WO2022027185A1 - Revêtement semi-conducteur ayant des effets antimicrobiens et de mesure, son procédé de préparation et son utilisation - Google Patents

Revêtement semi-conducteur ayant des effets antimicrobiens et de mesure, son procédé de préparation et son utilisation Download PDF

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WO2022027185A1
WO2022027185A1 PCT/CN2020/106595 CN2020106595W WO2022027185A1 WO 2022027185 A1 WO2022027185 A1 WO 2022027185A1 CN 2020106595 W CN2020106595 W CN 2020106595W WO 2022027185 A1 WO2022027185 A1 WO 2022027185A1
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semiconductor
current
substrate
semiconductor coating
microbial
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PCT/CN2020/106595
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English (en)
Chinese (zh)
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王国敏
唐楷为
孟哲一
王怀雨
朱剑豪
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深圳先进技术研究院
香港城市大学
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Priority to PCT/CN2020/106595 priority Critical patent/WO2022027185A1/fr
Publication of WO2022027185A1 publication Critical patent/WO2022027185A1/fr

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    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K33/00—Medicinal preparations containing inorganic active ingredients
    • A61K33/24—Heavy metals; Compounds thereof
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K33/00—Medicinal preparations containing inorganic active ingredients
    • A61K33/24—Heavy metals; Compounds thereof
    • A61K33/30—Zinc; Compounds thereof
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82B—NANOSTRUCTURES FORMED BY MANIPULATION OF INDIVIDUAL ATOMS, MOLECULES, OR LIMITED COLLECTIONS OF ATOMS OR MOLECULES AS DISCRETE UNITS; MANUFACTURE OR TREATMENT THEREOF
    • B82B1/00—Nanostructures formed by manipulation of individual atoms or molecules, or limited collections of atoms or molecules as discrete units
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82B—NANOSTRUCTURES FORMED BY MANIPULATION OF INDIVIDUAL ATOMS, MOLECULES, OR LIMITED COLLECTIONS OF ATOMS OR MOLECULES AS DISCRETE UNITS; MANUFACTURE OR TREATMENT THEREOF
    • B82B3/00—Manufacture or treatment of nanostructures by manipulation of individual atoms or molecules, or limited collections of atoms or molecules as discrete units
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
    • G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis

Definitions

  • the invention belongs to the field of biological detection, and in particular relates to a semiconductor coating with both anti-microbial and detection effects, and its use in anti-microbial and detection of microbial content.
  • Implantation surgery is one of the common clinical treatment options to improve the quality of life of patients, but a key factor leading to the failure of implantation surgery is bacterial infection.
  • Appropriate modification of the implant surface can achieve an antibacterial surface and effectively reduce the infection rate.
  • the antibacterial interface can realize real-time monitoring of the number of bacteria, it will bring great convenience to doctors to monitor the infection of patients in time.
  • Electron transfer is a common physical phenomenon that occurs at interfaces with potential differences, and studies have shown that electron transfer between materials and bacteria plays a key role in this type of antibacterial process. A small number of studies have shown that the surface of materials modified with charges can also rely on electron transfer for effective antibacterial properties. All of the above methods are advancing the development of antibacterial materials step by step (Wang, G. et al. An antibacterial platform based on capacitive carbon-doped TiO2 nanotubes after direct or alternating current charging. Nat. Commun. 9, 2055 (2018). Wang , G. et al. Extracellular electron transfer from aerobic bacteria to Au-loaded TiO 2 semiconductor without light: a new bacteria-killing mechanism other than localized surface plasmon resonance or microbial fuel cells.
  • Effective antibacterial can be achieved through the surface design of implants, thereby improving the success rate of biomedical applications.
  • most of the current antibacterial materials are release surfaces, and the design has the following defects.
  • grafting antibiotics and antimicrobial peptides to the surface of the material will cause Severe bacterial resistance, and mutations in resistant strains can exacerbate clinical infections.
  • various peptide materials are prone to immune reaction with the body, which increases the risk of implantation failure.
