) Application of various zinc compound-Glyp complexes to *Lysimachia japonica* An application test of various zinc compound-Glyp complexes was conducted on *Lysimachia japonica* plants. The above-ground parts of various plants with a height of 7-12 cm were treated with water (control), 0.1% glyphosate aqueous solution (Glyp), and amounts of ZnO-Glyp and ZnF equivalent to 0.1% glyphosate. ２ - Glyp, Zn ３ (PO ４ ) ２ -Glyp, ZnSO ４ Each aqueous suspension of Glyp was applied to the plant at a rate of 200 μL / plant. The SPAD value was measured 4 days after application. Each test was conducted with n=8 to 10.

[0137] Figure 24 shows the SPAD values ​​of *Lysimachia japonica* under each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. It was confirmed that the SPAD values ​​of *Lysimachia japonica* after application of ZnO-Glyp were significantly lower compared to the control and Glyp. On the other hand, ZnF ２ - Glyp, Zn ３ (PO ４ ) ２ -Glyp, ZnSO ４ - The SPAD value of *Epipogium aquilinum* after Glyp application did not show a significant difference compared to Glyp application alone. Among the various zinc compounds, it was confirmed that oxides in particular enhanced the herbicidal effect of Glyp.

[0138] [Example 14] Weed Control Effect Test with Magnesium Compound-Glyp Complex (14-1) Preparation of Various Magnesium Compound-Glyp Complexes Magnesium oxide-Glyp complex (MgO-Glyp) was prepared in the same manner as in Example 4. Instead of magnesium oxide, magnesium metal (Mg, manufactured by Fujifilm Wako Pure Chemical Corporation), magnesium fluoride (MgF ２ , manufactured by Fujifilm Wako Pure Chemical Corporation), magnesium phosphate octahydrate (Mg ３ (PO ４ ) ２ ·8H ２ O, manufactured by Fujifilm Wako Pure Chemical Corporation), magnesium sulfate heptahydrate (MgSO ４ ·7H ２ O, manufactured by Fujifilm Wako Pure Chemical Corporation) were used, and each was reacted with Glyp in the same manner as magnesium oxide (Mg-Glyp, MgF ２ -Glyp, Mg ３ (PO ４ ) ２ -Glyp, MgSO ４ -Glyp). For Mg-Glyp, MgF ２ -Glyp, Mg ３ (PO ４ ) ２ -Glyp, MgSO ４ -Glyp, the chemical bond between the magnesium compound and Glyp could not be confirmed.

[0139] (14-2) Application of Various Magnesium Compound-Glyp Complexes to Minato Kamogusa A test of applying various magnesium compound-Glyp complexes to the plants of Minato Kamogusa was carried out. On the above-ground parts of various plants with an above-ground height of 10-12 cm, water (control), 0.1% glyphosate aqueous solution (Glyp), an amount of MgO-Glyp corresponding to 0.1% glyphosate, Mg-Glyp, MgF ２ -Glyp, Mg ３ (PO ４ ) ２ -Glyp, MgSO ４ -Glyp aqueous suspensions were applied so that the amount was 200 μL / plant. The SPAD value 5 days after spraying was measured. The test was carried out with n = 8-10 for each.

[0140] Figure 25 shows the SPAD values ​​of *Lindernia procumbens* under each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. It was confirmed that the SPAD values ​​of *Lindernia procumbens* after application of MgO-Glyp were significantly lower compared to the control and Glyp. On the other hand, Mg-Glyp and MgF ２ - Glyp, Mg ３ (PO ４ ) ２ -Glyp, MgSO ４ - The SPAD values ​​of *Epipogium aquilinum* after Glyp application did not show a significant difference compared to Glyp application alone.

[0141] [Example 15] Magnesium oxide-ammonium sulfate complex (MgO-(NH ４ ) ２ SO ４ Growth promotion test using (15-1) MgO-(NH ４ ) ２ SO ４ Preparation: MgO reagent (particle size 50 nm) was supplied by Fujifilm Wako Pure Chemical Industries, and ammonium sulfate was supplied by Ishizu Pharmaceutical Co., Ltd. The bonding reaction of MgO and ammonium sulfate was carried out by mixing in solution.

[0142] Prepared MgO-(NH ４ ) ２ SO ４ Analysis using FT-IR revealed shifts in the Mg-O and -OH spectra. This indicates that MgO and (NH ４ ) ２ SO ４ It was confirmed that the two chemically bonded and formed a complex. Using a DLS analyzer, MgO-(NH ４ ) ２ SO ４ The number-average particle size was measured. ４ ) ２ SO ４ The particle size was 696.9 ± 124.4 nm.

[0143] (15-2)MgO-(NH ４ ) ２ SO ４Application to rice plants: MgO-(NH ４ ) ２ SO ４ Application tests were conducted. Water (control), 1.0% ammonium sulfate aqueous solution, and an amount equivalent to 1.0% ammonium sulfate (MgO-(NH4)) were applied to the above-ground parts of each plant, which were 13-17 cm tall. ４ ) ２ SO ４ The aqueous suspension was applied to each plant at a rate of 150 μL / plant. The height increase of the plants was measured 7 days after application. Each experiment was conducted with n=18 to 20 plants.

[0144] Figure 26 shows the height increase of rice plants under each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to the Tukey test. Control and (NH ４ ) ２ SO ４ In comparison, MgO-(NH ４ ) ２ SO ４ A significant increase in the height of rice plants after application was confirmed.

[0145] [Example 16] Zinc oxide-boric acid (ZnO-H ３ BO ３ Boron introduction amount confirmation test by (x-1)ZnO-H ３ BO ３ For the preparation of the reagent, the ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the boric acid was manufactured by Nacalai Tesque. The bonding reaction of ZnO and boric acid was carried out by mixing in solution.

[0146] Prepared ZnO-H ３ BO ３ Analysis using FT-IR revealed that both ZnO and boric acid exhibited the same absorption, as well as absorption originating from the B-O bond. This indicates that ZnO and H ３ BO ３ It was confirmed that the two chemically bond and form a complex. Using a DLS analyzer, ZnO-H ３ BO ３ The number-average particle size of the prepared ZnO-H was measured. ３ BO ３ The particle size was 765.4 ± 166.0 nm.

[0147] (16-2) ZnO-H ３ BO ３ Application to soybeans: ZnO-H ３ BO ３ Application tests were conducted. On the above-ground parts of each plant 18 days after sowing, water (control), 0.1% boric acid aqueous solution, and an amount of ZnO-H equivalent to 0.1% boric acid were applied. ３ BO ３ The aqueous suspension was sprayed at a rate of 1 mL per plant. Plants were collected three days after spraying, and the boron content in the leaves was measured. Each experiment was conducted with n=4 to 5 plants.

[0148] (16-3) Leaves of plant bodies were collected after boron content analysis and thoroughly dried in an oven. Each dried sample was dissolved in nitric acid solution using a microwave decomposition system (Multiwave GO, Anton Paar). The supernatant after dissolution was subjected to an inductively coupled plasma atomic emission spectrometer (ICP9000, Shimadzu Corporation) to measure the boron content.

[0149] Figure 27 shows the boron content for each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Control and H ３ BO ３ In comparison, ZnO-H ３ BO ３ A significant increase in the boron content of soybean leaves after application was confirmed.

[0150] [Example 17] Zinc oxide disodium molybdate dihydrate (ZnO-Na ２ MoO ４ ・2H ２ O) Molybdenum introduction amount confirmation test (17-1) ZnO-Na ２ MoO ４ ・2H ２ Preparation of O: ZnO reagent (particle size 20 nm) and disodium molybdate dihydrate were manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The bonding reaction between ZnO and disodium molybdate dihydrate was carried out by mixing in solution.

[0151] Prepared ZnO-Na ２ MoO ４ ・2H ２ Analysis of O using FT-IR revealed that both ZnO and disodium molybdate dihydrate showed the same absorption, as well as absorption originating from the Mo-O bond. This indicates that ZnO and Na ２ MoO ４ ・2H ２ It was confirmed that O and the compound are chemically bonded and form a complex. Using a DLS analyzer, ZnO-Na ２ MoO ４ ・2H ２ The number-average particle size of O was measured. ２ MoO ４ ・2H ２ The particle size of O was 960.2 ± 196.9 nm.

