Use of a combination comprising volatile oil of apium graveolens seeds and extract of chrysanthemum coronarium, polysaccharide composition

Abstract

The present application relates to the cosmetic technical field, especially to a compound containing volatile oil of celery seeds and extract of golden chamomile, and application of a polysaccharide composition. In the present application, the volatile oil of celery seeds is used in combination with the extract of golden chamomile, and the synergistic effect generated between the two within a certain proportion range can achieve the effect of 1+1>2 in terms of antioxidant, whitening, anti-ultraviolet, antibacterial and other functions. On this basis, after adding any one of kelp polysaccharide, sea haozi polysaccharide, ginkgo polysaccharide or platycladus orientalis polysaccharide, the obtained polysaccharide gel mask and cream have better moisturizing and antibacterial functions, and the shelf life of the product is prolonged.

Description

Technical Field

[0001] This invention relates to the field of cosmetic technology, and in particular to the application of compound and polysaccharide compositions containing celery seed volatile oil and calendula extract. Background Technology

[0002] Natural plant extracts, due to their safety and high efficacy, have gradually become a primary focus of research in cosmetics with whitening, moisturizing, anti-inflammatory, and antibacterial effects. Currently, cosmetic products containing natural plant extracts often incorporate multiple plant extracts as active ingredients. However, not all plant extracts produce synergistic effects when combined. The 1992 Sarriselka Protocol categorized the interactions between compounding agents into three types: additive, synergistic, and antagonistic. Synergistic effects refer to the effect of two or more substances combined being stronger than the effect of any single substance acting alone; antagonistic effects refer to the effect of two or more substances combined being less than the sum of the effects of a single substance; and additive effects refer to the effect of two or more substances combined being equal to the sum of the effects of a single substance. Different combinations of substances exhibit different effects, therefore, it is necessary to evaluate the effects of compounding agents, such as using synergy coefficients (SE) and co-occurrence indices (CI) to assess the effectiveness of compounding.

[0003] Currently, most cosmetics containing natural plant extracts simply mix different plant extracts, rarely focusing on the proportions and effects of different plant active ingredients. Existing research on the combination of multiple plant extracts primarily focuses on their antioxidant effects, with only a few studies investigating their antibacterial, whitening, and other functional properties. For example, Wang Kai's research found that rosemary extract and tea polyphenol palmitate exhibited the best synergistic antioxidant effect when combined at a ratio of 5:3. Chen Zhihua et al., through studying the combined antibacterial activity of berberine with ampicillin and ciprofloxacin against E. coli O78 and O0701 under different conditions, found that the relationship between the two drugs showed both unrelated and additive effects. Furthermore, studies have found that the same proportion of compound formulations can produce different effects on different antioxidant models due to different mechanisms of action. For example, Skroza et al. studied the synergistic antioxidant activity between resveratrol and catechins, gallic acid, and caffeic acid, and found that the compound formulations of resveratrol with catechins or caffeic acid had a synergistic effect on the reduction of iron ions, and the synergistic effect of caffeic acid and resveratrol was stronger than that of the catechin and resveratrol combination; however, only the compound formulation of resveratrol and catechins had a synergistic effect on scavenging DPPH free radicals, while the compound formulation of caffeic acid and resveratrol had an antagonistic effect. Enko et al. mixed ascorbic acid with green tea or black tea extracts in different proportions and measured the antioxidant activity using methods such as TEAC, DPPH, and FRAP, and found that the interactions varied under different mass ratios, with most mixtures showing additive or antagonistic effects.

[0004] The skin mainly consists of the epidermis, dermis, and subcutaneous tissue. The stratum corneum, being the outermost layer of the skin, is a major obstacle to the effectiveness of active substances. Besides physical methods of enhancing penetration, adding chemical penetration enhancers that interact with the stratum corneum offers advantages such as simplicity, low cost, and flexible application. However, these chemical penetration enhancers have high requirements, such as being non-toxic, non-irritating, and non-sensitizing, and acting unidirectionally. While enhancing drug penetration into the skin, they must also prevent drug loss from the body. Propylene glycol, azone, fatty acids, and sulfoxides are commonly used chemical penetration enhancers, but they are highly irritating. Surfactants have lower skin irritation but poor penetration. Therefore, there is an increasing demand for developing more natural and safe penetration enhancers, such as volatile oils, amino acids and their derivatives, and chitosan derivatives. However, celery seed volatile oil, as a safe and efficient plant volatile oil, has not yet been considered for its penetration-enhancing effects.

[0005] Current research on the compounding of plant-derived active ingredients mainly focuses on the combination of ethanol extracts from different plants, or the combination of phytoethanol extracts with antioxidants (such as vitamin C and vitamin E), or with antibacterial agents, or with whitening agents such as arbutin. Research on the combination of phytoethanol extracts with volatile oils and polysaccharides is extremely limited. Calendula, a dual-use medicinal and food species, possesses anti-inflammatory, antioxidant, antibacterial, and anti-aging properties, but its application in the cosmetics field is relatively limited. Celery seed volatile oil has antibacterial, antioxidant, anti-aging, lipid-lowering, and blood pressure-lowering effects, but its main applications are in the food and pharmaceutical industries, with very few applications in cosmetics. Polysaccharides have diverse pharmacological effects, such as antiviral, anti-aging, anti-damage, antioxidant activity, anti-inflammatory, and immune-enhancing effects. However, polysaccharide extracts are rarely used in functional cosmetics, and are mostly used for moisturizing purposes. There are few reports on the combination of polysaccharides with other species. One report, such as the study by Ai Zhilu et al., found that jujube polysaccharides and flavonoids have a positive synergistic effect on antioxidant activity, and this synergistic effect is positively correlated with the concentration of antioxidants and their respective antioxidant capacities. Wang Peng et al. found that a combination of black fungus polysaccharides and flavonoids has a synergistic antioxidant effect.

