Electroluminescent lamp and method for manufacturing the same

Information

  • Patent Grant
  • 6835112
  • Patent Number
    6,835,112
  • Date Filed
    Tuesday, March 12, 2002
    22 years ago
  • Date Issued
    Tuesday, December 28, 2004
    19 years ago
Abstract
An electroluminescent lamp (EL lamp) is formed by stacking a light-transmitting electrode-layer, an adhesive synthetic resin layer, a luminescent layer formed of the synthetic resin layer with phosphor particles fixed uniformly, a dielectric layer and a back electrode-layer on a transparent substrate sequentially. By this structure, a uniform EL lamp having improved brightness can be produced. A method for manufacturing the EL lamp includes following steps for fixing the phosphor particles in the synthetic resin layer uniformly. (1) sinking the phosphor particles in the synthetic resin layer by heating and pressing, after spraying the phosphor particles. (2) blowing the phosphor particles to the synthetic resin layer with heated air. As a result, the phosphor particles are uniformly fixed in the synthetic resin layer having uniform thickness.
Description




FIELD OF THE INVENTION




Recently, multifunction and diversification of an electronic apparatus (particularly a portable terminal device, e.g., a cellular phone) have progressed, so that electroluminescent lamp (EL lamp) is used for illuminating a display area or an operating section of the apparatus.




BACKGROUND OF THE INVENTION




A conventional electroluminescent lamp (EL lamp) will be described with reference to FIG.


6


.





FIG. 6

shows a sectional view of the conventional EL lamp. As shown in

FIG. 6

, light-transmitting electrode-layer


52


, e.g., indium tin oxide, is formed on a whole surface of transparent substrate


51


, e.g., a glass or a film, using a sputtering method or an electron beam method.




The conventional EL lamp is formed by the following elements:




(a) luminescent layer


53


formed of the synthetic resin layer


53


A in which phosphor particles


53


B, e.g., zinc sulfide, (base material of luminescence) disperse, and formed on transparent substrate


51


,




(b) dielectric layer


54


made of synthetic resin, where barium titanate disperses, and formed on luminescent layer


53


,




(c) back electrode-layer


55


made of silver or carbon resin, and formed on dielectric layer


54


, and




(d) insulating layer


56


made of epoxy resin or polyester resin and formed on back electrode-layer


55


.




The EL lamp mentioned above is installed in an electronic apparatus, and an AC voltage is applied between light-transmitting electrode-layer


52


and back electrode-layer


55


. As a result, phosphor particle


53


B of luminescent layer


53


emits light, and the light illuminates a display area or an operating section of the electronic apparatus from behind.




Luminescent layer


53


is formed by the following method. First, paste is made of cyano resin or fluororubber dissolved in organic solvent. Second, phosphor particles


53


B disperse in the paste. Third, the paste is formed by a reverse-roll coater or a die coater, or printed by a screen printing. Finally, the paste is dried and formed. By the coating method using the reverse-roll coater or the die coater, phosphor particles


53


B can be dispersed in luminescent layer


53


uniformly to a certain extent by changing composition of phosphor particles


53


B in the paste or thickness of the coating paste. By this coating method, the luminescent layer can coat on the whole surface of a rectangular substrate, however, can not coat the surface in a specific pattern.




When the specific pattern is required, the screen printing is usually used for forming luminescent layer


53


. A screen mask used for the screen printing is made of sheet which is formed by knitting stainless threads or polyester threads of diameter approximately 30 μm. The sheet is formed of opening-sections into which paste penetrates and closed-sections into which paste does not penetrate, so that a pattern of an electrode can be printed. As shown in

FIG. 6

, because the sheet is formed by knitting threads, area


53


C under the threads or under intersections of the threads printed with phosphor particles


53


B insufficiently or not printed tends to occur.




A mean diameter of phosphor particles


53


B is approximately 20 μm through 25 μm. As shown in

FIG. 6

, when phosphor particles


53


B are printed using a screen mask of thickness 60 μm, two or three of phosphor particles


53


B tends to pile up at an area


53


D under the opening-section.




In the conventional EL lamp discussed above, phosphor particles


53


B are difficult to disperse in luminescent layer


53


uniformly, so that an area on which phosphor particles


53


B do not disperse or pile up tends to occur. As a result, light emission from phosphor particles


53


B tends to produce uneven brightness.




