KR100341056B1 - Natural mosquito repellents - Google Patents

Abstract

The present invention includes p-cymene including eucalyptus leaf extract oil, lavender leaf extract oil, rosemary leaf extract oil, or thyme extract oil or separated from the thyme extract oil. ), α-terpinene, linalool, cavacrol (cavacrol) and thymol comprising a mosquito repellent comprising one or more compounds selected from the group consisting of. Eucalyptus globulus as the eucalyptus, Lavender officinalis as a lavender tree, Rosemarinus officinalis as a rosemary tree and Thymus vulgaris as a thyme are preferably used.

Description

NATURAL MOSQUITO REPELLENTS

Field of invention

The present invention relates to a natural mosquito repellent having excellent mosquito repellent activity and a sustaining effect, and more particularly, to a natural mosquito repellent comprising an extract oil prepared by steam distillation from a natural plant or a compound separated from the extract oil. .

Prior art

Mosquitoes are not only blood-sucking humans or animals, but also mediate various diseases such as malaria, encephalitis, yellow fever, and dengue fever. About 53 species of mosquitoes are known in Korea. Among them, the Chinese spotted mosquito ( Anopheles sinensis ) mediates malaria and inland Brugian Filariasis, and the Aedes togoi mosquitoes in the southwestern region. , The red conglomerate ( Culex triaeniorhynchus ) spreads Japanese encephalitis, and the red conglomerate ( Culex pipiens pallens ) and the underground conglomerate ( Culex pipiens molestus ) belong to the conglomerate and have recently been controlled by blood-sucking problems Is inevitable.

In order to control these mosquitoes, chemical control by insecticides is mainly used. However, these synthetic chemical insecticides have side effects such as development of drug resistance, toxicity to humans or animals, and environmental pollution. There has been a need to develop new methods of control or alternatives that can effectively protect humans from mosquitoes while minimizing this risk (Geroghiou and Saito, 1983; National Research Council, 1986; Brown, 1078).

Under these circumstances, the demand for mosquito repellents that can effectively prevent insect-borne diseases and have less environmental impact has increased. Conventionally known repellents include citronella oil, dimethylphthalate (DMP), etc., but lack repellent activity. Since then, N, N-diethyl-m-toluamide (DEET) with excellent repelling activity has been developed and used throughout pests such as mosquitoes, mosquitoes, flies, teeth, fleas and ticks. However, DEET has excellent repelling effect as a synthetic repellent, but it has an unpleasant irritant odor, damages glasses or watch bands by reacting with plastic or synthetic rubber, and has a high skin penetration, so it can cause brain disease, seizures, mental disorders, cardiovascular effects. There is a problem that causes toxicity, hypersensitivity, and the like. Therefore, pyridostigmine bromide or chloropyrifos in combination with DEET is used to suppress such side effects, but it is difficult to apply to children, patients with hypotension, and those who are sensitive to skin (Hongchun et al. al., 1998. Pharmacokinetic, formulation, and safety of insect repellent N, N-diethyl-3-methylbenzamide (DEET): a review.J. Am. Mosq.Control Assoc. 14 (1): 12-27)

Therefore, in recent years, research on natural extracts or compounds derived from natural products has been actively conducted. For example, many secondary metabolites such as plant extracts, terpenes, phenols, and alkaloids, have low toxicity to humans or animals, are simple to treat like conventional pesticides, are effective only for limited pests such as target pests, and have low impact on natural enemies. As a result, it has attracted attention as an alternative drug for synthetic repellents.

However, natural mosquito repellents that exhibit the same degree of repellent activity and sustaining effects as synthetic repellents such as DEET have not been developed.

It is an object of the present invention to provide a natural mosquito repellent which is not only excellent in mosquito repellent activity, but also has a sustained effect, no toxicity to humans or animals, a simple treatment method, no irritating odor, and no possibility of environmental pollution. It is to.

In order to achieve the above object of the present invention, mosquito repellents have excellent mosquito repellent activity Eucalyptus leaf (Eucalyptus) extract oil, lavender leaf (Lavender) extract oil, Rosemary leaf (Rosemary) extract oil, or Thyme extract oil To provide. In addition, one or more compounds selected from the group consisting of p-cymene, α-terpinene, linalool, cavacrol and thymol isolated from the thyme extract oil It provides a mosquito repellent containing.

Hereinafter, the present invention will be described in more detail.

