WO2017192057A1 - Modified porous coatings and a modular device for air treatment containing modified porous coatings. - Google Patents
Modified porous coatings and a modular device for air treatment containing modified porous coatings. Download PDFInfo
- Publication number
- WO2017192057A1 WO2017192057A1 PCT/PL2017/050024 PL2017050024W WO2017192057A1 WO 2017192057 A1 WO2017192057 A1 WO 2017192057A1 PL 2017050024 W PL2017050024 W PL 2017050024W WO 2017192057 A1 WO2017192057 A1 WO 2017192057A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- modified porous
- porous coatings
- modified
- nanotubes
- coatings according
- Prior art date
Links
- 238000000576 coating method Methods 0.000 title claims abstract description 35
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 96
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims abstract description 94
- 239000002096 quantum dot Substances 0.000 claims abstract description 34
- 239000002071 nanotube Substances 0.000 claims abstract description 32
- 239000000919 ceramic Substances 0.000 claims abstract description 30
- 230000005855 radiation Effects 0.000 claims abstract description 29
- 229910052697 platinum Inorganic materials 0.000 claims abstract description 28
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 claims abstract description 22
- 230000001699 photocatalysis Effects 0.000 claims abstract description 22
- 230000003647 oxidation Effects 0.000 claims abstract description 16
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 15
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims abstract description 10
- 238000006243 chemical reaction Methods 0.000 claims abstract description 9
- 238000001179 sorption measurement Methods 0.000 claims abstract description 8
- 239000000428 dust Substances 0.000 claims abstract description 6
- 230000002779 inactivation Effects 0.000 claims abstract description 6
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- FSJWWSXPIWGYKC-UHFFFAOYSA-M silver;silver;sulfanide Chemical compound [SH-].[Ag].[Ag+] FSJWWSXPIWGYKC-UHFFFAOYSA-M 0.000 claims description 12
- 229910052946 acanthite Inorganic materials 0.000 claims description 11
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 10
- 239000010936 titanium Substances 0.000 claims description 10
- 229910052719 titanium Inorganic materials 0.000 claims description 10
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 9
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 8
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- 150000001450 anions Chemical class 0.000 claims description 5
- 238000001354 calcination Methods 0.000 claims description 5
- 150000001768 cations Chemical class 0.000 claims description 5
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- OAYXUHPQHDHDDZ-UHFFFAOYSA-N 2-(2-butoxyethoxy)ethanol Chemical compound CCCCOCCOCCO OAYXUHPQHDHDDZ-UHFFFAOYSA-N 0.000 claims description 3
- DDFHBQSCUXNBSA-UHFFFAOYSA-N 5-(5-carboxythiophen-2-yl)thiophene-2-carboxylic acid Chemical compound S1C(C(=O)O)=CC=C1C1=CC=C(C(O)=O)S1 DDFHBQSCUXNBSA-UHFFFAOYSA-N 0.000 claims description 3
- 239000001856 Ethyl cellulose Substances 0.000 claims description 3
- ZZSNKZQZMQGXPY-UHFFFAOYSA-N Ethyl cellulose Chemical compound CCOCC1OC(OC)C(OCC)C(OCC)C1OC1C(O)C(O)C(OC)C(CO)O1 ZZSNKZQZMQGXPY-UHFFFAOYSA-N 0.000 claims description 3
- 229910020427 K2PtCl4 Inorganic materials 0.000 claims description 3
- PRXRUNOAOLTIEF-ADSICKODSA-N Sorbitan trioleate Chemical compound CCCCCCCC\C=C/CCCCCCCC(=O)OC[C@@H](OC(=O)CCCCCCC\C=C/CCCCCCCC)[C@H]1OC[C@H](O)[C@H]1OC(=O)CCCCCCC\C=C/CCCCCCCC PRXRUNOAOLTIEF-ADSICKODSA-N 0.000 claims description 3
- WUOACPNHFRMFPN-UHFFFAOYSA-N alpha-terpineol Chemical compound CC1=CCC(C(C)(C)O)CC1 WUOACPNHFRMFPN-UHFFFAOYSA-N 0.000 claims description 3
- 239000007864 aqueous solution Substances 0.000 claims description 3
- 230000015572 biosynthetic process Effects 0.000 claims description 3
- SQIFACVGCPWBQZ-UHFFFAOYSA-N delta-terpineol Natural products CC(C)(O)C1CCC(=C)CC1 SQIFACVGCPWBQZ-UHFFFAOYSA-N 0.000 claims description 3
- 235000019325 ethyl cellulose Nutrition 0.000 claims description 3
- 229920001249 ethyl cellulose Polymers 0.000 claims description 3
- 229910052751 metal Inorganic materials 0.000 claims description 3
- 239000002184 metal Substances 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- DOIRQSBPFJWKBE-UHFFFAOYSA-N phthalic acid di-n-butyl ester Natural products CCCCOC(=O)C1=CC=CC=C1C(=O)OCCCC DOIRQSBPFJWKBE-UHFFFAOYSA-N 0.000 claims description 3
- 239000002904 solvent Substances 0.000 claims description 3
- 229940116411 terpineol Drugs 0.000 claims description 3
- 238000009210 therapy by ultrasound Methods 0.000 claims description 3
- 238000002604 ultrasonography Methods 0.000 claims description 3
- 239000004147 Sorbitan trioleate Substances 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims description 2
- 235000019337 sorbitan trioleate Nutrition 0.000 claims description 2
- 229960000391 sorbitan trioleate Drugs 0.000 claims description 2
- SOQBVABWOPYFQZ-UHFFFAOYSA-N oxygen(2-);titanium(4+) Chemical compound [O-2].[O-2].[Ti+4] SOQBVABWOPYFQZ-UHFFFAOYSA-N 0.000 claims 1
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 36
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 11
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 9
- 230000000694 effects Effects 0.000 description 8
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- 229910052799 carbon Inorganic materials 0.000 description 7
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- 244000005700 microbiome Species 0.000 description 7
- VDQVEACBQKUUSU-UHFFFAOYSA-M disodium;sulfanide Chemical compound [Na+].[Na+].[SH-] VDQVEACBQKUUSU-UHFFFAOYSA-M 0.000 description 6
- 238000006385 ozonation reaction Methods 0.000 description 6
- 229910052979 sodium sulfide Inorganic materials 0.000 description 6
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 4
- FERIUCNNQQJTOY-UHFFFAOYSA-N Butyric acid Chemical compound CCCC(O)=O FERIUCNNQQJTOY-UHFFFAOYSA-N 0.000 description 4
- DNJIEGIFACGWOD-UHFFFAOYSA-N ethanethiol Chemical compound CCS DNJIEGIFACGWOD-UHFFFAOYSA-N 0.000 description 4
- GETQZCLCWQTVFV-UHFFFAOYSA-N trimethylamine Chemical compound CN(C)C GETQZCLCWQTVFV-UHFFFAOYSA-N 0.000 description 4
- 238000004065 wastewater treatment Methods 0.000 description 4
- 230000008901 benefit Effects 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 3
- 239000008367 deionised water Substances 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- -1 hydroxyl radicals Chemical class 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- BHAROVLESINHSM-UHFFFAOYSA-N toluene Chemical compound CC1=CC=CC=C1.CC1=CC=CC=C1 BHAROVLESINHSM-UHFFFAOYSA-N 0.000 description 3
- 238000012546 transfer Methods 0.000 description 3
- 229910021529 ammonia Inorganic materials 0.000 description 2
- PPNKDDZCLDMRHS-UHFFFAOYSA-N bismuth(III) nitrate Inorganic materials [Bi+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O PPNKDDZCLDMRHS-UHFFFAOYSA-N 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000011109 contamination Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000036541 health Effects 0.000 description 2
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 239000002086 nanomaterial Substances 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 150000002894 organic compounds Chemical class 0.000 description 2
- 244000052769 pathogen Species 0.000 description 2
- 238000007146 photocatalysis Methods 0.000 description 2
- 229910021650 platinized titanium dioxide Inorganic materials 0.000 description 2
- 239000013049 sediment Substances 0.000 description 2
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(I) nitrate Inorganic materials [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 description 2
- 239000002689 soil Substances 0.000 description 2
- 241000894006 Bacteria Species 0.000 description 1
