EP1244547A1 - Fluide de preparation de plaques d'impression et son procede d'utilisation - Google Patents

Fluide de preparation de plaques d'impression et son procede d'utilisation

Info

Publication number
EP1244547A1
EP1244547A1 EP00974752A EP00974752A EP1244547A1 EP 1244547 A1 EP1244547 A1 EP 1244547A1 EP 00974752 A EP00974752 A EP 00974752A EP 00974752 A EP00974752 A EP 00974752A EP 1244547 A1 EP1244547 A1 EP 1244547A1
Authority
EP
European Patent Office
Prior art keywords
marking fluid
printing
plate
inkjet
fluid
Prior art date
Legal status (The legal status 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 status listed.)
Withdrawn
Application number
EP00974752A
Other languages
German (de)
English (en)
Inventor
Moshe Frenkel
Murray Figov
Boaz Nitzan
Jankiel Kimelblat
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Scitex Vision Ltd
Original Assignee
Scitex Vision Ltd
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 Scitex Vision Ltd filed Critical Scitex Vision Ltd
Publication of EP1244547A1 publication Critical patent/EP1244547A1/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D11/00—Inks
    • C09D11/30—Inkjet printing inks
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B41—PRINTING; LINING MACHINES; TYPEWRITERS; STAMPS
    • B41C—PROCESSES FOR THE MANUFACTURE OR REPRODUCTION OF PRINTING SURFACES
    • B41C1/00—Forme preparation
    • B41C1/10—Forme preparation for lithographic printing; Master sheets for transferring a lithographic image to the forme
    • B41C1/1066—Forme preparation for lithographic printing; Master sheets for transferring a lithographic image to the forme by spraying with powders, by using a nozzle, e.g. an ink jet system, by fusing a previously coated powder, e.g. with a laser

