Natural plant essential oil composition, preparation method and application in invigorating patch

Abstract

The present application relates to the technical field of plant essential oil, and discloses a natural plant essential oil composition, a preparation method and application in a refreshing patch, comprising: synthesizing a hydroxylated nitrogen-containing silane coupling agent for targeted adsorption of hydrogen bond-containing acceptor or donor essential oil molecules, the silane coupling agent also non-specifically assisting in adsorption of hydrogen bond-containing acceptor or donor essential oil molecules and other essential oil molecules not containing hydrogen bond acceptors or donors through hydrophobic action of isobutenyl and cyclohexyl; modifying the surface and pores of nano mesoporous silica through the hydroxylated nitrogen-containing silane coupling agent, and loading natural plant essential oil molecules with anti-fatigue efficacy on the nano mesoporous silica based on hydrogen bond action and / or hydrophobic action, to obtain a natural plant essential oil composition for clearing the heart and refreshing the mind, reducing pressure and relieving fatigue, which can effectively prolong the release time of natural plant essential oil molecules, and the refreshing patch product prepared as an active ingredient has relatively optimal comprehensive performance and practical application value.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of plant essential oil, in particular to a natural plant essential oil composition, a preparation method and application in a refreshing patch. BACKGROUND

[0002] Menthol ( ), borneol ( ), patchouli alcohol ( ), linalool ( ), linalyl acetate ( ), citronellol ( ), 1,8-cineole ( ), limonene ( ), alpha-pinene ( ), beta-caryophyllene ( ) and other terpenes natural plant essential oil molecules, eugenol ( ), carvacrol ( ) and other phenolic natural plant essential oil molecules, can regulate the nervous system through olfactory stimulation to play an anti-fatigue role, so they are widely used in aromatherapy to achieve the purpose of refreshing the mind and relieving fatigue. Among them, the refreshing patch is a commonly used aromatherapy product, which uses natural plant essential oil molecules to stimulate local nerve endings through skin absorption and volatilization, helping to refresh the mind and relieve fatigue.

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

[0004] In the prior art, there are reports of using porous materials as carriers to regulate the slow release of essential oil molecules, improve the utilization rate and durability of essential oils. Among them, nano-mesoporous silica is a kind of nano material with highly ordered porous structure, which can provide more stable loading space for essential oil molecules and has great potential in the field of essential oil molecule loading and controlled release.

[0005] Research has found that the surface functional groups of nano-mesoporous silica affect the binding force between essential oil molecules and the carrier. The abundant silicon hydroxyl groups on the pore surface can be modified by different chemical groups to give different surface properties, 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 capacity. SUMMARY

[0006] The application utilizes hydrogen bonding and hydrophobic effect to load natural plant essential oil molecules with anti-fatigue effect on nano-mesoporous silica through adsorption solidification technology, and a natural plant essential oil composition with high utilization rate and durability for clearing the heart and refreshing the mind and relieving pressure and fatigue is prepared, which can effectively prolong the release time of natural plant essential oil molecules.

[0007] The preparation method of the natural plant essential oil composition comprises the following steps:

[0008] Step one: synthesis of a hydroxylated nitrogen-containing silane coupling agent for targeted adsorption of hydrogen bond-containing or hydrogen bond-containing essential oil molecules, which also non-specifically assists the adsorption of hydrogen bond-containing or hydrogen bond-containing essential oil molecules and other essential oil molecules without hydrogen bond-containing or hydrogen bond-containing through the hydrophobic effect of isobutenyl and cyclohexane groups, and the chemical structural formula is:

[0009] ;

[0010] Step two: based on the condensation mechanism of silicon hydroxyl groups, the surface and pores of nano-mesoporous silica rich in Si-OH are modified by the hydroxylated nitrogen-containing silane coupling agent to prepare nano-mesoporous silica with adsorption of essential oil molecules;

[0011] Step three: load natural plant essential oil molecules containing hydrogen bond-containing or hydrogen bond-containing and having anti-fatigue effect on the nano-mesoporous silica prepared in step two through hydrogen bonding and hydrophobic effect, and load other natural plant essential oil molecules without hydrogen bond-containing or hydrogen bond-containing and having anti-fatigue effect on the nano-mesoporous silica prepared in step two through hydrophobic effect, to obtain a natural plant essential oil composition for clearing the heart and refreshing the mind and relieving pressure and fatigue.

