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CN120113681A - A composite disinfectant containing chlorine dioxide and its preparation process - Google Patents

A composite disinfectant containing chlorine dioxide and its preparation process
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CN120113681A
CN120113681ACN202510594865.3ACN202510594865ACN120113681ACN 120113681 ACN120113681 ACN 120113681ACN 202510594865 ACN202510594865 ACN 202510594865ACN 120113681 ACN120113681 ACN 120113681A
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王新
王昆
张曼
王珊珊
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Shandong Zhaoguan Pharmaceutical Co ltd
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Abstract

The invention provides a composite disinfectant containing chlorine dioxide and a preparation process thereof, belonging to the technical field of preparation of composite disinfectants; the preparation process comprises the following steps of preparing a carrier stabilizer, preparing modified carboxymethyl chitosan, preparing sustained-release gel microspheres, preparing a modified chitosan derivative and preparing a chlorine dioxide composite disinfectant. The chlorine dioxide composite disinfectant prepared by the invention can avoid the initial burst release of the slow-release gel microsphere, so that the slow-release gel microsphere can stably and slowly release chlorine dioxide components, can play a role in disinfection and antibiosis for a long time and high efficiency, and can reduce the corrosion of chlorine dioxide to metals.

Description

Composite disinfectant containing chlorine dioxide and preparation process thereof
Technical Field
The invention relates to the technical field of preparation of composite disinfectants, in particular to a composite disinfectant containing chlorine dioxide and a preparation process thereof.
Background
The chlorine dioxide is used as a high-efficiency broad-spectrum disinfectant, can kill almost all microorganisms including bacteria, fungi and viruses, does not generate cancerogenic substances after sterilization, has strong oxidizing property, can be widely applied to a plurality of fields, for example, the field of water treatment, can effectively purify drinking water, remove peculiar smell and pigment in the water, can simultaneously show high-efficiency sterilization and virus killing capability under low concentration, has a sterilization effect obviously superior to that of chlorine and sodium chlorite, has higher virus inhibiting capability than that of chlorine and is stronger than that of ozone. The sterilizing agent can be used for sterilizing hospital sewage in the field of medical care, can effectively kill pathogens, enables the treated sewage to reach the national relevant standard, can sterilize food factories, beverage factories, meat factories and the like in the food industry, ensures the food safety, and plays an important role in sterilizing in other fields such as petroleum industry and the like.
However, chlorine dioxide itself has some drawbacks that are difficult to overcome. On the one hand, it is extremely unstable, extremely sensitive to sunlight and extremely easy to degrade under the sunlight, which brings great difficulty to transportation and storage and limits the application range. On the other hand, the chlorine dioxide is taken as a strong oxidant, and early researches consider that the chlorine dioxide has strong corrosiveness, and common stainless steel materials are corroded, so that the chlorine dioxide is prevented from being popularized and applied on a large scale.
Aiming at the pain point of unstable chlorine dioxide, the gas slow-release material has the advantages of realizing the sustained release of the chlorine dioxide, prolonging the disinfection aging, reducing frequent dosing operation and the like, and becomes an important technical direction for improving the disinfection effect, and although the gas slow-release material has a plurality of practical applications, the problems of gas burst release, unstable gas slow-release rate and the like in the release process of some gas slow-release materials currently used in commerce still exist.
Therefore, we propose a compound disinfectant containing chlorine dioxide which slows down the burst of gas, improves the stability and slows down the corrosion and a preparation process thereof.
Disclosure of Invention
Aiming at the defects existing in the prior art, the invention aims to provide a composite disinfectant containing chlorine dioxide and a preparation process thereof.
