An antibacterial mask with a catalytic sterilization function and a preparation method thereof

Abstract

The application discloses an antibacterial mask with a catalytic sterilization function, which comprises an outer non-woven fabric, a melt-blown layer and an inner non-woven fabric, wherein the melt-blown layer comprises an antibacterial layer formed by a single-atom / plant polyphenol-metal complex catalyst / RdCVFs composite bactericide; the single-atom catalyst is compounded with the plant polyphenol-metal complex by using the electrostatic adsorption effect, and then the single-atom catalyst is used as a carrier of the RdCVFs antibacterial and antiviral drug, so that the multifunctional synergistic antibacterial purpose of the material is achieved. The novel antibacterial mask provided by the application can quickly kill gram-negative bacteria (Escherichia coli), gram-positive bacteria (Staphylococcus aureus) and fungi (Candida albicans) without other auxiliary conditions (light, hydrogen peroxide).

Description

TECHNICAL FIELD

[0001] The application belongs to the technical field of protective articles, and particularly relates to an antibacterial mask with catalytic sterilization function and a preparation method thereof. BACKGROUND

[0002] A mask is a daily facial hygiene product, which can be worn on the mouth and nose to filter the air entering the mouth and nose and block harmful gas and droplets. The mask plays an important role in preventing and blocking the spread of bacteria. For bacteria and microorganisms (Escherichia coli, Staphylococcus aureus, Mycobacterium tuberculosis and Candida albicans), wearing a mask can greatly prevent the spread of bacteria through air, saliva, body contact and other means, thereby reducing the threat of pathogenic bacteria to human health. However, due to the short use cycle (8 h) of commercially available disposable medical masks, large production capacity and people's random disposal, mask pollution is inevitable. Medical masks carrying pathogenic bacteria cannot kill bacteria, on the contrary, the bacterial contamination source continues to adhere to the outer layer of non-woven fabric and continues to multiply, which is a great hidden danger to human health and the environment. If not properly handled, it may even cause the spread of pathogenic bacteria among people again.

[0003] Therefore, it is of positive significance to design and develop an antibacterial mask with catalytic sterilization function. SUMMARY

[0004] The application aims to provide an antibacterial mask with catalytic sterilization function and a preparation method thereof.

[0005] In order to achieve the above-mentioned purpose, the application adopts the following technical solutions:

[0006] An antibacterial mask with catalytic sterilization function comprises an outer layer of non-woven fabric, a melt-blown layer and an inner layer of non-woven fabric, and is prepared by the following steps:

[0007] Step 1: preparing a monatomic catalyst;

[0008] Step 2: preparing a plant polyphenol-metal complex;

[0009] Step 3: adding the monatomic catalyst and the plant polyphenol-metal complex to water, and stirring to obtain a monatomic / plant polyphenol-metal complex catalyst, wherein the mass ratio of the monatomic catalyst, the plant polyphenol-metal complex and water is 1:1:100;

[0010] Step 4: adding 1-1.5 mL of a Remdesivir solution to 100 mL of the monatomic / plant polyphenol-metal complex catalyst solution, and stirring to obtain a monatomic / plant polyphenol-metal complex catalyst / Remdesivir;

[0011] The remdesivir solution is obtained by dissolving 200 mg of remdesivir in 5 mL of an ethanol solution, and the monatomic / plant polyphenol-metal complex catalyst solution is obtained by dissolving 0.5-1.5 g of a monatomic / plant polyphenol-metal complex catalyst in 100 mL of water;

[0012] Step 5, dissolving the monatomic / plant polyphenol-metal complex catalyst / remdesivir in water to obtain solution A, dissolving disodium hydrogen phosphate dodecahydrate and citric acid in water to obtain solution B, placing the melt-blown fabric in solution A, then adding solution B, and drying after standing for 0.5-1 h to obtain a melt-blown layer;

[0013] The concentration of the monatomic / plant polyphenol-metal complex catalyst / remdesivir in solution A is 500 μg / mL-1000 μg / mL; the concentration of disodium hydrogen phosphate in solution B is 200 mmol / L-400 mmol / L, and the concentration of citric acid is 100 mmol / L-200 mmol / L;

[0014] For each 40 pieces of melt-blown fabric with a size of 2 cm*3 cm, 100 mL of solution A and 100 mL of solution B are used;

[0015] Step 6, assembling the outer non-woven fabric, the melt-blown layer, and the inner non-woven fabric to obtain the antibacterial mask.

