CN104258894B - There is visible light-responded metallic plate supported titanium2photocatalyst and preparation and application - Google Patents
There is visible light-responded metallic plate supported titanium2photocatalyst and preparation and application Download PDFInfo
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Abstract
The invention discloses and there is visible light-responded metallic plate supported titanium2Photocatalyst and preparation and purposes, it is characterised in that with metal ion manganese and zirconium and the TiO of the nitrogen co-doped modification of nonmetallic ion2For active component, (molecular formula is TiO2NxMnyZrz, 0 < x < 1,0 < y < 1,0 < z < 1) and load is on a metal plate；Ultrasonic assistant sol-gal process is used to prepare N Mn Zr codope TiO2Catalyst fines；Utilize electrostatic powder spraying by TiO2Powder loads to the surface of metallic plate uniformly and obtains catalyst.Present device easily operates, and raw material easily obtains, low cost；Simple for process, it is easy to accomplish large-scale production.Catalyst mass-transfer efficiency is high, and active component is firmly combined with carrier, difficult drop-off, and service life is long, and applied widely and plasticity by force, can prepare the shape of various beautiful practicality；Can be used for the finishing material of office, office building, living room, automobile, market, factory, hospital etc., can effectively the degrade formaldehyde in indoor and outdoor place, benzene homologues, total volatile organism etc..
Description
Technical field
The invention belongs to catalysis material preparation field, be specifically related to a kind of there is visible light-responded metallic plate supported titanium2Photocatalyst and preparation and application.
Technical background
Photocatalytic-oxidation formed material is processing in terms of air pollution, because it is simple to operate, mild condition and low energy consumption, does not produce the feature of secondary pollution, therefore has a wide range of applications at aspects such as air, the degraded of water environment pollution thing, antibacterial, deodorization.Wherein nano-TiO2The features such as semi-conducting material is cheap with it, nontoxic, stable, catalytic performance is good and gain great popularity.But TiO2Energy gap be 3.2eV, under the ultraviolet light conditions of λ 387.5nm, just need to can be inspired photocatalytic effect, produce the electron hole pair (h with Strong oxdiative and reducing power+-e-), make absorption at TiO2The O on surface2Acquisition electronically forms O2 -, OH simultaneously-Or H2O is combined the OH generating strong oxidizing property with hole.Absorption pollutant on catalyst surface are at O2 -With under the effect of OH, chemical reaction is occurred to degrade.And the energy in sunlight medium ultraviolet light district only accounts for the 3～5% of gross energy, it is impossible to utilize the visible ray accounting for gross energy 43%, had a strong impact on TiO2Actual application in terms of photocatalysis.The most how to make TiO2Photoresponse expand to visible region, it has also become the core difficult problem in current photochemical catalytic oxidation field.
Ion doping can change TiO2Band structure and absorption spectrum ranges, and then change TiO2Catalytic selectivity and activity, and become the focus of current research.According to the difference of dopant, it is broadly divided into metal ion mixing, nonmetallic ion-doped and codope.But single metal-doped can reduce TiO2Heat stability, and add h+-e-Recombination rate, reduce its photocatalysis efficiency.Then there is antioxidation reduction and acid and alkali-resistance equistability and the problem in service life in single nonmetal doping.And codope overcomes the deficiency of single ionic doping, and there is cooperative effect, improve photocatalysis performance.Therefore, codope is passed through at present to TiO2The modified Main Means having become its photocatalysis performance of raising.As: CN101108336 discloses the codope TiO of metal ion Sn and nonmetallic ion N2The preparation of catalyst, compared to pure TiO2Singly mixing Sn and N, catalyst all has lifting by a relatively large margin in Uv and visible light district.CN103240070A discloses two metal ion species Al and In codope TiO2The preparation of catalyst, metal ion mixing suppression TiO2The transformation of crystal formation, increases TiO2Lattice surface defect, expands TiO2Light abstraction width, improve TiO2Photocatalysis efficiency.CN102350369A then discloses two kinds of non-metal Ns, F codope TiO2The synthesis of catalyst, catalyst shows visible ray effect, and reduces (h+-e-) compound.But above-mentioned catalyst all exists with powdered form form, existing in the application of actual treatment atmospheric pollution, mass transfer rate is low, easily blocks, and under the effect of usual external environment condition, is easily generated loss and dust secondary pollution problems.Therefore, suitable TiO is found2It is to affect TiO that catalyst carrier carries out load to it2Photocatalyst can in air contaminant treatment the major issue of actual application.As CN102423701A (glass fabric is carrier), CN102151561A (CNT is carrier) etc. disclose loaded catalyst, but glass fabric absorption affinity is poor, need to repeatedly impregnate-lift-calcine, increase energy consumption cost；CNT poor plasticity, is difficult to make the various beautiful shape of commercialization demand, and expensive.The problems such as the most above-mentioned loaded catalyst there is also preparation technology poor repeatability, and active component is combined insecure with carrier, easy to fall off.