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- 229910021626 Tin(II) chloride Inorganic materials 0.000 description 1
- 230000001133 acceleration Effects 0.000 description 1
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- 239000000443 aerosol Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical group [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000010170 biological method Methods 0.000 description 1
- XIEPJMXMMWZAAV-UHFFFAOYSA-N cadmium nitrate Inorganic materials [Cd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XIEPJMXMMWZAAV-UHFFFAOYSA-N 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
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- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 1
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- AXZWODMDQAVCJE-UHFFFAOYSA-L tin(II) chloride (anhydrous) Chemical compound [Cl-].[Cl-].[Sn+2] AXZWODMDQAVCJE-UHFFFAOYSA-L 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
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- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 1
Classifications
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- B01J37/341—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation
- B01J37/344—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy
- B01J37/345—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy of ultraviolet wave energy
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- C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
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- 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
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- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
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- C23C18/00—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating
- C23C18/02—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating by thermal decomposition
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Definitions
- Modified porous coatings and a modular device for air treatment containing modified porous coatings are provided.
- the invention concerns porous coatings modified with Ti0 2 or Ti0 2 -Pt and quantum dots as well as a modular device for air treatment containing modified porous coatings.
- Waste waters and solid waste contain contaminants in a form of organic and non-organic compounds, including the aroma compounds, as well as numerous saprophytic or opportunistic microorganisms, and sometimes pathogens or facultative pathogens.
- contaminants during waste water treatment processes and under the applied waste management technologies can be introduced into the air in the form of vapours, dusts, aerosols and bioaerosols and, as a result, they may have negative impact on the health of workers and local residents, and also lead to secondary contamination of soils, waters and plants. They may also migrate with water to deeper soil layers.
- the description CN201399313 presents a device for indoor air treatment, consisting of a filtration fabric layer, two layers of active carbon fibres, a flat layer of granulated active carbon and an UV lamp.
- the activated carbon surface contains Ti0 2 with photocatalytic properties.
- the UV lamp is placed between two active carbon layers. The air flows from the lower to the upper part of the device, while noxious substances are filtered out, absorbed and degraded photocatalytically.
- Devices described in the state of the art do not contain quantum dots, which may be used for the construction of a heterojunction with Ti0 2 with the view to freeing the accumulated charges through the acceleration of transfer and migration of photogenerated charges; if they are constructed using a semi-conductor with the band gap ⁇ 2.8 eV, they can absorb radiation from the visible range, and then they can transfer the electron to the Ti0 2 conductive band.
- the quantum dots may also be used for resonance transfer of excitation energy according to the so- called FRET mechanism.
- the objective of the invention was to develop modified porous coatings and a device containing them, to be used for air treatment that could remove: (a) volatile organic compounds, NOx, S0 2 and (b) microorganisms, such as bacteria and fungi, what could among others enable a reduction of contaminants level and air deodorisation on the territory of landfills and waste water treatment plants, and thus the protect surface and ground waters through the elimination of a serious contamination source.
- Modified porous coatings according to the invention are formed from a porous deposit, preferably ceramic cubes or nanotubes, containing titanium oxide Ti0 2 or titanium oxide surface-modified with platinum Ti0 2 -Pt as well as quantum dots.
- a porous deposit preferably ceramic cubes or nanotubes, containing titanium oxide Ti0 2 or titanium oxide surface-modified with platinum Ti0 2 -Pt as well as quantum dots.
- Ti0 2 or Pt-Ti0 2 in the form of a paste is applied onto the surface of the deposit by means of cubes immersion in the paste, which are later dried and calcined.
- Ti0 2 or Pt-Ti0 2 paste is prepared by mixing and heating of terpineol, butyl carbitol, ethyl cellulose, sorbitan trioleate and dibutyl phtalate until uniform consistency has been obtained, after which Ti0 2 orTi0 2 -Pt is added to the mixture and the components are blended until uniform consistency has been obtained.
- Ti0 2 -Pt is obtained using a chemical reduction method, consisting in the introduction of aqueous solution of K 2 PtCl 4 into the suspension of Ti0 2 in alcohol solution, and the subsequent addition of a reducer in the form of sodium borohydride NaBH 4 .
- the resulting Ti0 2 -Pt sediment is rinsed with deionised water and ethanol and dried.
- quantum dots preferably Bi 2 S 3 , Ag 2 S, CdS and SnS
- a chemical bath deposition method consisting in immersing a photocatalyst successively in the cation and anion precursor of the quantum dot.
- a substrate in the form of titanium film is used. At the first stage the film is cleaned by means of immersion in at least one solvent and it is subject to ultrasound treatment.
- the substrate is rinsed with demineralised water stream, dried and placed in an electrolyte, consisting of ethylene glycol, water and ammonium fluoride, and later it is anodised using a platinum net as a cathode.
- formed nanostructures are dried and calcined.
- Platinum nanoparticles are deposited on the surface of Ti0 2 nanotubes using a photodeposition method.
- a titanium board with the formed Ti0 2 nanotubes is immersed in HC1 solution with pH 5.
- the board is immersed in the solution of K 2 Cl 6 Pt metal precursor. Then isopropanol is introduced into the photoreactor and it is run through N 2 solution to remove air. In order to immobilise nanoparticles of noble metals, the solutions together with the immersed titanium plate covered with Ti0 2 nanotubes are exposed to UV-Vis radiation. After completed photodeposition the board is subject to drying. Quantum dots are applied to photocatalysts in the form of TiO or Ti0 2 -Pt nanotubes, preferably Ag 2 S or Bi 2 S 3; ones using a chemical bath deposition method, consisting in immersing a photocatalyst successively in the cation and anion precursor of the quantum dot.
- a modular device for air treatment containing modified porous coatings contains a dust removal module for the removal of solid particles, an advanced oxidation module equipped with a reaction chamber for contacting ozone with the contaminated gas phase and a reaction chamber for conducting a photocatalytic reaction with the photocatalytic layer, located on the carrier in the form of a modified porous coating and a radiation source, a residual ozone inactivation module for the removal of ozone remains on the catalytic deposit, and also the adsorption module on activated carbon.
