Repelling and poisoning synergistic type artemisia apiacea-tolfenpyrad pharmaceutical composition and application thereof

Abstract

The invention discloses a repelling and poisoning synergistic type artemisia apiacea-tolfenpxrad pharmaceutical composition and application thereof, the active ingredients of the pharmaceutical composition are composed of artemisia apiacea extract and tolfenpxrad, and the mass ratio of the artemisia apiacea extract to the tolfenpxrad is 1: 0.1-1: 1. The pharmaceutical composition obtained by compounding the artemisia apiacea extract and the tolfenpyrad can generate better repelling and poisoning effects on the red weevil and the rhinoceros rhinoceros, the prevention and treatment effects on the red weevil and the rhinoceros rhinoceros are improved, the pollution to the environment and pesticide residues can be reduced, and the pharmaceutical composition is worthy of popularization and application. Ecological prevention and control of palm plant pests such as red palm weevils and rhinoceros rhinoceros are facilitated, and the method is of great significance to prevention and control of palm plant pests.

Description

Technical Field

[0001] This invention relates to the field of pesticide technology, and in particular to a synergistic repellent and toxic artemisinin-acetamide drug composition and its application. Background Technology

[0002] Palm trees are plants of extremely high economic value globally. Among them, oil palm and coconut are important woody oil crops that play a vital role in ensuring international edible oil security.

[0003] The red palm weevil and the two-spotted rhinoceros beetle are devastating pests of palm trees, including coconut, oil palm, and date palm. Red palm weevil larvae bore into the trunk, causing necrosis of the growing point and rapid plant death. Adult two-spotted rhinoceros beetles bore into the heart leaves of the crown, causing leaf breakage and crown deformities. Both pests are characterized by their insidious nature, difficulty in detection, and short window for control. Once they infest, conventional pesticides are often ineffective, resulting in significant economic losses and ecological damage.

[0004] Currently, the control of red palm weevils and rhinoceros beetles mainly relies on chemical pesticides, but this approach has significant limitations: First, while highly toxic organophosphate pesticides such as chlorpyrifos and phoxim are effective for a certain period, they lead to serious pesticide residues, environmental pollution, increased pest resistance, and the risk of poisoning in humans and animals. With increasing global environmental awareness and stricter pesticide regulations, these highly toxic pesticides are being gradually restricted or banned, necessitating the development of environmentally friendly alternatives. Second, existing conventional chemical pesticides have limited components and a single mode of action. Some currently used pesticides, such as neonicotinoids like imidacloprid and thiamethoxam, while having toxic effects, lack effective repellency. This means that pests can still come into contact with and feed on plants through non-application sites. Especially for boring pests like red palm weevils, preventing oviposition and initial invasion is the first line of defense (repellency) and a crucial element in demonstrating control effectiveness; relying solely on toxicity is passive and inefficient.

[0005] Therefore, based on the above reasons, developing a low-toxicity, highly effective, and repellent agent for the red palm weevil and the two-spotted rhinoceros beetle has become an urgent need for the palm industry to control pests. Summary of the Invention

[0006] The purpose of this invention is to provide a highly efficient and long-lasting artemisinin-acetamide synergistic repellent and toxic agent composition for the control of palm pests, the red palm weevil and the two-spotted rhinoceros beetle, achieving a synergistic effect of "repelling" and "killing" against the red palm weevil and the two-spotted rhinoceros beetle, thereby improving the control effect.

[0007] To achieve the objectives of this invention, a first aspect of this invention is to provide a synergistic repellent and toxic artemisinin-acetamide pharmaceutical composition, wherein the active ingredient of the pharmaceutical composition is composed of artemisia annua extract and acetamide, and the mass ratio of artemisia annua extract to acetamide is 1:0.1 to 1:1.

[0008] In one optional embodiment, the artemisia extract is an ethanol extract, methanol extract, water extract, petroleum ether extract, or volatile oil of artemisia.

[0009] A second aspect of the present invention is to provide a synergistic repellent and toxic artemisinin-azoxystrobin compound formulation, the compound formulation comprising the aforementioned pharmaceutical composition and pesticide-acceptable excipients.

[0010] In one optional embodiment, the dosage form of the compound preparation is a spray, powder, soluble concentrate, or granules.

