BE1014795A3 - Photosensitive solution for depositing metal on an insulating substrate comprises an iron(III) compound, a metal salt, a water-soluble film-forming polymer, a complexing agent and a solvent - Google Patents

Photosensitive solution for depositing metal on an insulating substrate comprises an iron(III) compound, a metal salt, a water-soluble film-forming polymer, a complexing agent and a solvent Download PDF

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BE1014795A3
BE1014795A3 BE2002/0278A BE200200278A BE1014795A3 BE 1014795 A3 BE1014795 A3 BE 1014795A3 BE 2002/0278 A BE2002/0278 A BE 2002/0278A BE 200200278 A BE200200278 A BE 200200278A BE 1014795 A3 BE1014795 A3 BE 1014795A3
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solution
iii
iron
metal salt
substrate
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BE2002/0278A
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French (fr)
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Blue Chips Holding
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    • CCHEMISTRY; METALLURGY
    • C23COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23CCOATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C18/00Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating
    • C23C18/16Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating by reduction or substitution, e.g. electroless plating
    • C23C18/1601Process or apparatus
    • C23C18/1603Process or apparatus coating on selected surface areas
    • C23C18/1607Process or apparatus coating on selected surface areas by direct patterning
    • C23C18/1612Process or apparatus coating on selected surface areas by direct patterning through irradiation means
    • CCHEMISTRY; METALLURGY
    • C23COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23CCOATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C18/00Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating
    • C23C18/16Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating by reduction or substitution, e.g. electroless plating
    • C23C18/1601Process or apparatus
    • C23C18/1603Process or apparatus coating on selected surface areas
    • C23C18/1607Process or apparatus coating on selected surface areas by direct patterning
    • C23C18/1608Process or apparatus coating on selected surface areas by direct patterning from pretreatment step, i.e. selective pre-treatment

Abstract

Photosensitive solution with adjustable viscosity for depositing metal on an insulating substrate, which comprises, in combination, an iron (III) compound, a metal salt, a water-soluble film-forming polymer an iron (III) complexing agent and / or the metal salt and a solvent chosen from water, ethanol, isopropanol, butanol and acetone, and its use.

Description


   <Desc / Clms Page number 1>
 



   "Photosensitive solution for depositing metal on an insulating substrate and its use"
The present invention relates to a photosensitive solution with adjustable viscosity for depositing metal on an insulating substrate and to its use.



   Applicant's patent EP 0 687 311 relates to a polymeric resin with adjustable viscosity and pH for the deposition of catalytic palladium on a substrate, comprising, in combination, a palladium salt, a complexing agent of the carboxylic acid or chloride type, a polymer containing water-soluble hydroxyl and / or carboxyl groups, a basic compound such as a basic salt or a base and a solvent chosen from water, methanol and ethanol, the pH value being between 1 and 10, as well as its applications for the deposition of catalytic palladium on the substrate surface and for the metallization of these surfaces.



   Although this type of palladium polymer resin has proved advantageous in a large number of metallization applications of polymeric and other substrates, in particular because of their stability over time and the adjustability of their viscosity and pH, it has however, a certain number of drawbacks, among which, the compulsory use of palladium which is a noble metal which is both expensive and extremely fluctuating on the market and the obligatory passage through an electroless bath for the metallization of the non-conductive substrate. and also due to the fact that the photosensitivity of the resin is reduced to a range of narrow wavelengths between 190 and 300 nm,

   thus greatly limiting the

 <Desc / Clms Page number 2>

 type of possible applications and the source of radiation usable in this regard.



   One of the essential aims of the present invention therefore consists in remedying the abovementioned drawbacks and in presenting a photosensitive solution with adjustable viscosity no longer necessarily requiring the use of a noble metal such as palladium and also calling upon other more common and less expensive metals whose photosensitivity is extended to a range of wavelengths between 190 and 450 nm and requiring a much lower irradiation energy than the polymeric resins known up to now, less than 100 mJ / cm2 and not requiring the obligatory passage by an autocatalytic bath for the metallization of the substrate, allowing therefore a direct electrolytic metallization.



   To this end, according to the invention, the photosensitive solution comprises, in combination, an iron (III) compound, a metal salt, a water-soluble film-forming polymer, a complexing agent for iron (III) and / or the metal salt and a solvent chosen from water, ethanol, isopropanol, butanol and acetone.



   According to an advantageous embodiment of the invention, the iron compound (III) is an iron salt (III) and in particular iron oxalate (III), iron citrate (III), iron tartrate ( III) or a mixture of at least two of these salts.