- the chamber for conducting a photocatalyst reaction with a photocatalyst layer and a radiation source operates in the contaminants degradation mode, corresponding to the radiation intensity scope from the radiation source of between 0.2 and 20 mW/cm 2 and in the mode of photocatalytic layer treatment, corresponding to the radiation intensity scope from the radiation source of between 10 and 60 mW/cm 2 .
- the time ratio of device operation in the contaminants degradation mode and in the photocatalytic layer treatment mode is between 5: 1 and 50: 1, preferably between 5: 1 and 15: 1.
- porous coatings modified with Ti0 2 or Ti0 2 -Pt and quantum dots according to the invention is high effectiveness of contaminants removal from the gas phase, and also the possibility of using radiation from the visible scope or low power emitters for the formation of active oxygen forms on the photocatalytic surface, which are responsible for the degradation of organic and non-organic contaminants as well as micro-organisms present in the air.
- a layer of Ti0 2 -Pt modified with quantum dots demonstrated longer usage stability when compared with layers made from Ti0 2 or Ti0 2 -Pt alone, since their surface is not subject to deactivation.
- the advantage of the modular device for air treatment containing modified porous coatings is the application of modern oxidation processes - the combination of photocatalytic oxidation and ozonisation for the removal of contaminants mixture generated on the territory of a waste water treatment plant and landfills.
- the application of the modular device enables the simultaneous degradation of contaminants using the mixture of two strongest oxidisers, hydroxyl radicals and ozone, as well as the inactivation of micro-organisms in the gas phase.
- Fig. 1 presents the pictures of obtained Ti0 2 and Ti0 2 -Pt pastes from the left to the right
- Fig. 2 presents the pictures of ceramic cubes immersed in the pastes and cubes after calcination
- Fig. 3 presents the diagram of the modular device for air treatment containing a dust removal module 1, an advanced oxidation- ozonisation module 2b, an advanced oxidation - photocatalysis module 2a, residual ozone removal module 3, and adsorption on active carbon module 4.
- Example 1 Obtaining T1O 2 surface-modified with platinum using a chemical reduction method.
- Ti0 2 10 g were added into the beaker containing 75 ml of deionised water and 75 ml of ethanol and the mixture was stirred using a magnetic stirrer for 1 hour. Then appropriate amount of aqueous solution of K 2 PtCl 4 with the concentration of 0.000125 M was added into Ti0 2 suspension and it was stirred for half an hour. At the next stage the reducer in the form of sodium borohydride NaBH 4 was added to the suspension and it was stirred for 1 h. Finally, Ti0 2 sediment modified with platinum was rinsed a couple of times with deionised water and ethanol, after which it was dried at the temperature of 50 °C for 5h. 0.1 mole % of platinum was sedimented on the surface of titanium dioxide.
- Example 2 Obtaining T1O 2 surface- modified with platinum and pure Ti0 2 paste
- 7.5 ml of terpineol, 120 ml of butyl carbitol, 4.5 g of ethyl cellulose, 7.5 ml of Span 85 and 7.5 ml of dibutyl phtalate were added into a ceramic vessel. Then the components were stirred and heated while maintaining the temperature of 70 °C until uniform consistency was obtained. Upon obtaining uniform consistency, 10 g of Ti0 2 orTi0 2 -Pt were added into the ceramic vessel and blended. The blending was conducted until obtaining uniform consistency.
- Fig. 1 presents the pictures of obtained Ti0 2 pastes.
- Each of the prepared Ti0 2 and Ti0 2 -Pt pastes was applied onto ceramic cubes with the dimensions of 2x3 cm by means of immersion of the cubes in the paste for 5 minutes, 2.5 minutes per each side. After removal from the paste the ceramic cubes were blown through with an air stream with the view to excess paste removal. All obtained layers were subject to drying at 120 °C for 3 hours and later to calcination at 450°C - with temperature increase of 10°C/min up to 450°C, which was maintained for 3h.
- Fig. 2 presents the picture of ceramic cubes immersed in the pastes and cubes after calcination.
- Example 4 The application of quantum dots onto Ti0 2 -Pt and pure Ti0 2 catalysts deposited on ceramic cubes.
- a chemical bath deposition method was used for the application of quantum dots on photocatalysts surface.
- this method consists in immersing a photocatalyst successively in the cation and anion precursor of the quantum dot.
- the detailed description of application of four different quantum dots onto the surface of Ti0 2 -Pt and pure Ti0 2 catalysts deposited on ceramic cubes has been presented below.
- ceramic cubes with the applied Ti0 2 -Pt and pure Ti0 2 photocatalyst were immersed for 5 minutes in 0.03 M of AgN0 3 solution, being the ethanol/ water solution in a volume-to-volume ration of 4/1 and they were rinsed with ethanol, and later immersed for the next 5 minutes in 0.03 M of Na 2 S solution, being the ethanol/ water solution in a volume-to-volume ration of 4/1 and rinsed with ethanol. These activities were repeated five times.
- the obtained photocatalysts were dried at the temperature of 60 °C for 6 hours.
- Bi 2 S 3 , Ag 2 S, CdS and SnS quantum dots were also applied onto clean ceramic cubes without photocatalysts in the form of pure Ti0 2 surface-modified with platinum.
- Ti0 2 cube A ceramic cube with Ti0 2 78% 0
- Ti0 2 cube A ceramic cube with Ti0 2 78% 0
- Example 5 Obtaining porous photocatalysts in the form of Ti0 2 nanotubes.
- a substrate in the form of titanium film is used for the formation of photocatalytic layers in the form of Ti0 2 nanotubes.
- Film preparation included its purification by means of subsequent immersion in acetone, isopropanol and methanol as well as ultrasound treatment in each of the above-mentioned solvents for 10 minutes. Then the substrate was rinsed with a demineralised water stream and dried in the air. During the next procedure stage a base material was placed in electrolyte consisting of 98 volume % of ethylene glycol, 2 volume % of water and 0.09 mole/dm 3 of ammonium fluoride, after which it was anodised for 60 minutes using a platinum net as a cathode under 30 V voltage.
- the matrix of Ti0 2 nanotubes was formed on the surface of base material during the electrochemical process.
- the base material with the formed matrix of Ti0 2 nanotubes was removed from the solution, rinsed with demineralised water and dried in the air for 12 h, after which it was placed in a vessel with demineralised water and exposed to ultrasounds for 5 minutes with the view to removal of surface contaminants. Then the formed nanostructures were dried at 80 °C for 24 h.
- the matrix of Ti0 2 nanotubes on the titanium base was placed in the furnace and it was calcined in air atmosphere with the temperature increase of 2°C/min until reaching the temperature of 450 °C, which was maintained for 1 h.
- Example 6 Obtaining porous photocatalysts in the form of Ti0 2 nanotubes surface- modified with platinum.
- Platinum nanoparticles on the surface of Ti0 2 nanotubes were deposited using a photodeposition method.