[0016] Further, the monatomic catalyst is composed of a transition metal and a carbon-based carrier, the transition metal is selected from one or more of Cu, Fe, and Mn, and the carrier is one of zeolitic imidazolate framework material (ZIF-8), mesoporous nitrogen-doped carbon sphere material, or carbon quantum dots. Preferably, the mass ratio of the transition metal to the carrier is 1:50-1:100.

[0017] In an embodiment of the present application, the preparation method of the monatomic catalyst with ZIF-8 as the carrier comprises the following steps:

[0018] Step 1, weighing dimethyl imidazole, zinc nitrate hexahydrate, and a metal salt into an aqueous solution, stirring at room temperature (20-30 ℃) for 1 h to obtain a precursor solution, wherein the mass ratio of dimethyl imidazole, zinc nitrate hexahydrate, and the metal salt is 10:10:1;

[0019] Step 2, centrifuging the precursor solution and drying to obtain metal-ZIF-8 material, wherein the centrifugation speed is 5000-6000 r / min, the time is 5-10 min, the drying temperature is 40-50 ℃, and the time is 1-2 h;

[0020] Step three, the obtained metal-ZIF-8 material is heated at 800-1000 ℃ for 4-6 h under nitrogen atmosphere to obtain the required monatomic catalyst.

[0021] In an embodiment of the present application, the preparation method of the monatomic catalyst with mesoporous nitrogen-doped carbon spheres as the carrier comprises the following steps:

[0022] Step one, weigh dopamine hydrochloride and poloxamer F127, dissolve them in an ethanol / water solution (volume ratio 1:1), stir at room temperature for 15 min, add 4 mL of 1,3,5-trimethylbenzene, and react at a speed of 500 r / min for 30 min to form a nanoemulsion system, then add 10 mL of ammonia water to initiate the reaction and polymerize for 30 min. Finally, add the metal salt at the same speed and react for 30 min to obtain a precursor solution; the mass ratio of dopamine hydrochloride, poloxamer F127 and metal salt is 100:200:1;

[0023] Step two, centrifuge the precursor solution, dry it, the centrifugation speed is 5000-6000 r / min, the time is 5-10 min, the drying temperature is 40-50 ℃, and the time is 1-2 h;

[0024] Step three, the obtained metal-mesoporous nitrogen-doped carbon sphere monatomic catalyst precursor material is heated at 800-1000 ℃ for 3-6 h under nitrogen atmosphere to obtain the required monatomic catalyst.

[0025] In an embodiment of the present application, the preparation method of the monatomic catalyst with carbon quantum dots as the carrier comprises the following steps:

[0026] Step one, weigh dopamine hydrochloride and citric acid monohydrate, dissolve them in water, stir at room temperature for 10 min, add 100 μL of ethylenediamine, then add the above-mentioned mixed solution to the reaction kettle, and react at 180 ℃ for 6 h to obtain a carbon quantum dot solution. After dialysis for 24 h, freeze-drying obtains carbon quantum dot powder; the mass ratio of dopamine hydrochloride and citric acid monohydrate is 84:1;

[0027] Step two: prepare a 2 mg / mL carbon quantum dot solution and a 50 mg / mL metal salt solution, mix them thoroughly, react at 37 ℃ for 2 h, dialyze for 24 h, and freeze-dry to obtain the required monatomic catalyst; the mass ratio of carbon quantum dots and metal salt is 10:1.