   According to another advantageous embodiment, the metal salt is a transition metal salt and in particular chosen from the group comprising copper, gold, platinum, palladium, nickel and cobalt, and is preferably sodium sulfate. copper (II), copper (II) chloride, palladium (II) chloride or a mixture of at least two of these salts.



   According to another advantageous embodiment of the invention, the polymer containing hydroxyl and / or carboxyl groups is chosen from the group comprising cellulosic polymers,

 <Desc / Clms Page number 3>

 acrylic polymers, polysaccharides, polyvinyl compounds of the polyvinyl pyrrolidone type and polyvinyl alcohol and mixtures thereof, and is preferably a polysaccharide such as a sodium salt of a mixed carboxymethyl and 2-hydroxypropyl ether of guar gum.



   The present invention also relates to a method of depositing metal on the surface of an insulating substrate, using the photosensitive solution, which consists in applying said solution in the form of a film to the substrate in a selective manner or not, to dry the film applied to said substrate and to irradiate using ultraviolet and / or laser radiation with a range of wavelengths between 190 and 450 nm and an energy between 25 mJ / cm2 and 100 mJ / cm2 until a selective or non-selective metal layer is obtained on the substrate.



   Other details and particularities of the invention will emerge from the description below, by way of nonlimiting example, of photosensitive solutions according to the invention and of their applications for the deposition of metal on the surface of insulating substrates as well as for the metallization of these surfaces.



   As already specified above, the purpose of the photosensitive solutions with variable viscosity of the invention is to replace the solutions and polymeric palladium resins known up to now, the main drawbacks of which have been specified, and to develop solutions. photosensitive with adjustable viscosity and of a much wider applicability than known resins comprising, in combination, an iron (III) compound, a metal salt, a water-soluble film-forming polymer, a complexing agent for iron (III) and / or the metal salt and a solvent chosen from water, ethanol, isopropanol, butanol and acetone.



   Iron (III) compounds are products well known to those skilled in the art and are used in all iron imaging systems and more particularly in the context of methods

 <Desc / Clms Page number 4>

 photographic and in particular silver-based photographic processes. Advantageous iron (III) compounds are the iron (III) salts and, more specifically, iron (III) oxalate, iron (III) citrate, iron (III) tartrate and mixtures of at least two of these.

   In fact, under the influence of ultraviolet and / or laser light the iron (III) compound breaks down into iron (II), which is a powerful reducing agent because it quickly gives an electron to transform back into iron (III) . This iron (II) thus reduces the metal salts in accordance with the following reaction:
 EMI4.1
 M representing the metal of the metal salt used.



  The metal salt can be introduced directly into the photosensitive solution of the invention or the reduction of the latter can be carried out separately. The metal of the metal salt is advantageously a transition metal chosen from Groups IB and IIIV of the Periodic Table of the Elements, and is more particularly copper, gold, silver, platinum, palladium, nickel or cobalt or a mixture of at least two of these.



   Advantageously, the water-soluble film-forming polymer is a polymer containing hydroxyl and / or carboxyl groups and has already been defined in the context of patent EP 0 687 311, of which question above. This film-forming polymer in fact serves as an agent for adjusting the viscosity of the photosensitive solution so as to thus obtain a continuous and homogeneous film on the surface of the substrate using various coating means such as spraying, soaking, application. by roller, screen printing, tempography or the like.

   Examples of suitable film-forming polymers are cellulosic polymers, acrylic polymers, polysaccharides, polyvinyl compounds of the polyvinyl pyrrolidone and polyvinyl alcohol type and mixtures thereof, a

 <Desc / Clms Page number 5>

 polysaccharide such as a sodium salt of a mixed carboxymethyl and 2-hydroxypropyl ether of guar gum which is particularly suitable for this purpose. The complexing agent for iron (III) and / or the metal salt is advantageously of the carboxylic acid, chloride or sulphate type. This complexing agent, by coordinating with iron (III), aims to dissolve the metal salt. Examples of complexing agents of the carboxylic acid type are tartaric acid, ethylenediaminetetraacetic acid (EDTA) and its derivatives and their mixtures.



   In addition to the aforementioned components and the solvent chosen from water, ethanol, isopropanol, butanol and acetone, agents of the dye or surfactant type will be added, depending on the specific application envisaged, to increase the wettability of the film of the deposited solution, antifoam and organic solvents to increase the adhesion of the film and therefore of the metallic deposit, or a combination of two or more of these agents.



