CN107530464A - Make the microorganism deactivated method of the floating in space - Google Patents
Make the microorganism deactivated method of the floating in space Download PDFInfo
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- CN107530464A CN107530464A CN201680028104.0A CN201680028104A CN107530464A CN 107530464 A CN107530464 A CN 107530464A CN 201680028104 A CN201680028104 A CN 201680028104A CN 107530464 A CN107530464 A CN 107530464A
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- chlorine dioxide
- chlorite
- medicament
- air
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Classifications
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L9/00—Disinfection, sterilisation or deodorisation of air
- A61L9/015—Disinfection, sterilisation or deodorisation of air using gaseous or vaporous substances, e.g. ozone
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L2/00—Methods or apparatus for disinfecting or sterilising materials or objects other than foodstuffs or contact lenses; Accessories therefor
- A61L2/16—Methods or apparatus for disinfecting or sterilising materials or objects other than foodstuffs or contact lenses; Accessories therefor using chemical substances
- A61L2/20—Gaseous substances, e.g. vapours
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L2/00—Methods or apparatus for disinfecting or sterilising materials or objects other than foodstuffs or contact lenses; Accessories therefor
- A61L2/26—Accessories or devices or components used for biocidal treatment
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L9/00—Disinfection, sterilisation or deodorisation of air
- A61L9/01—Deodorant compositions
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/16—Clays or other mineral silicates
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B11/00—Oxides or oxyacids of halogens; Salts thereof
- C01B11/02—Oxides of chlorine
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B11/00—Oxides or oxyacids of halogens; Salts thereof
- C01B11/02—Oxides of chlorine
- C01B11/022—Chlorine dioxide (ClO2)
- C01B11/023—Preparation from chlorites or chlorates
- C01B11/024—Preparation from chlorites or chlorates from chlorites
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L2202/00—Aspects relating to methods or apparatus for disinfecting or sterilising materials or objects
- A61L2202/10—Apparatus features
- A61L2202/11—Apparatus for generating biocidal substances, e.g. vaporisers, UV lamps
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L2202/00—Aspects relating to methods or apparatus for disinfecting or sterilising materials or objects
- A61L2202/20—Targets to be treated
- A61L2202/25—Rooms in buildings, passenger compartments
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L2209/00—Aspects relating to disinfection, sterilisation or deodorisation of air
- A61L2209/20—Method-related aspects
- A61L2209/21—Use of chemical compounds for treating air or the like
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- Animal Behavior & Ethology (AREA)
- General Health & Medical Sciences (AREA)
- Epidemiology (AREA)
- Veterinary Medicine (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Geology (AREA)
- Inorganic Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Dispersion Chemistry (AREA)
- Disinfection, Sterilisation Or Deodorisation Of Air (AREA)
- Catalysts (AREA)
Abstract
The present invention problem be：A kind of chlorine dioxide that enough requirements are supplied to space is provided, so as to making the microorganism deactivated method of floating.The present invention solution be：There is provided a kind of floating made in space microorganism deactivated method, include (1)：The step of preparation is carried with chloritic Porous material and the solid-state pharmacy of (B) metallic catalyst or metal oxide catalyst containing (A), herein, in aforementioned solid medicament, foregoing chlorite is 1 with the mass ratio of aforementioned metal catalyst or metal oxide catalyst：0.04 to 0.8；(2)：The step of visible ray is irradiated to aforementioned solid medicament；And (3)：The step of floating space existing for Institute of Micro-biology will be supplied in from chlorine dioxide caused by foregoing solid-state pharmacy.
Description
Technical field
The present invention relates to the chlorine dioxide using low concentration, makes the microorganism deactivated method of the floating in space.
Bei Jing Ji Intraoperative
It is well known that chlorine dioxide is such as at low concentration (for example, 0.3ppm (hundred a ten thousandths)), to the organic of animal
Body is a kind of safe gas, and on the other hand, under this low concentration, still having makes micro- lifes such as bacterium/fungi/virus
The facts such as the effect or smelly eliminating effect of thing inactivation.Due to such characteristic it is therefore, in chlorine dioxide, i.e., in the depollution of environment or food
In the purposes such as deodorization, sterilization, viral, the mould proof, anti-corrosion of removal when product convey, especially attract attention.
As described above, chlorine dioxide, the live body to animal is safe at low concentrations, therefore can be used for variety of applications.
For example, a kind of existing chlorine dioxide using low concentration is so that the motion of the method for the desactivation such as respiration system virus so far
(for example, patent document 1).However, because chlorine dioxide may be harmful to the live body of animal in higher concentrations, and also have blast
Danger it is therefore, in order to which towards practical, someone can make chlorine dioxide stably caused method in research and development.
From in the past, it is known that such as titanium dioxide can be produced whereby to acid adding in the chlorite of the chlorite aqueous solution or solid
The method of chlorine, however, when adopting this method, it is difficult to control reaction, usually because of environment or the condition of institute's acid adding, and have unexpected meeting
Produce the situation of the chlorine dioxide of high concentration.
Then, someone's motion irradiates ultraviolet to the gel-form composition as formed by chlorite and water-absorbing resins, borrows
To produce the method for chlorine dioxide (for example, patent document 2) or use through making to be impregnated with chlorite and alkalescence in porous carrier
Agent, and the stabilizing chlorine dioxide agent dried, make the stabilizing chlorine dioxide agent be in contact with air, so as to producing chlorine dioxide
Method (for example, patent document 3).
Prior art literature
Patent document
Patent document 1：WO/2007/061092；
Patent document 2：Japanese Unexamined Patent Publication 2005-224386 publications；
Patent document 3：Japanese Unexamined Patent Publication 2011-173758 publications.
The content of the invention
Invent the problem to be solved
The present inventor etc., in order to by so that in space floating it is microorganism deactivated for the purpose of and use chlorine dioxide side
Method is practical, and the method that can just stablize generation chlorine dioxide is repeatedly studied.As a result find, although patent document 2 or patent
Described method can control the generation of chlorine dioxide in document 3, but the generation efficiency that there are chlorine dioxide is bad, and be difficult to
The problem of chlorine dioxide of stable generation practicality amount.
Moreover, the present inventor etc. is investigated as the invention found out as described in Patent Document 2, in solid-state or gelatinous
The reason for chlorite is irradiated in the chlorine dioxide production method of the practice of ultraviolet, and the generation efficiency of chlorine dioxide is bad.Knot
Fruit has been surprisingly found that, when such as irradiating ultraviolet to the chloritic medicament containing solid-state, can not only produce chlorine dioxide, can also produce
Have ozone, and due to the ozone and the result of chlorine dioxide interference, the amount of chlorine dioxide caused by entirety can reduce (
It refer to the embodiment 1 and Fig. 3 of this case specification).
To the means to solve the problem
The present inventor etc. is according to above-mentioned gains in depth of comprehension, for will contain production of the chloritic composition of solid-state as chlorine dioxide
Source of students and the method used, for the purpose of increasing the amount of chlorine dioxide caused by entirety while the generation of ozone is suppressed,
Repeatedly studied again.As a result, do not use be once considered as from the chlorite of solid-state produce chlorine dioxide necessary to it is purple
Outside line, and use the light (luminous ray) of visibility region instead, the yield thus, it is possible to reduce ozone, while successfully by entirety
The yield of chlorine dioxide increases to the level of practicality.Also, it has been found that to compensate for because using the energy compared with ultraviolet
It is reactive low caused by the light of low visibility region, pass through mixed metal catalyst or metal oxide oxidation catalyst
Agent, it becomes possible to increase the amount of chlorine dioxide caused by chlorite, complete the present invention finally.
That is, method of the invention is in an embodiment, and to make the microorganism deactivated method of the floating in space, it is wrapped
Contain,
(1)：Prepare to be carried with chloritic Porous material and (B) metallic catalyst or metal oxidation containing (A)
The step of solid-state pharmacy of thing catalyst,
Here, in the solid-state pharmacy, the matter of chlorite and the metallic catalyst or metal oxide catalyst
Amount is than being 1：0.04 to 0.8；
(2)：To the solid-state pharmacy, the step of irradiating visible ray；And
(3)：It will be supplied from chlorine dioxide caused by the solid-state pharmacy to space existing for floating Institute of Micro-biology
The step of.
In addition, the method for the present invention is in an embodiment：The step (3) is that " will be produced from the solid-state pharmacy
Chlorine dioxide, space existing for supply to floating Institute of Micro-biology, and by the chlorine dioxide gas concentration in the space,
Being made animal can survive but the step of the floating microorganism is by the concentration of inactivation ".
In addition, the method for the present invention is in an embodiment：The animal can survive but the floating microorganism will be lost
Concentration living is 0.00001ppm to 0.3ppm.
In addition, the method for the present invention is in an embodiment：In the step (3), by the space
When chlorine dioxide gas concentration is made 0.1ppm to 0.3ppm, then by the chlorine dioxide supply into the space when
Between, it is set to 0.5 minute to 480 minutes.
In addition, the method for the present invention is in an embodiment：The floating microorganism, it is thin for floating virus or floating
Bacterium.
In addition, the method for the present invention is in an embodiment：The ripple of the visible ray irradiated in the step (2)
It is long, it is 360nm to 450nm.
In addition, the method for the present invention is in an embodiment：The metallic catalyst or metal oxide catalyst,
It is from by palladium (Pd), rubidium (Rb), nickel (Ni), titanium (Ti) and titanium dioxide (TiO2) select in the group that is formed.
In addition, the method for the present invention is in an embodiment：The Porous material, be from by sepiolite, palygorskite,
Selected in the group that montmorillonite, silica gel, diatomite, zeolite and pearlite are formed, and the chlorite, it is from by Asia
Selected in the group that sodium chlorate, potassium chlorite, lithium chlorite, calcium chlorite and barium chlorite are formed.
In addition, the method for the present invention is in an embodiment：Described " being carried with chloritic Porous material ", it is
By making chlorite be impregnated in Porous material, then it is set to dry and obtain.
In addition, the method for the present invention is in an embodiment：The Porous material is also carried with alkaline agent.
In addition, the method for the present invention is in an embodiment：The alkaline agent, be from by sodium hydroxide, potassium hydroxide,
Selected in the group that lithium hydroxide, sodium carbonate, potassium carbonate and lithium carbonate are formed.
In addition, the method for the present invention is in an embodiment：Mole between the chlorite and the alkaline agent
Than 1：0.1 to 2.0.
In addition, the method for the present invention is in an embodiment：It is described " to be carried with the Porous of chlorite and alkaline agent
Material ", it is by making chlorite and alkaline agent, by being impregnated in Porous material simultaneously or in order, then makes its drying
And obtain.
In addition, the method for the present invention is in an embodiment：The moisture of the Porous material is 10 weight %
Below.
The method of the present invention, in other embodiment, to make the microorganism deactivated method of the floating in space；Including
(1)：The step of preparing the chlorine dioxide generation unit with following compositions,
The unit possesses medicament storage portion and at least two light source portion,
The light source portion is essentially used for producing the light as formed by the wavelength of visibility region,
In the medicament storage portion, harvesting has containing the chloritic medicament of solid-state,
In the medicament storage portion, in the way of air can move inside and out the medicament storage portion, tool
One or more opening portion is had,
Here, be present in the medicament of the medicament storage portion, by by from the light caused by the light source portion
Line is irradiated, and produces chlorine dioxide；And
(2)：It will supply to floating Institute of Micro-biology and deposit from chlorine dioxide generation chlorine dioxide caused by unit
Space the step of.
In addition, the method for the present invention is in an embodiment：The medicament storage portion and at least two light source portion match somebody with somebody
Set as one, and the medicament irradiation that at least two light source portion is at least received and kept from 2 directions to the medicament storage portion
Light.
In addition, the method for the present invention is in an embodiment：The wavelength of the light of the irradiation is 360nm to 450nm.
