CN113845691B - Two-dimensional or three-dimensional cellulose-based porous antibacterial material and preparation method thereof - Google Patents
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Abstract
The invention discloses a two-dimensional or three-dimensional cellulose-based porous antibacterial material, which is prepared by taking cellulose as a main material, acid as a catalyst, alkyl dialdehyde as a cross-linking agent, grafting antibiotics through a chemical method, dissolving a sample in a low-temperature alkali/urea solution or ionic liquid, and adopting a sol-gel method. The cellulose-based antibacterial material is insoluble in water and conventional organic solvents, and effectively reduces the problem of water pollution caused by easy dissolution of antibiotics. The cellulose-based antibacterial material has obvious inhibition effect on gram-positive bacteria and gram-negative bacteria, is a stable, efficient, broad-spectrum and edible antibacterial agent, and has extremely low cytotoxicity. The two-dimensional cellulose-based antibacterial porous material and the three-dimensional cellulose-based antibacterial microsphere have good gastric acid resistance, can be used as an oral antibacterial material, and can directly inhibit intestinal bacteria after gastric acid passing.
Description
Technical Field
The invention belongs to the field of functional materials, relates to a two-dimensional or three-dimensional cellulose-based porous antibacterial material and a preparation method thereof, and in particular relates to a grafted modified cellulose-based antibacterial material and a preparation method thereof.
Background
It is well known that conventional medical procedures (e.g., surgery, intensive care medicine, and infection treatment) are not separated from antibiotics. However, the abuse of antibiotics results in the development of resistance to a large number of pathogenic bacteria, which severely jeopardizes human life health. Researchers predict that by 2050, antibiotic resistance will lead to death in more than 1000 tens of thousands of people, exceeding the mortality rate of cancer. Therefore, the development of a novel, efficient and safe antibacterial material different from the traditional antibiotics has great market value.
Chitosan-based antibacterial agents (CAMs), particularly chitosan micro-and nanoparticles, are considered as one of the antibiotic substitutes with application prospects. CAMs exhibit potent broad-spectrum antimicrobial activity against a variety of pathogens, do not cause toxicity in vitro and in cell lines, and produce little resistance to antibiotics for long periods of time. However, CAMs have relatively low antimicrobial activity against a variety of pathogens compared to antibiotics.
Cellulose is an inexhaustible natural polymer, has a large number of modifiable hydroxyl sites, is nontoxic and has good biocompatibility, and is stable in most solvents. Thus, cellulose is considered as an excellent host material for novel antibacterial materials. In recent years, various novel cellulose-based antibacterial materials, such as quaternized cellulose antibacterial materials, metal oxide/cellulose antibacterial materials, chitosan/cellulose antibacterial materials, and the like, have been studied. These cellulose-based antibacterial materials exhibit a remarkable inhibitory effect against many pathogenic bacteria by modifying functional antibacterial molecules or mixing with antibacterial materials. However, most of the cellulose antibacterial agents are mainly used for environmental sterilization because of the presence of quaternized functional molecules and metal oxides. In the chitosan/cellulose antibacterial material, the antibacterial property mainly comes from chitosan. The problem of low antimicrobial activity of chitosan against pathogens also limits the use of chitosan/cellulose materials.
Therefore, if a cellulose-based antibacterial material which is environment-friendly, stable, high in broad-spectrum bacteriostasis and low in cost can be developed, the cellulose-based antibacterial material has great market value.
Disclosure of Invention
The invention aims to provide an environment-friendly, stable, broad-spectrum and low-cost cellulose-based antibacterial material. The cellulose-based antibacterial material takes cellulose as a main material, and antibacterial components such as kanamycin sulfate, kanamycin hydrochloride and the like are grafted on hydrophilic water-insoluble cellulose through an acetal reaction, so that a powdery fiber-based antibacterial material is prepared; then, in order to further improve the specific surface area of the cellulose-based antibacterial material, dissolving the powdery cellulose-based antibacterial material in an alkali/urea aqueous solution or an ionic liquid, and preparing the two-dimensional porous cellulose-based antibacterial material and the three-dimensional porous cellulose-based antibacterial microsphere by a sol-gel method.
