JP6309361B2 - ポリビニルブチラールとポリビニルピロリドンバインダーを含む導電性金属インク - Google Patents
ポリビニルブチラールとポリビニルピロリドンバインダーを含む導電性金属インク Download PDFInfo
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- JP6309361B2 JP6309361B2 JP2014123751A JP2014123751A JP6309361B2 JP 6309361 B2 JP6309361 B2 JP 6309361B2 JP 2014123751 A JP2014123751 A JP 2014123751A JP 2014123751 A JP2014123751 A JP 2014123751A JP 6309361 B2 JP6309361 B2 JP 6309361B2
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- conductive
- polyvinyl butyral
- terpolymer
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- 229920002037 poly(vinyl butyral) polymer Polymers 0.000 title claims description 45
- 229920000036 polyvinylpyrrolidone Polymers 0.000 title claims description 34
- 239000001267 polyvinylpyrrolidone Substances 0.000 title claims description 34
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 title claims description 34
- 239000011230 binding agent Substances 0.000 title claims description 30
- 229910052751 metal Inorganic materials 0.000 title description 7
- 239000002184 metal Substances 0.000 title description 7
- 229920001897 terpolymer Polymers 0.000 claims description 41
- 239000002904 solvent Substances 0.000 claims description 33
- 239000004020 conductor Substances 0.000 claims description 19
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 18
- 229910052709 silver Inorganic materials 0.000 claims description 18
- 239000004332 silver Substances 0.000 claims description 18
- 125000004432 carbon atom Chemical group C* 0.000 claims description 17
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 claims description 12
- RTZKZFJDLAIYFH-UHFFFAOYSA-N ether Substances CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 12
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical group OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 11
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 claims description 9
- 125000000217 alkyl group Chemical group 0.000 claims description 9
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- 239000004416 thermosoftening plastic Substances 0.000 claims description 8
- 125000004169 (C1-C6) alkyl group Chemical group 0.000 claims description 7
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- 125000003118 aryl group Chemical group 0.000 claims description 4
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- 238000000151 deposition Methods 0.000 description 7
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- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 3
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- SVTBMSDMJJWYQN-UHFFFAOYSA-N 2-methylpentane-2,4-diol Chemical compound CC(O)CC(C)(C)O SVTBMSDMJJWYQN-UHFFFAOYSA-N 0.000 description 2
- FFWSICBKRCICMR-UHFFFAOYSA-N 5-methyl-2-hexanone Chemical compound CC(C)CCC(C)=O FFWSICBKRCICMR-UHFFFAOYSA-N 0.000 description 2
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- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- 239000004812 Fluorinated ethylene propylene Substances 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- DKGAVHZHDRPRBM-UHFFFAOYSA-N Tert-Butanol Chemical compound CC(C)(C)O DKGAVHZHDRPRBM-UHFFFAOYSA-N 0.000 description 2
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 2
- YRKCREAYFQTBPV-UHFFFAOYSA-N acetylacetone Chemical compound CC(=O)CC(C)=O YRKCREAYFQTBPV-UHFFFAOYSA-N 0.000 description 2
- 238000013019 agitation Methods 0.000 description 2
- 229910045601 alloy Inorganic materials 0.000 description 2
- 239000012298 atmosphere Substances 0.000 description 2
- BTANRVKWQNVYAZ-UHFFFAOYSA-N butan-2-ol Chemical compound CCC(C)O BTANRVKWQNVYAZ-UHFFFAOYSA-N 0.000 description 2
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- JHIVVAPYMSGYDF-UHFFFAOYSA-N cyclohexanone Chemical compound O=C1CCCCC1 JHIVVAPYMSGYDF-UHFFFAOYSA-N 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- SWXVUIWOUIDPGS-UHFFFAOYSA-N diacetone alcohol Chemical compound CC(=O)CC(C)(C)O SWXVUIWOUIDPGS-UHFFFAOYSA-N 0.000 description 2