[0012] Preferably, the preparation method of the hydroxylated nitrogen-containing silane coupling agent is:

[0013] Under the action of a phase transfer catalyst, nucleophilic substitution reaction occurs between the hydroxyl functional group of 1 mole equivalent of linalool and the chlorine functional group of 1.01-1.09 mole equivalents of 5-chloropentanal, to generate an isobutenyl aldehyde vinyl monomer;

[0014] Using the Schiff base reaction mechanism, Schiff base condensation reaction occurs between the aldehyde functional group of 1 mole equivalent of the isobutenyl aldehyde vinyl monomer and the amino functional group of 1.01-1.09 mole equivalents of 4-aminocyclohexanol, to generate an isobutenyl cyclohexanol nitrogen-containing vinyl monomer;

[0015] In the presence of a photoinitiator, a click reaction occurs between the vinyl functional group with less steric hindrance and higher activity in 1 mole equivalent of isobutenyl cyclohexanol group nitrogen-containing vinyl monomer and the mercapto functional group of 0.91-0.99 mole equivalent of 3-mercaptopropyl trimethoxysilane under the action of ultraviolet light to generate a hydroxylated nitrogen-containing silane coupling agent.

[0016] Preferably, the phase transfer catalyst is one of tetrabutylammonium hydrogen sulfate, tetraethylammonium chloride, benzyl triethyl ammonium chloride, tetrabutylammonium bromide.

[0017] Preferably, the photoinitiator is one of 2,2-dimethoxy-2-phenylacetophenone, 2-hydroxy-2-methyl-1-phenylpropanone, 2,2-diethoxyacetophenone.

[0018] The natural plant essential oil composition for clearing the heart and refreshing the mind and reducing pressure and relieving fatigue prepared according to the above method;

[0019] Preferably, the natural plant essential oil molecules containing hydrogen bond acceptors or donors and having anti-fatigue efficacy in the natural plant essential oil composition include one or a combination of several of menthol, borneol, pogostol, linalool, linalyl acetate, citronellol, eugenol, and 1,8-eucalyptol.

[0020] Preferably, the other natural plant essential oil molecules not containing hydrogen bond acceptors or donors and having anti-fatigue efficacy in the natural plant essential oil composition are limonene or / and α-pinene.

[0021] Preferably, the amount of hydroxylated nitrogen-containing silane coupling agent in the natural plant essential oil composition is 10-20wt% of the amount of nano-mesoporous silica.

[0022] A refreshing patch, which is composed of a PVC film underlayer, a patch middle layer, and a medical transparent adhesive surface layer.

[0023] Preferably, the patch is prepared by mixing the natural plant essential oil composition for clearing the heart and refreshing the mind and reducing pressure and relieving fatigue described above with a gel matrix type substrate and adding a softening agent.

[0024] Preferably, the gel matrix type substrate is composed of carbomer 940, polyvinylpyrrolidone, sodium polyacrylate, propylene glycol, glycerol, and polyethylene glycol 400, and the mass ratio is 1:(5-10):(0.8-1.2):(3-5):(0.3-0.8):(0.3-0.8).

[0025] Preferably, the softening agent is glycerol or propylene glycol.

[0026] Beneficial effects:

[0027] The present application is based on a molecular design mechanism, and uses natural plant essential oil molecules linalool, 5-chloropentanal, 4-aminocyclohexanol and 3-mercapto propyl trimethoxysilane as raw materials to synthesize a hydroxylated nitrogen-containing silane coupling agent;

[0028] Nano-mesoporous silica is prepared by a hydrothermal method using cetyltrimethylammonium bromide and sodium salicylate as co-templates and tetraethyl orthosilicate as a silicon source, and is grafted with the hydroxylated nitrogen-containing silane coupling agent to obtain nano-mesoporous silica with the function of adsorbing essential oil molecules;

[0029] Based on hydrogen bonding and hydrophobic interaction, natural plant essential oil molecules with hydrogen bond acceptors or donors and anti-fatigue effects, such as menthol, borneol, pogostol, linalool, citronellol, eugenol and 1,8-eucalyptol, and natural plant essential oil molecules without hydrogen bond acceptors or donors and anti-fatigue effects, such as limonene and alpha-pinene, are loaded onto nano-mesoporous silica to obtain a natural plant essential oil composition for clearing the heart and refreshing the mind and relieving pressure and fatigue, i.e., nano-mesoporous silica loaded with natural plant essential oil molecules with anti-fatigue effects;

