Chinese herbal medicine composite biological insect prevention preparation and its preparation method and application

Abstract

This application discloses a traditional Chinese medicine compound biological insect repellent preparation, its preparation method, and its application, belonging to the field of pest and disease control technology. This traditional Chinese medicine compound biological insect repellent preparation comprises, from the outside in, a fast-release insecticidal layer, an isolation buffer layer, and a slow-release layer. The fast-release insecticidal layer is loaded with traditional Chinese medicine extracts, the slow-release layer is loaded with compound functional bacterial powder, and the isolation buffer layer is located between the fast-release insecticidal layer and the slow-release layer to prevent direct contact between the traditional Chinese medicine extracts and the compound functional bacterial powder. The isolation buffer layer effectively solves the problem of antagonism between the traditional Chinese medicine extracts and functional bacterial strains. The fast-release layer quickly kills piercing-sucking pests, while the slow-release layer significantly improves the field survival rate and colonization ability of the bacterial strains, achieving long-term ovicidal and insecticidal control. This invention combines fast-acting insect control with long-term prevention of recurrence, is green and safe, and has strong stability, effectively solving the problems of poor efficacy and weak stability of traditional compound preparations, and is suitable for the needs of large-scale green pest control in the field.

Description

Technical Field

[0001] This application relates to a compound biological insect repellent preparation made from traditional Chinese medicine, its preparation method and application, belonging to the field of pest and disease control technology. Background Technology

[0002] Thrips, spider mites, and aphids are the most prevalent piercing-sucking pests in agricultural production. They are characterized by rapid reproduction, high concealment, significant generational overlap, and easy development of pesticide resistance, causing severe yield and quality losses to vegetables, fruit trees, and cash crops year after year. Currently, field control of these pests still relies primarily on chemical pesticides. However, long-term and excessive use of chemical agents easily leads to a series of problems, including increased pest resistance, pesticide residues in crops, soil and water pollution, and imbalances in natural enemies, which does not meet the development needs of green agriculture and ecological plant protection.

[0003] Existing green pest control technologies are mainly divided into two categories: herbal plant-derived pest control preparations and microbial agents. Among them, single herbal extract preparations are mostly applied by directly compounding the extract and spraying, such as Chinese patent CN 103609627 A. Although they have the effects of rapid contact killing and repelling pests, they generally have the defects of rapid volatilization, short-lasting effect, poor leaf adhesion, and no continuous pest control ability. They can only suppress the initial pest population in the short term, but cannot kill insect eggs and hidden pests, and the pests are very easy to rebound and recur.

[0004] Although single microbial insect repellent agents have advantages such as safety and no pollution, colonization and antibacterial properties, long-lasting insect control and low resistance, their field application has obvious shortcomings: lack of nutrient substrate in the natural environment, light and dry and wet stress can easily cause a large number of strains to die, slow germination of strains and delayed onset of action, making it impossible to quickly control outbreaks of pests.

[0005] Existing technologies also include compound insect repellents containing both pesticides and microorganisms. However, most of these are simple physical mixtures, which have technical drawbacks such as mutual inhibition between pesticides and microorganisms, significant loss of activity, and poor product storage stability. Furthermore, highly active plant volatile oils and alkaloids generally have broad-spectrum antibacterial effects. If they are directly mixed with beneficial microorganisms, they will inhibit the activity of the strains, causing bacterial inactivation and greatly reducing the insect repellent and insecticidal effects.

[0006] Therefore, it is crucial to develop a compound biological insect control agent based on traditional Chinese medicine to address the technical challenges of antagonistic interactions between traditional herbal medicines and fungi, loss due to essential oil volatilization, low survival rate of strains in the field, and the inability to balance fast and slow efficacy, so as to meet the needs of large-scale green control of piercing-sucking pests in the field. Summary of the Invention

[0007] To address the aforementioned issues, a compound biological insect repellent formulation based on traditional Chinese medicine is provided, along with its preparation method and application. This compound biological insect repellent formulation effectively solves the problem of antagonism between the extracts of traditional Chinese medicine and functional strains through an isolation buffer layer. The immediate-release layer rapidly kills piercing-sucking pests, while the slow-release layer significantly improves the field survival rate and colonization ability of the strains, achieving long-term ovicidal and insecticidal effects. This invention balances rapid insect control with long-term prevention of recurrence, is green and safe, and has strong stability. It effectively solves the problems of poor efficacy and weak stability of traditional compound formulations, and is suitable for the needs of large-scale green pest control in the field.

[0008] According to one aspect of this application, a traditional Chinese medicine compound biological insect repellent preparation is provided, comprising, from the outside to the inside, an immediate-release insecticidal layer, an isolation buffer layer, and a slow-release layer. The immediate-release insecticidal layer is loaded with traditional Chinese medicine extracts, the slow-release layer is loaded with compound functional bacterial powder, and the isolation buffer layer is disposed between the immediate-release insecticidal layer and the slow-release layer to prevent the traditional Chinese medicine extracts from directly contacting the compound functional bacterial powder.