The mosquito repellent according to the present invention includes p-cymene, α-terpinene, linarol, cabarcrol, including eucalyptus leaf extract oil, lavender leaf extract oil, rosemary leaf extract oil, or thyme extract oil. , One or more compounds of thymol. Eucalyptus globulus as eucalyptus, Lavender officinalis as lavender, Rosemarinus officinalis as rosemary and Thymus vulgaris as thyme are preferably used.

Extracted oil of the present invention is prepared by steam distillation. First, the plants to be extracted are dried well, cut, put into a flask, and about 10 times or more water is added to the flask containing the sample, and an organic solvent corresponding to 1/10 of the distilled water volume is added to the other flask. To reflux for several hours. Then, the mixture was slowly cooled, the organic solvent layer was taken out, dehydrated by addition of a dehydrating agent, and then filtered to remove the dehydrating agent, and the filtrate was prepared by evaporation.

The extract oil is a solution oil having a herb flavor, eucalyptus and lavender extract oil is a colorless oil and rosemary and thyme extract oil is a light tan oil. P-cymene, α-terpinene, linarol, carbacroll, and thymol, which are separated from the thyme extract oil, are in turn represented by the following chemical formula. Of course, the compounds may be synthesized by conventional techniques in the art.

p-cymene α-terpinene linarol carbacromol thymol

The natural mosquito repellent of the present invention may be used together with N, N-diethyl-m-toluamide (DEET) which is a plant extract oil or a compound separated therefrom. At this time, the mixing ratio of natural mosquito repellent and synthetic mosquito repellent is preferably 1: 0.1 to 0.4. If the mixing ratio is out of the range, there is a problem that the repellent effect is not high.

The following presents examples in more detail to help understand the present invention. However, the following examples are merely provided to more easily understand the present invention, and the present invention is not limited to the following examples.

Examples and Comparative Examples

Example 1

50 g of Eucalyptus globulus leaves were dried and cut, added to a 500 ml flask, distilled water was added, 50 ml of hexane was added to the other flasks, and the two flasks were connected with cooling water and heated to reflux for 5 hours. After refluxing, the mixture was slowly cooled and the flask containing hexane was separated, and MgSO ₄ was added to the hexane layer to dehydrate and filtered. The filtrate was evaporated at 25 ℃ to prepare a eucalyptus extract oil in a colorless solution. This extracted oil was diluted to 5000 ppm with 0.1% ethanol.

Examples 2-4

Instead of the eucalyptus tree used in Example 1, Lavender officinalis in Example 2, Rosemarius officinalis in Example 3, and used Thymus vulgaris in Example 4 Except for the extraction oil was prepared in the same manner as in Example 1. In the case of Examples 3 and 4, the extracted oil after distillation was light yellowish brown, and diluted with 5000 ppm by adding 0.1% ethanol to prepare a white extracted oil.

Comparative Example 1

24% N, N-diethyl-m-toluamide (DEET) (Mosquito Milk, Jaico N.V., Belgium) was used as a mosquito repellent.

Evasion Effect Test on Rats

F-265-day larvae of 500 female red- backed mosquitoes, Culex pipiens pallens Coquillett, were purchased from KFDA, with a temperature of 27 ± 2 ° C, 75-80% relative humidity, and 8% sugar / water pads under natural light conditions. Was fed to grow. Of these, 6 to 7 days old female mosquitoes were placed in a wire mesh cut to 30 × 30 × 30 cm, each with 100 mosquitoes. The sugar / water pad was removed from the wire net 12 hours before the experiment. Twenty-five male mice (SKH-1 HRBR Hairless mice, 7 weeks old, 26-38 g, Charles River, Japan) were placed in a cage in a temperature- and humidity-controlled room with five dogs and feed (Samyang Corporation). And water were paid indefinitely. Mice were identified by marking on the tail. Five rats were indiscriminately treated with 0.1% ethanol (control) and the extracted oils of Examples 1 to 4 by rubbing the whole body with sanitary cotton. Treated mice were transferred to a net containing 100 mosquitoes. The wire mesh was placed 10 cm above the workbench to ensure good air circulation during the test. The number of mosquito bites was recorded at 5 minute intervals for 1 hour and the total number of bites was investigated. The total number of bites and the avoidance time until three bites were measured five times, and the average is shown in Table 1 below. Protection rate is calculated according to the following formula and shown in Table 1.