In addition, the method for the present invention is in an embodiment：The light source portion possesses electric light or chip.
In addition, the method for the present invention is in an embodiment：The chip, it is LED (light emitting
diode；Light emitting diode).
In addition, the method for the present invention is in an embodiment：The light source portion is the light that can by light break irradiate
Source portion.
In addition, the method for the present invention is in an embodiment：Contain (A) containing the chloritic medicament of the solid-state to carry
Hold chloritic Porous material and the medicament of (B) metallic catalyst or metal oxide catalyst.
In addition, the method for the present invention is in an embodiment：Described " being carried with chloritic Porous material ", it is
By making the chlorite aqueous solution be impregnated in Porous material, then it is set to dry and obtain.
In addition, the method for the present invention is in an embodiment：The metallic catalyst or metal oxide catalyst,
It is to be selected from the group being made up of palladium, rubidium, nickel, titanium and titanium dioxide.
In addition, the method for the present invention is in an embodiment：The Porous material, it is from sepiolite, palygorskite, illiteracy
Selected in the group that de- stone, silica gel, diatomite, zeolite and pearlite are formed, and the chlorite, it is from by sub- chlorine
Selected in the group that sour sodium, potassium chlorite, lithium chlorite, calcium chlorite and barium chlorite are formed.
In addition, the method for the present invention is in an embodiment：It is described in the medicament in the medicament storage portion
Chlorite and the metallic catalyst or the mass ratio of metal oxide catalyst, are 1：0.04 to 0.8.
In addition, the method for the present invention is in an embodiment：The Porous material is also carried with alkaline agent.
In addition, the method for the present invention is in an embodiment：The alkaline agent be from by sodium hydroxide, potassium hydroxide,
Selected in the group that lithium hydroxide, sodium carbonate, potassium carbonate and lithium carbonate are formed.
In addition, the method for the present invention is in an embodiment：The chlorite and the alkalescence in the medicament
Mol ratio between agent, it is 1：0.1 to 2.0.
In addition, the method for the present invention is in an embodiment：It is described " to be carried with the Porous of chlorite and alkaline agent
Material ", be by making chlorite and alkaline agent be impregnated in Porous material simultaneously or in order, then dry it and
.
In addition, the method for the present invention is in other embodiments：Use the dioxy possessed described in any of the above-described
Change chlorine generation and implement this method with the chlorine dioxide generation device of unit.
In addition, chlorine dioxide generation device used in the method for the present invention is in an embodiment：It is also equipped with blowing
Portion, the medicament for being received and kept to the medicament storage portion in the chlorine dioxide generation unit blow air.
In addition, chlorine dioxide generation device used in the method for the present invention is in an embodiment：The air supplying part
Be for from the outside of the chlorine dioxide generation device toward the electric fan of internal inspiration air, or, for from the dioxy
Change the inside of chlorine generation device toward the electric fan of outside release air.
In addition, chlorine dioxide generation device used in the method for the present invention is in an implementation state：The medicament is received
At least one side for being present in the medicament storage portion in the opening portion in portion is deposited, and in the air given from the air supplying part
At least a portion by being present in the opening portion of the side of the medicament storage portion, deliver to medicament.
In addition, chlorine dioxide generation device used in the method for the present invention is in an implementation state：The medicament is received
The relative humidity deposited in portion is maintained at 30 to 80%RH (relative humidity) by the air sent from the air supplying part.
By above-mentioned one or more feature of the invention, not lance is pressed technically according to the viewpoint of one of ordinary skill in the art
The arbitrarily combined person of shield mode, is also included within the scope of the present invention certainly.
The effect of invention
The method for such as using the present invention, then it can stably produce the chlorine dioxide of the amount of practicality.In addition, by adjusting
The amount light of irradiation, then it can easily adjust the yield of chlorine dioxide.Can be realized by this and other effects animal can be survived and
The chlorine dioxide for the concentration that floating microorganism can but inactivate is stably supplied into space.
Brief description of the drawings
Fig. 1 represents the longitudinal sectional drawing of the assembled chlorine dioxide generation unit containing the chloritic medicament of solid-state.
Fig. 2 represents the longitudinal sectional drawing of the chlorine dioxide generation device of assembled Fig. 1 chlorine dioxide generation unit.
Fig. 3 is in the case of to chloritic medicament irradiation light containing solid-state, is represented when changing irradiation light
Wavelength when, the curve map of the actual measurement value changes of chlorine dioxide concentration and ozone concentration in air.
Fig. 4 is in Fig. 3 chlorine dioxide concentration and the measured value of ozone concentration, represents the measured value of ultraviolet range
Average value, and the bar graph of the average value of the measured value of visibility region.
Fig. 5 is in the situation to the chloritic medicament irradiation light containing solid-state, is represented because mixed by medicament
The curve map of the change of chlorine dioxide yield caused by the shape of metallic catalyst or metal oxide catalyst.
Fig. 6 represents to make containing solid-state chlorite and metallic catalyst or metal oxide catalyst (titanium dioxide)
When ratio between chlorite and titanium dioxide in medicament changes, the change of chlorine dioxide yield.
Fig. 7 represents to contain solid-state chlorite and the medicine of metallic catalyst or metal oxide catalyst (titanium dioxide)
Relation between the content of titanium dioxide in agent, with the maximum by chlorine dioxide concentration caused by radiation of visible light.
Fig. 8 is represented to containing solid-state chlorite and metallic catalyst or metal oxide catalyst (titanium dioxide)
When medicament continues to irradiate for a long time visible ray, the change of chlorine dioxide yield.
Fig. 9 represents stereogram, top view and the side view of the chlorine dioxide generation unit of an embodiment of the invention
Figure.
Figure 10 represents the chlorine dioxide generation device of the assembled chlorine dioxide generation unit of an embodiment of the invention
Skeleton diagram.
Figure 11 represented in the chlorine dioxide generation unit of an of the invention embodiment, to the medicament in medicament storage portion,
Only from the situation of 1 light source portion (one side) irradiation light, and from the dioxy between the situation of 2 light source portion (two-sided) irradiation lights
Change the comparison of chlorine yield.
Figure 12 is represented in the chlorine dioxide generation unit of an embodiment of the invention, by the medicine in medicament storage portion
Agent, the only situation from 1 light source portion (one side) irradiation light, and between the situation of 2 light source portion (two-sided) irradiation lights
The figure that the ratio of chlorine dioxide yield is marked and drawed.Here, due to the situation from 2 light source portion (two-sided) irradiation lights, compared with
Only from the situation of 1 light source portion (one side) irradiation light, the yield of its chlorine dioxide will show more than 2 times events, to calculate
For the sake of the ratio of chlorine dioxide yield, the chlorine dioxide yield of the situation of one side irradiation, then using 2 times of values.
Figure 13 is illustrated in the chlorine dioxide generation unit of an embodiment of the invention, for (double from 2 light source portions
Face) irradiation light situation, it can be efficiently to medicament storage portion compared with the situation from 1 light source portion (one side) irradiation light
In medicament inject light figure.
Figure 14 is shown in the chlorine dioxide generation unit of an embodiment of the invention, as changed in medicament storage portion
During the situation of relative humidity, the change of chlorine dioxide yield.Here, in Figure 14, represent only to irradiate from 1 light source portion (one side)
The data of the situation of light.
Figure 15 is shown in the chlorine dioxide generation unit of an embodiment of the invention, such as changes the phase of medicament storage portion
During to the situation of humidity, the time dependent change of chlorine dioxide yield.Here, in Figure 15, represent to shine from 2 light source portions are (two-sided)
Penetrate the data of the situation of light.
Figure 16 is shown in the chlorine dioxide generation unit of an embodiment of the invention, such as to the medicine in medicament storage portion
Agent, during situation by intermittent mode irradiation light (two-sided) from 2 light source portions, the time dependent change of chlorine dioxide yield.
Here, in figure, represent for " 10 seconds/80 seconds " to irradiate beginning repeatedly 2 minutes be prolonged exposure light, and irradiate beginning 2 minutes with
After carry out circulate operation, i.e. irradiation light 10 seconds (LED is set to ON (opening)), and stop irradiation light and (set LED for 80 seconds
For OFF (pass)).Equally, in figure, represent for " 20 seconds/80 seconds " to irradiate beginning repeatedly 2 minutes are prolonged exposure light, and are irradiated
Circulate operation, i.e. irradiation light 20 seconds (LED is set to ON) are carried out after starting 2 minutes, and stop irradiation 80 seconds (will
LED is set to OFF), represent for " 30 seconds/80 seconds " to irradiate beginning repeatedly 2 minutes are prolonged exposure light, and irradiate and start 2 minutes
Circulate operation, i.e. irradiation light 30 seconds (LED is set to ON), and stop irradiation light and (be set to LED for 80 seconds are carried out later
OFF)。
Figure 17 represents using method of the invention the skeleton diagram for floating microorganism deactivated experiment so that in space.
Figure 18 represent by chlorine dioxide concentration be made 0.05ppmv (partper million by volume, million/
One volume) when, the change of the virus titer (virous titer) in the air of chamber (chamber).
When Figure 19 represents chlorine dioxide concentration being made 0.1ppmv, the change of the virus titer in the air of chamber.
When Figure 20 represents chlorine dioxide concentration being made 0.3ppmv, the change of the virus titer in the air of chamber.
When Figure 21 represents chlorine dioxide concentration being made 0.3ppmv, the change of the virus titer in the air of chamber.
Figure 22 represents the skeleton diagram of the experiment of embodiment 9.
Figure 23 represents the result of the experiment of embodiment 9.
Figure 24 represents the skeleton diagram of the experiment of embodiment 10.
Figure 25 represents the result of the experiment of embodiment 10.
Embodiment
The method of the present invention, it is in an embodiment, makes the microorganism deactivated method of the floating in space, there is provided a kind of
Including；
(1)：Prepare to be carried with chloritic Porous material and (B) metallic catalyst or metal oxidation containing (A)
The step of solid-state pharmacy of thing catalyst,
Here, in the solid-state pharmacy, the chlorite and the metallic catalyst or metal oxide oxidation catalyst
The mass ratio of agent is 1：0.04 to 0.8；
(2)：The step of luminous ray is irradiated to the solid-state pharmacy；And
(3)：It will be supplied from chlorine dioxide caused by the solid-state pharmacy to the step in space existing for floating Institute of Micro-biology
Suddenly.
The space of the present invention can be applicable, is not limited especially, and applicable can take blocking or open
Put any space of state.For example, when using the present invention, it can be inactivated due to microorganism can be floated by animal survival
Concentration supplies chlorine dioxide, so the present invention can be applied to the space where animal.More specifically, can be applied to
Living space (for example, household, office), medical treatment office is (for example, the waiting room of hospital, therapeutic room, office treatment, operating room, preceding
Room, Admissions), research institute's (for example, the research department of university, cup), the medical facility of disaster is (for example, disaster counter, account
Paulin), in communal facility (for example, railway station, airport, school), vehicle is (for example, private vehicle, bus, electric car, fly
Machine) in.