When luminescent layer


53


is formed of paste, which is made of synthetic resin dissolved in organic solvent, and phosphor particles


53


B disperse in the resin, a state of dispersing phosphor particles


53


B tends to disperse unevenly even in the same printing condition. Because characteristics of printing is changed by diameters or shapes of phosphor particles


53


B, or changed by a surface shape of light-transmitting electrode-layer


52


.




SUMMARY OF THE INVENTION




The present invention addresses the problem discussed above, and aims to provide an electroluminescent lamp (EL lamp), of which brightness uniformity is improved, and provide a method for manufacturing the EL lamp.




The EL lamp of this invention includes the following elements:




(a) a transparent substrate,




(b) a light-transmitting electrode-layer formed on the transparent substrate,




(c) an adhesive synthetic resin layer formed on the light-transmitting electrode-layer,




(d) a luminescent layer which is formed of the synthetic resin layer with phosphor particles dispersed uniformly,




(e) a dielectric layer formed on the luminescent layer,




(d) a back electrode-layer formed on the dielectric layer.




Each phosphor particle disperses on the synthetic resin layer uniformly, and the luminescent layer is thus formed, so that the EL lamp having improved brightness uniformity is obtainable. Because a voltage is applied to the luminescent layer uniformly, an inexpensive and uniform EL lamp with high brightness using less phosphor particles is obtainable.




The method for manufacturing the EL lamp includes the following steps:




(a) forming a light-transmitting electrode-layer on a transparent substrate,




(b) forming an adhesive synthetic resin layer on the light-transmitting electrode-layer,




(c) sticking phosphor particles on the synthetic resin layer uniformly so that a luminescent layer is formed,




(d) forming a dielectric layer on the luminescent layer, and




(e) forming a back electrode-layer on the dielectric layer.




As a result, an inexpensive and uniform EL lamp having improved brightness can be produced.











BRIEF DESCRIPTION OF THE DRAWINGS





FIG. 1

shows a sectional view of an essential part of an electroluminescent lamp (EL lamp) in accordance with a first exemplary embodiment of the present invention.





FIG. 2A

shows an outward appearance of an EL lamp in accordance with a second exemplary embodiment of the present invention.





FIG. 2B

shows a sectional view of an essential part of the EL lamp in accordance with the second embodiment of the present invention.





FIGS. 3A through 3D

show sectional views illustrating a method for manufacturing an EL lamp in accordance with a third exemplary embodiment of the present invention.





FIG. 4

shows a sectional view of an essential part of a phosphor-particle-dispersing apparatus in accordance with the third exemplary embodiment of the present invention.





FIG. 5

shows a scanning electron microscope (SEM) photograph of a surface of a luminescent layer included in the EL lamp in accordance with the first embodiment through the third embodiment of the present invention.





FIG. 6

shows a sectional view of an essential part of a conventional EL lamp.











DESCRIPTION OF THE PREFERRED EMBODIMENTS




Exemplary embodiments of the present invention are demonstrated hereinafter with reference to FIG.


1


through FIG.


4


.




First Embodiment





FIG. 1

shows a sectional view of an essential part of an electroluminescent lamp (EL lamp) in accordance with the first exemplary embodiment of the present invention.




As shown in

FIG. 1

, the EL lamp is formed by the following elements:




(a) transparent substrate


1


made of glass, resin film, synthetic resin and the like,




(b) light-transmitting electrode-layer


2


formed on transparent substrate


1


,




(c) luminescent layer


3


formed of adhesive synthetic resin layer


3


A where phosphor particles


3


B, e.g., zinc sulfide, disperse uniformly, and formed on light-transmitting electrode-layer


2


,




(d) dielectric layer


4


made of synthetic resin, where barium titanate and so on disperses, and formed on luminescent layer


3


,




(e) back electrode-layer


5


made of silver or carbon resin and formed on dielectric layer


4


, and




(f) insulating layer


6


made of epoxy resin or polyester resin and formed on back electrode-layer


5


.




Light-transmitting electrode-layer


2


is formed by one of the following methods. One method is depositing indium tin oxide by using a sputtering method or an electron beam method, and another method is printing transparent synthetic resin where indium tin oxide disperses.