The invention aims at realizing the following technical scheme:
a two-dimensional or three-dimensional cellulose-based porous antibacterial material is prepared from cellulose serving as a main material, acid serving as a catalyst, alkyl dialdehyde serving as a cross-linking agent through grafting antibiotics by a chemical method, dissolving a sample in a low-temperature alkali/urea solution or ionic liquid, and preparing the two-dimensional cellulose-based porous antibacterial material or the cellulose-based porous antibacterial microsphere by a sol-gel method.
The cellulose is one or more of alpha-cellulose, cotton cellulose and paper pulp. The purity of cellulose in the pulp is more than 85%.
The antibiotics are kanamycin hydrochloride and kanamycin sulfate.
The mass ratio of the cellulose to the antibiotics is 1:0.001-1:1.
The alkyl dialdehyde is one or more of glutaraldehyde, glyoxal, hexanedial and nonanedial.
The mass ratio of the cellulose to the alkyl dialdehyde is 1:0.01-1:1.
The acid is hydrochloric acid, sulfuric acid, acetic acid solution and phosphoric acid solution with the concentration of 0.1-1M; the mass-volume ratio of the cellulose to the acid is 1:1-500 g/mu L.
The temperature of the low-temperature alkali/urea solution is less than or equal to-20 ℃, and the mass ratio of alkali to urea to water is 3-12:5-18:85-70; the ionic liquid is [ BmimCl ] ionic liquid.
Another object of the present invention is to provide a method for preparing the two-dimensional or three-dimensional cellulose-based porous antibacterial material, comprising the steps of:
step (1), dispersing cellulose and antibiotics in water, adding an acidic solution, and uniformly stirring;
adding alkyl dialdehyde into the solution obtained in the step (1) under the light-shielding condition, and stirring for 1-24 h at the temperature of 10-50 ℃;
filtering the sample after the reaction in the step (3) and the step (2), collecting particles, washing with water, and drying in vacuum;
and (4) dissolving the sample obtained in the step (3) in a low-temperature alkali/urea solution or an ionic liquid, and preparing the two-dimensional cellulose-based porous antibacterial material or the cellulose-based porous antibacterial microsphere by adopting a sol-gel method.
In the step (1), the acid solution is hydrochloric acid, sulfuric acid, acetic acid solution and phosphoric acid solution with the concentration of 0.1-1M; the mass-volume ratio of the cellulose to the acidic solution is 1:1-500 g/mu L.
In the step (4), the dosage ratio of the sample obtained in the step (3) to the low-temperature alkali/urea solution or the ionic liquid is 1:10-1:40 g/mL.
When the cellulose-based porous antibacterial material is a two-dimensional cellulose-based porous antibacterial material, dissolving the sample obtained in the step (3) in a low-temperature alkali/urea solution or ionic liquid, soaking the obtained solution (sol) in an acidic solution or an organic solvent, performing phase transition, converting a liquid phase into a solid phase, collecting the solid phase, washing the solid phase with water to be neutral, and performing vacuum drying or freeze-drying to constant weight at 20-60 ℃ to obtain the two-dimensional cellulose-based porous antibacterial material; wherein the acidic solution is acetic acid, hydrochloric acid or phosphoric acid, and the organic solvent is ethanol, methanol, glycol or acetone; or dissolving the sample obtained in the step (3) in low-temperature alkali/urea solution or ionic liquid, sealing, and performing heat treatment at 50 ℃ for at least 24 hours to obtain cellulose-based two-dimensional gel, washing the cellulose-based two-dimensional gel to be neutral by using an acidic aqueous solution or pure water, and performing vacuum drying or freeze-drying to be constant weight at 20-60 ℃ to obtain the two-dimensional cellulose-based porous antibacterial material.
When the cellulose-based porous antibacterial material is a cellulose-based porous antibacterial microsphere, dissolving the sample obtained in the step (3) in a low-temperature alkali/urea solution or an ionic liquid, dripping the obtained solution into a solvent, collecting a solid phase, washing with water to be neutral, and carrying out vacuum drying or freeze-drying at 20-60 ℃ to constant weight to obtain the cellulose-based porous antibacterial microsphere; wherein the solvent is acetic acid, hydrochloric acid, phosphoric acid or other acidic solution or ethanol, methanol, glycol, acetone or other polar organic solvent.
The invention also aims to provide the application of the two-dimensional or three-dimensional cellulose-based porous antibacterial material in preparing an oral antibacterial preparation.
