Plant-derived sterilization deodorant and application thereof in daily chemical products

Abstract

The invention relates to the field of daily chemicals, and discloses a plant-derived sterilization deodorant and application thereof in daily chemical products. The sterilizing deodorant comprises at least two, preferably three, of pepper leaf extract, celery leaf extract and syzygium jambos leaf extract, and is matched with decyl glucoside, citric acid, a chelating agent and an optional deep eutectic solvent to form a stable water-alcohol system. Through specific proportion compounding and process condition control, efficient bacteriostasis on staphylococcus aureus, staphylococcus epidermidis, candida albicans and trichophyton rubrum is achieved, meanwhile, the concentration of odor substances is remarkably reduced, and the deodorant has the functions of source bacteriostasis and direct deodorization. The physical stability and the antibacterial activity retention rate of the system are further improved by adopting a deep eutectic solvent composed of glycerol and choline chloride, so that the deep eutectic solvent is suitable for preparing daily chemical products such as shoe and sock spray, body spray and fabric freshener.

Description

Technical Field

[0001] This invention relates to the field of daily chemical technology, and in particular to a plant-derived bactericide and deodorizer and its application in daily chemical products. Background Technology

[0002] For odors such as foot odor and armpit odor caused by the decomposition of sweat and sebum, existing products mostly use sprays and wipes containing alcohol, quaternary ammonium salt bactericides, or synthetic preservatives to achieve odor removal through sterilization and fragrance masking. While these products have some antibacterial effect, they are prone to skin irritation, have limited inhibitory effect on fungi such as Trichophyton rubrum, and are not very efficient at removing malodorous molecules such as short-chain fatty acids, represented by isovaleric acid. Therefore, they fail to achieve both broad-spectrum sterilization and highly effective odor removal.

[0003] CN111773910A discloses a fulvic acid-based bactericide and deodorizer, which is a compound of modified fulvic acid with extracts of soapberry, camphor, ginger, and peppermint, used for the treatment of environmental odors from domestic waste, livestock farms, and industrial waste gases. This system contains cationic surfactants such as dodecyltrimethylammonium chloride, has a darker color, and is more suitable for environmental spraying; however, it has limitations in terms of safety, ingredient sourcing, and transparency when in long-term contact with skin, shoes, socks, and other close-fitting fabrics, and lacks a systematic evaluation for sweat odor, foot odor model substances, and fungi related to athlete's foot.

[0004] CN111150694A discloses a plant-based antibacterial agent that combines extracts of Rhodiola rosea, aloe vera, Sapindus mukorossi, and Phellodendron amurense with silver ions, lactic acid, polyvinylpyrrolidone, and capryloyl glycine for use in wet wipes and feminine washes as a preservative and antibacterial agent. This technology requires the introduction of metal ions such as silver sulfate or silver nitrate, and the system is not entirely plant-based. There are still concerns regarding long-term use and environmental accumulation. Furthermore, it primarily addresses the issues of antibacterial activity and formula stability, failing to provide rapid and efficient deodorization for typical body odors such as foot odor, and also neglecting to ensure the high light transmittance and long-term maintenance of antibacterial activity of multiple plant extracts in a water-alcohol system. Summary of the Invention

[0005] In view of the above-mentioned deficiencies of the prior art, the technical problem to be solved by the present invention is to provide a plant-derived bactericide and deodorizer with a clear source and without introducing quaternary ammonium salt bactericides and metal antibacterial components such as silver ions. This deodorizer has the ability to effectively inhibit common bacteria and fungi in daily chemical applications such as shoes, socks, sports shoe cavities, fabrics and human skin, and has a significant ability to remove isovaleric acid, the root cause of foot odor. At the same time, it has good physical stability and antibacterial activity retention in water-alcohol systems, and can be easily applied to various daily chemical products.

[0006] To achieve the above objectives, the present invention provides a plant-derived bactericide and deodorizer, comprising the following components: Plant extracts 1-15 wt%; Nonionic surfactant 0.1-5wt%; pH adjuster 0.05-3wt%; Chelating agent 0.01-1wt%; 1-40 wt% ethanol The remainder is water; The plant extract is selected from at least two of pepper leaf extract, celery leaf extract, and rose apple leaf extract.