The EL lamp is installed in an electronic apparatus, and an AC voltage is applied between light-transmitting electrode-layer


2


and back electrode-layer


5


from a circuit of the electronic apparatus (not shown). As a result, phosphor particles


3


B of luminescent layer


3


emit light, and the light illuminates a display area or an operating section of the electronic apparatus from behind.




In this embodiment, luminescent layer


3


is formed by uniformly dispersing phosphor particles


3


B on synthetic resin layer


3


A, so that the EL lamp having improved brightness uniformity is obtainable. As a result, because a voltage is applied to luminescent layer


3


uniformly, an inexpensive EL lamp with high brightness using less phosphor particles


3


B is obtainable.




Luminescent layer


3


is formed as follows. Phosphor particles


3


B disperse on a surface of synthetic resin layer


3


A, then layer


3


A is heated and pressed, so that phosphor particles


3


B sink in layer


3


A.




Synthetic resin not adhesive at a room temperature can be used as synthetic resin layer


3


A, so that transparent substrates


1


having layer


3


A can be stacked for a storage purpose. This storage allows the manufacturing of the EL lamp to be flexible.




A diameter of phosphor particles


3


B can be greater than a thickness of synthetic resin layer


3


A. In such a case, when transparent substrates


1


having layer


3


A are stacked for a storage purpose, non-adhesive phosphor particles


3


B come in contact with transparent substrates


1


, so that transparent substrates


1


is easy to be stored.




Cyano resin, fluororubber, polyester resin or phenoxy resin can be used as a principal ingredient of synthetic resin layer


3


A, whereby a dielectric constant of synthetic resin layer


3


A becomes large, and brightness of an EL lamp thus becomes high.




In general, lifetime of luminescence becomes longer as a diameter of phosphor particle


3


B becomes larger. In this invention, a diameter of 25 μm through 90 μm of phosphor particle


3


B is applicable, so that lifetime of the EL lamp of this invention becomes longer than that of a conventional EL lamp having a phosphor particle of which diameter is 20 μm through 25 μm.




When thickness of synthetic resin layer


3


A is 0.01 μm through 50 μm, and thinner than a diameter of phosphor particle


3


B, a brighter EL lamp can be obtained.




Second Embodiment





FIG. 2A

shows an outward appearance of an electroluminescent lamp (EL lamp) in accordance with the second exemplary embodiment of the present invention.

FIG. 2B

shows a sectional view of an essential part of the same EL lamp.




As shown in

FIG. 2A

, for example, the El lamp included in an electronic apparatus is formed of transparent substrate


11


and a luminescent section. Transparent substrate


11


made of synthetic resin, e.g., polycarbonate, is molded into a curved-surface substrate, and the luminescent section is formed inside transparent substrate


11


.




The luminescent section is detailed hereinafter with reference to FIG.


2


B.




First, paste is sprayed on an inner surface of transparent substrate


11


. The paste is made of epoxy resin (bis-phenol A liquid resin) of 98 wt % and imidazole hardening-agent (2E4MZ manufactured by Shikoku Corporation) of 7 wt % where transparent conductive particles of 400 wt % (SP-X manufactured by Sumitomo Metal Industries, Ltd.) disperse. Then, the paste hardens at 80° C. for 3 hours, light-transmitting electrode-layer


2


is thus formed.




Second, resin solution (isophorone solution where Daieru G502 manufactured by Daikin Industries, Ltd. is dissolved) is sprayed on light-transmitting electrode-layer


2


, and then dried up, synthetic resin layer


3


A is thus formed.




Third, phosphor particles


3


B are sprayed on a surface of synthetic resin layer


3


A at 80° C. using an air-spray gun, luminescent layer


3


is thus formed.




Then, paste is sprayed on luminescent layer


3


, where the paste is made of resin solution (isophorone solution where Daieru G502 manufactured by Daikin Industries, Ltd. is dissolved) of resin component 40 wt % where barium titanate (BT-01 manufactured by Kanto Kagaku Kabushiki Kaisha) of 60 wt % disperses. Then the paste is dried up, dielectric layer


4


is thus formed.




The paste of dielectric layer


4


is sprayed approximately 5 μm in thickness at one time, and dried. This process is repeated three times, phosphor particles


3


B are thus buried in synthetic resin layer


3


A.




Next, the same paste as light-transmitting electrode-layer


2


is sprayed on dielectric layer


4


, and hardens at 80° C. for 3 hours, back electrode-layer


5


is thus formed.