The invention has the beneficial effects that:
compared with the prior art that cellulose is modified by aldehyde and then grafted with antibacterial materials, the cellulose is not required to be modified before grafting, but cellulose and kanamycin are directly grafted by glutaraldehyde, and linked sites are hydroxyl groups of cellulose and hydroxyl groups of kana, so that the reaction is simpler and faster.
The cellulose-based antibacterial material is insoluble in water and conventional organic solvents, and effectively reduces the problem of water pollution caused by easy dissolution of antibiotics.
The cellulose-based antibacterial material has obvious inhibition effect on gram-positive bacteria and gram-negative bacteria, is a stable, efficient, broad-spectrum and edible antibacterial agent, and has extremely low cytotoxicity. The two-dimensional cellulose-based antibacterial porous material and the three-dimensional cellulose-based antibacterial microsphere have good gastric acid resistance, can be used as an oral antibacterial material, and can directly inhibit intestinal bacteria after gastric acid passing.
The three-dimensional cellulose-based antibacterial microsphere or the two-dimensional cellulose-based antibacterial porous material has a porous structure, has a large specific surface area and BSA adsorption capacity, and can fix medicines, proteins and the like.
Drawings
FIG. 1 is a graph showing the inhibition of E.coli by the cellulose-based antibacterial material of example 1 directly observed in a plate count method. A) Original bacterial liquid; b) Inhibition of E.coli by alpha-cellulose; c) Inhibition of E.coli by cellulose-based antibacterial materials.
FIG. 2 is a graph showing the inhibition of Staphylococcus aureus by the cellulose-based antibacterial material of example 2 directly observed in a plate count method. A) Original bacterial liquid; b) Inhibition of staphylococcus aureus by cotton cellulose; c) Inhibition of staphylococcus aureus by cellulose-based antibacterial materials.
FIG. 3 is a graph showing the inhibition of Salmonella by the cellulose-based antibacterial material of example 3 directly observed in a plate count method. A) Original bacterial liquid; b) Inhibition of salmonella by pulp; c) Inhibition of salmonella by cellulose-based antimicrobial materials.
FIG. 4 is a microstructure of the two-dimensional cellulose-based porous antimicrobial material of example 4.
Fig. 5 is a bacterial growth curve of the two-dimensional cellulose-based multi-Kong Yijun material of example 4 in intestinal fluid.
FIG. 6 is a microstructure of the cellulose-based porous antimicrobial microspheres of example 5.
FIG. 7 is a graph showing the bacterial growth in intestinal fluid of the cellulose-based porous antimicrobial microspheres of example 5.
Fig. 8 is a safety inspection result of the cellulose-based porous antimicrobial microsphere of example 5.
Detailed Description
The technical scheme of the invention is further described by the following specific examples.
Example 1
5g of alpha-cellulose and 0.058g of kanamycin sulfate were dispersed in 10mL of water, 5. Mu.L of 0.1M hydrochloric acid was added dropwise, and stirring was carried out for 30 minutes; dropwise adding 0.05g glutaraldehyde under the dark condition, and stirring for 2 hours at normal temperature; filtering, collecting particles, removing the incompletely reacted kanamycin sulfate by a large amount of pure water, and vacuum drying at 60 ℃ for 5 hours to obtain the kanamycin sulfate grafted cellulose-based antibacterial material.
The inhibition of E.coli (gram-negative bacteria) by the cellulose-based antibacterial material of this example was examined: inoculating Escherichia coli into liquid culture medium (LB medium), culturing at 37deg.C until bacterial liquid OD 600 =1.39, i.e. the original bacterial liquid. 1mL of the original bacterial liquid is taken, 50mg of the cellulose-based antibacterial material or alpha-cellulose of the embodiment is added, the mixture is vibrated for 3 hours at 37 ℃, a plate is coated, and the number of the escherichia coli growing on a nutrient agar plate is detected, and the result is shown in figure 1. The method shows that after the cellulose-based antibacterial material is added into the original bacterial liquid, the number of the escherichia coli growing on the nutrient agar plate is obviously reduced. The following is indicated: the kanamycin sulfate grafted cellulose-based antibacterial material has excellent escherichia coli inhibition capability.