[0009] Specifically, this application uses an isolation buffer layer to physically separate the fast-acting Chinese herbal extract from the compound bacterial strain, structurally solving the problem of direct contact and antagonistic inactivation between plant-derived antibacterial components and functional strains. The fast-release insecticidal layer is responsible for quickly killing adult and nymph insects in the field, while the slow-release layer carries the compound bacterial strain to achieve colonization and control in the later stage, realizing the synergistic unity of fast-acting insect control and long-term prevention of recurrence. The overall stability and control sustainability of the formulation are significantly improved.

[0010] Optionally, by weight, the quick-release insecticidal layer comprises 35-45 parts of herbal extract, 5-15 parts of water-soluble quick-release wall material, and 1-2 parts of penetrant; The isolation buffer layer comprises 3-5 parts sodium alginate and 2-3 parts chitosan; The slow-release layer comprises 10-15 parts of composite functional bacterial powder and 10-20 parts of slow-release wall material.

[0011] Specifically, this application specifies the composition and ratio of each layer. The herbal extract in the fast-release insecticidal layer ensures the basic fast-acting insecticidal effect, and the combination with water-soluble fast-release wall material and penetrant improves the molding and adhesion performance. The isolation layer uses sodium alginate and chitosan to form a dense cross-linked barrier membrane. The slow-release layer specifies the bacterial powder and slow-release wall material to ensure stable encapsulation and slow release of the bacterial strain, avoiding problems such as poor molding, disordered drug release, and bacterial inactivation caused by imbalance in the ratio, and greatly improving the formulation molding performance and field applicability.

[0012] Optionally, the water-soluble immediate-release wall material comprises pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester, and β-cyclodextrin; the mass ratio of the pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester, and β-cyclodextrin is (3~5):(1~2):(1~3):(1~2); The penetrant includes polyether-modified trisiloxane; The slow-release wall material comprises plant beeswax, stearic acid and hydrophobically modified cellulose, wherein the mass ratio of plant beeswax, stearic acid and hydrophobically modified cellulose is (6~8):(8~10):(6~7).

[0013] Specifically, this application defines water-soluble immediate-release and slow-release wall materials. The four wall materials in the water-soluble immediate-release wall material work synergistically, using β-cyclodextrin to encapsulate essential oils and polysaccharide wall materials to stabilize the extract, solving the problems of easy volatility of Chinese herbal essential oils and oil separation. It is combined with organosilicon penetrants to enhance the ability of the liquid to penetrate and adhere to the leaf surface. The three wall materials in the slow-release layer are gradient compounded to achieve slow dissolution and controlled release of bacteria, avoiding rapid loss of strains. The components work together to stabilize the efficacy and bacterial activity, and precisely control the release rhythm, significantly improving the storage stability of the formulation and the field control effect.

[0014] Optionally, the raw materials of the herbal extract are composed of the following components in the following weight ratio: 8-12 parts garlic, 6-10 parts chili pepper, 5-8 parts pine needles, 4-6 parts pine resin, 5-7 parts oregano, and 6-9 parts acorus calamus; The compound functional bacterial powder is composed of the following components in the following weight ratios: 4-6 parts of Bacillus belye powder, 2-4 parts of Bacillus pumilus powder, 2-4 parts of Beauveria bassiana powder, and 1-3 parts of Paecilomyces lilacinus powder.

[0015] Specifically, multiple Chinese herbs work synergistically to exert multiple effects of contact killing, repellency, and food rejection, targeting thrips, spider mites, and aphids on a broad spectrum. The four strains complement each other and work synergistically: Bacillus secretes insecticidal metabolites and inhibits bacterial growth, Beauveria bassiana infects insects and causes disease, and Paecilomyces lilacinus parasitizes and kills insect eggs, making up for the functional limitations of single strains. The multi-strain combination of drugs and bacteria avoids the problems of weak efficacy and single insecticidal target of single drugs, greatly improving the overall broad spectrum of insect control and synergistic effect.

[0016] Optionally, the extracts of garlic, pine needles, pine resin, oregano and acorus calamus in the herbal extract are volatile oils, and the extract of chili pepper is a concentrated extract; the mass ratio of volatile oil to concentrated extract in the herbal extract is (8~12):(20~25).

[0017] Specifically, the extraction forms and oil-ointment ratios of traditional Chinese medicine are limited. Volatile medicinal materials are made into volatile oils to achieve rapid fumigation and contact killing of insects, while chili peppers are made into concentrated extracts to improve the adhesion and retention of the pesticide solution. The precise ratio of the two achieves complementary effects of fast and slow efficacy. The volatile oil is responsible for quickly knocking down pests, while the extract leaves a long-lasting pesticide film to continuously repel them. At the same time, the oil and the extract have good compatibility and are not prone to delamination and failure when used with wall materials, maximizing the insecticidal activity of traditional Chinese medicine and solving the defects of traditional single-extract formulations such as slow onset, short retention and unstable efficacy.

[0018] Optionally, the effective viable count of the Bacillus vesiculosus powder is ≥8.0 × 10⁻⁶.8 CFU / g, the effective viable count of the *Bacillus pumilus* powder is ≥5.0 × 10⁻⁶. 8 CFU / g, the effective viable count of the *Beauveria bassiana* powder is ≥5.0 × 10⁻⁶. 8 CFU / g, conidia ≥4.0×10 8 The effective viable count of the *Paecilomyces lilacinus* powder is ≥5.0 × 10⁻⁶ cells / g; 8 CFU / g.