Finally, transparent polyester resin is sprayed on back electrode-layer


5


, insulating layer


6


is thus formed, so that the EL lamp is constructed.




The EL lamp is installed in the electronic apparatus, and an AC voltage is applied between light-transmitting electrode-layer


2


and back electrode-layer


5


from a circuit of the electronic apparatus (not shown). Then, phosphor particles


3


B of luminescent layer


3


emit light, and the light illuminates transparent substrate


11


from inside.




In this embodiment, respective layers are formed on transparent substrate


11


having a curved-surface, and the EL lamp is formed. As a result, the EL lamp, which can emit light depending on various shapes of display area or an operating section of the electronic apparatus, can be obtained.




Third Embodiment





FIGS. 3A through 3D

show sectional views illustrating a method for manufacturing an electroluminescent lamp (EL lamp) in accordance with the third exemplary embodiment of the present invention.




First, as shown in

FIG. 3A

, light-transmitting electrode-layer


2


is formed on transparent substrate


1


, and synthetic resin layer


3


A is printed on light-transmitting electrode-layer


2


. Cyano resin, fluororubber, polyester resin or phenoxy resin is used as material of synthetic resin layer


3


A. Because a dielectric constant of resin of luminescent layer


3


is required large enough for obtaining high brightness of the EL lamp, cyano resin or fluororubber is desired to have a large dielectric constant.




The resin discussed above is dissolved in organic solvent, and printed using a screen printing method and dried, then synthetic resin layer


3


A is formed. In the manufacturing of the EL lamp, because transparent substrate


1


having synthetic resin layer


3


A is piled up for a storage purpose, the synthetic resin having no adhesion is easier to handle than the synthetic resin having adhesion. If fluororubber, e.g., Daieru G502 manufactured by Daikin Industries, Ltd., having adhesion at a room temperature is used, inorganic particles or solid resin particles, of which diameters or composition are determined based on a glass transition point or a coefficient of elasticity, are dispersed in the fluororubber. As a result, synthetic resin layer


3


A, which does not have adhesion at a room temperature but gains adhesion by heating, is obtainable.




Second, as shown in

FIG. 3B

, phosphor particles


3


B disperse on synthetic resin layer


3


A.




Third, as shown in

FIG. 3C

, synthetic resin layer


3


A is heated, then obtains adhesion, so that phosphor particles


3


B are fixed uniformly on a surface of synthetic resin layer


3


A. Then phosphor particles


3


B not fixed on the surface of synthetic resin layer


3


A are removed.




Then phosphor particles


3


B are pressed using a rubber roller with synthetic resin layer


3


A heated. As a result, phosphor particles


3


B disperse uniformly in synthetic resin layer


3


A, luminescent layer


3


shown in

FIG. 3D

is thus formed.




Finally, dielectric layer


4


, back electrode-layer


5


and insulating layer


6


are sequentially stacked on luminescent layer


3


, then the EL lamp is formed (not shown).




In the method of manufacturing the EL lamp of this embodiment, after luminescent layer


3


is formed, phosphor particles


3


B sink in synthetic resin layer


3


A by heating and pressing layer


3


. As a result, because each phosphor particle


3


B uniformly disperses in synthetic resin layer


3


A, a uniform EL lamp with high brightness is obtainable.




Process of manufacturing luminescent layer


3


without heating and pressing is described as follows. Dielectric layer


4


is formed by coating and drying paste of a high dielectric constant which is similar to that of synthetic resin layer


3


A, where the paste includes organic solvent which dissolves or swells synthetic resin layer


3


A. In such a case, phosphor particles


3


B can disperse in synthetic resin layer


3


A uniformly without heating and pressing layer


3


.




In the process of coating paste of the high dielectric constant, the solvent in dielectric layer


4


dissolves or swells synthetic resin layer


3


A, and softens layer


3


A. Then phosphor particles


3


B sink in synthetic resin layer


3


A due to surface tension of dielectric layer


4


in a drying process. As a result, phosphor particles


3


B can disperse in synthetic resin layer


3


A uniformly.