[0007] Preferably, the plant-derived bactericide and deodorizer comprises the following components: Plant extracts 3-10 wt%; Nonionic surfactant 0.2-2wt%; pH adjuster 0.1-1 wt%; Chelating agent 0.02-0.5 wt%; 5-25 wt% ethanol The remainder is water.

[0008] During the research and development process, the inventors experimented with dozens of common antibacterial plant extracts and combinations thereof, including peppermint, mugwort, tea polyphenols, and honeysuckle. Experiments revealed that while some combinations were effective against Staphylococcus aureus, they were extremely ineffective against fungi such as Trichophyton rubrum; other combinations, while showing some antibacterial activity, produced an unpleasant odor when mixed with isovaleric acid. Through extensive screening, they unexpectedly discovered that a specific combination of pepper leaves, celery leaves, and rose apple leaves in a particular ratio could simultaneously achieve both antibacterial (especially against fungi) effects and highly effective chemical removal of isovaleric acid.

[0009] More preferably, the plant extract is a mixture of pepper leaf extract, celery leaf extract, and rose apple leaf extract in a mass ratio of 1-3:1-3:1-2. By combining these specific types of plant extracts, a synergistic effect can be achieved, significantly enhancing the inhibitory effect against Staphylococcus aureus, Staphylococcus epidermidis, Candida albicans, and Trichophyton rubrum. This combination can effectively adsorb, mask, or neutralize typical odor molecules such as short-chain fatty acids, represented by isovaleric acid, achieving a dual mechanism of sterilization at the source and direct chemical deodorization.

[0010] Preferably, the nonionic surfactant is decyl glucoside. The addition of a nonionic surfactant helps to disperse and stabilize the active ingredient and improves its wetting and penetration into skin and fabric surfaces.

[0011] Preferably, the pH adjuster is citric acid. The chelating agent is disodium ethylenediaminetetraacetate. The pH adjuster and the chelating agent work synergistically, on the one hand adjusting the system to a suitable acidic environment to enhance antibacterial activity and stability, and on the other hand binding metal ions to prevent discoloration and degradation of active ingredients.

[0012] Furthermore, to enhance the physical stability and activity retention of the plant-derived bactericide and deodorizer during long-term storage, the plant-derived bactericide and deodorizer also contains 1-8 wt% eutectic solvent. The eutectic solvent provides a stable microenvironment for the active ingredients in the plant extracts, inhibiting their aggregation and precipitation.

[0013] Preferably, the eutectic solvent is a combination of glycerol and choline chloride. Experiments show that the eutectic solvent formed by combining glycerol and choline chloride in a mass ratio of 1-2:1 is the most effective in inhibiting the increase of turbidity in the system and maintaining antibacterial activity, significantly better than adding glycerol or choline chloride alone.

[0014] The present invention also provides the application of the above-mentioned plant-derived bactericides and deodorizers in the preparation of daily chemical products, especially for the preparation of spray products with bactericide and deodorizer functions, such as shoe and sock deodorizing spray, body freshening spray, fabric deodorizing spray or wet wipe liquid.

[0015] The beneficial effects of this invention are: This invention primarily utilizes plant-derived active ingredients, avoiding or reducing the use of traditional chemical bactericides, metal ions, and irritating solvents. Simultaneously, this system is compatible with various daily chemical product bases, and is particularly suitable for formulating transparent or semi-transparent sprays, wet wipes, etc., such as shoe and sock deodorizing sprays, body freshening sprays, and fabric care products, meeting the market demand for natural, efficient, and multifunctional daily chemical products.

[0016] This invention utilizes a specific combination of at least two extracts from pepper leaves, celery leaves, and rose apple leaves, resulting in a significant synergistic effect of the active ingredients in these different extracts. Compared to using single plant extracts, this compound system exhibits a significantly enhanced inhibition rate against bacteria such as Staphylococcus aureus and Staphylococcus epidermidis, especially against fungi associated with athlete's foot and body odor, such as Candida albicans and Trichophyton rubrum. Test data shows that the combination of pepper leaf extract, celery leaf extract, and rose apple leaf extract can achieve an inhibition rate of over 99% against the aforementioned four test bacteria within 30 minutes, effectively blocking odors caused by microbial proliferation at the source.