  • release-type antimicrobial surfaces non-release antimicrobial surfaces that rely on physical action can reduce systemic side effects because of their local action, do not require the replenishment of antimicrobial substances, and achieve precise infection control at the implant site. .
  • the invention aims to design an antibacterial system that relies on electron transfer and can monitor the number of bacteria in real time.
  • a bacterial current is generated due to the interface potential difference.
  • the magnitude of the current can reflect the number of bacteria, and the bacterial current At the same time, it can interfere with the physiological activities of bacteria to achieve a precise non-release antibacterial process.
  • This clean and environmentally friendly antibacterial system overcomes the systemic side effects of existing release-type antibacterial surfaces and the shortcomings of requiring replenishment of antibacterial substances.
  • the real-time monitoring function is helpful for doctors to understand the infection status in real time and take corresponding measures in a timely manner.
  • the present invention includes two parts. First design a semiconductor coating on the surface of the implant, then contact the bacteria with the coating, and connect the entire system to an electrochemical workstation or a microcurrent meter.
  • the magnitude of the current can reflect the number of bacteria, and the bacterial current can be used in a short period of time. Interfering with the electron transfer of the bacterial respiratory chain and inhibiting its growth and reproduction.
  • One aspect of the present invention provides a semiconductor coating that is anti-microbial and can self-measure the number of microorganisms.
  • the semiconductor coating is in situ generated on a substrate. Titanium dioxide nanomaterial arrays, silicon arrays, etc.
  • the surface of the semiconductor nanoarray also includes the modification of metal nanoparticles, preferably, the metal nanoparticles are selected from gold nanoparticles, silver nanoparticles, platinum nanoparticles, palladium nanoparticles and the like.
  • the substrate is selected from metal substrates and non-metallic substrates;
  • the metal substrate is selected from titanium substrates, magnesium substrates, aluminum substrates, and the like; the non-metallic substrates are selected from silicon substrates and the like.
  • the nanomaterial size of the semiconductor nanoarray is 10-500 nm, preferably 80-150 nm.
  • the method for in-situ generation of semiconductor nanoarrays by the semiconductor coating on the substrate is: 1) forming epoxy groups on the surface of the substrate; Generate semiconductor nanoarrays on the substrate.
  • the method for forming epoxy groups on the surface of the substrate is to react the substrate with a silane coupling agent, preferably ⁇ -(2,3-glycidoxy)propyltrimethoxysilane, to obtain epoxy group.
  • a silane coupling agent preferably ⁇ -(2,3-glycidoxy)propyltrimethoxysilane
  • the method of generating zinc oxide semiconductor nanoarrays on epoxy groups by hydrothermal method is to react zinc salt solution and sodium hydroxide alcohol solution at 100-150 ° C to prepare a seed layer; then add ring ZnO semiconductor nanoarrays were generated by hydrothermal treatment in a mixed aqueous solution of hexamethylenetetramine and zinc acetate hexahydrate.
  • the method for modifying the metal nanoparticles on the surface of the semiconductor nano-array is to deposit the metal nanoparticles by a magnetron sputtering method.
  • the microorganisms are bacteria, fungi, viruses, preferably, the bacteria are Escherichia coli and Staphylococcus aureus.
  • the semiconductor nanoarray is a zinc oxide nanorod array, and the surface thereof is decorated with gold nanoparticles.
  • Another aspect of the present invention provides another method for preparing a semiconductor coating, comprising the steps of:
  • the method for forming epoxy groups on the surface of the substrate is to react the substrate with a silane coupling agent, preferably ⁇ -(2,3-glycidoxy)propyltrimethoxysilane, to obtain epoxy group.
  • a silane coupling agent preferably ⁇ -(2,3-glycidoxy)propyltrimethoxysilane
  • the method of generating zinc oxide semiconductor nanoarrays on epoxy groups by hydrothermal method is to react zinc salt solution and sodium hydroxide alcohol solution at 100-150 ° C to prepare a seed layer; then add ring ZnO semiconductor nanoarrays were generated by hydrothermal treatment in a mixed aqueous solution of hexamethylenetetramine and zinc acetate hexahydrate.
