CN108855061B - Laminated film photocatalyst for photocatalytic gas purification, preparation method and application - Google Patents
Laminated film photocatalyst for photocatalytic gas purification, preparation method and application Download PDFInfo
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- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/48—Silver or gold
- B01J23/52—Gold
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8678—Removing components of undefined structure
- B01D53/8687—Organic components
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/72—Copper
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- 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
- B01J35/39—Photocatalytic properties
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2255/00—Catalysts
- B01D2255/80—Type of catalytic reaction
- B01D2255/802—Photocatalytic
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/708—Volatile organic compounds V.O.C.'s
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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- Chemical Kinetics & Catalysis (AREA)
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- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
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- General Chemical & Material Sciences (AREA)
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Abstract
The invention belongs to the technical field of air purification, and discloses a laminated film photocatalyst for photocatalytic purification of gas, a preparation method and application thereof. The catalyst is in a heterogeneous multi-layer structure, a layer of carrier is uniformly attached to a substrate, and a layer of active component is uniformly loaded on the carrier. Uniformly depositing a carrier precursor corresponding to a carrier on the surface of a substrate material by adopting a chemical vapor deposition method, and then roasting to form a carrier film; loading active components on the carrier film by a deposition-precipitation method; activation results in a laminated thin film photocatalyst attached to the substrate. The laminated film photocatalyst or the sticky note thereof is placed in an air atmosphere, and volatile organic compounds in the air are removed through photocatalysis under certain temperature, humidity and illumination conditions. The method can be used at room temperature and normal pressure, has no secondary pollution and operation cost, and is suitable for indoor and outdoor places. Compared with the traditional powder type photocatalyst coating, the catalyst has the advantages of greatly reduced catalyst consumption and remarkably reduced cost.
Description
Technical Field
The invention belongs to the technical field of air purification, and particularly relates to a laminated film photocatalyst for photocatalytic purification of gas, a preparation method and application.
Background
Volatile Organic Compounds (VOCs) are one of the causes of haze and are also the main pollutants of indoor air. The removal of volatile organic compounds has great significance for the treatment of atmospheric environment and the improvement of human living environment.
The traditional VOCs treatment technology comprises an adsorption method, a condensation method, a combustion method, a catalytic combustion method, a biodegradation method and the like. The VOCs degradation technologies have good treatment effects on corresponding pollutant sources. However, due to the high operation cost, poor reliability, complex operation, secondary pollution and other factors, the above-mentioned conventional techniques are not suitable for the field of gas purification under normal temperature and pressure conditions. The photocatalysis technology can realize the oxidation (removal) reaction of VOCs under the conditions of normal temperature and normal pressure, and has the advantages of mild condition, simple and convenient operation, no secondary pollution, low operation cost and the like. In terms of external field energy density, the optical field energy density is lower than that of other thermal fields, electric fields and the like, so that the photocatalysis technology is a degradation and removal technology suitable for low-concentration VOCs pollutants in gas phase in the field of environment, particularly gas purification.
The photocatalytic reaction is a chemical reaction driven by a light energy field. When the light energy is larger than the forbidden band energy width of the catalyst, separated electron-hole pairs are generated, namely, the electron-hole pairs respectively transit to a conduction band and a valence band, and two half reactions occur at corresponding physical active sites formed on the surface of the catalyst. Oxidation half-reaction occurs at the physical active site corresponding to the valence band (hole); the reduction half-reaction occurs at the physically active site corresponding to the conduction band (electron). Therefore, the photocatalytic reaction is characterized by separate oxidation and reduction reactions, and is two half reactions separated from each other. Commonly used semiconductor photocatalysts (e.g. TiO)2) Due to the large bandwidth, the ultraviolet light with absorption of only 5% of the solar spectrum has photocatalytic activity. By modifying the catalyst, for example, by supporting plasmon metal nanoparticles on a semiconductor, the light absorption range of the semiconductor photocatalyst can be extended to the visible light region.