Floating microorganism in the method for the invention broadly refers to the microorganism that can be floated in above-mentioned space,
It can enumerate：Float virus, bacterioneuston, floating fungi.For floating virus, it can enumerate：Has tunicate disease
Malicious or acapsular virus, for example, varicella, herpes zoster virus, influenza virus (people, bird, pig etc.), herpes simplex disease
Poison, adenovirus, enterovirus, rhinovirus, HPV, Poxvirus, Coxsackie virus (RNA virus class
(Coxsackie virus), herpe simplex (herpes simplex virus), cytomegalovirus (cytomegalo
Virus (CMV)), Epstein-Barr virus (Epstein-Barr virus (IV types nerpes vinrus hominis)), adenovirus (adeno virus),
It is papillomavirus (Papilloma virus), the more nest white matter brain syndrome virus of progressive (JC virus), small DNA virus, B-mode
Hepatitis viruse (hepatitis B virus (HBV)), HCV (hepatitis C virus (HCV)), draw husky disease
Malicious (Lassa virus), feline rhinotracheitis virus (feline calici virus), norovirus (Noro virus), Sapporo
Viral (Sapo virus), coronavirus (corona virus) _, SARS virus, rubella virus, the scorching disease of popular parotid gland
Poison, measles virus, newborn child's airway infections virus, poliomyelitis virus, Coxsackie virus, Yi Ke enteroviruses (echo
Virus), Ma Buerke viruses, Ebola virus, yellow fever virus, the virus of this refined Viraceae, hydrophobin, respiratory tract intestines
The virus of road Viraceae, rotavirus, Human Immunodeficiency virus, the thermophilic T lymphoma virus of the mankind, ape and monkey immunological incompetence virus,
STLV (simlan T-cell leukemia virus, anthropoid cape T cell hyperleucocytosis syndrome virus) etc..In addition, to floating
For bacterium, it can enumerate：Gram-positive bacteria (Gram-positive bacteria) or Gram-negative bacteria (Gram-
Negative bacteria), such as：Staphylococcus aureus, MRSE, Pseudomonas aeruginosa, coliform, streptococcus, leaching
Bacterium, syphilis fungus, meningococcus, tulase, aciduric bacteria, Klebsiella pneumoniae (pneumobacillus) (kleb siella category), sand
It is door Salmonella, clostridium botulinum, proteus, bacillus pertussis, Sai Libai Salmonellas, V. parahaemolyticus, citric acid bacillus, acinetobacter calcoaceticus, curved
Curved bar bacterium, enterobacteria, branch protoplast, Chlamydia, clostruidium etc..Moreover, for floating fungi, can enumerate：Aspergillus
Category, tinea alba Pseudomonas, Malassezia, Mycotoruloides etc..
In the case of chlorine dioxide is supplied in using the method for the present invention to space, the chlorine dioxide in space is dense
Degree, is preferably made, although for example, animal can survive, floating microorganism is by the concentration of inactivation.In the present invention, though
Right animal can survive, but float microorganism and refer to the chlorine dioxide gas concentration of inactivation, for example, can be for 0.00001ppm extremely
0.3ppm, preferably 0.0001ppm to 0.3ppm, more preferably 0.001ppm to 0.3ppm, further preferably for 0.01ppm extremely
0.3ppm, most preferably 0.1ppm are to 0.3ppm.
Using the method for the present invention to supplying time of chlorine dioxide in space, there is no particular restriction, but also can be according to
The chlorine dioxide gas concentration that is supplied and suitably adjust the supplied time.For example, the chlorine dioxide gas concentration in air is made
, then still will not be problematic even in usually sustainable supply chlorine dioxide during into 0.00001ppm to 0.01ppm.When by space
Chlorine dioxide gas concentration when being made 0.01ppm to 0.1ppm, then the chlorine dioxide is preferably supplied into the time in space
It is set to 10 minutes to 480 minutes, is more preferably set to 15 minutes to 90 minutes, is further preferably set to 15 minutes to 60 minutes.In addition,
In the case of chlorine dioxide gas concentration in space is made into 0.1ppm to 0.3ppm, then preferably the chlorine dioxide is supplied
Time in space is set to 0.5 minute to 480 minutes, is more preferably set to 1 minute to 60 minutes, is further preferably set to 2 minutes to 15
Minute.
For the chlorite used in the method for the present invention, it can enumerate：Alkali metal chlorite or chlorous acid alkali
Earth metal salt.For alkali metal chlorite, it can enumerate：Sodium chlorite, potassium chlorite, lithium chlorite；And to chlorous acid alkali
For earth metal salt, then it can enumerate：Calcium chlorite, magnesium chlorite, barium chlorite.Wherein, from the point of view of easy obtain, preferably sub- chlorine
Sour sodium, potassium chlorite, and most preferably sodium chlorite.These chlorites can be used alone, such as and with two or more
It is harmless.
The present invention method used in Porous material, although can be used, for example, sepiolite, palygorskite, montmorillonite,
Silica gel, diatomite, zeolite, pearlite etc., but for the sake of not making chlorite decomposition, presented when it is suspended in water
Alkalescence, more preferably palygorskite and sepiolite, particularly preferably sepiolite.
In the method for the invention, although using chloritic Porous material is carried with, hold chlorite
It is not limited especially then in the method for Porous material.For example, " being carried with chloritic Porous material ", such as makes Asia
Chlorate aqueous solution is impregnated in Porous material, and makes its drying, you can is made." it is carried with chloritic Porous thing
The moisture content of matter ", preferably below 10 weight %, more preferably below 5 weight %.
Used in the method for the invention " being carried with chloritic Porous material ", although any grain can be used
Footpath, but average grain diameter is particularly suitable for using in 1mm to 3mm.
The average grain diameter of " being carried with chloritic Porous material " in the method for the invention, for example, available
Light microscope determines the particle diameter of " being carried with chloritic Porous material " used, and carries out statistical disposition to calculate
Average value and standard deviation calculate.
The chloritic concentration in " being carried with chloritic Porous material " used in the method for the present invention,
More than 1 weight % is effective, but because equivalent to severe toxicity, it is advantageous to 25 weights of more than 1 weight % if when more than 25 weight %
Below % is measured, more preferably more than 5 weight % below 20 weight %.
The metallic catalyst or metal oxide catalyst used in method as the present invention, can be enumerated：Palladium,
Rubidium, nickel, titanium, titanium dioxide.In these, particularly titanium dioxide is adapted to use.Here, titanium dioxide, only address be titanium oxide,
Or titanium dioxide.Metallic catalyst or metal oxide catalyst used in the present invention, powdery, granular can be used
Etc. a variety of forms, and from the sub- nitronic acid salt in medicament, with metallic catalyst or metal oxide catalyst formed by mixing ratio
Example, one of ordinary skill in the art can suitably select more preferably form.For example, metallic catalyst or metal oxygen in medicament
When the ratio of compound catalyst is more high, then granular metallic catalyst or metal oxide catalyst may be selected, and such as medicine
When the ratio of metallic catalyst or metal oxide catalyst in agent is more low, then may be selected powdery metallic catalyst or
Person's metal oxide catalyst, but it is not limited to these practices.
Moreover, in this specification, as the substantially standard of the size of " powdery " or " granular ", for example, powdery refer to it is flat
The solid content for the size that equal particle diameter is 0.01mm to 1mm, and the granular solid for referring to the size that average grain diameter is 1mm to 30mm
Matter, but it is not particularly limited to this.
In the method for the present invention in the medicament of solid-state used, chlorite and metallic catalyst or metal aoxidize
Mass ratio between thing catalyst can be chlorite：Metallic catalyst or metal oxide catalyst=1：0.04 to
0.8th, more preferably 1：0.07 to 0.6, more preferably 1：0.07 to 0.5.In medicament, as metallic catalyst or metal oxide are urged
The content of agent is more than 1 times of the situation higher than chlorite content, and metallic catalyst or metal oxide oxidation catalyst
The content of agent is any situation of the situation less than less than 0.04 times, the caused chlorine dioxide when irradiating luminous ray
Amount can reduce.
" being carried with chloritic Porous material " used is also capable of loading and carrying in the method for the present invention alkaline agent.
Alkaline agent in the method for the present invention used in the modulation of medicament used, it can use for example, sodium hydroxide, hydrogen
Potassium oxide, lithium hydroxide, cesium hydroxide, rubidium hydroxide, sodium carbonate, potassium carbonate, lithium carbonate, but can more preferably use hydroxide
Sodium.It is when it is held alkaline agent in " being carried with chloritic Porous material ", then used in the modulated present invention
Medicament pH, so as to improve the stability of medicament in itself, during suppressing not carrying out keeping of irradiation etc. of light need not
The release for the chlorine dioxide wanted.
The amount of the medicament used in the method for the present invention, with to chlorite (mol；Mole) to be more than 0.1 equivalent and
Be appropriate below 2.0 equivalents, preferably more than 0.1 equivalent and below 1.0 equivalents, more preferably more than 0.1 equivalent and 0.7 equivalent with
Under.When such as less than 0.1 equivalent, then the chlorite held still has the possibility of decomposition in normal temperature, and during more than 2.0 equivalent,
Although can improving stability, due to being difficult to produce chlorine dioxide, caused concentration can reduce, therefore improper.
When the medicament used in method of the invention is modulated, " being carried with chloritic Porous material " is set also to carry
The method for holding alkaline agent is not limited especially, can be used for example, make chlorite and alkaline agent, while or side in order
Formula, it is impregnated in the method after Porous material and dried.Moreover, in this specification, having makes Porous material, " spraying absorption "
Dried after the chlorite aqueous solution and/or alkaline agent, the practice so as to purpose composition is made, but in this specification, term " spray
Mist adsorbs ", it is contained in term " impregnation ".
The method of the present invention, in another embodiment, to make the microorganism deactivated method of the floating in space, there is provided one
The method that kind comprises the steps：
(1)：Preparation possesses the step of chlorine dioxide generation unit of following compositions,
The unit possesses：Medicament storage portion and at least two light source portion,
Light source portion light source substantially as formed by the wavelength of visibility region for generation,
In the medicament storage portion, harvesting has containing the chloritic medicament of solid-state,
In the medicament storage portion, by the side that can make movement of the air in the inside of the medicament storage portion and outside
Formula, possessing has one or more opening portion,
In this, it is present in the medicament of the inside of the medicament storage portion, by from institute caused by the light source portion
State light to be irradiated, produce chlorine dioxide；And
(2)：It will supply to floating Institute of Micro-biology and deposit from chlorine dioxide caused by the chlorine dioxide generation unit
Space the step of.
In the method for the present invention in chlorine dioxide generation unit used, possesses at least two light source portion (for example, 2
Individual, 3,4,5,6 or more light source portions), but the position relationship at least two light source portion, as long as can be to making
For chlorine dioxide generating source medicament at least from 2 directions (for example, 2,3,4,5,6 or more directions)
Irradiation light, then it is not limited especially.Preferably at least 2 light source portions, made using the medicament of the generating source as chlorine dioxide
Centered on, configure in symmetrical position.
In the present invention method used in light source, as long as can will be seen that region light with independent mode or comprising
The mode of visibility region and discharge, then can use known light source.Thus, the wavelength of light used from the method for the present invention,
The wavelength (360nm to 830nm) of the light source of visibility region is not only defined in, even if including the wavelength of ultraviolet range light
Even the light of the wavelength of (to 360nm) and infrared spectral range light (830nm rises).However, such as the wavelength by ultraviolet range
Light irradiation then easily produces the ozone as accessory substance, in addition, such as infrared spectral range when medicament chloritic containing solid-state
Wavelength light, then due to energy it is relatively low it is therefore, even if being irradiated in the chlorite containing solid-state, the amount of caused chlorine dioxide
Still it is less.Thus, light caused by the light source used in method of the invention, preferably substantially by the wavelength of visibility region
Light form.Light caused by light source used in the method for the present invention, optimal wavelength is 360nm to 450nm light, more excellent
The light that wavelength is 380nm to 450nm or 360nm to 430nm is selected, most preferably wavelength is 380nm to 430nm light.
In the case of whether the wavelength of light caused by light source substantially belongs in the range of specific wavelength region, such as
It known determining instrument can be used to determine from the wavelength or energy of light caused by light source to be confirmed.