[0152] (17-2) ZnO-Na ２ MoO ４ ・2H ２ Application of O to soybeans to wheat plants ZnO-Na ２ MoO ４ ・2H ２ An application test was conducted. Seven days after sowing, the above-ground parts of each plant were treated with water (control), a 0.1% disodium molybdate dihydrate aqueous solution, and an amount of ZnO-Na equivalent to 0.1% disodium molybdate dihydrate. ２ MoO ４ ・2H ２ A water suspension was sprayed at a rate of 500 μL per plant. Plants were collected two days after spraying, and the molybdenum content in the above-ground parts was measured. Each experiment was conducted with n=8 to 16.

[0153] (17-3) Plant specimens were collected after the molybdenum content analysis treatment and thoroughly dried in an oven. Each dried sample was dissolved in nitric acid solution using a microwave decomposition system (Multiwave GO, Anton Paar). The supernatant after dissolution was subjected to an inductively coupled plasma atomic emission spectrometer (ICP9000, Shimadzu Corporation) to measure the molybdenum content.

[0154] Figure 28 shows the molybdenum content for each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Control and Na ２ MoO ４ ・2H ２ Compared to O, ZnO-Na ２ MoO ４ ・2H ２ It was confirmed that the molybdenum content of wheat significantly increased after application of O.

[0155] [Example 18] Zinc oxide-glucose (ZnO-C ６ H １２ O ６ Growth promotion effect test by (18-1) ZnO-C ６ H １２ O ６ For the preparation of the reagent, ZnO reagent (particle size 20 nm) was supplied by Fujifilm Wako Pure Chemical Industries, and glucose was supplied by Katayama Chemical Industries. The bonding reaction between ZnO and glucose was carried out by mixing in solution.

[0156] Prepared ZnO-C ６ H １２ O ６ Analysis using FT-IR revealed that both ZnO and glucose exhibited the same absorption, as well as absorption originating from C-O and C-H bonds. ６ H １２ O ６ It was confirmed that the two chemically bond and form a complex. Using a DLS analyzer, ZnO-C ６ H １２ O ６ The number-average particle size of the prepared ZnO-C was measured. ６ H １２ O ６ The particle sizes were 726.2 ± 166.3 nm and 714.4 ± 171.2 nm.

[0157] (18-2) ZnO-C ６ H １２ O ６ Application of ZnO-C to wheat plants ６ H １２ O ６Application tests were conducted. On the above-ground parts of each plant 12 and 19 days after sowing, water (control), 1.0% glucose acid solution, and ZnO-C equivalent to 1.0% glucose were applied. ６ H １２ O ６ The aqueous suspension was sprayed at a rate of 500 μL per plant. The SPAD value of the plant leaves was measured 6 days after the second spraying. Each experiment was conducted with n=18 to 19 participants.

[0158] Figure 29 shows the SPAD values ​​for each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. ６ H １２ O ６ In comparison, ZnO-C ６ H １２ O ６ A significant increase in the SPAD value of wheat after application was confirmed.

[0159] [Example 19] Zinc oxide-trehalose (ZnO-C １２ H ２２ O １１ Growth maintenance effect test by (19-1) ZnO-C １２ H ２２ O １１ For the preparation of the reagent, the ZnO reagent (particle size 20 nm) was supplied by Fujifilm Wako Pure Chemical Industries, and the trehalose was supplied by Hayashibara Biochemical Co., Ltd. The binding reaction of ZnO and trehalose was carried out by mixing in solution.

[0160] Prepared ZnO-C １２ H ２２ O １１ Analysis using FT-IR revealed that both ZnO and trehalose exhibited the same absorption, as well as absorption originating from C-O and C-H bonds. １２ H ２２ O １１ It was confirmed that the two chemically bond and form a complex. Using a DLS analyzer, ZnO-C １２ H ２２ O １１ The number-average particle size of the prepared ZnO-C was measured. １２ H ２２ O１１ The particle size was 1093.3 ± 221.1 nm.

[0161] (19-2) ZnO-C １２ H ２２ O １１ Application to wheat: C １２ H ２２ O １１ Application tests were conducted. On the above-ground parts of each plant 15 days after sowing, water (control), a 0.1% trehalose aqueous solution, and an amount of ZnO-C equivalent to 0.1% trehalose were applied. １２ H ２２ O １１ The aqueous suspension was sprayed at a rate of 500 μL per plant. Plants were collected 13 days after spraying, and the fresh weight of the above-ground parts was measured. Water was withheld for two days after the solution treatment. Each experiment was conducted with n=11 to n=12.

[0162] Figure 30 shows the fresh above-ground weight for each condition. Error bars indicate the standard deviation. The asterisk (*) in the figure indicates that there is a statistically significant difference between the treatment intervals at the 5% level, as determined by a t-test. １２ H ２２ O １１ In comparison, ZnO-C １２ H ２２ O １１ A significant increase in the fresh weight of the above-ground parts of wheat was confirmed after application.

[0163] [Example 20] Zinc oxide-D(+)-raffinose pentahydrate (ZnO-C １８ H ３２ O １６ ・5H ２ Growth maintenance effect test by (20-1) ZnO-C １８ H ３２ O １６ ・5H ２ Preparation of O: ZnO reagent (particle size 20 nm) was supplied by Fujifilm Wako Pure Chemical Industries, and D(+)-raffinose pentahydrate was supplied by Fujifilm Wako Pure Chemical Industries. The bonding reaction of ZnO and D(+)-raffinose pentahydrate was carried out by mixing in solution.

[0164] Prepared ZnO-C １８ H ３２ O １６ ・5H２ Analysis of O using FT-IR revealed that both ZnO and D(+)-raffinose pentahydrate exhibited the same absorption, as well as absorption originating from the C-O bond. １８ H ３２ O １６ ・5H ２ It was confirmed that O and ZnO chemically bonded, forming a complex. Using a DLS analyzer, ZnO-C １８ H ３２ O １６ ・5H ２ The number-average particle size of O was measured. １８ H ３２ O １６ ・5H ２ The particle size of O was 1227.5 ± 276.3 nm.

[0165] (20-2) ZnO-C １８ H ３２ O １６ ・5H ２ Application of O to wheat to the wheat plant body C １８ H ３２ O １６ ・5H ２ An application test was conducted. Eight days after sowing, the above-ground parts of each plant were treated with water (control), a 10% D(+)-raffinose pentahydrate aqueous solution, and an amount of ZnO-C equivalent to 10% D(+)-raffinose pentahydrate. １８ H ３２ O １６ ・5H ２ A water suspension was sprayed at a rate of 500 μL per plant. Plants were collected 13 days after spraying, and the fresh weight of the above-ground parts was measured. No irrigation was performed between solution treatment and plant collection. Each experiment was conducted with n=30 to 35 participants.

[0166] Figure 31 shows the above-ground fresh weight for each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Control and C １８ H ３２ O １６ ・5H ２ Compared to O, ZnO-C １８ H ３２ O １６ ・5H ２It was confirmed that the fresh weight of the above-ground parts of wheat increased significantly after application of O.

[0167] [Example 21] Zinc oxide-alginate (ZnO-(C) ６ H ８ O ６ ) ｎ Growth maintenance effect test by (21-1)ZnO-(C ６ H ８ O ６ ) ｎ Preparation: The ZnO reagent (particle size 20 nm) and alginic acid were both manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The bonding reaction between ZnO and alginic acid was carried out by mixing in solution.

[0168] Prepared ZnO-(C ６ H ８ O ６ ) ｎ Analysis using FT-IR revealed that both ZnO and alginate showed the same absorption, as well as absorption originating from C-O and C=O bonds. This indicates that ZnO and (C ６ H ８ O ６ ) ｎ It was confirmed that the two are chemically bonded and form a complex. Using a DLS analyzer, ZnO-(C ６ H ８ O ６ ) ｎ The number-average particle size of the prepared ZnO-(C) was measured. ６ H ８ O ６ ) ｎ The particle size was 1119.8 ± 278.1 nm.

[0169] (21-2) ZnO-(C ６ H ８ O ６ ) ｎ Application to barley to the barley plant body (C ６ H ８ O ６ ) ｎ Application tests were conducted. Eight days after sowing, the above-ground parts of each plant were treated with water (control), a 1.0% alginic acid aqueous solution, and an amount of ZnO-(C) equivalent to 1.0% alginic acid. ６ H ８ O ６ )ｎ The aqueous suspension was sprayed at a rate of 300 μL per plant. Plants were collected 15 days after spraying, and the fresh weight of the above-ground parts was measured. No irrigation was performed between solution treatment and plant collection. Each experiment was conducted with n=24 to 25.