[0017] The compound system of this invention not only indirectly eliminates odors through antibacterial action but also directly and rapidly reduces the concentration of typical odor-causing substances in the environment. Experiments have shown that this system has a high removal rate for isovaleric acid, a model substance for foot odor. The deodorization rate of the compound extracts of pepper leaves, celery leaves, and rose apple leaves can reach over 83%, significantly better than that of pepper leaf extracts, celery leaf extracts, and rose apple leaf extracts alone or in pairs. This indicates that multiple plant active ingredients can work synergistically through adsorption, masking, neutralization, and other mechanisms to achieve highly efficient removal of malodorous molecules such as short-chain fatty acids.

[0018] This invention introduces a specific eutectic solvent, particularly a combination of glycerol and choline chloride, into an aqueous system to provide a stable microenvironment for active ingredients such as polyphenols and flavonoids in plant extracts. This eutectic solvent system effectively inhibits the aggregation and precipitation of active ingredients, enabling the product to maintain high transmittance and antibacterial activity retention under long-term room temperature storage, accelerated aging, and freeze-thaw cycles. It solves common problems in plant extract formulations such as turbidity, stratification, and activity attenuation, ensuring product shelf-life stability and consistent efficacy. Detailed Implementation

[0019] The parameters and sources of some raw materials in the examples are as follows: The following examples are provided to further illustrate the present invention, but do not constitute a limitation on the scope of protection of the present invention. Unless otherwise stated, those skilled in the art can use conventional equipment and reagents.

[0020] In the examples, pepper leaf extract, celery leaf extract, and rose apple leaf extract were all prepared according to the following general method.

[0021] Pepper leaves, taken from dried leaves of pepper (Piper nigrum L.), with a moisture content ≤12wt%; origin: Zhangzhou, Fujian.

[0022] Syzygium jambos leaves are dried leaves of Syzygium jambos (L.) Alston, a plant belonging to the genus Syzygium in the family Myrtaceae, with a moisture content of ≤12wt%; produced in Qingyuan, Guangdong.

[0023] The leaves of celery (Apium graveolens L.) were dried and had a moisture content of ≤12wt%; the celery leaves were produced in Weifang, Shandong.

[0024] Preparation methods of pepper leaf extract, celery leaf extract, and rose apple leaf extract: Take pepper leaves as an example (the same procedure applies to celery leaves and rose apple leaves). (1) Rinse commercially available dried pepper leaves with tap water, drain the surface moisture, and dry them in a hot air circulating drying oven at 45-50℃ until the moisture content is ≤10wt%; after coarse crushing in a pulverizer, pass through a 40-mesh sieve to obtain coarse pepper leaf powder for later use. (2) Take 1.0 kg of coarse pepper leaf powder and add it to a stainless steel extraction tank equipped with a stirring and reflux condenser. Add 10 L of 70 wt% ethanol aqueous solution. Reflux extract at 50 rpm and 60 ℃ for 2 h. Filter through a 40 mesh sieve and collect the filtrate. Add another 10 L of 70 wt% ethanol aqueous solution to the filter residue and repeat the above reflux extraction at 60 ℃ for 2 h. After filtering through a 40 mesh sieve, combine the two filtrates to obtain a combined extract of about 18-19 L. (3) Place the combined extracts in a rotary evaporator and concentrate them under reduced pressure at 0.08 MPa and 50°C to a relative density of about 1.05-1.15 (50°C); take the concentrate, dry it and determine the solid content, which should be controlled at (20±2) wt%. If the solid content is too high, add a small amount of 70 wt% ethanol aqueous solution to dilute it; if it is too low, further evaporate the water until the standard is met; the resulting paste is pepper leaf extract; store at 4°C for later use.

