WO1999033564A1 - Photocatalyseurs tres poreux pour la mise en oeuvre de lumiere visible - Google Patents

Photocatalyseurs tres poreux pour la mise en oeuvre de lumiere visible Download PDF

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Publication number
WO1999033564A1
WO1999033564A1 PCT/EP1998/008055 EP9808055W WO9933564A1 WO 1999033564 A1 WO1999033564 A1 WO 1999033564A1 EP 9808055 W EP9808055 W EP 9808055W WO 9933564 A1 WO9933564 A1 WO 9933564A1
Authority
WO
WIPO (PCT)
Prior art keywords
photocatalysts
light
visible light
tio
ions
Prior art date
Application number
PCT/EP1998/008055
Other languages
German (de)
English (en)
Inventor
Horst Kisch
Christian Lange
Wilhelm F. Maier
Ling Zang
Christian Lettmann
Original Assignee
Studiengesellschaft Kohle Mbh
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Studiengesellschaft Kohle Mbh filed Critical Studiengesellschaft Kohle Mbh
Publication of WO1999033564A1 publication Critical patent/WO1999033564A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/72—Treatment of water, waste water, or sewage by oxidation
    • C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
    • B01J35/39—Photocatalytic properties
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
    • H01G9/20—Light-sensitive devices
    • H01G9/2027—Light-sensitive devices comprising an oxide semiconductor electrode
    • H01G9/2031—Light-sensitive devices comprising an oxide semiconductor electrode comprising titanium oxide, e.g. TiO2
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/80—Type of catalytic reaction
    • B01D2255/802—Photocatalytic
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E10/00—Energy generation through renewable energy sources
    • Y02E10/50—Photovoltaic [PV] energy
    • Y02E10/542—Dye sensitized solar cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W10/00—Technologies for wastewater treatment
    • Y02W10/30—Wastewater or sewage treatment systems using renewable energies
    • Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy

Definitions

  • the invention relates to photocatalysts, essentially consisting of metal oxides doped with metal ions with special photocatalytic activity, their production and their use with light in the wavelength range of visible light.
  • this catalyst is decomposed during the reaction, a process that can only be partially suppressed by adding hydrogen peroxide (Bruemann, DW; Bockelmann, D .; Goslich, R .; Hilgendorff, M. In Aquatic and Surface Photochemistry; Schut GR ; Zepp, RG; Crosby, DG, Eds .; Lewis Publishers: Boca Raton, 1994, pp349-367.).
  • the photosensitization by a dye is one with a ruthenium (II) bipyridyl complex loaded nanocrstalline TiO 2 electrode (DE 4207659 A1). It is questionable whether the organic ligands are photostable with longer exposure times.
  • Examples of the photocatalytically active Pt-TiO 2 catalyst produced from Na 2 PtCI 6 x 6 H 2 O and titanium isopropoxide show the presence of atomically isolated PtCI 4 units in titanium dioxide.
  • ESCA investigations electron spectroscopy for chemical analysis
  • High-resolution transmission electron microscopic examinations show that the titanium oxide is present as an amorphous material with nanometer-sized crystalline domains enclosed therein, and Pt can be found homogeneously distributed throughout the material.
  • Suitable catalyst materials with a large surface are materials which essentially contain more than 60% a metal oxide or mixtures of metal oxides of titanium, zinc, iron, manganese, molybdenum or tungsten and less than 40% ions from the group Pt, Rh, Contain Mn, Cr, Ru, Ni, Pd, Fe, Co, Ir, Cu, Mo, Zr, Re, Ag, Au and absorb the light in the visible wavelength range.
  • TiO 2 is preferably used as the metal oxide, preferably doped with Pt or Rh.
  • Another embodiment consists of bringing the components together in the aqueous phase, e.g. B. by bringing together Na 2 PtCI 6 as an aqueous solution with a microporous TiO 2 powder.
  • porous titanium oxide can show photocatalytic activity with visible light if, due to the production process of the titanium oxide, 0.01-10% organic fragments or carbon deposits remain in the titanium dioxide.
  • Such a material that is photocatalytically active in visible light is characterized by a yellowish-brownish to black color.
  • the photocatalysts presented therefore work with visible light and are not subject to decomposition.
  • the production is preferably carried out wet-chemically according to a one-step sol-gel process.
  • the process has the advantage that it immediately provides materials with large surfaces and that both the pore size and the concentration of the active centers can be varied within wide limits by the process.
  • Fig. 1 shows the decrease in the 4-chlorophenol concentration when exposed to visible light (455 nm) in the presence of a conventional (Degussa P25) and a new hybrid catalyst.
  • Air purification indoors and outdoors by photocatalytic degradation of pollutants can also be carried out by coating such thin photocatalytically active layer on the interior walls of rooms, exterior walls of buildings including window and roof areas, walkway slabs and road surfaces.
  • the simplicity of manufacturing these photocatalysts and their adhesion to all mineral surfaces should have an advantageous effect.
  • Even when using the materials to purify water, the use of visible light allows much more effective applications: Since water itself is not for UV but for visible light is practically completely permeable, the coverage of the catalysts with water is much less critical than when using UV light according to the conventional technique.
  • the use of the materials as a solar cell to generate electricity from visible light opens up completely new uses for solar cells, because in contrast to silicon, the sol-gel materials presented here as a thin film at low cost on many materials, such as roof tiles, glass panes, building claddings etc. can be applied.
  • the loosely covered sol was now without stirring for a further 6 days and gelled during this time.
  • the gel was left in the hood without a cover for a further 10 days, during which time it hardened and became brittle.
  • the resulting glass was then heated to 65 ° C. at a heating rate of 0.1 ° C./min, held at this temperature for 100 minutes and then heated to 250 ° C. at the same heating speed.
  • the material was kept at this temperature for 5 h and then cooled to room temperature at a cooling rate of 0.5 ° C./min.
  • the loosely covered sol was now without stirring for a further 8 days and gelled during this time.
  • the gelled pieces were placed in a 250 ml autoclave filled and mixed with 5 bar N 2 .
  • the autoclave was heated slowly (1 ° C / min) to 270 ° C, the pressure rising to about 22 bar. After the end temperature had been reached, the autoclave was slowly let down at 0.1 bar / min. The heating was then switched off and, after reaching room temperature, the autoclave was opened and the finished catalyst was removed.
  • the catalyst was prepared as in Example 1, but instead of the metal salt (1 au), any organic compound soluble in EtOH was added to the sol.
  • the gel obtained was then dried in air, preferably under an inert gas, and fired.
  • a black to yellow colored TiO 2 resulted, which can be used analogously to Example 2-7 as a photocatalytically active material in visible light.
  • the catalyst (0.5 g / l) was suspended in an ultrasonic bath for 15 min in 14 ml of a solution of 4-chlorophenol (2.5x10 '4 M). The mixture was then magnetically stirred for 20 min and then exposed to an Osram XBO 150 W xenon lamp for 3 h with further stirring; an edge filter with wavelengths ⁇ > 400 nm and ⁇ > 455 nm ensured the elimination of UV radiation. The degradation of 4-chlorophenol was followed by high pressure liquid chromatography. Tab. 1
  • the glass plate was placed in the cell provided with rubber seals, covered with the redox electrolyte and with the second
  • Indium tin oxide plate tightly sealed. Exposure to visible light leads to the occurrence of photo tension.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Environmental & Geological Engineering (AREA)
  • Materials Engineering (AREA)
  • Power Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Water Supply & Treatment (AREA)
  • Biomedical Technology (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Hydrology & Water Resources (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Catalysts (AREA)

Abstract

L'invention concerne des oxydes métalliques dopés présentant une activité photocatalytique particulière, leur procédé de production et leur utilisation. Ces nouveaux matériaux permettent la mise en oeuvre de lumière visible dans des applications photocatalytiques, et notamment la purification de l'air et de l'eau, ainsi que la production de courant photoélectrique (cellule photovoltaïque) avec de la lumière dans la plage de longueurs d'onde de la lumière visible.
PCT/EP1998/008055 1997-12-23 1998-12-10 Photocatalyseurs tres poreux pour la mise en oeuvre de lumiere visible WO1999033564A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE1997157496 DE19757496A1 (de) 1997-12-23 1997-12-23 Hochporöse Photokatalysatoren zur Verwertung von sichtbarem Licht
DE19757496.3 1997-12-23

Publications (1)

Publication Number Publication Date
WO1999033564A1 true WO1999033564A1 (fr) 1999-07-08