[0170] Figure 32 shows the fresh above-ground weight for each condition. Error bars indicate the standard deviation. In the figure, "**" and "*" indicate that there is a significant difference between the treatment intervals at the 1% and 5% levels, respectively, as determined by t-tests. Control and (C ６ H ８ O ６ ) ｎ In comparison, ZnO-(C ６ H ８ O ６ ) ｎ A significant increase in the fresh weight of the above-ground parts of barley was confirmed after application.

[0171] [Example 22] Zinc oxide-glycine betaine (ZnO-C ５ H １１ NO ２ Growth maintenance effect test by (22-1) ZnO-C ５ H １１ NO ２ Preparation: The ZnO reagent (particle size 20 nm) and glycine betaine were manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The bonding reaction of ZnO and glycine betaine was carried out by mixing in solution.

[0172] Prepared ZnO-C ５ H １１ NO ２ Analysis using FT-IR revealed that both ZnO and glycine betaine exhibited the same absorption, as well as absorption originating from the C=O bond. ５ H １１ NO ２ It was confirmed that the two chemically bond and form a complex. Using a DLS analyzer, ZnO-C ５ H １１ NO ２ The number-average particle size of the prepared ZnO-C was measured. ５ H １１ NO ２The particle size was 483.1 ± 133.0 nm.

[0173] (22-2) ZnO-C ５ H １１ NO ２ Application to wheat: C ５ H １１ NO ２ Application tests were conducted. Seven days after sowing, the above-ground parts of each plant were treated with water (control), 1.0% glycine betaine aqueous solution, 1.0% glycine betaine, and ZnO-C equivalent to 0.05 mg / mL. ５ H １１ NO ２ The aqueous suspension was sprayed at a rate of 500 μL per plant. Plants were collected 14 days after spraying, thoroughly dried in an oven, and the dry weight of the above-ground parts was measured. Water was withheld for 3 days after the solution treatment. Each experiment was conducted with n=10.

[0174] Figure 33 shows the above-ground dry weight for each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Compared to the control, ZnO-C ５ H １１ NO ２ A significant increase in the dry weight of the above-ground parts of wheat was confirmed after application.

[0175] [Example 23] Zinc oxide-glutamic acid (ZnO-C ５ H ９ NO ４ Growth promotion effect test by (23-1) ZnO-C ５ H ９ NO ４ Preparation: The ZnO reagent (particle size 20 nm) and glutamic acid were both manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The binding reaction between ZnO and glutamic acid was carried out by mixing in solution.

[0176] Prepared ZnO-C ５ H ９ NO ４ Analysis using FT-IR revealed that both ZnO and glutamic acid exhibited the same absorption, as well as absorption originating from the C=O bond. ５ H ９NO ４ It was confirmed that the two chemically bond and form a complex. Using a DLS analyzer, ZnO-C ５ H ９ NO ４ The number-average particle size of the prepared ZnO-C was measured. ５ H ９ NO ４ The particle sizes were 774.7 ± 191.6 nm and 620.1 ± 111.3 nm.

[0177] (23-2) ZnO-C ５ H ９ NO ４ Application to wheat: C ５ H ９ NO ４ Application tests were conducted. On the above-ground parts of each plant 6 and 13 days after sowing, water (control), 0.01% glutamic acid aqueous solution, and ZnO-C equivalent to 0.01% glutamic acid were applied. ５ H ９ NO ４ A water suspension was sprayed at a rate of 500 μL per plant. Plants were collected 7 days after the second spraying, thoroughly dried in an oven, and the dry weight of the underground parts was measured. Each experiment was conducted with 4 individuals as one replicate, with n=4 to 5.

[0178] Figure 34 shows the dry weight of the underground portion under each condition. Error bars indicate the standard deviation. The asterisk (*) in the figure indicates that there is a statistically significant difference between the treatment intervals at the 5% level, as determined by a t-test. ５ H ９ NO ４ In comparison, ZnO-C ５ H ９ NO ４ A significant increase in the dry weight of the underground parts of wheat was confirmed after application.

[0179] [Example 24] Zinc oxide-glutamine (ZnO-C ５ H １０ N ２ O ３ Growth promotion effect test by (24-1) ZnO-C ５ H １０ N ２ O ３Preparation: The ZnO reagent (particle size 20 nm) and glutamine were manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The binding reaction of ZnO and glutamine was carried out by mixing in solution.

[0180] Prepared ZnO-C ５ H １０ N ２ O ３ Analysis using FT-IR revealed that both ZnO and glutamine exhibited the same absorption, as well as absorption originating from the C=O bond. ５ H １０ N ２ O ３ It was confirmed that the two chemically bond and form a complex. Using a DLS analyzer, ZnO-C ５ H １０ N ２ O ３ The number-average particle size of the prepared ZnO-C was measured. ５ H １０ N ２ O ３ The particle sizes were 634.9 ± 148.3 nm and 911.6 ± 209.7 nm.

[0181] (24-2) ZnO-C ５ H １０ N ２ O ３ Application to wheat: C ５ H １０ N ２ O ３ Application tests were conducted. On the above-ground parts of each plant 8 and 15 days after sowing, water (control), 0.02% glutamine aqueous solution, and 0.02% glutamine equivalent amount of ZnO-C were applied. ５ H １０ N ２ O ３ A water suspension was sprayed at a rate of 500 μL per plant. Six days after the second spraying, plant bodies were collected, thoroughly dried in an oven, and the dry weight of the underground parts was measured. Each experiment was conducted with 4 plants as one replicate, with n=3 to 5.

[0182] Figure 35 shows the dry weight of the underground portion under each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Control and C ５ H １０ N ２ O ３ In comparison, ZnO-C ５ H １０ N ２ O ３ A significant increase in the dry weight of the underground parts of wheat was confirmed after application.

[0183] [Example 25] Zinc oxide-arginine (ZnO-C ６ H １４ N ４ O ２ Growth promotion effect test by (25-1) ZnO-C ６ H １４ N ４ O ２ For the preparation of the reagent, the ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the arginine was manufactured by Nacalai Tesque. The binding reaction of ZnO and arginine was carried out by mixing in solution.

[0184] Prepared ZnO-C ６ H １４ N ４ O ２ Analysis using FT-IR revealed that both ZnO and arginine exhibited the same absorption, as well as absorption originating from the C=O bond. ６ H １４ N ４ O ２ It was confirmed that the two chemically bond and form a complex. Using a DLS analyzer, ZnO-C ６ H １４ N ４ O ２ The number-average particle size of the prepared ZnO-C was measured. ６ H １４ N ４ O ２ The particle sizes were 810.0 ± 200.3 nm and 992.8 ± 234.3 nm.

[0185] (25-2) ZnO-C ６ H １４ N４ O ２ Application to wheat: C ６ H １４ N ４ O ２ Application tests were conducted. On the above-ground parts of each plant 8 and 13 days after sowing, water (control), a 0.02% arginine aqueous solution, and an amount of ZnO-C equivalent to 0.02% arginine were applied. ６ H １４ N ４ O ２ A water suspension was sprayed at a rate of 500 μL per plant. Plants were collected 9 days after the second spraying, thoroughly dried in an oven, and the dry weight of the underground parts was measured. Each experiment was conducted with 4 individuals as one replicate, with n=4 to 5.

[0186] Figure 36 shows the dry weight of the underground portion under each condition. Error bars indicate the standard deviation. The asterisk (*) in the figure indicates that there is a statistically significant difference between the treatment intervals at the 5% level, as determined by a t-test. ６ H １４ N ４ O ２ In comparison, ZnO-C ６ H １４ N ４ O ２ A significant increase in the dry weight of the underground parts of wheat was confirmed after application.

[0187] [Example 26] Mineral absorption test using zinc oxide-fulvic acid (26-1) Preparation of ZnO-fulvic acid The ZnO reagent (particle size 20 nm) and fulvic acid were manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The bonding reaction of ZnO and fulvic acid was carried out by mixing in solution.