[0025] Example 1 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 was prepared by adding 0.10 g of disodium ethylenediaminetetraacetate and 0.80 g of citric acid to 60 g of deionized water under stirring at 300 rpm, and stirring until completely dissolved to obtain an aqueous phase. S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3. Under stirring at 300 rpm, 3.00 g of pepper leaf extract, 3.00 g of celery leaf extract, and 2.00 g of rose apple leaf extract were added to the aqueous phase prepared in step S1 and stirred for 20 min. The ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min. Deionized water was added to bring the total mass to 100 g and the mixture was stirred evenly. 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5. The mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0026] Example 2 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 was prepared by adding 0.10 g of disodium ethylenediaminetetraacetate and 0.80 g of citric acid to 60 g of deionized water under stirring at 300 rpm, and stirring until completely dissolved to obtain an aqueous phase. S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3: Under stirring at 300 rpm, 4.00 g of pepper leaf extract and 4.00 g of rose apple leaf extract were added to the aqueous phase prepared in step S1 and stirred for 20 min; the ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min; deionized water was added to bring the total mass to 100 g and mixed evenly; 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5; the mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0027] Example 3 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 was prepared by adding 0.10 g of disodium ethylenediaminetetraacetate and 0.80 g of citric acid to 60 g of deionized water under stirring at 300 rpm, and stirring until completely dissolved to obtain an aqueous phase. S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3: Under stirring at 300 rpm, 4.00 g of celery leaf extract and 4.00 g of rose apple leaf extract were added to the aqueous phase prepared in step S1 and stirred for 20 min; the ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min; deionized water was added to bring the total mass to 100 g and mixed evenly; 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5; the mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0028] Example 4 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 was prepared by adding 0.10 g of disodium ethylenediaminetetraacetate and 0.80 g of citric acid to 60 g of deionized water under stirring at 300 rpm, and stirring until completely dissolved to obtain an aqueous phase. S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3: Under stirring at 300 rpm, 4.00 g of pepper leaf extract and 4.00 g of celery leaf extract were added to the aqueous phase prepared in step S1 and stirred for 20 min; the ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min; deionized water was added to bring the total mass to 100 g and mixed evenly; 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5; the mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0029] Comparative Example 1 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 was prepared by adding 0.10 g of disodium ethylenediaminetetraacetate and 0.80 g of citric acid to 60 g of deionized water under stirring at 300 rpm, and stirring until completely dissolved to obtain an aqueous phase. S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3: 8.00 g of pepper leaf extract was added to the aqueous phase prepared in step S1 and stirred for 20 min under stirring at 300 rpm; the ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min; deionized water was added to bring the total mass to 100 g and mixed evenly; 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5; the mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0030] Comparative Example 2 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 was prepared by adding 0.10 g of disodium ethylenediaminetetraacetate and 0.80 g of citric acid to 60 g of deionized water under stirring at 300 rpm, and stirring until completely dissolved to obtain an aqueous phase. S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3: Under stirring at 300 rpm, 8.00 g of celery leaf extract was added to the aqueous phase prepared in step S1 and stirred for 20 min; the ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min; deionized water was added to bring the total mass to 100 g and mixed evenly; 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5; the mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0031] Comparative Example 3 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 was prepared by adding 0.10 g of disodium ethylenediaminetetraacetate and 0.80 g of citric acid to 60 g of deionized water under stirring at 300 rpm, and stirring until completely dissolved to obtain an aqueous phase. S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3: 8.00 g of Syzygium aromaticum leaf extract was added to the aqueous phase prepared in step S1 and stirred for 20 min under stirring at 300 rpm; the ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min; deionized water was added to bring the total mass to 100 g and mixed evenly; 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5; the mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0032] Example 5 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 adds 0.10g of disodium ethylenediaminetetraacetate, 0.80g of citric acid and 3.00g of eutectic solvent to 60g of deionized water under stirring at 300rpm, and stirs until completely dissolved to obtain an aqueous phase; the eutectic solvent is composed of 2.0g of glycerol and 1.0g of choline chloride.

