Natural plant essential oil composition, preparation method and application of natural plant essential oil composition in resuscitation inducing patch

Abstract

The invention relates to the technical field of plant essential oil, and discloses a natural plant essential oil composition, a preparation method and an application of the natural plant essential oil composition in a resuscitation inducing paste.The preparation method comprises the steps that a hydroxylated nitrogen-containing type silane coupling agent used for targeted adsorption of hydrogen-bond-containing acceptor or donor essential oil molecules is synthesized, the silane coupling agent further assists in adsorbing essential oil molecules containing hydrogen bond acceptors or donors and other essential oil molecules not containing hydrogen bond acceptors or donors in a non-specific manner through the hydrophobic effect of isobutylene and cyclohexyl; the surface and pore channels of nano mesoporous silica are modified by a hydroxylated nitrogen-containing silane coupling agent, and natural plant essential oil molecules with an anti-fatigue effect are loaded on the nano mesoporous silica based on hydrogen-bond interaction and / or hydrophobic interaction, so that the natural plant essential oil composition for clearing away heart-fire, inducing resuscitation, reducing pressure and relieving fatigue is obtained. The release time of natural plant essential oil molecules can be effectively prolonged, and the resuscitation inducing patch product prepared by taking the natural plant essential oil as an active component is relatively excellent in comprehensive performance and has practical application value.

Description

Technical Field

[0001] The present invention relates to the technical field of plant essential oils, in particular to a natural plant essential oil composition, a preparation method and application in a mind-refreshing patch. Background Art

[0002] Menthol ( )、Borneol( ), Patchouli alcohol ( ), linalool ( ), linalyl acetate ( )、Citronellol( )、1,8-cineole( ), limonene ( ), α-pinene ( ), β-caryophyllene ( ) and other terpenoid natural plant essential oil molecules, eugenol ( )、Carvacrol( Phenolic natural plant essential oil molecules, such as phenolic oils, can regulate the nervous system through olfactory stimulation, exerting anti-fatigue effects. Therefore, they are widely used in aromatherapy to achieve the goals of refreshing the mind, stress relief, and fatigue relief. Among them, the "refreshing patch" is a commonly used aromatherapy product. It uses natural plant essential oil molecules, absorbed through the skin and volatile, to stimulate local nerve endings, helping to refresh the mind and relieve fatigue.

[0003] However, the rapid oxidation and high volatility of natural plant essential oil molecules easily lead to their short half-life, which not only reduces their utilization rate but also seriously weakens the sustained effect of the essential oil molecules.

[0004] Prior art reports have used adsorption and solidification techniques using porous materials as carriers to control the slow release of essential oil molecules, improving their utilization and durability. Nano-mesoporous silica, a nanomaterial with a highly ordered porous structure, can provide a more stable loading space for essential oil molecules, demonstrating significant potential in the field of controlled release of essential oil molecules.

[0005] The study found that the surface functional groups of nano-mesoporous silica affect the binding force between essential oil molecules and carriers. The rich silanol groups on its pore surface can be given different surface properties through grafting modification with different chemical groups, and the internal pores can be used to store essential oil molecules, thereby ensuring better essential oil delivery, higher essential oil adsorption and sustained release capabilities. Summary of the Invention

[0006] The present invention utilizes hydrogen bonding and hydrophobic interactions to load natural plant essential oil molecules with anti-fatigue efficacy onto nano-mesoporous silica through adsorption and solidification technology, thereby preparing a natural plant essential oil composition with high utilization rate and durability for refreshing the mind, relieving stress and relieving fatigue, which can effectively prolong the release time of the natural plant essential oil molecules.

[0007] The preparation method of the natural plant essential oil composition comprises the following steps: Step 1: Synthesize a hydroxylated nitrogen-containing silane coupling agent for targeted adsorption of hydrogen bond acceptor or donor essential oil molecules. The silane coupling agent also non-specifically assists in the adsorption of hydrogen bond acceptor or donor essential oil molecules and other essential oil molecules without hydrogen bond acceptor or donor through the hydrophobic interaction of the isobutylene group and the cyclohexane group. Its chemical structure is: ; Step 2: Based on the silanol condensation mechanism, the surface and pores of Si-OH-rich nano-mesoporous silica are modified by hydroxylating nitrogen-containing silane coupling agents to prepare nano-mesoporous silica with the function of adsorbing essential oil molecules; Step three: natural plant essential oil molecules containing hydrogen bond acceptors or donors and having anti-fatigue effects are loaded onto the nano-mesoporous silica prepared in the step two through hydrogen bonding and hydrophobic interactions, and other natural plant essential oil molecules that do not contain hydrogen bond acceptors or donors and have anti-fatigue effects are loaded onto the nano-mesoporous silica prepared in the step two through hydrophobic interactions, to obtain a natural plant essential oil composition for refreshing the mind, relieving stress and relieving fatigue.

