WO2004044486A2 - Substrat emetteur de lumiere pourvu d'un revetement absorbant la lumiere - Google Patents

Substrat emetteur de lumiere pourvu d'un revetement absorbant la lumiere Download PDF

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Publication number
WO2004044486A2
WO2004044486A2 PCT/IB2003/004747 IB0304747W WO2004044486A2 WO 2004044486 A2 WO2004044486 A2 WO 2004044486A2 IB 0304747 W IB0304747 W IB 0304747W WO 2004044486 A2 WO2004044486 A2 WO 2004044486A2
Authority
WO
WIPO (PCT)
Prior art keywords
light
coating
transmitting substrate
lamp
pigment
Prior art date
Application number
PCT/IB2003/004747
Other languages
English (en)
Other versions
WO2004044486A3 (fr
Inventor
Rémy C. BROERSMA
Rene J. Hendriks
Hendrik-Jan Dreuning
Original Assignee
Koninklijke Philips Electronics N.V.
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 Koninklijke Philips Electronics N.V. filed Critical Koninklijke Philips Electronics N.V.
Priority to AU2003272016A priority Critical patent/AU2003272016A1/en
Publication of WO2004044486A2 publication Critical patent/WO2004044486A2/fr
Publication of WO2004044486A3 publication Critical patent/WO2004044486A3/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C17/00—Surface treatment of glass, not in the form of fibres or filaments, by coating
    • C03C17/001—General methods for coating; Devices therefor
    • C03C17/003—General methods for coating; Devices therefor for hollow ware, e.g. containers
    • C03C17/005—Coating the outside
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C17/00—Surface treatment of glass, not in the form of fibres or filaments, by coating
    • C03C17/006—Surface treatment of glass, not in the form of fibres or filaments, by coating with materials of composite character
    • C03C17/007—Surface treatment of glass, not in the form of fibres or filaments, by coating with materials of composite character containing a dispersed phase, e.g. particles, fibres or flakes, in a continuous phase
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C17/00—Surface treatment of glass, not in the form of fibres or filaments, by coating
    • C03C17/006—Surface treatment of glass, not in the form of fibres or filaments, by coating with materials of composite character
    • C03C17/008—Surface treatment of glass, not in the form of fibres or filaments, by coating with materials of composite character comprising a mixture of materials covered by two or more of the groups C03C17/02, C03C17/06, C03C17/22 and C03C17/28
    • C03C17/009—Mixtures of organic and inorganic materials, e.g. ormosils and ormocers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J61/00—Gas-discharge or vapour-discharge lamps
    • H01J61/02—Details
    • H01J61/30—Vessels; Containers
    • H01J61/35—Vessels; Containers provided with coatings on the walls thereof; Selection of materials for the coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01K—ELECTRIC INCANDESCENT LAMPS
    • H01K1/00—Details
    • H01K1/28—Envelopes; Vessels
    • H01K1/32—Envelopes; Vessels provided with coatings on the walls; Vessels or coatings thereon characterised by the material thereof
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C2217/00—Coatings on glass
    • C03C2217/40—Coatings comprising at least one inhomogeneous layer
    • C03C2217/43—Coatings comprising at least one inhomogeneous layer consisting of a dispersed phase in a continuous phase
    • C03C2217/44—Coatings comprising at least one inhomogeneous layer consisting of a dispersed phase in a continuous phase characterized by the composition of the continuous phase
    • C03C2217/45—Inorganic continuous phases
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C2217/00—Coatings on glass
    • C03C2217/40—Coatings comprising at least one inhomogeneous layer
    • C03C2217/43—Coatings comprising at least one inhomogeneous layer consisting of a dispersed phase in a continuous phase
    • C03C2217/46—Coatings comprising at least one inhomogeneous layer consisting of a dispersed phase in a continuous phase characterized by the dispersed phase
    • C03C2217/47—Coatings comprising at least one inhomogeneous layer consisting of a dispersed phase in a continuous phase characterized by the dispersed phase consisting of a specific material
    • C03C2217/475—Inorganic materials
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C2217/00—Coatings on glass
    • C03C2217/40—Coatings comprising at least one inhomogeneous layer
    • C03C2217/43—Coatings comprising at least one inhomogeneous layer consisting of a dispersed phase in a continuous phase
    • C03C2217/46—Coatings comprising at least one inhomogeneous layer consisting of a dispersed phase in a continuous phase characterized by the dispersed phase
    • C03C2217/48—Coatings comprising at least one inhomogeneous layer consisting of a dispersed phase in a continuous phase characterized by the dispersed phase having a specific function
    • C03C2217/485—Pigments