Definitions

  • the present invention generally relates to the preparation of printing plates using computer-to-plate (CTP) methods involving inkjet printing, and more particularly, to a novel inkjet marking fluid and to a method for direct CTP preparation of offset lithographic printing plates.
  • CTP computer-to-plate
  • Offset lithographic printing has been a popular method of printing for many years, primarily because of the relative ease with which printing plates can be produced.
  • the most widely- used method for plate preparation has remained that which utilizes specially-prepared masking films through which pre-sensitized printing blanks are selectively hardened or softened — according to the chemistry of the plate — by exposure to ultra-violet light.
  • the plate then undergoes a development process, during which the more soluble regions of the plate are washed away.
  • a detailed description of a typical system and the plates used is found in Chapter 20 of the book entitled: Printing Materials: Science and Technology, by Bob Thompson (Pira Int., Leatherhead, Surrey, UK, 1998).
  • a plate-making process is required which has the utmost simplicity, eliminates all chemical processing, and can be effected at a minimal cost for the plate production and for associated equipment.
  • the process should also be rapid.
  • Inkjet printing is a non-impact, digital printing method which allows images to be produced and printed under computer control. Inkjet ink is jetted through very fine nozzles and the resultant ink droplets form an image directly on a substrate. There are two main types of inkjet processes. In one process, usually termed “continuous inkjet printing", a stream of ink drops is electrically charged and then is deflected by an electric field, either directly or indirectly, onto a substrate. The viscosity of inks used in such systems is typically 2 or 3 centipoise.
  • the ink supply is regulated by an actuator such as a piezoelectric actuator of the type used in the Trident Ultrajet Printhead.
  • the pressure produced during the actuation forces a droplet through a nozzle onto the substrate.
  • Inks for DOD inkjet printing do not need to be conductive and their viscosity is typically between 2 and 40 centipoise.
  • European Patent EP503621 owned by Nippon Paint Co., describes two approaches. One approach describes jetting inks onto a presensitized plate which then needs further treatment, including a developing stage with a liquid developer. The other approach uses a non-presensitized plate and the inkjet ink is photosensitive so that it can be hardened onto the plate.
  • European Patent EP533168 owned by Nippon Paint Co., describes the use of a photopolymeric-based inkjet ink together with an ink-absorbing layer on the lithographic plate surface.
  • European Patent EP697282 to Leanders and owned by Agfa, describes a two-component system whereby one reactive component is in the ink and the other in the lithographic plate surface so that when the ink hits the plate it produces an oleophilic, reduced silver image that can be used in the offset printing process.
  • Both water-based and solvent-based inks have problems of spreading of the ink on the high-surface-energy, hydrophilic plate surface due to the properties needed to jet the ink.
  • Phase-change inks have problems with bonding of the wax-like ink to the plate.
  • the present invention overcomes the disadvantages associated with prior art computer-to-plate methods, by providing a simple and inexpensive method of producing an offset lithographic printing plate by use of the inkjet process.
  • the method uses a novel inkjet fluid that, while giving excellent jetting properties with high consistency and quality, can be easily dried on an uncoated lithographic printing plate.
  • a method for the direct CTP preparation of a printing plate comprising the steps of: providing a digital image generated by a computer system; providing an inkjet marking fluid having a preselected viscosity, wherein said marking fluid is comprised of a two-phase emulsion system consisting of an oleophilic inner phase and a continuous, aqueous, external phase; jetting said marking fluid onto a printing surface; and drying said marking fluid on said printing surface.
  • inkjet marking fluid is deposited in a pattern that is digitally-determined to provide the information directly from a computer to a plate.
  • the dot size of the inkjet fluid deposited on the printing surface of an offset printing press is controlled by controlling the viscosity of the fluid, thus achieving excellent control over the quality of the image to be printed.
  • the novel inkjet marking fluid is used directly in a plateless lithographic printing system to form a strong, stable, oleophilic image from which large quantities of good-quality impressions can be printed.
  • Figures la, lb, and lc show enlarged sectional views of a typical, multi-layered offset lithographic printing plate, as known in the prior art, depicting the process of imaging said plate using UN light.
  • Figures 2a, 2b, and 2c show enlarged sectional views of a typical, multi-layered offset lithographic printing plate, as known in the prior art, depicting the process of imaging said plate using an infra-red laser ablation process;
  • Figure 3 shows a computer-to-plate inkjet system, featuring the drop-wise deposition of inkjet marking fluid from an inkjet printing head onto a printing plate in accordance with the present invention
  • Figure 4 shows a computer-to-plate inkjet system, depicting an offset lithographic plate, prepared in accordance with the present invention, mounted onto an offset printing press;