[0008] Preferably, the preparation method of the hydroxylated nitrogen-containing silane coupling agent is: Under the action of a phase transfer catalyst, a nucleophilic substitution reaction occurs between the hydroxyl functional group of 1 molar equivalent of linalool and the chlorine functional group of 1.01-1.09 molar equivalents of 5-chlorovaleraldehyde to generate an isobutylene aldehyde vinyl monomer; Using the Schiff base reaction mechanism, the aldehyde functional group of 1 molar equivalent of the isobutylene aldehyde vinyl monomer and the amino functional group of 1.01-1.09 molar equivalents of 4-aminocyclohexanol undergo a Schiff base condensation reaction to generate an isobutylene cyclohexanol-based nitrogen-containing vinyl monomer; In the presence of a photoinitiator, a hydroxylated nitrogen-containing silane coupling agent is generated by a click reaction between the vinyl functional group with less steric hindrance and higher activity in 1 molar equivalent of isobutylene cyclohexanol-based nitrogen-containing vinyl monomer and the mercapto functional group of 0.91-0.99 molar equivalent of 3-mercaptopropyltrimethoxysilane under the action of ultraviolet light.

[0009] Preferably, the phase transfer catalyst is one of tetrabutylammonium hydrogen sulfate, tetraethylammonium chloride, benzyltriethylammonium chloride, and tetrabutylammonium bromide.

[0010] Preferably, the photoinitiator is one of 2,2-dimethoxy-2-phenylacetophenone, 2-hydroxy-2-methyl-1-phenylpropanone, and 2,2-diethoxyacetophenone.

[0011] A natural plant essential oil composition prepared according to the above method for refreshing the mind, decompressing and relieving fatigue; Preferably, the natural plant essential oil molecules containing hydrogen bond acceptors or donors and having anti-fatigue effects in the natural plant essential oil composition include one or a combination of menthol, borneol, patchouli alcohol, linalool, linalyl acetate, citronellol, eugenol, and 1,8-cineole.

[0012] Preferably, the other natural plant essential oil molecules in the natural plant essential oil composition that do not contain hydrogen bond acceptors or donors and have anti-fatigue effects include one or a combination of limonene, α-pinene, and β-caryophyllene.

[0013] Preferably, the amount of the hydroxylated nitrogen-containing silane coupling agent in the natural plant essential oil composition is 10-20 wt % of the amount of the nano-mesoporous silica.

[0014] A mind-awakening patch, comprising a PVC film lower layer, a patch middle layer, and a medical transparent adhesive surface layer; Preferably, the patch is prepared by mixing the above-mentioned natural plant essential oil composition for refreshing the mind, relieving stress and relieving fatigue with a gel skeleton type matrix and adding a softener.

[0015] Preferably, the gel skeleton matrix is ​​composed of carbomer 940, polyvinyl pyrrolidone, sodium polyacrylate, propylene glycol, glycerol and polyethylene glycol 400, and the mass ratio thereof is 1: (5-10): (0.8-1.2): (3-5): (0.3-0.8): (0.3-0.8).

[0016] Preferably, the softener is glycerol or propylene glycol. Beneficial effects