Definitions

  • Light-transmitting substrate provided with a light-absorbing coating
  • the present invention relates to a light-transmitting substrate that is at least partly provided with a light-absorbing coating, said coating comprising a pigment which absorbs part of the visible light.
  • the invention further relates to an electric lamp comprising a light-transmitting lamp vessel that accommodates a light source, wherein said lamp vessel comprises the above light-transmitting substrate.
  • the present invention relates to the light absorbing coating itself.
  • Light-transmitting substrates provided with a light-absorbing coating may be used as color layers on or in front of (incandescent) lamps for general lighting purposes.
  • the substrate may comprise, for example, a colored filter made of a - flat or non-flat shaped - piece of glass, which is designated to be placed in a trajectory of light, said light being generated by a lamp.
  • a light-transmitting substrate is a lamp vessel that is placed over a light source of an electric lamp.
  • Such electric lamps are predominantly used as indicator lamps in vehicles, for example as red-colored light sources in red tail and brake lights of automobiles. Said electric lamps may also be used in traffic lights.
  • the pigments in the light-absorbing coating can scatter the light coming from the lamp filament. If the light-absorbing coating is applied on the lamp vessel of an electric lamp that is placed in an automotive luminaire, the scattering effect can be a real problem for the efficiency of such an automotive luminaire.
  • the automotive luminaire is designed to reflect the light coming from the filament of the lamp. If the light-absorbing coating on the lamp bulb scatters the light, the lamp bulb itself can also be seen as a light source. The light is then distributed differently within the luminaire, resulting in a bad beam pattern of the light on the road.
  • the present invention aims to provide a light-transmitting substrate according to the preamble in which the above disadvantages are obviated. Moreover, the present invention aims to provide a coating that does not show the above disadvantages.
  • the present invention provides a light-transmitting substrate according to the preamble that is characterized in that aluminum oxide is added to the coating during preparation thereof.
  • the aluminum oxide added to the pigment dispersion during preparation thereof acts as a grinding aid. This results in a smaller particle size distribution of the pigments and therefore in a reduction of the scattering of the coating.
  • the hardness index of aluminum oxide is 9. This means that aluminum oxide is a very hard material. Reference is made to diamond, iron oxide, and organic pigments in this connection, which have hardness indices of 10, 5.5 and less than 5, respectively.
  • the aluminum oxide not only contributes to a reduced scattering of the coating, it also acts as a stabilizer for the pigments in the coating.
  • the aluminum oxide prevents pigments from agglomerating during the application and curing processes.
  • Another effect of the addition of aluminum oxide to the pigments in the coating is that the temperature stability thereof is significantly increased.
  • the color point shift of lamps without aluminum oxide in the coating is greater than the color point shift of lamps with aluminum oxide in the coating.
  • the aluminum oxide has a particle size of 10-40 nm, preferably 20-30 nm.
  • a source of Al 2 O 3 that is advantageously used is Alon-C from Degussa ® .
  • the light-absorbing coating comprises pigment particles that are incorporated in a sol-gel matrix.
  • EP-A-1 129 470 in the name of the Applicant discloses a light-absorbing coating that comprises pigment particles incorporated in a sol-gel matrix. Such a coating can resist temperatures of up to 400°C and can be applied in relatively thick layers.
  • the pigment in the light-absorbing coating comprises an organic pigment.
  • organic pigments give a relatively high lumen output in lamps, but have a low temperature stability.
  • inorganic pigments give a relatively low lumen output, but have higher temperature stability. This applies, for example, to red colored lamps for automotive applications.
  • Another problem of pigments is that they suffer from a thermochromic effect, which means that the transmission - or lumen output - of a colored coating decreases as a function of temperature.