[0028] Further, the plant polyphenol-metal complex is formed by coordination between the hydroxyl functional group (-OH) of the polyphenol compound and the metal ion. The metal ion is Cu 2+ , Fe 3+Mn 2+ one or more of tannins, flavonoids and lignins.

[0029] In an embodiment of the present application, the preparation method of the plant polyphenol-metal complex comprises the following steps:

[0030] Step 1: weigh the plant polyphenol, dissolve the metal salt in deionized water, and stir for 1 h; wherein the mass ratio of plant polyphenol, metal salt and water is 1:0.6:100;

[0031] Step 2: centrifuge the obtained plant polyphenol-metal complex, and dry to obtain the plant polyphenol-metal complex; wherein the centrifugation speed is 8000-10000 r / min, the time is 8-10 min, the drying temperature is 40-50 ℃, and the time is 4-6 h.

[0032] Further, the specific process of step 3 is: weigh the monatomic catalyst, dissolve the plant polyphenol-metal complex in deionized water, and stir for 1 h, wherein the mass ratio of monatomic catalyst, plant polyphenol-metal complex and water is 1:1:100; centrifuge the obtained monatomic / plant polyphenol-metal complex solution, and dry to obtain the monatomic / plant polyphenol-metal complex catalyst, wherein the centrifugation speed is 8000-10000 r / min, the time is 8-10 min, the drying temperature is 40-50 ℃, and the time is 4-6 h.

[0033] The melt-blown layer containing the antibacterial coating in the present application adopts a monatomic / plant polyphenol-metal complex catalyst / remdesivir composite bactericide, which has the functions of high-efficiency and rapid sterilization and virus killing. Based on the oxidase-like enzyme characteristics of the monatomic catalyst, the bactericide can quickly catalyze the oxygen in the air into superoxide free radicals, thereby killing bacteria; at the same time, the release of the plant polyphenol-metal complex and remdesivir can also play a synergistic bactericidal purpose.

[0034] The novel antibacterial mask provided by the present application can quickly kill gram-negative bacteria (Escherichia coli), gram-positive bacteria (Staphylococcus aureus) and fungi (Candida albicans) without other auxiliary conditions (light, hydrogen peroxide). In addition, the novel antibacterial mask provided by the present application can effectively avoid the secondary pollution to the environment caused by discarded masks.

[0035] The present application has the following beneficial effects:

[0036] 1. The enzyme-like activity of the self-developed monatomic catalyst is utilized to realize high-efficiency antibacterial function without any additional conditions (light, hydrogen peroxide);

[0037] 2. The single-atom catalyst is combined with the plant polyphenol-metal complex by using the electrostatic adsorption effect, and then it is used as the carrier of the antiviral drug remdesivir, so as to realize the multifunctional synergistic antibacterial purpose of the material;

[0038] 3. The single-atom catalyst / plant polyphenol-metal complex / remdesivir composite antibacterial agent forms a uniform and stable antibacterial layer on the melt-blown cloth layer of the mask by using the film-forming property of the plant polyphenol, so as to achieve the purpose of high-efficiency, rapid and continuous sterilization. BRIEF DESCRIPTION OF DRAWINGS

[0039] Figure 1 The TEM image of the single-atom catalyst in Example 1.

[0040] Figure 2 The XRD spectrum of the single-atom catalyst in Example 1.

[0041] Figure 3 The XPS spectrum of the single-atom catalyst in Example 1.

[0042] Figure 4 The catalytic activity test results of the single-atom catalyst in Example 1.

[0043] Figure 5 The Zeta potential test results of the single-atom catalyst (Cu / Fe SACs), tannic acid-metal complex (TA+Cu 2+ ), single-atom catalyst / tannic acid-metal complex (TA+Cu 2+ +Cu / Fe SACs) in Example 1.