  • the method for modifying the metal nanoparticles on the surface of the semiconductor nano-array is to deposit the metal nanoparticles by a magnetron sputtering method.
  • Yet another aspect of the present invention provides the use of the semiconductor coating, which provides the antimicrobial activity of the substrate while being capable of detecting the microbial content on the surface of the substrate.
  • the use of the semiconducting coating to provide the substrate antimicrobial activity is in an air environment, rather than a liquid environment.
  • Yet another aspect of the present invention provides an implant having the above-mentioned semiconductor coating.
  • Another aspect of the present invention provides a method for detecting microorganisms on the surface of an object, comprising the following steps:
  • the microbial liquid of known concentration is at least 3 microbial liquids of different known concentrations, preferably 3-6 microbial liquids of different known concentrations.
  • the concentration of the microorganism liquid of known concentration is 1-10 6 CFU mL -1 .
  • the microorganism is Escherichia coli
  • CFU is the concentration of E. coli.
  • CFU is the mixed concentration of Escherichia coli and Staphylococcus aureus.
  • the current reading time is within 5 minutes.
  • the device for detecting the current on the surface of the object is selected from an electrochemical workstation or a microcurrent meter.
  • the device for detecting the current on the surface of the object is a device capable of detecting a current of 100 ⁇ A or less.
  • the electrolyte used in the device for detecting the current on the surface of the object is selected from broth culture medium, physiological saline and phosphate buffered saline (PBS).
  • Another aspect of the present invention provides a system for controlling and detecting microorganisms on the surface of an object, which includes a current detection device, at least three microbial liquids with known concentrations, and forming the semiconductor coating described in any one of claims 1-3 on the surface of the object the material of the layer;
  • the device for detecting the current on the surface of the object is a device capable of detecting a current below 100 ⁇ A;
  • the material for forming the semiconductor coating according to any one of claims 1-3 on the surface of the object comprises silane coupling agent, zinc salt solution, sodium hydroxide, cyclohexamethylenetetramine, zinc acetate hexahydrate and metal nanoparticles.
  • the current generated by the interaction of the coating with the semiconductor characteristics of the present invention and the microorganisms can be used as a parameter for real-time monitoring of the number of microorganisms, and at the same time, it is a factor that interferes with the bacterial respiratory chain to achieve rapid non-release antibacterial.
  • the antibacterial system can perform antibacterial and real-time monitoring of the number of bacteria without interfering with the biocompatibility of the implant, and has the advantages of environmental protection and controllability.
  • the present invention relates to an antibacterial surface based on electron transfer with real-time monitoring of bacterial population. Compared with previous antibacterial surface designs, it has the following advantages:
  • the semiconductor coating provided by the present invention can achieve antimicrobial activity while providing the microbial contamination of the coating substrate product, and realizes the integration of antimicrobial and detection functions for the first time.
  • the semiconductor coating used in the present invention has a simple preparation process, high antibacterial efficiency, and can achieve high-efficiency inactivation in a short period of time. Because it utilizes physical properties for sterilization, the use of antibiotics is avoided, thereby avoiding antibiotic resistance caused by antibiotics. occur. And due to its limitations, inactivation is only limited to the surface of the semiconductor coating, which relies on contact with microorganisms. Compared with antibacterial surfaces that release ions or drugs, it can accurately kill microorganisms near the implanted surgical wound to achieve high-efficiency anti-infection avoidance. The use of antimicrobial peptides, antibiotics, etc., will produce systemic circulation after acting on the human body, resulting in potential safety hazards.
  • the present invention directly grows the semiconductor nano-array on the surface of the implant in situ, the surface modification is more firmly combined with the substrate, and the leakage of the modification does not occur.
  • metal oxides such as zinc oxide have antimicrobial activity, which is based on the antimicrobial activity of zinc ions, and the present invention does not utilize the antimicrobial activity of zinc ions, but is based on the current generated by microorganisms on the surface of the material. Therefore, the semiconductor coating of the present invention The antimicrobial activity is independent of the liquid environment, and antimicrobial activity can also be achieved in the air environment.