[0011] A third aspect of the invention is to provide the application of the pharmaceutical composition or the compound formulation described herein in the control of pests on palm trees.

[0012] In one alternative embodiment, the palm pests are the red palm weevil and the two-spotted rhinoceros beetle.

[0013] A fourth aspect of the present invention is to provide a method for controlling pests on palm plants, comprising applying an effective amount of the pharmaceutical composition or a compound preparation thereof to the palm plant, its growing environment, or the parts of the plant that are damaged.

[0014] In one alternative embodiment, the application method includes spraying, sprinkling, and packing.

[0015] In one alternative embodiment, the spraying method involves diluting the sprayable liquid and spraying it onto the trunk, leaf sheath base, and growing point; the spreading method involves applying the powder to the leaf axils, leaf sheath crevices, and tree wounds; and the sachets method involves placing a carrier loaded with the drug composition or compound preparation into a breathable packaging bag, and then fixing the packaging bag to the leaf axils, growing point base, or pest intrusion holes.

[0016] Compared with the prior art, the present invention has the following beneficial effects: This invention presents a pharmaceutical composition obtained by combining artemisia annua extract with acetamiprid, which has a highly effective repellent effect on pests, low toxicity, and good killing effect. It can prevent pests from laying eggs and feeding at the initial stage of contact with crops through strong repellency, while simultaneously exerting a highly effective killing effect on those pests that persist in invading despite being repelled, forming a dual defense line of "repellency-killing". This achieves synergistic effect, delays resistance development, reduces pesticide dosage, and improves the overall protection level of palm plants, which is of great significance for the control of palm plant pests. Detailed Implementation

[0017] The following examples are used to illustrate the present invention, but are not intended to limit the scope of the invention. Unless otherwise specified, the technical means used in the examples are conventional means well known to those skilled in the art, and the raw materials used are all commercially available products.

[0018] I. Preparation of Combination Drugs

[0019] Example 1 Weigh 50 g of Artemisia annua ethanol extract (obtained by reflux extraction of dried Artemisia annua powder with ethanol and then concentration). Slowly add 60 g of silica to the extract in a mixer, stirring and crushing continuously until a dry, flowable Artemisia annua extract mother powder is formed. Premix 25 g of 95% acetamiprid with 865 g of diatomaceous earth filler, and pulverize to 800 mesh using an air jet mill to obtain acetamiprid-diatomaceous earth premix. Add the Artemisia annua extract mother powder and the acetamiprid-diatomaceous earth premix to the mixer and mix. After mixing evenly, a compound powder is obtained.

[0020] Example 2 Weigh 100 g of Artemisia annua ethanol extract (obtained by reflux extraction of dried Artemisia annua powder with ethanol and then concentration) and 20 g of 95% acetamiprid, dissolve them in 120 g of mixed solvent (composed of xylene and cyclohexanone, xylene:cyclohexanone = 1:1), then add 25 g of agricultural emulsion 500, stir well to form a drug solution, and slowly add the above drug solution to 735 g of melted petrolatum (heated in a 65°C water bath) while stirring, continue stirring until it cools and solidifies to form a uniform coating.

[0021] Example 3 Weigh 36 g of 95% acetamiprid and dissolve it in 135 mL of acetone. Stir until completely dissolved to prepare an acetamiprid-acetone solution. Weigh 45 g of Artemisia annua ethanol extract and dissolve it in 20 mL of ethanol to prepare an Artemisia annua ethanol extract solution. Under continuous mechanical stirring, slowly add the Artemisia annua ethanol extract solution to the above acetamiprid-acetone solution to mix thoroughly. Add 15 g of soybean oil and 5 g of Tween-80 and continue stirring for 30 minutes to form a homogeneous mixture. Remove acetone and ethanol by vacuum distillation (water bath temperature 45℃, vacuum degree 0.09 MPa) until no solvent is distilled off. After distillation, cool to room temperature to obtain the compound oil.