[0044] Figure 6 The FT-IR spectrum of the single-atom catalyst (Cu / Fe SACs), tannic acid-metal complex (TA+Cu 2+ ), remdesivir, single-atom catalyst / tannic acid-metal complex (TA+Cu 2+ +Cu / Fe SACs), single-atom catalyst / tannic acid-metal complex / remdesivir (TA+Cu 2+ +Cu / Fe SACs+remdesivir) in Example 1.

[0045] Figure 7 The antibacterial performance results of the single-atom catalyst / tannic acid-metal complex melt-blown layer and the single-atom catalyst / tannic acid-metal complex / remdesivir melt-blown layer on Escherichia coli E. coli ), Staphylococcus aureus S. aureus ) and Candida albicans C. albicans ) in Example 1. IMPLEMENTATION

[0046] The preferred embodiments of the present application will be described in detail below with reference to the embodiments. It should be understood that the following embodiments are given only for the purpose of illustration and are not intended to limit the scope of the present application. Those skilled in the art can make various modifications and substitutions to the present application without departing from the spirit and principles of the present application.

[0047] The experimental methods used in the following examples are conventional methods unless otherwise specified.

[0048] The materials, reagents, etc. used in the following examples can be obtained commercially unless otherwise specified. Example 1

[0049] Preparation of a new type of antibacterial mask with catalytic sterilization function

[0050] Step 1, weigh 1.314 g of 2-methylimidazole, 1.19 g of Zn(NO3)2•6H2O, 0.1 g of iron acetylacetone, and 0.15 g of copper acetylacetone, and dissolve them in 40 mL of methanol solution. Stir at room temperature for 1 h, then transfer the solution to a reaction kettle, and react at 120°C for 4 h. Centrifuge the obtained product Cu / Fe-ZIF-8 solution at a speed of 5000-6000 r / min for 8 min, and dry at 50°C for 1 h to obtain Cu / Fe-ZIF-8 powder. In a N2 atmosphere, calcine in a tube furnace at 800°C for 3 h to obtain Cu / Fe single-atom catalyst (Cu / Fe SACs).

[0051] Step 2, weigh 2.041 g of tannic acid and 1.227 g of CuCl2, and dissolve them in 200 mL of deionized water. Stir for 1 h, then centrifuge at 8000 r / min for 8 min, and dry at 50°C for 4 h to obtain tannic acid-metal complex (TA+Cu 2 + ).

[0052] Step 3, weigh 1 g of Cu / Fe single-atom catalyst and 1 g of tannic acid-metal complex, and dissolve them in 100 mL of deionized water. Stir for 1 h to obtain single-atom / tannic acid-metal complex catalyst (TA+ Cu 2+ + Cu / Fe SACs).

[0053] Step 4, 200 mg of remdesivir powder was weighed, dissolved in 5 mL of ethanol solution, stirred at room temperature for 10 min, 1 g of monatomic / tannic acid-metal complex catalyst in step 3 was weighed, added to 100 mL of deionized water, stirred at room temperature for 10 min, then 1.5 mL of remdesivir solution was added, stirred at room temperature for 10 min, to obtain a monatomic / tannic acid-metal complex catalyst / remdesivir solution. Centrifugal separation at 8000 r / min for 8 min, and drying at 40 ℃ for 4 h, to obtain a monatomic / tannic acid-metal complex catalyst / remdesivir powder (TA+Cu 2+ +Cu / Fe SACs+remdesivir).

[0054] Step 5, 0.1 g of monatomic / tannic acid-metal complex catalyst / remdesivir was weighed and dissolved in 100 mL of deionized water, stirred uniformly, to obtain a monatomic / tannic acid-metal complex catalyst / remdesivir solution with a concentration of 1000 μg / mL, labeled as solution A; 14.3 g of Na2HPO4·12H2O and 3.84 g of citric acid were weighed and added to 100 mL of deionized water, to obtain a concentration of 400 mmol / L of Na2HPO4·12H2O and a concentration of 200 mmol / L of citric acid, labeled as solution B; 40 pieces of melt-blown cloth with a size of 2 cm*3 cm were cut and placed in the A solution, and the B solution was quickly added, and left to stand for 0.5 h, and then air-dried at 25 ℃ to obtain a melt-blown layer of monatomic / tannic acid-metal complex catalyst / remdesivir antibacterial coating.