  • the present invention integrates the functions of monitoring microorganisms and anti-microbials, and can realize real-time monitoring of the infection status during the anti-infection process and prompt the user to take corresponding measures in time.
  • the monitoring and sterilization mechanism of the antibacterial system is based on the electron transfer between the material and the bacteria. Compared with the previous bifunctional surface that integrates traditional bacterial sensing devices and drug release, the working mechanism is simpler and the working system is more concise.
  • the semiconductor coating of the present invention can be combined with a wearable energy device, and can use autologous mechanical motion energy to monitor the number of bacteria and antibacterial.
  • the invention integrates the functions of monitoring bacteria and antibacterial, and can realize real-time monitoring of the infection status during the anti-infection process and prompt the user to take corresponding measures in time.
  • Figure 1 a Array of ZnO nanorods decorated with gold nanoparticles under scanning electron microscope.
  • Figure 1b shows the distribution of elements on the surface of the nano-gold-modified ZnO array.
  • Figure 2 Scatter plot of bacterial number and bacterial current and linear fit.
  • Fig. 3a The change curve of bacterial current within 1h of bacteria interacting with the material.
  • Figure 3b The antibacterial effect of bacteria and materials within 1 h.
  • Figure 4 Scatter diagram and linear fitting of bacterial number and bacterial current in the mixed bacterial solution composed of Escherichia coli and Staphylococcus aureus.
  • One aspect of the present invention provides a semiconductor coating that is anti-microbial and can self-measure the number of microorganisms.
  • the semiconductor coating is in situ generated on a substrate. Titanium dioxide nanomaterial arrays, silicon nanoarrays, etc.
  • the surface of the semiconductor nanoarray further includes modification of metal nanoparticles, preferably, the metal nanoparticles are selected from gold nanoparticles, silver nanoparticles, platinum nanoparticles, palladium nanoparticles and the like.
  • the substrate is selected from metal substrates and non-metallic substrates; preferably, the metal substrate is selected from titanium substrates, magnesium substrates, aluminum substrates, etc.; the non-metallic substrates are selected from silicon substrates Wait.
  • the nanomaterial size of the semiconductor nanoarray is 10-500 nm, preferably 80-150 nm.
  • the method for in-situ generation of semiconductor nanoarrays by the semiconductor coating on the substrate is: 1) forming epoxy groups on the surface of the substrate; The semiconductor nanoarrays are formed on the oxides.
  • the method for forming epoxy groups on the surface of the substrate is to react the substrate with a silane coupling agent, preferably ⁇ -(2,3-glycidoxy)propyltrimethoxysilane, to obtain epoxy groups.
  • a silane coupling agent preferably ⁇ -(2,3-glycidoxy)propyltrimethoxysilane
  • the method for generating zinc oxide semiconductor nanoarrays on epoxy groups by hydrothermal method is to react zinc salt solution and sodium hydroxide alcohol solution at 100-150 ° C to prepare a seed layer; then add ZnO semiconductor nanoarrays were generated by hydrothermal treatment in a mixed aqueous solution of cyclohexamethylenetetramine and zinc acetate hexahydrate.
  • the method for modifying the metal nanoparticles on the surface of the semiconductor nanoarray is to deposit the metal nanoparticles by magnetron sputtering.
  • the microorganisms are bacteria, fungi and viruses, preferably, the bacteria are Escherichia coli and Staphylococcus aureus.
  • the semiconductor nanoarray is a zinc oxide nanorod array, and the surface thereof is decorated with gold nanoparticles.
  • Another aspect of the present invention provides a method for preparing a semiconductor coating, comprising the steps of:
  • the method for forming epoxy groups on the surface of the substrate is to react the substrate with a silane coupling agent, preferably ⁇ -(2,3-glycidoxy)propyltrimethoxysilane, to obtain epoxy groups.
  • a silane coupling agent preferably ⁇ -(2,3-glycidoxy)propyltrimethoxysilane.