[0019] Specifically, this application sets minimum viable cell and spore content standards for four types of strains to ensure the basic biological activity and infectivity of the compound strains. Different strains are set with appropriate viable cell thresholds to ensure both the antibacterial and insecticidal metabolic capacity of Bacillus and the spore germination and insect infectivity of Beauveria bassiana and Paecilomyces lilacinus. Standardized viable cell parameters can avoid long-term control failure caused by insufficient strain activity, ensure the stable performance of the synergistic colonization, ovicidal and antibacterial functions of multiple strains, and greatly improve the reliability and repeatability of the long-term insect control of the formulation.

[0020] Optionally, the isolation buffer layer further includes 0.5 to 1.5 parts of porous diatomaceous earth powder; the slow-release layer further includes 15 to 20 parts of nutrient carrier and 1 to 3 parts of humic acid powder; the nutrient carrier includes soybean meal powder and corn starch powder, with a mass ratio of 1:(1 to 1.3).

[0021] Specifically, this application adds porous diatomaceous earth to the isolation layer, utilizing its porous structure to adsorb free antibacterial components of traditional Chinese medicine, further enhancing the drug-bacterial barrier effect and protecting the activity of the inner strains. The slow-release layer contains a composite nutrient carrier of soybean meal and corn starch, along with humic acid powder, providing endogenous nutrition for dormant strains and solving the problem of strains easily starving and becoming inactive in the field due to lack of substrate. Simultaneously, humic acid can induce and enhance the metabolic activity of the strains. This significantly improves the germination rate, colonization ability, and long-term control stability of the formulation.

[0022] According to another aspect of this application, a method for preparing the above-mentioned herbal compound biological insect repellent is also provided, comprising the following steps: (1) Crush garlic, pine needles, pine resin, oregano, and sweet flag and add them to a distillation kettle. Add deionized water and perform normal pressure steam distillation. Let the distillate stand to separate into layers. Take the upper transparent oil phase, dehydrate and remove impurities to obtain volatile oil. Crush chili peppers and add 50-60% ethanol as a solvent for ultrasonic extraction 2-3 times. The mass-volume ratio of chili peppers to ethanol is 1:(3-4). Collect the filtrate and concentrate it under vacuum to obtain concentrated extract. Mix the volatile oil and concentrated extract according to the weight ratio and set aside. (2) Mix and stir the Bacillus vesiculosus powder, Bacillus pumilus powder, Beauveria bassiana powder and Paecilomyces lilacinus powder evenly and set aside. (3) Preparation of slow-release core: Plant beeswax, stearic acid and hydrophobic modified cellulose are heated to 60~70℃ and melted according to the formula. Stirred until completely liquefied to obtain molten slow-release wall material; Composite functional bacterial powder, nutrient carrier, humic acid micro powder and molten slow-release wall material are mixed evenly, and microspheres are formed by centrifugal granulation and dried at low temperature to obtain slow-release core. (4) Coating the isolation buffer layer: Sodium alginate, chitosan and porous diatomaceous earth powder are mixed with water to form a uniform film-forming liquid with a solid content of 2%~3%. The slow-release core is placed in a fluidized bed coating machine and sprayed onto the surface of the slow-release core using fluidized bed atomization. The air inlet temperature is 35~40℃. After cross-linking and curing, a 5~10μm isolation buffer layer is formed. (5) Coating with an instant-release insecticidal layer: Pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester, and β-cyclodextrin are mixed, and volatile oil, concentrated chili extract, and polyether-modified trisiloxane are added. The mixture is stirred at room temperature to prepare a viscosity coating solution. The instant-release insecticidal layer is coated under hot air conditions at 40~45℃ and dried to obtain a traditional Chinese medicine compound biological insect repellent preparation.

[0023] Specifically, this invention defines a step-by-step preparation process, adopts a mixed co-extraction process to simplify the preparation process of Chinese herbal essential oils, and uses low-temperature ultrasonic extraction to preserve the activity of chili extract; first, stable slow-release sclerotia are prepared, and then the isolation layer and the immediate-release layer are coated in layers. The step-by-step molding can avoid the inactivation of strains caused by high temperature and contact with the drug solution. The process has strong adaptability and can stably prepare insect repellents with regular structure, intact drug and bacterial activity, and precise drug release sequence, with good mass production repeatability.

[0024] Optionally, in step (1), the amount of deionized water added is 4 to 6 times the total mass of the Chinese herbal medicine, the temperature of steam distillation is 95 to 100℃, and the distillation time is 2 to 3 hours; the extraction temperature of ultrasonic extraction is 40 to 50℃, the ultrasonic power is 300 to 500W, and the extraction time is 60 to 90 minutes per extraction; in step (3), the particle size of the microspheres is 100 to 200 μm, the temperature of low-temperature drying is 40 to 45℃, and the drying time is 2 to 3 hours.

[0025] Specifically, this application limits the key process parameters for extraction, granulation, and drying, and precisely controls the distillation and extraction conditions to retain the insecticidal active ingredients of traditional Chinese medicine to the maximum extent. It also limits the microsphere particle size and low-temperature drying parameters, which can ensure the regularity of the core shape while avoiding the inactivation of strains and spores caused by high temperature. The precise process parameters ensure the stability of product activity and uniformity of structure, and reduce problems such as fluctuations in efficacy, uneven viable cell rate, and unstable product quality.