Compared with the traditional powder photocatalyst, the laminated film photocatalyst has uniqueness in structure, namely, the carrier film is used as a photocatalyst bottom layer, and the later-supported (plasmon type metal) active component is used as a top layer, so that the laminated film photocatalyst is formed. For the absorption of a two-dimensional light energy field, the utilization rate of the film is higher than that of the powder-shaped photocatalyst, so that the using amount of the photocatalyst is greatly reduced (the cost is reduced), and the adhesion of the laminated film photocatalyst on a substrate is enhanced (the durability is improved). After the catalyst is deactivated, the laminated film photocatalyst is convenient to stick and easy to remove and update. Because the preparation technology of the carrier film and the process of loading the metal nano particles are more difficult, at present, a laminated film photocatalyst for photocatalytic gas purification and a sticky note technology thereof do not exist, and particularly the laminated film photocatalyst for photocatalytic gas purification and the sticky note technology thereof under the condition of facing visible light (sunlight and indoor light source).
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides a laminated film photocatalyst for photocatalytic gas purification, a preparation method and application.
The specific technical scheme is as follows:
a laminated film photocatalyst for photocatalytic purification of gas is a heterogeneous multilayer structure, wherein a layer of carrier is uniformly attached to a substrate, and a layer of active component is uniformly loaded on the carrier; wherein the carrier is TiO2、CdS、ZnO、SiO2、Al2O3、ZrO2、CeO2、Fe2O3One or more than two of the components are mixed, and the active component is one or more than two of Au, Ag and Cu.
Further, the thickness of the film formed by the carrier is nano-scale to micron-scale; the active component accounts for 0.1-60% of the catalyst by mass percent, and the supporting amount of the active component per unit area is 0.01 mu g/cm2–1g/cm2。
Further, the method for preparing the laminated thin film photocatalyst for photocatalytic purification of gas is characterized by comprising the following steps:
(1) uniformly depositing a carrier precursor corresponding to a carrier on the surface of a substrate material by adopting a chemical vapor deposition method to form a carrier film;
(2) loading active components on the carrier film by a deposition-precipitation method;
(3) activation results in a laminated thin film photocatalyst attached to the substrate.
Further, the catalyst side of the substrate material is treated by plasma method before the carrier precursor is uniformly deposited on the substrate material, so as to enhance the adhesion of the laminated film photocatalyst on the surface of the substrate material.
Further, the substrate is a polymer film material or a hard substrate material; the polymer film material is polyimide, polytetrafluoroethylene, polyether-ether-ketone, polyethylene or polypropylene; the hard substrate material is quartz glass, common glass or metal sheet.
Further, the carrier precursor in the step (1) is uniformly deposited on the surface of the substrate material and then is roasted, wherein the roasting temperature is 300-900 ℃, and the roasting time is 0.5-5 h, so that the catalyst carrier film has a certain crystallization degree and is firmer and more reliable.
Further, the activation of the step (3) adopts a roasting and/or plasma method.
Further, the roasting temperature of the activation is 100-500 ℃, and the roasting time is 0.5-5 h.
Further, the plasma method is to adopt one or more of oxygen, argon or nitrogen, and discharge to generate plasma for surface treatment.
In the application of the laminated film photocatalyst for photocatalytic purification of gas, the other side of the substrate, which is opposite to the carrier, is coated with the adhesive adhering function to form the laminated film photocatalyst sticky note; under the illumination condition, the laminated film photocatalyst or the convenient paste thereof is placed in the air atmosphere to carry out photocatalysis to remove volatile organic compounds in the air; the air atmosphere is indoor and outdoor air with fluidity, the temperature is room temperature or outdoor temperature, the humidity is indoor and outdoor atmospheric natural humidity or humidity with humidification, and the illumination is indoor and outdoor sunlight, a visible light source or an ultraviolet light source.
Since illumination is a two-dimensional energy field, illumination is a necessary condition for photocatalytic reactions. The absorption of visible light and the contribution of visible light catalytic reactions are mainly from the active components. The active component in the laminated thin film photocatalyst has higher efficiency for light absorption than the powder type photocatalyst. Because all active components in the laminated film photocatalyst are only on the surface of the catalyst, the efficiency of the active components in the photocatalytic reaction is higher.