A preparation process of a composite disinfectant containing chlorine dioxide comprises the following steps:
S1 preparation of Carrier stabilizer
Mixing sodium hydroxide, sodium aluminate and deionized water, adding sodium silicate nonahydrate, and reacting to prepare a carrier stabilizer;
s2, preparation of modified carboxymethyl chitosan
Preparing modified carboxymethyl chitosan by mixing 3-carboxyl-5-nitrobenzoic acid, 1-ethyl- (3-dimethylaminopropyl) carbodiimide hydrochloride, N-hydroxysuccinimide and dimethyl sulfoxide to modify carboxymethyl chitosan;
S3, preparation of sustained release gel microspheres
Adding a carrier stabilizer into deionized water, then adding a modified carboxymethyl chitosan solution and sodium chlorite to obtain a mixed system, dripping the mixed system into a zinc nitrate hexahydrate solution by using a rubber head dropper, then adding the mixed system into a tannic acid solution, and freeze-drying to obtain slow-release gel microspheres;
s4 preparation of modified chitosan derivative
The modified chitosan derivative is prepared by adopting 5-chloromethyl-8-hydroxyquinoline hydrochloride modified chitosan cinnamaldehyde Schiff base;
s5, preparation of chlorine dioxide composite disinfectant
And (3) dissolving the modified chitosan derivative in acetic acid solution, adding magnesium lithium silicate activating solution to obtain wrapping liquid, spraying the wrapping liquid into the slow-release gel microspheres in a sugar coating machine, and then freeze-drying to obtain the chlorine dioxide composite disinfectant.
Further, the preparation of the carrier stabilizer in the step S1 specifically comprises the following steps:
s1.1, mixing 2-3 parts by weight of sodium hydroxide, 0.5-0.8 part by weight of sodium aluminate and 29-32 parts by weight of deionized water, and stirring at 2000-3000r/min for 20-30min to obtain a mixed solution;
S1.2, adding 3.81-4.23 parts by weight of sodium silicate nonahydrate into the mixed solution, stirring and mixing for 6-8 hours, then placing the mixed solution into a stainless steel high-pressure reaction kettle, reacting for 14-15 hours at 80-82 ℃, then washing the mixed solution to be neutral by adopting deionized water, drying the mixed solution in vacuum, then reacting for 4-5 hours at 500-520 ℃ under nitrogen atmosphere, and then grinding and crushing the mixed solution to obtain the carrier stabilizer.
Further, the preparation of the modified carboxymethyl chitosan in the step S2 specifically comprises the following steps:
S2.1, adding 0.6-0.8 part by weight of 3-carboxyl-5-nitrobenzoic acid, 0.52-0.69 part by weight of 1-ethyl- (3-dimethylaminopropyl) carbodiimide hydrochloride and 0.33-0.46 part by weight of N-hydroxysuccinimide into 30-35 parts by weight of dimethyl sulfoxide, stirring and mixing for 4-5 hours at 200-300r/min to obtain an activated liquid;
s2.2, adding 3-5 parts by weight of carboxymethyl chitosan into 400-420 parts by weight of deionized water, stirring and mixing for 20-30min to obtain carboxymethyl chitosan solution;
S2.3, dropwise adding the activated solution into carboxymethyl chitosan solution by using a syringe, stirring for 10-12h at room temperature, adding 0.1M sodium hydroxide solution to adjust the pH to 9-9.2, then filling into a dialysis bag, dialyzing for 3-4d, changing water every 4-5h, and freeze-drying after the dialysis is completed to obtain the modified carboxymethyl chitosan.
Further, the preparation of the sustained-release gel microsphere in the step S3 specifically comprises the following steps:
S3.1, adding 3-5 parts by weight of modified carboxymethyl chitosan into deionized water, stirring and mixing for 20-30min to obtain a 4wt% modified carboxymethyl chitosan solution, adding 2-3 parts by weight of tannic acid into a phosphate buffer salt solution, and stirring and mixing for 20-30min to obtain a 5wt% tannic acid solution;
S3.2, adding 2-3 parts by weight of carrier stabilizer into 10-12 parts by weight of deionized water, performing ultrasonic treatment for 20-30min to obtain a mixture, adding 4wt% of modified carboxymethyl chitosan solution and sodium chlorite, and stirring for 1-2h at room temperature to obtain a mixed system;
s3.3, dripping the mixed system into 12-15 parts by weight of 10% zinc nitrate hexahydrate solution by using a rubber head dropper, then adding the zinc nitrate hexahydrate solution into 5wt% tannic acid solution, mixing for 3-5min, and freeze-drying to obtain the slow-release gel microspheres.