[0026] According to another aspect of this application, the application of the above-mentioned herbal compound biological insect repellent preparation in the control of thrips, spider mites and aphids is also provided.

[0027] The beneficial effects of this application include, but are not limited to: 1. The herbal compound biological insect repellent formulation of this application effectively blocks the penetration of antibacterial active ingredients such as volatile oils and capsaicin from the herbal medicines through the sodium alginate-chitosan cross-linked isolation membrane combined with the adsorption effect of diatomaceous earth, thus preventing the functional strains from being inhibited and inactivated. It overcomes the defects of traditional herbal compound formulations, such as simple mixing, mutual antagonism, rapid activity decay during storage, and poor batch stability. It achieves a balance between the rapid effect of the herbal medicine and the long-term effect of the microorganisms. The structure is layered and does not interfere with each other, which significantly improves the storage stability and field use reliability of the formulation.

[0028] 2. The herbal compound biological insecticide formulation of this application uses a mixture of volatile oils from multiple Chinese herbs combined with concentrated chili extract, and combines β-cyclodextrin inclusion modification with the synergistic effect of polysaccharide fast-release wall materials to effectively reduce essential oil volatilization loss, enhance the wetting and penetration of the pesticide solution and its adhesion to the leaf surface. After application, it can quickly release insecticidal active ingredients, and through multiple actions such as contact killing, antifeedant, and fumigation, it can quickly kill thrips, spider mites, and aphid nymphs, rapidly suppressing the insect population in the field in a short period of time. This solves the shortcomings of single microbial agents, such as slow onset of action and inability to cope with insect outbreaks, and achieves rapid pest control.

[0029] 3. The herbal compound biological insect repellent formulation of this application uses a four-component compound functional strain. Bacillus, Beauveria bassiana, and Paecilomyces lilacinus complement each other and work synergistically to control insects, covering multiple mechanisms of insecticidal, antibacterial, ovicidal, and parasitic control. At the same time, soybean meal-corn starch compound nutrient carrier and humic acid micro powder are introduced to provide endogenous nutrients for dormant strains, solving the problems of lack of substrate in the field and easy death of strains. This can ensure that the strains can germinate, colonize and proliferate smoothly after spraying, effectively kill hidden eggs and residual pests, significantly extend the effective period, and prevent repeated outbreaks of pests.

[0030] 4. The preparation method of the herbal compound biological insect repellent agent according to this application avoids high-temperature inactivation of strains throughout the process, retains the dual activity of the drug and bacteria to the greatest extent, and the product has a uniform structure, stable quality, no chemical residues, and is not prone to causing insect resistance. It can effectively solve the problems of traditional chemical pesticide residues, environmental pollution, and imbalance of natural enemies, and takes into account both rapid insecticidal effect and long-term insect control, which meets the application needs of green agriculture, ecological plant protection and large-scale pollution-free crop production. Detailed Implementation

[0031] The present application is described in detail below with reference to the embodiments, but the present application is not limited to these embodiments.

[0032] Unless otherwise specified, the raw materials used in the embodiments and comparative examples of this application were all purchased commercially.

[0033] Unless otherwise specified, the methods used in the embodiments and comparative examples of this application are conventional methods in the prior art. The *Bacillus belyssus*, *Bacillus pumilus*, *Beauveria bassiana*, and *Paecilomyces lilacinus* used in the following embodiments are all existing strains available for purchase from the China Microbiological Culture Collection Center. This does not involve the development of new strains, but only the application of these existing strains. Furthermore, in the following embodiments and comparative examples, the mass ratio of soybean meal powder to corn starch powder in the nutrient carrier is 1:1.2; the *Bacillus belyssus* used is selected from strain with accession number CGMCC 1.12669, with an effective viable count ≥8.0 × 10⁻⁶. 8 CFU / g; Bacillus pumilus was selected from strain with accession number CGMCC 1.10291, with an effective viable count ≥5.0×10⁻⁶. 8 CFU / g; Beauveria bassiana was selected from strain with accession number CGMCC 3.11099, with an effective viable count ≥5.0×10⁻⁶. 8 CFU / g, conidia ≥4.0×10 8 CFU / g; Paecilomyces lilacinus was selected from strain ACCC 32162, with an effective viable count ≥5.0×10⁻⁶. 8 CFU / g.