The invention has the beneficial effects that: the invention uses the laminated film photocatalyst or the sticky note to purify the gas by photocatalysis, under the conditions of natural illumination or artificial illumination (especially visible light illumination), certain temperature and humidity, the volatile organic compounds in the gas (such as air) are degraded by catalysis and/or the photocatalysis into nontoxic and harmless substances, so as to achieve the effect of purifying the gas (air), and the invention is mainly suitable for improving the living environment of people. The method can be used under the conditions of room temperature and normal pressure, has no secondary pollution and operation cost, and has wide application scenes. In the laminated film photocatalyst for photocatalytic gas purification and the sticky note thereof, the adhesive force of the laminated film photocatalyst on the substrate is extremely strong, so that the durability is greatly improved, and the catalyst is convenient to remove and update after being deactivated. The laminated film photocatalyst is essentially different from the traditional powder photocatalyst coating in structure, the catalyst consumption of the laminated film photocatalyst is greatly reduced, and the cost is obviously reduced.
Drawings
Fig. 1 is a schematic structural view of a laminated film sticky note (multilayer) for photocatalytic purification of gas.
Fig. 2 is a schematic view of a laminated thin film photocatalyst (single layer) structure for photocatalytic purification gas.
Fig. 3 is an indoor application scenario of a laminated film sticky note for photocatalytic purification of gases.
In the figure: 1 an active component; 2, a carrier; 3 a catalyst thin film; 4 a plasma treated substrate; 5 is non-adhesive glue; 6 a substrate which has not been plasma treated; 7 laminated film sticky note for photocatalytic purification of gas; 8, a ventilator; 9 indoor wall.
Detailed Description
Example 1
Step one, preparing a carrier film: the method is characterized in that quartz glass (2.5cm x 2.5cm) is used as a substrate, and titanium dioxide generated by the reaction of tetraisopropyl titanate and water vapor is uniformly deposited on the quartz glass by adopting an atmospheric pressure chemical vapor deposition method.
Step two, roasting the carrier film: and (3) heating the carrier film on the quartz glass to 500 ℃ at the heating rate of 5 ℃/min, and keeping the temperature for 2 hours to prepare the anatase titanium dioxide film.
Step three, loading active components: adding urea and chloroauric acid solution into deionized water, and vigorously stirring to obtain a mixed solution, wherein the concentration of urea in the mixed solution is 0.062mol/L, and the concentration of chloroauric acid in the mixed solution is 0.0005 mol/L. And (3) putting the prepared anatase titanium dioxide film into the mixed solution, and heating the mixed solution in a water bath at the temperature of 80 ℃ for 4 hours. And then taking out the film, washing the film by using deionized water, and drying the film at the temperature of 80 ℃ for 1 hour.
Step four, activation: the catalyst film is activated by roasting, and is heated to 250 ℃ at the heating rate of 10 ℃/min and kept for 2 hours. The actual content of the active component Au in the catalyst film is 0.017mg/cm2The mass percentage of the active component in the catalyst film is 27%.
Step five, evaluating the activity of the catalyst film; simulated air with formaldehyde concentration of 46.5 +/-1.5 ppm and relative humidity of 32 percent is subjected to Au/TiO2The film has a reaction temperature of 25 +/-1 ℃, a residence time of 0.75s and a light intensity of 354mW/cm of a xenon lamp provided with a UVCUT 420 filter2Finally, the formaldehyde conversion was 31%.
Example 2
After nitrogen plasma treatment is carried out on polytetrafluoroethylene serving as a substrate, a method for preparing a carrier film in the step one in the example 1 and a method for loading active components in the step three in the example 1 are adopted, and a catalyst film is activated in an oxygen plasma mode to prepare Au/TiO2A film. The actual content of the active component Au in the catalyst film is 0.01 mu g/cm2The mass percentage of the active component in the catalyst film is 0.1%. And coating non-sticky glue on the other side (without the catalyst) of the substrate to finally obtain the laminated film sticky note for the photocatalytic purification gas. The film is attached to the wall of the bedroom facing to the light side, and the indoor air is purified through photocatalysis. In order to improve the air purification effect, the fan can be opened, and when the humidity is lower, the air humidifier is started at the same time.
Example 3
The method for preparing the carrier film by the first step of example 1 and the method for loading the active component by the third step of example 1 are adopted to prepare Au/TiO by activating the catalyst film in the argon plasma mode by using polyethylene as a substrate2The actual content of active component Au in the film of the catalyst is 1g/cm2The mass percentage of the active component in the catalyst film is 60 percent. Placing it inThe device is placed on the floor of a toilet, the light source is turned on, the ventilation fan is started, and indoor air is purified through photocatalysis.