Further, the preparation of the modified chitosan derivative in the step S4 specifically comprises the following steps:
S4.1, mixing 10-12 parts by weight of 8-hydroxyquinoline, 11-13 parts by weight of concentrated hydrochloric acid and 11-13 parts by weight of 37wt% formaldehyde, introducing hydrogen chloride gas at 25-28 ℃, stirring and reacting for 10-12 hours, and then carrying out suction filtration, washing and drying to obtain 5-chloromethyl-8-hydroxyquinoline hydrochloride;
S4.2, adding 1.38-1.42 parts by weight of chitosan cinnamaldehyde Schiff base into 100-120 parts by weight of acetic acid solution with the concentration of 3%, swelling and reacting for 1-2 hours, then adding 1.78-1.83 parts by weight of 5-chloromethyl-8-hydroxyquinoline hydrochloride, heating to 80-83 ℃, reacting for 24-28 hours, then adding 10% sodium hydroxide solution, regulating the pH to be neutral, and finally carrying out suction filtration, washing and drying to obtain the modified chitosan derivative.
Further, the preparation of the chlorine dioxide compound disinfectant in the step S5 specifically comprises the following steps:
s5.1, uniformly mixing 2-3 parts by weight of lithium magnesium silicate with 30-38 parts by weight of deionized water, placing in a 15-30 ℃ water bath, stirring, and placing at room temperature to obtain a lithium magnesium silicate activation solution;
S5.2, adding 2-4 parts by weight of modified chitosan derivative into 10-12 parts by weight of acetic acid solution with the concentration of 2-3%, stirring and mixing for 20-30min at 200-300r/min, then adding magnesium lithium silicate activation solution, stirring and mixing for 10-12min to obtain wrapping solution;
s5.3, spraying 32-45 parts by weight of wrapping liquid into 10-12 parts by weight of slow-release gel microspheres in a sugar coating machine, and then freeze-drying to obtain the chlorine dioxide composite disinfectant.
Further, the addition amount of the 4wt% modified carboxymethyl chitosan solution in the step S3.1 is 8-10% (W/V) of the mixture.
Further, the sodium chlorite added in the step S3.1 is 20-23% (W/V) of the mixture.
A chlorine dioxide-containing composite disinfectant prepared by any one of the preparation processes of the chlorine dioxide-containing composite disinfectant.
Compared with the prior art, the invention has at least the following beneficial effects:
1. According to the invention, the sustained-release gel microsphere coated with sodium chlorite is prepared and is used for sustained release of chlorine dioxide gas, so that the durable antibacterial effect is achieved, the carrier stabilizer is added in the preparation process of the sustained-release gel microsphere, the carrier stabilizer can shorten the gel time, the purpose of enhancing the gelation performance of the material is achieved, the gel stability can be improved after the carrier stabilizer is added, the sustained-release time is improved, the initial burst release of the sustained-release gel microsphere can be avoided, the chlorine dioxide component can be stably and slowly released, and the sterilizing antibacterial effect can be effectively exerted for a long time.
2. When the slow-release gel microsphere is prepared, zinc nitrate hexahydrate is firstly reacted, then the zinc nitrate hexahydrate is added into tannic acid solution, the modified carboxymethyl chitosan and Zn2+ are quickly crosslinked into gel to wrap chlorine dioxide gas, then the gel is added into tannic acid solution, tannic acid is further crosslinked with the modified carboxymethyl chitosan, secondary crosslinking fills the pores of a primary network to form a denser double network structure, the dense network structure can slow down the problems of sudden release and unstable gas slow release rate of the chlorine dioxide gas, the effect of stably and slowly releasing the chlorine dioxide is further achieved, meanwhile, zn2+ and tannic acid can produce synergistic antibacterial effect with the chlorine dioxide, and the antibacterial capability of the disinfectant is improved.
3. According to the invention, the slow-release gel microspheres are wrapped by wrapping liquid, so that the embedding stability can be effectively improved, the slow-release gel microspheres are kept in a stable state, the stability of the chlorine dioxide composite disinfectant is further improved, meanwhile, when the composite disinfectant is mixed with water for spraying and disinfecting, the surface wrapping layer swells when meeting water, and the modified chitosan derivative in the wrapping layer can be adsorbed on the metal surface to form a protective film, so that the corrosion of chlorine dioxide gas on the metal material is slowed down.
Drawings
The accompanying drawings, which are incorporated herein and form a part of the specification, illustrate embodiments of the present invention and, together with the description, further serve to explain the principles of the invention and to enable a person skilled in the pertinent art to make and use the invention.