  • Figure 5 shows another embodiment of the method of the present invention, wherein the image to be formed is provided by the direct deposition of inkjet marking fluid onto a lithographic printing cylinder in a plateless system.
  • Figure la shows a film 2 which contains, in negative form, the image 4 to be printed.
  • Presensitized printing plate 6 is comprised of a grained, anodized aluminum substrate 8 and coated with a photopolymeric layer 10, which is comprised of a photosensitive pre-polymer and a carrier resin.
  • Film 2 is placed in emulsion-to-emulsion contact with presensitized plate 6 and, as shown in Figure lb, is flood-irradiated with ultraviolet light 12.
  • Transparent areas 4 of negative film 2 which represent the image areas to be printed, permit the penetration of UN light 12 to photopolymeric layer 10 which reacts to form hard, insoluble oleophilic areas 14.
  • Negative film 2 is then removed and plate 6 is processed - usually with a high pH aqueous solution in which the unpolymerized portions of layer 10 are readily soluble. This exposes the grained anodized surface 16 of substrate 8 and provides the hydrophilic background areas for the processed printing plate, as shown in Figure 1 c, now ready to be mounted in a conventional offset lithographic printing press..
  • Figures 2a, 2b, and 2c show, in an enlarged depiction, the steps in a simplified, infrared-ablatable, computer-to-plate process as known in the prior art.
  • Figure 2a depicts an unprocessed plate 26 comprising: a substrate 8, which may be, for example, aluminum; an infrared-absorbing layer 22; and a hydrophilic, top coating 24.
  • plate 26 is imaged by digitally-modulated infrared radiation 28 that is absorbed by layer 22. The energy absorbed causes an extremely fast rise in temperature resulting in ablation of layer 22 which takes with it portions of the hydrophilic coating 24.
  • Figure 2c shows the resulting plate with portions of coating 24 providing the hydrophilic background areas of plate 26 and the exposed portions of surface 16 of substrate 8 providing the oleophilic imaged portions of plate 26.
  • FIG. 3 there is shown a computer-to-plate inkjet printing system 30, constructed and operated in accordance with the principles of the present invention.
  • a data pulse train 42 is generated which activates a transducer 45.
  • Transducer 45 emits an electrical signal which actuates a piezo-electric crystal 36.
  • Crystal 36 produces a pressure wave inside ink chamber 38 causing inkjet fluid 32 in ink chamber 38 to be ejected in a stream of droplets 40 through inkjet printer nozzle 34 onto surface 16 of a typical printing plate substrate 8.
  • Substrate 8 may be any type of substrate known to the art from which offset lithographic plates are fabricated, but in the preferred embodiment, it is aluminum-based with a grained, anodized, hydrophilic surface.
  • Figure 3 shows a generic impulse, drop-on-demand, system as this is the preferred system of the invention.
  • plate 46 is heated by any means known to the art to evaporate any water in the fluid and to fuse the resins onto substrate 8.
  • Figure 4 shows a further embodiment of the method of the present invention, wherein a printing plate 46, prepared in accordance with the method of the present invention as described above and as shown in Figure 3, is mounted onto a cylinder 48 of an offset lithographic press 56 used in combination with a CTP inkjet system 30.
  • Inkjet marking fluid is deposited in a pattern that is digitally-determined to provide the information directly from a computer to a plate.
  • a data pulse train 42 generated from computer workstation 20, activates transducer 45 which controls the flow of inkjet marking fluid provided by inkjet system 30 thereby causing said marking fluid to be ejected in a stream of drops 40 through inkjet printer nozzle 34 onto the surface of printing plate 46.
  • Drops 40 produce a pattern of dots 44 as the inkjet head 39 traverses the surface of plate 46, thus forming an image on the surface of printing plate 46.
  • drying system 62 which may be any drying system known to the art, is used to heat printing plate 46 to evaporate any water remaining on the surface of printing plate 46 and to fuse the resins to the substrate of printing plate 46.
  • Printing plate 46 is then wetted by fountain solution applied by wetting cylinder 58 and the imaged areas are inked by inking cylinder 60 and transferred to blanket cylinder 50 by rotation of the cylinder press. Thus the inked image is further transferred to paper 54, as it is pressed between blanket cylinder 50 and impression cylinder 52.
  • the printing image is erasable and offset lithographic printing press 56 is plateless.
  • Inkjet system 30 is depicted jetting marking fluid 40 onto the surface of erasable cylinder 48.
  • Erasable cylinder 48 acts as a substrate for the direct deposition of marking fluid drops 40 and is comprised of any type of hydrophilic surface known to the art.
  • cylinder 48 is comprised of a grained, anodized, aluminum surface.
  • Figure 5 shows a generic impulse, drop-on-demand system 30, as this is the preferred system.
  • a data pulse train 42 is generated which activates a transducer 45.
  • Transducer 45 emits an electrical signal which controls the jetting of inkjet marking fluid ejected in a stream of droplets 40 from inkjet head 39 via nozzle 34 which produces a pattern of dots 44 as inkjet head 39 traverses the surface of erasable cylinder 48.
  • the inkjet marking fluid in the form of drops 44 is deposited in a pattern that is digitally-determined to provide the information directly from computer workstation 20 to erasable cylinder 48 which is plateless.