  • Organic pigments that can be used comprise, but are not limited to, Pigment
  • Red 177 anthraquinone
  • Pigment Red 264 diketo-pyrrolo-pyrrole
  • Pigment Red 166 azo condensation
  • Chromophtal Yellow (3RT) Further suitable pigments are Red 149 (perylene), Red 122 (quinacridone), Red 257 (Ni-isoindoline), Violet 19 (quinacridone), Blue 15:1 (Cu-phthalocyanine), Green 7 (hal.Cu-phthalocyanine), and Yellow 83 (dyaryl) from "Clariant”.
  • Mixtures of inorganic and organic pigments are also very suitable, for example a mixture of Chromophtal Yellow (3RT) and (zinc)iron oxide, or a mixture of Sicotrans Red 2816L and iron oxide.
  • the present invention also relates to an electric lamp comprising a light- transmitting lamp vessel which accommodates a light source, said lamp vessel comprising a light-transmitting substrate according to the above.
  • At least part of the lamp vessel is provided with the above light- absorbing coating.
  • said electric lamps may advantageously be used as indicator lamps in vehicles, for example as red-colored light sources in red tail and brake lights of automobiles.
  • the lamp vessel of the electric lamp may also be coated with an amber coating, thereby providing an amber-colored light source.
  • the present invention relates to a light-absorbing coating according to the above.
  • Fig. 1 is a side view, partly cut away and partly in cross-section, of an electric lamp in accordance with the invention comprising a lamp cap;
  • Fig. 2 shows an electric lamp provided with a reflector and an adapter
  • Fig. 3 schematically shows a cross-section of the light-absorbing coating according to the invention, applied on a glass substrate;
  • Fig. 4 shows a graph in which the diffuse transmission of two coatings is represented
  • Fig. 5 shows the result of luminance measurements determining the "haze" of coatings.
  • the Figures are purely schematic and not drawn to scale. Particularly for clarity, some dimensions are exaggerated strongly, hi the Figures, like reference numerals refer to like parts whenever possible.
  • Fig. 1 shows an electric lamp in accordance with the invention, part of which is shown in side view, partly cut away, and another part of which is shown in cross-section.
  • the electric lamp comprises a light-transmitting lamp vessel 1, for example made of glass, which is closed in a gaslight manner and in which an electric element 2, being a (spiral- shaped) tungsten incandescent body with a center 4 in the Figure, is axially positioned on an axis 5 and is connected to current conductors 6 which issue from the lamp vessel to the exterior.
  • the lamp shown has a filling of an inert gas, for example an Ar/Ne mixture, with a filling pressure slightly above 5 bar.
  • a lamp cap 10 is firmly connected to the lamp vessel 1.
  • the lamp cap 10 has a synthetic resin housing 11.
  • the housing 11 comprises a flat base portion 7 that is at least substantially perpendicular to the axis 5.
  • the lamp vessel 1 is closed off in a gastight manner by means of a plate 8 of an insulating material, which plate lies in a plane that is at least substantially perpendicular to the axis 5.
  • Electric element 2 is mounted in a previously defined position with respect to the plate 8 during the manufacture of the lamp.
  • the plate 8 of the lamp vessel 1 is pressed home against the base portion by locking means 9, for example ridges, such that the electric element 2 will enter a previously defined position with respect to the reference means 12, for example studs.
  • the studs 12 form part of the lamp cap and are designed to abut against a support 30, for example a reflector, as is visible in Fig. 2.
  • the lamp cap also comprises contact members 14 which are provided with a screen 13 and to which the current conductors 6 of the lamp vessel 1 are connected.
  • the resilient action of the intermediate portion is obtained in that the intermediate portion is made hollow, so that no more than a wall remains as the intermediate portion, whereupon a major portion of the wall is removed by means of two grooves 18 which run perpendicularly to the axis 5.
  • the remaining portion of the wall forms a bridge 19, which is rotated, near the next groove, through an angle of, for example, 180° about the axis 5.
  • the lamp vessel 1 of the electric lamp has a relatively small axial dimension of approximately 22 mm and is suitable for consuming a relatively high power of, for example, 5 to 25 W.
  • the electric lamp has a service life of approximately 6000 hours in this case.