[0188] Analysis of the prepared ZnO-fulvic acid by FT-IR revealed that both ZnO and fulvic acid exhibited the same absorption, as well as absorption originating from C-O and C=O bonds. This confirmed that ZnO and fulvic acid were chemically bonded, forming a complex. The number-average particle size of the ZnO-fulvic acid was measured using a DLS analyzer. The particle sizes of the prepared ZnO-fulvic acid were 424.2 ± 110.3 nm (0.05% fulvic acid) and 442.5 ± 129.9 nm (0.2% fulvic acid).

[0189] (26-2) Application of ZnO-fulvic acid to wheat A study was conducted on wheat plants to test the application of ZnO-fulvic acid. Eight days after sowing, 500 μL of water (control), 0.05% fulvic acid solution, 0.2% fulvic acid solution, ZnO suspension, ZnO-fulvic acid aqueous suspension equivalent to 0.05% fulvic acid, and ZnO-fulvic acid aqueous suspension equivalent to 0.2% fulvic acid were sprayed onto the above-ground parts of each plant. Plants were collected 12 days after spraying, and the magnesium and zinc content in the above-ground parts was measured. The tests were conducted with n=7 to 16 each.

[0190] (26-3) Plant specimens were collected after analysis for magnesium and zinc content and thoroughly dried in an oven. Each dried sample was dissolved in nitric acid solution using a microwave decomposition system (Multiwave GO, Anton Paar). The supernatant after dissolution was subjected to an inductively coupled plasma atomic emission spectrometer (ICP9000, Shimadzu Corporation) to measure the content of each element.

[0191] Figure 37A shows the magnesium content for each condition. Error bars indicate the standard deviation. "***" and "**" in the figure indicate that there is a significant difference between the treatment intervals at the 0.1% and 1% levels, respectively, as determined by t-tests. It was confirmed that the magnesium content of wheat after application of ZnO-fulvic acid was significantly increased compared to the control and fulvic acid.

[0192] Figure 37B shows the zinc content under each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Compared to the control and ZnO and fulvic acid, a significant increase in the zinc content of wheat after application of ZnO-fulvic acid was confirmed.

[0193] [Example 27] Growth-promoting effect test of zinc oxide-fulvic acid (27-1) Preparation of ZnO-fulvic acid The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the fulvic acid was manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The bonding reaction of ZnO and fulvic acid was carried out by mixing in solution.

[0194] Analysis of the prepared ZnO-fulvic acid by FT-IR revealed that both ZnO and fulvic acid exhibited the same absorption, as well as absorption originating from C-O and C=O bonds. This confirmed that ZnO and fulvic acid were chemically bonded, forming a complex. The number-average particle size of the ZnO-fulvic acid was measured using a DLS analyzer. The particle size of the prepared ZnO-fulvic acid was 603.0 ± 143.0 nm.

[0195] (27-2) Application of ZnO-fulvic acid to soybeans An application test of ZnO-fulvic acid was conducted on soybean plants. Nineteen days after sowing, water (control), a 0.05% fulvic acid solution, and a ZnO-fulvic acid aqueous suspension equivalent to 0.05% fulvic acid were sprayed onto the above-ground parts of each plant at a rate of 1 mL / plant. Plants were collected 16 days after spraying, thoroughly dried in an oven, and the dry weight of the above-ground parts was measured. Each test was conducted with n=9 to 10.

[0196] Figure 38 shows the above-ground dry weight for each condition. Error bars indicate the standard deviation. "**" and "*" in the figure indicate that there is a significant difference between the treatment intervals at the 1% and 5% levels, respectively, as determined by t-tests. It was confirmed that the above-ground dry weight of soybeans increased significantly after application of ZnO-fulvic acid compared to the control and fulvic acid.

[0197] [Example 28] Test of herbicidal effect of zinc oxide-paraquat complex (ZnO-Paraquat) (28-1) Preparation of ZnO-Paraquat ZnO reagent (particle size 20 nm) was used, and paraquat was manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.

[0198] Analysis of the prepared ZnO-Paraquat by FT-IR revealed no binding between ZnO and paraquat. The number-average particle size of the ZnO-Paraquat was measured using a DLS analyzer. The particle size of the prepared ZnO-Paraquat was 1087.5 ± 230.1 nm.

[0199] (28-2) Application of ZnO-Paraquat to Lathyrus japonica An application test of ZnO-Paraquat was conducted on Lathyrus japonica plants. 44 days after sowing, 100 μL / plant was applied to the above-ground parts of each plant: water (control), a 0.01% paraquat aqueous solution, and a ZnO-Paraquat aqueous suspension equivalent to 0.01% paraquat. The SPAD value was measured 8 days after application. Each test was conducted with n=8 to 9 plants.

[0200] Figure 39 shows the SPAD values ​​of *Lindernia procumbens* under each condition. Error bars indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. It was confirmed that the SPAD values ​​of *Lindernia procumbens* after application of ZnO-Paraquat were significantly lower compared to the control and Paraquat.

[0201] [Example 29] Herbicidal efficacy test using zinc oxide-2,4-dichlorophenoxyacetic acid complex (ZnO-2,4-D) (29-1) Preparation of ZnO-2,4-D The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, Ltd., and the 2,4-dichlorophenoxyacetic acid was manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The binding reaction of ZnO and 2,4-dichlorophenoxyacetic acid was carried out by mixing in solution.

[0202] Analysis of the prepared ZnO-2,4-D by FT-IR revealed that both ZnO and 2,4-dichlorophenoxyacetic acid exhibited the same absorption, as well as absorption originating from C-H and C=C bonds. This confirmed that ZnO and 2,4-dichlorophenoxyacetic acid were chemically bonded, forming a complex. The number-average particle size of ZnO-2,4-D was measured using a DLS analyzer. The particle size of the prepared ZnO-2,4-D was 792.9 ± 175.8 nm.

[0203] (29-2) Application of ZnO-2,4-D to clover An application test of ZnO-2,4-D was conducted on clover plants. On the above-ground parts of each plant 24 days after sowing, 1 mL / 25 cm was applied to a 0.01% aqueous solution of 2,4-dichlorophenoxyacetic acid and an aqueous suspension of ZnO-2,4-D equivalent to 0.01% 2,4-dichlorophenoxyacetic acid. ２The plants were sprayed in this manner. The mortality rate was measured 8 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=4 to 5 plants.

[0204] Figure 40 shows the clover mortality rate under each condition. Error bars indicate the standard deviation. "***" in the figure indicates a statistically significant difference between the treatment intervals at the 0.1% level, as determined by Student's t-test. It was confirmed that the clover mortality rate increased significantly after application of ZnO-2,4-D compared to 2,4-D.

[0205] [Example 30] Test of herbicidal effect of zinc oxide-dicamba complex (ZnO-dicamba) (30-1) Preparation of ZnO-dicamba The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the dicamba was manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The binding reaction of ZnO and dicamba was carried out by mixing in solution.

[0206] Analysis of the prepared ZnO-dicamba by FT-IR revealed that both ZnO and dicamba exhibited the same absorption, as well as absorption originating from C-H and C-O bonds. This confirmed that ZnO and dicamba were chemically bonded, forming a complex. The number-average particle size of the ZnO-dicamba was measured using a DLS analyzer. The particle size of the prepared ZnO-dicamba was 739.4 ± 169.6 nm.

[0207] (30-2) Application of ZnO-dicamba to clover An application test of ZnO-dicamba was conducted on clover plants. 24 days after sowing, 1 mL / 25 cm was applied to the above-ground parts of each plant to a 0.01% dicamba aqueous solution and a ZnO-dicamba aqueous suspension equivalent to 0.01% dicamba. ２ The plants were sprayed in this manner. The mortality rate was measured 11 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=4 to 5 plants.

[0208] Figure 41 shows the clover mortality rates under each condition. Error bars indicate the standard deviation. "***" in the figure indicates a statistically significant difference between the treatment intervals at the 0.1% level, as determined by Student's t-test. It was confirmed that the clover mortality rate increased significantly after application of ZnO-dicamba compared to dicamba.

[0209] [Example 31] Test of herbicidal effect of zinc oxide-DCMU wettable powder complex (ZnO-DCMU) (31-1) Preparation of ZnO-DCMU The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the DCMU wettable powder was manufactured by ADAMA (Carmex granular wettable powder). The binding reaction of ZnO and DCMU wettable powder was carried out by mixing in solution.