  • a fount solution is applied to erasable cylinder 48 by wetting cylinder 58 and the imaged areas composed of the pattern of dots 44 are inked by ink cylinder 60 and transferred to blanket cylinder 50 by rotation of the cylinders in lithographic press 56, thus the inked image is transferred to the print surface consisting, in the example shown, of paper 54, which is pressed between the blanket cylinder 50 which receives the inked image and impression cylinder 52.
  • the dried image can be erased either by abrasion or with the aid of an aqueous fluid of either high or low pH or by application of high temperature to decompose the cured image remaining and to clean erasable cylinder 48 which is then ready to accept a new image.
  • the inkjet medium is provided in the form of a dispersion since it is known to those skilled in the art that true solutions, whether they be water-based, oil-based, or solvent-based, give poor imaged plates because of their tendency to spread over the surface of the plates.
  • the present invention comes to solve this difficulty by utilizing a two-phase fluid comprising a combination of resin dispersion in water.
  • a two-phase fluid comprising a combination of resin dispersion in water.
  • the outer, aqueous phase of the inkjet fluid is separated from the internal phase by both capillary action onto the hydrophilic plate surface, and by evaporation, leaving the relatively high-viscosity internal phase of the dispersion which coalesces to give a smooth sharp print image on the printing plate.
  • the preferred embodiment of the invention utilizes an inkjet marking fluid which is based on an internal, dispersion phase and a continuous aqueous, external phase.
  • the particle size of the internal phase is from 4 nm to 3 microns.
  • the inkjet marking fluid in the preferred embodiment is characterized by a viscosity greater than 2 centipoise and less than 40 centipoise, and, more specifically, by a viscosity of between 3 and 25 centipoise.
  • Surface tension of the marking fluid should be within the range of between 28-60 dyne/cm.
  • the amount of polymer binder which constitutes the internal phase of the dispersion should be at least 5% and, in the preferred embodiment, in the range of between 8- 20% by weight.
  • the internal phase of the dispersion is a polymer selected from the following group:
  • ingredients present in the inkjet fluid are those known to the art. These include humectants, dyes, pigments, cosolvents, and coalescing agents.
  • a preferred additive in these fluids is a water-soluble, low molecular-weight polymer that acts as a surfactant in stabilization of the system and at the same time helps maintain the sharpness of print on the finished, imaged plate.
  • Another preferred type of ingredient is a coalescing agent which is necessary to ensure that the dispersed polymer particles form a smooth image after the image coalesces on the surface of the plate and the water leaves the system.
  • carbon black which is in itself oleophilic, serves this purpose, but it is limited to a concentration of not greater than 15% by weight in order to optimize the mechanical resistance of the image to the printing process.
  • the above rheological properties enable the inkjet marking fluid to produce small (down to 3 picoliter) droplets to give high resolution.
  • the combination of the high viscosity and surface tension of dispersions restricts spreading of the inkjet marking fluid on the high surface-energy face of the hydrophilic plate.
  • the particle dot size in the image may be controlled by a suitable combination of marking fluid properties, especially by controlling the viscosity of the marking fluid.
  • abrasion resistance of the jetted image it is possible to further improve the abrasion resistance of the jetted image to increase run length by means of injecting various forms of energy. This may be done by heating the image-bearing printing plate up to approximately 200° C to increase the cross-linking density of the polymer. In the preferred embodiment, the imaged printing plate is heated to a temperature between 100-140° C. Alternatively, drying is done by exposure of the imaged plate to UN light when the composition of the inkjet marking fluid is based on photosensitive monomers or oligomers in conjunction with photoinitiators.
  • the inkjet printing system can operate on its own, functioning solely as a plate-maker, or it can be incorporated directly into a lithographic printing press. In the latter case, printing may commence immediately after application of the image to a blank plate and drying, thereby reducing press set-up time considerably.
  • the inkjet imaging system can be configured either as a flatbed printing system or as a cylinder printing sytem wherein the lithographic plate blank is mounted on the flatbed or attached to the exterior of the cylindrical surface.
  • the inkjet marking fluid is deposited directly onto an erasable cylinder in an offset printing press which serves as the printing surface in a plateless system.
  • An inkjet marking fluid consisting of 7 parts of acrylic polymer emulsion, sold under the trade name of Joncryl 538 by S.C Johnson, 12 parts of Ethylenglycol, 1 part of di-propyleneglycol-monomethylether (DPM), 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta Dye sold under the trade name of Bayscript Magenta by BAYER) and 12 parts of deionized water, was prepared.
  • a 200 micron thick grained anodized aluminum plate was then placed on an XY bed where it was imaged (600 dpi image) using the inkjet printhead described in EP640481 assigned to Scitex using the above liquid. The plate was then heated to 140°C for 2 minutes and then mounted on a Heidleberg GTO printing machine where 50,000 good impressions were printed on high-quality coated paper.