   As regards the concentrations of the various components of the photosensitive solution of the invention, these will of course depend on the nature of these components and on the solvent used. However, in general, according to the invention, the iron (III) compound will be used in a concentration, per liter of solution, of 0.5 to 100 g and preferably of 1.5 to 60 g, the metal salt in a concentration, per liter of solution, of 0.1 to 5 g and preferably of 0.5 to 3 g, the film-forming polymer in a concentration, per liter of solution, of 0.1 to 100 g and preferably from 1 to 50 g and the complexing agent in a concentration, per liter of solution, of 0.1 to 50 g and preferably of 0.4 to 25 g.

   The concentration of additional agents can range from 0.01 to 1% by weight of the solution for each type of agent, the organic solvents as additions used to increase the adhesion of the film to the substrate being able to be used in weight percentages ranging from 0.01 to 30%.

 <Desc / Clms Page number 6>

 



   The deposition of metal on the surface of an insulating substrate can be done according to the invention in two different ways. According to a first embodiment, all the components constituting the photosensitive solution are mixed, namely the iron (III) compound, the metal salt, the film-forming polymer, the complexing agent and the solvent as well as any additions and said solution is applied. in the form of a film on the substrate in a selective manner or not depending on the application envisaged. Then, the film applied to the substrate is dried and irradiated using ultraviolet and / or laser radiation with a range of wavelengths between 190 and 450 nm and an energy between 25 mJ / cm2 and 100 mJ / cm2 until a selective or non-selective metal layer is obtained on the substrate.

   Or, according to a second embodiment, a part of the photosensitive solution comprising at least the iron (III) compound and the polymer is applied to the insulating substrate, in the form of a film in a selective or non-selective manner. , the film applied to said substrate is dried, irradiated using ultraviolet and / or laser radiation with a range of wavelengths between 190 and 450 nm and an energy between 25 mJ / cm2 and 100 mJ / cm2 and the substrate thus irradiated is quenched in the remaining part of the solution comprising at least the metal salt and the complexing agent until a layer of metal, selective or not, is obtained on the substrate.

   It will be noted in this regard that the final viscosity of the photosensitive solution is generally between 1 cps and 30,000 cps and is adjusted as a function of the concentration therein of the film-forming polymer used.



   Examples of photosensitive solutions of the invention are given below, as well as their implementation techniques.

 <Desc / Clms Page number 7>

 



     Example 1
Photosensitive solution for the deposition of conductive copper on an insulating substrate, in two stages Composition of the resin:
Concentration
 EMI7.1
 
<tb> Oxalate <SEP> of <SEP> iron <SEP> [Fe2 (C2O4) 3] <SEP> 1,2 <SEP> to <SEP> 60 <SEP> g / liter
<Tb>
<tb> Salt <SEP> sodium <SEP> of ether <SEP> mixed <SEP> carboxy-
<Tb>
<tb> methyl <SEP> and <SEP> 2-hydroxypropyl
<Tb>
<tb> from <SEP> eraser <SEP> from <SEP> guar <SEP> 1 <SEP> to <SEP> 50 <SEP> g / liter
<Tb>
<tb> Water <SEP> quantity <SEP> for <SEP> make <SEP> 1 <SEP> liter
<Tb>
 
The above solution is applied to a non-conductive substrate, by soaking, screen printing, spraying or roller application, and then is air dried, air dried which is accelerated by hot air at a temperature maximum of 80 C.

   The film thus obtained is irradiated using commonly used UV lamps and / or laser (for example by means of diodes) and having a spectrum at least between 250 and 450 nm, the time necessary for the film to receive a minimum energy of 25 mJ / cm2. If a selective metallization is desired, the irradiation will be done through a mask put in contact with the substrate. The substrate is then immersed in an aqueous solution of copper (II). This solution can consist of a concentrated solution of copper sulphate, copper chloride or even a copper electroless bath. This results in the deposition of a selective or non-selective conductive copper layer. In the case of selective metallization, the non-irradiated parts are dissolved in an aqueous solution of tartaric acid.

   An electrolytic metal overload is then made possible, the substrate being made conductive.

 <Desc / Clms Page number 8>

 



   Example 2
Photosensitive solution for the deposition of catalytic palladium on an insulating substrate, in two stages
The same solution composition is used as that of Example 1 and the procedure is as in Example 1 but instead of using an aqueous solution of copper (II) an aqueous solution of palladium (II) is used. This gives the deposition of a layer of catalytic palladium, selective or not. In the case of selective metallization, the non-irradiated parts are also dissolved in an aqueous solution of tartaric acid. The catalytic palladium thus obtained can be metallized by then immersing the substrate in an autocatalytic bath.