[0033] S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3. Under stirring at 300 rpm, 3.00 g of pepper leaf extract, 3.00 g of celery leaf extract, and 2.00 g of rose apple leaf extract were added to the aqueous phase prepared in step S1 and stirred for 20 min. The ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min. Deionized water was added to bring the total mass to 100 g and the mixture was stirred evenly. 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5. The mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0034] Example 6 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 adds 0.10g of disodium ethylenediaminetetraacetate, 0.80g of citric acid and 3.00g of eutectic solvent to 60g of deionized water under stirring at 300rpm, and stirs until completely dissolved to obtain an aqueous phase; the eutectic solvent is glycerol.

[0035] S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3. Under stirring at 300 rpm, 3.00 g of pepper leaf extract, 3.00 g of celery leaf extract, and 2.00 g of rose apple leaf extract were added to the aqueous phase prepared in step S1 and stirred for 20 min. The ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min. Deionized water was added to bring the total mass to 100 g and the mixture was stirred evenly. 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5. The mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0036] Example 7 A method for preparing a plant-derived bactericide and deodorizer includes the following steps: S1 adds 0.10 g of disodium ethylenediaminetetraacetate, 0.80 g of citric acid and 3.00 g of eutectic solvent to 60 g of deionized water under stirring at 300 rpm, and stirs until completely dissolved to obtain an aqueous phase; the eutectic solvent is choline chloride.

[0037] S2 added 1.50 g of decyl glucoside to 5.00 g of anhydrous ethanol under stirring at 300 rpm; stirred until uniformly mixed to obtain a homogeneous ethanol-surfactant phase; S3. Under stirring at 300 rpm, 3.00 g of pepper leaf extract, 3.00 g of celery leaf extract, and 2.00 g of rose apple leaf extract were added to the aqueous phase prepared in step S1 and stirred for 20 min. The ethanol-surfactant phase obtained in step S2 was added and stirred for 10 min. Deionized water was added to bring the total mass to 100 g and the mixture was stirred evenly. 0.1 mol / L citric acid aqueous solution was added to adjust the pH to 4.5. The mixture was filtered through a 0.45 μm filter membrane to remove particulate impurities, thus obtaining the plant-derived bactericide and deodorizer.

[0038] Test Example 1 The bacterial / fungal antimicrobial test shall be performed in accordance with GB / T20944.3-2008 "Evaluation of antimicrobial properties of textiles - Part 3: Shaking method" with appropriate adjustments, for the evaluation of antimicrobial properties of liquid sprays.

[0039] Test subject: Staphylococcus aureus, commercially available, strain number ATCC 6538.

[0040] Staphylococcus epidermidis, commercially available, strain number ATCC 12228.

[0041] Candida albicans, commercially available, strain number ATCC10231.

[0042] Trichophyton rubrum, commercially available, strain number ATCC 28188.

[0043] (1) Culture medium Bacteria: Tryptone soybean broth (TSB) and tryptone soybean agar (TSA). Fungi: Sabouraud glucose broth and Sabouraud agar plates (SDA).

[0044] (2) Preparation of bacterial suspension Each strain was cultured at 37°C (30°C for fungi) on its corresponding solid culture medium for 24 hours.

[0045] The bacterial cells were eluted with sterile physiological saline, and the concentration of the bacterial suspension was adjusted to approximately 1 × 10⁻⁶ using a spectrophotometer or plate counting method. 6 CFU / mL.

[0046] (3) Sample processing The original spray solutions of Examples 1-4 and Comparative Examples 1-3 were used as test samples, and blank matrices containing the same excipients but without plant extracts were set up.

[0047] (4) Inoculation and Effect Take an Erlenmeyer flask, add 9.0 mL of each sample spray, add 1.0 mL of bacterial suspension (10-fold dilution), mix well, and place in a 37℃ (30℃ for fungi) constant temperature shaking incubator for 30 min at a shaking speed of 120 rpm.

[0048] Meanwhile, a bacterial suspension without samples was set up as a control group (N0).

[0049] (5) Sampling and counting After the reaction was completed, an appropriate amount of the mixture was taken from each tube and serially diluted tenfold. 100 μL of the appropriate dilution was spread on the corresponding solid culture medium plate and incubated at 37°C (30°C for fungi) for 48 h.

[0050] Count the number of colonies on the plate and convert them into the number of viable bacteria per mL of suspension, Nt (sample group) and N0 (control group).