[0006] Therefore, it remains crucial to explore and obtain compositions with synergistic antioxidant, whitening, anti-UV, antibacterial, penetration-enhancing, and moisturizing functions to provide new options for skincare and cosmetic products. Summary of the Invention

[0007] To address the aforementioned problems, the present invention aims to provide an application of a compound containing celery seed volatile oil and calendula extract, and a polysaccharide composition, within the field of cosmetics technology. This invention adds a compound of celery seed volatile oil and calendula extract, along with solutions of different plant polysaccharides, to gel masks and creams. The synergistic antioxidant, antibacterial, whitening, UV-blocking, and transdermal absorption-promoting bioactivities of the compound are measured. Gel masks or creams containing the compound and moisturizing polysaccharides are prepared, and their physicochemical properties and sensory evaluations are conducted according to current industry standards. The resulting gel masks and creams containing the compound and polysaccharides possess advantages such as high safety, significant synergistic effects, and extended shelf life.

[0008] The objective of this invention can be achieved through the following technical solutions:

[0009] The first objective of this invention is to provide the application of a compound containing celery seed volatile oil and calendula extract in the preparation of products with synergistic anti-UV, antibacterial, and penetration-enhancing functions. The compound containing celery seed volatile oil and calendula extract comprises the following components in the indicated mass ratios:

[0010] Celery seed volatile oil: Calendula extract = 1:1-9.

[0011] In one embodiment of the present invention, the compound containing celery seed volatile oil and calendula extract comprises the following components in the following mass ratios:

[0012] Celery seed volatile oil: Calendula extract = 1:3;

[0013] Alternatively, celery seed volatile oil: calendula extract = 1:5;

[0014] Alternatively, celery seed volatile oil: calendula extract = 1:7.

[0015] In one embodiment of the present invention, the compound containing celery seed volatile oil and calendula extract comprises the following components in the following mass ratios:

[0016] Celery seed volatile oil: Calendula extract = 1:5.

[0017] In one embodiment of the present invention, a compound containing celery seed volatile oil and calendula extract is used in the preparation of a product with synergistic antioxidant, whitening, anti-ultraviolet, antibacterial, and penetration-enhancing functions.

[0018] In one embodiment of the present invention, the celery seed volatile oil is prepared by the following method:

[0019] Celery seeds were mixed with sodium chloride solution, heated to extract the oil, and then the water was removed to obtain celery seed volatile oil.

[0020] In one embodiment of the present invention, the calendula extract is prepared by the following method:

[0021] (S1) After mixing calendula with ethanol, heat and reflux, filter under reduced pressure, concentrate and evaporate the ethanol to obtain the pretreated product.

[0022] (S2) After dissolving the pretreated product obtained in step (S1), extract it sequentially with petroleum ether and ethyl acetate to obtain calendula extract.

[0023] A second objective of this invention is to provide a polysaccharide composition comprising a compound containing celery seed volatile oil and calendula extract in a mass ratio of 1:1 and a polysaccharide.

[0024] The compound containing celery seed volatile oil and calendula extract includes celery seed volatile oil and calendula extract in a mass ratio of 1:5.

[0025] In one embodiment of the present invention, the polysaccharide is selected from one of kelp polysaccharide, seaweed polysaccharide, ginkgo polysaccharide or platycodon polysaccharide.

[0026] In one embodiment of the present invention, the polysaccharide is kelp polysaccharide.

[0027] The third objective of this invention is to provide an application of a polysaccharide composition in the preparation of products with synergistic antioxidant, whitening, anti-ultraviolet, antibacterial, penetration-enhancing, and moisturizing functions.

[0028] In this invention, celery seed volatile oil and calendula extract are compounded, and various polysaccharides are added to form a composition. Celery seed volatile oil has a good transdermal absorption promoting effect, which can enhance the transdermal absorption of calendula extract. Adding the compounded celery seed volatile oil and polysaccharides to creams or gel masks can also increase the effectiveness of the active ingredients on the skin. Furthermore, celery seed volatile oil, calendula extract, and their compound have good whitening, antioxidant, antibacterial, and anti-UV absorption activities, while polysaccharides have good moisturizing and antibacterial effects. The resulting polysaccharide gel masks and creams containing calendula compound have synergistic antioxidant, whitening, anti-UV, antibacterial, moisturizing, and penetration-promoting effects.

[0029] Celery seed volatile oil has antioxidant, anti-tumor, lipid-lowering, blood pressure-lowering, antibacterial, anti-aging, anti-edema-reducing, and skin-smoothing effects. Calendula has anti-inflammatory, antioxidant, antibacterial, anti-aging, and wound-healing effects.

[0030] Kelp polysaccharides possess immunomodulatory, antioxidant, anti-radiation, and microcirculation-improving activities, and also have a certain regulatory effect on anti-skin aging, especially on skin collagen metabolism. Seaweed polysaccharides have antioxidant, hypoglycemic, antitumor, antibacterial, and lipid-lowering biological activities; ginkgo polysaccharides have immunomodulatory, antitumor, antibacterial, and anti-aging biological activities; and platycodon polysaccharides have good antioxidant, metabolic-regulating, anti-inflammatory, and immune-boosting effects.

[0031] When celery seed volatile oil is combined with calendula extract, the synergistic effect between the two within a certain ratio range can achieve antioxidant, whitening, anti-ultraviolet, and antibacterial effects, with 1+1>2. On this basis, the addition of kelp polysaccharide, seaweed polysaccharide, ginkgo polysaccharide, or platycodon polysaccharide results in polysaccharide gel masks and creams with better moisturizing and antibacterial functions, while extending the shelf life of the products.

