JPS631016A - Electrolyte for capacitor - Google Patents
Electrolyte for capacitorInfo
- Publication number
- JPS631016A JPS631016A JP14458386A JP14458386A JPS631016A JP S631016 A JPS631016 A JP S631016A JP 14458386 A JP14458386 A JP 14458386A JP 14458386 A JP14458386 A JP 14458386A JP S631016 A JPS631016 A JP S631016A
- Authority
- JP
- Japan
- Prior art keywords
- quaternary phosphonium
- electrolyte
- capacitor
- silicic acid
- solvents
- 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.)
- Pending
Links
- 239000003990 capacitor Substances 0.000 title claims description 10
- 239000003792 electrolyte Substances 0.000 title description 6
- 150000004714 phosphonium salts Chemical group 0.000 claims description 10
- 239000008151 electrolyte solution Substances 0.000 claims description 7
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 claims description 7
- 235000012239 silicon dioxide Nutrition 0.000 claims description 7
- 239000002904 solvent Substances 0.000 description 14
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 8
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 6
- PCYIUVKHYVQEPD-UHFFFAOYSA-N CC[PH3]CC Chemical compound CC[PH3]CC PCYIUVKHYVQEPD-UHFFFAOYSA-N 0.000 description 3
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 3
- XCPGSFBEQZMSTL-UHFFFAOYSA-N butyl(triethyl)phosphanium Chemical compound CCCC[P+](CC)(CC)CC XCPGSFBEQZMSTL-UHFFFAOYSA-N 0.000 description 3
- 239000000428 dust Substances 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- OZJPLYNZGCXSJM-UHFFFAOYSA-N 5-valerolactone Chemical compound O=C1CCCCO1 OZJPLYNZGCXSJM-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- ZXULZCCIIYDGCE-UHFFFAOYSA-N CC[PH3]C Chemical compound CC[PH3]C ZXULZCCIIYDGCE-UHFFFAOYSA-N 0.000 description 2
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 2
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 description 2
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- PMDCZENCAXMSOU-UHFFFAOYSA-N N-ethylacetamide Chemical compound CCNC(C)=O PMDCZENCAXMSOU-UHFFFAOYSA-N 0.000 description 2
- ATHHXGZTWNVVOU-UHFFFAOYSA-N N-methylformamide Chemical compound CNC=O ATHHXGZTWNVVOU-UHFFFAOYSA-N 0.000 description 2
- LKMVFSZYGHUDKW-UHFFFAOYSA-N dibutyl(diethyl)phosphanium Chemical compound CCCC[P+](CC)(CC)CCCC LKMVFSZYGHUDKW-UHFFFAOYSA-N 0.000 description 2
- UUWXBQMAEMOZSL-UHFFFAOYSA-N dimethyl(dipropyl)phosphanium Chemical compound CCC[P+](C)(C)CCC UUWXBQMAEMOZSL-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- GAEKPEKOJKCEMS-UHFFFAOYSA-N gamma-valerolactone Chemical compound CC1CCC(=O)O1 GAEKPEKOJKCEMS-UHFFFAOYSA-N 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- OOWFYDWAMOKVSF-UHFFFAOYSA-N 3-methoxypropanenitrile Chemical compound COCCC#N OOWFYDWAMOKVSF-UHFFFAOYSA-N 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
- 239000005977 Ethylene Substances 0.000 description 1
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 1
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 1
- SUAKHGWARZSWIH-UHFFFAOYSA-N N,N‐diethylformamide Chemical compound CCN(CC)C=O SUAKHGWARZSWIH-UHFFFAOYSA-N 0.000 description 1
- OHLUUHNLEMFGTQ-UHFFFAOYSA-N N-methylacetamide Chemical compound CNC(C)=O OHLUUHNLEMFGTQ-UHFFFAOYSA-N 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- 150000008043 acidic salts Chemical class 0.000 description 1
- 239000005456 alcohol based solvent Substances 0.000 description 1