When a thickness of synthetic resin layer


3


A is not less than 0.01 μm and not more than 50 μm, synthetic resin layer


3


A has enough adhesion to stick phosphor particle


3


B. The EL lamp having high brightness can be thus manufactured. Cyanoethyl pullulan, e.g., CR-M manufactured by Shin-Etsu Chemical Co., Ltd. or Daieru G201 manufactured by Daikin Industries, Ltd., is used as synthetic resin layer


3


A. In such a case, when a thickness of layer


3


A is less than 0.01 μm, layer


3


A has not enough adhesion, so that phosphor particles


3


B occasionally come off, and when a thickness of layer


3


A is more than 50 μm, brightness of the EL lamp occasionally decreases. More desirable thickness of synthetic resin layer


3


A is 2 μm through 25 μm.




A phosphor-particle-dispersing apparatus used for manufacturing the EL lamp in accordance with the third embodiment is described hereinafter with reference to FIG.


4


.





FIG. 4

shows a sectional view of an essential part of the phosphor-particle-dispersing apparatus in accordance with the third exemplary embodiment of the present invention.




In

FIG. 4

, the phosphor-particle-dispersing apparatus includes sucking nozzle


16


surrounding blowing nozzle


15


. However, sucking nozzle


16


is not necessarily placed surrounding blowing nozzle


15


, but it can be placed next to blowing nozzle


15


. Transparent substrate


1


, on which light-transmitting electrode-layer


2


and adhesive synthetic resin layer


3


A are piled up, is disposed under nozzle


15


and nozzle


16


.




Phosphor particles


3


B are continuously blown to a surface of synthetic resin layer


3


A with heated air at approximately 50° C. through 180° C. from blowing nozzle


15


. Synthetic resin layer


3


A obtains enough adhesion by the heated air, so that blown phosphor particles


3


B are fixed on the surface of synthetic resin layer


3


A uniformly. However, an area, where phosphor particles


3


B are not fixed on a surface of synthetic resin layer


3


A, may occur at first. Even in such a case, phosphor particles


3


B, which include various sizes of particles, are continuously blown to layer


3


A, so that phosphor particles


3


B having appropriate sizes are fixed on the area, phosphor particles


3


B are thus fixed on a whole surface of synthetic resin layer


3


A uniformly.




When phosphor particles


3


B are blown, air is sucked from sucking nozzle


16


, so that phosphor particles


3


B not fixed on the surface of synthetic resin layer


3


A are removed.




When sucking power of sucking nozzle


16


is greater than blowing power of blowing nozzle


15


, dispersion of particles


3


B to an undesirable area can be prevented, and particles


3


B dispersed by static electricity on an area, where layer


3


A is not formed, can be removed.




Then synthetic resin layer


3


A is heated and pressed, luminescent layer


3


having layer


3


A,where phosphor particles


3


B are dispersed uniformly, is formed. When the paste having a high dielectric constant and including solvent which dissolves or swells synthetic resin layer


3


A is used, a heating and a pressing processes are not necessary. In such a case, when dielectric layer


4


is formed on luminescent layer


3


, phosphor particles


3


B can sunk in synthetic resin layer


3


A.




Finally, dielectric layer


4


, back electrode-layer


5


and insulating layer


6


are sequentially stacked on luminescent layer


3


, the EL lamp is thus formed.




As shown in

FIG. 4

, in the phosphor-particle-dispersing apparatus of this invention, phosphor particles


3


B continuously disperse on the surface of synthetic resin layer


3


A, then phosphor particles


3


B not fixed on the surface of synthetic resin layer


3


A can be removed by sucking nozzle


16


. As a result, the phosphor particles can be uniformly dispersed and filled on the surface of synthetic resin layer


3


A, and dispersion of the phosphor particles to an undesirable area can be prevented.





FIG. 5

shows a scanning electron microscope (SEM) photograph of a surface of a luminescent layer included in the EL lamp in accordance with the first embodiment through the third embodiment of the present invention. As shown in

FIG. 5

, in the EL lamp of this invention, small phosphor particles are filled among large phosphor particles. An area, on which phosphor particles do not disperse or pile up, is not observed in the luminescent layer included in the EL lamp of this invention.