[0032] Compared with the prior art, the present invention has the following beneficial effects:

[0033] (1) The present invention adds a polysaccharide solution such as kelp to a compound containing celery seed volatile oil and calendula extract, which has certain synergistic antioxidant, whitening, antibacterial and anti-ultraviolet effects, and improves the product’s moisturizing, antioxidant and antibacterial abilities. The prepared product also has the effects of promoting transdermal absorption, moisturizing, antibacterial and anti-inflammatory, and long shelf life.

[0034] (2) The creams and gel masks prepared by this invention have natural plant extracts as their main active ingredients. They are highly safe and gentle on the skin. Celery seed volatile oil has antioxidant, anti-tumor, lipid-lowering, blood pressure-lowering, antibacterial, anti-aging, edema-reducing, and skin-smoothing effects. Calendula has anti-inflammatory, antioxidant, antibacterial, anti-aging, and wound-healing effects. Kelp and other plant polysaccharides also have moisturizing, antibacterial, anti-inflammatory, microcirculation-improving, and immune-regulating effects.

[0035] (3) In this invention, a compound containing celery seed volatile oil and calendula extract, along with polysaccharides, is used as the active ingredients. This is not merely a simple combination of these substances, but rather a rational formulation that achieves good results in synergistic antioxidant, whitening, antibacterial, anti-UV, and penetration-enhancing and moisturizing bioactivities. By measuring the antioxidant, whitening, and antibacterial properties of the compound containing celery seed volatile oil and calendula extract, it was found that the composition can produce a synergistic effect within a certain proportion range, further enhancing antioxidant capacity and inhibiting tyrosinase activity, thereby effectively reducing melanin production, more effectively protecting the skin, and preventing skin aging. Furthermore, the compound containing celery seed volatile oil and calendula extract has certain synergistic antibacterial and anti-UV activities. The addition of polysaccharides further enhances the moisturizing, antibacterial, and anti-inflammatory effects, and also significantly extends the product's shelf life. Attached Figure Description

[0036] Figure 1 This is a schematic diagram showing the results of the determination of the ABTS free radical scavenging ability of the compound;

[0037] Figure 2 This is a schematic diagram showing the results of the determination of the DPPH free radical scavenging ability of the compound;

[0038] Figure 3 A schematic diagram showing the results of the assay for the inhibitory activity of the compound on tyrosinase.

[0039] Figure 4 This is a schematic diagram showing the results of the UV absorption determination of the compound.

[0040] Figure 5 This is a schematic diagram showing the results of the determination of the permeability of the compound.

[0041] Figure 6 This is a schematic diagram showing the results of the polysaccharide moisturizing activity assay.

[0042] Figure 7 This is a schematic diagram of gel matrix film formation;

[0043] Figure 8 This is a schematic diagram illustrating the moisturizing activity of a gel mask.

[0044] Figure 9 A schematic diagram of a cream that does not contain compound ingredients and polysaccharides (Example 24);

[0045] Figure 10 This is a schematic diagram of a cream containing a compound (Example 25). Detailed Implementation

[0046] This invention provides the application of a compound containing celery seed volatile oil and calendula extract in the preparation of products with synergistic anti-UV, antibacterial, and penetration-enhancing functions. The compound containing celery seed volatile oil and calendula extract comprises the following components in the following mass ratio:

[0047] Celery seed volatile oil: Calendula extract = 1:1-9.

[0048] Furthermore, the compound containing celery seed volatile oil and calendula extract comprises the following components in the following mass ratios:

[0049] Celery seed volatile oil: Calendula extract = 1:3;

[0050] Alternatively, celery seed volatile oil: calendula extract = 1:5;

[0051] Alternatively, celery seed volatile oil: calendula extract = 1:7.

[0052] Furthermore, the compound containing celery seed volatile oil and calendula extract comprises the following components in the following mass ratios:

[0053] Celery seed volatile oil: Calendula extract = 1:5.

[0054] Furthermore, the compound containing celery seed volatile oil and calendula extract is used in the preparation of products with synergistic antioxidant, whitening, anti-UV, antibacterial, and penetration-enhancing functions.

[0055] Furthermore, the celery seed volatile oil is prepared by the following method:

[0056] Celery seeds were mixed with sodium chloride solution, heated to extract the oil, and then the water was removed to obtain celery seed volatile oil.

[0057] Furthermore, the calendula extract is prepared by the following method:

[0058] (S1) After mixing calendula with ethanol, heat and reflux, filter under reduced pressure, concentrate and evaporate the ethanol to obtain the pretreated product.

[0059] (S2) After dissolving the pretreated product obtained in step (S1), extract it sequentially with petroleum ether and ethyl acetate to obtain calendula extract.

[0060] This invention provides a polysaccharide composition comprising a compound containing celery seed volatile oil and calendula extract in a mass ratio of 1:1, and a polysaccharide.

[0061] The compound containing celery seed volatile oil and calendula extract includes celery seed volatile oil and calendula extract in a mass ratio of 1:5.

[0062] Furthermore, the polysaccharide is selected from one of kelp polysaccharide, seaweed polysaccharide, ginkgo polysaccharide, or platycodon polysaccharide.

[0063] Furthermore, the polysaccharide is kelp polysaccharide.

[0064] This invention provides the application of a polysaccharide composition in the preparation of products with synergistic antioxidant, whitening, anti-UV, antibacterial, penetration-enhancing, and moisturizing functions. The invention will now be described in detail with reference to the accompanying drawings and specific embodiments.

[0065] Unless otherwise specified, all reagents used in the following embodiments are commercially available reagents, and all detection methods and techniques used are conventional detection methods and techniques in the art.