- a titanium board with the formed Ti0 2 nanotubes is immersed in HC1 solution with pH 5 during 10 minutes. Then the board was immersed in 30 cm 3 solution of K 2 Cl 6 Pt metal precursor without previous rinsing. After 2 h 0.69 cm 3 of isopropanol was introduced into the photoreactor and it was run through N 2 solution for 1 h with the view to air removal. With the view to immobilising nanoparticles of noble metals, the solutions together with the immersed titanium plate covered with Ti0 2 nanotubes were exposed to UV-Vis radiation for 2 h using a xenon lamp with the power of 250 W.
- Example 7 Applying quantum dots onto photocatalysts in the form of Ti0 2 nanotubes surface-modified with platinum nanoparticles.
- Ti0 2 nanotubes surface-modified with platinum were immersed for 5 minutes in 0.03 M of AgN0 3 solution, being the ethanol/ water solution in a volume-to-volume ration of 4/1, they were rinsed with ethanol and later immersed for the next 5 minutes in 0.03 M of Na 2 S solution, being the ethanol/ water solution in a volume-to-volume ration of 4/1 and they were rinsed with ethanol. These activities were repeated 2, 4, 6 and 8 times.
- the obtained photocatalysts were dried at the temperature of 60 °C for 6 hours.
- Ti0 2 nanotubes surface-modified with platinum were immersed for 5 minutes in 4 mM of Bi(N0 3 ) 3 solution in acetone, rinsed with acetone and later immersed for the next 5 minutes in 0.25 M of aqueous Na 2 S solution and rinsed with water. These activities were repeated 2, 4 and 6 times.
- the obtained photocatalysts were dried at the temperature of 60 °C for 6 hours.
- Bi 2 S 3 and Ag 2 S quantum dots were also applied to clean T1O 2 nanotubes which were not surface modified with platinum.
- the activity of toluene samples degradation using different variants of photocatalyst nanotubes was measured in the presence of a LED 375 nm diode after 20 minutes and a LED 465 nm diode after 60 minutes.
- the best conditions correspond to the content of platinum and/ or quantum dot on the surface of T1O 2 nanotubes, at which the highest degree of toluene degradation was observed.
- Example 8 A modular device for air treatment and deodorising
- a device for the air treatment and deodorising consists of four basic modules: dust removal 1, advanced oxidation- ozonisation 2b, advanced oxidation - photocatalysis 2a, residual ozone removal 3, and adsorption on active carbon 4.
- the diagram of a modular device has been presented in Fig. 3.
- Equipping the installation in the preliminary dust removal module 1 enables the removal of solids particles from the air stream entering the advanced oxidation module and thus it extends the operation time and effectiveness of this module.
- the advanced oxidation module enables the degradation of contaminants using hydroxyl radicals with the oxidation potential of 2.80 V in the photocatalytic part 2a and then the oxidation of contaminants using strong oxidation in the form of ozone with the oxidation potential of 2.07 V in the ozonising part 2b.
- the combination of nonselective hydroxyl radicals and selective oxidiser in the form of ozone enables the increase of degradation effectiveness of contaminants and micro-organisms which contaminate the air, including highly resistant malodorous compounds.
- a chamber for conducting a photocatalyst reaction 2a with a photocatalyst layer and a radiation source operates in the mode of contaminants degradation, corresponding to the radiation intensity scope from the radiation source of 0.2 mW/cm 2 and in the mode of photocatalytic layer treatment, corresponding to the radiation intensity scope from the radiation source of 10 mW/cm 2 .
- the time ratio of device operation in the contaminants degradation mode and in the photocatalytic layer treatment mode is 5: 1.
- the residual ozone inactivation module 3 enables the destruction of unreacted ozone and thus it protects against 0 3 emissions into the environment.
- Equipping the installation in the module of adsorption on active carbon 4 enables the removal of volatile remains of organic contaminants in the outlet stream.
- the installation is equipped with sensors enabling the monitoring of both ozone content and the content of a model organic substance in the outlet stream, which enables constant control of effectiveness of device operation, which has not been presented in Fig. 3.
- the essential element of the device is an advanced oxidation module equipped with a reaction chamber for contacting ozone with the contaminated gas phase and a reaction chamber for conducting a photocatalytic reaction with the photocatalytic layer, located on the carrier in the form of a modified porous coating and a radiation source.
- the modular system enables easy adaptation of the installation to individual requirements in the application site, depending on the volume of contaminated air stream, the type and concentration of contaminants and the requirements concerning the contaminants content in the treated air.
- the effectiveness of the installation can be easily increased by multiplying specific modules.
- the installation can also be used for internal air treatment in production halls, public utility buildings, sports facilities and health service buildings.
- An air stream in the volume of 60 m 3 /h was introduced into the modular installation with the view to determining the effectiveness of contaminants removal, which corresponded to linear flow speed through specific modules equal to 0.1 m/s.
- Two ozonisation modules were used at the advanced oxidation stage, each of them containing 10 ozone lamps, which together ensured the production of ozone in the amount corresponding to the concentration of at least 25 ppm.
- photocatalytic layers of which (each with the geometrical surface of 0.16 m 2 ) were constructed from porous ceramic material with the thickness of 20 mm, onto which Ti0 2 based pastes were applied, subsequently subject to drying at 120°C and calcination at 450°C.
- the surface of photocatalytic layers was evenly lit with lamps emitting radiation within the UV-A range with the intensity of 20 mW/cm 2 .
- the air stream leaving the photocatalytic and ozonisation modules connected in series only contained trace remains of organic contaminants, i.e.
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Abstract
Modified porous coatings formed from a porous deposit, preferably ceramic cubes or nanotubes, containing titanium oxide Ti02 or titanium oxide surface-modified with platinum TiO2-Pt as well as quantum dots. A modular device for air treatment containing modified porous coatings characterised in that it contains a dust removal module (1) for the removal of solid particles, an advanced oxidation module equipped with a chamber for conducting a photocatalytic reaction (2a) with the photocatalytic layer placed on the carrier in the form of a modified porous coating and a radiation source as well as a reaction chamber (2b) for contacting ozone with the contaminated gas phase, a residual ozone inactivation module (3) for the removal of ozone remains on the catalytic deposit, and also the adsorption module on activated carbon (4).
Description
Modified porous coatings and a modular device for air treatment containing modified porous coatings.
The invention concerns porous coatings modified with Ti02 or Ti02-Pt and quantum dots as well as a modular device for air treatment containing modified porous coatings.
Waste waters and solid waste contain contaminants in a form of organic and non-organic compounds, including the aroma compounds, as well as numerous saprophytic or opportunistic microorganisms, and sometimes pathogens or facultative pathogens. Such contaminants during waste water treatment processes and under the applied waste management technologies can be introduced into the air in the form of vapours, dusts, aerosols and bioaerosols and, as a result, they may have negative impact on the health of workers and local residents, and also lead to secondary contamination of soils, waters and plants. They may also migrate with water to deeper soil layers.