[0030] On the one hand, the hydroxyl groups and nitrogen atoms of the nano-mesoporous silica are directionally combined with the natural plant essential oil molecules through hydrogen bonding, and on the other hand, the isobutenyl groups and cyclohexane groups of the nano-mesoporous silica are non-specifically adsorbed with the natural plant essential oil molecules through hydrophobic interaction;

[0031] It is found through experimental results that, compared with the release rate of 93.5% of natural plant essential oil molecules with anti-fatigue effects at the same concentration and used directly without loading for 120 min, the release rate of the natural plant essential oil composition for clearing the heart and refreshing the mind and relieving pressure and fatigue prepared by the present application is only 80.4% for 240 min, i.e., the beneficial technical effect of effectively slowing down the volatilization speed of natural plant essential oil molecules with anti-fatigue effects is achieved.

[0032] The mixed material of the natural plant essential oil composition for clearing the heart and refreshing the mind and relieving pressure and fatigue prepared by the present application and the gel matrix type substrate can be used as an intermediate layer patch of a refreshing patch, and the refreshing patch prepared therefrom has excellent comprehensive performance and practical application value. DETAILED DESCRIPTION

[0033] 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:

[0034] The preparation steps of the hydroxylated nitrogen-containing silane coupling agent are as follows:

[0035] 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:

[0036] ;

[0037] 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;

[0038] 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:

[0039] ;

[0040] 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:

[0041] ;

[0042] The photoinitiator can be selected from one of 2,2-dimethoxy-2-phenylacetophenone, 2-hydroxy-2-methyl-1-phenylpropanone, and 2,2-diethoxyacetophenone. In this embodiment, 2,2-dimethoxy-2-phenylacetophenone is selected for use.

[0043] The specific experimental steps for preparing the hydroxylated nitrogen-containing silane coupling agent are as follows:

[0044] In a three-necked flask, 1.5 g of linalool, 10 mL of 5 wt% sodium hydroxide aqueous solution, and 10 mL of N,N-dimethylformamide were added and stirred at room temperature for 30 min. Then, 10 mL of N,N-dimethylformamide containing 1.2 g of 5-chloropentanal and 10 mL of N,N-dimethylformamide containing 1.7 g of tetrabutylammonium hydrogen sulfate were sequentially added to the flask. The mixture was stirred at 70°C for 6 h, cooled to room temperature, and then rotary evaporated to remove the solvent. The product was washed with deionized water and ethanol sequentially, and dried under vacuum to obtain an isobutenyl aldehyde vinyl monomer.

[0045] In a three-necked flask, 1.2 g of the isobutenyl aldehyde vinyl monomer and 20 mL of N,N-dimethylformamide were added and stirred at room temperature until completely dissolved. Then, 5 mL of N,N-dimethylformamide containing 0.6 g of 4-aminocyclohexanol and 2 drops of glacial acetic acid were sequentially added to the flask. The mixture was stirred at 60°C for 8 h, cooled to room temperature, and then rotary evaporated to remove the solvent. The product was washed with deionized water and ethanol sequentially, and dried under vacuum to obtain an isobutenyl cyclohexanol nitrogen-containing vinyl monomer.

[0046] Under the protection of nitrogen, 1.1 g of the isobutenyl cyclohexanol 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. Then, 0.6 mL of 3-mercaptopropyltrimethoxysilane was slowly added to the flask under ultraviolet light irradiation (365 nm, 10 cm). After the addition was completed, the mixture was continuously stirred under ultraviolet light irradiation for 30 min. The solvent was then removed by rotary evaporation. The product was washed with deionized water and ethanol sequentially, and dried under vacuum to obtain a hydroxylated nitrogen-containing silane coupling agent.