[0066] In the following embodiments, the synergy coefficient (SE) is the ratio between the actual clearance rate (or inhibition rate, i.e., ESC) and the theoretical clearance rate (or inhibition rate, i.e., TSC) of the compound, i.e.: SE = ESC / TSC.

[0067] The formula for calculating TSC is as follows:

[0068] TSC(%)=(ESC1+ESC2)-(ESC1×ESC2) / 100

[0069] In the formula: ESC is the actual scavenging rate or actual inhibition rate of the compound, ESC1 is the actual scavenging rate or actual inhibition rate of celery seed volatile oil / %, and ESC2 is the actual scavenging rate or actual inhibition rate of calendula extract / %.

[0070] When SE>1, it indicates that the compound has a synergistic effect; when SE=1, the compound exhibits an additive effect; when SE<1, it exhibits an antagonistic effect.

[0071] Example 1

[0072] This embodiment provides a method for extracting volatile oil from celery seeds (steam distillation).

[0073] Celery seed volatile oil was mixed with distilled water containing 3% sodium chloride at a material-to-liquid ratio of 1:30. The mixture was soaked at room temperature for 3 hours, then heated at 130°C for 5 hours to extract the water. The water was removed with anhydrous sodium sulfate, the mixture was weighed, and stored in a refrigerator for later use.

[0074] Example 2

[0075] This embodiment provides a method for preparing calendula extract.

[0076] Calendula with a material-to-liquid ratio of 1:10 and 75% ethanol were heated and refluxed at 105°C for 3 hours. The mixture was then filtered under reduced pressure and the ethanol was concentrated and evaporated to obtain the pretreated product.

[0077] The pretreated product was dissolved in distilled water (the content of the pretreated product was 4 wt%), and then extracted with equal amounts of petroleum ether and ethyl acetate to obtain calendula extract, which was then refrigerated for later use.

[0078] Example 3

[0079] This embodiment provides a method for extracting kelp polysaccharides.

[0080] Pretreatment: Pure ethanol and pulverized kelp were mixed at a material-to-liquid ratio of 1:8 and extracted by reflux at 80°C for 2 hours. Most of the inorganic salts, pigments, lipids, mannitol and other impurities were removed by filtration. The extraction was repeated twice.

[0081] Extraction: Hot water extraction was used. The pretreated kelp powder was placed in water (solid-to-liquid ratio 1:40), and the extraction temperature was 90℃. The mixture was refluxed for 4 hours, and the extraction was performed once. The resulting polysaccharide solution was filtered through gauze, concentrated, and precipitated with a 4% (w / w) calcium chloride aqueous solution. The alginic acid was removed by filtration. The amount added was one-quarter of the polysaccharide solution volume. After standing overnight, pure ethanol was added until the ethanol content in the solution reached 70% (w / w). The solution was allowed to stand overnight again, centrifuged to obtain the polysaccharide, and then washed three times with pure ethanol to obtain the kelp polysaccharide.

[0082] Example 4

[0083] This embodiment provides a method for extracting polysaccharides from Artemisia annua.

[0084] Pretreatment: Soak the washed and dried seaweed seeds in pure ethanol (material-to-liquid ratio of 1:20) at room temperature for 0.5 h, then heat and reflux at 70 °C twice for 3 h each time, filter, and dry the residue for later use.

[0085] Extraction: Hot water extraction was used. The pretreated seaweed powder was placed in water (solid-to-liquid ratio 1:20), and the extraction temperature was 100℃. The mixture was heated under reflux for 2 hours and the extraction was repeated twice. The mixture was filtered through gauze, concentrated by rotary evaporation to a viscous state, and 4 times the volume of 95% ethanol was added. The mixture was precipitated in a refrigerator for 24 hours, filtered through gauze, washed three times with 95% ethanol, and centrifuged to obtain seaweed polysaccharide.

[0086] Example 5

[0087] This embodiment provides a method for extracting ginkgo polysaccharides.

[0088] Pretreatment: Freeze fresh ginkgo nuts in a refrigerator for 24 hours, then dry them in a 60℃ oven until constant weight, crush them, and set aside. Extract them with pure ethanol at a material-to-liquid ratio of 1:45 and heat at 95℃ under reflux for 3 hours. Repeat the extraction three times, filter with gauze, and dry the residue for later use.

[0089] Extraction: The hot water extraction method was used. The pretreated ginkgo powder was placed in water (solid-liquid ratio 1:45), the extraction temperature was 95℃, and the mixture was heated under reflux for 3 hours. The extraction was repeated three times. After filtering with gauze, the mixture was concentrated by rotary evaporation to a viscous state. Three times the volume of 95% ethanol was added, and the mixture was precipitated in a refrigerator for 24 hours. After filtering with gauze, the mixture was washed three times with 95% ethanol and centrifuged to obtain ginkgo polysaccharide.

[0090] Example 6

[0091] This embodiment provides a method for extracting polysaccharides from Platycodon grandiflorus.

[0092] Pretreatment: Wash, dry, and crush the fresh platycodon root for later use; mix with 80% ethanol at a material-to-liquid ratio of 1:20 and heat under reflux for 2 hours, repeat the extraction twice, filter with gauze, discard the supernatant, and dry the filter residue for later use.

[0093] Extraction: Hot water extraction was used. The pretreated Platycodon grandiflorus powder was placed in water (solid-to-liquid ratio 1:25), and the extraction temperature was 80℃. The mixture was heated under reflux for 2 hours and the extraction was repeated twice. After filtration through gauze, the mixture was concentrated by rotary evaporation to a viscous state. Pure ethanol was added until the mass fraction of ethanol in the solution was 80%. The mixture was precipitated in a refrigerator for 24 hours. After filtration through gauze, the mixture was washed three times with pure ethanol and centrifuged to obtain Platycodon grandiflorus polysaccharide.