[0210] Analysis of the prepared ZnO-DCMU by FT-IR revealed that both ZnO and DCMU exhibited the same absorption, as well as absorptions originating from C-O and C-H bonds. This confirmed that ZnO and DCMU were chemically bonded, forming a complex. The number-average particle size of the ZnO-DCMU was measured using a DLS analyzer. The particle size of the prepared ZnO-DCMU was 678.2 ± 103.3 nm.

[0211] (31-2) Application of ZnO-DCMU to clover An application test of ZnO-DCMU was conducted on clover plants. 29 days after sowing, 1 mL / 25 cm was applied to the above-ground parts of each plant to either a 0.16% DCMU aqueous solution or a ZnO-DCMU aqueous suspension equivalent to 0.16% DCMU. ２ The plants were sprayed in this manner. The mortality rate was measured 14 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=4 to 5 plants.

[0212] Figure 42 shows the clover mortality rate under each condition. Error bars indicate the standard deviation. "***" in the figure indicates a statistically significant difference between the treatment intervals at the 0.1% level, as determined by Student's t-test. It was confirmed that the clover mortality rate increased significantly after application of ZnO-DCMU compared to DCMU.

[0213] [Example 32] Test of herbicidal effect of zinc oxide-tepraloxidime complex (ZnO-tepraloxidime) (32-1) Preparation of ZnO-tepraloxidime The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, Ltd., and the tepraloxidime was manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The binding reaction of ZnO and tepraloxidime was carried out by mixing in solution.

[0214] Analysis of the prepared ZnO-tepraloxidium by FT-IR revealed that both ZnO and tepraloxidium exhibited the same absorption, as well as absorption originating from the C=O bond. This confirmed that ZnO and tepraloxidium were chemically bonded, forming a complex. The number-average particle size of the ZnO-tepraloxidium was measured using a DLS analyzer. The particle size of the prepared ZnO-tepraloxidium was 457.8 ± 111.5 nm.

[0215] (32-2) Application of ZnO-tepraloxidim to Goosegrass A test of application of ZnO-tepraloxidim to goosegrass plants was conducted. On the above-ground parts of each plant 18 days after sowing, 2 mL / 25 cm was applied to a 0.1% tepraloxidim aqueous solution and a ZnO-tepraloxidim aqueous suspension equivalent to 0.1% tepraloxidim. ２ The plants were sprayed in this manner. The mortality rate was measured 11 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=3.

[0216] Figure 43 shows the mortality rate of goosegrass under each condition. Error bars indicate the standard deviation. The asterisk (*) in the figure indicates a statistically significant difference between the treatment groups at the 5% level, as determined by Student's t-test. It was confirmed that the mortality rate of goosegrass increased significantly after application of ZnO-tepraloxidim compared to tepraloxidim.

[0217] [Example 33] Herbicidal efficacy test using zinc oxide-alachlor emulsion complex (ZnO-alachlor) (33-1) Preparation of ZnO-alachlor The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the alachlor emulsion was manufactured by Nippon Soda Co., Ltd. (Nichinou Lasso Emulsion). The binding reaction of ZnO and alachlor emulsion was carried out by mixing in solution.

[0218] Analysis of the prepared ZnO-alachlor by FT-IR revealed that both ZnO and alachlor exhibited the same absorption, as well as absorption originating from the C-H bond. This confirmed that ZnO and alachlor were chemically bonded, forming a complex. The number-average particle size of the ZnO-alachlor was measured using a DLS analyzer. The particle size of the prepared ZnO-alachlor was 594.9 ± 164.5 nm.

[0219] (33-2) Application of ZnO-alachlor to Goosegrass A ZnO-alachlor application test was conducted on goosegrass plants. Ten days after sowing, a 0.043% alachlor aqueous solution or a ZnO-alachlor aqueous suspension equivalent to 0.043% alachlor was sprayed onto the above-ground parts of each plant at a rate of 100 μL / plant. The mortality rate was measured 40 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each test was conducted with n=4.

[0220] Figure 44 shows the mortality rates of goosegrass under each condition. Error bars indicate the standard deviation. "**" in the figure indicates a statistically significant difference between the treatment groups at the 1% level, as determined by Student's t-test. It was confirmed that the mortality rate of goosegrass increased significantly after application of ZnO-alachlor compared to alachlor.

[0221] [Example 34] Herbicidal efficacy test using zinc oxide-oxadiclomefon wettable powder complex (ZnO-oxadiclomefon) (34-1) Preparation of ZnO-oxadiclomefon The ZnO reagent (particle size 20 nm) used was Fujifilm Wako Pure Chemical Industries, Ltd., and the oxadiclomefon wettable powder was manufactured by EnviroScience Japan, Inc. (Full House Turf Flowable). The binding reaction of ZnO and oxadiclomefon wettable powder was carried out by mixing in solution.

[0222] Analysis of the prepared ZnO-oxadichromefone by FT-IR revealed that both ZnO and oxadichromefone exhibited the same absorption, as well as absorptions originating from C-H, C=C, and C=O bonds. This confirmed that ZnO and oxadichromefone were chemically bonded, forming a complex. The number-average particle size of ZnO-oxadichromefone was measured using a DLS analyzer. The particle size of the prepared ZnO-oxadichromefone was 395.1 ± 91.3 nm.

[0223] (34-2) Application of ZnO-oxadiclomefone to Goosegrass A test of ZnO-oxadiclomefone application was conducted on goosegrass plants. On the above-ground parts of each plant 14 days after sowing, 2 mL / 25 cm was applied to the 0.03% oxadiclomefone aqueous solution and an equivalent amount of ZnO-oxadiclomefone aqueous suspension. ２ The plants were sprayed in this manner. The mortality rate was measured 15 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=4.

[0224] Figure 45 shows the mortality rates of goosegrass under each condition. Error bars indicate the standard deviation. The asterisk (*) in the figure indicates a statistically significant difference between the treatment groups at the 5% level, as determined by Student's t-test. It was confirmed that the mortality rate of goosegrass increased significantly after application of ZnO-oxadiclomefone compared to oxadiclomefone.

[0225] [Example 35] Herbicidal efficacy test using zinc oxide-penoxthlam wettable powder complex (ZnO-penoxthlam) (35-1) Preparation of ZnO-penoxthlam The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the penoxthlam wettable powder was manufactured by Corteva Japan (Wide Attack SC). The binding reaction of ZnO and penoxthlam wettable powder was carried out by mixing in solution.

[0226] Analysis of the prepared ZnO-penox slam by FT-IR revealed that both ZnO and penox slam exhibited the same absorption, as well as absorptions originating from C-H and C-F bonds. This confirmed that ZnO and penox slam were chemically bonded, forming a complex. The number-average particle size of the ZnO-penox slam was measured using a DLS analyzer. The particle size of the prepared ZnO-penox slam was 842.6 ± 159.1 nm.

[0227] (35-2) Application of ZnO-Penokislam to Clover A ZnO-Penokislam application experiment was conducted on clover plants. On the above-ground parts of each plant 21 days after sowing, 2 mL / 25 cm was applied to the 0.0018% Penokislam aqueous solution and a ZnO-Penokislam aqueous suspension equivalent to 0.0018% Penokislam. ２The plants were sprayed in this manner. The mortality rate was measured 9 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=4 to 5 plants.

[0228] Figure 46 shows the clover mortality rate under each condition. Error bars indicate the standard deviation. "***" in the figure indicates a statistically significant difference between the treatment intervals at the 0.1% level, as determined by Student's t-test. It was confirmed that the clover mortality rate increased significantly after application of ZnO-penokislam compared to penokislam.

[0229] [Example 36] Test of herbicidal effect of zinc oxide-IPC emulsion complex (ZnO-IPC) (36-1) Preparation of ZnO-IPC The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, Ltd., and the IPC emulsion was manufactured by Ishihara Bioscience Co., Ltd. (ChloroIPC "Ishihara"). The binding reaction of ZnO and IPC emulsion was carried out by mixing in solution.

[0230] Analysis of the prepared ZnO-IPC by FT-IR revealed that both ZnO and IPC exhibited the same absorption, as well as absorptions originating from C-O, C=C, and C=O bonds. This confirmed that ZnO and IPC were chemically bonded, forming a complex. The number-average particle size of the ZnO-IPC was measured using a DLS analyzer. The particle size of the prepared ZnO-IPC was 359.5 ± 107.2 nm.