[0034] Example 1 (1) Take 8 parts garlic, 6 parts chili pepper, 5 parts pine needle, 4 parts pine resin, 5 parts oregano and 6 parts calamus according to the weight ratio. Crush the garlic, pine needle, pine resin, oregano and calamus to 100 mesh and add them to the distillation kettle. Add 4 times the total mass of Chinese herbal medicines of deionized water and carry out normal pressure steam distillation. The temperature of steam distillation is 95℃ and the distillation time is 2h. Let the distillate stand to separate into layers. Take the upper transparent oil phase and dehydrate and remove impurities with anhydrous sodium sulfate to obtain volatile oil. Crush the chili pepper to 100 mesh and add 50% ethanol as a solvent for ultrasonic extraction twice. The mass-volume ratio of chili pepper to ethanol is 1:3 (g / mL). The extraction temperature of ultrasonic extraction is 40℃ and the ultrasonic power is 300W. The extraction time is 60min per extraction. Collect the filtrate and concentrate it under vacuum to obtain concentrated extract. Mix the volatile oil and concentrated extract at a weight ratio of 2:5 and set aside. (2) Take 4 parts of Bacillus vesicles powder, 2 parts of Bacillus pumilus powder, 2 parts of Beauveria bassiana powder and 1 part of Paecilomyces lilacinus powder according to the weight ratio. Mix the Bacillus vesicles powder, Bacillus pumilus powder, Beauveria bassiana powder and Paecilomyces lilacinus powder evenly and set aside. (3) Preparation of slow-release core: Take raw materials in the mass ratio of plant beeswax, stearic acid and hydrophobic modified cellulose of 6:8:6. Heat the plant beeswax, stearic acid and hydrophobic modified cellulose at 60℃ to melt and stir until completely liquefied to obtain molten slow-release wall material. Mix 10 parts of composite functional bacterial powder, 15 parts of nutrient carrier and 1 part of humic acid micro powder with 10 parts of molten slow-release wall material evenly, and make 100μm microspheres by centrifugal granulation. Dry at low temperature at 40℃ for 2 hours to obtain slow-release core. (4) Coating the isolation buffer layer: Add water to 3 parts sodium alginate, 2 parts chitosan and 0.5 parts porous diatomaceous earth powder to make a uniform film-forming liquid with a solid content of 2%. Place the slow-release core in a fluidized bed coating machine and spray it onto the surface of the slow-release core using fluidized bed atomization. The air inlet temperature is 35℃. After cross-linking and curing, a 5μm isolation buffer layer is formed. (5) Coating with an instant-release insecticidal layer: Take the raw materials according to the mass ratio of pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester and β-cyclodextrin of 3:1:1:1. Mix the pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester and β-cyclodextrin, take 5 parts, add 35 parts of Chinese herbal medicine extract and 1 part of polyether modified trisiloxane, stir at room temperature to prepare a viscosity coating liquid, coat the instant-release insecticidal layer under hot air at 40℃, and dry to obtain the Chinese herbal medicine compound biological insect repellent preparation.

[0035] Example 2 (1) Take 12 parts garlic, 10 parts chili pepper, 8 parts pine needle, 6 parts pine resin, 7 parts oregano and 9 parts calamus according to the weight ratio. Crush the garlic, pine needle, pine resin, oregano and calamus to 100 mesh and add them to the distillation kettle. Add 6 times the total mass of Chinese herbal medicines of deionized water and carry out normal pressure steam distillation. The temperature of steam distillation is 100℃ and the distillation time is 3h. Let the distillate stand to separate into layers. Take the upper transparent oil phase and dehydrate and remove impurities with anhydrous sodium sulfate to obtain volatile oil. Crush the chili pepper to 100 mesh and add 60% ethanol as a solvent for ultrasonic extraction 3 times. The mass-volume ratio of chili pepper to ethanol is 1:4 (g / mL). The extraction temperature of ultrasonic extraction is 50℃ and the ultrasonic power is 500W. The extraction time is 90min per extraction. Collect the filtrate and concentrate it under vacuum to obtain concentrated extract. Mix the volatile oil and concentrated extract at a weight ratio of 12:25 for later use. (2) Take 6 parts of Bacillus vesicles powder, 4 parts of Bacillus pumilus powder, 4 parts of Beauveria bassiana powder and 3 parts of Paecilomyces lilacinus powder according to the weight ratio. Mix the Bacillus vesicles powder, Bacillus pumilus powder, Beauveria bassiana powder and Paecilomyces lilacinus powder evenly and set aside. (3) Preparation of the slow-release core: Take the raw materials according to the mass ratio of plant beeswax, stearic acid and hydrophobic modified cellulose of 8:10:7. Heat the plant beeswax, stearic acid and hydrophobic modified cellulose at 70℃ to melt and stir until completely liquefied to obtain the melt slow-release wall material. Mix 15 parts of composite functional bacterial powder, 20 parts of nutrient carrier and 3 parts of humic acid micro powder with 20 parts of melt slow-release wall material evenly, and make 200μm microspheres by centrifugal granulation. Dry at low temperature. The temperature of low temperature drying is 45℃ and the drying time is 3h to obtain the slow-release core. (4) Coating the isolation buffer layer: 5 parts sodium alginate, 3 parts chitosan and 1.5 parts porous diatomaceous earth powder are mixed with water to form a uniform film-forming liquid with a solid content of 3%. The slow-release core is placed in a fluidized bed coating machine and sprayed onto the surface of the slow-release core by fluidized bed atomization. The air inlet temperature is 40℃. After cross-linking and curing, a 10μm isolation buffer layer is formed. (5) Coating with an instant-release insecticidal layer: Take raw materials in a mass ratio of 5:2:3:2 for pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester and β-cyclodextrin. Mix the pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester and β-cyclodextrin, take 15 parts, add 45 parts of traditional Chinese medicine extract and 2 parts of polyether modified trisiloxane, stir at room temperature to prepare a viscosity coating liquid, coat the instant-release insecticidal layer under hot air at 45℃, and dry to obtain a traditional Chinese medicine compound biological insect repellent preparation.