- 125000001931 aliphatic group Chemical group 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- YQPAAVMEUPILEE-UHFFFAOYSA-N butyl(trimethyl)phosphanium Chemical compound CCCC[P+](C)(C)C YQPAAVMEUPILEE-UHFFFAOYSA-N 0.000 description 1
- ARTHGSQAXVXICL-UHFFFAOYSA-N butyl(tripropyl)phosphanium Chemical compound CCCC[P+](CCC)(CCC)CCC ARTHGSQAXVXICL-UHFFFAOYSA-N 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- BBWVMXYKVQQWCK-UHFFFAOYSA-N dibutyl(dimethyl)phosphanium Chemical compound CCCC[P+](C)(C)CCCC BBWVMXYKVQQWCK-UHFFFAOYSA-N 0.000 description 1
- RBECNRCKEQGFRU-UHFFFAOYSA-N diethyl(dimethyl)phosphanium Chemical compound CC[P+](C)(C)CC RBECNRCKEQGFRU-UHFFFAOYSA-N 0.000 description 1
- 239000003759 ester based solvent Substances 0.000 description 1
- ATSROVAZOQKRJM-UHFFFAOYSA-N ethyl(tripropyl)phosphanium Chemical compound CCC[P+](CC)(CCC)CCC ATSROVAZOQKRJM-UHFFFAOYSA-N 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 239000003925 fat Substances 0.000 description 1
- 238000000855 fermentation Methods 0.000 description 1
- 230000004151 fermentation Effects 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 235000011187 glycerol Nutrition 0.000 description 1
- 150000002596 lactones Chemical class 0.000 description 1
- 231100000053 low toxicity Toxicity 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- AJFDBNQQDYLMJN-UHFFFAOYSA-N n,n-diethylacetamide Chemical compound CCN(CC)C(C)=O AJFDBNQQDYLMJN-UHFFFAOYSA-N 0.000 description 1
- KERBAAIBDHEFDD-UHFFFAOYSA-N n-ethylformamide Chemical compound CCNC=O KERBAAIBDHEFDD-UHFFFAOYSA-N 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
- OYLRFHLPEAGKJU-UHFFFAOYSA-N phosphane silicic acid Chemical group P.[Si](O)(O)(O)O OYLRFHLPEAGKJU-UHFFFAOYSA-N 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- XYFCBTPGUUZFHI-UHFFFAOYSA-O phosphonium Chemical compound [PH4+] XYFCBTPGUUZFHI-UHFFFAOYSA-O 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 1
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 1
- 239000012487 rinsing solution Substances 0.000 description 1
- 239000000565 sealant Substances 0.000 description 1
- BJQWBACJIAKDTJ-UHFFFAOYSA-N tetrabutylphosphanium Chemical compound CCCC[P+](CCCC)(CCCC)CCCC BJQWBACJIAKDTJ-UHFFFAOYSA-N 0.000 description 1
- -1 tetrabutylphosphonium silicic acid Chemical compound 0.000 description 1
- BXYHVFRRNNWPMB-UHFFFAOYSA-N tetramethylphosphanium Chemical compound C[P+](C)(C)C BXYHVFRRNNWPMB-UHFFFAOYSA-N 0.000 description 1
- XOGCTUKDUDAZKA-UHFFFAOYSA-N tetrapropylphosphanium Chemical compound CCC[P+](CCC)(CCC)CCC XOGCTUKDUDAZKA-UHFFFAOYSA-N 0.000 description 1
- HOMONHWYLOPSLL-UHFFFAOYSA-N tributyl(ethyl)phosphanium Chemical compound CCCC[P+](CC)(CCCC)CCCC HOMONHWYLOPSLL-UHFFFAOYSA-N 0.000 description 1
- XKFPGUWSSPXXMF-UHFFFAOYSA-N tributyl(methyl)phosphanium Chemical compound CCCC[P+](C)(CCCC)CCCC XKFPGUWSSPXXMF-UHFFFAOYSA-N 0.000 description 1
- WJLSOXBTGDOFOQ-UHFFFAOYSA-N tributyl(propyl)phosphanium Chemical compound CCCC[P+](CCC)(CCCC)CCCC WJLSOXBTGDOFOQ-UHFFFAOYSA-N 0.000 description 1
- WVLBCYQITXONBZ-UHFFFAOYSA-N trimethyl phosphate Chemical compound COP(=O)(OC)OC WVLBCYQITXONBZ-UHFFFAOYSA-N 0.000 description 1
Landscapes
- Electric Double-Layer Capacitors Or The Like (AREA)
- Networks Using Active Elements (AREA)
Abstract
(57)【要約】本公報は電子出願前の出願データであるた
め要約のデータは記録されません。(57) [Summary] This bulletin contains application data before electronic filing, so abstract data is not recorded.