[0231] (36-2) Application of ZnO-IPC to clover An application test of ZnO-IPC was conducted on clover plants. 21 days after sowing, 2 mL / 25 cm was applied to the above-ground parts of each plant to either a 0.458% IPC aqueous solution or a ZnO-IPC aqueous suspension equivalent to 0.458% IPC. ２ The plants were sprayed in this manner. The mortality rate was measured 22 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=4.

[0232] Figure 47 shows the clover mortality rate under each condition. Error bars indicate the standard deviation. The asterisk (*) in the figure indicates a statistically significant difference between the treatment intervals at the 5% level, as determined by Student's t-test. Compared to IPC, a significant increase in clover mortality was confirmed after application of ZnO-IPC.

[0233] [Example 37] Herbicidal efficacy test using zinc oxide-bentazone wettable powder complex (ZnO-bentazone) (37-1) Preparation of ZnO-bentazone The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the bentazone wettable powder was manufactured by Sumitomo Chemical Co., Ltd. (Basagran liquid formulation). The binding reaction of ZnO and bentazone wettable powder was carried out by mixing in solution.

[0234] Analysis of the prepared ZnO-bentazone by FT-IR revealed that both ZnO and bentazone exhibited the same absorption, as well as absorption originating from the C=C bond. This confirmed that ZnO and bentazone were chemically bonded, forming a complex. The number-average particle size of ZnO-bentazone was measured using a DLS analyzer. The particle size of the prepared ZnO-bentazone was 1351.3 ± 287.8 nm.

[0235] (37-2) Application of ZnO-bentazone to clover An application test of ZnO-bentazone was conducted on clover plants. 2 mL / 25 cm was applied to the above-ground parts of each plant 20 days after sowing, using either a 0.04% bentazone aqueous solution or a ZnO-bentazone aqueous suspension equivalent to 0.04% bentazone. ２ The plants were sprayed in this manner. The mortality rate was measured 23 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=4 to 5 plants.

[0236] Figure 48 shows the clover mortality rate under each condition. Error bars indicate the standard deviation. The asterisk (*) in the figure indicates a statistically significant difference between the treatment intervals at the 5% level, as determined by Student's t-test. Compared to bentazone, the clover mortality rate after application of ZnO-bentazone was confirmed to be significantly higher.

[0237] [Example 38] Test of herbicidal effect of zinc oxide-endotar monohydrate complex (ZnO-endotar) (38-1) Preparation of ZnO-endotar The ZnO reagent (particle size 20 nm) was supplied by Fujifilm Wako Pure Chemical Industries, and the endotar monohydrate was supplied by Fujifilm Wako Pure Chemical Industries, Ltd. The bonding reaction of ZnO and endotar monohydrate was carried out by mixing in solution.

[0238] Analysis of the prepared ZnO-endotar by FT-IR revealed that both ZnO and endotar monohydrate exhibited the same absorption, as well as absorption originating from the C-O bond. This confirmed that ZnO and endotar monohydrate were chemically bonded, forming a complex. The number-average particle size of the ZnO-endotar was measured using a DLS analyzer. The particle size of the prepared ZnO-endotar was 633.6 ± 144.9 nm.

[0239] (38-2) Application of ZnO-endotar to clover An application test of ZnO-endotar was conducted on clover plants. On the above-ground parts of each plant 15 days after sowing, 2 mL / 25 cm was applied to the 0.003% endotar monohydrate aqueous solution and an amount of ZnO-endotar aqueous suspension equivalent to 0.003% endotar monohydrate. ２ The plants were sprayed in this manner. The mortality rate was measured two days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=4.

[0240] Figure 49 shows the clover mortality rate under each condition. Error bars indicate the standard deviation. The asterisk (*) in the figure indicates a statistically significant difference between the treatment groups at the 5% level, as determined by Student's t-test. It was confirmed that the clover mortality rate increased significantly after application of ZnO-endotar compared to endotar.

[0241] [Example 39] Test of herbicidal effect of zinc oxide-mesotrione complex (ZnO-mesotrione) (39-1) Preparation of ZnO-mesotrione The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the mesotrione was manufactured by Tokyo Chemical Industries, Ltd. The binding reaction of ZnO and mesotrione was carried out by mixing in solution.

[0242] Analysis of the prepared ZnO-mesotriones using FT-IR revealed that both ZnO and mesotrione exhibited the same absorption, as well as absorption originating from the C=O and S=O bonds. This confirmed that ZnO and mesotrione were chemically bonded, forming a complex. The number-average particle size of the ZnO-mesotriones was measured using a DLS analyzer. The particle size of the prepared ZnO-mesotriones was 1064.3 ± 222.6 nm.

[0243] (39-2) Application of ZnO-mesotrione to clover An application test of ZnO-mesotrione was conducted on clover plants. On the above-ground parts of each plant 14 days after sowing, 2 mL / 25 cm was applied to a 0.01% mesotrione aqueous solution and a ZnO-mesotrione aqueous suspension equivalent to 0.01% mesotrione. ２ The plants were sprayed in this manner. The mortality rate was measured 14 days after spraying. The criterion for mortality was the loss of green color in the stems and leaves. Each experiment was conducted with n=5.

[0244] Figure 50 shows the clover mortality rate under each condition. Error bars indicate the standard deviation. The asterisk (*) in the figure indicates a statistically significant difference between the treatment intervals at the 5% level, as determined by Student's t-test. It was confirmed that the clover mortality rate increased significantly after application of ZnO-mesotrione compared to mesotrione.

[0245] [Example 40] Insecticidal efficacy test using zinc oxide-acephate wettable powder complex (ZnO-acephate) (40-1) Preparation of ZnO-acephate The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the acephate wettable powder was manufactured by Arista LifeSciences (Ortran® wettable powder). The binding reaction of ZnO and acephate wettable powder was carried out by mixing in solution.

[0246] Analysis of the prepared ZnO-acephate by FT-IR revealed that both ZnO and acephate exhibited the same absorption, as well as absorption originating from the P-O bond. This confirmed that ZnO and acephate were chemically bonded, forming a complex. The number-average particle size of the ZnO-acephate was measured using a DLS analyzer. The particle size of the prepared ZnO-acephate was 1102.7 ± 215.6 nm.

[0247] (40-2) Application of ZnO-acephate to soybeans Soybean seeds (variety: Fukuyutaka) were sown in poly pots filled with soil and cultivated for 21 days. Water (control), a 0.0125% acephate aqueous solution, and a ZnO-acephate aqueous suspension equivalent to 0.0125% acephate were sprayed onto the above-ground parts of each plant at a rate of 1 mL / plant. Four days after solution treatment, 10 soybeans and 3 beet armyworms were sealed in a sealed container. Seven days after sealing, soybean leaves were collected, thoroughly dried in an oven, and the dry weight of the leaves was measured. The degree of damage caused by beet armyworms was quantified by the above measurement, and the effectiveness of the insecticide was evaluated. Each experiment was conducted with n=10.

[0248] Figure 51 shows the dry weight of soybean leaves under each condition. Error bars in the figure indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Compared to the control and acephate, a significant increase in the dry weight of soybean leaves was confirmed after application of ZnO-acephate.

[0249] [Example 41] Insecticidal efficacy test using zinc oxide-methomyl complex (ZnO-methomyl) (41-1) Preparation of ZnO-methomyl The ZnO reagent (particle size 20 nm) and the methomyl reagent were manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The binding reaction of ZnO and methomyl was carried out by mixing in solution.

[0250] Analysis of the prepared ZnO-methomyl by FT-IR revealed that it exhibited the same absorption as both ZnO and acephate, as well as absorption originating from C-N and N-H bonds. This confirmed that ZnO and methomyl were chemically bonded, forming a complex. The number-average particle size of ZnO-methomyl was measured using a DLS analyzer. The particle size of the prepared ZnO-methomyl was 916.3 ± 200.5 nm.

[0251] (41-2) Application of ZnO-methomyl to soybeans Soybean seeds (variety: Fukuyutaka) were sown in poly pots filled with soil and cultivated for 21 days. Water (control), a 0.025% methomyl aqueous solution, and a ZnO-methomyl aqueous suspension equivalent to 0.025% methomyl were sprayed onto the above-ground parts of each plant at a rate of 1 mL / plant. Seven days after solution treatment, eight soybeans and five beet armyworms were sealed in a sealed container. Seven days after sealing, soybean leaves were collected, thoroughly dried in an oven, and the dry weight of the leaves was measured. The degree of damage caused by beet armyworms was quantified by the above measurement, and the effectiveness of the insecticide was evaluated. Each experiment was conducted with n=8.