[0036] Example 3 (1) Take 10 parts garlic, 8 parts chili pepper, 6 parts pine needle, 5 parts pine resin, 6 parts oregano and 8 parts calamus according to the weight ratio. Crush the garlic, pine needle, pine resin, oregano and calamus to 100 mesh and add them to the distillation kettle. Add 5 times the total mass of Chinese herbal medicines of deionized water and carry out normal pressure steam distillation. The temperature of steam distillation is 100℃ and the distillation time is 2h. Let the distillate stand to separate into layers. Take the upper transparent oil phase and dehydrate and remove impurities with anhydrous sodium sulfate to obtain volatile oil. Crush the chili pepper to 100 mesh and add 55% ethanol as a solvent for ultrasonic extraction 3 times. The mass-volume ratio of chili pepper to ethanol is 1:3 (g / mL). The extraction temperature of ultrasonic extraction is 45℃ and the ultrasonic power is 400W. The extraction time is 75min per extraction. Collect the filtrate and concentrate it under vacuum to obtain concentrated extract. Mix the volatile oil and concentrated extract at a weight ratio of 10:23 for later use. (2) Take 5 parts of Bacillus vesicles powder, 3 parts of Bacillus pumilus powder, 3 parts of Beauveria bassiana powder and 2 parts of Paecilomyces lilacinus powder according to the weight ratio. Mix the Bacillus vesicles powder, Bacillus pumilus powder, Beauveria bassiana powder and Paecilomyces lilacinus powder evenly and set aside. (3) Preparation of slow-release core: Take raw materials in the mass ratio of plant beeswax, stearic acid and hydrophobic modified cellulose of 7:9:6. Heat the plant beeswax, stearic acid and hydrophobic modified cellulose at 65°C to melt and stir until completely liquefied to obtain molten slow-release wall material. Mix 12 parts of composite functional bacterial powder, 18 parts of nutrient carrier and 2 parts of humic acid micro powder with 15 parts of molten slow-release wall material evenly. Form 150μm microspheres by centrifugal granulation and dry at low temperature. The low temperature drying temperature is 40°C and the drying time is 3h to obtain the slow-release core. (4) Coating the isolation buffer layer: Add 4 parts of sodium alginate, 2 parts of chitosan and 1 part of porous diatomaceous earth powder to water to make a uniform film-forming liquid with a solid content of 2.5%. Place the slow-release core in a fluidized bed coating machine and spray it onto the surface of the slow-release core using fluidized bed atomization. The air inlet temperature is 35~40℃. After cross-linking and curing, a 5μm isolation buffer layer is formed. (5) Coating with an instant-release insecticidal layer: Take raw materials in a mass ratio of 4:2:2:1 for pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester and β-cyclodextrin. Mix the pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester and β-cyclodextrin. Take 10 parts, add 40 parts of traditional Chinese medicine extract and 1 part of polyether modified trisiloxane. Stir at room temperature to prepare a viscosity coating solution. Coat the instant-release insecticidal layer under hot air at 40℃ and dry to obtain a traditional Chinese medicine compound biological insect repellent preparation.

[0037] Example 4 The difference between Example 4 and Example 3 is that the immediate-release insecticidal layer does not include a penetrant, but all other aspects are the same.

[0038] Example 5 The difference between Example 5 and Example 3 is that the water-soluble quick-release wall material does not include sucrose esters, but all other aspects are the same.

[0039] Example 6 The difference between Example 6 and Example 3 is that the herbal extract does not include Acorus tatarinowii, but all other ingredients are the same.

[0040] Example 7 The difference between Example 7 and Example 3 is that the same amount of pine needles are used to replace the pine resin, while the rest are the same.

[0041] Example 8 The difference between Example 8 and Example 3 is that in the compound functional bacterial powder, an equal amount of Beauveria bassiana powder is used to replace Paecilomyces lilacinus powder, while the rest are the same.

[0042] Example 9 The difference between Example 9 and Example 3 is that chili peppers, garlic, pine needles, pine resin, oregano, and calamus are steam distilled together to obtain volatile oils, while the rest are the same.

[0043] Example 10 The difference between Example 10 and Example 3 is that the isolation buffer layer does not include porous diatomaceous earth micropowder, but the rest are the same.

[0044] Example 11 The difference between Example 11 and Example 3 is that the slow-release layer does not include humic acid micro powder, but all other aspects are the same.

[0045] Example 12 The difference between Example 12 and Example 3 is that the sustained-release layer does not include a nutrient carrier, but all other aspects are the same.

[0046] Example 13 The difference between Example 13 and Example 3 is that the nutrient carrier is corn starch powder, while the rest are the same.

[0047] Comparative Example 1 The difference between Comparative Example 1 and Example 3 is that the isolation buffer layer is not included, but all other aspects are the same.

[0048] Comparative Example 2 The difference between Comparative Example 2 and Example 3 is that an equal amount of Beauveria bassiana powder was used to replace the compound functional bacterial powder, while the rest were the same.

[0049] Comparative Example 3 The difference between Comparative Example 3 and Example 3 is that the herbal extract and the compound functional bacterial powder were directly mixed and granulated, while the rest were the same.

[0050] Comparative Example 4 The difference between Comparative Example 4 and Example 3 is that the immediate-release insecticidal layer is loaded with compound functional bacterial powder, and the slow-release layer is loaded with traditional Chinese medicine extracts; all other aspects are the same.