Evasion rate = number of bites in rats treated with 1-extract oil / number of control bites × 100

Processed material Total number of bites ^* Evasion rate (%) Evasion time until 3 bites ^* No treatment (control) 17.2 ± 1.64 - 17.8 ± 1.92 min Example 1 5.2 ± 0.84 70 33.2 ± 4.09 min Example 2 6.0 ± 1.00 65 31.0 ± 3.67 min Example 3 4.0 ± 1.71 77 47.0 ± 8.28 min Example 4 1.6 ± 1.34 91 65.4 ± 12.22 min

Note) *: Mean ± Standard Deviation

As described in Table 1, it can be seen that the rat treated with the extract oil of the present invention has excellent repellent activity.

P-cymene, α-terpinene, linarol, carbacroll and thymol isolated from the extracting oil of Example 4 were tested in the same manner as in the respiratory activity experiment in mice of the extracting oils of Examples 1 to 4 Table 2 shows.

Processed material Total number of bites ^* Evasion rate (%) Evasion time until 3 bites ^* p-cymen 2.6 ± 0.98 85 59.1 ± 9.22 min α-terpinene 1.7 ± 1.30 90 62.7 ± 10.27 min Linarol 1.9 ± 1.54 89 60.3 ± 11.15 min Kabakrole 1.1 ± 1.23 96 70.0 ± 13.21 min Thymol 1.0 ± 1.43 97 72.1 ± 12.32 min

Note) *: Mean ± Standard Deviation

In addition, the extraction oil of Examples 1 to 4 for the extracted oil of Example 4 and N, N-diethyl-m-toluamide (DEET), which is a conventional synthetic mosquito repellent, at a mixing ratio shown in Table 3 below. The experiment was carried out in the same manner as the repellent activity test for rats are shown in Table 3 below.

Mixing ratio of treated materials Total number of bites ^* Evasion rate (%) Evasion time until 3 bites ^* 1: 0.1 1.8 ± 0.98 91 66.1 ± 7.25 min 1: 0.2 1.9 ± 2.30 89 61.2 ± 8.15 min 1: 0.3 2.9 ± 1.09 86 60.3 ± 10.21 min 1: 0.4 3.0 ± 1.23 84 58.0 ± 13.07 min

Note) *: Mean ± Standard Deviation

In case of 20% concentration of N, N-diethyl-m-toluamide (DEET), which is a synthetic mosquito repellent, it was reported that the avoidance time until 3 bites of Anopheles ditus was 52.5 min. Frances et al. (1993) Response of Anopheles dirus and Aedes albopictus to repellents in the laboratory, J. Am. Mosq. Conrol. Assoc., 9; 474-476).

Evasion effect test on human

F-265-day larvae of 750 female red- crowned mosquitoes, Culex pipiens pallens Coquillett, were purchased from KFDA, with a temperature of 27 ± 2 ° C, 75-80% relative humidity, and 8% sugar / water pads under natural light conditions. Was fed to grow. Six to seven days old female mosquitoes were placed in a wire mesh cut into 30 × 30 × 30 cm of 50 mosquitoes each. The sugar / water pad was removed from the wire net 12 hours before the experiment. A 5 cm2 wrist joint of a healthy man 176 cm tall and weighing 60 kg, using a sanitary cotton, 0.1% ethanol (control), 5000 ppm extracted oil (Example 4), and 24% N, N-diethyl -m-toluamide (Comparative Example 1) was rubbed. The treated arms were placed in a net containing 50 mosquitoes. The wire mesh was placed 10 cm above the workbench to ensure good air circulation during the test. The number of mosquitoes gathered in the arm was recorded at 2 minute intervals for 30 minutes and the total number was examined. The total number of mosquitoes and the evacuation time until 3 bites were measured repeatedly for 30 minutes, and the average value and the evasion rate were also calculated from Table 4 below.

Processed material Total number of bites ^* Evasion rate (%) Evasion time until 3 bites ^* No treatment (control) 18.0 ± 2.24 - 5.6 ± 2.24 min Example 4 1.0 ± 0.71 94 71.6 ± 9.18 min Comparative Example 1 2.0 ± 0.71 89 47.2 ± 13.74 min

Note) *: Mean ± Standard Deviation

As shown in Table 4, the extraction oil of Example 4 of the present invention has a repellency rate and repellency time, even though the concentration of the extract oil was diluted 1000 times or more than that of N, N-diethyl-m-toluamide (DEET) of Comparative Example 1. All were found to be excellent.