Example 2
5g of cotton cellulose and 5.8g of kanamycin hydrochloride are dispersed in 50mL of water, 2.5mL of 0.1M acetic acid aqueous solution is added dropwise, and stirring is carried out for 30 minutes; dropwise adding 5g of glyoxal under the condition of avoiding light, and stirring for 6 hours at normal temperature; the particles were collected by filtration, and the unreacted kanamycin hydrochloride was removed by a large amount of pure water, and dried in vacuo at 40℃for 10 hours to give a kanamycin hydrochloride grafted cellulose-based antibacterial material, the adsorption amount of BSA was 162.5mg/g.
The inhibition of staphylococcus aureus (gram positive bacteria) by the cellulose-based antibacterial material of this example was examined: inoculating Staphylococcus aureus into liquid culture medium (LB culture medium), culturing at 37deg.C until bacterial liquid OD 600 =1.18, i.e. the original bacterial liquid. 1mL of the original bacterial liquid is taken, 50mg of the cellulose-based antibacterial material or cotton cellulose of the embodiment is added, the mixture is vibrated for 3 hours at 37 ℃, a plate is coated, and the number of staphylococcus aureus growing on a nutrient agar plate is detected, and the result is shown in figure 2. The display shows that the fiber is added into the original bacterial liquidAfter the element-based antibacterial material, the number of staphylococcus aureus growing on the nutrient agar plate is obviously reduced. The following is indicated: the kanamycin hydrochloride grafted cellulose-based antibacterial material has excellent staphylococcus aureus inhibition capability.
Example 3
5g of pulp (free of water, cellulose content > 85%) and 2g of kanamycin sulfate were dispersed in 20mL of water, 500. Mu.L of 0.5M phosphoric acid aqueous solution was added dropwise, and stirred for 1 hour; 3g of glyoxal is added dropwise under the condition of light shielding, and stirring is carried out for 12 hours at normal temperature; filtering, collecting particles, removing the incompletely reacted kanamycin sulfate by a large amount of pure water, and vacuum drying at normal temperature for 24 hours to obtain the kanamycin sulfate grafted cellulose-based antibacterial material.
The inhibition of salmonella (gram-negative bacteria) by the cellulose-based antimicrobial material of this example was examined: inoculating Salmonella into liquid culture medium (LB medium), culturing at 37deg.C to reach solution OD 600 =2.19. 1mL of the original bacterial liquid is taken, 50mg of the cellulose-based antibacterial material or paper pulp of the embodiment is added, the mixture is vibrated for 3 hours at 37 ℃, a plate is coated, and the number of salmonella grown on a nutrient agar plate is detected, and the result is shown in figure 3. The method shows that after the cellulose-based antibacterial material is added into the original bacterial liquid, the number of salmonella grown on the nutrient agar plate is obviously reduced. The following is indicated: the kanamycin sulfate grafted cellulose-based antibacterial material has excellent salmonella inhibition capability.
Example 4
Taking 5g of the cellulose-based antibacterial material prepared in the example 1, dissolving in 100mL of an alkali/urea water system (prepared by sodium hydroxide, urea and water according to a mass ratio of 7:12:81) at a temperature of-20 ℃ to obtain a cellulose-based antibacterial material solution; then the solution is soaked in 1M acetic acid aqueous solution to obtain the two-dimensional cellulose-based porous antibacterial material (figure 4), the outer surface and the inner surface of the two-dimensional cellulose-based porous antibacterial material both contain a large number of pore structures, and the adsorption quantity of BSA reaches 217.3mg/g.
50mg of the two-dimensional cellulose-based porous antibacterial material of the embodiment is taken and soaked in 1mL of simulated gastric acid (artificial gastric juice (source leaf organism), and the manufacturer is Shanghai source leaf biotechnology Co., ltd., product number is R30388) to vibrate3 hours, take out and transfer to 1mL simulated intestinal fluid (artificial small intestinal fluid (Source leaf organism), manufacturer: shanghai Source leaf Biotechnology Co., ltd., product number: R22156); adding Escherichia coli original bacterial liquid 100 μl (OD of original bacterial liquid) 600 =1.39), shaking at 37 ℃ for 6 hours. OD detection of bacteria-containing intestinal juice per hour 600 Values (fig. 5). Experimental results show that the two-dimensional cellulose-based porous antibacterial material still has good escherichia coli inhibition capability after being soaked in gastric acid for 3 hours. OD in intestinal juice containing two-dimensional cellulose-based porous antibacterial material 600 The values were lower than those of the bacteria-containing intestinal juice (without cellulose material) containing the two-dimensional porous cellulose material of comparative example 1. It can be seen that the two-dimensional cellulose-based porous antibacterial material has good gastric acidity resistance. The two-dimensional cellulose-based porous antibacterial material can be used as an oral antibacterial material, and intestinal bacteria can be directly inhibited after gastric acid is passed.