Description
【発明の詳細な説明】
産業上の利用分野
本発明によれば、電導塵の高い優れたコンデンサ用電解
液（以下単Ｋｔ解液と称することがある）が得られる。DETAILED DESCRIPTION OF THE INVENTION Industrial Field of Application According to the present invention, an excellent electrolytic solution for capacitors (hereinafter sometimes referred to as a single Kt solution) with high conductive dust can be obtained.
従来の技術
］ンデンサの特性は種々の要因によって決定されている
が、特にコンデンサ素子とともに外装ケースに収納され
る電解液のＩＦＩ性は、インピーダンスあるいは等価直
列抵抗（ＥＳＲ）に大きな影響を及ぼすことが判明して
いる。[Prior art] The characteristics of a capacitor are determined by various factors, but in particular, the IFI properties of the electrolyte that is housed in the outer case together with the capacitor element can have a large effect on the impedance or equivalent series resistance (ESR). It's clear.
たとえば、電解コンデンサには、従来よりエチレングリ
コール−アジピンｒ皮アンモニウム系の′Ｌ孔酵解液使
用されている。For example, in electrolytic capacitors, ethylene glycol-adipine ammonium-based L-pore fermentation solution has been used.
発明が解決しようとする問題点
しかし、近年のスイッチングレギニレーターの高周波化
に伴ない、更に低インピーダンスあるいは低等価直列抵
抗のコンデンサが必要となり、高電導度の電解液の開発
が望まれている。Problems to be Solved by the Invention However, as the frequency of switching regulators has increased in recent years, capacitors with even lower impedance or lower equivalent series resistance are required, and the development of electrolytes with high conductivity is desired. .
問題点を解決するための手段
本発明者らは、電導塵の高い電解液を見い出すべく鋭意
検討を行ない、硅酸の四級ホスホニウム塩が高い電導塵
を示すことを見い出し本発明を完成した。Means for Solving the Problems The present inventors conducted intensive studies to find an electrolytic solution with high conductive dust, and found that a quaternary phosphonium salt of silicic acid exhibits high conductive dust, and completed the present invention.
即ち、本発明は硅酸の四級ホスホニウム塩を溶質として
使用することを特徴とするコンデンサ用濯解腹を提供す
るものである。That is, the present invention provides a rinsing solution for a capacitor characterized in that a quaternary phosphonium salt of silicic acid is used as a solute.
発明の詳細な説明
本発明において溶質として用いられる硅酸の四級ホスホ
ニウムにおける四級ホスホニウム塩としては、テトラメ
チルホスホニウム、テトラエテルホスホニウム、テトラ
プロピルホスホニウム、テトラブチルホスホニウム、メ
チルトリエテルホスホニウム、メチルトリプロピルホス
ホニウム、メチルトリブチルホスホニウム、ジメチルジ
エチルホスホニウム、ジメチルジプロピルホスホニウム
、ジメチルジブチルホスホニウム、トリメデルエチルホ
スホニウム、トリエチルブチルホスホニウム、トリメチ
ルブチルホスホニウム、エチルトリプロピルホスホニウ
ム、エチルトリブチルホスホニウム、ジメチルジプロピ
ルホスホニウム、ジエチルジブチルホスホニウム、トリ
エチルブチルホスホニウム、トリエチルブチルホスホニ
ウム、プロピルトリブチルホスホニウム、ジエチルジブ
チルホスホニウム、トリプロピルブチルホスホニウム等
の脂肪族四級ホスホニウム塩および、１゜１−ジメチル
ホスホラニウム、１−メチル−１−エチルホスホラニウ
ム、１，１−ジエチルホスホラニウム、１，１−ジエチ
ルホスホラニウム、１−メチル−１−エチルホスホラニ
ウム、１．１−ジエチルホスホラニウム、１，１−ペン
タメチレンホスホリナニウム等の脂環式四級ホスホニウ