  • Fig. 2 shows the electric lamp provided with a support 30, being a reflector with a transparent plate 33 in the drawing, as well as with an adapter 25.
  • the reflector is provided with a rubber ring 31 retained in a groove 32
  • the rubber ring seals off the opening 26 between the lamp cap and the reflector in a gastight manner.
  • the adapter is provided with standardized contact points 27 which are passed through the bottom plate 28 of the adapter in a gastight manner and are connected to contact members 14 of the lamp cap 10.
  • the lamp cap 10 falls substantially entirely within a cone 36 which has its apex 35 in the center 4 of the electric element 2 and has an apex half angle ⁇ of 25°.
  • the light originating from the electric element 2 can reach the reflecting surface 34 substantially without obstruction and is reflected there at least substantially axially in the direction of the transparent plate 33.
  • Fig. 3 shows a cross-section of the light-absorbing coating according to the invention, applied on a glass substrate.
  • the glass substrate is represented by reference numeral 41, while numeral 42 represent the sol-gel coating matrix.
  • the pigment particles 43 are surrounded by the Al 2 O particles 44 .
  • a sol-gel hydrolysis mixture was made by mixing 4.5 g ethanol, 40.0 g methyltrimethoxysilane (MTMS), 0.86 g tetraethoxysilane (TEOS), and 0.14 g acetic acid, followed by the addition of in 32.0 g water and subjecting said mixture to hydrolysis for 48 hours at room temperature under continuous stirring.
  • MTMS methyltrimethoxysilane
  • TEOS tetraethoxysilane
  • acetic acid 0.14 g
  • a pigment dispersion was made consisting of 50% w/w iron oxide and 50% w/w organic red pigment.
  • Disperbyk 190 a pigment stabilizer consisting of polyethyleneoxide/polypropyleneoxide
  • the inorganic-organic pigment mixture comprising 25 g Sicotrans Red 2816L (commercially available from BASF ® ), which is an iron oxide (Fe 2 O 3 ) needle-shaped pigment with an average particle size of about 35 nm and 25 g Cromophtal Red A2B (Pigment Red 177 - anthraquinone) was added to the solution.
  • the mixture was pre-dispersed with a dissolver for about 15 minutes, subsequently the mixture was dispersed in a Dispermat SL for 8 hours with 1.25 mm yttrium-stabilized zirconia milling beads. The dispersion was filtered over a 7 ⁇ m nylon filter before use.
  • the pigment dispersion and the sol-gel hydrolysis mixture were mixed in a weight ratio of 240 g to 80 g and 20%> methoxypropanol is added.
  • a wetting agent (LO50 from Wacker) was also added.
  • the coating liquid was filtered over a 1 ⁇ m filter.
  • Example IB Preparation of a light-absorbing coating as in 1A, including Al 2 O 3
  • a coating was prepared in the same way as in example 1 A, but in this case 15 g Al 2 O 3 (Alon-C, commercially available from Degussa ® ) was added to the pigment dispersion during preparation thereof.
  • the level of "haze” was determined with a luminance camera for the coatings according to examples 1 A and IB.
  • the percentage of "haze” was 2.25% for the coating according to example 1A.
  • the coating according to example IB gave a "haze” of merely 1.3%.
  • the "haze” is reduced by 40% by the addition of Alon-C.
  • Example 2 Light-absorbing, yellow coating
  • coatings were prepared comprising yellow organic PY110 as the pigment.
  • Coating 2A was prepared without the addition of Al 2 O 3
  • coating 2B was prepared using Al 2 O 3 (Alon-C, commercially available from Degussa ® ) in an amount of 30% by weight with regard to the pigment in the dispersion.
  • Fig. 4 shows the diffuse transmission of the coatings 2 A and 2B. It is clear that the diffuse transmission is reduced in coating 2B.
  • Fig. 5 shows that also in this case the addition of aluminum oxide results in a reduction of the "haze" by 40%.
  • an effect of the addition of aluminum oxide to the pigments in the coating is that the temperature stability thereof is significantly increased.
  • the color point shift of lamps without aluminum oxide in the coating is greater than the color point shift of lamps with aluminum oxide in the coating.
  • Coatings 2A and 2B were tested at temperatures of 300°C, and it was found that the transmissions after exposure to this temperature differed considerably (see table below). Thus coating 2B showed an increased temperature stability of the organic pigment as well as an improved lumen maintenance, compared with coating 2A.