[0094] Examples 7-17: Compounds containing celery seed volatile oil and calendula extract

[0095] The celery seed volatile oil prepared in Example 1 and the calendula extract prepared in Example 2 were combined to obtain a compound (the specific dosage ratio is shown in Table 1).

[0096] Table 1. Summary of the mass ratio of celery seed volatile oil to calendula extract in each example.

[0097] Example Celery seed volatile oil: Calendula extract Example 7 13：1 Example 8 9：1 Example 9 7：1 Example 10 5：1 Example 11 3：1 Example 12 1：1 Example 13 1：3 Example 14 1：5 Example 15 1：7 Example 16 1：9 Example 17 1：13

[0098] 1) Determination of antioxidant activity of the compound of celery seed volatile oil and calendula extract

[0099] 1 mL of sample (celery seed volatile oil, calendula extract, and their compound, hereinafter the same) was thoroughly mixed with 3 mL of ABTS+ working solution (ABTS free radicals and potassium persulfate aqueous solution were mixed uniformly at a volume ratio of 8:12, incubated in the dark for 18 h, and then diluted with anhydrous ethanol to obtain an absorbance value of 0.700±0.020 at 734 nm, thus obtaining the ABTS+ working solution). The mixture was incubated at room temperature in the dark for 10 min, and the absorbance was measured at 734 nm. The blank control was anhydrous ethanol, and the positive control was V... C The test was performed in triplicate. The ABTS+ clearance rate of the sample was calculated using the formula:

[0100]

[0101] In the formula, Ai is the absorbance value of 1 mL of sample and 3 mL of ABTS+ working solution; Aj is the absorbance value of 1 mL of sample and 3 mL of anhydrous ethanol; Ac is the absorbance value of 1 mL of anhydrous ethanol and 3 mL of ABTS+ working solution.

[0102] ABTS free radical scavenging ability test results are as follows Figure 1 As shown, through Figure 1It was found that when the mass ratio of celery seed volatile oil to calendula extract was between 3:1 and 13:1, the SE value was greater than 1 (between 1.14 and 1.56), indicating a synergistic effect. This means that the compound exhibited a synergistic effect when the overall mass proportion of celery seed volatile oil was relatively small. The synergistic effect was strongest at a ratio of 1:9, with the highest SE value of 1.56 and an actual clearance rate of 41.99%.

[0103] 2) Determination of the DPPH free radical scavenging capacity of the compound of celery seed volatile oil and calendula extract

[0104] Equal volumes of sample were uniformly mixed with 0.16 mmol / L DPPH anhydrous ethanol solution and incubated at room temperature in the dark for 40 min. The absorbance was measured at 517 nm. Three parallel groups were set up, with anhydrous ethanol as the blank control and vitamin C as the positive control.

[0105] Calculate the sample's DPPH using the following formula. + Clearance rate:

[0106]

[0107] In the formula, A i A represents the absorbance values ​​of 2 mL of sample and 2 mL of anhydrous ethanol solution of DPPH. j The absorbance values ​​are for 2 mL of sample and 2 mL of anhydrous ethanol; A c The absorbance values ​​are for 2 mL of anhydrous ethanol and 2 mL of DPPH in anhydrous ethanol solution.

[0108] DPPH free radical scavenging ability test results are as follows Figure 2 As shown, through Figure 2 It can be found that in the compound system of celery seed volatile oil and calendula extract in a ratio of 13:1 to 1:13, the compound has a synergistic effect, with SE values ​​ranging from 1.27 to 1.71. The synergistic effect is strongest when the ratio is 1:1, with the highest SE value of 1.71 and an actual clearance rate of 35.99%.

[0109] 3) Determination of the tyrosinase activity inhibition of the compound of celery seed volatile oil and calendula extract

[0110] The experimental reaction solution included 1 mL of 0.05 mM PBS (pH = 6.8) buffer solution, 1 mL of sample and 0.5 mL of tyrosinase solution. After standing at room temperature for 10 min, 1 mL of L-DOPA (0.01 M) solution was added, mixed well, and reacted at room temperature for 10 min. The absorbance value (A) was detected at 475 nm.

[0111] The control group was replaced with an equal volume of sample solvent (deionized water), and the test was performed in triplicate. The positive control was arbutin. Specific ratios are shown in Table 2.

[0112] Table 2 Composition of the reaction solution

[0113]

[0114] Calculate the tyrosinase inhibition rate (%) using the following formula:

[0115]

[0116] Results of tyrosinase activity inhibition assay: Figure 3 As shown, through Figure 3 It can be found that the mass ratio of celery seed volatile oil to calendula extract has a synergistic effect in the range of 1:1 to 1:9, with an SE value range of 1.25 to 1.48. The synergistic effect is strongest at a ratio of 1:5, with the highest SE value of 1.48 and an actual inhibition rate of 52.73%.

[0117] Based on the results of three sets of experiments, the compound ratio that simultaneously exhibits synergistic antioxidant and enzyme-inhibiting activities was obtained, as shown in Table 3.

[0118] Table 3 shows the compound ratios that simultaneously possess synergistic antioxidant and enzyme-inhibiting activities.

[0119]

[0120] As shown in Table 3, when the mass ratio of celery seed volatile oil to calendula extract is 1:1 to 1:9, it exhibits synergistic antioxidant and enzyme-inhibiting activities. When the celery seed volatile oil and calendula extract are combined at a ratio of 1:5, the SE values ​​of the compound for synergistic antioxidant and tyrosinase inhibition are both high, indicating strong antioxidant and whitening effects.

[0121] 4) Determination of UV absorption of the compound of celery seed volatile oil and calendula extract

[0122] Using the sample solvent as a blank reference, the sample was scanned across the entire wavelength range of 280-400 nm (UVA: 320-400 nm, UVB: 280-320 nm) to observe whether any ultraviolet absorption peaks appeared. Three parallel measurements were performed, and the average value was taken.