[0017] The invention is based on a molecular design mechanism and uses natural plant essential oil molecules linalool, 5-chlorovaleraldehyde, 4-aminocyclohexanol and 3-mercaptopropyltrimethoxysilane as raw materials to synthesize a hydroxylated nitrogen-containing silane coupling agent. Nano-mesoporous silica was prepared by a hydrothermal method using hexadecyltrimethylammonium bromide and sodium salicylate as co-templates and tetraethyl orthosilicate as a silicon source. Nano-mesoporous silica with the ability to adsorb essential oil molecules was obtained by grafting with a hydroxylated nitrogen-containing silane coupling agent. Based on hydrogen bonding and hydrophobic interactions, natural plant essential oil molecules containing hydrogen bond acceptors or donors and having anti-fatigue effects, such as menthol, borneol, patchouli alcohol, linalool, citronellol, eugenol, and 1,8-cineole, and based on hydrophobic interactions, natural plant essential oil molecules not containing hydrogen bond acceptors or donors and having anti-fatigue effects, such as limonene and α-pinene, are co-loaded onto nano-mesoporous silica to obtain a natural plant essential oil composition for refreshing the mind, relieving stress, and relieving fatigue, i.e., nano-mesoporous silica loaded with natural plant essential oil molecules having anti-fatigue effects; On the one hand, the hydroxyl and nitrogen atoms carried by nano-mesoporous silica bind to the molecules of natural plant essential oils through hydrogen bonds. On the other hand, the isobutylene and cyclohexane groups carried by nano-mesoporous silica non-specifically adsorb to the molecules of natural plant essential oils through hydrophobic interactions. Experimental results show that, compared with the release rate of 93.5% of natural plant essential oil molecules with anti-fatigue efficacy used directly without loading at the same concentration in 120 minutes, the release rate of the natural plant essential oil composition for refreshing the mind, relieving stress and relieving fatigue prepared by the present invention is only 80.4% in 240 minutes, which means that the beneficial technical effect of effectively slowing down the volatilization rate of natural plant essential oil molecules with anti-fatigue efficacy is achieved. The mixed material composed of the natural plant essential oil composition and the gel skeleton matrix for refreshing the mind, relieving stress and relieving fatigue prepared by the present invention can be used as the middle layer patch of the refreshing patch. The refreshing patch prepared in this way has better comprehensive performance and practical application value. DETAILED DESCRIPTION

[0018] The present invention uses menthol, borneol, lime oil (mainly composed of limonene), lavender oil (mainly composed of linalool and linalyl acetate), sweet basil oil (mainly composed of linalool), geranium oil (mainly composed of citronellol and linalool), eucalyptus globulus leaf oil (mainly composed of 1,8-cineole and α-pinene), patchouli oil (mainly composed of patchouli alcohol) and clove oil (mainly composed of eugenol) as essential oil raw materials for providing natural plant essential oil molecules with anti-fatigue effects. The essential oils are loaded onto independently developed nano-mesoporous silica with the function of adsorbing essential oil molecules through adsorption and solidification technology, thereby preparing a natural plant essential oil composition with high utilization rate and durability for refreshing the mind, decompression and fatigue relief. Example 1:

[0019] The preparation steps of the hydroxylated nitrogen-containing silane coupling agent are as follows: Step 1: Using linalool as the base raw material, a nucleophilic substitution reaction is carried out between 1 molar equivalent of the hydroxyl functional group of linalool and 1.04 molar equivalents of the chlorine functional group of 5-chlorovaleraldehyde in the presence of a phase transfer catalyst to generate an isobutylene aldehyde vinyl monomer having the chemical formula: ; Among them, the phase transfer catalyst can be selected from one of tetrabutylammonium hydrogen sulfate, tetraethylammonium chloride, benzyltriethylammonium chloride, and tetrabutylammonium bromide; in this embodiment, tetrabutylammonium hydrogen sulfate is selected; Step 2: Using the Schiff base reaction mechanism, the aldehyde functional group of 1 molar equivalent of the isobutylene aldehyde vinyl monomer and the amino functional group of 1.03 molar equivalents of 4-aminocyclohexanol undergo a Schiff base condensation reaction to generate an isobutylene cyclohexanol nitrogen-containing vinyl monomer, the chemical structure of which is: ; Step 3: In the presence of a photoinitiator, a click reaction occurs between the sterically less hindered and more active vinyl functional group in the isobutylene cyclohexanol-based nitrogen-containing vinyl monomer and the mercapto functional group in 0.95 molar equivalents of 3-mercaptopropyltrimethoxysilane under the action of ultraviolet light to generate a hydroxylated nitrogen-containing silane coupling agent, the chemical structure of which is as follows: ; Among them, the photoinitiator can be selected from one of 2,2-dimethoxy-2-phenylacetophenone, 2-hydroxy-2-methyl-1-phenylacetone, and 2,2-diethoxyacetophenone; in this embodiment, 2,2-dimethoxy-2-phenylacetophenone is selected; The specific experimental steps for preparing hydroxylated nitrogen-containing silane coupling agent are as follows: 1.5 g of linalool, 10 mL of a 5 wt% aqueous sodium hydroxide solution, and 10 mL of N,N-dimethylformamide were added to a three-necked flask and stirred at room temperature for 30 min. Then, 10 mL of an N,N-dimethylformamide solution containing 1.2 g of 5-chlorovaleraldehyde and 10 mL of an N,N-dimethylformamide solution containing 1.7 g of tetrabutylammonium hydrogen sulfate were added to the three-necked flask in sequence. The mixture was heated to 70° C. and stirred for 6 h. The mixture was cooled to room temperature and the solvent was removed by rotary evaporation. The mixture was washed with deionized water and ethanol in sequence and dried in vacuo to obtain an isobutylene aldehyde vinyl monomer. 1.2 g of isobutylene aldehyde vinyl monomer and 20 mL of N,N-dimethylformamide were added to a three-necked flask and stirred at room temperature until completely dissolved. Then, 5 mL of N,N-dimethylformamide solution containing 0.6 g of 4-aminocyclohexanol and 2 drops of glacial acetic acid were added to the three-necked flask in sequence. The temperature was raised to 60° C. and stirred for 8 h. The mixture was cooled to room temperature and the solvent was removed by rotary evaporation. The mixture was washed with deionized water and ethanol in sequence and dried in vacuo to obtain an isobutylene cyclohexanol nitrogen-containing vinyl monomer. Under nitrogen protection, 1.1 g of isobutylcyclohexanol-based nitrogen-containing vinyl monomer, 0.5 g of 2,2-dimethoxy-2-phenylacetophenone photoinitiator, and 30 mL of N,N-dimethylformamide were added to a three-necked flask and stirred at room temperature until completely dissolved. Under ultraviolet light irradiation (365 nm, 10 cm), 0.6 mL of 3-mercaptopropyltrimethoxysilane was slowly added dropwise to the three-necked flask. After the addition was complete, the mixture was stirred and reacted under ultraviolet light for 30 minutes. The solvent was removed by rotary evaporation, and the mixture was washed with deionized water and ethanol in sequence and dried in vacuo to obtain a hydroxylated nitrogen-containing silane coupling agent. The nuclear magnetic resonance hydrogen spectrum of the hydroxylated nitrogen-containing silane coupling agent is characterized as follows: 1 H NMR (DMSO-d6, 400 MHz) δ: 0.75-0.79(t, 2H), 1.24(s, 3H), 1.56-1.80(m, 22H), 1.90-1.93(t, 2H), 2.04-2.09(m, 2H), 2.20-2.25(m, 2H), 2.47-2.50(t, 2H), 2.61-2 .64(t, 2H), 3.08-3.16(m, 1H), 3.34-3.37(t, 2H), 3.57(s, 9H), 3.64- 3.73 (m, 1H), 4.00-4.02 (d, 1H), 5.06-5.09 (t, 1H), 7.57-7.61 (t, 1H). Example 2:

[0020] Nano-mesoporous silica I with the function of adsorbing essential oil molecules is prepared, and the preparation process is as follows: (1) Preparation of nano-mesoporous silica: Using hexadecyltrimethylammonium bromide and sodium salicylate as co-templates and tetraethyl orthosilicate as silicon source, nano-mesoporous silica was synthesized under hydrothermal conditions. The specific experimental steps were as follows: 0.5 g of triethanolamine was dissolved in 150 mL of deionized water, heated to 80 °C and stirred for 30 min, 2 g of hexadecyltrimethylammonium bromide and 0.9 g of sodium salicylate were added, and the stirring was continued for 1 h, and then 20 mL of tetraethyl orthosilicate was added, and the reaction was maintained at 80 °C and stirred for 12 h, and then cooled to room temperature, and 50 mL of ethanol was added and centrifuged at 12000 rpm for 5 min to collect the precipitate, which was repeatedly washed with ethanol, vacuum dried, and ultrasonically dispersed in a mixed solution of 100 mL of ethanol / hydrochloric acid (volume ratio of 96:4), heated to 60 °C and stirred for 12 h, cooled to room temperature, and centrifuged at 12000 rpm for 5 min to collect the precipitate, which was repeatedly washed with ethanol, and vacuum dried to obtain nano-mesoporous silica; (2) Preparation of nano-mesoporous silica I with the function of adsorbing essential oil molecules: 0.8 parts by weight of hydroxylated nitrogen-containing silane coupling agent was used to hydrolyze the silanol functional groups obtained by the dehydration condensation reaction with the silanol functional groups in 5 parts by weight of nano-mesoporous silica, and the hydroxylated nitrogen-containing silane coupling agent was modified to the pores and surface of nano-mesoporous silica to obtain nano-mesoporous silica I with the function of adsorbing essential oil molecules. The specific experimental steps are as follows: under nitrogen protection, 5g of nano-mesoporous silica, 60 mL N,N-dimethylformamide and 40 mL deionized water were added to a three-necked flask and ultrasonically dispersed at room temperature for 30 minutes. Then, 10 mL of N,N-dimethylformamide solution containing 0.8 g of hydroxylated nitrogen-containing silane coupling agent and 2 drops of glacial acetic acid were added to the three-necked flask in sequence. The temperature was raised to 80°C and stirred for 10 hours. The precipitate was collected by centrifugation at 12000 rpm for 5 minutes, washed repeatedly with ethanol, and vacuum dried to obtain nano-mesoporous silica I with the function of adsorbing essential oil molecules. Example 3:

[0021] Preparation of nano-mesoporous silica II with the function of adsorbing essential oil molecules: the silanol functional groups obtained by hydrolysis reaction of 0.5 weight parts of hydroxylated nitrogen-containing silane coupling agent are subjected to a dehydration condensation reaction with the silanol functional groups in 5 weight parts of nano-mesoporous silica, and the hydroxylated nitrogen-containing silane coupling agent is modified into the pores and surface of the nano-mesoporous silica to obtain nano-mesoporous silica II with the function of adsorbing essential oil molecules. The specific experimental steps are different from those of nano-mesoporous silica I with the function of adsorbing essential oil molecules only in that the amount of hydroxylated nitrogen-containing silane coupling agent used is 0.5g. Example 4:

[0022] Preparation of nano-mesoporous silica III with the function of adsorbing essential oil molecules: using 1 weight part of hydroxylated nitrogen-containing silane coupling agent to undergo a hydrolysis reaction to obtain silanol functional groups and 5 weight parts of nano-mesoporous silica to undergo a dehydration condensation reaction, and modifying the hydroxylated nitrogen-containing silane coupling agent into the pores and surface of the nano-mesoporous silica to obtain nano-mesoporous silica III with the function of adsorbing essential oil molecules. The specific experimental steps differ from those of nano-mesoporous silica I with the function of adsorbing essential oil molecules only in that the amount of hydroxylated nitrogen-containing silane coupling agent used is 1.0 g. Embodiment 5:

[0023] Preparation of a natural plant essential oil composition for refreshing the mind, decompressing and relieving fatigue: Based on hydrogen bonding and hydrophobic interactions, natural plant essential oil molecules with anti-fatigue effects are loaded onto nano-mesoporous silica with the ability to adsorb essential oil molecules through adsorption solidification technology to prepare a natural plant essential oil composition for refreshing the mind, decompressing and relieving fatigue; Among them, the natural plant essential oil component formula for providing natural plant essential oil molecules with anti-fatigue effect is: 2.5 parts by weight of menthol (providing a natural plant essential oil molecule menthol containing a hydrogen bond acceptor or donor and having anti-fatigue effect), 1.3 parts by weight of borneol (providing a natural plant essential oil molecule borneol containing a hydrogen bond acceptor or donor and having anti-fatigue effect), 1.3 parts by weight of lime oil (mainly providing other natural plant essential oil molecules limonene that do not contain a hydrogen bond acceptor or donor and have anti-fatigue effect), 1.0 part by weight of patchouli oil (mainly providing a natural plant essential oil molecule patchouli alcohol containing a hydrogen bond acceptor or donor and having anti-fatigue effect), 1.0 part by weight of lavender oil (mainly providing a hydrogen bond acceptor or donor and having anti-fatigue effect linalool and linalyl acetate, a natural plant essential oil molecule containing a hydrogen bond acceptor or donor and having anti-fatigue efficacy), 1.0 part by weight of sweet basil oil (mainly providing linalool, a natural plant essential oil molecule containing a hydrogen bond acceptor or donor and having anti-fatigue efficacy), 0.9 part by weight of geranium oil (mainly providing citronellol and linalool, natural plant essential oil molecules containing a hydrogen bond acceptor or donor and having anti-fatigue efficacy), 0.5 part by weight of clove oil (mainly providing eugenol, a natural plant essential oil molecule containing a hydrogen bond acceptor or donor and having anti-fatigue efficacy), and 0.5 part by weight of eucalyptus globulus leaf oil (mainly providing 1,8-cineole, a natural plant essential oil molecule containing a hydrogen bond acceptor or donor and having anti-fatigue efficacy, and α-pinene, a natural plant essential oil molecule not containing a hydrogen bond acceptor or donor and having anti-fatigue efficacy); The specific experimental steps for preparing a natural plant essential oil composition for refreshing the mind, decompressing and relieving fatigue are as follows: 2.5g of menthol, 1.3g of borneol, 1.3g of lime oil, 1.0g of patchouli oil, 1.0g of lavender oil, 1.0g of sweet basil oil, 0.9g of geranium oil, 0.5g of clove oil, 0.5g of eucalyptus globulus leaf oil and 100mL of acetonitrile are added to a stoppered test tube, and the mixture is shaken and mixed on a vortex shaker for 10 minutes. Then, 13g of nano-mesoporous silica with the function of adsorbing essential oil molecules is added to the stoppered test tube, and the mixture is shaken and mixed on a vortex shaker for 5 minutes. The mixture is kept on a rotary constant temperature shaker at 25°C at a speed of 200 rpm for 48 hours, centrifuged, the supernatant is removed, and the mixture is dried at room temperature to obtain a natural plant essential oil composition for refreshing the mind, decompressing and relieving fatigue; Among them, the nano-mesoporous silica with the function of adsorbing essential oil molecules is one of nano-mesoporous silica I, nano-mesoporous silica II, and nano-mesoporous silica III; When the nano-mesoporous silica capable of adsorbing essential oil molecules is nano-mesoporous silica I, the prepared product is recorded as natural plant essential oil composition I for refreshing the mind, decompressing and relieving fatigue; When the nano-mesoporous silica capable of adsorbing essential oil molecules is nano-mesoporous silica II, the prepared product is recorded as natural plant essential oil composition II for refreshing the mind, decompressing and relieving fatigue; When the nano-mesoporous silica capable of adsorbing essential oil molecules is nano-mesoporous silica III, the prepared product is recorded as natural plant essential oil composition III for refreshing the mind, reducing stress and relieving fatigue. Example 6:

[0024] The preparation of the refreshing patch comprises the following steps: Step 1: Prepare a gel skeleton matrix: add 100 mL of water to 1 g of carbomer 940 and 8 g of polyvinyl pyrrolidone, respectively, mix them evenly to prepare a carbomer 940 solution and a polyvinyl pyrrolidone solution, respectively, place the mixture in a boiling water bath, heat and stir for 30 minutes, take out and add a viscous paste formed by grinding 1 g of sodium polyacrylate and 4 g of propylene glycol with water, finally add 0.5 g of glycerol and 0.5 g of polyethylene glycol 400, and concentrate in a water bath to obtain a gel skeleton matrix; Step 2, preparing a refreshing patch: 10g of the gel skeleton matrix and 0.8g of a natural plant essential oil composition for refreshing the mind, decompression and fatigue relief are mixed evenly, and then 0.2g of propylene glycol is added, the temperature is raised to 60°C, and the mixture is slowly stirred for 1h. The film is spread on a mold while hot by a casting method, and the film thickness is 1.2mm. It is dried overnight and vacuum-dried at 50°C for 1h until the surface is solidified and elastic. It is placed at room temperature, demolded, and the lower layer is covered with a PVC film, the middle layer is a patch, and the surface layer is covered with medical transparent tape to obtain a refreshing patch; The natural plant essential oil composition for refreshing the mind, decompressing and relieving fatigue is one of natural plant essential oil composition I, natural plant essential oil composition II and natural plant essential oil composition III; When the natural plant essential oil composition for refreshing the mind, decompressing and relieving fatigue is natural plant essential oil composition I, a refreshing patch I is prepared; When the natural plant essential oil composition for refreshing the mind, decompressing and relieving fatigue is natural plant essential oil composition II, a refreshing patch II is prepared; When the natural plant essential oil composition used for refreshing the mind, invigorating the spirit, and relieving stress and fatigue is the natural plant essential oil composition III, a refreshing patch III is prepared. Performance testing:

[0025] 1. Load performance test of the natural plant essential oil composition for refreshing the mind, relieving stress and relieving fatigue: The load capacity of the natural plant essential oil composition was inferred by drawing a standard curve equation. The specific test steps are as follows: (1) A natural plant essential oil component consisting of 2.5 g menthol, 1.3 g borneol, 1.3 g lime oil, 1.0 g patchouli oil, 1.0 g lavender oil, 1.0 g sweet basil oil, 0.9 g geranium oil, 0.5 g clove oil and 0.5 g eucalyptus leaf oil was scanned at full wavelength using a UV-visible spectrophotometer, and the maximum absorption wavelength λmax was recorded. The above natural plant essential oil components were dissolved in acetonitrile to prepare natural plant essential oil component solutions of different concentrations (including 7 groups with concentrations of 0.01, 0.03, 0.08, 0.1, 0.13, 0.18 and 0.2 g / mL). The absorbance values ​​of the natural plant essential oil component solutions of different concentrations were read at λmax using a UV-visible spectrophotometer. Linear regression analysis was performed with concentration as the horizontal axis and absorbance as the vertical axis to draw a standard curve equation. (2) The supernatant obtained by centrifugation during the preparation of the natural plant essential oil composition for refreshing the mind, decompressing and relieving fatigue in Example 5 was collected, and the absorbance value of the supernatant was tested at λmax using an ultraviolet-visible spectrophotometer. The concentration of the unloaded natural plant essential oil component was substituted into the standard curve equation to obtain C1 (g / mL). The initial concentration of the natural plant essential oil component in 100 mL of acetonitrile before loading was: C0 = (2.5 + 1.3 + 1.3 + 1.0 + 1.0 + 1.0 + 0.9 + 0.5 + 0.5) / 100 = 0.1 g / mL. The loading rate was calculated as follows: Load rate (%) = (1-C1 / C0) × 100%; The above test results are shown in Table 1 below; Table 1 Load performance test results of natural plant essential oil compositions for refreshing the mind, decompressing and relieving fatigue

[0026] Note: The difference between the comparative example in Table 1 and the natural plant essential oil composition I is that nano-mesoporous silica is used to replace the nano-mesoporous silica I having the function of adsorbing essential oil molecules; The experimental results in Table 1 indicate that the nano-mesoporous silica obtained by modifying the nano-mesoporous silica with the independently developed hydroxylated nitrogen-containing silane coupling agent has a significant improvement in the loading rate of natural plant essential oils compared to conventional nano-mesoporous silica without modification, and exhibits excellent loading capacity. 2. Test on the sustained-release performance of natural plant essential oil compositions for refreshing the mind, stress relief and fatigue relief: The natural plant essential oil component without Mg loading and the natural plant essential oil composition I loaded with Mg were respectively placed in dialysis bags and placed in V mL of acetonitrile. After 120 min and 240 min, the absorbance value of the solution was tested at λmax using a UV-visible spectrophotometer. The concentrations of essential oil dialyzed from the natural plant essential oil component in the dialysis bag (C2 (g / mL)) and the concentration of essential oil dialyzed from the natural plant essential oil composition I in the dialysis bag (C3 (g / mL)) were substituted into the standard curve equation, and the release rate was calculated as follows: Release rate of unloaded natural plant essential oil components (%) = [(C2 × V) / M] × 100%; Release rate of natural plant essential oil composition I (%) = [(C3×V) / M]×100%; The above test results are shown in Table 2 below; Table 2 Test results of sustained-release performance of natural plant essential oil compositions for refreshing the mind, reducing stress and relieving fatigue

[0027] Note: The concentration of the natural plant essential oil molecules with anti-fatigue effect in the unloaded natural plant essential oil component and the natural plant essential oil composition I in Table 2 is the same; The experimental results in Table 2 indicate that the natural plant essential oil composition for refreshing the mind, relieving stress and relieving fatigue prepared by the present invention has excellent sustained-release properties, which can prolong the release time of the natural plant essential oil components, thereby improving the utilization rate and durability of the essential oil molecules. 3. Basic performance test of the wake-up patch. The test results are shown in Table 3 below. Table 3 Basic performance test results of the wake-up patch

[0028] The experimental results in Table 3 indicate that the wake-up patch prepared by the present invention has both the stickiness and peel strength that meet the technical requirements of the YY / T 0148-2006 standard, and has excellent overall performance and is therefore valuable for practical application.