Summary of the invention
Present invention aims to the deficiencies in the prior art, it is proposed that a kind of have visible light-responded metallic plate supported titanium2Photocatalyst, it is a further object of the present invention to provide the preparation method and application of above-mentioned photocatalyst.
The technical scheme is that there is visible light-responded metallic plate supported titanium2Photocatalyst, it is characterised in that with metal ion manganese and zirconium and the TiO of the nitrogen co-doped modification of nonmetallic ion2Load on a metal plate for active component；Wherein the molecular formula of active component is TiO2NxMnyZrz, 0 < x < 1,0 < y < 1,0 < z < 1.
The molecular formula of the most above-mentioned active component is TiO2NxMnyZrz, wherein 0.0005≤x≤0.2,0.001≤y≤0.2,0.001≤z≤0.25.
Present invention also offers and above-mentioned there is visible light-responded metallic plate supported titanium2The method of photocatalyst, prepares TiO with ultrasonic assistant sol-gel process2Photocatalyst powder, uses electrostatic powder spraying by the N-Mn-Zr codope TiO of preparation2Photocatalyst powder loads on metallic plate；It specifically comprises the following steps that
(1) it is TiO by molecular formula2NxMnyZrz, 0 < x < 1,0 < y < 1,0 < z < 1 weighs raw material titanium source, manganese source, zirconium source, nitrogen source；Being added drop-wise in organic solvent in titanium source under magnetic stirring apparatus effect, obtain solution A, wherein titanium source is 0.01～1:1 with the amount ratio of organic solvent material；
(2) it is added to water droplet in the organic solvent with step (1) equivalent be mixed to get aqueous solutions of organic solvent under magnetic stirring apparatus effect, wherein the amount ratio of the material of water and organic solvent is 0.01～1:1, it is subsequently adding acid, regulation pH value, again manganese source, zirconium source, nitrogen source are joined in aqueous solutions of organic solvent, obtain solution B；
(3) under the effect of magnetic stirring apparatus, solution B is added drop-wise in solution A, completely after dropping, continues stirring 0.5h～2h, be then placed into supersound process in Ultrasound Instrument, until forming gel, taking out ageing, obtaining stable gel；
(4) the gel obtained in step (3) be placed in thermostatic drying chamber be dried, it is thus achieved that xerogel, be ground into powder, be placed in Muffle kiln roasting, i.e. obtain N-Mn-Zr codope TiO2Photocatalyst powder；
(5) take thermosets to mix with the photocatalyst powder of preparation, after stirring, put into electrostatic powder spraying chamber, use and suppress the surface charged powder spray to metallic plate, form the coating of powdery；
(6) by the metallic plate after spraying to high temperature furnace, make that powder is dense melts solidification, obtain that there is visible light-responded metallic plate supported titanium2Photocatalyst.
Being added drop-wise to solution B in solution A in preferred steps (3) control nitrogen source, zirconium source, manganese source is (0.0005～0.2) with the amount ratio of the material in titanium source: (0.001～0.2): (0.001～0.25): 1；In preferred steps (5), thermosets is 0.001～0.1:1 with the mass ratio of photocatalyst powder.
In preferred steps (2), regulation pH value is 1～6；The temperature of the supersound process in step (3) is 0～20 DEG C, and supersonic frequency is 50～100HZ；The temperature being dried in step (4) is 50～100 DEG C, drying time 12～24h；Sintering temperature 350 in step (4)～600 DEG C, the time 0.5～6h；The pressure suppressed in step (5) is 0.1Mpa～1Mpa；In step (6), the dense temperature melting solidification is 100～200 DEG C, the time 10～60min.