[0123] Results of UV absorption resistance are as follows Figure 4 As shown, through Figure 4It was found that the combination of celery seed volatile oil and calendula extract, except at a 1:1 ratio, showed good absorption of UV light in the 280nm-400nm range at ratios of 1:3, 1:5, 1:7, and 1:9. The maximum absorbance values ​​for these ratios were 2.553, 2.555, 2.612, and 2.615, respectively. The maximum absorbance of calendula extract was measured to be 2.164. Celery seed volatile oil only showed a relatively low amount of UV absorption around 280nm. Therefore, the synergistic anti-UVA and UVB absorption effects were better at ratios of 1:3, 1:5, 1:7, and 1:9.

[0124] From Table 3, Figure 3 and Figure 4 It was found that the synergistic effect of the compound on ABTS, DPPH, tyrosinase activity inhibition, and UV absorption was high at a ratio of 1:5, indicating a strong synergistic effect. Therefore, the optimal compound ratio of celery seed volatile oil and calendula extract was determined to be 1:5. The antioxidant properties and tyrosinase activity inhibition of the compound compared with those of its single components are shown in Table 4. As shown in Table 4, at the same concentration, the scavenging rate of ABTS and DPPH free radicals and the inhibition of tyrosinase activity of the compound were higher than those of the single components, indicating a better synergistic effect. Compared with calendula extract, the scavenging rate of ABTS free radicals of the compound increased from 23.75% to 36.52%, which is 1.54 times the original; the scavenging rate of DPPH free radicals increased from 21.63% to 45.17%, which is 2.09 times the original; and the inhibition of tyrosinase activity increased from 29.02% to 52.73%, which is 1.82 times the original.

[0125] Table 4. Comparison of synergistic antioxidant and enzyme-inhibiting effects of compound formulations with those of single species.

[0126]

[0127] 5) Skin permeability test of the compound of celery seed volatile oil and calendula extract

[0128] The transdermal absorption enhancement effect of each sample was detected using a modified Franz diffusion cell method. Fresh pigskin was used to simulate human skin; subcutaneous fat was removed, but the dermis was retained. The skin was washed with 0.01 mol / L PBS (pH 7.4) and ready for use. PBS was used as the receiving solution, and a sample concentration of 1 mg / mL was used as the diffusion solution. The pigskin was sandwiched between the diffusion cell and the receiving cell. The experimental temperature was 32℃, and the magnetic flux rotation speed was 550 r / min. The receiving solution was collected after 12 hours for analysis. The sample concentration was determined, and the cumulative permeation per unit area was calculated using the following formula:

[0129]

[0130] In the formula: Q is the cumulative permeability per unit area, mg / cm² 2 ρ is the sample concentration at 12h, mg / mL; V is the volume of the receiving cell, 6.0 mL; A is the effective skin penetration area, 2.26 cm². 2 .

[0131] Skin permeability such as Figure 5 As shown, through Figure 5 It was observed that when celery seed volatile oil and calendula extract were used alone, the cumulative penetration of celery seed volatile oil was significantly higher than that of calendula extract. When calendula extract and celery seed volatile oil were combined, the cumulative skin penetration increased significantly compared to when they were used alone, reaching 1.88 times the amount when used alone. Therefore, celery seed volatile oil can promote the skin penetration of calendula extract, further enhancing the efficacy of the combined product.

[0132] 6) Antibacterial assay of the compound of celery seed volatile oil and calendula extract

[0133] MIC is the lowest concentration of a sample that inhibits microbial growth, and MBC is the lowest concentration of a sample that kills microorganisms. Both can demonstrate the antibacterial effect of a sample.

[0134] Using sterilized tweezers, pick up pre-treated filter paper discs containing different mass concentrations of samples (celery seed volatile oil filter paper, calendula extract filter paper, compound filter paper, and streptomycin sulfate filter paper), and affix them to plates coated with bacterial suspension. Invert the plates and incubate them at 37°C for 24 hours. Remove the plates and measure the diameter of the inhibition zone. The lowest concentration at which an inhibition zone appears is the minimum inhibitory concentration (MIC) of the sample. Continue incubating the plates with inhibition zones (MIC measured) for another 24 hours, and measure the diameter of the inhibition zone again. The lowest concentration at which the diameter of the inhibition zone remains the same after 24 hours of incubation is the minimum inhibitory concentration (MBC).

[0135] The MIC and MBC values ​​of celery seed volatile oil, calendula extract, compound, and positive control streptomycin sulfate were determined, and the experimental results are shown in Table 5.

[0136] Table 5. Results of the study on the antibacterial activity of celery seed volatile oil, calendula extract and their compound.

[0137]

[0138] Note: In the compound, the mass ratio of celery seed volatile oil to calendula extract is 1:5.

[0139] Table 5 shows that the compound had the lowest MIC and MBC values ​​against *Escherichia coli* and *Staphylococcus aureus*, at 1.56 mg / mL and 3.125 mg / mL, and 0.39 mg / mL and 0.78 mg / mL, respectively. Calendula extract and celery seed volatile oil followed. Compared to calendula extract, the compound's MIC and MBC values ​​against *E. coli* decreased from 3.125 mg / mL to 1.56 mg / mL and from 6.25 mg / mL to 3.125 mg / mL, respectively, both approximately half the original values. Against *Staphylococcus aureus*, the MIC and MBC values ​​decreased from 1.56 mg / mL to 0.39 mg / mL and from 3.125 mg / mL to 0.78 mg / mL, respectively, both approximately quarter the original values. The experimental results indicate that the compound has a good synergistic antibacterial effect, with a stronger synergistic effect against *Staphylococcus aureus*.