- DOIRQSBPFJWKBE-UHFFFAOYSA-N dibutyl phthalate Chemical compound CCCCOC(=O)C1=CC=CC=C1C(=O)OCCCC DOIRQSBPFJWKBE-UHFFFAOYSA-N 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 description 2
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- 150000002576 ketones Chemical class 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- UAEPNZWRGJTJPN-UHFFFAOYSA-N methylcyclohexane Chemical compound CC1CCCCC1 UAEPNZWRGJTJPN-UHFFFAOYSA-N 0.000 description 2
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 2
- XNLICIUVMPYHGG-UHFFFAOYSA-N pentan-2-one Chemical compound CCCC(C)=O XNLICIUVMPYHGG-UHFFFAOYSA-N 0.000 description 2
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- WUOACPNHFRMFPN-SECBINFHSA-N (S)-(-)-alpha-terpineol Chemical compound CC1=CC[C@@H](C(C)(C)O)CC1 WUOACPNHFRMFPN-SECBINFHSA-N 0.000 description 1
- RUJPNZNXGCHGID-UHFFFAOYSA-N (Z)-beta-Terpineol Natural products CC(=C)C1CCC(C)(O)CC1 RUJPNZNXGCHGID-UHFFFAOYSA-N 0.000 description 1
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- LTMRRSWNXVJMBA-UHFFFAOYSA-L 2,2-diethylpropanedioate Chemical compound CCC(CC)(C([O-])=O)C([O-])=O LTMRRSWNXVJMBA-UHFFFAOYSA-L 0.000 description 1
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- CATSNJVOTSVZJV-UHFFFAOYSA-N heptan-2-one Chemical compound CCCCCC(C)=O CATSNJVOTSVZJV-UHFFFAOYSA-N 0.000 description 1
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- 125000004051 hexyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 1
- 229940051250 hexylene glycol Drugs 0.000 description 1
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- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 1
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- 229940035429 isobutyl alcohol Drugs 0.000 description 1
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- OQAGVSWESNCJJT-UHFFFAOYSA-N isovaleric acid methyl ester Natural products COC(=O)CC(C)C OQAGVSWESNCJJT-UHFFFAOYSA-N 0.000 description 1
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- 238000001459 lithography Methods 0.000 description 1
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- 238000004519 manufacturing process Methods 0.000 description 1
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- 229910001092 metal group alloy Inorganic materials 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- 229940017219 methyl propionate Drugs 0.000 description 1
- GYNNXHKOJHMOHS-UHFFFAOYSA-N methyl-cycloheptane Natural products CC1CCCCCC1 GYNNXHKOJHMOHS-UHFFFAOYSA-N 0.000 description 1
- 238000000813 microcontact printing Methods 0.000 description 1
- 230000003278 mimic effect Effects 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 1
- JTHNLKXLWOXOQK-UHFFFAOYSA-N n-propyl vinyl ketone Natural products CCCC(=O)C=C JTHNLKXLWOXOQK-UHFFFAOYSA-N 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- JCGNDDUYTRNOFT-UHFFFAOYSA-N oxolane-2,4-dione Chemical compound O=C1COC(=O)C1 JCGNDDUYTRNOFT-UHFFFAOYSA-N 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 238000000059 patterning Methods 0.000 description 1
- 125000001147 pentyl group Chemical group C(CCCC)* 0.000 description 1
- TWSRVQVEYJNFKQ-UHFFFAOYSA-N pentyl propanoate Chemical compound CCCCCOC(=O)CC TWSRVQVEYJNFKQ-UHFFFAOYSA-N 0.000 description 1
- 229920003023 plastic Polymers 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
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- 239000004014 plasticizer Substances 0.000 description 1
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- 229920001483 poly(ethyl methacrylate) polymer Polymers 0.000 description 1
- 229920001200 poly(ethylene-vinyl acetate) Polymers 0.000 description 1
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 1
- 229920002647 polyamide Polymers 0.000 description 1
- 229920001083 polybutene Polymers 0.000 description 1
- 229920000515 polycarbonate Polymers 0.000 description 1
- 239000004417 polycarbonate Substances 0.000 description 1