At the moment in Poland air streams emitted on the territory of a waste water treatment plant or on landfills are either not subject to any treatment/ deodorising, or biological methods are used, including biofilters. An undoubted advantage of biofiltration is a low cost of air treatment when compared with chemical methods. However, such technologies only enable the treatment of streams with low contaminants load. The effectiveness of work performed by microorganisms depends not only on the type and concentration of contaminants in the gas phase, but also on the temperature of the environment. Therefore, the operation of biofilters is not stable upon seasonal temperature variations. A sophisticated matrix in case of air streams emitted in such plants, being a mixture of organic and non-organic compounds as well as micro-organisms, and also huge negative impact on the environment and local residents require the development of modern and effective technologies of removing contaminants from the gas phase.
Filters containing photocatalyst particles on their surface are known in the state of art. The description KR100535940 presents a device for air treatment, containing a semi-permanent photocatalytic filter. The device contains a Ti02 layer for the treatment of air leaving the pre-treatment filter, as well as an UV lamp which activates Ti02, sterilizes and treats contaminated air.
The description CN201399313 presents a device for indoor air treatment, consisting of a filtration fabric layer, two layers of active carbon fibres, a flat layer of granulated active carbon and an UV lamp. The activated carbon surface contains Ti02 with photocatalytic properties. The UV lamp is placed between two active carbon layers. The air flows from the lower to the upper part of the device, while noxious substances are filtered out, absorbed and degraded photocatalytically.
Devices described in the state of the art do not contain quantum dots, which may be used for the construction of a heterojunction with Ti02 with the view to freeing the accumulated charges through the acceleration of transfer and migration of photogenerated charges; if they are constructed using a semi-conductor with the band gap <2.8 eV, they can absorb radiation from the visible range, and then they can transfer the electron to the Ti02 conductive band. The quantum dots may also be used for resonance transfer of excitation energy according to the so- called FRET mechanism. The objective of the invention was to develop modified porous coatings and a device containing them, to be used for air treatment that could remove: (a) volatile organic compounds, NOx, S02 and (b) microorganisms, such as bacteria and fungi, what could among others enable a reduction of contaminants level and air deodorisation on the territory of landfills and waste water treatment plants, and thus the protect surface and ground waters through the elimination of a serious contamination source.
Modified porous coatings according to the invention are formed from a porous deposit, preferably ceramic cubes or nanotubes, containing titanium oxide Ti02 or titanium oxide surface-modified with platinum Ti02-Pt as well as quantum
dots. In the case of modified porous coatings in the form of ceramic cubes, Ti02 or Pt-Ti02 in the form of a paste is applied onto the surface of the deposit by means of cubes immersion in the paste, which are later dried and calcined. Ti02 or Pt-Ti02 paste is prepared by mixing and heating of terpineol, butyl carbitol, ethyl cellulose, sorbitan trioleate and dibutyl phtalate until uniform consistency has been obtained, after which Ti02 orTi02-Pt is added to the mixture and the components are blended until uniform consistency has been obtained. Ti02-Pt is obtained using a chemical reduction method, consisting in the introduction of aqueous solution of K2PtCl4 into the suspension of Ti02 in alcohol solution, and the subsequent addition of a reducer in the form of sodium borohydride NaBH4. The resulting Ti02-Pt sediment is rinsed with deionised water and ethanol and dried. Then quantum dots, preferably Bi2S3, Ag2S, CdS and SnS, are applied to TiO or Ti02-Pt photocatalysts surface using a chemical bath deposition method, consisting in immersing a photocatalyst successively in the cation and anion precursor of the quantum dot. In a case of modified porous coatings in a form of Ti02 or Ti02-Pt nanotubes, a substrate in the form of titanium film is used. At the first stage the film is cleaned by means of immersion in at least one solvent and it is subject to ultrasound treatment. Then the substrate is rinsed with demineralised water stream, dried and placed in an electrolyte, consisting of ethylene glycol, water and ammonium fluoride, and later it is anodised using a platinum net as a cathode. The matrix of Ti02 nanotubes formed during the electrochemical process on the surface of the base material, which is later rinsed with demineralised water, dried and exposed to ultrasounds with the view to removal of surface contaminants. Thus formed nanostructures are dried and calcined. Platinum nanoparticles are deposited on the surface of Ti02 nanotubes using a photodeposition method. A titanium board with the formed Ti02 nanotubes is immersed in HC1 solution with pH 5. During the subsequent stage the board is immersed in the solution of K2Cl6Pt metal precursor. Then isopropanol is introduced into the photoreactor and it is run through N2 solution to remove air. In order to immobilise nanoparticles of noble metals, the solutions together with the
immersed titanium plate covered with Ti02 nanotubes are exposed to UV-Vis radiation. After completed photodeposition the board is subject to drying. Quantum dots are applied to photocatalysts in the form of TiO or Ti02-Pt nanotubes, preferably Ag2S or Bi2S3; ones using a chemical bath deposition method, consisting in immersing a photocatalyst successively in the cation and anion precursor of the quantum dot.
A modular device for air treatment containing modified porous coatings according to the invention contains a dust removal module for the removal of solid particles, an advanced oxidation module equipped with a reaction chamber for contacting ozone with the contaminated gas phase and a reaction chamber for conducting a photocatalytic reaction with the photocatalytic layer, located on the carrier in the form of a modified porous coating and a radiation source, a residual ozone inactivation module for the removal of ozone remains on the catalytic deposit, and also the adsorption module on activated carbon. The chamber for conducting a photocatalyst reaction with a photocatalyst layer and a radiation source operates in the contaminants degradation mode, corresponding to the radiation intensity scope from the radiation source of between 0.2 and 20 mW/cm2 and in the mode of photocatalytic layer treatment, corresponding to the radiation intensity scope from the radiation source of between 10 and 60 mW/cm2. The time ratio of device operation in the contaminants degradation mode and in the photocatalytic layer treatment mode is between 5: 1 and 50: 1, preferably between 5: 1 and 15: 1.
The advantage of porous coatings modified with Ti02 or Ti02-Pt and quantum dots according to the invention is high effectiveness of contaminants removal from the gas phase, and also the possibility of using radiation from the visible scope or low power emitters for the formation of active oxygen forms on the photocatalytic surface, which are responsible for the degradation of organic and non-organic contaminants as well as micro-organisms present in the air. A layer of Ti02-Pt modified with quantum dots demonstrated longer usage stability when compared with layers made from Ti02 or Ti02-Pt alone, since their surface is not subject to deactivation.
The advantage of the modular device for air treatment containing modified porous coatings is the application of modern oxidation processes - the combination of photocatalytic oxidation and ozonisation for the removal of contaminants mixture generated on the territory of a waste water treatment plant and landfills. The application of the modular device enables the simultaneous degradation of contaminants using the mixture of two strongest oxidisers, hydroxyl radicals and ozone, as well as the inactivation of micro-organisms in the gas phase.
The subject of the invention was presented in the Examples in the figures, in which Fig. 1 presents the pictures of obtained Ti02 and Ti02-Pt pastes from the left to the right, Fig. 2 presents the pictures of ceramic cubes immersed in the pastes and cubes after calcination, Fig. 3 presents the diagram of the modular device for air treatment containing a dust removal module 1, an advanced oxidation- ozonisation module 2b, an advanced oxidation - photocatalysis module 2a, residual ozone removal module 3, and adsorption on active carbon module 4.
Example 1. Obtaining T1O2 surface-modified with platinum using a chemical reduction method.