[0055] Step 6, after assembling the outer non-woven fabric, the melt-blown layer and the inner non-woven fabric, a new antibacterial mask with catalytic function was obtained.

[0056] Meanwhile, a melt-blown layer of monatomic / tannic acid-metal complex antibacterial coating was prepared by the method of step 5 using a monatomic / tannic acid-metal complex catalyst.

[0057] The TEM morphology of the Cu / Fe monatomic atom with enzyme-like catalytic activity in this example is shown in Figure 1 The TEM morphology of the Cu / Fe monatomic atom with enzyme-like catalytic activity in this example is shown in

[0058] The XRD pattern of the Cu / Fe monatomic atom with enzyme-like catalytic activity prepared in this example is shown in Figure 2As shown in the figure, the prepared Cu / Fe single atom only presents carbon structure characteristic diffraction peaks, specifically carbon material (002) and (101) diffraction peaks, and no obvious Cu / Fe metal diffraction peak is observed, indicating that the Cu / Fe single atom is successfully prepared.

[0059] The XPS spectrum of the Cu / Fe single atom prepared in this example is shown in Figure 3 The C 1s and N 1s spectra present a typical N-doped C structure, and in addition, the Cu 2p and Fe 2p spectra show that the Cu and Fe single atoms have valence states, indicating that they are successfully coordinated with the C-based material, i.e., the single atom catalyst can be successfully prepared by the space confinement / pyrolysis method.

[0060] The enzyme-like activity of the Cu / Fe single atom prepared in this example is shown in Figure 4 The specific experimental process is as follows: Cu / Fe single atom catalyst solutions with concentrations of 0 μg / mL, 100 μg / mL, 200 μg / mL and 300 μg / mL are prepared; tetramethyl benzidine (TMB) solution (solvent: dimethyl sulfoxide) is added to the four single atom catalyst solutions with different concentrations, wherein the working concentration of the TMB solution is 1 mM; then the absorbance of the four solutions at 652 nm is measured by an enzyme marker every 30 s for 10 min. The results show that the enzyme-like activity of the Cu / Fe single atom catalyst is concentration-dependent, and in the presence of O2, the Cu / Fe single atom catalyst rapidly exhibits oxidase-like activity, catalyzing O2 molecules into superoxide radicals (O2• - ), which further oxidize tetramethyl benzidine to generate a blue product and continuously enhance the optical density (O.D.) at 652 nm.

[0061] The changes in the Zeta potential values of the single atom catalyst, tannic acid-metal complex and single atom / tannic acid-metal complex catalyst prepared in this example are shown in Figure 5 The specific experimental process is as follows: single atom catalyst (Cu / Fe SACs), tannic acid-metal complex (TA+Cu 2+ ) and single atom / tannic acid-metal complex catalyst (TA+ Cu 2+ + Cu / Fe SACs) with a concentration of 100 μg / mL are prepared and placed in a Zeta potential capillary sample cell, respectively, and the surface charge is measured by a Malvern Zetasizer Nano-ZS-90 laser particle size instrument. The results show that the tannic acid-metal complex (TA+Cu 2+The potential of the single-atom catalyst is -4.167 mV, and the potential of the single-atom catalyst is 17.933 mV. After equal volume mixing, the zeta potential of the single-atom / tannic acid-metal complex catalyst is 6.89 mV, indicating that the single-atom catalyst and the tannic acid-metal complex are combined through electrostatic interaction.