[0051] (6) Calculation of antibacterial rate Antibacterial rate (%) = (1-Nt / N0)×100%.

[0052] Table 1 Results of antibacterial rate test Note: The blank matrix is ​​a formulation that does not contain plant extracts but contains the same excipients, used to exclude the influence of surfactants and ethanol itself.

[0053] The blank matrix showed inhibition rates of 7.5%-12.3% against the four test bacteria, indicating only a very limited inhibitory effect. This suggests that the basic system of decyl glucoside, a small amount of ethanol, and citric acid does not possess significant broad-spectrum antibacterial activity. After introducing plant extracts, the inhibition rates of all examples and comparative examples were significantly higher than those of the blank matrix, demonstrating that pepper leaf extract, celery leaf extract, and rose apple leaf extract themselves have strong inhibitory effects on bacterial / fungal activity.

[0054] Example 2 (pepper leaf extract and rose apple leaf extract) showed antibacterial rates of over 98.5% against bacteria and 96.2% and 95.8% against fungi, respectively, significantly higher than the three single extracts, especially against Candida albicans and Trichophyton rubrum, with an increase of approximately 8-12%. Examples 3 (celery leaf extract and rose apple leaf extract) and 4 (pepper leaf extract and celery leaf extract) showed antibacterial rates exceeding 93% against all four bacteria, generally higher than the single formulations that showed the best effect against the corresponding two plants, reflecting a certain synergistic effect produced by the combination. The antibacterial spectrum of the combined samples was also relatively balanced, showing good inhibition against both bacteria and fungi, without any significant weakness against any particular bacterial species.

[0055] Example 1 showed that the inhibition rate of the four bacteria was above 99.0% within 30 minutes, achieving near-complete eradication. Compared with Comparative Examples 1-3, the inhibition rate against Candida albicans and Trichophyton rubrum was significantly improved. For example, the inhibition rate against Candida albicans increased from 84.2% (Comparative Example 1) to 99.2%, an increase of about 15%. Compared with the combination of the two, Example 1 still showed an increase of 1-3% in the inhibition rate against the four bacteria, and the inhibition rates of the four bacteria were more consistent, indicating that when the three plant extracts work together, they can form a better spectral synergy among different bacterial species.

[0056] Test Example 2 Odor removal performance test 1. Odor Model and Principle Odors from shoes and sports equipment primarily originate from the decomposition of sweat and dander by resident skin bacteria and environmental fungi, producing various volatile organic compounds, including short-chain fatty acids (such as isovaleric acid), organic amines, ammonia, and thiols. Isovaleric acid has a typical "foot odor" and is a commonly used odor model substance.

[0057] This test uses isovaleric acid to simulate body odor / foot odor, and evaluates the deodorizing ability by measuring the change in isovaleric acid concentration in the head space before and after spray treatment.

[0058] 2. Test method (isovaleric acid deodorization rate) (1) Preparation of simulated odor source: Dissolve 0.1g of isovaleric acid in 5mL of anhydrous ethanol and dilute to 1L with deionized water to obtain an aqueous solution of isovaleric acid with a concentration of 100mg / L.

[0059] (2) Take 10 mL of 100 mg / L isovaleric acid aqueous solution and add it to a 500 mL stoppered glass bottle. Let it stand for 30 min to establish a stable head space concentration as the initial state.

[0060] (3) In the initial state, a certain volume of gas in the head space of the bottle is extracted by gas chromatography (GC), and the peak area or mass concentration of isovaleric acid is measured and recorded as C0. 2.0 g of the test spray is sprayed into the bottle, the stopper is quickly tightened, and then it is left to stand for 30 min.

[0061] The gas in the headspace was extracted again for GC analysis, and the concentration of isovaleric acid (Ct) was measured.

[0062] Each sample should be measured in parallel at least 3 times.

[0063] (4) Deodorization rate calculation Deodorization rate (%) = (1-Ct / C0)×100%.

[0064] 3. Results illustration Table 2. Deodorization rate of isovaleric acid Note: The blank matrix is ​​a formulation that does not contain plant extracts but contains the same excipients.