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PCT/EP1998/008055 WO1999033564A1 (fr) 1997-12-23 1998-12-10 Photocatalyseurs tres poreux pour la mise en oeuvre de lumiere visible

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DE (1) DE19757496A1 (fr)
WO (1) WO1999033564A1 (fr)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1359237A1 (fr) * 2002-05-01 2003-11-05 Ube Industries, Ltd. Fibre photocatalytique contenant de la silice ayant une activité dans une zone de lumière visible et procédé pour sa production
DE102009012461A1 (de) 2009-03-12 2010-09-16 Kme Germany Ag & Co. Kg Schadstoffabbauendes Metallband für das Bauwesen
US8172951B2 (en) 2000-12-21 2012-05-08 Massholder Karl F Method of cleaning with an aqueous composition containing a semiconductor
CN107597145A (zh) * 2017-09-21 2018-01-19 柳州若思纳米材料科技有限公司 一种碳复合硫代钨酸锰催化剂的制备方法

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DE19920753A1 (de) * 1999-04-23 2000-10-26 Bayer Ag Verfahren zur Herstellung von amorphen, edelmetallhaltigen Titan-Silizium-Mischoxiden
EP1214124A1 (fr) * 1999-09-22 2002-06-19 Carrier Corporation Catalyseurs pour la destruction de composes d'organophosphonate
US6596915B1 (en) 1999-09-22 2003-07-22 Carrier Corporation Catalysts for destruction of organophosphonate compounds
DE10013934A1 (de) * 2000-03-21 2001-09-27 Studiengesellschaft Kohle Mbh Poröse dotierte Titanoxide als selektive Oxiations- und Dehydrierkatalysatoren
NL1015634C2 (nl) * 2000-07-06 2002-01-08 Korea Clean Air System Co Werkwijze voor de bereiding van een ferroelektrische fotohalfgeleidende bekleding en inrichting voor het verwijderen van milieuluchtverontreinigingen onder toepassen van deze bekleding en elektrische energie.
FR2813393B1 (fr) * 2000-08-22 2002-10-18 Commissariat Energie Atomique Fabrication d'un capteur chimique a fibre optique comprenant un indicateur colore, utilisable notamment pour la mesure de l'acidite nitrique
DE20120403U1 (de) * 2001-10-11 2002-06-06 Boehme Mario Vorrichtung zur Entkeimung von Wasser
DE102007019166A1 (de) * 2007-04-20 2008-10-30 Fachhochschule Kiel Verfahren zur Herstellung von Substraten für die Oberflächen-verstärkte Raman-Spektroskopie
DE102008020977A1 (de) 2007-04-30 2008-11-06 Henkel Ag & Co. Kgaa Deodorans
EP2722370B1 (fr) 2012-10-17 2014-05-28 STO SE & Co. KGaA Revêtements photocatalytiques avec matières de remplissage
CN104230067B (zh) * 2013-06-08 2017-02-15 中国科学院理化技术研究所 含有机污染物废水的处理装置及方法

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WO1997026991A1 (fr) * 1996-01-22 1997-07-31 Petroleum Energy Center Photocatalyseur, procede de production de ce photocatalyseur, et procede de reaction photocatalytique
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EP0826531A2 (fr) * 1996-08-30 1998-03-04 Kabushiki Kaisha Equos Research Filtre pour la purification de l'air et dispositif de purification de l'air pour automobile

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8172951B2 (en) 2000-12-21 2012-05-08 Massholder Karl F Method of cleaning with an aqueous composition containing a semiconductor
EP1359237A1 (fr) * 2002-05-01 2003-11-05 Ube Industries, Ltd. Fibre photocatalytique contenant de la silice ayant une activité dans une zone de lumière visible et procédé pour sa production
KR100936447B1 (ko) * 2002-05-01 2010-01-13 우베 고산 가부시키가이샤 가시광 활성을 갖는 실리카-기초 광촉매 섬유 및 그제조방법
DE102009012461A1 (de) 2009-03-12 2010-09-16 Kme Germany Ag & Co. Kg Schadstoffabbauendes Metallband für das Bauwesen
CN107597145A (zh) * 2017-09-21 2018-01-19 柳州若思纳米材料科技有限公司 一种碳复合硫代钨酸锰催化剂的制备方法

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