[0022] II. Killing and repelling effects of the drug composition on adult red brown weevils and two-spotted rhinoceros beetles in their chambers. (a) Indoor toxicity effect experiment The agents obtained in Examples 1, 2, and 3 were used to conduct indoor toxicity experiments on adult red brown weevils and two-spotted rhinoceros beetles, respectively: 1) Experimental Method 1: Take 24 insect rearing boxes of 40×35×25cm. Sprinkle the powder of Example 1 evenly on the bottom of 6 of the insect rearing boxes. Place 25 adult two-spotted rhinoceros beetles in 3 of the boxes and 25 adult red brown weevils in 3 of the boxes. The other 12 insect rearing boxes are used as controls. Control I (no pesticide, 6 insect rearing boxes), Control II (sprinkled with acetamiprid powder, 6 insect rearing boxes), and Control III (sprinkled with powdered Artemisia annua ethanol extract (the obtained Artemisia annua ethanol extract (same as in Example 1) is prepared into powder using conventional production process (vacuum drying + pulverization)), 6 insect rearing boxes). Place 25 adult two-spotted rhinoceros beetles in 3 of the boxes in Control I and 25 adult red brown weevils in the other 3 boxes. The same applies to Control II and Control III.

[0023] 2) Experimental Method Two: The agent obtained in Example 2 was applied to the base of the leaf sheaths of coconut palm leaves after they were cut and trimmed. Then, 25 adult *Rhinoceros beetle* and 25 adult *Red brown weevil* were inoculated onto each of the 10 leaf sheath bases (5 of which were inoculated with *Rhinoceros beetle* and the other 5 with *Red brown weevil*, averaging 5 *Rhinoceros beetle* and 5 *Red brown weevil* per leaf sheath base). Leaf sheath bases without agent treatment were used as Control I, leaf sheath bases treated with acetamiprid were used as Control II, and leaf sheath bases treated with powdered *Artemisia annua* ethanol extract (prepared as in Experimental Method One) were used as Control III. Each treatment was repeated 3 times.

[0024] 3) Experimental Method Three: The compound oil preparation obtained in Example 3 was sprayed evenly and thoroughly onto the base of the cut and trimmed coconut leaf sheaths using a sprayer. Then, 25 adult two-spotted rhinoceros beetles and 25 adult red-brown weevils were inoculated separately (a total of 10 leaf sheath bases were used, with 5 inoculated with two-spotted rhinoceros beetles and the other 5 with red-brown weevils, averaging 5 two-spotted rhinoceros beetles and 5 red-brown weevils per leaf sheath base). Leaf sheath bases without pesticide treatment were used as Control I, leaf sheath bases sprayed with acetamiprid were used as Control II, and leaf sheath bases sprayed with the Artemisia annua ethanol extract (the Artemisia annua ethanol extract prepared in Example 1 was slowly added to preheated soybean oil (preheating temperature 45℃) under continuous stirring, with a mass ratio of Artemisia annua ethanol extract to soybean oil of 1:3) were used as Control III. Each treatment was repeated 3 times.

[0025] Effects: The inability of test insects to crawl normally was used as the criterion for mortality. The number of dead insects was counted 120 hours after treatment, and the mortality rate was calculated. The experimental results on the effect on the two-spotted rhinoceros beetle are shown in Table 1, and the experimental results on the effect on the red-brown weevil are shown in Table 2.

[0026] Table 1. Mortality rates of *Rhinoceros tigrinus* under different treatments.

[0027]

[0028] Table 2. Mortality rates of red-brown weevils under different treatments.

[0029]

[0030] The results of the indoor studies shown in Table 1 above demonstrate that the toxic effect of the pharmaceutical composition provided by this invention against *Rhinoceros beetle* is significantly higher than that of control I (average mortality rate of 6.7%) in experimental method 1 without application, control I (average mortality rate of 4.0%) in experimental method 2 without application, and control I (average mortality rate of 2.7%) in experimental method 3 without application; control II (average mortality rate of 61.3%) in experimental method 1 with acetamiprid alone, control II (average mortality rate of 65.3%) in experimental method 2, and control II (average mortality rate of 76.0%) in experimental method 3 with acetamiprid alone; control III (average mortality rate of 17.3%) in experimental method 1 with Artemisia annua extract alone; control III (average mortality rate of 18.7%) in experimental method 2 with Artemisia annua extract alone; and control III (average mortality rate of 20.0%) in experimental method 3 with Artemisia annua extract alone. In treatment of 96... After h, the mortality rate of adult two-spotted rhinoceros beetles reached over 90%, demonstrating a good killing effect on adult two-spotted rhinoceros beetles and achieving excellent control results.