[0047] The hydrogen nuclear magnetic resonance spectrum of the hydroxylated nitrogen-containing silane coupling agent is as follows: 1H 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:

[0048] Nano-mesoporous silica I with the function of adsorbing essential oil molecules is prepared, and the preparation process is as follows:

[0049] (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;

[0050] (2) Preparation of nano-mesoporous silica I with adsorption of essential oil molecules: 0.8 parts by weight of hydroxylated nitrogen-containing silane coupling agent is subjected to hydrolysis reaction to obtain silicon hydroxyl functional groups, which are subjected to dehydration condensation reaction with silicon hydroxyl functional groups in 5 parts by weight of nano-mesoporous silica, so as to modify the hydroxylated nitrogen-containing silane coupling agent to the pore channel and surface of the nano-mesoporous silica, thereby obtaining the nano-mesoporous silica I with adsorption of essential oil molecules. The specific experimental steps are as follows: 5 g of nano-mesoporous silica, 60 mL of N,N-dimethylformamide and 40 mL of deionized water are added into a three-necked flask under nitrogen protection, and ultrasonic dispersion is performed at room temperature for 30 min. 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 are sequentially added into the three-necked flask, and the temperature is raised to 80°C for stirring reaction for 10 h. After cooling to room temperature, the precipitate is collected by centrifugation at a speed of 12000 rpm for 5 min, and repeatedly washed with ethanol and vacuum dried, thereby obtaining the nano-mesoporous silica I with adsorption of essential oil molecules. Example Three

[0051] Preparation of nano-mesoporous silica II with adsorption of essential oil molecules: 0.5 parts by weight of hydroxylated nitrogen-containing silane coupling agent is subjected to hydrolysis reaction to obtain silicon hydroxyl functional groups, which are subjected to dehydration condensation reaction with silicon hydroxyl functional groups in 5 parts by weight of nano-mesoporous silica, so as to modify the hydroxylated nitrogen-containing silane coupling agent to the pore channel and surface of the nano-mesoporous silica, thereby obtaining the nano-mesoporous silica II with adsorption of essential oil molecules. The specific experimental steps are different from those of the nano-mesoporous silica I with adsorption of essential oil molecules only in that the amount of the hydroxylated nitrogen-containing silane coupling agent is 0.5 g. Example Four

[0052] Preparation of nano-mesoporous silica III with adsorption of essential oil molecules: 1 part by weight of hydroxylated nitrogen-containing silane coupling agent is subjected to hydrolysis reaction to obtain silicon hydroxyl functional groups, which are subjected to dehydration condensation reaction with silicon hydroxyl functional groups in 5 parts by weight of nano-mesoporous silica, so as to modify the hydroxylated nitrogen-containing silane coupling agent to the pore channel and surface of the nano-mesoporous silica, thereby obtaining the nano-mesoporous silica III with adsorption of essential oil molecules. The specific experimental steps are different from those of the nano-mesoporous silica I with adsorption of essential oil molecules only in that the amount of the hydroxylated nitrogen-containing silane coupling agent is 1.0 g. Example Five

[0053] Preparation of natural plant essential oil composition for clearing heart and refreshing spirit, reducing pressure and relieving fatigue: based on hydrogen bonding and hydrophobic interaction, natural plant essential oil molecules with anti-fatigue effect are loaded onto the nano-mesoporous silica with adsorption of essential oil molecules by adsorption solidification technology, thereby obtaining the natural plant essential oil composition for clearing heart and refreshing spirit, reducing pressure and relieving fatigue.

[0054] wherein the natural plant essential oil component formula of natural plant essential oil molecules with anti-fatigue efficacy is: 2.5 parts by weight of menthol (natural plant essential oil molecule menthol with hydrogen bond acceptor or donor and with anti-fatigue efficacy), 1.3 parts by weight of borneol (natural plant essential oil molecule borneol with hydrogen bond acceptor or donor and with anti-fatigue efficacy), 1.3 parts by weight of lime oil (mainly other natural plant essential oil molecule limonene without hydrogen bond acceptor or donor and with anti-fatigue efficacy), 1.0 part by weight of patchouli oil (mainly natural plant essential oil molecule patchoulol with hydrogen bond acceptor or donor and with anti-fatigue efficacy), 1.0 part by weight of lavender oil (mainly natural plant essential oil molecules linalool and linalyl acetate with hydrogen bond acceptor or donor and with anti-fatigue efficacy), 1.0 part by weight of sweet basil oil (mainly natural plant essential oil molecule linalool with hydrogen bond acceptor or donor and with anti-fatigue efficacy), 0.9 part by weight of geranium oil (mainly natural plant essential oil molecules citronellol and linalool with hydrogen bond acceptor or donor and with anti-fatigue efficacy), 0.5 part by weight of clove oil (mainly natural plant essential oil molecule eugenol with hydrogen bond acceptor or donor and with anti-fatigue efficacy), and 0.5 part by weight of eucalyptus globulus leaf oil (mainly natural plant essential oil molecules 1,8-cineole with hydrogen bond acceptor or donor and with anti-fatigue efficacy and natural plant essential oil molecule α-pinene without hydrogen bond acceptor or donor and with anti-fatigue efficacy);