10 g of Ti02 were added into the beaker containing 75 ml of deionised water and 75 ml of ethanol and the mixture was stirred using a magnetic stirrer for 1 hour. Then appropriate amount of aqueous solution of K2PtCl4 with the concentration of 0.000125 M was added into Ti02 suspension and it was stirred for half an hour. At the next stage the reducer in the form of sodium borohydride NaBH4 was added to the suspension and it was stirred for 1 h. Finally, Ti02 sediment modified with platinum was rinsed a couple of times with deionised water and ethanol, after which it was dried at the temperature of 50 °C for 5h. 0.1 mole % of platinum was sedimented on the surface of titanium dioxide.
Example 2. Obtaining T1O2 surface- modified with platinum and pure Ti02paste
At first, 7.5 ml of terpineol, 120 ml of butyl carbitol, 4.5 g of ethyl cellulose, 7.5 ml of Span 85 and 7.5 ml of dibutyl phtalate were added into a
ceramic vessel. Then the components were stirred and heated while maintaining the temperature of 70 °C until uniform consistency was obtained. Upon obtaining uniform consistency, 10 g of Ti02 orTi02-Pt were added into the ceramic vessel and blended. The blending was conducted until obtaining uniform consistency. Fig. 1 presents the pictures of obtained Ti02 pastes.
Example 3. Pastes application onto ceramic cubes
Each of the prepared Ti02 and Ti02-Pt pastes was applied onto ceramic cubes with the dimensions of 2x3 cm by means of immersion of the cubes in the paste for 5 minutes, 2.5 minutes per each side. After removal from the paste the ceramic cubes were blown through with an air stream with the view to excess paste removal. All obtained layers were subject to drying at 120 °C for 3 hours and later to calcination at 450°C - with temperature increase of 10°C/min up to 450°C, which was maintained for 3h. Fig. 2 presents the picture of ceramic cubes immersed in the pastes and cubes after calcination. Example 4. The application of quantum dots onto Ti02-Pt and pure Ti02 catalysts deposited on ceramic cubes.
A chemical bath deposition method was used for the application of quantum dots on photocatalysts surface. In short this method consists in immersing a photocatalyst successively in the cation and anion precursor of the quantum dot. The detailed description of application of four different quantum dots onto the surface of Ti02-Pt and pure Ti02 catalysts deposited on ceramic cubes has been presented below.
• A CdS quantum dot
At first, ceramic cubes with the applied Ti02-Pt and pure Ti02 photocatalyst were immersed for 5 minutes in 0.5 M of pure Cd(N03)2 solution in ethanol, rinsed with ethanol and later immersed for the next 5 minutes in 0.2 M of Na2S solution in methanol and rinsed with methanol. These activities were repeated five times. The obtained photocatalysts were dried at the temperature of 60 °C for 6 hours.
• A SdS quantum dot
At first, ceramic cubes with the applied Ti02-Pt and pure Ti02 photocatalyst were immersed for 5 minutes in 0.5 M of aqueous SnCl2 solution, rinsed with water and later immersed for the next 5 minutes in 0.2 M of aqueous Na2S solution and rinsed with water. These activities were repeated five times. The obtained photocatalysts were dried at the temperature of 60 °C for 6 hours.
• An Ag2S quantum dot
At first, ceramic cubes with the applied Ti02-Pt and pure Ti02 photocatalyst were immersed for 5 minutes in 0.03 M of AgN03 solution, being the ethanol/ water solution in a volume-to-volume ration of 4/1 and they were rinsed with ethanol, and later immersed for the next 5 minutes in 0.03 M of Na2S solution, being the ethanol/ water solution in a volume-to-volume ration of 4/1 and rinsed with ethanol. These activities were repeated five times. The obtained photocatalysts were dried at the temperature of 60 °C for 6 hours.
• A Bi2S3 quantum dot
At first, ceramic cubes with the applied Ti02-Pt and pure Ti02 photocatalyst were immersed for 5 minutes in 4 M of Bi(N03)3 solution in acetone, rinsed with acetone and later immersed for the next 5 minutes in 0.25 M of aqueous Na2S solution and rinsed with water. These activities were repeated five times. The obtained photocatalysts were dried at the temperature of 60 °C for 6 hours.
Bi2S3, Ag2S, CdS and SnS quantum dots were also applied onto clean ceramic cubes without photocatalysts in the form of pure Ti02 surface-modified with platinum.
The activity of toluene samples degradation using different variants of photocatalyst cubes was measured in the presence of a LED 375 nm diode after 20 minutes and a LED 465 nm diode after 60 minutes.
Table 1 Toluene degradation in the presence of CdS QD - Pt - Ti02 photocatalyst cube
Table 3 Toluene degradation in the presence of Ag2S QD - Pt - Ti02 photocatalyst cube
Sample name Short sample description Toluene Toluene
degradation [%] degradation [%] of the LED 375 of the LED 465 nm diode after nm diode after 20 minutes 60 minutes a cube A ceramic cube 0 0
Ti02 cube A ceramic cube with Ti02 78% 0
Pt - Ti02 cube A ceramic cube with Ti02 86% 30%
surface-modified with platinum
an Ag2S QD - ΤΊ02 cube A ceramic cube bearing a 88% 50%
quantum dot
an Ag2S QD - Pt - Ti02 A ceramic cube with Ti02 96% 61% cube surface-modified with platinum
bearing a quantum dot
Table 4 Toluene degradation in the presence of Bi2S3 QD - Pt - Ti02 photocatalyst cube
Sample name Short sample description Toluene Toluene
degradation [%] degradation [%] of the LED 375 of the LED 465 nm diode after nm diode after
20 minutes 60 minutes a cube A ceramic cube 0 0
Ti02 cube A ceramic cube with Ti02 78% 0
Pt - Ti02 cube A ceramic cube with Ti02 86% 30%
surface-modified with platinum
a Bi2S3 QD - Ti02 cube A ceramic cube bearing a 89% 47%
quantum dot
a Bi2S3 QD - Pt - Ti02 cube A ceramic cube with Ti02 95% 56%
surface-modified with platinum
bearing a quantum dot
Both in the case of UV radiation (LED 375 nm) and in the case of Vis radiation (LED 465 nm), a significant growth of effectiveness of toluene removal from the gas phase was observed.
Example 5. Obtaining porous photocatalysts in the form of Ti02 nanotubes.
A substrate in the form of titanium film is used for the formation of photocatalytic layers in the form of Ti02 nanotubes. Film preparation included its purification by means of subsequent immersion in acetone, isopropanol and methanol as well as ultrasound treatment in each of the above-mentioned solvents for 10 minutes. Then the substrate was rinsed with a demineralised water stream and dried in the air. During the next procedure stage a base material was placed in electrolyte consisting of 98 volume % of ethylene glycol, 2 volume % of water and 0.09 mole/dm3 of ammonium fluoride, after which it was anodised for 60 minutes
using a platinum net as a cathode under 30 V voltage. The matrix of Ti02 nanotubes was formed on the surface of base material during the electrochemical process. The base material with the formed matrix of Ti02 nanotubes was removed from the solution, rinsed with demineralised water and dried in the air for 12 h, after which it was placed in a vessel with demineralised water and exposed to ultrasounds for 5 minutes with the view to removal of surface contaminants. Then the formed nanostructures were dried at 80 °C for 24 h. During the last stage the matrix of Ti02 nanotubes on the titanium base was placed in the furnace and it was calcined in air atmosphere with the temperature increase of 2°C/min until reaching the temperature of 450 °C, which was maintained for 1 h.