[0031] The results of the indoor studies in Table 2 show that the toxic effect of the pesticide composition provided by this invention against the red palm weevil is as follows: Compared to the control group I (average mortality rate of 8.0%) of Experiment 1 without pesticide application, the control group I (average mortality rate of 2.7%) of Experiment 2 without pesticide application, the control group I (average mortality rate of 5.3%) of Experiment 3 without pesticide application, the control group II (average mortality rate of 60.0%) of Experiment 1 with acetamiprid alone, the control group II (average mortality rate of 69.3%) of Experiment 2 with acetamiprid alone, and the control group II (average mortality rate of 74.7%) of Experiment 3 with acetamiprid alone, the control group III (average mortality rate of 21.3%) of Experiment 1 with Artemisia annua extract alone, the control group III (average mortality rate of 17.3%) of Experiment 2 with Artemisia annua extract alone, and the control group III (average mortality rate of 22.7%) of Experiment 3 with Artemisia annua extract alone, in the treatment of 96... After h, the mortality rate of adult two-spotted rhinoceros beetles reached over 91%, and it had a good killing effect on adult red-brown weevils, achieving a very good control effect.

[0032] (II) Indoor Attraction / Repulsion Effect Experiment The agents obtained in Examples 1, 2, and 3 were used to conduct indoor repellency experiments against adult two-spotted rhinoceros beetles and red brown weevils: Take the agents obtained in Examples 1, 2, and 3, and apply them evenly (Example 2), spray (Example 3), or sprinkle (Example 1) on the fresh coconut leaf sheaths that have been pruned. Specifically, make multiple wounds on the pruned coconut leaf sheaths, apply the agent to these wounds, and then place the coconut leaf sheaths on one side of a homemade insect rearing box measuring 160×120×80cm. Introduce 30 two-spotted rhinoceros beetles and 30 red brown weevils into different insect rearing boxes. Coconut leaf sheaths without pesticides were used as control I (blank treatment); coconut leaf sheaths treated with camphor oil (1.5% concentration) were used as control II (containing only 30 *Hemiberlesia lataniae*); coconut leaf sheaths treated with garlic oil (1.5% concentration) were used as control III (containing only 30 *Hemiberlesia lataniae*); coconut leaf sheaths treated with *Artemisia argyi* extract (powder, prepared according to "Experimental Method 1" above) were used as control IV (containing only 30 *Hemiberlesia lataniae*); and coconut leaf sheaths treated with *Artemisia argyi* extract (powder, prepared according to "Experimental Method 1" above) were used as control V (containing only 30 *Hemiberlesia lataniae*). Each treatment was repeated three times, and the number of crawling insects on the coconut leaf sheaths was counted after 72 h to calculate the effectiveness rate. Temperature and humidity parameters were kept consistent in all rearing boxes. The results are shown in Tables 3 and 4. Table 3. Climbing behavior of *Rhinoceros tigrinus* under different treatments

[0033] Table 4 Climbing behavior of red-brown weevils under different treatments

[0034] The experimental data in Tables 3 and 4 above show that the composition provided by the present invention effectively combines acetamiprid and artemisia annua extract, and has a good repellent effect on rhinoceros beetle and red palm weevil, with an efficacy rate of 90% or more. This is beneficial for the ecological control of palm plant pests and is of great significance for protecting palm plants from damage.

[0035] III. The therapeutic effects of the drug composition on the two-warted rhinoceros beetle or the red-brown weevil. (I) Experimental Materials: Three coconut plantations were selected in Wenchang City, Hainan Province, and labeled A1, A2, and A3 respectively. Forty mature coconut trees were selected from each plantation as experimental trees, for a total of 120 coconut trees. They were divided into Group I (A1), Group II (A2), and Group III (A3).