P-cymene, α-terpinene, linarol, carbacroll and thymol isolated from the extracted oil of Example 4 was tested in the same manner as the repellent activity test for humans of the extracted oil of Example 4 Shown in

Processed material Total number of bites ^* Evasion rate (%) Evasion time until 3 bites ^* p-cymen 2.1 ± 1.55 85 45.2 ± 3.70 min α-terpinene 1.5 ± 0.88 92 69.5 ± 15.12 min Linarol 1.3 ± 0.52 90 65.1 ± 10.29 min Kabakrole 0.9 ± 0.77 96 78.8 ± 11.28 min Thymol 0.7 ± 0.74 98 81.5 ± 8.20 min

Note) *: Mean ± Standard Deviation

In addition, the extracted oil of Example 4 and N, N-diethyl-m-toluamide (DEET), which is a conventional synthetic mosquito repellent agent, was prepared at a mixing ratio of the following Table 6, and the human oil of Example 4 In experiments in the same manner as the repellent activity for the shown in Table 6 below.

Mixing ratio of treated materials Total number of bites ^* Evasion rate (%) Evasion time until 3 bites ^* 1: 0.1 1.1 ± 1.11 93 70.2 ± 3.70 min 1: 0.2 1.2 ± 0.93 91 67.5 ± 11.40 min 1: 0.3 1.8 ± 2.01 88 60.1 ± 8.17 min 1: 0.4 1.9 ± 0.86 86 47.8 ± 9.48 min

Note) *: Mean ± Standard Deviation

Insecticidal test

F-265-day larvae of 120 red- billed mosquitoes ( Clulex pipiens pallens Coquillett) were purchased from KFDA without discrimination between male and female, and had a temperature of 27 ± 2 ° C, 75-80% relative humidity, and 8% sugar / in natural light conditions. Water pads were fed to grow. Twenty mosquitoes were placed in a wire mesh cut into 30 × 30 × 30 cm of 6 to 7 day old female mosquitoes. 2 ml of 0.1% ethanol and the extracting oils of Examples 1 to 4 were dropped onto a 3 × 4 × 0.5 cm sanitary swab. The sanitary cotton and Home Mat ^TM (Electronic Mosquito Flavor, Donghwa Pharm. Co., Ltd.) were fumerated with an electronic fumigator in the wire mesh. The wire mesh was placed 10 cm above the workbench so that the air circulated well during the test. The number of dead mosquitoes and the number of mosquitoes dropped to the bottom were investigated every 30 minutes for 30 minutes and are shown in Table 7 below.

Time (min) Ethanol (Control) Example 1 Example 2 Example 3 Example 4 Home Mat ^TM 2 0 0 0 0 0 0 4 0 0 0 0 0 0 6 0 0 0 0 0 One 8 0 0 0 0 0 One 10 0 0 0 0 0 2 12 0 0 0 0 0 2 14 0 0 0 0 0 2 16 0 0 0 0 0 3 18 0 0 0 0 0 2 20 0 0 0 0 0 5 22 0 0 0 0 0 2 24 0 0 0 0 0 - 26 0 0 0 0 0 - 28 0 0 0 0 0 - 30 0 0 0 0 0 -

As shown in Table 3, Home Mat ^™ was found to die after 6 minutes and all of the mosquitoes died after 22 minutes. However, the extracted oil of the present invention did not show a pesticidal effect for 30 minutes after fumigation.

The mosquito repellent agent according to the present invention is an oil extracted from a plant or a compound separated therefrom, which not only has excellent mosquito repellent activity but also has a long-lasting effect, has no toxicity to humans or animals, and has a simple treatment method for skin. No irritant, no pungent odor and no influence on environmental pollution.

Simple modifications or changes of the present invention can be easily carried out by those skilled in the art, and all such modifications or changes can be seen to be included in the scope of the present invention.

Claims (4)

(Correction) Natural mosquito repellent, including Lavender Extract Oil, Rosemary Extract Oil, or Thyme Extract Oil. (Correction) The natural mosquito repellent of Claim 1, wherein the lavender tree is Lavender officinalis , the rosemary tree is Rosemarinus officinalis and the thyme tree is Thymus vulgaris . Selected from the group consisting of p-cymene, α-terpinene, linalool, cavacrol and thymol isolated or synthesized from (corrected) thyme extract oil. Natural mosquito repellents comprising one or more compounds. (Correction) Lavender extract oil, Rosemary extract oil, Thyme extract oil, p-cymene, α-terpinene, linalool, cabarcroll cavacrol) and thymol mosquito repellent mixed with one or more substances selected from the group consisting of N, N-diethyl-m-toluamide (DEET).