FIG. 1 is a graph showing the sustained-release effect test of examples 1-3 and comparative examples 1-3 and 6 of the present invention.
Detailed Description
The preparation process of the composite disinfectant containing chlorine dioxide provided by the invention is described in detail below with reference to the accompanying drawings and specific examples. While the invention has been described herein in detail in order to make the embodiments more detailed, the following embodiments are preferred and can be embodied in other forms as well known to those skilled in the art, and the accompanying drawings are only for the purpose of describing the embodiments more specifically and are not intended to limit the invention to the specific forms disclosed herein.
Example 1
A preparation process of a composite disinfectant containing chlorine dioxide comprises the following steps:
S1 preparation of Carrier stabilizer
S1.1, mixing 2 parts by weight of sodium hydroxide, 0.5 part by weight of sodium aluminate and 29 parts by weight of deionized water, and stirring at 2000r/min for 20min to obtain a mixed solution;
S1.2, adding 3.81 parts by weight of sodium silicate nonahydrate into the mixed solution, stirring and mixing for 6 hours, then placing the mixed solution into a stainless steel high-pressure reaction kettle, reacting for 14 hours at 80 ℃, then washing the mixed solution to be neutral by adopting deionized water, drying the mixed solution in vacuum, then reacting for 4 hours at 500 ℃ in a nitrogen atmosphere, and grinding and crushing the mixed solution to obtain a carrier stabilizer;
s2, preparation of modified carboxymethyl chitosan
S2.1, adding 0.6 weight part of 3-carboxyl-5-nitrobenzoic acid, 0.52 weight part of 1-ethyl- (3-dimethylaminopropyl) carbodiimide hydrochloride and 0.33 weight part of N-hydroxysuccinimide into 30 weight parts of dimethyl sulfoxide, stirring and mixing for 4 hours at 200r/min to obtain an activation solution;
S2.2, adding 3 parts by weight of carboxymethyl chitosan into 400 parts by weight of deionized water, stirring and mixing for 20min to obtain carboxymethyl chitosan solution;
S2.3, dropwise adding the activated solution into carboxymethyl chitosan solution by using a syringe, stirring for 10 hours at room temperature, adding 0.1M sodium hydroxide solution to adjust the pH to 9, then filling into a dialysis bag, dialyzing for 3d, changing water every 4 hours, and freeze-drying after the dialysis is completed to obtain modified carboxymethyl chitosan;
S3, preparation of sustained release gel microspheres
S3.1, adding 3 parts by weight of modified carboxymethyl chitosan into deionized water, stirring and mixing for 20min to obtain a 4wt% modified carboxymethyl chitosan solution, adding 2 parts by weight of tannic acid into a phosphate buffer salt solution, and stirring and mixing for 20min to obtain a 5wt% tannic acid solution;
s3.2, adding 2 parts by weight of carrier stabilizer into 10 parts by weight of deionized water, performing ultrasonic treatment for 20min to obtain a mixture, then adding 8% (W/V) of 4wt% modified carboxymethyl chitosan solution and 20% (W/V) of sodium chlorite, and stirring for 1h at room temperature to obtain a mixed system;
S3.3, dripping the mixed system into 12 parts by weight of zinc nitrate hexahydrate solution with the concentration of 10 percent by using a rubber head dropper, then adding the zinc nitrate hexahydrate solution into 5 weight percent tannic acid solution, mixing for 3min, and freeze-drying to obtain slow-release gel microspheres;
s4 preparation of modified chitosan derivative
S4.1, mixing 10 parts by weight of 8-hydroxyquinoline, 11 parts by weight of concentrated hydrochloric acid and 11 parts by weight of 37wt% formaldehyde, introducing hydrogen chloride gas at 25 ℃, stirring for reaction for 10 hours, and then carrying out suction filtration, washing and drying to obtain 5-chloromethyl-8-hydroxyquinoline hydrochloride;
S4.2, adding 1.38 parts by weight of chitosan cinnamaldehyde Schiff base into 100 parts by weight of acetic acid solution with the concentration of 3%, carrying out swelling reaction for 1h, then adding 1.78 parts by weight of 5-chloromethyl-8-hydroxyquinoline hydrochloride, heating to 80 ℃, carrying out reaction for 24h, then adding 10% sodium hydroxide solution, regulating the pH to be neutral, and finally carrying out suction filtration, washing and drying to obtain the modified chitosan derivative;
s5, preparation of chlorine dioxide composite disinfectant
S5.1, uniformly mixing 2 parts by weight of lithium magnesium silicate with 30 parts by weight of deionized water, placing in a 15 ℃ water bath, stirring, and placing at room temperature to obtain a lithium magnesium silicate activation solution;
S5.2, adding 2 parts by weight of modified chitosan derivative into 10 parts by weight of acetic acid solution with the concentration of 2%, stirring and mixing for 20min at 200r/min, then adding magnesium lithium silicate activation solution, stirring and mixing for 10min to obtain wrapping solution;
s5.3, spraying 32 parts by weight of wrapping liquid into 10 parts by weight of slow-release gel microspheres in a sugar coating machine, and then freeze-drying to obtain the chlorine dioxide composite disinfectant.