[0140] 7) Determination of the moisturizing rate of polysaccharide solutions

[0141] Using medical tape to simulate human skin, a 2cm*2cm piece of medical tape was applied to a 50mm petri dish. A polysaccharide solution or glycerin aqueous solution was evenly spread on the tape surface, with an application amount of 0.5g. The dish was then placed in a 25℃ oven, and weighed every 30 minutes. Three parallel measurements were performed, and the average value was taken. The moisture retention rate was calculated using the following formula.

[0142]

[0143] Where: m t t represents the mass of the sample after it has been stored for t hours; m0 represents the initial mass.

[0144] The moisturizing rate of different polysaccharide solutions and a positive control glycerol aqueous solution was determined. The results of the moisturizing rate determination are as follows: Figure 6 As shown, through Figure 6 It can be observed that the moisturizing rate gradually decreases over time, and the order of moisturizing performance is kelp polysaccharide > ginkgo polysaccharide > seaweed polysaccharide > platycodon polysaccharide. Except for platycodon polysaccharide, which is comparable to the positive control (glycerol aqueous solution), the other three polysaccharides are higher than the positive control.

[0145] Example 18

[0146] This embodiment provides a gel matrix.

[0147] Xanthan gum: konjac gum: pectin = 0.8g: 0.8g: 0.6g, add a certain amount of 80℃ deionized water, stir to dissolve, stirring at 300r / min, then add 4g of glycerol, and add more deionized water to make the total mass 100g. Stir in a constant temperature water bath for 1 hour. After mixing, a uniformly distributed gel-like liquid (gel matrix) is obtained. After standing, it looks like... Figure 7 As shown, through Figure 7It can be observed that the surface of the gel matrix is ​​smooth, flat, uniform, and transparent, and has good stretchability and hardness.

[0148] Examples 19-23

[0149] Following the gel matrix formulation process in Example 18, xanthan gum: konjac gum: pectin: glycerin = 0.8g: 0.8g: 0.6g: 4g was dissolved in water and stirred. The compound from Example 14 was then added and mixed well. Different polysaccharide solutions were added as shown in Table 6, and deionized water was added to each mixture to bring the total mass to 100g, thus obtaining each mixture. The mixture was then placed in a gel mask mold, allowed to cool, and pressed into a film to obtain the gel masks of Examples 19 to 23 (specific formulations are shown in Table 6).

[0150] Table 6 Gel Mask Formulas

[0151]

[0152] After adding the compound and polysaccharide, the properties of the gel mask, such as stretchability, hardness, and smoothness, remained unchanged, and the surface was smooth and flat, indicating that the addition of the compound and polysaccharide had no adverse effect on the gel matrix.

[0153] The gel masks with different added polysaccharides were observed, and the results are shown in Table 7. After adding the compound, the physicochemical properties of the gel masks did not change significantly, indicating that the addition of the compound had no effect on the gel masks and they exhibited good stability. Compared with the blank gel mask (Example 18), the gel mask with the added compound (Example 19) was slightly pale yellow and had a slight aroma of celery seed volatile oil. Adding different plant polysaccharides (Examples 20-23) had no adverse effects on the physicochemical properties and sensory evaluation of the gel masks, but different plant polysaccharides had different effects on the shelf life of the gel masks. The gel mask with added kelp polysaccharide (Example 20) had a relatively long shelf life of 12 days, followed by those with added seaweed polysaccharide (Examples 21, 8 days), ginkgo polysaccharide (Example 22, 7 days), and platycodon polysaccharide (Example 23, 6 days).

[0154] Table 7 Effects of different plant polysaccharides on gel masks

[0155]

[0156] In addition, the moisturizing effects of the four types of gel masks with added polysaccharides are as follows: Figure 8 As shown, the moisturizing rate gradually decreased over time, and the order of moisturizing performance was kelp polysaccharide > ginkgo polysaccharide > seaweed polysaccharide > platycodon polysaccharide. Except for platycodon polysaccharide, which was comparable to the positive control (glycerol aqueous solution), the other three polysaccharides were higher than the positive control.

[0157] In summary, referring to the current industry standard QB / T 2872-2017 "Facial Masks", the obtained gel masks were tested for heat resistance and cold resistance. The results showed that after the polysaccharide gel masks naturally returned to room temperature at the end of the experiment, there was no significant difference, and the corresponding test results met the industry standard. Adding polysaccharides can increase the shelf life and moisturizing properties of gel masks, and the application effect is also better. Among them, the shelf life of the kelp polysaccharide gel mask (Example 20) can be extended to 3 times that of the blank group (Example 18).

[0158] Examples 24-29

[0159] A polysaccharide cream containing a blend of celery seed volatile oil and calendula extract mainly comprises the following components by weight percentage: 4% squalane, 3% olive oil, 3% monoglyceride, 2% glyceryl stearate, 2% alkyl glycoside, 2% cetearyl alcohol, 3% 1,3-butanediol, 4% glycerin, 3% polyethylene glycol, 0.2% hydroxyethyl cellulose, 0.2% gum arabic, 1% celery seed volatile oil and calendula extract blend (Example 14), and 1% different polysaccharide solutions, with deionized water as the balance; its preparation method includes the following steps:

[0160] (S1) Under stirring conditions of 75℃ and 350r / min, squalane, olive oil, monoglycoside, glyceryl stearate, alkyl glycoside, and cetearyl alcohol are stirred and dissolved evenly, and kept warm for 10min. This mixture is recorded as phase A for later use.

[0161] (S2) Raise the temperature to 90°C, mix 1,3-butanediol, glycerol, polyethylene glycol and deionized water at 300 r / min, keep for 15 min, sterilize, and then cool to 75°C, which is designated as phase B.