[0051] Comparative Example 5 The difference between Comparative Example 5 and Example 3 is that Comparative Example 5 does not include the compound functional bacterial powder, but all other aspects are the same.

[0052] Comparative Example 6 The difference between Comparative Example 6 and Example 3 is that Comparative Example 6 does not include the herbal extract, but all other aspects are the same.

[0053] Experimental Example 1 The insect repellent preparations obtained in the above examples and comparative examples were stored in a room temperature, sealed, and light-protected environment for 30 days. The initial viable bacterial count and the viable bacterial count after 30 days of storage were measured, and the viable bacterial retention rate was calculated. The viable bacteria retention rate (%) = number of viable bacteria after storage / initial number of viable bacteria × 100%. The test results are shown in Table 1.

[0054] Table 1 Results of viable bacteria retention rate test

[0055] Table 1 shows that the viable bacterial retention rate in Examples 1-3 remained above 82%, with Example 3 having the highest rate at 89.8%. Examples 4-13 showed varying degrees of decrease in viable bacterial retention rate due to the absence of certain components, indicating that each component had a synergistic effect on improving strain stability. In Comparative Examples 1 and 3, the removal of the isolation layer or direct mixing of the herbal medicine and bacteria resulted in a significant decrease in viable bacterial retention rate due to the inhibition of the strain by the herbal ingredients; in Comparative Example 4, the inverted layer structure weakened the protective effect on the strain.

[0056] Experiment Example 2 The experimental plots were selected from crop fields where thrips, spider mites, and aphids were naturally occurring. The experiment used a randomized block design, with each treatment constituting one plot, each plot measuring 15 m², and each treatment being replicated three times. Isolation rows were set between plots to prevent cross-interference between pesticides. All plots were managed with uniform water and fertilizer, and no other pesticides were applied.

[0057] Dilute the above-mentioned insect repellent preparation with water at a mass ratio of 1:500. Spray the preparation evenly on the crop plants, leaves and flowers during a windless period in the evening, ensuring that both sides of the leaves, tender shoots and flowers are completely wet. Spray the blank control group with an equal amount of water.

[0058] Each plot used a five-point sampling method, marking two crops at each point to count the basic insect population.

[0059] 24 hours after application, the number of live insects at the same marked points was investigated, and the corrected knockdown rate was calculated: Insect population reduction rate (%) = (Number of insects before pesticide application - Number of insects after pesticide application) / Number of insects before pesticide application × 100% Corrected knockdown rate (%) = (Treatment insect population reduction rate - Blank insect population reduction rate) / (1 - Blank insect population reduction rate) × 100%; Twenty days after application, the number of residual insects on marked plants was investigated, and the corrected control efficacy was calculated. Corrected control efficacy (%) = (reduction rate of treated insect population - reduction rate of blank insect population) / (1 - reduction rate of blank insect population) × 100%.

[0060] The test results are shown in Table 2.

[0061] Table 2 Insecticidal Efficacy Test Results

[0062] Examples 1-3 exhibit both excellent rapid and long-lasting control effects, with Example 3 showing the best overall performance, achieving a 92.7% corrected knockdown rate at 24 hours and a 86.5% corrected control efficacy at 20 days. Examples 4-13 showed decreased rapid or long-lasting effects due to missing or replaced components, indicating that the components synergistically achieve a combination of rapid and slow pest control. Comparative Examples 1 and 3, lacking an isolation layer, resulted in strain inactivation and significantly reduced long-lasting efficacy; Comparative Example 4, with its inverted layer structure, led to disordered drug release, resulting in a substantial decrease in both rapid and long-lasting effects; Comparative Examples 5 and 6, respectively lacking strains or traditional Chinese medicine, failed to achieve both rapid insecticidal action and long-term pest suppression.

[0063] The above description is merely an embodiment of this application, and the scope of protection of this application is not limited to these specific embodiments, but is determined by the claims of this application. Various modifications and variations can be made to this application by those skilled in the art. Any modifications, equivalent substitutions, improvements, etc., made within the technical concept and principles of this application should be included within the scope of protection of this application.

Claims

1. A compound biological insect repellent preparation made from traditional Chinese medicine, characterized in that, From the outside to the inside, it includes an immediate-release insecticidal layer, an isolation buffer layer, and a slow-release layer. The immediate-release insecticidal layer is loaded with traditional Chinese medicine extracts, the slow-release layer is loaded with compound functional microbial powder, and the isolation buffer layer is located between the immediate-release insecticidal layer and the slow-release layer to prevent the traditional Chinese medicine extracts from directly contacting the compound functional microbial powder. According to the weight percentages, the quick-release insecticidal layer comprises 35-45 parts of traditional Chinese medicine extract, 5-15 parts of water-soluble quick-release wall material, and 1-2 parts of penetrant; The isolation buffer layer comprises 3-5 parts sodium alginate and 2-3 parts chitosan; The slow-release layer comprises 10-15 parts of composite functional bacterial powder and 10-20 parts of slow-release wall material.