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- 229920002959 polymer blend Polymers 0.000 description 1
- 239000002952 polymeric resin Substances 0.000 description 1
- 239000004926 polymethyl methacrylate Substances 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 229920005996 polystyrene-poly(ethylene-butylene)-polystyrene Polymers 0.000 description 1
- 239000011118 polyvinyl acetate Substances 0.000 description 1
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- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
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- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- 229940116423 propylene glycol diacetate Drugs 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 239000005060 rubber Substances 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000010008 shearing Methods 0.000 description 1
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- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000011877 solvent mixture Substances 0.000 description 1
- 238000004528 spin coating Methods 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
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- 229920006132 styrene block copolymer Polymers 0.000 description 1
- 229920000468 styrene butadiene styrene block copolymer Polymers 0.000 description 1
- 229920003002 synthetic resin Polymers 0.000 description 1
- QJVXKWHHAMZTBY-GCPOEHJPSA-N syringin Chemical compound COC1=CC(\C=C\CO)=CC(OC)=C1O[C@H]1[C@H](O)[C@@H](O)[C@H](O)[C@@H](CO)O1 QJVXKWHHAMZTBY-GCPOEHJPSA-N 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- KKEYFWRCBNTPAC-UHFFFAOYSA-L terephthalate(2-) Chemical compound [O-]C(=O)C1=CC=C(C([O-])=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-L 0.000 description 1
- 229920006029 tetra-polymer Polymers 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
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- ZIBGPFATKBEMQZ-UHFFFAOYSA-N triethylene glycol Chemical compound OCCOCCOCCO ZIBGPFATKBEMQZ-UHFFFAOYSA-N 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
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- 238000009281 ultraviolet germicidal irradiation Methods 0.000 description 1
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 description 1
- 229920002554 vinyl polymer Polymers 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
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Images
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
- C09D11/52—Electrically conductive inks
-
- 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
- C09D11/02—Printing inks
- C09D11/10—Printing inks based on artificial resins
- C09D11/106—Printing inks based on artificial resins containing macromolecular compounds obtained by reactions only involving carbon-to-carbon unsaturated bonds
Landscapes
- Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Wood Science & Technology (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Inks, Pencil-Leads, Or Crayons (AREA)
- Conductive Materials (AREA)
Description
を有するポリビニルブチラールターポリマーバインダーと、ポリビニルピロリドンと、溶媒とで構成される導電性インクを記載する。
ポリビニルブチルターポリマーおよびポリビニルピロリドンのポリマーブレンドの種々のサンプルを、ブチルカルビトールの15重量%溶液として調製した。PVBターポリマーとして、上述の式のPVBターポリマー(R1が結合であり、R2が3個の炭素原子を含むアルキル基であり、R3が1個の炭素原子を含むアルキル基である)を使用した。PVBターポリマーは、Mwが40,000〜150,000であり、Tgが72〜78℃である。PVPは、MWが55,000である。種々のサンプルの相対的なポリマー比を以下の表1にまとめる。
2〜5ミクロンの銀フレーク、PVPおよびPVBターポリマーバインダーおよび溶媒を用い、サンプルインクを調製した。バインダーとしてPVPのみを用い、比較例のインクも調製した。インクは以下の組成を有していた。
Claims (9)
- 導電性材料と、ポリビニルブチラールターポリマーおよびポリビニルピロリドンを含む熱可塑性バインダーと、溶媒とで構成され、
ポリビニルピロリドンとポリビニルブチラールターポリマーとの重量比は、1:3〜1:30である、導電性インク。 - 導電性材料は、平均粒径が0.5〜10ミクロンであり、アスペクト比として少なくとも3対1の導電性粒状物である、請求項1に記載の導電性インク。
- 導電性材料は、平均粒径が2〜10ミクロンの銀フレークである、請求項2に記載の導電性インク。
- ポリビニルブチラールターポリマーは、重量平均分子量が10,000〜600,000ダルトンであり、ガラス転移温度が60℃〜100℃である、請求項4に記載の導電性インク。
- 溶媒が、エチレングリコールジ−C1−C6−アルキルエーテル、プロピレングリコールジ−C1−C6−アルキルエーテル、ジエチレングリコールジ−C1−C6−アルキルエーテル、ジプロピレングリコールジ−C1−C6−アルキルエーテル、およびこれらの組み合わせからなる群から選択されるグリコールエーテル溶媒である、請求項1〜5のいずれか1項に記載の導電性インク。