[0162] (S3) Under stirring conditions of 75℃ and 300r / min, phase B is slowly added to phase A and stirred until homogeneous to obtain a mixture;

[0163] (S4) When the mixture cools down to 40°C, add hydroxyethyl cellulose and gum arabic, stir until completely dissolved, stop heating, add celery seed volatile oil and calendula extract compound, add polysaccharide solution, stir and cool to room temperature to prepare cream.

[0164] The blank matrix (Example 24) contained no compound and polysaccharide; Example 25 contained only compound; Example 26 contained compound and kelp polysaccharide; Example 27 contained compound and seaweed polysaccharide; Example 28 contained compound and ginkgo polysaccharide; and Example 29 contained compound and platycodon polysaccharide. Referring to industry standard QB / T1857-2013 "Skin Creams", the creams obtained in the examples were subjected to corresponding physicochemical properties and sensory evaluations. For each sensory evaluation result, the categories were: Excellent: ++, Good: +, Poor: -, Very Poor: --.

[0165] All test results met the requirements (see Table 8). The addition of compounding agents to the cream base formula had no adverse effects on the cream matrix and exhibited good stability. Figure 9 and Figure 10 ).

[0166] Table 8. Effects of different plant polysaccharides on ointments and creams

[0167]

[0168] Compared with the blank group cream (Example 24), Figure 9 Compared to creams containing compound ingredients (Example 25), creams containing compound ingredients... Figure 10 The cream is slightly yellowish with a subtle, aromatic scent of celery seed volatile oil. When applied to the skin, the texture is evenly distributed, smooth, and free of granules, making it easy to apply and absorb. It leaves a moisturizing and cooling sensation. The cooling sensation is likely related to the skin-absorbing properties of celery seed volatile oil, which can quickly penetrate the inner layers of the skin, accelerating the absorption of the cream. Further addition of various plant polysaccharides significantly extends the cream's shelf life. This relative extension of shelf life may be related to the presence of antioxidant and antibacterial ingredients in the composition. Different polysaccharides have different effects on the shelf life of creams. The cream with added kelp polysaccharide (Example 26) has a relatively long shelf life of 75 days, which is 2.5 times that of the blank group (Example 24). The cream with added seaweed polysaccharide (Example 27, 60 days), ginkgo polysaccharide (Example 28, 50 days), and platycodon polysaccharide (Example 29, 45 days) has a better moisturizing effect than the original.

[0169] In summary, the addition of a compound with synergistic antioxidant, whitening, anti-UV, and antibacterial effects to polysaccharide gel masks and creams with good texture and appearance, and its physicochemical properties and sensory evaluation according to current industry standards, all met the requirements, and its properties had no adverse effects on the control group. After adding the compound and different plant polysaccharides to the creams and gel masks, celery seed volatile oil facilitated the penetration of the active ingredients, resulting in increased moisturizing properties and a significantly extended shelf life. The polysaccharide gel mask showed increased moisturizing properties and a shelf life three times longer than the control group; the cream's shelf life was 2.5 times longer than the control group.

[0170] The above description of the embodiments is provided to enable those skilled in the art to understand and use the invention. It will be apparent to those skilled in the art that various modifications can be made to these embodiments, and the general principles described herein can be applied to other embodiments without inventive effort. Therefore, the present invention is not limited to the above embodiments, and any improvements and modifications made by those skilled in the art based on the interpretation of the present invention, without departing from the scope of the invention, should be within the protection scope of the present invention.

Claims

1. The use of a complex containing volatile oil of Apium graveolens seeds and extract of Calendula officinalis in the preparation of a product with synergistic anti-UV, antibacterial and penetration-promoting functions, characterized in that, The complex containing celery seed volatile oil and extract of golden chamomile includes the following mass ratio of each component: Celery seed volatile oil: golden chamomile extract = 1:1-9.

2. Use according to claim 1, characterized in that, The complex containing celery seed volatile oil and extract of golden chamomile includes the following mass ratio of each component: Celery seed volatile oil: golden chamomile extract = 1:3; Or, celery seed volatile oil: golden chamomile extract = 1:5; Or, celery seed volatile oil: golden chamomile extract = 1:

7.

3. Use according to claim 1, characterized in that, The complex containing celery seed volatile oil and extract of golden chamomile includes the following mass ratio of each component: Celery seed volatile oil: golden chamomile extract = 1:

5.

4. Use according to claim 1, characterized in that, The celery seed volatile oil is prepared by the following method: The celery seed is mixed with sodium chloride solution, heated for extraction, and then the water is absorbed to obtain the celery seed volatile oil.

5. The use according to claim 1, characterized in that, The golden chamomile extract is prepared by the following method: (S1) The golden chamomile is mixed with ethanol and then heated for reflux treatment, vacuum filtration, and ethanol concentration and evaporation to obtain a pretreated product; (S2) The pretreated product obtained in step (S1) is dissolved and then extracted with petroleum ether and ethyl acetate in sequence to obtain the golden chamomile extract.

6. Use of a polysaccharide composition in the preparation of a product having synergistic anti-UV, anti-bacterial, and penetration enhancing properties, characterized in that, The polysaccharide composition includes a complex containing celery seed volatile oil and extract of golden chamomile and polysaccharide in a mass ratio of 1:1, The complex containing celery seed volatile oil and extract of golden chamomile includes celery seed volatile oil and golden chamomile extract in a mass ratio of 1:

5.

7. Use according to claim 6, characterized in that, The polysaccharide is selected from one of kelp polysaccharide, sea asparagus polysaccharide, ginkgo polysaccharide, or platycladus polysaccharide.

8. Use according to claim 6, characterized in that, The polysaccharide is kelp polysaccharide.

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