Example 2
A preparation process of a composite disinfectant containing chlorine dioxide comprises the following steps:
S1 preparation of Carrier stabilizer
S1.1, mixing 2 parts by weight of sodium hydroxide, 0.5 part by weight of sodium aluminate and 29 parts by weight of deionized water, and stirring at 3000r/min for 30min to obtain a mixed solution;
S1.2, adding 3.81 parts by weight of sodium silicate nonahydrate into the mixed solution, stirring and mixing for 8 hours, then placing the mixed solution into a stainless steel high-pressure reaction kettle, reacting for 15 hours at 82 ℃, then washing the mixed solution to be neutral by adopting deionized water, drying the mixed solution in vacuum, then reacting for 5 hours at 520 ℃ in a nitrogen atmosphere, and grinding and crushing the mixed solution to obtain a carrier stabilizer;
s2, preparation of modified carboxymethyl chitosan
S2.1, adding 0.6 weight part of 3-carboxyl-5-nitrobenzoic acid, 0.52 weight part of 1-ethyl- (3-dimethylaminopropyl) carbodiimide hydrochloride and 0.33 weight part of N-hydroxysuccinimide into 30 weight parts of dimethyl sulfoxide, stirring and mixing for 5 hours at 300r/min to obtain an activation solution;
s2.2, adding 3 parts by weight of carboxymethyl chitosan into 400 parts by weight of deionized water, stirring and mixing for 30min to obtain carboxymethyl chitosan solution;
S2.3, dropwise adding the activated solution into carboxymethyl chitosan solution by using a syringe, stirring for 12 hours at room temperature, adding 0.1M sodium hydroxide solution to adjust the pH to 9, then filling into a dialysis bag, dialyzing for 4d, changing water every 5 hours, and freeze-drying after the dialysis is completed to obtain modified carboxymethyl chitosan;
S3, preparation of sustained release gel microspheres
S3.1, adding 3 parts by weight of modified carboxymethyl chitosan into deionized water, stirring and mixing for 30min to obtain a 4wt% modified carboxymethyl chitosan solution, adding 2 parts by weight of tannic acid into a phosphate buffer salt solution, and stirring and mixing for 30min to obtain a 5wt% tannic acid solution;
S3.2, adding 2 parts by weight of carrier stabilizer into 10 parts by weight of deionized water, performing ultrasonic treatment for 30min to obtain a mixture, then adding 8% (W/V) of 4wt% modified carboxymethyl chitosan solution and 20% (W/V) of sodium chlorite, and stirring for 2h at room temperature to obtain a mixed system;
S3.3, dripping the mixed system into 12 parts by weight of zinc nitrate hexahydrate solution with the concentration of 10% by using a rubber head dropper, then adding the zinc nitrate hexahydrate solution into 5wt% tannic acid solution, mixing for 5min, and freeze-drying to obtain slow-release gel microspheres;
s4 preparation of modified chitosan derivative
S4.1, mixing 10 parts by weight of 8-hydroxyquinoline, 11 parts by weight of concentrated hydrochloric acid and 11 parts by weight of 37wt% formaldehyde, introducing hydrogen chloride gas at 28 ℃, stirring for reaction for 12 hours, and then carrying out suction filtration, washing and drying to obtain 5-chloromethyl-8-hydroxyquinoline hydrochloride;
S4.2, adding 1.38 parts by weight of chitosan cinnamaldehyde Schiff base into 100 parts by weight of acetic acid solution with the concentration of 3%, carrying out swelling reaction for 2 hours, then adding 1.78 parts by weight of 5-chloromethyl-8-hydroxyquinoline hydrochloride, heating to 83 ℃, carrying out reaction for 28 hours, then adding 10% sodium hydroxide solution, regulating the pH to be neutral, and finally carrying out suction filtration, washing and drying to obtain the modified chitosan derivative;
s5, preparation of chlorine dioxide composite disinfectant