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  • Chemical & Material Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Geochemistry & Mineralogy (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Composite Materials (AREA)
  • Inorganic Chemistry (AREA)
  • Dispersion Chemistry (AREA)
  • Paints Or Removers (AREA)
  • Vessels And Coating Films For Discharge Lamps (AREA)
  • Non-Portable Lighting Devices Or Systems Thereof (AREA)

Abstract

La présente invention concerne un substrat émetteur de lumière pourvu au moins partiellement d'un revêtement absorbant le lumière. Ce revêtement comprend un pigment qui absorbe une partie de la lumière visible. Par ailleurs, on ajoute de l'oxyde d'aluminium à ce revêtement pendant la préparation de ce dernier. Cette invention concerne aussi une lampe électrique, cette lampe comprenant une ampoule émettrice de lumière qui s'adapte à une source lumineuse. Cette ampoule de lampe comprend le substrat émetteur de lumière susmentionné. Cette invention concerne aussi un revêtement absorbant la lumière.
PCT/IB2003/004747 2002-11-14 2003-10-24 Substrat emetteur de lumiere pourvu d'un revetement absorbant la lumiere WO2004044486A2 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU2003272016A AU2003272016A1 (en) 2002-11-14 2003-10-24 Light-transmitting substrate provided with a light-absorbing coating

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
EP02079742.9 2002-11-14
EP02079742 2002-11-14

Publications (2)

Publication Number Publication Date
WO2004044486A2 true WO2004044486A2 (fr) 2004-05-27
WO2004044486A3 WO2004044486A3 (fr) 2004-07-29

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Application Number Title Priority Date Filing Date
PCT/IB2003/004747 WO2004044486A2 (fr) 2002-11-14 2003-10-24 Substrat emetteur de lumiere pourvu d'un revetement absorbant la lumiere

Country Status (4)

Country Link
CN (1) CN1711488A (fr)
AU (1) AU2003272016A1 (fr)
TW (1) TW200500571A (fr)
WO (1) WO2004044486A2 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2006054227A2 (fr) * 2004-11-18 2006-05-26 Koninklijke Philips Electronics N.V. Revetement pour lampes et lampe au moins partiellement recouverte de ce revetement

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3531677A (en) * 1966-12-14 1970-09-29 Sylvania Electric Prod Quartz glass envelope with radiation-absorbing glaze
JP2000323097A (ja) * 1999-05-11 2000-11-24 Matsushita Electronics Industry Corp 蛍光ランプおよび照明器具
EP1077471A1 (fr) * 1999-08-14 2001-02-21 Philips Patentverwaltung GmbH Dispositif émetteur de lumière colorée muni d'une lampe revêtue d'une couche pigmentée
WO2001020641A1 (fr) * 1999-09-13 2001-03-22 Koninklijke Philips Electronics N.V. Lampe electrique
US6287639B1 (en) * 1996-11-15 2001-09-11 Institut für Neue Materialien Gemeinnützige GmbH Composite materials

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3531677A (en) * 1966-12-14 1970-09-29 Sylvania Electric Prod Quartz glass envelope with radiation-absorbing glaze
US6287639B1 (en) * 1996-11-15 2001-09-11 Institut für Neue Materialien Gemeinnützige GmbH Composite materials
JP2000323097A (ja) * 1999-05-11 2000-11-24 Matsushita Electronics Industry Corp 蛍光ランプおよび照明器具
EP1077471A1 (fr) * 1999-08-14 2001-02-21 Philips Patentverwaltung GmbH Dispositif émetteur de lumière colorée muni d'une lampe revêtue d'une couche pigmentée
WO2001020641A1 (fr) * 1999-09-13 2001-03-22 Koninklijke Philips Electronics N.V. Lampe electrique

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
PATENT ABSTRACTS OF JAPAN vol. 2000, no. 14, 5 March 2001 (2001-03-05) -& JP 2000 323097 A (MATSUSHITA ELECTRONICS INDUSTRY CORP), 24 November 2000 (2000-11-24) *

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2006054227A2 (fr) * 2004-11-18 2006-05-26 Koninklijke Philips Electronics N.V. Revetement pour lampes et lampe au moins partiellement recouverte de ce revetement
WO2006054227A3 (fr) * 2004-11-18 2006-08-17 Koninkl Philips Electronics Nv Revetement pour lampes et lampe au moins partiellement recouverte de ce revetement

Also Published As

Publication number Publication date
AU2003272016A8 (en) 2004-06-03
CN1711488A (zh) 2005-12-21
AU2003272016A1 (en) 2004-06-03
WO2004044486A3 (fr) 2004-07-29
TW200500571A (en) 2005-01-01

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