[0062] The FT-IR spectrum of the single-atom / tannic acid-metal complex catalyst / remdesivir prepared in this embodiment is as follows: Figure 6 As shown, the single-atom / tannic acid-metal complex catalyst / remdesivir material at 1600 cm⁻¹ -1 The characteristic absorption peak of the antibacterial drug remdesivir was observed at the location, indicating that the single-atom / tannic acid-metal complex catalyst can serve as a carrier for antibacterial drugs.

[0063] The single-atom / tannic acid-metal complex catalyst meltblown layer and the single-atom / tannic acid-metal complex catalyst / remdesivir meltblown layer prepared in this embodiment are effective against Escherichia coli (E. coli). Escheruchia coli , E. coli (), Staphylococcus aureus , S. aureus ) and Candida albicans ( Candida albicans , C. albicans The killing ability of ) is as follows Figure 7 As shown, the specific experimental procedure is as follows: The prepared single-atom / tannic acid-metal complex catalyst meltblown layer and the single-atom / tannic acid-metal complex catalyst / remdesivir meltblown layer were dried and set aside for later use. 100 μL of Staphylococcus aureus, Escherichia coli, and Candida albicans bacterial solutions (concentration 1×10⁻⁶) were prepared. 4 ~9×10 4 A CFU / mL solution was dropped onto the surface of cloth strips containing the corresponding sample. After incubation for 0.5 min, 1 min, 2 min, 5 min, 10 min, and 20 min, the contaminated cloth strips were immersed in LB liquid medium and shaken thoroughly. The antibacterial properties of the material were then verified using the dilution plating method. Results showed that the single-atom / tannic acid-metal complex catalyst meltblown layer exhibited antibacterial activity against bacteria for 0.5 min. E. coli and S. aureus The bactericidal performance reached 8.06% and 9.77%. Within 20 min, the single-atom / tannic acid-metal complex catalyst meltblown layer showed bactericidal performance of 51%, 67%, and 38% against the three bacteria, indicating that the Cu / Fe single-atom catalyst's oxidase-like activity and the ion release behavior of the tannic acid-metal complex have significant rapid bactericidal effects. Furthermore, after loading the antibacterial drug remdesivir, the single-atom / tannic acid-metal complex catalyst / remdesivir meltblown layer showed bactericidal performance of 8.06% and 9.77% against the three bacteria, respectively. E. coli and S. aureusThe killing performance of the single atom / tannic acid-metal complex catalyst / Remdesivir melt-blown layer on the three bacteria reached 55%, 70%, and 47% within 2 min, indicating that after loading the drug, the longer the time within 2 min, the stronger the ability to kill bacteria, indicating that the melt-blown layer has a rapid sterilization function. Example 2

[0064] Preparation and application of a novel antibacterial mask with catalytic sterilization function

[0065] Step 1, weigh 2 g of poloxamer F127, 1 g of dopamine hydrochloride, and dissolve in 200 mL of ethanol / water solution (volume ratio 1:1), stir at room temperature for 15 min, then add 4 mL of 1,3,5-trimethylbenzene dropwise, stir for 30 min, then add 0.005 g of MnCl2 and 0.005 g of FeCl2 to the above solution, stir for 30 min, then centrifuge the resulting Fe / Mn-mesoporous carbon sphere solution at a speed of 5000-6000 r / min for 8 min, and dry at 50°C for 1 h to obtain Fe / Mn-mesoporous carbon sphere powder. In a N2 atmosphere, calcine in a tube furnace at 350°C and 800°C for 3 h and 5 h respectively to obtain Fe / Mn single atom catalyst.

[0066] Step 2, weigh 2.041 g of tea polyphenol, 1.227 g of FeCl2, and dissolve in 200 mL of deionized water, stir for 1 h, then centrifuge at 8000 r / min for 8 min, and dry at 50°C for 4 h to obtain tea polyphenol-metal complex.

[0067] Step 3, weigh 1 g of Fe / Mn single atom catalyst, 1 g of tea polyphenol-metal complex, and dissolve in 100 mL of deionized water, stir for 1 h to obtain single atom / tea polyphenol-metal complex catalyst.