S5.1, uniformly mixing 2 parts by weight of lithium magnesium silicate with 30 parts by weight of deionized water, placing in a water bath at 30 ℃, stirring, and placing at room temperature to obtain a lithium magnesium silicate activation solution;
S5.2, adding 2 parts by weight of modified chitosan derivative into 10 parts by weight of acetic acid solution with the concentration of 2%, stirring and mixing for 30min at 300r/min, then adding magnesium lithium silicate activation solution, stirring and mixing for 12min to obtain wrapping solution;
s5.3, spraying 32 parts by weight of wrapping liquid into 10 parts by weight of slow-release gel microspheres in a sugar coating machine, and then freeze-drying to obtain the chlorine dioxide composite disinfectant.
Example 3
A preparation process of a composite disinfectant containing chlorine dioxide comprises the following steps:
S1 preparation of Carrier stabilizer
S1.1, mixing 3 parts by weight of sodium hydroxide, 0.8 part by weight of sodium aluminate and 32 parts by weight of deionized water, and stirring at 2000r/min for 20min to obtain a mixed solution;
S1.2, adding 4.23 parts by weight of sodium silicate nonahydrate into the mixed solution, stirring and mixing for 6 hours, then placing the mixed solution into a stainless steel high-pressure reaction kettle, reacting for 14 hours at 80 ℃, then washing the mixed solution to be neutral by adopting deionized water, drying the mixed solution in vacuum, then reacting for 4 hours at 500 ℃ in a nitrogen atmosphere, and grinding and crushing the mixed solution to obtain a carrier stabilizer;
s2, preparation of modified carboxymethyl chitosan
S2.1, adding 0.8 weight part of 3-carboxyl-5-nitrobenzoic acid, 0.69 weight part of 1-ethyl- (3-dimethylaminopropyl) carbodiimide hydrochloride and 0.46 weight part of N-hydroxysuccinimide into 35 weight parts of dimethyl sulfoxide, stirring and mixing for 4 hours at 200r/min to obtain an activation solution;
s2.2, adding 5 parts by weight of carboxymethyl chitosan into 420 parts by weight of deionized water, stirring and mixing for 20 minutes to obtain carboxymethyl chitosan solution;
S2.3, dropwise adding the activated solution into carboxymethyl chitosan solution by using a syringe, stirring for 10 hours at room temperature, adding 0.1M sodium hydroxide solution to adjust the pH to 9.2, then filling into a dialysis bag, dialyzing for 3d, changing water every 4 hours, and freeze-drying after the dialysis is completed to obtain modified carboxymethyl chitosan;
S3, preparation of sustained release gel microspheres
S3.1, adding 5 parts by weight of modified carboxymethyl chitosan into deionized water, stirring and mixing for 20min to obtain a 4wt% modified carboxymethyl chitosan solution, adding 3 parts by weight of tannic acid into a phosphate buffer salt solution, and stirring and mixing for 20min to obtain a 5wt% tannic acid solution;
S3.2, adding 3 parts by weight of a carrier stabilizer into 12 parts by weight of deionized water, carrying out ultrasonic treatment for 20min to obtain a mixture, then adding 8% (W/V) of a 4wt% modified carboxymethyl chitosan solution and 20% (W/V) of sodium chlorite, and stirring for 2h at room temperature to obtain a mixed system;
s3.3, dripping the mixed system into 15 parts by weight of zinc nitrate hexahydrate solution with the concentration of 10% by using a rubber head dropper, then adding the zinc nitrate hexahydrate solution into 5wt% tannic acid solution, mixing for 3min, and freeze-drying to obtain slow-release gel microspheres;
s4 preparation of modified chitosan derivative
S4.1, mixing 12 parts by weight of 8-hydroxyquinoline, 13 parts by weight of concentrated hydrochloric acid and 13 parts by weight of 37wt% formaldehyde, introducing hydrogen chloride gas at 25 ℃, stirring for reaction for 10 hours, and then carrying out suction filtration, washing and drying to obtain 5-chloromethyl-8-hydroxyquinoline hydrochloride;