Organic solvent described in preferred steps (1) and (2) is the one in dehydrated alcohol, methanol or isopropanol or a combination thereof；The one that titanium source is butyl titanate, isopropyl titanate, titanium tetrachloride or titanium sulfate in step (1) or a combination thereof；The one that acid is glacial acetic acid, hydrochloric acid or nitric acid in step (2) or a combination thereof；Nitrogen source is one or a combination thereof of ammonium carbonate, carbamide, triethylamine or ammonium acetate；Manganese source is one or a combination thereof of manganese nitrate, manganese acetate or manganese chloride；Zirconium source is zirconium oxychloride, zirconium chloride or the zirconium acetate one that is or a combination thereof；The one that thermosets is epoxy powder, polyurethane powder or acrylic clear powder in step (5) or a combination thereof.
Catalyst activity component can firmly be loaded on metallic plate by the carrying method that the present invention uses, metallic plate refers to all sheet material with metallicity, or preferable iron plate, copper coin, aluminium sheet, titanium plate, zine plate, corrosion resistant plate, the one of magnesium plate and alloy thereof.
Present invention also offers and above-mentioned there is visible light-responded metallic plate supported titanium2Photocatalyst is applied in finishing material.Can be used for the finishing material of office, office building, living room, automobile, market, factory, hospital etc., can effectively the degrade formaldehyde in indoor and outdoor place, benzene homologues, total volatile organism etc..
Beneficial effect:
The present invention is with two metal ion species Mn and Zr and a kind of nonmetallic ion N codope TiO2/ metallic plate loaded photocatalyst preparation method, makes TiO2Photocatalyst can carry out large-scale industrial production and be applied in the middle of reality.The non-metal N of this catalyst doping and two kinds of metal Mn and Zr, energy and TiO2Form synergism, reduce light-catalysed energy gap, reduce h+-e-Compound, thus increase TiO2Utilization rate to sunlight, improves its photocatalytic activity.The equipment that the present invention uses is easily operated, and raw material is easily obtained, low cost；Simple for process, it is easy to accomplish large-scale production.The catalyst prepared, mass-transfer efficiency is high, active component is firmly combined with carrier, difficult drop-off, service life is long, applied widely and plasticity is strong, the shape of various beautiful practicality can be prepared, meet commercialization demand, can be used for the finishing material of office, office building, living room, automobile, market, factory, hospital etc., can effectively the degrade formaldehyde in indoor and outdoor place, benzene homologues, total volatile organism etc..
Accompanying drawing explanation
Fig. 1 is the TiO of N-Mn-Zr codope in embodiment 12With unadulterated TiO2XRD figure spectrum；Wherein ● anatase, rutile；
Fig. 2 is the TiO of N-Mn-Zr codope in embodiment 12With unadulterated TiO2DRS collection of illustrative plates；
Fig. 3 is gas photocatalysis evaluating apparatus schematic diagram；A is visible light source, and B is catalyst placement platform, and C is gas sample mouth, D blast velocity control instrument, and E is gas sampling mouth；
Fig. 4 is N-Mn-Zr codope TiO in embodiment 12Catalyst oxidation of formaldehyde performance test figure；
Fig. 5 is metallic plate (aluminium sheet) support type N-Mn-Zr codope TiO in embodiment 12The performance test figure of catalyst oxidation of formaldehyde；
Fig. 6 is embodiment 2 metallic plate (corrosion resistant plate) support type N-Mn-Zr codope TiO2The performance for stability test figure of photocatalyst catalytic degradation formaldehyde；
Fig. 7 is embodiment 3 metallic plate (titanium plate) support type N-Mn-Zr codope TiO2The performance test figure of catalyst oxidation gaseous mixture (formaldehyde and toluene).
Detailed description of the invention
The following is the specific embodiment of the present invention, to metallic plate support type N-Mn-Zr codope TiO involved in the present invention2The preparation method of visible light catalyst is described further, but protection scope of the present invention is not limited to these embodiments.Within every change without departing substantially from present inventive concept or equal replacement are included in protection scope of the present invention.
Embodiment 1
(1) taking 0.1mol butyl titanate, under magnetic stirring apparatus effect, be added dropwise in the dehydrated alcohol of 0.1mol, be sufficiently stirred for, mix homogeneously obtains solution A.