2. The herbal compound biological insect repellent preparation according to claim 1, characterized in that, The water-soluble, fast-release wall material comprises pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester, and β-cyclodextrin; the mass ratio of the pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester, and β-cyclodextrin is (3~5):(1~2):(1~3):(1~2); The penetrant includes polyether-modified trisiloxane; The slow-release wall material comprises plant beeswax, stearic acid and hydrophobically modified cellulose, wherein the mass ratio of plant beeswax, stearic acid and hydrophobically modified cellulose is (6~8):(8~10):(6~7).

3. The herbal compound biological insect repellent preparation according to claim 1, characterized in that, The raw materials of the herbal extract are composed of the following components in the following weight ratio: 8-12 parts garlic, 6-10 parts chili pepper, 5-8 parts pine needles, 4-6 parts pine resin, 5-7 parts oregano, and 6-9 parts calamus. The compound functional bacterial powder is composed of the following components in the following weight ratios: 4-6 parts of Bacillus belye powder, 2-4 parts of Bacillus pumilus powder, 2-4 parts of Beauveria bassiana powder, and 1-3 parts of Paecilomyces lilacinus powder.

4. The herbal compound biological insect repellent preparation according to claim 3, characterized in that, The extracts of garlic, pine needles, pine resin, oregano, and acorus calamus in the herbal extracts are volatile oils, and the extract of chili pepper is a concentrated extract; the mass ratio of volatile oil to concentrated extract in the herbal extracts is (8~12):(20~25).

5. The herbal compound biological insect repellent preparation according to claim 3, characterized in that, The effective viable count of the *Bacillus vesiculosus* powder is ≥8.0 × 10⁻⁶. 8 CFU / g, the effective viable count of the *Bacillus pumilus* powder is ≥5.0 × 10⁻⁶. 8 CFU / g, the effective viable count of the *Beauveria bassiana* powder is ≥5.0 × 10⁻⁶. 8 CFU / g, conidia ≥4.0×10 8 The effective viable count of the *Paecilomyces lilacinus* powder is ≥5.0 × 10⁻⁶ cells / g; 8 CFU / g.

6. The herbal compound biological insect repellent preparation according to claim 2, characterized in that, The isolation buffer layer also includes 0.5 to 1.5 parts of porous diatomaceous earth powder; the slow-release layer also includes 15 to 20 parts of nutrient carrier and 1 to 3 parts of humic acid powder; the nutrient carrier includes soybean meal powder and corn starch powder, with a mass ratio of 1:(1 to 1.3).

7. The method for preparing the herbal compound biological insect repellent preparation according to any one of claims 1 to 6, characterized in that, Includes the following steps: (1) Crush garlic, pine needles, pine resin, oregano, and sweet flag and add them to a distillation kettle. Add deionized water and perform normal pressure steam distillation. Let the distillate stand to separate into layers. Take the upper transparent oil phase, dehydrate and remove impurities to obtain volatile oil. Crush chili peppers and add 50-60% ethanol as a solvent for ultrasonic extraction 2-3 times. The mass-volume ratio of chili peppers to ethanol is 1:(3-4). Collect the filtrate and concentrate it under vacuum to obtain concentrated extract. Mix the volatile oil and concentrated extract according to the weight ratio and set aside. (2) Mix and stir the Bacillus vesiculosus powder, Bacillus pumilus powder, Beauveria bassiana powder and Paecilomyces lilacinus powder evenly and set aside. (3) Preparation of slow-release core: Plant beeswax, stearic acid and hydrophobic modified cellulose are heated to 60~70℃ and melted according to the formula. Stirred until completely liquefied to obtain molten slow-release wall material; Composite functional bacterial powder, nutrient carrier, humic acid micro powder and molten slow-release wall material are mixed evenly, and microspheres are formed by centrifugal granulation and dried at low temperature to obtain slow-release core. (4) Coating the isolation buffer layer: Sodium alginate, chitosan and porous diatomaceous earth powder are mixed with water to form a uniform film-forming liquid with a solid content of 2%~3%. The slow-release core is placed in a fluidized bed coating machine and sprayed onto the surface of the slow-release core using fluidized bed atomization. The air inlet temperature is 35~40℃. After cross-linking and curing, a 5~10μm isolation buffer layer is formed. (5) Coating with an instant-release insecticidal layer: Pregelatinized starch, sodium carboxymethyl cellulose, sucrose ester, and β-cyclodextrin are mixed, and volatile oil, concentrated chili extract, and polyether-modified trisiloxane are added. The mixture is stirred at room temperature to prepare a viscosity coating solution. The instant-release insecticidal layer is coated under hot air conditions at 40~45℃ and dried to obtain a traditional Chinese medicine compound biological insect repellent preparation.

8. The preparation method of the herbal compound biological insect repellent preparation according to claim 7, characterized in that, In step (1), the amount of deionized water added is 4 to 6 times the total mass of the Chinese herbal medicine, the temperature of steam distillation is 95 to 100℃, and the distillation time is 2 to 3 hours; the extraction temperature of ultrasonic extraction is 40 to 50℃, the ultrasonic power is 300 to 500W, and the extraction time is 60 to 90 minutes per extraction; in step (3), the particle size of the microspheres is 100 to 200 μm, the temperature of low-temperature drying is 40 to 45℃, and the drying time is 2 to 3 hours.

9. The application of the herbal compound biological insect repellent preparation according to any one of claims 1 to 6 in the control of thrips, spider mites, and aphids.

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