S4.2, adding 1.42 parts by weight of chitosan cinnamaldehyde Schiff base into 120 parts by weight of acetic acid solution with the concentration of 3%, carrying out swelling reaction for 1h, then adding 1.83 parts by weight of 5-chloromethyl-8-hydroxyquinoline hydrochloride, heating to 80 ℃, carrying out reaction for 24h, then adding 10% sodium hydroxide solution, regulating the pH to be neutral, and finally carrying out suction filtration, washing and drying to obtain the modified chitosan derivative;
s5, preparation of chlorine dioxide composite disinfectant
S5.1, uniformly mixing 3 parts by weight of lithium magnesium silicate with 38 parts by weight of deionized water, placing in a 15 ℃ water bath, stirring, and placing at room temperature to obtain a lithium magnesium silicate activation solution;
s5.2, adding 4 parts by weight of modified chitosan derivative into 12 parts by weight of acetic acid solution with the concentration of 3%, stirring and mixing for 20min at 200r/min, then adding magnesium lithium silicate activation solution, stirring and mixing for 10min to obtain wrapping solution;
s5.3, spraying 45 parts by weight of wrapping liquid into 12 parts by weight of slow-release gel microspheres in a sugar coating machine, and then freeze-drying to obtain the chlorine dioxide composite disinfectant.
Comparative example 1
Comparative example 1 was different from example 1 in that comparative example 1 was a removal step S1, S3.2 was replaced with "8% (W/V) of a 4wt% modified carboxymethyl chitosan solution and 20% (W/V) of sodium chlorite were added to 10 parts by weight of deionized water, and stirred at room temperature for 1 hour to obtain a mixed system", and the remaining steps were unchanged to prepare a chlorine dioxide composite disinfectant, which was designated as comparative example 1.
Comparative example 2
Comparative example 2 is different from example 1 in that comparative example 2 is a removal step S2, the modified carboxymethyl chitosan in step S3.1 is replaced by carboxymethyl chitosan, and the rest steps are unchanged to prepare a chlorine dioxide composite disinfectant, which is denoted as comparative example 2.
Comparative example 3
Compared with example 1, the difference of comparative example 3 is that comparative example 3 is to replace step S3.3 with "12 parts by weight of zinc nitrate hexahydrate solution with concentration of 10% and 5wt% tannic acid solution are mixed first, then a mixed system is dripped by using a rubber head dropper, mixing is carried out for 3min, freeze drying is carried out, and a slow-release gel microsphere is obtained, and the rest steps are used for preparing chlorine dioxide composite disinfectant unchanged, which is recorded as comparative example 3.
Comparative example 4
Compared with example 1, the difference of comparative example 4 is that comparative example 4 is removal steps S4-S5, and the slow release gel microsphere prepared in step S3 is chlorine dioxide composite disinfectant, which is denoted as comparative example 4.
Comparative example 5
Comparative example 5 is different from example 1 in that comparative example 5 is a removal step S4, the modified chitosan derivative in step S5.2 is replaced with chitosan cinnamaldehyde schiff base, and the rest steps are unchanged to prepare a chlorine dioxide composite disinfectant, which is denoted as comparative example 5.
Comparative example 6
Comparative example 6 is different from example 1 in that comparative example 6 is a tannic acid solution removed in step S3.3, and the remaining steps are unchanged to prepare a chlorine dioxide complex disinfectant, which is denoted as comparative example 6.