[0036] (II) Experimental Methods: In August 2025, 10 trees were randomly selected from the experimental trees in each plantation as drug-treated trees and 30 trees were selected as control trees. The drug-treated trees in different plantations were treated with the drug compositions obtained in Examples 1, 2 and 3 respectively. Specifically, drug packets (the powder obtained in Example 1 was taken and put into a customized breathable non-woven fabric bag, each packet containing 15 g of powder, sealed, and made into a repellent and insecticide packet) were fixed at the canopy of the drug-treated trees in Group I, drug packets were applied to the canopy of the drug-treated trees in Group II (Example 2), and drug packets were sprayed at the canopy of the drug-treated trees in Group III (Example 3). The control trees were divided into: 10 trees in Control I (no drug applied to the canopy), 10 trees in Control II (azathioprine applied to the canopy), and 10 trees in Control III (camphor balls hung at the canopy). In this case, the form of the acetamiprid applied in Control II was the same as that in each of the embodiments. Specifically, in comparison with Example 1, the acetamiprid applied in Control II was in the form of a sachet (the same amount of powder as in Example 1 was placed in a custom-made breathable non-woven fabric bag). In comparison with Example 2, the acetamiprid applied in Control II was a topical application (the same dosage as in Example 2). In comparison with Example 3, the acetamiprid applied in Control II was an oil (the same dosage as in Example 3).

[0037] Fine sticky insect nets were placed in the heart of the tree canopy. The presence of red-brown weevils or two-spotted rhinoceros beetles on the sticky insect nets was used to determine whether an invasion had occurred.

[0038] (III) Experimental results: In September 2025, a comprehensive survey was conducted on coconut plantations “A1, A2, A3”. The number of pests (two-spotted rhinoceros beetle or red palm weevil) on the webs was counted and the effectiveness rate was calculated. The results are shown in Table 5.

[0039] Table 5. Effects of the drug composition on the prevention and control of red-brown weevils or two-warted rhinoceros beetles.

[0040] The results in Table 5 above show that the combined pesticide provided by the present invention has a higher efficacy against pests than the blank treatment (control I) with a maximum effective rate of 60.0%, the single chlorpyrifos treatment (control II) with a maximum effective rate of 80.0%, and the single hanging repellent treatment (control III) with a maximum effective rate of 70%. The present invention can achieve a maximum effective rate of 100%, effectively preventing the invasion of red palm weevil larvae or two-spotted rhinoceros beetle larvae from the tree canopy, and has a better control effect.

[0041] Although the present invention has been described in detail above with general descriptions and specific embodiments, modifications or improvements can be made to it, which will be obvious to those skilled in the art. Therefore, all such modifications or improvements made without departing from the spirit of the present invention fall within the scope of protection claimed by the present invention.

Claims

1. A synergistic repellent and toxic artemisinin-azoxystrobin drug composition, characterized in that, The active ingredient of the pharmaceutical composition consists of artemisia annua extract and acetamiprid, wherein the mass ratio of artemisia annua extract to acetamiprid is 1:0.1 to 1:

1.

2. The artemisinin-azoxystrobin synergistic repellent and toxic drug composition according to claim 1, characterized in that, The artemisia extract is an ethanol extract, methanol extract, water extract, petroleum ether extract, or volatile oil of artemisia.

3. A synergistic repellent and toxic artemisinin-azoxystrobin compound formulation, characterized in that, The compound formulation comprises the pharmaceutical composition of any one of claims 1-2, and pesticide-acceptable excipients.

4. The synergistic repellent and toxic artemisinin-azoxystrobin compound formulation according to claim 3, characterized in that, The dosage form of the compound preparation is a spray, powder, soluble solution, or granules.

5. The use of the pharmaceutical composition according to any one of claims 1-2 or the compound preparation according to any one of claims 3-4 in the control of pests on palm trees.

6. The application according to claim 5, characterized in that, The palm pests mentioned are the red palm weevil and the two-spotted rhinoceros beetle.

7. A method for controlling pests on palm trees, characterized in that, Apply an effective amount of the pharmaceutical composition according to any one of claims 1-2, or an effective amount of the compound preparation according to any one of claims 3-4, to a palm plant, its growing environment, or its affected parts.

8. The method for controlling pests of palm trees according to claim 7, characterized in that, The application methods include spraying, sprinkling, and packing.

9. The method for controlling pests of palm trees according to claim 8, characterized in that, The spraying method involves diluting the sprayable liquid and spraying it onto the trunk, leaf sheath base, and growing point; the spreading method involves applying the powder to the leaf axils, leaf sheath crevices, and tree wounds; and the sachets method involves placing a carrier containing the drug composition or compound preparation into a breathable packaging bag, and then fixing the packaging bag to the leaf axils, growing point base, or insect intrusion holes.

Images