Example 4
Quartz glass is used as a substrate, the method of the first step of the example 1 is adopted to prepare the carrier film, then the carrier film is roasted for 5 hours at the temperature of 600 ℃, the method of the third step of the example 1 to load the active component is adopted, and then the catalyst film is activated in an oxygen plasma mode to prepare Cu/ZrO2And coating a non-sticky adhesive on the other side (without the catalyst) of the substrate to finally obtain the laminated film sticky note for the photocatalytic purification gas. The photocatalytic air purifier is attached to a kitchen wall, when cooking, the light source and the range hood are turned on, and the laminated film sticky note can be used for photocatalytic air purification in a room.
Claims (8)
1. A laminated film photocatalyst for photocatalytic purification of gas is characterized in that the laminated film photocatalyst is of a heterogeneous multilayer structure, a layer of carrier is uniformly attached to a substrate, and a layer of active component is uniformly loaded on the carrier; wherein the carrier is TiO2、CdS、ZnO、SiO2、Al2O3、ZrO2、CeO2、Fe2O3One or more than two of the components are mixed, and the active component is one or more than two of Au, Ag and Cu;
the thickness of the film formed by the carrier is nano-scale to micron-scale; the active component accounts for 0.1-60% of the catalyst by mass percent, and the supporting amount of the active component per unit area is 0.01 mu g/cm2– 1g/cm2；
The preparation method of the laminated thin film photocatalyst comprises the following steps:
(1) reacting a carrier precursor corresponding to a carrier with water vapor by adopting an atmospheric pressure chemical vapor deposition method, and uniformly depositing the carrier precursor on the surface of a substrate material to form a carrier film;
(2) carrying out a deposition-precipitation method by using urea, thereby loading an active component on the carrier film;
(3) activation results in a laminated thin film photocatalyst attached to the substrate.
2. The laminated thin film photocatalyst for photocatalytic purification gas as recited in claim 1, wherein a base material is used to which the catalyst side is attached, and a surface treatment is performed by a plasma method before the carrier precursor is uniformly deposited on the base material.
3. The laminated thin film photocatalyst for photocatalytic purification gas as recited in claim 1 or 2, wherein said substrate is a polymer film material or a hard substrate material; the polymer film material is polyimide, polytetrafluoroethylene, polyether-ether-ketone, polyethylene or polypropylene; the hard substrate material is quartz glass, common glass or metal sheet.
4. The laminated thin-film photocatalyst for photocatalytic purification gas as recited in claim 1 or 2, wherein the carrier precursor in step (1) is uniformly deposited on the surface of the base material and then calcined at a temperature of 300 to 900 ℃oAnd C, roasting for 0.5-5 h.
5. The laminated thin film photocatalyst for photocatalytic purification gas as recited in claim 1, wherein the activation in step (3) is performed by a baking and/or plasma method.
6. The laminated thin-film photocatalyst for photocatalytic purification gas as recited in claim 5, wherein the calcination temperature for activation is 100 to 500%oAnd C, roasting for 0.5-5 h.
7. The laminated film photocatalyst for photocatalytic purification gas as recited in claim 2 or 5, wherein said plasma treatment is performed by using one or more of oxygen, argon, and nitrogen, and plasma generated by electric discharge.
8. Use of the laminated film photocatalyst for photocatalytic purification gas as recited in any one of claims 1 to 7, wherein an adhesive having an adhesive attachment function is coated on the other side of said substrate with respect to said support to form a laminated film photocatalyst sticky note; under the illumination condition, the laminated film photocatalyst or the convenient paste thereof is placed in the air atmosphere to carry out photocatalysis to remove volatile organic compounds in the air; the air atmosphere is indoor and outdoor air with fluidity, the temperature is room temperature or outdoor temperature, the humidity is indoor and outdoor atmospheric natural humidity or humidity with humidification, and the illumination is indoor and outdoor sunlight, a visible light source or an ultraviolet light source.
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| CN101673021A (en) * | 2009-09-27 | 2010-03-17 | 中国科学院上海硅酸盐研究所 | Gold nanoparticle loaded mesoporous titanium oxide composite film and preparation thereof |
| CN107149872B (en) * | 2017-05-10 | 2020-06-12 | 大连理工大学 | Preparation method of photocatalytic gas purification sticky note |
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