Determination of sustained release properties:
For the slow release performance measurement of examples 1-3 and comparative examples 1-3 and 6, a chlorine dioxide composite disinfectant was prepared into a solution according to the water ratio of 1g to 1L, placed in a watering can according to the usual environment disinfection habit, then placed in a 30dm3 sealed glass instrument, started to time, and the released chlorine dioxide amount was measured at normal temperature using a portable chlorine dioxide detector, the chlorine dioxide release amount was recorded every 20min, and the release rate was calculated according to the release amount, as shown in the following formula:
Release rate (ppm/min) = (C-C0)/T;
wherein the release rate is the slow release rate of chlorine dioxide (ppm/min), C is the concentration at the end of the test (ppm), C0 is the initial concentration (ppm), T is the total time of the test (min), and the test results are shown in FIG. 1.
According to the slow release rate curve shown in fig. 1, the chlorine dioxide composite disinfectant prepared by the invention can achieve the effect of stable and long-acting slow release, and according to the data of comparative example 1, the carrier stabilizer is added in the preparation process of the slow release gel microsphere, so that the initial burst release of the slow release gel microsphere can be avoided.
From the data of comparative example 2, it can be seen that the modified carboxymethyl chitosan is adopted to prepare the slow-release gel microsphere, so that the chlorine dioxide component can be released smoothly and slowly, because the modified carboxymethyl chitosan can improve the crosslinking effect, the stability of the gel network can be enhanced, and the slow-release effect can be achieved.
As can be seen from the data of comparative examples 3 and 6, when preparing the sustained release gel microspheres, zinc nitrate hexahydrate reaction is performed first, and then the problems of burst release of chlorine dioxide gas and unstable gas sustained release rate can be alleviated when the zinc nitrate hexahydrate is added into tannic acid solution.
Stability determination:
the stability (the reduction rate of the content of the effective components is less than or equal to 10%) of examples 1-3 and comparative example 4 is measured according to GB/T26366-2021 "hygienic requirement for chlorine dioxide disinfectant", and the test results are shown in Table 1.
TABLE 1 determination of stability of chlorine dioxide composite disinfectant
From the data in table 1, it can be seen that the encapsulation liquid is used for encapsulating the slow-release gel microspheres, so that the embedding stability can be effectively improved, the slow-release gel microspheres are kept in a stable state, the stability of the chlorine dioxide composite disinfectant is further improved, and the storage time is prolonged.
The chlorine dioxide composite disinfectants prepared in examples 1-3 and comparative examples 4-5 were prepared into solutions with 1g of 1L water, placed in a watering can according to the usual practice of environmental disinfection, and then tested for corrosiveness to the disinfectants according to item 2.2.4 of the disinfection technical Specification (2002 edition), and the test results are referred to Table 2.
TABLE 2 corrosiveness determination of examples 1-3 and comparative examples 4-5
As can be seen from the data in table 2, the addition of the modified chitosan derivative to the coating liquid can slow down the corrosion of stainless steel metal materials by chlorine dioxide gas, and the modified chitosan derivative can further improve the corrosion inhibition effect.
And (3) determining the microbial killing performance:
The chlorine dioxide composite disinfectant prepared in examples 1-3 and comparative example 6 is prepared into a solution according to the water ratio of 1g to 1L, and is placed in a spray can according to the usual environment disinfection habit, the microorganism killing performance is measured according to GB/T26366-2021 "chlorine dioxide disinfectant sanitary requirement", and the test results are shown in Table 3:
TABLE 3 results of the microbiocidal performance measurements of examples 1-3 and comparative example 6
As can be seen from Table 3, the chlorine dioxide composite disinfectant prepared by the invention has good disinfection effect, and the addition of the tannic acid solution can improve the antibacterial effect.
The above embodiments are merely illustrative of the principles of the present invention and its effectiveness, and are not intended to limit the invention. Modifications and variations may be made to the above-described embodiments by those skilled in the art without departing from the spirit and scope of the invention. Accordingly, it is intended that all equivalent modifications and variations of the invention be covered by the claims, which are within the ordinary skill of the art, be within the spirit and scope of the present disclosure.

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CN114848582A (en)*2022-05-052022-08-05江苏春申堂生物科技有限公司Slow-release antibacterial gel for treating female leukoplakia vulvae and preparation method thereof
CN116019125A (en)*2023-03-292023-04-28山东华实药业有限公司Chlorine dioxide slow-release gel and preparation method thereof
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CN101669518A (en)*2009-09-302010-03-17北京欧凯纳斯科技有限公司Germicidal antiviral composite containing chlorine dioxide
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