Comparative example 1
5g of alpha-cellulose was taken and dissolved in 100mL of an alkali/urea aqueous system at-20 ℃ (same as in example 4), and then the above solution was immersed in a 1M aqueous acetic acid solution to obtain a two-dimensional porous cellulose material.
Example 5
Taking 5g of the cellulose-based antibacterial material prepared in example 2, and dissolving the cellulose-based antibacterial material in 100mL of [ BmimCl ] ionic liquid to obtain a cellulose-based antibacterial material solution; the above cellulose-based antibacterial material solution (volume 1 μl) was then added dropwise to ethanol (volume 1 mL), the solid phase was collected, washed with water to neutrality, and dried under vacuum at 20deg.C to constant weight to obtain three-dimensional cellulose-based porous antibacterial microspheres (FIG. 6). The cellulose-based porous antibacterial microsphere is in a standard sphere shape, the surface of the cellulose-based porous antibacterial microsphere contains a large number of hole structures, the size of the microsphere is 1-10 mu m, and the BSA adsorption capacity of the three-dimensional cellulose-based porous antibacterial microsphere reaches 429.2mg/g.
50mg of the three-dimensional cellulose-based porous antibacterial microspheres of the embodiment are taken, soaked in simulated gastric acid (same as embodiment 4) and oscillated for 5 hours, taken out and transferred into simulated intestinal juice (same as embodiment 4); 100. Mu.L of the original bacterial liquid of staphylococcus aureus (OD of the original bacterial liquid) is added 600 =1.18), shaking at 37 ℃ for 6 hours. OD detection of bacteria-containing intestinal juice per hour 600 Values (fig. 7). Experimental resultsThe three-dimensional cellulose-based porous antibacterial material still has good staphylococcus aureus inhibition ability after 3 hours of gastric acid soaking. OD in intestinal juice containing three-dimensional cellulose-based porous antibacterial microspheres 600 The values were far lower than the bacteria-containing intestinal fluid (without cellulose material) and the bacteria-containing intestinal fluid containing the three-dimensional cellulose microspheres of comparative example 2. The three-dimensional cellulose-based porous antibacterial microspheres have good gastric acid resistance, can be used as an oral antibacterial material, and can directly inhibit intestinal bacteria after gastric acid passing.
Culture medium for Vero cells: dulbecco's Modified Eagle Medium (DMEM) medium: 10% of fetal bovine serum, 1% of antibiotic solution and 10% of amino acid.
The Vero cells cultured in the cell bottle are inoculated in a 96-well plate after being digested, and are placed in a 37 ℃ incubator for culturing for 24 hours; 200. Mu.L of the three-dimensional cellulose-based porous antimicrobial microsphere aqueous dispersion of the present example (200. Mu.g/mL, 100. Mu.g/mL, 50. Mu.g/mL, 25. Mu.g/mL, 12.5. Mu.g/mL, 0. Mu.g/mL) at different concentrations was added to the above-mentioned culture plate, and incubated in an incubator at 37℃for 6 hours. To each well after the above treatment, 10. Mu.L of CCK-8 solution was added, and incubated at 37℃for 1 hour, and OD450 values were measured (FIG. 8). The result shows that when the content of the three-dimensional cellulose-based antibacterial microsphere reaches 50 mug/mL, the cell survival rate is 90%, and the three-dimensional cellulose-based antibacterial microsphere has extremely low cytotoxicity.
Comparative example 2
5g of cotton cellulose is taken and dissolved in 100mL of [ BmimCl ] ionic liquid, then the solution (volume 1 mu L) is dropwise added into ethanol (volume 1 mL), the solid phase is collected, washed to be neutral by water, and dried to constant weight at 20 ℃ in vacuum, thus obtaining the three-dimensional cellulose microsphere.