  • An inkjet marking fluid consisting of 7 parts of acrylic polymer emulsion, sold under the trade name of Joncryl 537 by S.C Johnson, 12 parts of Ethylenglycol, 1 part of DPM, 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta Dye sold under the trade name of Bayscript Magenta by BAYER) and 13 parts of de-ionized water, was prepared. Imaging, heat treatment, and testing were performed as described in Example 1. This process gave results similar to those reported in Example 1.
  • An inkjet marking fluid consisting of 7 parts of acrylic emulsion, sold under the trade name of Joncryl 2177 by S.C Johnson, 12 parts of Ethylenglycol, 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta Dye sold under the trade name of Bayscript Magenta by BAYER) and 13 parts of de-ionized water, was prepared. Imaging , heat treatment, and testing as described in Example 1 gave results similar to those reported there.
  • An inkjet marking fluid consisting of 7 parts of acrylic emulsion polymer, sold under the trade name of Lucidene 366 by Morton, 12 parts of Ethylenglycol, 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta Dye sold under the trade name of Magenta Bayscript by BAYER) and 14 parts of de-ionized water, was prepared. Imaging , heat treatment, and testing as described in Example 1 gave results similar to those in Example 1.
  • An inkjet marking fluid consisting of 8 parts of acrylic emulsion polymer, sold under the trade name of Lucidene 388 by Morton, 12 parts of Ethylenglycol, 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta Dye sold under the trade name of Magenta Bayscript by BAYER) and 13 parts of de-ionized water, was prepared. Imaging, heat treatment and testing as described in Example 1 gave results similar to those in Example 1.
  • An inkjet marking fluid consisting of 11 parts of styren/acrylic emulsion polymer, sold under the trade name of Lucidene 410 by Morton, 12 parts of Ethylenglycol, 1 part of DPM , 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta Dye sold under the trade name of Magenta Bayscript by BAYER) and 9 parts of de-ionized water, was prepared. Imaging, heat treatment, and testing as described in Example 1 gave results similar to those in Example 1.
  • An inkjet marking fluid consisting of 7 parts of styrene/acrylic emulsion polymer, sold under the trade name of Lucidene 5025 by Morton, 12 parts of Ethylenglycol, 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta Dye sold under the trade name of Magenta Bayscript by BAYER) and 13 parts of de-ionized water, was prepared. Imaging, heat treatment, and testing as described in Example 1 gave results similar those reported in Example 1.
  • An inkjet marking fluid consisting of 6 parts of vinylidene chloride acrylic copolymer emulsion, sold under the trade name of Permax 801 by BF-Goodrich, 12 parts of Ethylenglycol, 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta Dye sold under the trade name of Magenta Bayscript by BAYER) and 13 parts of de-ionized water, was prepared. Imaging , heat treatment, and testing as described in Example 1 gave results similar to those in Example 1.
  • An inkjet marking fluid consisting of 10 parts of aliphatic urethane polymer dispersion, sold under the trade name of Sancure 776 by BF-Goodrich, 0.6 parts from the polymer dispersion solids of the photoinitiator Melamine, 12 parts of Ethylenglycol, 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta Dye sold under the trade name of Bayscript Magenta by BAYER) and 11 parts of de-ionized water, was prepared. Imaging , heat treatment, and testing as described in Example 1 gave results similar to those in Example 1. The plate can be cured in order to give extra abrasion resistance by crosslinking the polymeric system.
  • An inkjet marking fluid consisting of 10 parts of aliphatic urethane polymer dispersion, sold under the trade name of Sancure 850 by BF-Goodrich, 0.6 parts from the polymer dispersion solids of the photoinitiator sold under the trade name Quantacure ITX by Biddle Sawyar, 12 parts of Ethylenglycol, 1 part of black pigment sold under the trade name of Hostafine Black TS by Clariant GmbH (or magenta dye sold under the trade name of Magenta Bayscript by BAYER), and 11 parts of de-ionized water, was prepared. Imaging , heat treatment, and testing as described in Example 1 gave results similar to those in Example 1. The plate can be UN-cured in order to give extra abrasion resistance by crosslinking the polymeric system.
  • This Example most-clearly demonstrates the relationship between the viscosity of the inkjet marking fluid and the dot size on a commercially-available, brush-grained and post-anodic treated, uncoated aluminum offset plate.
  • An inkjet marking fluid consisting of variable parts of acrylic polymer emulsion, sold under the trade name of Joncryl 538 by S.C Johnson and other components as described in Example 1 was prepared and imaged.
  • Table I shows the dot diameter (in microns) obtained by using the above-described inkjet marking fluid in different viscosities.
  • This Example demonstrates the relationship between the viscosity of the inkjet marking fluid and the dot size on a commercially-available, brush-grained and post-anodic-treated, uncoated aluminum offset plate.
  • An inkjet marking fluid consisting of variable parts of aliphatic urethane polymer dispersion, sold under the trade name of Sancure 850 by BF-Goodrich and other components as described in Example 10, was prepared and imaged.
  • Table II shows the dot diameter (in microns) obtained by using the above-described inkjet marking fluid with different viscosities.