[0055] The specific experimental steps for preparing the natural plant essential oil composition for clearing the heart and refreshing the mind, reducing pressure and relieving fatigue are: 2.5 g of menthol, 1.3 g of borneol, 1.3 g of lime oil, 1.0 g of patchouli oil, 1.0 g of lavender oil, 1.0 g of sweet basil oil, 0.9 g of geranium oil, 0.5 g of clove oil, 0.5 g of eucalyptus globulus leaf oil, and 100 mL of acetonitrile are added to a test tube with a plug, shaken and mixed on a vortex oscillator for 10 min, then 13 g of nano-mesoporous silica with adsorption of essential oil molecules is added to the test tube with a plug, shaken and mixed for 5 min using a vortex oscillator, kept on a rotary constant temperature oscillator at 25°C at a speed of 200 revolutions per minute for 48 h, centrifuged, the supernatant is removed, and dried at room temperature to obtain the natural plant essential oil composition for clearing the heart and refreshing the mind, reducing pressure and relieving fatigue;

[0056] wherein the nano-mesoporous silica with adsorption of essential oil molecules is one of nano-mesoporous silica I, nano-mesoporous silica II, and nano-mesoporous silica III;

[0057] when the nano-mesoporous silica with adsorption of essential oil molecules is nano-mesoporous silica I, the product obtained is recorded as natural plant essential oil composition I for clearing the heart and refreshing the mind, reducing pressure and relieving fatigue;

[0058] When the nano-mesoporous silica with the function of adsorbing essential oil molecules is nano-mesoporous silica II, the product prepared is recorded as natural plant essential oil composition II for clearing the heart and refreshing the mind and relieving pressure and relieving fatigue.

[0059] When the nano-mesoporous silica with the function of adsorbing essential oil molecules is nano-mesoporous silica III, the product prepared is recorded as natural plant essential oil composition III for clearing the heart and refreshing the mind and relieving pressure and relieving fatigue. Example six:

[0060] Preparation of refreshing paste, including the following steps:

[0061] Step one, preparation of gel skeleton type matrix: 100 mL water is added to 1 g carbomer 940 and 8 g polyvinylpyrrolidone respectively, and mixed uniformly to prepare carbomer 940 solution and polyvinylpyrrolidone solution respectively, then the two are mixed and put into a boiling water bath for heating and stirring for 30 min, then 0.5 g glycerol and 0.5 g polyethylene glycol 400 are added, and the water bath is concentrated to obtain the gel skeleton type matrix;

[0062] Step two, preparation of refreshing paste: 10 g of the gel skeleton type matrix and 0.8 g of the natural plant essential oil composition for clearing the heart and refreshing the mind and relieving pressure and relieving fatigue are mixed uniformly, then 0.2 g of propylene glycol is added, and the mixture is slowly stirred and mixed at 60°C for 1 h, then the casting method is used to spread the mixture on the mold while it is hot, the film thickness is 1.2 mm, it is air-dried overnight, and vacuum drying at 50°C is performed for 1 h until the surface is solidified and elastic, then it is placed at room temperature, demolded, covered with PVC film on the lower layer, with the paste in the middle, and covered with medical transparent adhesive on the surface, to obtain the refreshing paste;

[0063] The natural plant essential oil composition for clearing the heart and refreshing the mind and relieving pressure and relieving fatigue is one of the natural plant essential oil composition I, the natural plant essential oil composition II, and the natural plant essential oil composition III.

[0064] When the natural plant essential oil composition for clearing the heart and refreshing the mind and relieving pressure and relieving fatigue is the natural plant essential oil composition I, the refreshing paste I is prepared.

[0065] When the natural plant essential oil composition for clearing the heart and refreshing the mind and relieving pressure and relieving fatigue is the natural plant essential oil composition II, the refreshing paste II is prepared.

[0066] When the natural plant essential oil composition for clearing the heart and refreshing the mind and relieving pressure and relieving fatigue is the natural plant essential oil composition III, the refreshing paste III is prepared.