[0065] The deodorization rate of the blank matrix for isovaleric acid was 18.0%, mainly due to the partial dissolution and partitioning effect of ethanol and surfactants on isovaleric acid, as well as the partial ionization effect of citric acid on isovaleric acid; indicating that without the addition of plant extracts, the basic system has limited adsorption / removal capacity for foot odor model substances.

[0066] The deodorization rates of Comparative Examples 1-3 were 58.0%, 55.0%, and 59.0%, respectively, all of which were significantly improved compared with the blank matrix. This indicates that the polyphenols, flavonoids, and aromatic volatile oils contained in each plant extract can adsorb or mask isovaleric acid to a certain extent, while also changing the overall odor perception through their own odor. The deodorization rates of the three single plant extracts were close (55-59%), with little difference, indicating that although the chemical removal ability of isovaleric acid is enhanced when any plant extract is used alone, it still does not have a highly efficient and rapid deodorization effect.

[0067] Example 2 (pepper leaf extract and rose apple leaf extract) had a deodorization rate of 73.0%, which was about 14-18% higher than all single plant samples. Example 3 (celery leaf extract and rose apple leaf extract) and Example 4 (pepper leaf extract and celery leaf extract) had deodorization rates of 71.0% and 74.0%, respectively, both significantly better than the average level of their respective single plant combinations. This indicates that the combination of these two plants can introduce richer plant components in addition to the basic dissolution / adsorption effect, forming multi-site interactions on odor molecules (such as hydrogen bonds, hydrophobic interactions, and π-π interactions), and synergistically weakening the odor perception of isovaleric acid through a more complex plant odor composition.

[0068] Example 1 achieved a deodorization rate of 83.0%, significantly higher than all the paired and single plant samples, and approximately 24% higher than the highest value (59.0%) in the control group. Within the same action time, Example 1 reduced the concentration of isovaleric acid in the headspace from 50.0 mg / m³. 3 Reduced to 8.5 mg / m³ 3 The odor removal rate was nearly complete; compared with Examples 2-4, the deodorization rate of Example 1 increased by 9-12%, indicating that pepper leaf extract, celery leaf extract, and rose apple leaf extract have a significant synergistic effect in the removal of isovaleric acid, a typical odor molecule. This may be because the various phenolic, flavonoid, and volatile oil components in pepper leaf extract, celery leaf extract, and rose apple leaf extract can synergistically adsorb and partially chemically neutralize short-chain fatty acids such as isovaleric acid, thus enhancing the overall deodorization effect.

[0069] Comprehensive antibacterial and deodorizing tests show that the compound system of pepper leaf extract, celery leaf extract and rose apple leaf extract of the present invention can effectively inhibit common bacteria and fungi related to sweat and dandruff, and can also efficiently reduce the concentration of isovaleric acid, a typical model substance of foot odor, in the air. It achieves a dual deodorizing mechanism of inhibiting bacteria at the source and directly reducing odor, which is significantly better than single plant extract formulations.

[0070] Test Example 3 Stability test Storage at room temperature: Conditions: 25±2℃, protected from light; Time: 6 months.

[0071] Accelerated storage: Conditions: 40±2℃ constant temperature incubator, protected from light; Time: 3 months.

[0072] Freeze-thaw cycle: Conditions: Freeze at -5℃ for 24 hours, then thaw at 25℃ for 24 hours as one cycle; Number of cycles: 5.

[0073] The transmittance at 600 nm was used as a quantitative indicator of turbidity change. Antibacterial activity retention rate: Referring to test example 1, using Staphylococcus aureus as the representative bacterial species, the antibacterial rate was measured 30 min before and after storage under the same conditions; antibacterial activity retention rate = (antibacterial rate after storage / initial antibacterial rate) × 100%.

[0074] Table 3. Stability test of the bactericide and deodorizer in Example 1 Table 4. Stability test of the bactericide and deodorizer in Example 5 Table 5. Stability test of the bactericide and deodorizer in Example 6 Table 6. Stability test of the bactericide and deodorizer in Example 7 In Example 1, the transmittance decreased from 98.0% to 93.0% after 6 months at room temperature (25°C), further decreased to 90.0% after 3 months of accelerated treatment at 40°C, and reached 92.5% after 5 freeze-thaw cycles. This indicates that although there was no obvious stratification or large particle precipitation under long-term and accelerated conditions, the turbidity of Example 1 increased, indicating a certain degree of colloidal aggregation or fine precipitate formation.