[0252] Figure 52 shows the dry weight of soybean leaves under each condition. Error bars in the figure indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Compared to the control and methomyl, a significant increase in the dry weight of soybean leaves was confirmed after application of ZnO-methomyl.

[0253] [Example 42] Insecticidal efficacy test using zinc oxide-clothianidin wettable powder complex (ZnO-clothianidin) (42-1) Preparation of ZnO-clothianidin Fujifilm Wako Pure Chemical Industries used ZnO reagent (particle size 20 nm), and Sumitomo Chemical Co., Ltd. used clothianidin aqueous solution (Dantotsu aqueous solution). The bonding reaction of ZnO and clothianidin aqueous solution was carried out by mixing in solution.

[0254] Analysis of the prepared ZnO-clothianidin by FT-IR revealed that both ZnO and clothianidin exhibited the same absorption, as well as absorption originating from N-O and C-H bonds. This confirmed that ZnO and clothianidin were chemically bonded, forming a complex. The number-average particle size of the ZnO-clothianidin was measured using a DLS analyzer. The particle size of the prepared ZnO-clothianidin was 1178.6 ± 341.0 nm.

[0255] (42-2) Application of ZnO-clothianidin to soybeans Soybean seeds (variety: Fukuyutaka) were sown in poly pots filled with soil and cultivated for 13 days. Water (control), a 0.008% clothianidin aqueous solution, and a ZnO-clothianidin aqueous suspension equivalent to 0.008% clothianidin were sprayed onto the above-ground parts of each plant at a rate of 1 mL / plant. After 15 days of treatment, the above-ground parts of the soybeans were collected, thoroughly dried in an oven, and the dry weight of the above-ground parts was measured. Based on the above measurement, the degree of damage caused by naturally occurring aphids and bean leafminers indoors was quantified, and the effectiveness of the insecticide was evaluated. Each experiment was conducted with n=10 to 11.

[0256] Figure 53 shows the dry weight of soybean leaves under each condition. Error bars in the figure indicate the standard deviation. "**" and "***" in the figure indicate that there is a significant difference between the treatment intervals at the 1% and 0.1% levels, respectively, as determined by t-tests. Compared to the control and clothianidin, a significant increase in the above-ground dry weight of soybeans after application of ZnO-clothianidin was confirmed.

[0257] [Example 43] Bactericidal Efficacy Test of Zinc Oxide-Kresoxime Methyl Wettable Powder Complex (ZnO-Kresoxime Methyl) (43-1) Preparation of ZnO-Kresoxime Methyl The ZnO reagent (particle size 20 nm) used was from Fujifilm Wako Pure Chemical Industries, and the kresoxime methyl wettable powder was from Nippon Soda Co., Ltd. (Nisso Stroby Flowable). The bonding reaction of ZnO and kresoxime methyl wettable powder was carried out by mixing in solution.

[0258] Analysis of the prepared ZnO-kresoximemethyl by FT-IR revealed that both ZnO and kresoximemethyl exhibited the same absorption, as well as absorption originating from C=O, C=N, and C-O bonds. This confirmed that ZnO and kresoximemethyl were chemically bonded, forming a complex. The number-average particle size of ZnO-kresoximemethyl was measured using a DLS analyzer. The particle size of the prepared ZnO-kresoximemethyl was 621.5 ± 136.3 nm.

[0259] (43-2) Application of ZnO-Kresoxime Methyl to Wheat Seeds of wheat (variety: white wheat) were sown in poly pots filled with soil and cultivated for 35 days. A 0.01105% kresoxime methyl aqueous solution and a ZnO-Kresoxime methyl aqueous suspension equivalent to 0.01105% kresoxime methyl were sprayed onto the above-ground parts of each plant at a rate of 1 mL / plant.

[0260] (43-3) Test to confirm the effectiveness of the fungicide A 1.5% agar medium containing benzimidazole was prepared in a φ9 cm petri dish, and a 3 cm wide section was excised from the center. Six days after solution treatment, three 3.5 cm long leaf fragments were cut from each wheat plant and inserted into the agar medium so that both ends of the leaf fragments were fixed. Then, a wound was made in the center of each leaf fragment, and the same amount of Fusarium spore suspension was dropped onto each leaf fragment. The extent of the disease after four days was scored according to the following scoring criteria to evaluate the effectiveness of the fungicide. Each test was conducted with n=11 to 12. Scoring criteria: Based on the length of the diseased area, the evaluation was as follows: 1: 1 mm, 2: 2-5 mm, 3: 6-10 mm, 4: 10-15 mm, 5: >15 mm.

[0261] Figure 54 shows the score values ​​under each condition. Error bars in the figure indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Compared to the control and kresoxime methyl, it was confirmed that the score values ​​of wheat after application of ZnO-kresoxime methyl were significantly lower.

[0262] [Example 44] Bactericidal Efficacy Test of Zinc Oxide-Pidiflumetofen Wettable Powder Complex (ZnO-Pidiflumetofen) (44-1) Preparation of ZnO-Pidiflumetofen The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, and the pidiflumetofen wettable powder was manufactured by Syngenta Japan (Miravis Flowable). The binding reaction of ZnO and pidiflumetofen wettable powder was carried out by mixing in solution.

[0263] Analysis of the prepared ZnO-pidiflumetofen by FT-IR revealed that both ZnO and pidflumetofen exhibited the same absorption, as well as absorption originating from C=O, C=C, and C-F bonds. This confirmed that ZnO and pidflumetofen were chemically bonded, forming a complex. The number-average particle size of ZnO-pidiflumetofen was measured using a DLS analyzer. The particle size of the prepared ZnO-pidiflumetofen was 898.7 ± 207.0 nm.

[0264] (44-2) Application of ZnO-Pidiflumetofen to Wheat Seeds of wheat (variety: white wheat) were sown in poly pots filled with soil and cultivated for 28 days. A 0.0022875% didiflumetofen aqueous solution and a ZnO-pidiflumetofen aqueous suspension equivalent to 0.0022875% didiflumetofen were sprayed onto the above-ground parts of each plant at a rate of 1 mL / plant.

[0265] (44-3) Test to confirm the effectiveness of the fungicide A 1.5% agar medium containing benzimidazole was prepared in a φ9 cm petri dish, and a 3 cm wide section was excised from the center. Four days after solution treatment, three 3.5 cm long leaf fragments were cut from each wheat plant and inserted into the agar medium so that both ends of the leaf fragments were fixed. Then, a wound was made in the center of each leaf fragment, and the same amount of Fusarium spore suspension was dropped onto each leaf fragment. The extent of the disease after four days was scored according to the following scoring criteria to evaluate the effectiveness of the fungicide. Each test was conducted with n=12. Scoring criteria: Based on the length of the diseased area, the scores were evaluated as follows: 1: 1 mm, 2: 2-5 mm, 3: 6-10 mm, 4: 10-15 mm, 5: >15 mm.

[0266] Figure 55 shows the score values ​​under each condition. Error bars in the figure indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. Compared to the control and pidflumetofen, it was confirmed that the score values ​​of wheat after application of ZnO-pidiflumetofen were significantly lower.

[0267] [Example 45] Bactericidal Efficacy Test of Zinc Oxide-Thiophanate-Methyl Hydrate Complex (ZnO-Thiophanate-Methyl) (45-1) Preparation of ZnO-Thiophanate-Methyl The ZnO reagent (particle size 20 nm) was manufactured by Fujifilm Wako Pure Chemical Industries, Ltd., and the thiophanate-methyl hydrate was manufactured by Nisso Green Co., Ltd. (Topjin M hydrate). The binding reaction of ZnO and thiophanate-methyl hydrate was carried out by mixing in solution.

[0268] Analysis of the prepared ZnO-thiophanate-methyl by FT-IR revealed that both ZnO and thiophanate-methyl exhibited the same absorption, as well as absorption originating from C=O, C=S, C-O, and N-H bonds. This confirmed that ZnO and thiophanate-methyl were chemically bonded, forming a complex. The number-average particle size of ZnO-thiophanate-methyl was measured using a DLS analyzer. The particle size of the prepared ZnO-thiophanate-methyl was 1390.2 ± 207.4 nm.