   Example 3
Photosensitive solution for depositing conductive copper on an insulating substrate, in one step Composition of the solution:
Concentration
 EMI8.1
 
<tb> Citrate <SEP> of <SEP> iron <SEP> (III) <SEP> (C6H5FeO7) <SEP> 1,2 <SEP> to <SEP> 60 <SEP> g / liter
<Tb>
<tb> Sulphate <SEP> of <SEP> copper <SEP> (II) <SEP> and / or <SEP> chloride
<Tb>
<tb> from <SEP> copper <SEP> (II) <SEP> (CUS04 <SEP> and / or <SEP> CuCI2) <SEP> 0.5 <SEP> to <SEP> 3 <SEP> g / liter
<Tb>
<tb> Tartaric acid <SEP> <SEP> (C4H606) <SEP> 0,

  4 <SEP> to <SEP> 21 <SEP> g / liter
<Tb>
<tb> Salt <SEP> sodium <SEP> of ether <SEP> mixed <SEP> carboxy-
<Tb>
<tb> methyl <SEP> and <SEP> 2-hydroxypropyl
<Tb>
<tb> from <SEP> eraser <SEP> from <SEP> guar <SEP> 1 <SEP> to <SEP> 50 <SEP> g / liter
<Tb>
<tb> Water <SEP> sufficient <SEP> quantity <SEP> for <SEP> to make <SEP> 1 <SEP> liter
<Tb>
 
The photosensitive solution is applied to a non-conductive substrate by soaking, screen printing, spraying, application with a roller or the like and is then air dried, accelerated drying with hot air at a maximum temperature of 80 C.

   The film thus obtained is irradiated using commonly used UV lamps and / or laser

 <Desc / Clms Page number 9>

 (by means of diodes) and having a spectrum at least between 250 and 450 nm, the time necessary for the film to receive a minimum energy of 25 mJ / cm2. If a selective metallization is desired, the irradiation will be done through a mask put in contact with the substrate. This results in the deposition of a selective or non-selective conductive copper layer.



  In the case of selective metallization, the non-irradiated parts are dissolved in an aqueous solution of tartaric acid. An electrolytic metal overload is then made possible, the substrate being made conductive.



   Example 4
Photosensitive solution for the deposition of catalytic palladium on an insulating substrate, in one step Composition of the solution:
Concentration Iron (III) oxalate [Fe2 (C204) 3] 1.2 to 60 g / liter Palladium (II) chloride (PdCb) 0.5 to 3 g / liter Tartaric acid (C4H606) 0.4 to 21 g / liter Sodium salt of mixed carboxy-methyl and 2-hydroxypropyl ether of guar gum 1 to 50 g / liter Water sufficient to make 1 liter
The procedure is as in Example 3 and a layer of catalytic palladium, selective or not, is obtained. In the case of selective metallization, the non-irradiated parts are dissolved in an aqueous solution of tartaric acid.

   The catalytic palladium thus obtained can be metallized by then immersing the substrate in an autocatalytic bath.



   The substrates tested in the context of the above examples are ceramics, glass, plastics of the polyimide type,

 <Desc / Clms Page number 10>

 polyetherimide, PVC, epoxy, ABS, polycarbonate, polyamide or the like.



   In addition to the clearly defined advantages of the photosensitive solution of the invention compared to known polymeric resins, it should be noted that it does not contain any basic or base compound of the potassium hydroxide, sodium hydroxide or other type, which are always compounds which are difficult to handle due to their toxicity.



   It should be understood that the present invention is in no way limited to the embodiments described above and that many modifications can be made without departing from the scope of this patent.

Claims (18)