Claims
  • 1. The method for manufacturing an EL lamp comprising the steps of:(a) forming a light-transmitting electrode-layer on a transparent substrate; (b) forming an adhesive synthetic resin layer on the light-transmitting electrode layer; (c) forming a luminescent layer by: (i) dispersing phosphor particles on the resin layer, (ii) heating the synthetic resin layer, and (iii) pressing the phosphor particles such that the phosphor particles sink into the resin layer; (d) forming a dielectric layer on the luminescent layer; and (e) forming a back electrode-layer on the dielectric layer.
  • 2. The method for manufacturing the EL lamp of claim 1, wherein the synthetic resin layer is not adhesive at a room temperature, and gains adhesion by heating the synthetic resin layer.
  • 3. The method for manufacturing the EL lamp of claim 1,wherein a diameter of one of the phosphor particles is greater than a thickness of the synthetic resin layer.
  • 4. The method for manufacturing the EL lamp of claim 1,wherein a thickness of the synthetic resin layer is not less than 0.01 μm and not more than 50 μm.
  • 5. The method for manufacturing the EL lamp of claim 1,wherein a diameter of one of the phosphor particles is not less than 25 μm and not more than 90 μm.
  • 6. The method for manufacturing an EL lamp comprising the steps of:(a) forming a light-transmitting electrode-layer on a transparent substrate; (b) forming a synthetic resin layer on the light-transmitting electrode layer; (c) forming a luminescent layer by sticking phosphor particles on the surface of the resin layer; (d) forming a dielectric layer on the luminescent layer by coating and drying paste of a high dielectric constant, and solvent which one of dissolves and swells the synthetic resin layer is used as organic solvent included in the paste of a high dielectric constant; and (e) forming a back electrode-layer on the dielectric layer.
  • 7. The method for manufacturing an EL lamp comprising the steps of:(a) forming a light-transmitting electrode-layer on a transparent substrate; (b) forming an adhesive synthetic resin layer on the light-transmitting electrode layer; (c) forming a luminescent layer by: (i) dispersing phosphor particles on the resin layer, and (ii) heating and pressing the synthetic resin layer such that the phosphor particles sink into the resin layer; (d) forming a dielectric layer on the luminescent layer; and (e) forming a back electrode-layer on the dielectric layer, wherein in step (c), after the phosphor particles are dispersed by blowing a surface of the synthetic resin layer with heated air, the phosphor particles not fixed on the surface of the synthetic resin layer are removed by a sucking nozzle.
  • 8. The method for manufacturing an EL lamp comprising the steps of:(a) forming a light-transmitting electrode layer on a transparent substrate; (b) forming an adhesive synthetic resin layer on the light-transmitting electrode layer; (c) forming a luminescent layer by blowing phosphor particles to a surface of the synthetic resin layer with heated air and removing the phosphor particles not fixed on the surface of the synthetic resin by a sucking nozzle; (d) forming a dielectric layer on the luminescent layer; and (e) forming a back electrode-layer on the dielectric layer.
  • 9. The method for manufacturing the EL lamp of claim 8,wherein the synthetic resin layer is not adhesive at a room temperature and gain adhesion by heating the synthetic resin layer.
  • 10. The method of manufacturing an EL lamp comprising the steps of:(a) forming a light-transmitting electrode-layer on a transparent substrate; (b) forming an adhesive synthetic resin layer on the light-transmitting electrode layer; (c) forming a luminescent layer by: (i) dispersing phosphor particles on the resin layer, and (ii) heating and pressing the synthetic resin layer such that the phosphor particles sink into the resin layer; (d) forming a dielectric layer on the luminescent layer; and (e) forming a back electrode-layer on the dielectric layer. wherein in step (c), removing the phosphor particles not fixed on the surface of synthetic resin layer before heating and pressing the synthetic resin layer.
  • 11. The method of manufacturing the EL lamp of claim 6,wherein the step (c) includes heating and pressing the synthetic resin layer such that the phosphor particles sink into the resin layer.
Priority Claims (3)
Number Date Country Kind
2001-077863 Mar 2001 JP
2001-305035 Oct 2001 JP
2001-371250 Dec 2001 JP
US Referenced Citations (3)
Number Name Date Kind
4289799 Sarvas Sep 1981 A
4902567 Eilersten et al. Feb 1990 A
5598067 Vincent et al. Jan 1997 A
Foreign Referenced Citations (6)
Number Date Country
0 323 218 Jul 1989 EP
4-36993 Feb 1992 JP
8-148278 Oct 1996 JP
2001-284053 Oct 2001 JP
WO 8804467 Jun 1988 WO
WO 0042825 Jul 2000 WO