[0269] (45-2) Application of ZnO-thiophanate-methyl to wheat Seeds of wheat (variety: white wheat) were sown in poly pots filled with soil and cultivated for 27 days. A 0.07% thiophanate-methyl aqueous solution and a ZnO-thiophanate-methyl aqueous suspension equivalent to 0.07% thiophanate-methyl were sprayed onto the above-ground parts of each plant at a rate of 1 mL / plant.

[0270] (45-3) Test to confirm the effectiveness of the fungicide A 1.5% agar medium containing benzimidazole was prepared in a φ9 cm petri dish, and a 3 cm wide section was excised from the center. Five days after solution treatment, three 3.5 cm long leaf fragments were cut from each wheat plant and inserted into the agar medium so that both ends of the leaf fragments were fixed. Then, the center of each leaf fragment was scratched, and the same amount of Fusarium spore suspension was dropped onto each leaf fragment. The extent of the disease after four days was scored according to the following scoring criteria to evaluate the effectiveness of the fungicide. Each test was conducted with n=12. Scoring criteria: Based on the length of the diseased area, the scores were evaluated as follows: 1: 1 mm, 2: 2-5 mm, 3: 6-10 mm, 4: 10-15 mm, 5: >15 mm.

[0271] Figure 56 shows the score values ​​under each condition. Error bars in the figure indicate the standard deviation. Different letters in the figure indicate a statistically significant difference at the 5% level according to Tukey's test. A significant decrease in the score value of wheat after application of ZnO-thiophanate-methyl was confirmed compared to the control and thiophanate-methyl. All publications, patents and patent applications cited herein are incorporated herein by direct reference.

Claims

1. An oxide complex containing oxide aggregates and a useful substance for delivering a useful substance into a plant.

2. The oxide composite according to claim 1, wherein the oxide composite is an oxide composite formed by bonding an oxide aggregate and a useful substance.

3. The oxide composite according to claim 2, wherein the bond is a covalent bond, a coordination bond, an ionic bond, or a hydrogen bond.

4. The oxide composite according to claim 2, wherein the bond is a covalent bond mediated by a hydroxyl group contained in the oxide aggregate and a hydroxyl group contained in the useful substance.

5. The oxide composite according to claim 1, wherein the number-average particle diameter is 100 nm or more and 2000 nm or less.

6. The oxide composite according to claim 1, wherein the oxide is a metal oxide and / or a nonmetal oxide.

7. The oxide composite according to claim 6, wherein the metal oxide comprises at least one selected from the group consisting of zinc (Zn) oxide, iron (Fe) oxide, potassium (K) oxide, calcium (Ca) oxide, magnesium (Mg) oxide, silver (Ag) oxide, manganese (Mn) oxide, molybdenum (Mo) oxide, copper (Cu) oxide, cobalt (Co) oxide, nickel (Ni) oxide, and aluminum (Al) oxide.

8. The oxide composite according to claim 6, wherein the nonmetallic oxide comprises at least one selected from the group consisting of silicon (Si) oxide, boron (B) oxide, and phosphorus (P) oxide.

9. The oxide complex according to claim 1, wherein the useful substance is selected from a) herbicides; b) fertilizer components; c) amino acids, peptides, or proteins; d) sugars; e) biostimulants; f) plant growth regulators; g) fungicides; and h) insecticides.

10. The aforementioned herbicides include phenoxy acid herbicides, carbamate herbicides, acid amide herbicides, urea herbicides, sulfonium urea herbicides, pyrimidyloxybenzoic acid herbicides, triazine herbicides, dianodine herbicides, diazole herbicides, bipyridium herbicides, dinitroaniline herbicides, aromatic carboxylic acid herbicides, fatty acid herbicides, organophosphorus herbicides, amino acid herbicides, ioxynyl herbicides, biphenox herbicides, DBN herbicides, DCBN herbicides, cethoxidim herbicides, cretoxidim herbicides, teproxidim herbicides, ACN herbicides, and chlor The oxide complex according to claim 9, comprising at least one selected from the group consisting of phthalim, flumioxazine, scinmethilin, carphetrazone ethyl, endotal disodium salt, benfresate, pentoxazone, pyraflufen ethyl, carbam, oxadiclomefone, indanophan, phentrazamide, benzobicyclon, butaphenacil, azaphenidine, pyrifthalide, fluthiaset methyl, oxaziargyl, oxadiazone, and decyl alcohol.

11. The oxide composite according to claim 9, wherein the fertilizer component comprises at least one selected from the group consisting of compounds containing at least one of carbon (C), hydrogen (H), oxygen (O), nitrogen (N), phosphorus (P), potassium (K), calcium (Ca), magnesium (Mg), sulfur (S), boron (B), chlorine (Cl), zinc (Zn), copper (Cu), iron (Fe), manganese (Mn), molybdenum (Mo), nickel (Ni), sodium (Na), silicon (Si), selenium (Se), cobalt (Co), aluminum (Al), chromium (Cr), and cadmium (Cd).

12. The oxide complex according to claim 9, wherein the amino acid, peptide, or protein is an amino acid, peptide, or protein that has a physiological function in the plant body.

13. The oxide composite according to claim 9, wherein the sugars include at least one selected from the group consisting of monosaccharides, disaccharides, oligosaccharides, and polysaccharides.

14. The oxide complex according to claim 9, wherein the biostimulant comprises at least one selected from the group consisting of peptides, amino acids, monosaccharides, disaccharides, oligosaccharides, polysaccharides, seaweed extracts, humic substances, organic acids, nucleic acids, plant extracts, food residues, and microbial metabolites.

15. The oxide complex according to claim 9, wherein the plant growth regulator comprises at least one selected from the group consisting of ethylene agents, auxin agents, auxin antagonists, cytokinin agents, cytokinin antagonists, gibberellin agents, dwarfing agents, isoprothiolanes, oxin sulfate agents, cyanamide agents, choline agents, decyl alcohol agents, piperonyl butoxide agents, bendimetaline agents, MCPA agents, MCPB agents, NAC agents, quinoxaline-based / DEP agents, pyraflufen ethyl agents, prohydrojasmone agents, abscisic acid agents, brassinosteroid agents, jasmonic acid agents, florigen agents, chlorella extract agents, and shiitake mushroom mycelium extract agents.

16. The aforementioned fungicides include copper fungicides, organosulfur fungicides, organophosphorus fungicides, organochlorine agents, melanin biosynthesis inhibitors, benzimidazole fungicides, dicarboxyimide fungicides, acid amide fungicides, sterol biosynthesis inhibitors, methoxyacrylate fungicides, anilinopyrimidine fungicides, synthetic antibacterial agents, soil fungicides, antibiotic fungicides, natural fungicides, probenazole agents, isoprothiolane agents, ferimzon agents, diclomezin agents, pencyclon agents, fluorimide agents, captan agents, sulfenic acid agents, and di The oxide complex according to claim 9, comprising at least one selected from the group consisting of thianon, quinoxaline, diflumetrim, fludioxonil, bentazole, acibenzoral S-methyl, triazine, fluazinam, diethofencarb, cymoxanil, iminoctadine acetate, iminoclazine albesilate, propamocarb hydrochloride, dimethomorph, diclocimet, famoxadone, cyazofamide, cyflufenamide, and thiadinil.

17. The oxide complex according to claim 9, wherein the insecticide comprises at least one selected from the group consisting of organophosphate insecticides, carbamate insecticides, pyrethroid insecticides, nereistoxin insecticides, neonicotinoid insecticides, insect growth regulators, natural insecticides, acaricides, nematicides, pine wood nematode control agents, slug control agents, benzoepins, fibronils, chlorfenavirs, diafenthiurons, pyrometrozines, emamectin benzoic acid, sodium oleate, DBEDCs, indoxacarbs, and tolfenpyrads.

18. The oxide complex according to claim 1, wherein the plant is selected from the group consisting of monocots and dicots.

19. A composition for delivering useful substances into a plant body, comprising the oxide complex described in claim 1.

20. A method for delivering a useful substance into a plant, comprising applying the oxide complex described in claim 1 to a plant or to soil, culture medium, or water surrounding the plant.

21. A method for delivering a useful substance into a plant, comprising the steps of: preparing an oxide complex by combining an oxide aggregate with a useful substance; and applying the oxide complex to a plant or to soil, culture medium, or water surrounding the plant.

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