  1.  CLAIMS 1. Photosensitive solution with adjustable viscosity for depositing metal on an insulating substrate, characterized in that it comprises, in combination, an iron (III) compound, a metal salt, a film-forming polymer soluble in water, a complexing agent for iron (III) and / or the metal salt and a solvent chosen from water, ethanol, isopropanol, butanol and acetone.
  2.  2. Solution according to claim 1, characterized in that the iron compound (III) is an iron (III) salt.
  3.  3. Solution according to claim 2, characterized in that the iron salt (III) is chosen from iron oxalate (III), iron citrate (III), iron tartrate (III) and mixtures of 'at least two of these.
  4.  4. Solution according to any one of claims 1 to 3, characterized in that the metal salt is a transition metal salt.
  5.  5. Solution according to claim 4, characterized in that the transition metal is chosen from the group comprising copper, gold, silver, platinum, palladium, nickel and cobalt.
  6.  6. Solution according to claim 5, characterized in that the transition metal salt is chosen from copper (II) sulphate, copper (II) chloride, palladium (II) chloride and mixtures of minus two of these.
  7.  7. Solution according to any one of claims 1 to 6, characterized in that the water-soluble film-forming polymer is a polymer containing hydroxyl and / or carboxyl groups.
  8.  8. Solution according to claim 7, characterized in that the polymer containing hydroxyl and / or carboxyl groups is chosen from the group comprising cellulosic polymers, acrylic polymers, polysaccharides, polyvinyl compounds of the polyvinyl pyrrolidone type and polyvinyl alcohol and their mixtures.  <Desc / Clms Page number 12>  
  9.  9. Solution according to any one of claims 1 to 8, characterized in that the complexing agent for iron (III) and / or the metal salt is of the carboxylic acid, chloride or sulfate type.
  10.  10. Solution according to claim 9, characterized in that the complexing agent of the carboxylic acid type is tartaric acid, ethylenediamine tetraacetic acid or a mixture of these.
  11.  11. Solution according to any one of claims 8 to 10, characterized in that it comprises, as polysaccharide, a sodium salt of a mixed carboxymethyl and 2-hydroxypropyl ether of guar gum.
  12.  12. Solution according to any one of claims 1 to 11, characterized in that it further comprises at least one dye, a surfactant, an anti-foaming agent, an organic solvent or a combination of two or more of these agents.
  13.  13. Solution according to any one of claims 1 to 12, characterized in that the concentration of iron compound (III), per liter of solution, is from 0.5 to 100 g and preferably from 1.2 to 60 g.
  14.  14. Solution according to any one of claims 1 to 13, characterized in that the concentration of metal salt, per liter of solution, is from 0.1 to 5 g and preferably from 0.5 to 3 g.
  15.  15. Solution according to any one of claims 1 to 14, characterized in that the concentration of water-soluble film-forming polymer, per liter of solution, is from 0.1 to 100 g and preferably from 1 to 50 g .
  16.  16. Solution according to any one of claims 1 to 15, characterized in that the concentration of complexing agent, per liter of solution, is from 0.1 to 50 g and preferably from 0.4 to 25 g.
  17.  17. A method of depositing metal on the surface of an insulating substrate, using the photosensitive solution according to any one of claims 1 to 16, characterized in that it comprises the application of said solution under the film form on the substrate  <Desc / Clms Page number 13>  in a selective manner or not, the drying of the film applied to said substrate and the irradiation using ultraviolet and / or laser radiation of a range of wavelengths between 190 and 450 nm and d '' an energy of between 25 mJ / cm 2 to 100 mJ / cm 2 until a selective or non-selective metal layer is obtained on the substrate.
  18.  18. A method of depositing metal on the surface of an insulating substrate, using the photosensitive solution according to any one of claims 1 to 16, characterized in that it comprises the application of a part of said solution comprising at least the iron compound (III) and the polymer, in the form of a film on the substrate in a selective manner or not, drying the film applied to said substrate, irradiation using ultraviolet and / or laser radiation with a range of wavelengths between 190 and 450 nm and an energy between 25 mJ / cm2 and 100 mJ / cm2 and the soaking of the substrate thus irradiated in the part remaining of the above-mentioned solution comprising at least the metal salt and the complexing agent until a selective or non-selective metal layer is obtained on said substrate.
BE2002/0278A 2002-04-23 2002-04-23 Photosensitive solution for depositing metal on an insulating substrate comprises an iron(III) compound, a metal salt, a water-soluble film-forming polymer, a complexing agent and a solvent BE1014795A3 (en)

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BE2002/0278A BE1014795A3 (en) 2002-04-23 2002-04-23 Photosensitive solution for depositing metal on an insulating substrate comprises an iron(III) compound, a metal salt, a water-soluble film-forming polymer, a complexing agent and a solvent

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH03250074A (en) * 1990-02-28 1991-11-07 Pentel Kk Water-based ink composition for ball-point pen
EP0687311B1 (en) * 1994-01-05 1998-04-01 Blue Chips Holding Polymeric resin for depositing catalytic palladium on a substrate
US6210781B1 (en) * 1994-06-06 2001-04-03 International Business Machines Corporation Method for photoselective seeding and metallization of three-dimensional materials

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH03250074A (en) * 1990-02-28 1991-11-07 Pentel Kk Water-based ink composition for ball-point pen
EP0687311B1 (en) * 1994-01-05 1998-04-01 Blue Chips Holding Polymeric resin for depositing catalytic palladium on a substrate
US6210781B1 (en) * 1994-06-06 2001-04-03 International Business Machines Corporation Method for photoselective seeding and metallization of three-dimensional materials

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
DATABASE WPI Section Ch Week 199151, Derwent World Patents Index; Class A11, AN 1991-372762, XP002227057 *

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