- インクは、1s−1の剪断での粘度が20Pa・s以上であり、50s−1の剪断での粘度がこの値から低下する、請求項1〜6のいずれか1項に記載の導電性インク。
- 導電性材料と、ポリビニルブチラールターポリマーおよびポリビニルピロリドンを含む熱可塑性バインダーと、溶媒とで構成され、
ポリビニルピロリドンとポリビニルブチラールターポリマーとの重量比は、1:3〜1:30であり、
インクは、シート抵抗が11mΩ/sq./mil以下である、導電性インク。 - 平均粒径が2〜5ミクロンの銀フレークと、
以下の式
〔式中、R1は、化学結合または1〜20個の炭素を含む二価の炭化水素結合であり;R2およびR3は、独立して、1〜20個の炭素原子を含むアルキル基、芳香族基または置換芳香族基であり;x、yおよびzは、独立して、それぞれ重量%としてあらわされる対応する繰り返し単位の比率をあらわし、それぞれの繰り返し単位は、ポリマー鎖にランダムに分布しており、x、yおよびzの合計は100重量%であり、xは、5重量%〜40重量%であり、yは、50重量%〜95重量%であり、zは、0.1重量%〜15重量%である〕を有するポリビニルブチラールターポリマーバインダーと、
ポリビニルピロリドンと、
溶媒とで構成され、
ポリビニルピロリドンとポリビニルブチラールターポリマーとの重量比は、1:3〜1:30である、導電性インク。
Applications Claiming Priority (2)
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US13/925,352 US20140374671A1 (en) | 2013-06-24 | 2013-06-24 | Conductive metal inks with polyvinylbutyral and polyvinylpyrrolidone binder |
US13/925,352 | 2013-06-24 |
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JP2015007231A JP2015007231A (ja) | 2015-01-15 |
JP6309361B2 true JP6309361B2 (ja) | 2018-04-11 |
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JP2014123751A Expired - Fee Related JP6309361B2 (ja) | 2013-06-24 | 2014-06-16 | ポリビニルブチラールとポリビニルピロリドンバインダーを含む導電性金属インク |
Country Status (5)
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US (1) | US20140374671A1 (ja) |
JP (1) | JP6309361B2 (ja) |
CN (1) | CN104231749A (ja) |
CA (1) | CA2852317C (ja) |
DE (1) | DE102014211911A1 (ja) |
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JP6323666B2 (ja) * | 2014-03-31 | 2018-05-16 | セイコーエプソン株式会社 | インクジェット記録方法 |
ES2663623T3 (es) * | 2015-01-12 | 2018-04-16 | Heraeus Deutschland GmbH & Co. KG | Uso de una composición eléctricamente conductora como adhesivo eléctricamente conductor para conectar mecánica y eléctricamente conductores eléctricos con los contactos eléctricos de células solares |
EP3380571B1 (en) | 2016-03-24 | 2023-08-09 | Ferro Corporation | Fast conductivity polymer silver |
KR102069420B1 (ko) * | 2017-10-11 | 2020-01-22 | 국립암센터 | 표피 침투형 잉크 조성물 |
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JPS60186574A (ja) * | 1984-03-07 | 1985-09-24 | Mitsubishi Pencil Co Ltd | 金属光沢を有するボールペン用インキ |
JPH0529738A (ja) * | 1991-07-19 | 1993-02-05 | Tatsuta Electric Wire & Cable Co Ltd | フレキシブルプリント回路基板 |
JP4719473B2 (ja) * | 2005-01-12 | 2011-07-06 | バンドー化学株式会社 | 導電インクおよびその利用 |
US7691294B2 (en) * | 2005-03-04 | 2010-04-06 | Inktec Co., Ltd. | Conductive inks and manufacturing method thereof |
JP4754273B2 (ja) * | 2005-06-06 | 2011-08-24 | 日立マクセル株式会社 | インクジェット用導電性インク、導電性パターンおよび導電体 |
DK1917111T3 (en) * | 2005-08-24 | 2015-04-27 | A M Ramp & Co Gmbh | A process for the preparation of articles with electrically conductive coating |
US8158032B2 (en) * | 2010-08-20 | 2012-04-17 | Xerox Corporation | Silver nanoparticle ink composition for highly conductive features with enhanced mechanical properties |
JP6185229B2 (ja) * | 2011-11-04 | 2017-08-23 | ヘレウス プレシャス メタルズ ノース アメリカ コンショホーケン エルエルシー | 電気伝導性ペースト用有機媒体 |
US8952245B2 (en) * | 2012-01-23 | 2015-02-10 | Heraeus Precious Metals North America Conshohocken Llc | Conductive thick film paste for solar cell contacts |
-
2013
- 2013-06-24 US US13/925,352 patent/US20140374671A1/en not_active Abandoned
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2014
- 2014-05-21 CA CA2852317A patent/CA2852317C/en not_active Expired - Fee Related
- 2014-06-13 CN CN201410264452.0A patent/CN104231749A/zh active Pending
- 2014-06-16 JP JP2014123751A patent/JP6309361B2/ja not_active Expired - Fee Related
- 2014-06-20 DE DE201410211911 patent/DE102014211911A1/de not_active Withdrawn
Also Published As
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JP2015007231A (ja) | 2015-01-15 |
CA2852317C (en) | 2016-10-11 |
CN104231749A (zh) | 2014-12-24 |
CA2852317A1 (en) | 2014-12-24 |
DE102014211911A1 (de) | 2014-12-24 |
US20140374671A1 (en) | 2014-12-25 |
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