ム塩を例示することができる。Detailed Description of the Invention Examples of quaternary phosphonium salts of quaternary phosphonium silicic acid used as solutes in the present invention include tetramethylphosphonium, tetraetherphosphonium, tetrapropylphosphonium, tetrabutylphosphonium, methyltrietherphosphonium, and methyltripropyl. Phosphonium, methyltributylphosphonium, dimethyldiethylphosphonium, dimethyldipropylphosphonium, dimethyldibutylphosphonium, trimedelethylphosphonium, triethylbutylphosphonium, trimethylbutylphosphonium, ethyltripropylphosphonium, ethyltributylphosphonium, dimethyldipropylphosphonium, diethyldibutylphosphonium, Aliphatic quaternary phosphonium salts such as triethylbutylphosphonium, triethylbutylphosphonium, propyltributylphosphonium, diethyldibutylphosphonium, tripropylbutylphosphonium, 1゜1-dimethylphosphoranium, 1-methyl-1-ethylphosphoranium, Fats such as 1,1-diethylphosphoranium, 1,1-diethylphosphoranium, 1-methyl-1-ethylphosphoranium, 1,1-diethylphosphoranium, 1,1-pentamethylenephosphoranium, etc. Examples include cyclic quaternary phosphonium salts.
本発明の硅酸の四級ホスホニウム塩を溶解させる溶媒と
しては、Ｎ−メチルホルムアミド、Ｎ−エチルホルムア
ミド、Ｎ、Ｎ−ジメチルホルムアミド、Ｎ、Ｎ−ジエチ
ルホルムアミド、Ｎ−メチルアセトアミド、Ｎ−エチル
アセトアミド、Ｎ、Ｎ−ジメチルアセトアミド、Ｎ、Ｎ
−ジエチルアセトアミド、Ｎ−メチルピロリジノン等の
アミド溶媒、γ−ブチロラクトン、γ−バレロラクトン
、δ−バレロラクトン等のラクトン溶媒、エチレンカー
ボネート、フロピレンカーボ＊ −） 、７’ ｆ ｖ
ンカーボネート等のカーボネート溶媒、エチレングリ
コール、グリセリン、メチルセロソルプ等のアルコール
溶媒、３−メトキシプロピオニトリル等のニトリル溶媒
、およびトリメチルホスフェート等の燐酸エステル溶媒
の単独あるいは混合溶媒を例示することができる。これ
らの中でもγ−ブチロラクトンを主体とする溶媒が毒性
が低く、コンデンサの封孔剤のアタックやノ・ロゲンの
混入が少ない等のことから特に好ましい。Examples of solvents for dissolving the quaternary phosphonium salt of silicic acid of the present invention include N-methylformamide, N-ethylformamide, N,N-dimethylformamide, N,N-diethylformamide, N-methylacetamide, and N-ethylacetamide. , N, N-dimethylacetamide, N, N
- Amide solvents such as diethylacetamide and N-methylpyrrolidinone, lactone solvents such as γ-butyrolactone, γ-valerolactone, and δ-valerolactone, ethylene carbonate, propylene carb* -), 7' f v
Examples include carbonate solvents such as carbonate, alcohol solvents such as ethylene glycol, glycerin, and methyl cellosolp, nitrile solvents such as 3-methoxypropionitrile, and phosphate ester solvents such as trimethyl phosphate, either alone or in combination. Among these, a solvent mainly composed of γ-butyrolactone is particularly preferred because it has low toxicity and is less likely to attack the capacitor sealant or be contaminated with nitrogen.
上記溶媒に対する硅酸の四級ホスホニウム塩の溶解量は
飽和濃度以下、好ましくは１〜４０重量シである。The amount of the quaternary phosphonium salt of silicic acid dissolved in the above solvent is below the saturation concentration, preferably 1 to 40% by weight.
また、上記電解液中の溶解塩は中性塩でも酸性塩でも良
い。Further, the dissolved salt in the electrolytic solution may be a neutral salt or an acidic salt.