  • the epoxy group can make the semiconductor nano-array and the substrate contact more closely, thereby enhancing the electron transfer process, which is beneficial to improve the antibacterial effect.
  • the method for generating zinc oxide semiconductor nanoarrays on epoxy groups by hydrothermal method is to react zinc salt solution and sodium hydroxide alcohol solution at 100-150 ° C to prepare a seed layer; then add ZnO semiconductor nanoarrays were generated by hydrothermal treatment in a mixed aqueous solution of cyclohexamethylenetetramine and zinc acetate hexahydrate.
  • the method for modifying the metal nanoparticles on the surface of the semiconductor nanoarray is to deposit the metal nanoparticles by magnetron sputtering.
  • Yet another aspect of the present invention provides the use of the semiconductor coating, which provides the antimicrobial activity of the substrate while being capable of detecting the microbial content on the surface of the substrate.
  • Yet another aspect of the present invention provides an implant having the above-mentioned semiconductor coating.
  • Another aspect of the present invention provides a method for detecting microorganisms on the surface of an object, comprising the following steps:
  • the microbial liquid of known concentration is at least 3 microbial liquids of different known concentrations, preferably 3-6 microbial liquids of different known concentrations.
  • the concentration of the microbial liquid of known concentration is 1-10 6 CFU mL -1 .
  • the current reading time is within 5 minutes.
  • the device for detecting the current on the surface of the object is selected from an electrochemical workstation or a micro-galvanometer.
  • the device for detecting the current on the surface of the object is a device capable of detecting a current of less than 100 ⁇ A.
  • the electrolyte used in the device for detecting the current on the surface of the object is selected from broth culture medium, physiological saline and phosphate buffered saline (PBS).
  • PBS phosphate buffered saline
  • a method for establishing microbial concentration assessment on an object surface comprising the following steps:
  • the microorganism liquid of known concentration is mixed microorganism liquid, and the microorganism liquid of known concentration is 100 kinds of microorganism liquid of known concentration.
  • the microorganism liquid of known concentration is more than 1000 kinds of microorganism liquid of different known concentration.
  • a coating composed of semiconductors is first designed, and then the material is interacted with bacteria, and an electrochemical workstation or a microcurrent meter is connected to test the interface current.
  • the number of bacteria can be known by the magnitude of the current. In a short time, it can interfere with the electron transfer of the bacterial respiratory chain and inhibit its growth and reproduction.
  • the titanium alloy was processed into a rectangular parallelepiped with a length, width and height of 30mm, 30mm and 0.5mm, polished and ground, and then ultrasonically cleaned in acetone, ethanol and water for 10 minutes, and dried with nitrogen for use. Soak the above titanium alloy material in NaOH aqueous solution (10M) for 2h, and react with ⁇ -(2,3-glycidoxy)propyltrimethoxysilane KH-560 (2%v/v) for 10h to form epoxy function group.
  • the above-mentioned titanium alloy loaded with nano-gold-modified zinc oxide nanorods was connected to the electrochemical workstation, and bacterial liquid was added on the surface of the material.
  • the bacterial liquid concentration was 1-10 6 CFU mL -1 , and the bacterial current was recorded and the bacteria were drawn.
  • Bacterial liquid was dropped onto the surface of the above materials, the concentration of the bacterial liquid was 1-10 6 CFU mL -1 , the material was interacted with the bacteria for a certain time (1-180 min), and the bacteria were coated and tested for physiological activity to verify the antibacterial effect.
  • the titanium alloy was processed into a rectangular parallelepiped with a length, width and height of 30mm, 30mm, and 0.5mm, polished and ground, and then ultrasonically cleaned in acetone, ethanol, and water for 10 minutes, and dried with nitrogen for use.
  • the above titanium alloy materials were soaked in NaOH aqueous solution (10M) for 2h, and reacted with KH-560 (2%v/v) for 10h to form epoxy functional groups. Then prepare a methanol solution of Zn(CH 3 COO) 2 ⁇ 2H 2 O (10 mM) and NaOH (30 mM), pipette 10 ⁇ L drop onto the sample surface and treat at 120° C. for 5 min and repeat three times to prepare a seed layer.