Example 6. Obtaining porous photocatalysts in the form of Ti02 nanotubes surface- modified with platinum.
Platinum nanoparticles on the surface of Ti02 nanotubes were deposited using a photodeposition method. A titanium board with the formed Ti02 nanotubes is immersed in HC1 solution with pH 5 during 10 minutes. Then the board was immersed in 30 cm3 solution of K2Cl6Pt metal precursor without previous rinsing. After 2 h 0.69 cm3 of isopropanol was introduced into the photoreactor and it was run through N2 solution for 1 h with the view to air removal. With the view to immobilising nanoparticles of noble metals, the solutions together with the immersed titanium plate covered with Ti02 nanotubes were exposed to UV-Vis radiation for 2 h using a xenon lamp with the power of 250 W. After the completed photodeposition the board was dried at the temperature of 110°C during 12h. Three different platinum quantities were deposited on the surface of Ti02 nanotubes: 0.5, 1.0 and 1.5 mole %. Example 7. Applying quantum dots onto photocatalysts in the form of Ti02 nanotubes surface-modified with platinum nanoparticles.
• An Ag2S quantum dot
At first, Ti02 nanotubes surface-modified with platinum were immersed for 5 minutes in 0.03 M of AgN03 solution, being the ethanol/ water solution in a
volume-to-volume ration of 4/1, they were rinsed with ethanol and later immersed for the next 5 minutes in 0.03 M of Na2S solution, being the ethanol/ water solution in a volume-to-volume ration of 4/1 and they were rinsed with ethanol. These activities were repeated 2, 4, 6 and 8 times. The obtained photocatalysts were dried at the temperature of 60 °C for 6 hours.
• A Bi2S3 quantum dot
At first, Ti02 nanotubes surface-modified with platinum were immersed for 5 minutes in 4 mM of Bi(N03)3 solution in acetone, rinsed with acetone and later immersed for the next 5 minutes in 0.25 M of aqueous Na2S solution and rinsed with water. These activities were repeated 2, 4 and 6 times. The obtained photocatalysts were dried at the temperature of 60 °C for 6 hours.
Bi2S3 and Ag2S quantum dots were also applied to clean T1O2 nanotubes which were not surface modified with platinum.
The activity of toluene samples degradation using different variants of photocatalyst nanotubes was measured in the presence of a LED 375 nm diode after 20 minutes and a LED 465 nm diode after 60 minutes. The best conditions correspond to the content of platinum and/ or quantum dot on the surface of T1O2 nanotubes, at which the highest degree of toluene degradation was observed.
Table 5 Toluene degradation in the presence of Bi2S3 QD - Pt - T1O2 NTs photocatalyst
Sample name Short sample Toluene Toluene description degradation degradation
[%] of the [%] of the
LED 375 nm LED 465 nm diode after 20 diode after 60 minutes minutes
Ti02 NTs Clean nanotubes 65% 3%
0.5%Pt-TiO2 NTs Samples differing by 77% 25%
1.0%Pt-TiO2 NTs platinum content 80% 30%
1.5%Pt-Ti02 NTs 72% 22%
10Bi2S3-TiO2 NTs The samples which 85% 33%
20Bi2S3-TiO2 NTs differed by the amount 90% 40%
30Bi2S3-TiO2 NTs of the quantum dot on 81% 36%
the nanotubes surface
20Bi2S3-1.0%Pt -Ti02 Best conditions 100% 47% NTs
Table 6 Toluene degradation in the presence of Ag2S QD - Pt - Ti02 NTs photocatalyst
Example 8. A modular device for air treatment and deodorising
A device for the air treatment and deodorising consists of four basic modules: dust removal 1, advanced oxidation- ozonisation 2b, advanced oxidation - photocatalysis 2a, residual ozone removal 3, and adsorption on active carbon 4.
The diagram of a modular device has been presented in Fig. 3. Equipping the installation in the preliminary dust removal module 1 enables the removal of solids particles from the air stream entering the advanced oxidation module and thus it extends the operation time and effectiveness of this module. The advanced oxidation module enables the degradation of contaminants using hydroxyl radicals with the oxidation potential of 2.80 V in the photocatalytic part 2a and then the oxidation of contaminants using strong oxidation in the form of ozone with the
oxidation potential of 2.07 V in the ozonising part 2b. The combination of nonselective hydroxyl radicals and selective oxidiser in the form of ozone enables the increase of degradation effectiveness of contaminants and micro-organisms which contaminate the air, including highly resistant malodorous compounds. A chamber for conducting a photocatalyst reaction 2a with a photocatalyst layer and a radiation source operates in the mode of contaminants degradation, corresponding to the radiation intensity scope from the radiation source of 0.2 mW/cm2 and in the mode of photocatalytic layer treatment, corresponding to the radiation intensity scope from the radiation source of 10 mW/cm2. The time ratio of device operation in the contaminants degradation mode and in the photocatalytic layer treatment mode is 5: 1. The residual ozone inactivation module 3 enables the destruction of unreacted ozone and thus it protects against 03 emissions into the environment. Equipping the installation in the module of adsorption on active carbon 4 enables the removal of volatile remains of organic contaminants in the outlet stream. The installation is equipped with sensors enabling the monitoring of both ozone content and the content of a model organic substance in the outlet stream, which enables constant control of effectiveness of device operation, which has not been presented in Fig. 3.
The essential element of the device is an advanced oxidation module equipped with a reaction chamber for contacting ozone with the contaminated gas phase and a reaction chamber for conducting a photocatalytic reaction with the photocatalytic layer, located on the carrier in the form of a modified porous coating and a radiation source.
The modular system enables easy adaptation of the installation to individual requirements in the application site, depending on the volume of contaminated air stream, the type and concentration of contaminants and the requirements concerning the contaminants content in the treated air. The effectiveness of the installation can be easily increased by multiplying specific modules. The installation can also be used for internal air treatment in production halls, public utility buildings, sports facilities and health service buildings.
An air stream in the volume of 60 m3/h was introduced into the modular installation with the view to determining the effectiveness of contaminants removal, which corresponded to linear flow speed through specific modules equal to 0.1 m/s. The air contained the following model contaminants: toluene (50 ppm), ethanethiol (20 ppm), trimethylamine (20 ppm), butyric acid (10 ppm) and ammonia (20 ppm). Two ozonisation modules were used at the advanced oxidation stage, each of them containing 10 ozone lamps, which together ensured the production of ozone in the amount corresponding to the concentration of at least 25 ppm. Apart from ozonisation modules, two photocatalytic modules were used during the advanced oxidation stage, the photocatalytic layers of which (each with the geometrical surface of 0.16 m2) were constructed from porous ceramic material with the thickness of 20 mm, onto which Ti02 based pastes were applied, subsequently subject to drying at 120°C and calcination at 450°C. The surface of photocatalytic layers was evenly lit with lamps emitting radiation within the UV-A range with the intensity of 20 mW/cm2. The air stream leaving the photocatalytic and ozonisation modules connected in series only contained trace remains of organic contaminants, i.e. <2 ppm (toluene, ethanethiol, trimethylamine, butyric acid), which were later fully absorbed in the first part of the adsorption module containing the active carbon deposit. Ammonia was fully removed in the second part of the adsorption module containing the deposit of 5A molecular sieves. Ozone remains were completely removed in the residual ozone inactivation module, containing a catalyst deposit on the basis of manganese oxide.
