JPH0218688B2 - - Google Patents
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- Publication number
- JPH0218688B2 JPH0218688B2 JP12416384A JP12416384A JPH0218688B2 JP H0218688 B2 JPH0218688 B2 JP H0218688B2 JP 12416384 A JP12416384 A JP 12416384A JP 12416384 A JP12416384 A JP 12416384A JP H0218688 B2 JPH0218688 B2 JP H0218688B2
- Authority
- JP
- Japan
- Prior art keywords
- polymer material
- electrolyte solution
- voltage
- polymeric material
- bending
- 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.)
- Expired
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- 239000008151 electrolyte solution Substances 0.000 claims description 37
- 239000000463 material Substances 0.000 claims description 26
- 238000005452 bending Methods 0.000 claims description 18
- 125000000524 functional group Chemical group 0.000 claims description 13
- 238000000034 method Methods 0.000 claims description 11
- 230000008961 swelling Effects 0.000 claims description 10
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 claims description 2
- RWSOTUBLDIXVET-UHFFFAOYSA-O sulfonium group Chemical group [SH3+] RWSOTUBLDIXVET-UHFFFAOYSA-O 0.000 claims description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-O ammonium group Chemical group [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 claims 1
- 125000001174 sulfone group Chemical group 0.000 claims 1
- 239000002861 polymer material Substances 0.000 description 52
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 15
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 10
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 9
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 8
- 239000007864 aqueous solution Substances 0.000 description 8
- JHJLBTNAGRQEKS-UHFFFAOYSA-M sodium bromide Chemical compound [Na+].[Br-] JHJLBTNAGRQEKS-UHFFFAOYSA-M 0.000 description 8
- 150000002500 ions Chemical class 0.000 description 7
- 230000005684 electric field Effects 0.000 description 6
- 239000003792 electrolyte Substances 0.000 description 5
- 229920000642 polymer Polymers 0.000 description 5
- 230000002441 reversible effect Effects 0.000 description 5
- MYRTYDVEIRVNKP-UHFFFAOYSA-N 1,2-Divinylbenzene Chemical compound C=CC1=CC=CC=C1C=C MYRTYDVEIRVNKP-UHFFFAOYSA-N 0.000 description 4
- 238000010494 dissociation reaction Methods 0.000 description 4
- 230000005593 dissociations Effects 0.000 description 4
- 210000003205 muscle Anatomy 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- 239000011780 sodium chloride Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 3
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 3
- 239000004020 conductor Substances 0.000 description 3
- 229920006037 cross link polymer Polymers 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 230000003204 osmotic effect Effects 0.000 description 3
- -1 polyethylene acrylic acid Polymers 0.000 description 3
- 230000004044 response Effects 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- CPELXLSAUQHCOX-UHFFFAOYSA-M Bromide Chemical compound [Br-] CPELXLSAUQHCOX-UHFFFAOYSA-M 0.000 description 2
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- TWRXJAOTZQYOKJ-UHFFFAOYSA-L Magnesium chloride Chemical compound [Mg+2].[Cl-].[Cl-] TWRXJAOTZQYOKJ-UHFFFAOYSA-L 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- 229920002873 Polyethylenimine Polymers 0.000 description 2
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- VSCWAEJMTAWNJL-UHFFFAOYSA-K aluminium trichloride Chemical compound Cl[Al](Cl)Cl VSCWAEJMTAWNJL-UHFFFAOYSA-K 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 238000006073 displacement reaction Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- ZIUHHBKFKCYYJD-UHFFFAOYSA-N n,n'-methylenebisacrylamide Chemical compound C=CC(=O)NCNC(=O)C=C ZIUHHBKFKCYYJD-UHFFFAOYSA-N 0.000 description 2
- 229920003023 plastic Polymers 0.000 description 2
- 239000004033 plastic Substances 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 229920002401 polyacrylamide Polymers 0.000 description 2
- BWHMMNNQKKPAPP-UHFFFAOYSA-L potassium carbonate Chemical compound [K+].[K+].[O-]C([O-])=O BWHMMNNQKKPAPP-UHFFFAOYSA-L 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- 239000001124 (E)-prop-1-ene-1,2,3-tricarboxylic acid Substances 0.000 description 1
- WJTWUYGNXWHIAP-UHFFFAOYSA-N 1-butylsulfanylbutane;hydrochloride Chemical compound Cl.CCCCSCCCC WJTWUYGNXWHIAP-UHFFFAOYSA-N 0.000 description 1
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 1
- KFDVPJUYSDEJTH-UHFFFAOYSA-N 4-ethenylpyridine Chemical compound C=CC1=CC=NC=C1 KFDVPJUYSDEJTH-UHFFFAOYSA-N 0.000 description 1
- DEXFNLNNUZKHNO-UHFFFAOYSA-N 6-[3-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperidin-1-yl]-3-oxopropyl]-3H-1,3-benzoxazol-2-one Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C1CCN(CC1)C(CCC1=CC2=C(NC(O2)=O)C=C1)=O DEXFNLNNUZKHNO-UHFFFAOYSA-N 0.000 description 1
- HRPVXLWXLXDGHG-UHFFFAOYSA-N Acrylamide Chemical compound NC(=O)C=C HRPVXLWXLXDGHG-UHFFFAOYSA-N 0.000 description 1