Claims

1. A method for preparing a natural plant essential oil composition, characterized in that: The following steps are involved: Step 1: Synthesize a hydroxylated nitrogen-containing silane coupling agent for targeted adsorption of hydrogen bond acceptor or donor essential oil molecules. The silane coupling agent also non-specifically assists in the adsorption of hydrogen bond acceptor or donor essential oil molecules and other essential oil molecules without hydrogen bond acceptor or donor through the hydrophobic interaction of the isobutylene group and the cyclohexane group. Its chemical structure is: ； Step 2: Based on the silanol condensation mechanism, the surface and pores of Si-OH-rich nano-mesoporous silica are modified by hydroxylating nitrogen-containing silane coupling agents to prepare nano-mesoporous silica with the function of adsorbing essential oil molecules; Step three: natural plant essential oil molecules containing hydrogen bond acceptors or donors and having anti-fatigue effects are loaded onto the nano-mesoporous silica prepared in the step two through hydrogen bonding and hydrophobic interactions, and other natural plant essential oil molecules that do not contain hydrogen bond acceptors or donors and have anti-fatigue effects are loaded onto the nano-mesoporous silica prepared in the step two through hydrophobic interactions, to obtain a natural plant essential oil composition for refreshing the mind, relieving stress and relieving fatigue.

2. The preparation method of natural plant essential oil composition according to claim 1, wherein The preparation method of the hydroxylated nitrogen-containing silane coupling agent is: Under the action of a phase transfer catalyst, a nucleophilic substitution reaction occurs between the hydroxyl functional group of 1 molar equivalent of linalool and the chlorine functional group of 1.01-1.09 molar equivalents of 5-chlorovaleraldehyde to generate an isobutylene aldehyde vinyl monomer; Using the Schiff base reaction mechanism, the aldehyde functional group of 1 molar equivalent of the isobutylene aldehyde vinyl monomer and the amino functional group of 1.01-1.09 molar equivalents of 4-aminocyclohexanol undergo a Schiff base condensation reaction to generate an isobutylene cyclohexanol-based nitrogen-containing vinyl monomer; In the presence of a photoinitiator, a hydroxylated nitrogen-containing silane coupling agent is generated by a click reaction between the vinyl functional group with less steric hindrance and higher activity in 1 molar equivalent of isobutylene cyclohexanol-based nitrogen-containing vinyl monomer and the mercapto functional group of 0.91-0.99 molar equivalent of 3-mercaptopropyltrimethoxysilane under the action of ultraviolet light.

3. The preparation method of the natural plant essential oil composition according to claim 2, wherein The phase transfer catalyst is one of tetrabutylammonium hydrogen sulfate, tetraethylammonium chloride, benzyltriethylammonium chloride and tetrabutylammonium bromide.

4. The preparation method of the natural plant essential oil composition according to claim 2, wherein The photoinitiator is one of 2,2-dimethoxy-2-phenylacetophenone, 2-hydroxy-2-methyl-1-phenylpropanone, and 2,2-diethoxyacetophenone.

5. The natural plant essential oil composition prepared according to the method described in any one of claims 1 to 4, characterized in that The natural plant essential oil molecules containing hydrogen bond acceptors or donors and having anti-fatigue effects in the natural plant essential oil composition include one or a combination of menthol, borneol, patchouli alcohol, linalool, linalyl acetate, citronellol, eugenol, and 1,8-cineole.

6. The natural plant essential oil composition according to claim 5, wherein Other natural plant essential oil molecules in the natural plant essential oil composition that do not contain hydrogen bond acceptors or donors and have anti-fatigue effects include one or a combination of limonene, α-pinene, and β-caryophyllene.

7. The natural plant essential oil composition according to claim 5, wherein The amount of the hydroxylated nitrogen-containing silane coupling agent in the natural plant essential oil composition is 10-20 wt % of the amount of the nano-mesoporous silica.

8. A refreshing patch, characterized in that: The wake-up patch is composed of a PVC film lower layer, a patch middle layer and a medical transparent adhesive surface layer; The patch is prepared by mixing the natural plant essential oil composition according to claim 5 with a gel skeleton type matrix and adding a softener.

9. The refreshing patch according to claim 8, characterized in that: The gel skeleton matrix is ​​composed of carbomer 940, polyvinyl pyrrolidone, sodium polyacrylate, propylene glycol, glycerol and polyethylene glycol 400, and the mass ratio thereof is 1: (5-10): (0.8-1.2): (3-5): (0.3-0.8): (0.3-0.8).

10. The refreshing patch according to claim 9, characterized in that: The softener is glycerin or propylene glycol.

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