[0067] Performance test:

[0068] I. The loading performance test of the natural plant essential oil composition for clearing heart and refreshing mind, reducing pressure and relieving fatigue: the standard curve equation is drawn to deduce the loading capacity of the natural plant essential oil composition, and the specific test steps are as follows:

[0069] (1) The natural plant essential oil components composed of 2.5 g of menthol, 1.3 g of borneol, 1.3 g of lime oil, 1.0 g of patchouli oil, 1.0 g of lavender oil, 1.0 g of sweet basil oil, 0.9 g of rosemary oil, 0.5 g of clove oil and 0.5 g of blue eucalyptus oil are scanned by using a UV-visible spectrophotometer at full wavelength, the maximum absorption wavelength λmax is recorded, and the natural plant essential oil components are dissolved in acetonitrile to prepare natural plant essential oil component solutions with 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 with different concentrations are read by using a UV-visible spectrophotometer at λmax, and the standard curve equation is drawn by linear regression analysis with concentration as abscissa and absorbance as ordinate;

[0070] (2) The supernatant obtained by centrifugation during the preparation of the natural plant essential oil composition for clearing heart and refreshing mind, reducing pressure and relieving fatigue in Example 5 is collected, the absorbance value of the supernatant is tested by using a UV-visible spectrophotometer at λmax, and the concentration of the unloaded natural plant essential oil components is obtained by substituting the standard curve equation as C1(g / mL), the initial concentration of the natural plant essential oil components before loading in 100 mL of acetonitrile is C0= (2.5+1.3+1.3+1.0+1.0+1.0+0.9+0.5+0.5) / 100=0.1 g / mL, and the loading rate is calculated as follows:

[0071] Loading rate (%) = (1-C1 / C0) x 100%;

[0072] The test results are shown in Table 1 as follows:

[0073] Table 1 Test results of the loading performance of the natural plant essential oil composition for clearing heart and refreshing mind, reducing pressure and relieving fatigue

[0074]

[0075] Note: The difference between the comparative example in Table 1 and the natural plant essential oil composition I is that the nano-mesoporous silica is replaced by nano-mesoporous silica I which has the function of adsorbing essential oil molecules;

[0076] The following conclusions can be drawn from the experimental results in Table 1: the nano-mesoporous silica obtained by modifying the nano-mesoporous silica with the self-developed hydroxylated nitrogen-containing silane coupling agent has a significantly improved loading rate of natural plant essential oil compared to the conventional nano-mesoporous silica without modification, and exhibits excellent loading capacity;

[0077] II. Release performance test of the natural plant essential oil composition for clearing the heart and refreshing the mind, reducing pressure and relieving fatigue:

[0078] The Mg-unloaded natural plant essential oil component and the natural plant essential oil composition I loaded with Mg were respectively loaded into dialysis bags and placed in 500 mL acetonitrile, and at 120 min and 240 min, the absorbance value of the solution was tested at λmax using a UV-visible spectrophotometer, and the essential oil concentration C2 (g / mL) of the natural plant essential oil component dialyzed in the dialysis bag and the essential oil concentration C3 (g / mL) of the natural plant essential oil composition I dialyzed in the dialysis bag were obtained by substituting the standard curve equation, and the release rate was calculated, and the specific method is as follows:

[0079] The release rate (%) of the unloaded natural plant essential oil component is [(C2 x V) / M] x 100%;

[0080] The release rate (%) of the natural plant essential oil composition I is [(C3 x V) / M] x 100%;

[0081] The test results are shown in Table 2 below;

[0082] Table 2 Release performance test results of the natural plant essential oil composition for clearing the heart and refreshing the mind, reducing pressure and relieving fatigue

[0083]

[0084] Note: The concentration of 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;

[0085] The following conclusions can be drawn from the experimental results in Table 2: the natural plant essential oil composition for clearing the heart and refreshing the mind, reducing pressure and relieving fatigue prepared by the present application has excellent release performance, can prolong the release time of the natural plant essential oil component, and thus improve the utilization rate and persistence of the essential oil molecules;

[0086] III. Basic performance test of the refreshing patch, and the test results are shown in Table 3 below;

[0087] Table 3 Basic performance test results of the refreshing patch

[0088]

[0089] From the experimental results in Table 3, the following conclusions can be drawn: the holding adhesion and the peeling strength of the Xingshen patch prepared in the application can reach the technical requirements specified in the YY / T 0148-2006 standard, and the comprehensive performance is relatively optimal, and has practical application value.

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 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 are limonene and / or α-pinene.

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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