Abstract

L'invention concerne un procédé d'écriture directe des plaques simple et peu coûteux permettant d'obtenir une plaque offset lithographique dans une opération faisant intervenir un nouveau fluide de jet d'encre qui, tout en faisant preuve d'excellentes propriétés de jet, une forte consistance et une bonne qualité, peut être facilement séché sur une plaque lithographique non revêtue. Le fluide de jet d'encre présente une viscosité présélectionnée et comprend un système d'émulsion biphasée : une phase interne oléophile et une phase externe aqueuse en continu. La régulation de la viscosité du fluide de jet d'encre permet de réguler la taille des points du fluide déposé sur la surface d'impression, assurant une meilleure qualité, une image imprimée robuste même après de nombreuses opérations de la presse offset.
EP00974752A 1999-11-07 2000-11-07 Fluide de preparation de plaques d'impression et son procede d'utilisation Withdrawn EP1244547A1 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
IL13278999A IL132789A0 (en) 1999-11-07 1999-11-07 A fluid for preparation of printing plates and method for use of same
IL13278999 1999-11-07
PCT/IL2000/000722 WO2001034394A1 (fr) 1999-11-07 2000-11-07 Fluide de preparation de plaques d'impression et son procede d'utilisation

Publications (1)

Publication Number Publication Date
EP1244547A1 true EP1244547A1 (fr) 2002-10-02

Family

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EP00974752A Withdrawn EP1244547A1 (fr) 1999-11-07 2000-11-07 Fluide de preparation de plaques d'impression et son procede d'utilisation

Country Status (5)

Country Link
EP (1) EP1244547A1 (fr)
JP (1) JP2003513824A (fr)
AU (1) AU1296301A (fr)
IL (1) IL132789A0 (fr)
WO (1) WO2001034394A1 (fr)

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WO2001034394A1 (fr) 2001-05-17
IL132789A0 (en) 2001-03-19
JP2003513824A (ja) 2003-04-15
AU1296301A (en) 2001-06-06

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