(2) deionized water taking 0.1mol dehydrated alcohol and 0.1mol is being mixed to get ethanol water under magnetic stirring apparatus effect, add glacial acetic acid, the value of the PH of regulation ethanol water is 3, under magnetic stirring apparatus effect, add 0.00005mol ammonium carbonate, 0.001mol zirconium oxychloride and 0.025mol manganese nitrate, being sufficiently stirred for, mix homogeneously obtains solution B.
(3) under the effect of magnetic stirring apparatus, solution B is dropwise added drop-wise in solution A, after being added dropwise to complete, continues stirring 1h.It is then placed in Ultrasound Instrument (temperature is 0 DEG C, and frequency is 50HZ), age gelation.
(4) gel obtained in (3) is placed on thermostatic drying chamber, 50 DEG C of dry 24h, it is thus achieved that xerogel, it is ground into powder, is placed in 500 DEG C of roasting 2.5h of Muffle furnace, i.e. obtains N-Mn-Zr codope TiO2Visible light catalyst powder.
Shown from Fig. 1 result, through the TiO of N-Mn-Zr codope2Catalyst, its characteristic peak display TiO2The all anatase phase of crystalline phase, and unadulterated TiO2Catalyst is the mixed phase of anatase and rutile.Shown from Fig. 2 result, through the TiO of N-Mn-Zr codope2Catalyst, is keeping TiO2Photocatalyst, while ultraviolet catalytic ability, absorbs in visible region and substantially increases.N-Mn-Zr codope TiO by preparation2Photocatalyst powder is placed on (such as Fig. 3) in gas photocatalysis evaluating apparatus and carries out the performance test of degradation of formaldehyde.Reaction condition is: device volume 0.22m3, temperature 22 DEG C, relative humidity 46%, wind speed 0.3m/s, 45w electricity-saving lamp is visible light source, and concentration of formaldehyde is 1.0mg/m3.Shown in the result of the test of Fig. 4, N-Mn-Zr codope TiO2Catalyst shows the highest catalytic capability.Can be by 1.0mg/m in 12h3Gaseous formaldehyde is degraded to 0.077mg/m3, catalysis degradation modulus reaches 92.3%.
(5) photocatalyst powder in step (4) is taken, adding with its mass ratio is the epoxy powder of 0.001, it is uniformly mixed, use electrostatic powder spraying (pressure is 0.5Mpa) that mixed-powder sprays to metallic plate (aluminium sheet) surface of a size of 50*100cm, form the coating of powdery.
(6) by the plate after spraying as the high temperature furnace 60min of 100 DEG C, make powder dense melt, solidify, i.e. obtain metallic plate (aluminium sheet) support type N-Mn-Zr codope TiO2Photocatalyst.
Metallic plate (aluminium sheet) support type N-Mn-Zr codope TiO by preparation2Photocatalyst is placed on (such as Fig. 3) in gas photocatalysis evaluating apparatus and carries out the performance test of degradation of formaldehyde.Reaction condition is: device volume 0.22m3, temperature 22 DEG C, relative humidity 46%, wind speed 0.3m/s, 45w electricity-saving lamp is visible light source, and concentration of formaldehyde is 1.0mg/m3.Shown in the result of the test of Fig. 5, metallic plate (aluminium sheet) support type N-Mn-Zr codope TiO2Catalyst shows the highest catalytic capability.Can be by 1.0mg/m in 18h3Gaseous formaldehyde is degraded to 0.076mg/m3, catalysis degradation modulus reaches 92.4%.
Embodiment 2
(1) taking 0.1mol isopropyl titanate, under magnetic stirring apparatus effect, be added dropwise in the methanol of 10mol, be sufficiently stirred for, mix homogeneously obtains solution A.
(2) deionized water taking 10mol methanol and 0.1mol is being mixed to get methanol aqueous solution under magnetic stirring apparatus effect, add nitric acid, the value of the PH of regulation methanol aqueous solution is 1, under magnetic stirring apparatus effect, add 0.001mol carbamide, 0.02mol zirconium acetate and 0.0001mol manganese acetate, under magnetic stirring apparatus effect, being sufficiently stirred for, mix homogeneously obtains solution B.
(3) under the effect of magnetic stirring apparatus, solution B is dropwise added drop-wise in solution A, after being added dropwise to complete, continues stirring 0.5h.It is then placed in Ultrasound Instrument (water temperature is 20 DEG C, and frequency is 75HZ), age gelation.