Light source used in the method for the present invention, as long as the light of the wavelength of visibility region can be produced, i.e., do not add especially
To limit, but electric light (incandescent lamp, LED), chip, electric injection device of the light for for example producing visibility region etc. can be used, it is a variety of
Utensil.From the viewpoint of viewpoint from the directive property of light caused by light source and the miniaturization from device, preferably using chip
The light source of form.Due to the light source directivity relatively narrower of chip form it is therefore, light is not to spread, can to the object of irradiation with
High efficiency mode irradiation light, as a result, can lifting device chlorine dioxide generation efficiency.In addition, from restriction as caused by light source
The wavelength of light, in a manner of being set to the light without ultraviolet range or infrared spectral range from the viewpoint of, preferably as light source, and
Using the LED that can produce visible ray.Particularly, from the viewpoint of the miniaturization of device, and from the generation efficiency of chlorine dioxide
From the point of view of viewpoint, the light source used in the present invention, the LED chip of visible ray can be preferably produced.
In addition, the light source used in the method for the present invention, can be the light source of the intermittent mode irradiation light of energy.For example, this
Light source used in the method for invention, can be a kind of repeatedly after certain time irradiation light, certain time stops the photograph of light
The light source of the circulation for the mode penetrated.To make light not limited especially by the control method of the light source of intermittent mode irradiation
Fixed, art technology can arbitrarily be implemented using known method.That is, in the method for the present invention, solid-state pharmacy is irradiated
The step of visible ray, can be the step of irradiating visible ray by intermittent mode to solid-state pharmacy.
, can be with one in the method for the present invention between the light source portion of chlorine dioxide generation unit used and medicament storage portion
Body mode configures, and the mode that can also be separated configures, but to make light caused by light source portion efficiently irradiate medicament storage portion
Middle received and kept medicament, is preferably configured in a manner of integraty.Here, between light source portion and medicament storage portion, can be by inseparable
Form integraty mode configure or connect, can also separable form integraty mode configure or connect.Such as light source portion
It is the situation for configuring or being connected in a manner of separable form integraty with medicament storage portion, then medicament storage portion can be to exchange
Cassette.
Medicament storage portion used in the method for the present invention, as long as can possess by air internally and in the way of outside movement
There is one or more opening portion, be not then limited on its material or construction.For example, by the way that medicament storage portion is (special
That in medicament storage portion, the light from light source portion is by the face of direct irradiation) material be set to known photopermeability material, then
The illumination that can be irradiated light source portion is incident upon the medicament inside medicament storage portion.It is preferred that essence is made in the material of medicament storage portion
On can make the resin-made of visible transmission, thus can make to be unlikely to be absorbed by resin and expose to from light caused by light source portion
The medicament of the inside of medicament storage portion.In this specification, substantially refer to the resin that the light of the wavelength of visibility region passes through, example
Such as, can be the wavelength for making irradiated visibility region light through more than 80% resin or preferably make to be irradiated
Visibility region wavelength light transmission more than 90% resin, can also be the wavelength for more preferably making irradiated visibility region
Light transmission more than 95% resin.Specifically, in medicament storage portion, as the light from light source portion by direct irradiation face
It material, can use for example, acrylic acid system, vinyl chloride system, the material of polyester, but be not particularly limited to this.
In addition, for example, medicament storage portion can be by forming with will not the be scattered reticular lamina of sieve screen apertures of degree of harvesting thing.
If using such a composition, the air of the outside of medicament storage portion can just move inside and out medicament storage portion, from
And light caused by light source portion can be irradiated in the medicament of the inside of medicament storage portion by sieve screen apertures.
In addition, one or more opening portion of medicament storage portion used in the method for the present invention, also can be by gas permeability
Piece is covered.In this specification, " gas permeability piece " although refer to can make gas (for example, air, gas, moisture etc.) by,
Substantially the sheet structure that solid matter (for example, powdered substance, granular object) passes through is not made." gas permeability in the present invention
Piece ", can have substantially does not make the property that gas (for example, water droplet) passes through yet.The material of gas permeability piece in the present invention is not
It is limited, but can illustrates：By fiber by thermal mechanical either chemically operation and make after being binded or being entwined in blocks
The material of shape, by micro-porous film (film with the material in most very small holes) by independent mode or through multiple weights
The material of folded fitting, although or for non-porous matter but still can make gas or air, moisture (vapor) movement material, to height
The material for the painting cap-type that density textile is handled through applying the hydrophobic of strength, or the material that these combined materials are formed.
Moreover, specifically, as the gas permeability piece in the present invention, for example, can use：Non-woven fabrics (road bass (registration mark, by
Buddhist nun Supreme Being adds company system), AXTAR (registration mark, TORAY company systems) etc.), Gore-Tex (registration mark) or EXEPOL (registrations
Trade mark), Resins Corporation of Mitsubishi system：Gas permeability/penetrability of combined micro-porous polyolefin film and various non-woven fabrics etc./
The excellent material of water proofing property), ENTRANT E (registration mark, TORAY company systems) etc..Here, the gas permeability piece in the present invention,
For the sake of being easily installed on medicament storage portion, heat sealability (hot amalgamation) has been preferably provided with.
The shape or thickness of gas permeability piece used in medicament storage portion, as long as can be in medicament storage portion in the gas permeability piece
Border between internal and outside, realize " although gas or air, humidity can be made by not making big more than to a certain degree
Small object passes through " in the range of purpose, art technology arbitrarily can be selected suitably.For example, as being used as gas permeability piece
And use the situation of non-woven fabrics, then it can be used：The weight of non-woven fabrics unit area is 15 to 120g/m2(preferably 40 to 100g/m2、
More preferably 50 to 80g/m2), thickness be 0.1 to 1.0mm (preferably 0.2 to 0.5mm, more preferably 0.2 to 0.4mm).
The method of the present invention, also it can use the chlorine dioxide generation unit for possessing the present invention in an embodiment
Chlorine dioxide generation device is implemented.Chlorine dioxide generation device used, can also possess air supplying part use in the method for the present invention
The medicament received and kept in the medicament storage portion to chlorine dioxide generation unit send air.The air supplying part, available for from device
Outside taken toward inside into air, it can also be used to from inside the device toward outside release air.
In the method for the present invention in chlorine dioxide generation device used, for the medicament to being received and kept in medicament storage portion
The air supplying part of air is sent, can be such as fan or air exhauster (AIR PUMP), but preferred fan.Such as possessing has such a air-supply
Portion, then it can supply more air to the medicament of the inside of medicament storage portion.Due to having supplied more air to medicament, as a result
Contact frequency containing the chloritic medicament of solid-state and the moisture (vapor) in air increases, and the solid-state irradiated by light is sub-
Chlorate easily produces chlorine dioxide.
In the method for the present invention in chlorine dioxide generation device used, using the air sent from the air supplying part, i.e.,
Can be 30 to 80%RH (preferably 40 to 70%RH, more preferably 40 to 60%RH) by the regulation of relative humidity in medicament storage portion.
By being the scope by the regulation of relative humidity in medicament storage portion, the yield of chlorine dioxide can be made increase.
In addition, in chlorine dioxide generation device used in the method for the present invention, as being supplied into medicament storage portion
To other methods of the vapor in air, can also be used the hydrogenesis in air and the Peltier element (Po Er that gathers
Note effect (Peltier's effect)) (can also turn one's coat using vapor intrusion or produce condense Peltier element lack
Put and it is acted on the rising of temperature aspect.).
The control method of relative humidity, is not any limitation as especially in device, and art ordinary artisan can adopt
It is appropriately carried out with known techniques.For example, the hygrometer of measure humidity is set inside device body, while monitoring amount of moisture, one
Side adjusts the air output from air supplying part.Or the regulation of the hygroscopic capacity of Peltier element can also be used, it is relatively wet so as to controlling
Degree.
Further, since chlorine dioxide generation used in the method for the present invention is small-sized with unit, so also can be assembled
In not in the method for being produced as after grade, implementing in family's electrical article of main purpose the present invention of chlorine dioxide.For example, can be not yet
In family's electrical article for the purpose of the generation of chlorine dioxide etc., it is single to assemble chlorine dioxide generation used in the method for the present invention
Member, and chlorine dioxide is supplied, the method so as to implementing the present invention.For example, in heater unit machine, air-cooling system machine, sky
Chlorine dioxide generation unit used in the method for the present invention is assembled in the air-conditioning equipment of gas defecator, humidifier etc., then may be used
Promote by the effect of the wind discharged from air-conditioning equipment same caused by the chlorine dioxide in chlorine dioxide generation unit
When, chlorine dioxide can also be multiplied and be loaded in the wind discharged from air-conditioning equipment toward space and be effectively spread in space.
The term used in this specification, it is that the specific embodiment of explanation is used, and the non-limiting content of the invention
Intention.
In addition, term "comprising" used in this specification, for except the situation for substantially having different understanding on article unity and coherence in writing
In addition, expression there are the meaning of described item (component, step, key element or number etc.), it is not excluded that there are and removes
Item (component, step, key element or number etc.) beyond this.
As long as no the definition differed, whole terms as used herein (include technical terms and scientific words), have
The meaning same with the meaning understood extensively by those skilled in the art of the invention.Term as used herein, as long as without
Expressing has different definition, then should be interpreted that the meaning of the meaning with conformability with this specification and in corresponding technology field,
Without that should be idealized or be explained with the excessively formal meaning.
Sometimes embodiment of the invention illustrates the situation of book in reference view simultaneously, but such as with the feelings of schematic diagram
Shape, then for the sake of being clearly illustrated, showed sometimes in a manner of being exaggerated.
In this specification, for example, the situation showed in the way of " 1 to 10% ", one of ordinary skill in the art will manage
Solve and represented for the manifestation mode by 1,2,3,4,5,6,7,8,9 or 10% by indivedual concrete modes.
In this specification, all numerical value used in expression composition content or number range, except non-specifically being expressed, with bag
Mode including the meaning containing term " about " is explained.For example, " 10 times ", except non-specifically being expressed, it will be appreciated that represented " about to refer to
10 times " the meaning.
Cited document, all enlightenments that should be regarded as these are applied in this specification in this specification, and affiliated
The art personnel then article unity and coherence in writing according to this specification, and under without departing from the spirit or scope of the invention, will be described existing
There are related enlightenment content, as part of this specification in technical literature to be quoted and understood.
Hereinafter, will be with reference to embodiment, to be illustrated the present invention in more detail.However, the present invention can by a variety of forms and
It is subject to specific manifestation, non-explanation is only to be defined in embodiment described herein.
[embodiment]
Embodiment 1：The change of chlorine dioxide yield caused by the wavelength of the light irradiated
In the present embodiment, use chlorine dioxide generation unit described in Fig. 1 and Fig. 2 and chlorine dioxide generation device with
Tested.
Fig. 1 is shown in the medicament storage portion of chlorine dioxide generation unit used in the present embodiment and the inside in light source portion
The profilograph of construction.As shown in figure 1, chlorine dioxide, which produces, uses unit 10, possess medicament storage portion 11 and produce visible ray
Light source portion (LED chip 12 and operation substrate 13).Medicament storage portion 11, contain experiment medicament 14.Medicament storage portion 11, by sky
The mode that gas can move inside and out, possessing has opening portion 16.Chlorine dioxide produces and uses unit 10, possesses and is used for device
Outside air is directed to the flexible pipe 15 in device.
Air through being imported from flexible pipe 15, after by opening portion 16, it is supplied in the inside of medicament storage portion 11.Supplied
Contained vapor, then absorbed by the chlorite in experiment medication agent 14 in the air given.From can caused by light source portion
See light, behind the bottom surface by medicament storage portion 11, the experiment medicament 14 present in the inside of medicament storage portion 11 will be irradiated in.
Chlorite containing vapor, then with after the light reaction irradiated, producing chlorine dioxide.With being contained in experiment together with chlorite
With the titanium dioxide in medicament 14, by by radiation of visible light, promote to produce chlorine dioxide from chlorite.Caused dioxy
Change chlorine, then by opening portion 16 after, be discharged to outside.