  • the above samples were placed in a mixed aqueous solution of cyclohexamethylenetetramine (50 mM) and zinc acetate hexahydrate (50 mM), and hydrothermally treated at 96 °C for 10-12 h to generate ZnO nanorod semiconductors.
  • the sample was rinsed with 5 mL of water for 2 min and blown dry with nitrogen.
  • Gold nanoparticles were then deposited onto the nanorods by magnetron sputtering to enhance the electron transport capability of the semiconductor.
  • the microscopic morphology of the sample surface was observed by scanning electron microscope, and the microscopic morphology shown in Fig. 1a was obtained. It can be seen from the figure that the diameter of the zinc oxide nanorods is 100 nm, and the gold nanoparticles are attached to the nanorods or filled between the nanorods (as shown by the arrows in Figure 1).
  • Elemental content analysis was performed on the surface of the sample treated in Example 1.
  • the energy spectrum (Fig. 1b) shows that zinc, oxygen, gold, and titanium elements are uniformly distributed on the surface of the sample, indicating that the zinc oxide coating and the gold nanoparticles are uniformly distributed.
  • Example 2 The samples obtained in Example 1 were reacted with different concentrations of Escherichia coli (concentrations of 1, 10 3 , 10 5 and 10 6 CFU mL -1 ) to make a scatter plot of bacterial number and bacterial current, and fit. The results are shown in Figure 2.
  • the logarithmic number of bacteria was linearly related to bacterial current with a correlation coefficient as high as 0.98. It shows that the current obtained by the detection has a linear relationship with the bacterial content, and the bacterial content can be predicted by the current detection.
  • Example 1 The sample obtained in Example 1 was acted on with different concentrations of Escherichia coli and Staphylococcus aureus mixed bacterial solution (concentrations were 1, 10 3 , 10 5 and 10 6 CFU mL -1 ) to make a scatter plot of bacterial number and bacterial current , to fit.
  • concentrations were 1, 10 3 , 10 5 and 10 6 CFU mL -1
  • the results are shown in Figure 4.
  • the logarithm of the mixed bacterial count was linearly related to the bacterial current with a correlation coefficient as high as 0.96. It shows that the current obtained by the detection has a linear relationship with the mixed bacterial content, and the number of bacteria in the mixed bacterial solution of various bacterial species can be predicted by current detection.

Abstract

La présente invention concerne un revêtement semi-conducteur ayant des effets antimicrobiens et de mesure, son procédé de préparation et son utilisation et, en particulier, la divulgation concerne un revêtement semi-conducteur antimicrobien qui peut mesurer automatiquement la quantité de microbes, le revêtement semi-conducteur est sur un nanoréseau semi-conducteur généré in situ sur un groupe époxy généré sur un substrat, le nanoréseau de semi-conducteurs étant choisi parmi un réseau de nanomatériau d'oxyde de zinc, un réseau de nanomatériaux de dioxyde de titane ou un réseau de silicium ; et une surface du nanoréseau semi-conducteur comprend en outre une modification de nanoparticules métalliques. La divulgation concerne également l'utilisation d'un revêtement semi-conducteur, le revêtement semi-conducteur fournissant une activité antimicrobienne de substrat et étant susceptible de mesurer une teneur en microbes sur une surface du substrat. La présente invention intègre des fonctions de surveillance bactérienne et des fonctions antibactériennes, et peut être mise en œuvre lors de la lutte contre une infection pour effectuer une surveillance en temps réel de l'état d'une infection et notifier à un utilisateur de prendre les mesures correspondantes d'une manière opportune.
PCT/CN2020/106595 2020-08-03 2020-08-03 Revêtement semi-conducteur ayant des effets antimicrobiens et de mesure, son procédé de préparation et son utilisation WO2022027185A1 (fr)

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CN114657766B (zh) * 2022-03-19 2024-01-19 郑州大学 一种基于氧化锌纳米阵列的抗菌织物及其制备方法和应用

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