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonium chloride Substances [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 1
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 1
- LSNNMFCWUKXFEE-UHFFFAOYSA-M Bisulfite Chemical compound OS([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-M 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- CNCOEDDPFOAUMB-UHFFFAOYSA-N N-Methylolacrylamide Chemical compound OCNC(=O)C=C CNCOEDDPFOAUMB-UHFFFAOYSA-N 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 229920002845 Poly(methacrylic acid) Polymers 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- 239000004793 Polystyrene Substances 0.000 description 1
- OFOBLEOULBTSOW-UHFFFAOYSA-N Propanedioic acid Natural products OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 description 1
- VMHLLURERBWHNL-UHFFFAOYSA-M Sodium acetate Chemical compound [Na+].CC([O-])=O VMHLLURERBWHNL-UHFFFAOYSA-M 0.000 description 1
- 229920002125 Sokalan® Polymers 0.000 description 1
- 239000004809 Teflon Substances 0.000 description 1
- 229920006362 Teflon® Polymers 0.000 description 1
- BZHJMEDXRYGGRV-UHFFFAOYSA-N Vinyl chloride Chemical compound ClC=C BZHJMEDXRYGGRV-UHFFFAOYSA-N 0.000 description 1
- 229940091181 aconitic acid Drugs 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- 235000019270 ammonium chloride Nutrition 0.000 description 1
- 239000000908 ammonium hydroxide Substances 0.000 description 1
- 125000000129 anionic group Chemical group 0.000 description 1
- KCXMKQUNVWSEMD-UHFFFAOYSA-N benzyl chloride Chemical compound ClCC1=CC=CC=C1 KCXMKQUNVWSEMD-UHFFFAOYSA-N 0.000 description 1
- 229940073608 benzyl chloride Drugs 0.000 description 1
- 229910000019 calcium carbonate Inorganic materials 0.000 description 1
- 125000002091 cationic group Chemical group 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000008602 contraction Effects 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 238000004132 cross linking Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 230000005489 elastic deformation Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 230000009477 glass transition Effects 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 238000007654 immersion Methods 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 230000002427 irreversible effect Effects 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 229910001629 magnesium chloride Inorganic materials 0.000 description 1
- VZCYOOQTPOCHFL-UPHRSURJSA-N maleic acid Chemical compound OC(=O)\C=C/C(O)=O VZCYOOQTPOCHFL-UPHRSURJSA-N 0.000 description 1
- 239000011976 maleic acid Substances 0.000 description 1
- 239000012567 medical material Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 239000012046 mixed solvent Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 125000004433 nitrogen atom Chemical group N* 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 239000003973 paint Substances 0.000 description 1
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 1
- 239000004584 polyacrylic acid Substances 0.000 description 1
- 229920000120 polyethyl acrylate Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 229920001444 polymaleic acid Polymers 0.000 description 1
- 239000004926 polymethyl methacrylate Substances 0.000 description 1
- 229920002223 polystyrene Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 229920000036 polyvinylpyrrolidone Polymers 0.000 description 1
- 239000001267 polyvinylpyrrolidone Substances 0.000 description 1
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 description 1
- 229910000027 potassium carbonate Inorganic materials 0.000 description 1
- OTYBMLCTZGSZBG-UHFFFAOYSA-L potassium sulfate Chemical compound [K+].[K+].[O-]S([O-])(=O)=O OTYBMLCTZGSZBG-UHFFFAOYSA-L 0.000 description 1
- 229910052939 potassium sulfate Inorganic materials 0.000 description 1
- 235000011151 potassium sulphates Nutrition 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 230000004043 responsiveness Effects 0.000 description 1
- 238000002791 soaking Methods 0.000 description 1
- 239000001632 sodium acetate Substances 0.000 description 1
- 235000017281 sodium acetate Nutrition 0.000 description 1
- MNCGMVDMOKPCSQ-UHFFFAOYSA-M sodium;2-phenylethenesulfonate Chemical group [Na+].[O-]S(=O)(=O)C=CC1=CC=CC=C1 MNCGMVDMOKPCSQ-UHFFFAOYSA-M 0.000 description 1
- XFTALRAZSCGSKN-UHFFFAOYSA-M sodium;4-ethenylbenzenesulfonate Chemical compound [Na+].[O-]S(=O)(=O)C1=CC=C(C=C)C=C1 XFTALRAZSCGSKN-UHFFFAOYSA-M 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- VZCYOOQTPOCHFL-UHFFFAOYSA-N trans-butenedioic acid Natural products OC(=O)C=CC(O)=O VZCYOOQTPOCHFL-UHFFFAOYSA-N 0.000 description 1
Description
【発明の詳細な説明】
〔産業上の利用分野〕
本発明は、電気的エネルギーによつて、高分子
材料を曲折させる方法に関するものであり、スイ
ツチ素子、人工筋肉等へ応用することができるも
のである。[Detailed Description of the Invention] [Industrial Application Field] The present invention relates to a method of bending a polymer material using electrical energy, and can be applied to switch elements, artificial muscles, etc. It is.