(4) gel obtained in (3) is placed on thermostatic drying chamber, 100 DEG C of dry 12h, it is thus achieved that xerogel, it is ground into powder, is placed in 350 DEG C of roasting 6h of Muffle furnace, i.e. obtains N-Mn-Zr codope TiO2Visible light catalyst powder.
(5) photocatalyst powder of preparation in (4) is taken, and addition is 0.1 polyurethane powder with its mass ratio, it is uniformly mixed, use electrostatic powder spraying (pressure is 0.1Mpa) that mixed-powder sprays to a diameter of 100cm, it is shaped as hemispheric metallic plate (corrosion resistant plate) surface, forms the coating of powdery.
(6) by the metallic plate after spraying as the high temperature furnace 10min of 200 DEG C, make powder dense melt, solidify, i.e. obtain metallic plate (corrosion resistant plate) support type N-Mn-Zr codope TiO2Visible light catalyst.
Metallic plate (corrosion resistant plate) support type N-Mn-Zr codope TiO by preparation2Photocatalyst is placed on (such as Fig. 3) in gas photocatalysis evaluating apparatus and carries out the performance for stability test of degradation of formaldehyde.Reaction condition is: device volume 0.22m3, temperature 22 DEG C, relative humidity 46%, wind speed 0.3m/s, 45w electricity-saving lamp is visible light source, and concentration of formaldehyde is 1.0mg/m3.Shown in the result of the test of Fig. 6, catalyst shows the highest stability, and through the test of continuous 11 times, catalysis degradation modulus all maintains more than 92%.
Embodiment 3
(1) taking 0.1mol titanium tetrachloride, under magnetic stirring apparatus effect, be added dropwise in the isopropanol of 1mol, be sufficiently stirred for, mix homogeneously obtains solution A.
(2) deionized water taking 1mol isopropanol and 0.2mol is being mixed to get isopropanol water solution under magnetic stirring apparatus effect, add hydrochloric acid, the value of the PH of regulation isopropanol water solution is 6, under magnetic stirring apparatus effect, add 0.02mol ammonium acetate, 0.0001mol zirconium chloride and 0.0025mol manganese chloride, under magnetic stirring apparatus effect, being sufficiently stirred for, mix homogeneously obtains solution B.
(3) under the effect of magnetic stirring apparatus, solution B is dropwise added drop-wise in solution A, after being added dropwise to complete, continues stirring 2h.It is then placed in Ultrasound Instrument (water temperature is 20 DEG C, and frequency is 75HZ), age gelation.
(4) gel obtained in (3) is placed on thermostatic drying chamber, 90 DEG C of dry 16h, it is thus achieved that xerogel, it is ground into powder, is placed in 600 DEG C of roasting 0.5h of Muffle furnace, i.e. obtains N-Mn-Zr codope TiO2Visible light catalyst powder.(5) photocatalyst powder of preparation in (4) is taken, and addition is 0.05 acrylic clear powder with its mass ratio, it is uniformly mixed, use electrostatic powder spraying (pressure is 1Mpa) that mixed-powder sprays to metallic plate (titanium plate) surface that the length of side is 50cm rhombus, form the coating of powdery.
(6) by the metallic plate after spraying as the high temperature furnace 45min of 150 DEG C, make powder dense melt, solidify, i.e. obtain metallic plate (titanium plate) support type N-Mn-Zr codope TiO2Visible light catalyst.
Metallic plate (titanium plate) support type N-Mn-Zr codope TiO by preparation2Photocatalyst is placed on (such as Fig. 3) in gas photocatalysis evaluating apparatus and carries out gaseous mixture (formaldehyde and toluene) performance test of degrading.Reaction condition is: device volume 0.44m3, temperature 22 DEG C, relative humidity 46%, wind speed 0.2m/s, 60w electricity-saving lamp is visible light source, and concentration of formaldehyde is 1.0mg/m3, toluene concentration is 1.0mg/m3.Shown in the result of the test of Fig. 7, metallic plate (titanium plate) support type N-Mn-Zr codope TiO2Catalyst shows the highest catalytic capability.Can be by 1.0mg/m in 20h3Gaseous formaldehyde is degraded to 0.079mg/m3, catalysis degradation modulus reaches 92.1%, 1.0mg/m3Gaseous state degradation of toluene is to 0.191mg/m3, catalysis degradation modulus reaches 80.9%.