Fig. 2 is shown in the profilograph of all constructions of chlorine dioxide generation device used in the present embodiment.Such as Fig. 2 institutes
Show, chlorine dioxide generation device 20 internally possess chlorine dioxide generation unit 21.The device of chlorine dioxide generation device 20
Body 22 possesses：For by the air supply mouth 23 inside the air unit outside device and for by inside device
Air outlet 25 outside air removal unit.Then it is effectively to import air in device moreover, chlorine dioxide generation device 20
For the sake of inside, possesses fan 24 in inside.
By the driving of fan 24, air is directed into the inside of device body 22 from air supply mouth 23.Imported
Air, then it is discharged by the chlorine dioxide generation set by device inside with after unit 21 from air outlet 25.In dioxy
Change chlorine to produce with unit 21, due to producing the event of chlorine dioxide in the mechanism same with the device that Fig. 1 is recorded, discharged from air
Contain chlorine dioxide in the air that mouth 25 is discharged.
10wt% sodium chlorite aqueous solutions 70g is sprayed after being adsorbed in 100g sepiolite and drying it, then suction of spraying
Attached 10wt% sodium hydrate aqueous solutions 20g simultaneously makes its drying.It is mixed and handles modulated powder through implementing to burn till to titanium powder
The titanium dioxide 20g of shape, as the experiment medicament used in the present embodiment.
In medicament storage portion in the chlorine dioxide generation device described in Fig. 2, above-mentioned medicament is stored.From medicine
The opening portion of agent storage portion, by 1L/min speed to importing air in medicament storage portion, and from LED chip to medicament storage portion
Interior medicament irradiation light.The wavelength for the light for making to be irradiated from LED chip is only changed from 80nm to 430nm by every 2nm, to survey
Contained chlorine dioxide concentration and ozone concentration in the fixed air discharged from chlorine dioxide generation device.Moreover, the present embodiment,
Chlorine dioxide generation device is accommodated in about 7 liters of chamber and carried out, and chlorine dioxide concentration and the measure of ozone concentration pass through
Determine the chlorine dioxide concentration in the chamber and ozone concentration and implement.It the results are shown in Fig. 3 and Fig. 4.Moreover, in this
In experiment, use：Frequency counter (MCA3000, Tektronix company), spectrum analyzer (BSA, Agilent
Technologies companies), wavelength sweep light source (TSL-510, suntech company), ultraviolet accumulated light meter (UIT-250,
USHIO Motor Corporations), and ultraviolet accumulated light meter light-receiving device (VUV-S172, UVD-C405, USHIO Motor Corporation).
Fig. 3, the chlorine dioxide concentration and the curve of the measured value of ozone concentration being shown in the wavelength of a variety of light, air
Figure, Fig. 4, be in said determination value, will be in the average value of the measured value of ultraviolet range (80nm to 358nm), and in visible
The average value of the measured value in region (360nm to 430nm), the chart being compared.Here, in Fig. 4, in ultraviolet range and
The average value of the measured value of chlorine dioxide in visibility region be respectively about 2.25ppm, about 4.87ppm, and ultraviolet range and
The average value of the measured value of ozone in visibility region is respectively about 7.04ppm, about 3.04ppm.
As shown in figure 3, display such as make to be irradiated in the wavelength of medicament from ultraviolet range toward visibility region gradually move when, then
Ozone concentration in air turns into maximum in ultraviolet range, and the feelings gradually decreased from ultraviolet range toward visibility region
Condition.On the other hand, be worth surprisingly, there is the chlorine dioxide concentration in air, from ultraviolet range toward visibility region have by
Situation about gradually rising.From this result, one of ordinary skill in the art can be appreciated that：It is adapted to the scope of wavelength used in the present invention,
Though surmount the 430nm of the upper limit for the measurement range for belonging to the present embodiment, for example, still can under at least 450nm or so wavelength
Use without problems.
Moreover, as shown in Figure 4, the ozone concentration and two being such as compared in the air in ultraviolet range and visibility region
When aoxidizing each average value of cl concn, then understanding, ozone concentration is gradually reduced to about 43% from ultraviolet range toward visibility region,
In contrast, chlorine dioxide concentration then gradually rises up to about 213% from ultraviolet range toward visibility region.
That is, learning such as can to the irradiation of the mixture of solid-state chlorite and metallic catalyst or metal oxide catalyst
When seeing light, then compared to the situation for the light for irradiating ultraviolet range, chlorine dioxide can be produced in a manner of very effective.
Embodiment 2：The change of chlorine dioxide yield caused by the shape of catalyst
The sample 1 used in the present embodiment, (modulated two are handled through titanium is burnt till except granular titanium dioxide is used
Titanium oxide) beyond, remaining is then according to method similarly to Example 1 to modulate medicament.Reagent 2 and reagent used in the present embodiment
3, then modulate medicament according to method similarly to Example 1.
The medicament (sample 1 to 3) that the above method is modulated, it is separately stored in chlorine dioxide described in embodiment 1
The medicament storage portion of generation device.For sample 1 and sample 2, then 1L/min speed is pressed from the opening portion of medicament storage portion
Air is imported in toward device, and 405nm light is irradiated from the LED chip in light source portion.For sample 3, then from medicament storage portion
Speed of the opening portion only by 1L/min toward air is imported in device, have no irradiation light.To after 11 hours since irradiation, from
Contained chlorine dioxide concentration is determined in the air that device is discharged.By each measurement result of sample 1 to 3, Fig. 5 is shown in
In.
As shown in figure 5, such as mixing the situation (sample 1) of granular titanium dioxide in medicament, then learn compared to medicament
The situation (sample 2) of the titanium dioxide of middle mixing powdery, the more effective mode of energy produce chlorine dioxide.
Embodiment 3：About the investigation to the containing ratio between the chlorite and titanium dioxide in medicament
10wt% sodium chlorite aqueous solutions 70g is sprayed after being adsorbed in 100g foaming stone and drying, then absorption of spraying
10wt% sodium hydrate aqueous solutions 20g and drying.On the other hand, powdered titanium dioxide is mixed in the way of addition is changed,
As experiment medicament used in the present embodiment.Irradiation to the visible ray of experiment medicament, then by similarly to Example 1
Chlorine dioxide generation device and illuminating method carry out, and the measure of chlorine dioxide concentration, also mode is entered similarly to Example 1
OK.
When Fig. 6 represents the rate of change between chlorite and titanium dioxide in the tissue through making the present invention, titanium dioxide
The figure of the change of chlorine yield.By the content (wt%) of the titanium dioxide in the medicament shown in Fig. 6, and the sub- chlorine in medicament
Mass ratio between hydrochlorate and titanium dioxide, and contained chlorine dioxide in the air after radiation of visible light starts 1 hour
Relation between concentration (ppm), is shown in table 1.In addition, Fig. 7 represent the present invention medicament in content of titanium dioxide, with by means of
Relation between the maximum of chlorine dioxide concentration as caused by radiation of visible light.
[table 1]
| Content of titanium dioxide | Chlorite: titanium dioxide | Chlorine dioxide concentration in air |
| 0wt% | 1∶0 | 1.3ppm |
| 0.5wt% | 1∶0.04 | 1.6ppm |
| 1wt% | 1∶0.09 | 3.3ppm |
| 2wt% | 1∶0.17 | 3.8ppm |
| 3wt% | 1∶0.26 | 4.2ppm |
| 5wt% | 1∶0.43 | 3.3ppm |
| 7wt% | 1∶0.60 | 2.3ppm |
| 9wt% | 1∶0.77 | 2.0ppm |
| 11wt% | 1∶0.94 | 0.80ppm |
| 13wt% | 1∶1.11 | 0.55ppm |
| 21wt% | 1∶1.79 | 0.30ppm |
As shown in Fig. 6, Fig. 7, table 1, the caused chlorine dioxide when irradiating visible ray to experiment medicament is shown
Amount, rise as the mass ratio relative to the chloritic titanium dioxide in medicament from 0 to about 0.3 increases, and as relatively
Situation about will then be reduced insensibly when the mass ratio of chloritic titanium dioxide is more than about 0.3.Further, in composition
Relatively chloritic titanium dioxide mass ratio be more than about 1.0 when compared to the unmixed situation for having titanium dioxide, dioxy
Changing the yield of chlorine can reduce.
Fig. 8 by the experiment to the present embodiment with medicament long-time Continuous irradiation visible ray in the case of, chlorine dioxide produce
The figure of the change of amount.As shown in figure 8, even across the situation of long-time observation, it is still confirmed with being tied shown in Fig. 6 or Fig. 7
Fruit is similar, will be such as made in experiment with the blending ratio of the chlorite in medicament and titanium dioxide (mass ratio), 1: 0.04 to
0.8 (more preferably 1: 0.07 to 0.6, more preferably 1：0.07 to 0.5), the situation phase with being made blending ratio during scope in addition
Compare, more the chlorine dioxide of high concentration can stably be continued to discharge.
Embodiment 4：With regard to the investigation of the sandwich structure in light source portion
Implement the experiment of the validity of the sandwich structure in the light source portion of the present invention.In the present embodiment, using being remembered in Fig. 9
The dioxy salt dissolving generation of load is with dioxy salt dissolving generation device described in unit and Figure 10 to be tested.
Fig. 9 represents that the chlorine dioxide of an embodiment of the invention produces the in-built figure with unit 30.Such as Fig. 9 institutes
Show, chlorine dioxide of the invention produces and uses unit 30, possesses light source portion (electric substrate caused by medicament storage portion 32 and visible ray
33 and LED chip 34).Medicament storage portion 32 contains contains the chloritic medicament of solid-state in inside.Medicament storage portion 32 is by sky
The mode that gas can move inside and out, possesses opening portion (gas produces mouth 31, air induction port 36).
The air imported from air introduction part 36, the inside of medicament storage portion 32 will be supplied in.The air supplied
In contained vapor, then absorbed by the experiment medicament received and kept in medicament storage portion 32.From can caused by light source portion
See the light in region, by the externally mounted part 35 of medicament storage portion 32, be irradiated in the medicament that the inside of medicament storage portion 32 is received and kept.Contain
There is the experiment medicament of vapor, reacted with institute irradiation light, and produce chlorine dioxide.Caused chlorine dioxide, then lead to
Gas is crossed to produce mouth 31 and discharge to outside.
In Figure 10 expressions embodiment of the invention, the in-built figure of chlorine dioxide generation device 40.Such as Figure 10 institutes
Show, chlorine dioxide generation device 40 of the invention internally possess the chlorine dioxide generation unit of an embodiment of the invention
(LED chip device substrate 41 and medicament storage portion 42).Chlorine dioxide generation device 40 internally possesses Air Blast fan 44 again, and
By the driving of Air Blast fan 44, and to supply air inside chlorine dioxide generation unit.By the driving of Air Blast fan 44,
The relative humidity in medicament storage portion in adjustable chlorine dioxide generation unit.
By the driving of Air Blast fan 44, from the air induction port of chlorine dioxide generation unit toward medicament storage portion in
Portion supplies air.Contained vapor is absorbed by the experiment medicament received and kept in medicament storage portion in the air supplied.
The externally mounted part of medicament storage portion is passed through from the light of visibility region caused by light source portion, the inside for being irradiated in medicament storage portion is received
The medicament deposited.Experiment medicament containing vapor, reacts, and produce chlorine dioxide with the light irradiated.Caused two
Chlorine monoxid, then mouth is produced by gas to be discharged toward outside.
After 10wt% sodium chlorite aqueous solutions 70g sprayings is adsorbed in 100g sepiolite and drying, then make 10wt%
Sodium hydrate aqueous solution 20g sprayings are adsorbed and dried.On the other hand, the titanium dioxide about 1.8g of mixing powdery, and be made in this implementation
Experiment medicament used in example.The experiment medicament that will be modulated, receive and keep in the chlorine dioxide generation unit described in Fig. 9
Medicament storage portion, and from the light source portion in 2 faces (be respectively 100mm2) irradiation visible ray.This experiment is in 1m3Chamber in carry out, and
Temperature in chamber is about 26 DEG C, and relative humidity is about 40%.In comparative example, then remove by the light source portion of 1 face (one side) with for
Beyond the irradiation of visible ray, remaining is then same with embodiment to be tested.