本発明の電解液は、本質的には、硅酸の四級ホスホニウ
ム塩と溶媒よりなるが、電蝕防止、漏れば流の低減等、
種々の目的で少量の助溶質を添加しても差し支えない。The electrolytic solution of the present invention essentially consists of a quaternary phosphonium salt of silicic acid and a solvent, but it can prevent galvanic corrosion, reduce flow if it leaks, etc.
Small amounts of co-solutes may be added for various purposes.
発明の効果
本発明で溶質として使用する硅酸の四級ホスホニウム塩
は溶媒に対する溶解性が良く、その電解液は高い電導度
を示し、凝固点〜沸点範囲の広い溶媒と伴に用いること
により、使用温度範囲の広いコンデンサ用電解液となる
。Effects of the Invention The quaternary phosphonium salt of silicic acid used as a solute in the present invention has good solubility in solvents, and its electrolyte exhibits high conductivity. This is an electrolyte for capacitors that has a wide temperature range.
実倹例 以下に実施例を挙げて本発明を更に具体的に説明する。practical example The present invention will be explained in more detail with reference to Examples below.
実施例１
γ−プチロジクトン溶媒に２０重計％の硅酸のテトラブ
チルホスホニウム塩をｄ解させて電解液を得た。この１
攬解夜の２５℃における電導度は４．５ ｍＳ／ｃＷｔ
であり、＋、−一組のアルミニウム平滑箔に４ｍＡ／ｃ
Ｊの定を流印加時の火花発生ル圧は４１０ｖであった。Example 1 An electrolytic solution was obtained by dissolving 20% by weight of tetrabutylphosphonium silicic acid in a γ-butyrodictone solvent. This one
The conductivity at 25°C on the night of extraction is 4.5 mS/cWt.
4 mA/c to a set of + and - aluminum smooth foils.
The spark generation pressure when a constant J current was applied was 410V.
実施例２
実施例１において、γ−ブチロラクトン溶媒の代わりに
、Ｎ、Ｎ−ジメチルホルムアミド溶媒を使用した電解液
の電導度および火花発生屯田はそれぞれ６−１ ｍｓ／
ｏｎ、 ５００ ｖであった。Example 2 In Example 1, the conductivity and spark generation rate of the electrolytic solution using N,N-dimethylformamide solvent instead of the γ-butyrolactone solvent were 6-1 ms/1, respectively.
on, 500v.
実施例３
実施例１において、γ−ブチロラクトン溶媒の代わ９に
、プロピレンカーボネート溶媒を防用した電解液の電導
度および火花発生磁圧はそれぞれ４ 、７ ｍｓ／ ｏ
ｎ、５００ｖであった。Example 3 In Example 1, a propylene carbonate solvent was used instead of the γ-butyrolactone solvent, and the conductivity and spark generation magnetic pressure of the electrolyte were 4 and 7 ms/o, respectively.
n, 500v.
Claims (1)
を特徴とするコンデンサ用電解液。An electrolytic solution for capacitors characterized by using a quaternary phosphonium salt of silicic acid as a solute.
Priority Applications (4)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP14458386A JPS631016A (en) | 1986-06-20 | 1986-06-20 | Electrolyte for capacitor |
| EP87304335A EP0246825B1 (en) | 1986-05-20 | 1987-05-15 | Quaternary salt solution electrolyte for electrolytic capacitors |
| DE8787304335T DE3768141D1 (en) | 1986-05-20 | 1987-05-15 | ELECTROLYTIC SOLUTION OF QUATERNAIAL SALTS FOR ELECTROLYTIC CAPACITOR. |
| US07/050,574 US4774011A (en) | 1986-05-20 | 1987-05-18 | Electrolyte for aluminum electrolytic capacitor |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP14458386A JPS631016A (en) | 1986-06-20 | 1986-06-20 | Electrolyte for capacitor |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS631016A true JPS631016A (en) | 1988-01-06 |
Family
ID=15365495
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP14458386A Pending JPS631016A (en) | 1986-05-20 | 1986-06-20 | Electrolyte for capacitor |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS631016A (en) |
-
1986
- 1986-06-20 JP JP14458386A patent/JPS631016A/en active Pending
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