Claims (6)
1. there is visible light-responded metallic plate supported titanium2Photocatalyst, it is characterised in that with metal ion manganese and
Zirconium and the TiO of the nitrogen co-doped modification of nonmetallic ion2Load on a metal plate for active component；Wherein activity group
The molecular formula divided is TiO2NxMnyZrz, 0.0005≤x≤0.2,0.001≤y≤0.2,0.001≤z≤0.250.
2. prepare there is visible light-responded metallic plate supported titanium as claimed in claim 1 for one kind2Photocatalyst
Method, it specifically comprises the following steps that
(1) it is TiO by molecular formula2NxMnyZrz, 0.0005≤x≤0.2,0.001≤y≤0.2,0.001≤z≤0.250 weighs former
Material titanium source, manganese source, zirconium source, nitrogen source；Under magnetic stirring apparatus effect, titanium source is added drop-wise in organic solvent,
To solution A, wherein titanium source is 0.01～1:1 with the amount ratio of organic solvent material；
(2) under magnetic stirring apparatus effect, water droplet is added to the organic solvent of step (1) equivalent in be mixed to get organic molten
Agent aqueous solution, wherein the amount ratio of the material of water and organic solvent is 0.01～1:1, is subsequently adding acid, regulates pH
Value, then manganese source, zirconium source, nitrogen source are joined in aqueous solutions of organic solvent, obtain solution B；
(3) under the effect of magnetic stirring apparatus, solution B is added drop-wise in solution A, completely after dropping, continues stirring
0.5h～2h, is then placed into supersound process in Ultrasound Instrument, until forming gel, taking out ageing, being stablized
Gel；
(4) the gel obtained in step (3) be placed in thermostatic drying chamber be dried, it is thus achieved that xerogel, be ground into powder, put
In Muffle kiln roasting, i.e. obtain N-Mn-Zr codope TiO2Photocatalyst powder；
(5) take thermosets to mix with the photocatalyst powder of preparation, put into electrostatic powder spraying chamber after stirring, adopt
With the surface suppressed charged powder spray to metallic plate, form the coating of powdery；
(6) by the metallic plate after spraying to high temperature furnace, make that powder is dense melts solidification, obtain that there is visible light-responded metal
Plate supported titanium2Photocatalyst.
3. method as claimed in claim 2, it is characterised in that solution B is added drop-wise to solution A in (3) by step
Middle control nitrogen source, zirconium source, manganese source with the amount ratio of the material in titanium source are
(0.0005～0.2): (0.001～0.2): (0.001～0.25): 1；Thermosets and photocatalyst powder in step (5)
Mass ratio be 0.001～0.1:1.
4. method as claimed in claim 2, it is characterised in that in step (2), regulation pH value is 1～6；Step
(3) temperature of the supersound process in is 0～20 DEG C, and supersonic frequency is 50～100Hz；Step (4) is dried
Temperature be 50～100 DEG C, drying time 12～24h；Sintering temperature 350 in step (4)～600 DEG C, time
Between 0.5～6h；The pressure suppressed in step (5) is 0.1Mpa～1Mpa；Dense in step (6) melt solidification
Temperature is 100～200 DEG C, the time 10～60min.
5. method as claimed in claim 2, it is characterised in that the organic solvent described in step (1) and (2)
It is the one in dehydrated alcohol, methanol or isopropanol or a combination thereof；Titanium source in step (1) is metatitanic acid four
The one of butyl ester, isopropyl titanate, titanium tetrachloride or titanium sulfate or a combination thereof；Acid in step (2) is ice
The one of acetic acid, hydrochloric acid or nitric acid or a combination thereof；Nitrogen source is the one of ammonium carbonate, carbamide, triethylamine or ammonium acetate
Plant or a combination thereof；Manganese source is one or a combination thereof of manganese nitrate, manganese acetate or manganese chloride；Zirconium source be zirconium oxychloride,
Zirconium chloride or the one of zirconium acetate or a combination thereof；Thermosets in step (5) be epoxy powder,
Polyurethane powder or the one of acrylic clear powder or a combination thereof.
There is visible light-responded metallic plate supported titanium the most as claimed in claim 12Photocatalyst is at finishing material
Material is applied.
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