The result that the chlorine dioxide concentration in chamber changes with time will be determined in embodiment and comparative example, represented
In Figure 11.In addition, by each time since irradiation, the ratio of the chlorine dioxide concentration in chamber in embodiment and comparative example
Value, is shown in Figure 12.Moreover, in Figure 12, in the situation from 2 light source portion (two-sided) irradiation lights, compared to only from 1 light source
During portion (one side) irradiation light, because the yield of chlorine dioxide will be displayed as more than 2 times events, to calculate chlorine dioxide yield
Ratio used in one side irradiation situation chlorine dioxide yield, then using 2 times value.
As shown in FIG. 11 and 12, in irradiation visible ray (two-sided) from 2 light source portions, it is worth surprised, compared to only
From the situation of 1 light source portion (one side) irradiation visible ray, will be turned into by showing the yield of chlorine dioxide by more than 2 times.Moreover, as schemed
Shown in 12, relative to the chlorine dioxide yield in comparative example, the ratio of the chlorine dioxide yield in embodiment, display that
Process over time and situation about more rising.
Above-mentioned result, it can be illustrated by Figure 13.That is, because luminous intensity is will be by index side when light is by medium
Formula reduces event, and the only irradiation by one side, then light is difficult to reach inside medicament or the inside, so that being difficult to all to medicament efficient
Mode irradiation light.But by medicament from 2 direction (or more than 2 directions) irradiation lights, then required for reacting
The light of amount is supplied to medicament, and chlorine dioxide is produced in a cost-effective manner with enable.
Embodiment 5：With regard to the investigation of the relative humidity of medicament storage portion
Using the chlorine dioxide generation device described in the chlorine dioxide generation unit and Figure 10 described in Fig. 9, to grind
Beg for the change with regard to the chlorine dioxide yield caused by the relative humidity in medicament storage portion.
With regard to receiving and keeping in the medicament of medicament storage portion, it is seen that the illuminating method of light, and the measure of chlorine dioxide concentration, then adopt
With condition similarly to Example 4.Using the driving of Air Blast fan to control the amount of the air supplied to medicament storage portion (also
That is, the amount of the vapor supplied to medicament), the relative humidity in regulating agent storage portion.Will be relative in medicament storage portion
The relation between chlorine dioxide concentration in humidity, with chamber is shown in Figure 14 and Figure 15.Figure 14 is represented will be from 0.5 hour to 2
The chlorine dioxide concentration determined for several times in the light irradiation of hour is subject to average value and its standard deviation, and Figure 15 is then represented in chamber
Chlorine dioxide concentration time dependent change.
As shown in figure 14, represent such as by the regulation of relative humidity in medicament storage portion for 30 to 80%RH (more preferably 50 to
70%RH, more preferably 40 to 60%RH), then the fact that can make the yield increase of chlorine dioxide.In addition, it is believed that：Such as medicament
When relative humidity in storage portion turns into less than 30%, then the moisture meeting required for the reaction for producing chlorine dioxide from chlorite
Deficiency, when turning into more than 80% such as relative humidity, then by chlorine dioxide will be dissolved in event in condensed water, as gas
The amount of the chlorine dioxide disengaged can be reduced.
In addition, as shown in figure 15, the relative humidity in medicament storage portion is such as made 30 to 80%RH (more preferably 40 to
70%RH, more preferably 40 to 60%RH), then the situation compared to relative humidity below 30%, although cross since irradiation with
The time come, it is height that still can maintain discharged chlorine dioxide concentration.Moreover, even if relative humidity is made to 20% feelings
Shape, the reason for chlorine dioxide concentration at irradiation beginning initial stage still raises, may be irradiation beginning medicament contained in itself
The event of moisture to a certain degree.
Embodiment 6：With regard to the investigation of the serviceability of intermittent irradiation
Using chlorine dioxide generation unit described in Fig. 9, to carry out the intermittence of the visible ray in the just present invention
The investigation of the serviceability of irradiation.
The medicament that medicament storage portion is deposited, and, for the measure of chlorine dioxide concentration, then use and embodiment 4
Similarity condition.The intermittent irradiation of visible ray from light source portion, by LED ON (opening)/OFF (pass) switching, and replace
The irradiation and stopping for carrying out visible ray are implemented.Specifically, by the condition of following (1) to (3), intermittent irradiation is carried out.
(1) irradiation for 2 minutes lasting lights that irradiation starts, after irradiation starts 2 minutes, then repeatedly：Irradiation light 10 seconds
After (LED ON), stop the circulation of the irradiation 80 seconds (LED OFF) of light.
(2) irradiation for 2 minutes lasting lights that irradiation starts, after irradiation starts 2 minutes, then repeatedly：Irradiation light 20 seconds
After (LED ON), stop the circulation of the irradiation 80 seconds (LED OFF) of light.
(3) irradiation for 2 minutes lasting lights that irradiation starts, after irradiation starts 2 minutes, then repeatedly：Irradiation light 30 seconds
After (LED ON), stop the circulation of the irradiation 80 seconds (LED OFF) of light.
The result of this experiment is shown in Figure 16.Moreover, in Figure 16 curve map " with respect to ClO2Gas concentration ", represent
During irradiating the chlorine dioxide concentration after starting 2 minutes as 1, the relative value of the chlorine dioxide concentration among each time.
As shown in figure 16, in the present invention, visible ray is intermittently irradiated by from light source portion, and adjusts intermittence photograph
It the irradiation time and the result of the balance of dwell time hit, can produce the chlorine dioxide of desired concentration.
In addition, in the present invention, visible ray is intermittently irradiated by from light source portion, can prevent that terminating in irradiation beginning works as initial stage
The chlorine dioxide of middle release higher concentration.Such as from light source portion Continuous irradiation visible ray when (that is, do not implement the feelings of intermittent irradiation
Shape), then as such as Fig. 6 curve map, chlorine dioxide, which produces concentration, among irradiation beginning initial stage turns into maximum, and thereafter by
Degradation subtracts.That is, in the present invention, by implementation from light source portion intermittent irradiation visible ray, chlorine dioxide can more stably be discharged.
Moreover, in the nature of things, such as from light source portion intermittent irradiation visible ray when, then compared to from light source portion Continuous irradiation
The situation of visible ray, the consumption for including the medicament including solid-state chlorite of the supply source as chlorine dioxide can be suppressed.
That is, when use can implement the light source of the intermittent irradiation of visible ray in the present invention, then chlorine dioxide generation unit can be extended
Life expectancy.
Embodiment 7：Use the inactivation (1) of the floating microorganism of chlorine dioxide generation device
To prove that the chlorine dioxide generation device of assembled chlorine dioxide generation unit of the invention can effective be
Make the floating in space microorganism deactivated, carry out following experiments.
1. experiment material and testing machines
(experiment virus)
Coliphage (Escherichia coli pHage) pHiX174 (NBRC 103405)
(Host Strains)
Escherichia coli(NBRC 13898)
(gas generation apparatus)
It is assembled with the chlorine dioxide generation device of the chlorine dioxide generation unit of the present invention
(experimental apparatus)
1m3Chamber (especially orders product)
14ml flexible pipes (Tube) (352059, FALCON)
Platinum loop (INO-001, IWAKI)
AC FAN (MU1225S-11, ORIX)
Sprayer (NE-C29, OMRON)
High-performance particulate air filtration machine (the special air filtration machine of exhaust microminiature, OSHITARI LABORATORY) is used in exhaust
Impact dust analyzer (Biosampler (biological sampling device), 5ml, SKC)
(laboratory apparatus)
Shaking table culture machine (AT12R, THOMAS)
Chlorine dioxide body sensor (ClO21000ppb, INTERSCAN)
Chlorine dioxide body sensor (Midas GAS Detector (Midas's gas detecting machine), ClO2MIDAS-E-
BR2, Honeywell)
Particulate tester (KC-52, RION)
Particulate removes and uses filter (MAC-11FR-UL, Japanese air technique society)
Spectrophotometer (V-560, JASCO)
Thermostat (MCO-175, SANYO)
Air pump (SPP-25GA, TECHNO TAKATSUKI)
Hygrothermograph (PC-5000TRH, SATO)
Chromatography of ions (HIC-20ASP, SHIMADZU)
(experiment material)
NB culture mediums (234000, Nutrient Broth, Difco)
702 culture mediums (poly- peptone 10g, yeast extract 2g, bitter salt 1g, distilled water 1L)
Common agar culture medium (E-MP21, Rong Yan chemistry system)
Agar (Bacto Agar 214010, BD)
2. experimental method
(modulation of experiment virus liquid)
By the preservation strain Escherichia coli previously cultivated (Escherichia coli), it is inoculated in 5ml NB+0.5%
In NaCl fluid nutrient mediums, by 30 DEG C, 200rpm, shaking table culture is carried out 6 hours.By the Escherichia coli after culture
(about 1 × 109Cell/ml) 100 μ l and bacteriophage green bacterium pHiX174 (pHage pHiX174) (about 1 × 105PFU/ml)in
After the μ l of NB+0.5%NaCl fluid nutrient mediums 500 are subject to mixing, cultivated 5 minutes at 37 DEG C.3ml NB is added in its mixed liquor
+ 0.5%NaCl culture mediums (0.6% agar (agar)) are simultaneously mixed, through with after common agar culture medium lamination,
37 DEG C are cultivated 18 hours.To surface agar addition 2ml NB+0.5%NaCl fluid nutrient mediums after reclaimed, will through with
After the fluid nutrient medium liquid relief of 0.22 μm of filter filtering, preserved at -85 DEG C.One part is implemented into spot inspection according to well-established law
It is fixed, and obtain about 1 × 1010PFU/ml virus liquid, by after making experiment so -85 DEG C of viruses freezed are melted, with distilled water
10 times of dilution, as experiment virus liquid (spray liquid；1×108 to 9PFU/ml)。
(experimental method)
By the outline of the experiment in the present embodiment, Figure 17 is shown in.
In 1m3The central portion of chamber sets the chlorine dioxide generation device of the present invention, utilizes timer one side control device
On, off while make its running, so as to the chlorine dioxide gas concentration in adjusting cavity room can turn into 0.05,0.1 or
0.3ppmv mode.In in the stable chamber of gas concentration, using sprayer, by pHiX174 phage virus (about 1 × 108 to 9PFU/ml) sprayed 5 minutes according to 0.2mL/min speed.In through making chlorine dioxide concentration be made in about 0.05ppmv chamber
0th, after 30,60,75,90 minutes, in through making chlorine dioxide concentration be made in about 0.1ppmv chamber at 0,15,30,45,60 point
Zhong Hou, in through making chlorine dioxide concentration be made in about 0.3ppmv chamber then after 0,5,10,15,30 minute, collected using impact
Dirt analyzer will contain virulent air and be reclaimed.The virus reclaimed is subjected to spot calibrating, so as to obtaining in air 10L
Viral number and evaluated.The same manner, by the LED of chlorine dioxide generation device it is normal when be set to OFF, make as a control group
With.
(monitoring of chlorine dioxide gas concentration)
By chlorine dioxide Sensor monitoring 1m3Chlorine dioxide gas concentration in chamber.Chlorine dioxide passes
The concentration value of sensor, then compared with by the gas concentration value calculated by the chromatography of ions after be corrected for.
3. result
By through being shown in the change of the virus titer in the air of chamber that chlorine dioxide concentration is made about 0.05ppmv
Figure 18, by through making the change of the virus titer in the air of chamber that chlorine dioxide concentration is made about 0.1ppmv be shown in Figure 19,
By through making the change of the virus titer in the air of chamber that chlorine dioxide concentration is made about 0.3ppmv be shown in Figure 20.Moreover,
Experiment shown in Figure 18, in temperature：23.1 ± 0.2 DEG C, relative humidity：Implement under conditions of 57.2 ± 0.4%, institute in Figure 19
The experiment shown, in temperature：22.9 ± 0.2 DEG C, relative humidity：Implement under conditions of 59.4 ± 0.7%, the reality shown in Figure 20
Test, in temperature：23.1 ± 0.3 DEG C, relative humidity：Implement under conditions of 59.3 ± 0.5%.