[0075] In Example 6, the transmittance decreased to 91.5% after 3 months at 40°C, and in Example 7, it decreased to 89.0%. Example 7 showed the largest decrease in transmittance, reaching only 90.5% after freeze-thaw cycles. This indicates that adding glycerol or choline chloride alone is insufficient to effectively inhibit the self-aggregation of polyphenols, flavonoids, and other components in plant extracts or their adverse interactions with the surfactant system. In contrast, Example 5 exhibited significantly better physical stability under the same conditions: after 6 months at 25°C, the transmittance remained at 97.0%, a decrease of only 1.0%; after 3 months of accelerated processing at 40°C, the transmittance remained at 96.5%, an increase of 6.5% compared to 90.0% in Example 1, 5.0% compared to 91.5% in Example 6, and 7.5% compared to 89.0% in Example 7; after 5 freeze-thaw cycles, the transmittance was 96.8%, essentially close to the initial value. The possible reason is that the deep eutectic solvent system composed of glycerol and choline chloride in a certain proportion (Example 5) can provide a more stable microenvironment for the extracts of pepper leaves, celery leaves, and rose apple leaves. This system inhibits the aggregation of active ingredients through hydrogen bonding networks and ionic interactions, significantly improving the physical stability of the formulation. Compared to Examples 1, 6, and 7, Example 5 shows a significant advantage in light transmittance exceeding 5%.

[0076] In terms of antibacterial activity retention rate, the antibacterial activity retention rate of Example 5 is significantly better than that of Examples 1, 6, and 7. This indicates that the deep eutectic solvent system composed of glycerol and choline chloride not only improves physical stability but also significantly enhances the ability to retain plant antibacterial activity during storage.

[0077] The preferred embodiments of the present invention have been described in detail above. It should be understood that those skilled in the art can make numerous modifications and variations based on the concept of the present invention without creative effort. Therefore, all technical solutions that can be obtained by those skilled in the art based on the concept of the present invention through logical analysis, reasoning, or limited experimentation on the basis of existing technology should be within the scope of protection defined by the claims.

Claims

1. A plant-based bactericide and deodorizer, characterized in that, Includes the following components: Plant extracts 1-15 wt%; Nonionic surfactant 0.1-5wt%; pH adjuster 0.05-3wt%; Chelating agent 0.01-1wt%; 1-40 wt% ethanol The remainder is water; The plant extract is selected from at least two of pepper leaf extract, celery leaf extract, and rose apple leaf extract.

2. The plant-derived bactericide and deodorizer as described in claim 1, characterized in that, It consists of the following components: Plant extracts 3-10 wt%; Nonionic surfactant 0.2-2wt%; pH adjuster 0.1-1 wt%; Chelating agent 0.02-0.5 wt%; 5-25 wt% ethanol The remainder is water.

3. The plant-derived bactericide and deodorizer as described in claim 1 or 2, characterized in that: The plant extract is a mixture of pepper leaf extract, celery leaf extract and rose apple leaf extract in a mass ratio of 1-3:1-3:1-2.

4. The plant-derived bactericide and deodorizer as described in claim 1 or 2, characterized in that: The nonionic surfactant is decyl glucoside.

5. The plant-derived bactericide and deodorizer as described in claim 1 or 2, characterized in that: The pH adjuster is citric acid.

6. The plant-derived bactericide and deodorizer as described in claim 1 or 2, characterized in that: The chelating agent is disodium ethylenediaminetetraacetate.

7. The plant-derived bactericide and deodorizer as described in claim 1 or 2, characterized in that: The plant-derived bactericide and deodorizer also contains 1-8 wt% eutectic solvent.

8. The plant-derived bactericide and deodorizer as described in claim 7, characterized in that: The eutectic solvent is a combination of glycerol and choline chloride.

9. The use of the plant-derived bactericide and deodorizer as described in any one of claims 1-8 in the preparation of daily chemical products.

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