[0068] Step 4, weigh 200 mg of Remdesivir powder, dissolve in 5 mL of ethanol solution, stir at room temperature for 10 min. Weigh 0.5 g of single atom / tea polyphenol-metal complex catalyst from step 3, add to 100 mL of deionized water, stir at room temperature for 10 min, then add 1 mL of Remdesivir solution, stir at room temperature for 10 min to obtain single atom / tea polyphenol-metal complex catalyst / Remdesivir solution. Centrifuge at 8000 r / min for 8 min and dry at 40°C for 4 h to obtain single atom / tea polyphenol-metal complex catalyst / Remdesivir powder.

[0069] Step 5, 0.1 g of monatomic / tea polyphenol-metal complex catalyst / Remdesivir was weighed and dissolved in 100 mL of deionized water, stirred uniformly to obtain a monatomic / tea polyphenol-metal complex catalyst / Remdesivir solution with a concentration of 1000 μg / mL, labeled as solution A; 10.73 g of Na2HPO4·12H2O and 2.88 g of citric acid were added to 100 mL of deionized water to obtain a concentration of 300 mmol / L of Na2HPO4·12H2O and a concentration of 150 mmol / L of citric acid, labeled as solution B; 40 pieces of melt-blown cloth with a size of 2 cm*3 cm were cut and placed in the A solution, and the B solution was quickly added, and then left to stand for 0.5 h, and then dried at 25 ℃ to obtain a melt-blown layer of monatomic / tea polyphenol-metal complex catalyst / Remdesivir antibacterial coating.

[0070] Step 6, after assembling the outer non-woven fabric, the melt-blown layer and the inner non-woven fabric, a new antibacterial mask with catalytic function was obtained. Example 3

[0071] Preparation and application of a new antibacterial mask with catalytic sterilization function

[0072] Step 1, 0.05 g of dopamine hydrochloride and 4.2 g of citric acid monohydrate were dissolved in 60 mL of aqueous solution, then 100 μL of ethylenediamine was added to the above solution, and then the mixed solution was transferred to a high-pressure reaction kettle and heated at 180 ℃ for 6 h. The obtained carbon quantum dot solution was dialyzed for 24 h and freeze-dried for 72 h to obtain carbon quantum dot powder. A 2 mg / mL carbon quantum dot and 50 mg / mL CuCl2 solution was prepared. Then, 10 mL of carbon quantum dot solution and 60 μL of CuCl2 solution were mixed and stirred at 37 ℃ for 2 h. The obtained product was dialyzed for 24 h to remove uncoordinated CuCl2. Finally, the dialysate was freeze-dried to obtain a Cu monatomic catalyst.

[0073] Step 2, 2.041 g of lignin and 1.227 g of MnCl2 were dissolved in 200 mL of deionized water, stirred for 1 h, then centrifuged at 8000 r / min for 8 min, and dried at 50 ℃ for 4 h to obtain a lignin-metal complex.

[0074] Step 3, 1 g of Cu monatomic catalyst and 1 g of lignin-metal complex were dissolved in 100 mL of deionized water, stirred for 1 h to obtain a monatomic / lignin-metal complex catalyst.

[0075] Step 4, 200 mg of remdesivir powder was weighed and dissolved in 5 mL of ethanol solution, stirred at room temperature for 10 min, and then gradually diluted to the desired concentration. 1.5 g of monatomic / lignin-metal complex catalyst in step 3 was weighed and added to 100 mL of deionized water, stirred at room temperature for 10 min, then 1.3 mL of remdesivir solution was added, stirred at room temperature for 10 min, to obtain a monatomic / lignin-metal complex catalyst / remdesivir solution. Centrifugal separation was performed at 8000 r / min for 8 min, and drying was performed at 40 °C for 4 h to obtain a monatomic / lignin-metal complex catalyst / remdesivir powder.