Such as by the present invention chlorine dioxide generation device LED it is normal when be made OFF control group situation, virus titer,
It was 1.5 × 10 at 75 minutes5PFU/10L (such as Figure 18), 45 minutes be 9.3 × 104PFU/10L (such as Figure 19), at 15 minutes it was
1.2×106PFU/10L (such as Figure 20).
On the other hand, the LED of chlorine dioxide generation device is made into its running by ON, and is making chlorine dioxide gas concentration
0.05ppmv situation is made, in exposure time 75 minutes, then virus titer turned into 8.3 × 102PFU/10L, compared with control group
(1.5×105PFU/10L 2log) is reduced10Above (more than 99%) (such as Figure 18).
Chlorine dioxide gas concentration is such as made to 0.08ppmv situation, in exposure time 45 minutes, then virus titer into
For 2.0 × 102PFU/10L, compared with control group (9.3 × 104PFU/10L it is) reduction 2log10Above (more than 99%) (such as Figure 19).
Chlorine dioxide gas concentration is such as made to 0.27ppm situation, in exposure time 15 minutes, then virus titer turned into
1.7×103PFU/10L, compared with control group (1.2 × 106PFU/10L 2log) is reduced10Above (more than 99%) (such as Figure 20).
Result above proves：Dress is produced by using the chlorine dioxide for the chlorine dioxide generation unit for being assembled with the present invention
Put, and to supply chlorine dioxide into space to concentration (0.3ppm below) of the mankind as safety, it can make in very short time
Floating in space is microorganism deactivated.And, it was demonstrated that：By using the two of the chlorine dioxide generation unit for being assembled with the present invention
Chlorine monoxid generation device, and with about 0.3ppm or so concentration to supplying chlorine dioxide in space, can be in very short time
(less than 15 minutes) make floating microorganism in space slightly fully desactivation.
4. investigate
Hereby have by the floating influenza virus number in the written portions of hospital emergency after measured of Bu Laijieli (Blachere) et al.
Report (Blachere, M.F., et.al.Measurement of airborne influenza virus in a
hospital emergency department.Clin.Infect.Dis.48,438-440(2009)).In the document, note
It is loaded with：Using the smog matter sampler (National of the graduate two sections of cyclones of Occupational spy safety and medical skill
Institute for Occupational Safty and Health 2-stage cyclone aerosol sampler),
By 3.5L/min, the air in the mode suction chamber of 4 hours, to determine the result of the influenza virus number in the presence of air,
Waiting room tests out 16,278 virion subnumbers.When such as calculating contained virus concentration in space from this result, then turn into about 1.9 ×
102Virion subnumber/10L.That is, in the high space of the how existing possibility of influenza virus (for example, influenza virus most patients come
The hospital of institute) in, the influenza virus concentration in space, it is believed that about 1.9 × 102Population/10L or so.
It is about 7.5 × 10 that this 0.05ppm chlorine dioxide, which exposes virus used in experiment to the open air,5PFU/10L, and
Although being about 3900 times of denseer conditions of virus concentration when compared with the example in above-mentioned hospital emergency portion, but still display fully obtains
Obtain viral Inactivation Effect.Thus, if the influenza virus concentration in space is about 1.9 × 102Virion subnumber/10L's or so
Situation, the then it is believed that mistake of virus can be carried out with the chlorine dioxide gas concentration of about 0.00001ppm (0.05ppm/3900) left and right
It is living.
Embodiment 8：Use the inactivation (2) of the floating microorganism of chlorine dioxide generation device
For prove the chlorine dioxide generation device of assembled chlorine dioxide generation unit of the invention can with it is extremely short when
Between (such as less than 10 minutes) make the floating in space microorganism deactivated, carry out following additional experiment.
1. experiment material and testing machines
Using same as Example 7.
2. experimental method
For testing the adjustment of virus liquid and the monitoring of chlorine dioxide gas concentration, using method same as Example 7.
(experimental method)
In 1m3The central portion of chamber sets the chlorine dioxide generation device of the present invention, while being filled using timer with controlling
On, off for putting can turn into about 0.3ppmv mode so as to the chlorine dioxide gas concentration in adjusting cavity room while make its running.
In in the stable chamber of gas concentration, using sprayer, by pHiX174 phage virus (about 1 × 108 to 9PFU/ml) with
0.2mL/min speed is sprayed 1 minute.After 0,2,4,6 minute, it will be contained using impact dust analyzer in from the spraying of virus
Virulent air is reclaimed.The virus reclaimed is subjected to spot calibrating, so as to obtaining the viral number in air 10L and adding
With evaluation.The same manner, by the LED of chlorine dioxide generation device it is normal when be set to OFF, use as a control group.
3. result
The OFF situation of control group, 1m are set to when the LED of the chlorine dioxide generation device of the present invention is normal3In chamber
Air 10L in virus titer, 2 minutes be 9.2 × 104PFU/10L, 4 minutes be 8.5 × 104PFU/10L, at 6 points
Clock is 6.3 × 104PFU/10L (Figure 21).
On the other hand, the LED of the chlorine dioxide generation device of the present invention is made into its running by ON, and is making chlorine dioxide
Gas concentration is made 0.28ppmv situation, the virus titer in air, then as exposure time 2 minutes be 1.6 × 104PFU/
10L, exposure time 4 minutes are 2.8 × 103PFU/10L, exposure time 6 minutes are 9.1 × 102PFU/10L and compared with control group,
82.9% (exposing to the open air for 2 minutes), 96.8% (exposing to the open air for 4 minutes), 98.6% (6 clocks point expose to the open air) (such as Figure 21) are reduced respectively.
Result more than, it is verified：By the titanium dioxide using the chlorine dioxide generation unit for being assembled with the present invention
Chlorine generation device, and to supply chlorine dioxide into space to concentration (0.3ppm below) of the mankind as safety, can be in pole
Make the floating microorganism desactivation in space in short time.
Embodiment 9：Use the inactivation (3) of the floating microorganism of chlorine dioxide generation device
To prove that the chlorine dioxide generation device of assembled chlorine dioxide generation unit of the invention can effective be
Make the microorganism deactivated chlorine dioxide generation device of a variety of floatings, carry out following experiments.
1. experiment material and testing machines
(experiment virus)
Cat family calicivirus (Feline Calicivirus) (FCV, F9, ATCC VR-782)；As replacing for norovirus
In generation, uses
(host cell)
Cat family herpesviral cat family kidney cell (Crandell Reesefeline kidney cells) (CRFK, ATCC
CCL-94)
(gas generation apparatus)
The chlorine dioxide generation device of assembled chlorine dioxide generation unit of the invention
(experimental apparatus)
The stainless steel chambers (especially ordering product) of 100L
96 hole micro-plates (353072, FALCON)
96 hole depth well disks (BM6030, BM Bio)
Reagent container (Reagent Reservoirs)/inclination basin (Tip-Tub) (022265806, eppendorf)
Ac fan (AC FAN) (MU825S-13N, ORIX)
Sprayer (NE-C29, OMRON)
High efficiency particulate air clarifier (the special air filter of air draft microminiature, OSHITARI are used in exhaust
LABORATORY)
Impact dust analyzer (Biosampler, 5ml, SKC)
Centriprep 50K milipore filters (4310, Merck Millipore)
Amicon Ultra 50K milipore filters (UFC505024, Merck Millipore)
(testing machines)
Shaking table culture machine (AT12R, THOMAS)
Chlorine dioxide body sensor (Midas GAS Detector, ClO2MIDAS-E-BR2, Honeywell)
Data logger (GL220, GRAPHTEC)
The grand timer (H5CX, OMRON) of ohm
Corpuscular counter (KC-52, RION)
CO2Constant Temperature and Humidity Chambers (MCO-175AICUVH, PANASONIC)
Air pump (SPP-25GA, TECHNO TAKATSUKI)
Hygrothermograph (TR-72wf, T＆D)
Chromatography of ions (HIC-20ASP, SHIMADZU)
Humidity regulator (ADPAC-N1000-AH, ADTEC)
Peace and quiet air feeder (ADFRESH-1000, ADTEC)
Humiture unit (TH-RS12, ADTEC)
Hygrothermograph (TR-72wf, T＆D CORPORATION)
Flowmeter (RK3300, KOFLOC)
Chromatography of ions art (ICS-3000, DIONEX)
Phase contrast microscope (CK30, OLYMPUS)
(experiment material)
Dulbecco is using a large amount glucose to improve the middle amount dextrose culture-medium (Dulbecco ' s of eagle
Modified Eagle ' s Medium-high glucose) (D-MEM, D5796, SIGMA)
Dulbecco phosphate buffered saline (Dulbecco ' s PHospHate Buffered Saline) (D8537,
SIGMA)
0.25% trypsin solution (Trypsin Solution) (35555-54, Nacalai tesque)
Hyclone (Fetal Bovine Serum) (FBS, 30-2020, ATCC)
EDTA (ethylenediamine tetra-acetic acid) disodium salt (Disodium Salt) 2% in DBS (phosphate buffered saline) salt solution
Solution (2820549, MP)
(impacting dust analyzer with viral recovered liquid (neutralizer))
The 0.1%FBS D-MEM (being added with antibiotic substance) that 1mm hypo solutions * (as explained) will be contained
5mL, the viral recovered liquid as impact dust analyzer.
Explain *：1mm hypo solutions, for when enable 0.3ppmv chlorine dioxide ventilate 12.5L when nothing ask
The concentration that topic ground neutralizes.
2. experimental method
(adjustment of viral spray liquid)
By the Feline calicivirus (10 of institute's freezen protective in -80 DEG C8.5TCID50/ 50 μ L) by 0.1%FBS
Solution is diluted 10 times, as viral spray liquid (107.5TCID50/50μL)。
(experimental method)
The chlorine dioxide generation device of the present invention is set in the central portion of 100L stainless steel chamber, and utilizes timing
Device, on, off of one side control device can be turned into the chlorine dioxide gas concentration adjusted in chamber while make its running
0.3ppmv mode (such as Figure 22).Sprayer is used in the chamber stablized to gas concentration, by cat family calicivirus
(107.5TCID50/ 50 μ L) sprayed 1 minute by 0.2mL/min speed, and after 0,2.5,5,10 minute, use impact dust
Analyzer and virus is reclaimed.5mL viral recovered liquid, then about 50 μ L are concentrated into (in air by 2 kinds of milipore filters
12.5L virus).Titre is determined from this viral concentration liquid, to obtain the viral infection valency in air 10L and be evaluated.Separately
Outside, as a control group, in the chlorine dioxide generation unit in chlorine dioxide generation device, medicine is not received and kept in medicament storage portion
Agent, carry out experiment similar to the above.
(chlorine dioxide gas concentration)
Utilize the chlorine dioxide gas concentration in chlorine dioxide Sensor monitoring 100L chambers.Chlorine dioxide passes
The concentration value of sensor, then with relatively and being corrected for according to the gas concentration value calculated by the chromatography of ions.
3. experimental result
In a device without using medicament control group situation, the virus titer after 10 minutes, be 104.0TCID50/ 10L is empty
Gas.On the other hand, to assembling the situation tested after medicament in the device of the present invention, the chlorine dioxide gas concentration in chamber
For average 0.25ppmv (minimum (min)；0.22ppmv, highest (max)；0.32ppmv), and the virus titer after 10 minutes then
As 100.6TCID50/ 10L air, and reduce 2log compared with control group10Above (more than 99%) (such as Figure 23).