Claims (8)
1. A two-dimensional or three-dimensional cellulose-based porous antimicrobial material, characterized in that: the cellulose-based porous antibacterial material is prepared by taking cellulose as a main material, acid as a catalyst, alkyl dialdehyde as a cross-linking agent, grafting antibiotics through a chemical method, dissolving a sample in a low-temperature alkali/urea solution or ionic liquid, and preparing a two-dimensional cellulose-based porous antibacterial material or cellulose-based porous antibacterial microsphere by adopting a sol-gel method;
the antibiotics are kanamycin hydrochloride or kanamycin sulfate;
the mass ratio of the cellulose to the antibiotics is 1:0.001-1:1;
when the cellulose-based porous antibacterial material is a two-dimensional cellulose-based porous antibacterial material, dissolving a sample in a low-temperature alkali/urea solution or ionic liquid, soaking the obtained solution in an acidic solution or an organic solvent, performing phase transition, converting from a liquid phase to a solid phase, collecting the solid phase, washing with water to be neutral, and performing vacuum drying or freeze drying to constant weight at 20-60 ℃ to obtain the two-dimensional cellulose-based porous antibacterial material; wherein the acidic solution is acetic acid, hydrochloric acid or phosphoric acid, and the organic solvent is ethanol, methanol, glycol or acetone; or dissolving the sample in low-temperature alkali/urea solution or ionic liquid, sealing, and performing heat treatment at 50 ℃ for at least 24 hours to obtain cellulose-based two-dimensional gel, washing the cellulose-based two-dimensional gel to be neutral by using acidic aqueous solution or pure water, and performing vacuum drying or freeze-drying to be constant weight at 20-60 ℃ to obtain the two-dimensional cellulose-based porous antibacterial material;
when the cellulose-based porous antibacterial material is a cellulose-based porous antibacterial microsphere, dissolving a sample in a low-temperature alkali/urea solution or ionic liquid, dripping the obtained solution into a solvent, collecting a solid phase, washing with water to be neutral, and carrying out vacuum drying or freeze-drying to constant weight at 20-60 ℃ to obtain the cellulose-based porous antibacterial microsphere; wherein the solvent is acetic acid, hydrochloric acid, phosphoric acid, ethanol, methanol, glycol or acetone;
the temperature of the low-temperature alkali/urea solution is less than or equal to-20 ℃, and the mass ratio of alkali to urea to water is 3-12:5-18:85-70; the ionic liquid is [ BmimCl ] ionic liquid.
2. The two-or three-dimensional cellulose-based porous antimicrobial material according to claim 1, wherein: the cellulose is one or more of alpha-cellulose, cotton cellulose and paper pulp.
3. The two-or three-dimensional cellulose-based porous antimicrobial material according to claim 1, wherein: the alkyl dialdehyde is one or more of glutaraldehyde, glyoxal, hexanedial and nonanedial.
4. A two-or three-dimensional cellulose-based porous antimicrobial material according to claim 1 or 3, characterized in that: the mass ratio of the cellulose to the alkyl dialdehyde is 1:0.01-1:1.
5. The two-or three-dimensional cellulose-based porous antimicrobial material according to claim 1, wherein: the acid is hydrochloric acid, sulfuric acid, acetic acid solution or phosphoric acid solution with the concentration of 0.1-1M; the mass-volume ratio of the cellulose to the acid is 1:1-500 g/. Mu.L.
6. A method of preparing a two-or three-dimensional cellulose-based porous antimicrobial material according to claim 1, characterized in that: the method comprises the following steps:
step (1), dispersing cellulose and antibiotics in water, adding an acidic solution, and uniformly stirring;
adding alkyl dialdehyde into the solution obtained in the step (1) under the light-shielding condition, and stirring for 1-24 h at the temperature of 10-50 ℃;
filtering the sample obtained by the reaction in the step (3) and the step (2), collecting particles, washing with water, and drying in vacuum;
and (4) dissolving the sample obtained in the step (3) in a low-temperature alkali/urea solution or an ionic liquid, and preparing the two-dimensional cellulose-based porous antibacterial material or the cellulose-based porous antibacterial microsphere by adopting a sol-gel method.
7. The method of preparing a two-or three-dimensional cellulose-based porous antimicrobial material according to claim 6, wherein: in the step (4), the dosage ratio of the sample obtained in the step (3) to the low-temperature alkali/urea solution or the ionic liquid is 1:10-1:40 g/mL.
8. Use of the two-or three-dimensional cellulose-based porous antibacterial material of claim 1 for the preparation of an oral bacteriostatic formulation.
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