[0076] Step 5, 0.1 g of monatomic / lignin-metal complex catalyst / remdesivir was weighed and dissolved in 100 mL of deionized water, stirred uniformly to obtain a monatomic / lignin-metal complex catalyst / remdesivir solution with a concentration of 1000 μg / mL, labeled as solution A; 7.15 g of Na2HPO4•12H2O and 1.92 g of citric acid were weighed and added to 100 mL of deionized water to obtain a concentration of 200 mmol / L of Na2HPO4•12H2O and 100 mmol / L of citric acid, labeled as solution B; 40 pieces of melt-blown cloth with a size of 2 cm*3 cm were cut and placed in the A solution, and the B solution was quickly added, and then left to stand for 0.5 h, and then air-dried at 25 °C to obtain a melt-blown layer of monatomic / lignin-metal complex catalyst / remdesivir antibacterial coating.

[0077] Step 6, after assembling the outer non-woven fabric, melt-blown layer and inner non-woven fabric, a novel antibacterial mask with catalytic function was obtained.

Claims

1. An antibacterial mask with catalytic sterilization function, comprising an outer nonwoven fabric layer, a meltblown layer, and an inner nonwoven fabric layer, characterized in that, The antibacterial mask is prepared using the following steps: Step 1: Prepare a single-atom catalyst; Step 2: Prepare plant polyphenol-metal complexes; Step 3: Add the single-atom catalyst and the plant polyphenol-metal complex to water. The mass ratio of the single-atom catalyst, the plant polyphenol-metal complex and water is 1:1:

100. After stirring, the single-atom / plant polyphenol-metal complex catalyst is obtained. Step 4: Add 1~1.5 mL of remdesivir solution to 100 mL of single-atom / plant polyphenol-metal complex catalyst solution, stir, and then prepare single-atom / plant polyphenol-metal complex catalyst / remdesivir. The remdesivir solution is obtained by dissolving 200 mg of remdesivir in 5 mL of ethanol solution, and the single-atom / plant polyphenol-metal complex catalyst solution is obtained by dissolving 0.5~1.5 g of single-atom / plant polyphenol-metal complex catalyst in 100 mL of water. Step 5: Dissolve the single-atom / plant polyphenol-metal complex catalyst / remdesivir in water to obtain solution A, disodium hydrogen phosphate dodecahydrate and citric acid in water to obtain solution B, place the meltblown layer in solution A, then add solution B, let stand for 0.5~1 h and then air dry to obtain the meltblown layer. The concentration of the single-atom / plant polyphenol-metal complex catalyst / remdesivir in solution A is 500 μg / mL to 1000 μg / mL; the concentration of disodium hydrogen phosphate in solution B is 200 mmol / L to 400 mmol / L, and the concentration of citric acid is 100 mmol / L to 200 mmol / L. For every 40 pieces of meltblown fabric with a specification of 2 cm*3 cm, use 100 mL of solution A and 100 mL of solution B; Step 6: Assemble the outer nonwoven fabric, meltblown layer and inner nonwoven fabric to obtain the antibacterial mask.

2. The mask according to claim 1, characterized in that, The single-atom catalyst is composed of a transition metal and a carbon-based support. The transition metal is selected from one or more of Cu, Fe, and Mn, and the support is selected from one of zeolite imidazole ester framework materials, nitrogen-doped mesoporous carbon spheres, or carbon quantum dots.

3. The mask according to claim 1, characterized in that, The plant polyphenol-metal complex is formed through coordination between the hydroxyl functional groups of polyphenolic compounds and metal ions; wherein the metal ion is Cu. 2+ Fe 3+ Mn 2 + One or more of the plant polyphenols, wherein the plant polyphenols are one of tannins, flavonoids or lignins.

4. The mask according to claim 1, characterized in that, The stirring time in step 3 is 1 hour.

5. The mask according to claim 1, characterized in that, The stirring time in step 4 is 10 minutes.

Images