Embodiment 10：Use the inactivation (4) of the floating microorganism of chlorine dioxide generation device
To prove that the chlorine dioxide generation device of assembled chlorine dioxide generation unit of the invention also can be effective
To inactivate bacterioneuston, following experiments are carried out.
1. experiment material and testing machines
(experiment microorganism)
MRSE (StapHylococcus epidermidis) (NBRC 12993)
(gas generation apparatus)
It is assembled with the chlorine dioxide generation device of the chlorine dioxide generation unit of the present invention
(experimental apparatus)
1m3Chamber (especially orders product)
Platinum loop (INO-001, IWAKI)
96 hole depth well disks (BM6030, BM Bio)
Reagent container/inclination basin (022265806, eppendorf)
Ac fan (MU1225S-11, ORIX)
Sprayer (NE-C29, OMRON)
High efficiency particulate air clarifier (the special peace and quiet film of exhaust microminiature, OSHITARI are used in exhaust
LABORATORY)
Impact dust analyzer (Biosampler, 5ml, SKC)
(testing machines)
Chlorine dioxide body sensor (Midas GAS Detector, ClO2MIDAS-E-BR2, Honeywell)
Corpuscular counter (KC-52, RION)
Particle removes and uses filter (MAC-11FR-UL, Japanese AIRTECH)
Spectrophotometer (V-560, JASCO)
Thermostat (MCO-175, SANYO)
Air pump (SPP-25GA, TECHNO TAKATSUKI)
Hygrothermograph (PC-5000TRH, SATO)
Flowmeter (RK3300, KOFLOC)
Chromatography of ions (HIC-20ASP, SHIMADZU)
(experiment material)
SCD culture mediums (393-00185, day water pharmacy)
SCD agars culture medium (396-00175, day water pharmacy)
Common agar culture medium (E-MP21, Rong Yan chemistry)
Pancreas casein soybean agar culture medium (236950, BD Biosciences)
0.1mol/l hypo solutions (191-03625, wako)
(impact dust analyzer floating bacterium recovered liquid (neutralizer))
1mm hypo solutions will be contained (as explained*) SCD culture medium 5mL, as impact dust analyzer
Float bacterium recovered liquid.
Explain *：1mm hypo solutions, for the nothing when enabling 0.05ppmv chlorine dioxide to pass through 12.5L
The concentration neutralized to problem.
2. experimental method
(adjustment of experiment bacterium solution)
The preservation bacterial strain MRSE (StapHylococcus epidermidis) cultivated is planted into bacterium in general
In logical agar culture medium, and cultivated at 30 DEG C.By through being used as test organisms using the thalline of sterilization purification water dilution gained
Liquid (spray liquid；1×108 to 9CFU/ml) use.
(experimental method)
In 1m3The central portion of chamber sets the chlorine dioxide generation device of the present invention, and utilizes timer, while control dress
On, off for putting are while make its running, (the figure in a manner of adjusting the chlorine dioxide gas concentration in chamber and can turn into 0.05ppmv
24).Sprayer is used in the chamber stablized to gas concentration, by bacterium suspension (about 1 × 108 to 9CFU/ml 0.2mL/min) is pressed
Speed spray 1 minute, and after 0,30,60,90 minute, floating bacterium is reclaimed using impact dust analyzer.Return
After receipts, the measure evaluation of the viable count of each time is carried out by dilution-plate method.As a control group, by the present invention dioxy
When the LED of change chlorine generation device maintains OFF, experiment similar to the above is carried out.
(chlorine dioxide gas concentration)
Utilize chlorine dioxide Sensor monitoring 1m3Chlorine dioxide gas concentration in chamber.Chlorine dioxide passes
The concentration value of sensor, then with relatively and being corrected for according to the gas concentration value calculated by the chromatography of ions.
3. experimental result
In the situation for lower the carried out control group that the LED in device is maintained to OFF, viable count, it was at 90 minutes
4.1×103CFU/10L air.On the other hand, in the situation that the LED of the device of the present invention is set into ON to be tested, chamber
Interior chlorine dioxide gas concentration is average 0.05ppmv, viable count then turns into 3.4 when exposure time is 90 minutes ×
102CFU/10L air, and reduce 1log compared with control group10Above (more than 90%) (Figure 25).
Symbol description
10 chlorine dioxide produce and use the medicament storage portion of unit 11
12 LED chips 13 operate basal disc
The flexible pipe of 14 medicament 15
The chlorine dioxide generation device of 16 opening portion 20
21 chlorine dioxide produce and use the device body of unit 22
The fan of 23 air supply mouth 24
The chlorine dioxide generation unit of 25 air outlet 30
31 gases produce the medicament storage portion of mouth 32
The LED chip of 33 electric substrate 34
The air induction port of 35 externally mounted part 36
The LED chip of 40 chlorine dioxide generation device 41 loads substrate
The frame of 42 medicament storage portion 43
44 Air Blast fans.
Claims (14)
1. a kind of make to float microorganism deactivated method in space, comprising：
(1)：Preparation is carried with chloritic Porous material and (B) metallic catalyst containing (A) or metal oxide is urged
The step of solid-state pharmacy of agent,
Here, in the solid-state pharmacy, chlorite and the metallic catalyst or the mass ratio of metal oxide catalyst
For 1：0.04 to 0.8；
(2)：The step of visible ray is irradiated to the solid-state pharmacy；And
(3)：The step of floating space existing for Institute of Micro-biology will be supplied from chlorine dioxide caused by the solid-state pharmacy.
2. the method according to claim 11, wherein,
The step (3)：By chlorine dioxide caused by the solid-state pharmacy, sky existing for supply floating Institute of Micro-biology
Between, and the chlorine dioxide gas concentration in the space is made to animal can survive but the floating microorganism is by the dense of inactivation
The step of spending.
3. the method according to claim 2, wherein,
The animal can be survived but the concentration of inactivation is 0.00001ppm to 0.3ppm by the floating microorganism.
4. the method according to claim 11, wherein,
In the step (3), when the chlorine dioxide gas concentration in the space is made into 0.1ppm to 0.3ppm, by described in
The time that chlorine dioxide is supplied in the space is set to 0.5 minute to 480 minutes.
5. method according to any one of claim 1 to 4, wherein,
The floating microorganism is floating virus or bacterioneuston.
6. method according to any one of claim 1 to 5, wherein,
The wavelength of the visible ray irradiated in the step (2) is 360nm to 450nm.
7. method according to any one of claim 1 to 6, wherein,
The metallic catalyst or metal oxide catalyst, are formed from by palladium, rubidium, nickel, titanium and titanium dioxide
Selected in group.
8. method according to any one of claim 1 to 7, wherein,
The Porous material, it is from by sepiolite, palygorskite, montmorillonite, silica gel, diatomite, zeolite and pearlite institute group
Into group in select,
And the chlorite, it is from by sodium chlorite, potassium chlorite, lithium chlorite, calcium chlorite and barium chlorite institute group
Into group in select.
9. method according to any one of claim 1 to 8, wherein,
Described to be carried with chloritic Porous material be by making chlorite be impregnated in Porous material, then makes it dry
It is dry and obtain.
10. method according to any one of claim 1 to 9, wherein,
The Porous material is also carried with alkaline agent.
11. the method according to claim 11, wherein,
The alkaline agent, it is from by sodium hydroxide, potassium hydroxide, lithium hydroxide, sodium carbonate, potassium carbonate and lithium carbonate institute group
Into group in select.
12. the method according to claim 10 or 11, wherein,
Mol ratio between the chlorite and the alkaline agent is 1：0.1 to 2.0.
13. the method according to any one of claim 10 to 12, wherein,
The Porous material for being carried with chlorite and alkaline agent, be by make chlorite and alkaline agent simultaneously or by
Order is impregnated in Porous material, then it is dried and is obtained.
14. the method according to any one of claim 1 to 13, wherein,
The moisture of the Porous material is below 10 weight %.
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2015113290 | 2015-06-03 | ||
| JP2015-113290 | 2015-06-03 | ||
| PCT/JP2016/065949 WO2016194884A1 (en) | 2015-06-03 | 2016-05-31 | Method for inactivating airborne microorganisms |
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| CN107530464A true CN107530464A (en) | 2018-01-02 |
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ID=57440464
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| CN201680028104.0A Pending CN107530464A (en) | 2015-06-03 | 2016-05-31 | Make the microorganism deactivated method of the floating in space |
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| Country | Link |
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| JP (1) | JP6725153B2 (en) |
| KR (1) | KR102534711B1 (en) |
| CN (1) | CN107530464A (en) |
| HK (1) | HK1245683A1 (en) |
| TW (1) | TWI754614B (en) |
| WO (1) | WO2016194884A1 (en) |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109701053A (en) * | 2018-12-26 | 2019-05-03 | 宁波大学 | Sterilization method |
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| PT3672405T (en) * | 2018-11-13 | 2020-11-04 | Csp Technologies Inc | Antimicrobial gas releasing agents and systems and methods for using the same |
| JP7464463B2 (en) | 2019-06-28 | 2024-04-09 | 日揮触媒化成株式会社 | Chlorine Compound Adsorbent |
| US20220339596A1 (en) * | 2019-10-01 | 2022-10-27 | Acenet Inc. | Method for producing radicals, method for sterilizing spores, and cancer treatment drug |
| WO2021224673A1 (en) * | 2020-05-05 | 2021-11-11 | CO2Apps S.R.L. | Substance and method for preventing the transmission of viruses in the respiratory system |
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| CN102834350A (en) * | 2010-03-26 | 2012-12-19 | 大幸药品株式会社 | Device for generating chlorine dioxide |
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| JP2005224386A (en) | 2004-02-12 | 2005-08-25 | Daiichi Seidenki Kk | Apparatus for chlorine dioxide gas sterilization |
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| JP5605744B2 (en) | 2010-02-25 | 2014-10-15 | ダイソー株式会社 | Stabilized chlorine dioxide agent and stable generation method of chlorine dioxide |
| CN102847181B (en) * | 2012-09-26 | 2014-05-28 | 深圳万和制药有限公司 | Product capable of delaying generation and releasing of chlorine dioxide and preparation method thereof |
| JP2015077268A (en) * | 2013-10-17 | 2015-04-23 | シャープ株式会社 | Deodorization method |
| EP3088355B1 (en) * | 2013-12-27 | 2019-10-02 | Taiko Pharmaceutical Co., Ltd. | Unit for chlorine dioxide generation and chlorine dioxide generation device |
-
2016
- 2016-05-30 TW TW105116846A patent/TWI754614B/en active
- 2016-05-31 KR KR1020177033260A patent/KR102534711B1/en active IP Right Grant
- 2016-05-31 WO PCT/JP2016/065949 patent/WO2016194884A1/en active Application Filing
- 2016-05-31 CN CN201680028104.0A patent/CN107530464A/en active Pending
- 2016-05-31 JP JP2017521944A patent/JP6725153B2/en active Active
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1355768A (en) * | 1999-05-18 | 2002-06-26 | 西南研究院 | Energy-activated compositions for controlled sustained release of gas |
| CN101316617A (en) * | 2005-11-28 | 2008-12-03 | 大幸药品株式会社 | Countermeasure against infection with floating virus |
| CN102834350A (en) * | 2010-03-26 | 2012-12-19 | 大幸药品株式会社 | Device for generating chlorine dioxide |
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| CN109701053A (en) * | 2018-12-26 | 2019-05-03 | 宁波大学 | Sterilization method |
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| WO2016194884A1 (en) | 2016-12-08 |
| TW201701906A (en) | 2017-01-16 |
| JP6725153B2 (en) | 2020-07-15 |
| JPWO2016194884A1 (en) | 2018-04-05 |
| KR102534711B1 (en) | 2023-05-19 |
| HK1245683A1 (en) | 2018-08-31 |
| KR20180015624A (en) | 2018-02-13 |
| TWI754614B (en) | 2022-02-11 |
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