Claims
1. Modified porous coatings characterised in that they are formed from a porous deposit, preferably ceramic cubes or nanotubes, the porous deposit containing titanium oxide Ti02 or titanium oxide surface-modified with platinum Ti02-Pt as well as quantum dots.
2. Modified porous coatings according to claim 1, characterised in that Ti02 or Pt-Ti02 in the form of paste is applied onto the surface of ceramic cubes by means of cubes immersion in the paste, drying and calcination.
3. Modified porous coatings according to claim 2 characterised in that Ti02 or Pt-Ti02 paste is prepared by mixing and heating of terpineol, butyl carbitol, ethyl cellulose, sorbitan trioleate and dibutyl phtalate,
4. Modified porous coatings according to claim 3 characterised in that Ti02 or Ti02-Pt is added to the mixture.
5. Modified porous coatings according to claim 4 characterised in that Ti02- Pt is obtained using a chemical reduction method, consisting in the introduction of aqueous solution of K2PtCl4 into the suspension of Ti02 in alcohol solution, and the subsequent addition of a reducer in the form of sodium borohydride NaBH4.
6. Modified porous coatings according to claim 1 or 2 or 3 or 4 or 5, characterised in that quantum dots are applied to the surface of ceramic cubes containing titanium oxide Ti02 or titanium oxide surface-modified with platinum Ti02-Pt, preferably Bi2S3, Ag2S, CdS and SnS; ones using a chemical bath deposition method, consisting in immersing a photocatalyst successively in the cation and anion precursor of the quantum dot.
7. Modified porous coatings according to claim 1, characterised in that a substrate in the form of titanium film is used for the formation of porous coatings in the form of Ti02 or Ti02-Pt nanotubes.
8. Modified porous coatings according to claim 7 characterised in that at the first stage the film is purified by means of immersion in at least one solvent and it is subject to ultrasound treatment.
9. Modified porous coatings according to claim 8 characterised in that the purified film is rinsed with demineralised water streams, dried and placed in an electrolyte, and later is anodised using a platinum net as a cathode.
10. Modified porous coatings according to claim 9 characterised in that the electrolyte contains ethylene glycol and/ or water and/ or ammonium fluoride.
11. Modified porous coatings according to claim 9 or 10 characterised in that the matrix of Ti02 nanotubes formed during the electrochemical process on the surface of the base material is rinsed with demineralised water, dried and exposed to ultrasounds with the view to removal of surface contaminants, after which it is dried and calcined.
12. Modified porous coatings according to claim 7 or 8 or 9 or 10 or 11, characterised in that platinum nanoparticles are deposited on the surface of Ti02 nanotubes using a photodeposition method in a photoreactor.
13. Modified porous coatings according to claim 12 characterised in that a titanium board with the formed Ti02 nanotubes is immersed in HC1 solution with pH 5, and later in the K2Ci6Pt metal precursor solution, after which isopropanol is introduced into the photoreactor and run through N2 solution for air removal, and then the solutions together with the immersed titanium plate covered with Tio2 nanotubes are exposed to UV-Vis radiation and dried.
14. Modified porous coatings according to claim 7 or 8 or 9 or 10 or 1 1 or 12 or 13, characterised in that quantum dots are applied to porous surfaces in the form of Ti02 or Ti02-Pt nanotubes, preferably Ag2S or Bi2S3; using a chemical bath deposition method, consisting in immersing a photocatalyst successively in the cation and anion precursor of the quantum dot.
15. A modular device for air treatment containing modified porous coatings characterised in that it contains a dust removal module (1) for the removal of solid particles, an advanced oxidation module equipped with a chamber for conducting a photocatalytic reaction (2a) with the photocatalytic layer placed on the carrier in the form of a modified porous coating according to
claim 1, or 2, or 3, or 4, or 5, or 6, or 7, or 8, or 9, or 10, or 11 and a radiation source as well as a reaction chamber (2b) for contacting ozone with the contaminated gas phase, a residual ozone inactivation module (3) for the removal of ozone remains on the catalytic deposit, and also the adsorption module on activated carbon (4).
16. A modular device according to the claim 15 characterised in that the chamber for conducting a photocatalyst reaction (2a) with a photocatalyst layer and a radiation source operates in the mode of contaminants degradation, corresponding to the radiation intensity scope from the radiation source of between 0.2 and 20 mW/cm2 and in the mode of photocatalytic layer treatment, corresponding to the radiation intensity scope from the radiation source of between 10 and 60 mW/cm2.
17. A modular device according to the claim 16 characterised in that the time ratio of device operation in the contaminants degradation mode and in the photocatalytic layer treatment mode is between 5: 1 and 50: 1 respectively, preferably between 5: 1 and 15: 1.
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| PL417116A PL417116A1 (en) | 2016-05-05 | 2016-05-05 | Modified porous coatings and the modular device for purification of air that contains the modified porous coatings |
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| CN110550617A (en) * | 2019-10-25 | 2019-12-10 | 广州工程技术职业学院 | Preparation method of carbon quantum dots |
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| CN113101947A (en) * | 2021-03-22 | 2021-07-13 | 华南理工大学 | Silver sulfide-reduced graphene oxide-titanium dioxide composite material and preparation method and application thereof |
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| CN110550617A (en) * | 2019-10-25 | 2019-12-10 | 广州工程技术职业学院 | Preparation method of carbon quantum dots |
| CN111922340A (en) * | 2020-06-30 | 2020-11-13 | 吉林大学 | A method for preparing medical titanium alloy material by laser sintering |
| CN111889137A (en) * | 2020-07-03 | 2020-11-06 | 湖北科技学院 | Full-solar spectrum responsive dual-network hydrogel-based photocatalyst and preparation method thereof |
| CN111889137B (en) * | 2020-07-03 | 2023-08-04 | 湖北科技学院 | Full solar spectrum response type double-network hydrogel-based photocatalyst and preparation method thereof |
| CN113101947A (en) * | 2021-03-22 | 2021-07-13 | 华南理工大学 | Silver sulfide-reduced graphene oxide-titanium dioxide composite material and preparation method and application thereof |
| CN113101947B (en) * | 2021-03-22 | 2022-05-24 | 华南理工大学 | A kind of silver sulfide-reduced graphene oxide-titanium dioxide composite material and preparation method and application thereof |
Also Published As
| Publication number | Publication date |
|---|---|
| EP3452216A1 (en) | 2019-03-13 |
| WO2017192057A4 (en) | 2018-01-25 |
| PL417116A1 (en) | 2017-11-06 |
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