近年、熱、光、電気等のエネルギーを機械的エ
ネルギーに変換する機能を有する高分子材料を用
いて、スイツチ、ケミカルエンジン、人工筋肉、
ロボツトの触手などに応用しようとする試みがな
されている。かかる機能を起させるためには、そ
の機械的運動が可逆的な伸縮．曲折であり、また
迅速で、充分に大きいことが必要である。
In recent years, switches, chemical engines, artificial muscles,
Attempts are being made to apply it to robot tentacles, etc. In order to cause such a function, the mechanical movement must be reversible expansion and contraction. It needs to be tortuous, fast, and large enough.
従来、上記運動を生じせしめる方法として、熱
あるいは応力によるものがある。しかし、熱によ
る場合、上記高分子材料はガラス転移点付近の温
度で使用するため、高分子材料の寸法安定性に欠
け、更に熱履歴の問題も生じてしまう。また、応
力による場合、弾性変形内ではその変形は可逆的
であるが、塑性変形の領域になると、不可逆的と
なり、疲労やクリープが生じ、前記のスイツチ等
の用途に応用することは困難である。 Conventionally, methods for producing the above-mentioned motion include using heat or stress. However, in the case of heating, the polymeric material is used at a temperature near the glass transition point, so the polymeric material lacks dimensional stability and furthermore, problems with thermal history occur. In addition, in the case of stress, the deformation is reversible within the elastic deformation range, but becomes irreversible when it reaches the plastic deformation range, causing fatigue and creep, making it difficult to apply it to applications such as the above-mentioned switches. .
また、最近、電場によつて高分子材料に機械的
運動を起こさせることが考えられている。例えば
ポリフツ化ビニリデンに代表される圧電樹脂を用
いるもの、あるいは、ポリアクリルアミドゲル等
の高分子化合物に電場をかけて、その体積変化の
利用により、機械的運動を起こそうとする試みが
なされている。しかし、これらの方法において
は、伸縮運動を生じせしめることはできるもの
の、曲折運動は、起こすことができない。特に、
スイツチ、人工筋肉等の種々の用途に高分子材料
を利用するためには、曲折運動が必要であり、電
場を用いる従来の方法では、曲折運動は得られ
ず、実用化は困難である。 Also, recently, it has been considered to induce mechanical movement in polymeric materials using an electric field. For example, attempts have been made to generate mechanical motion by applying an electric field to a piezoelectric resin such as polyvinylidene fluoride, or by applying an electric field to a polymer compound such as polyacrylamide gel and utilizing the volume change. . However, in these methods, although it is possible to cause an elastic movement, a bending movement cannot be caused. especially,
In order to utilize polymeric materials for various applications such as switches and artificial muscles, bending motion is necessary, and conventional methods using electric fields cannot achieve bending motion and are difficult to put into practical use.
本発明は、従来の上記問題を解決して、電場を
用いて高分子材料に曲折運動を生じせしめる方法
を提供しようとしてなされたものである。
The present invention has been made in an attempt to solve the above-mentioned conventional problems and provide a method for causing bending motion in a polymeric material using an electric field.
本発明の高分子材料の曲折方法は、電解質溶液
中に浸漬した正電極及び負電極の間に、イオン性
の官能基を有する分子構造の高分子材料を前記電
解質溶液と膨潤平衡関係となるように配置すると
共に、前記正及び負の電極間に直流電圧を印加す
ることを特徴とするものである。
The method of bending a polymeric material of the present invention is such that a polymeric material having a molecular structure having an ionic functional group is placed between a positive electrode and a negative electrode immersed in an electrolyte solution so that the polymer material has a swelling equilibrium relationship with the electrolyte solution. The present invention is characterized in that the electrode is placed in the positive and negative electrodes, and a DC voltage is applied between the positive and negative electrodes.
本発明において、電解質溶液は、電気伝導体で
あるとともに、高分子材料を膨潤させて、高分子
材料を曲折させる媒体となるものである。膨潤平
衡関係とは、高分子材料が電解質溶液により膨潤
して、電解質溶液の浸透が平衡に達している状態
である。しかして、この膨潤平衡関係にするため
には、高分子材料を電解質溶液に浸漬して十分に
電解質溶液が膨潤し、イオン性の官能基のイオン
解離が平衡に達するようにする。 In the present invention, the electrolyte solution is an electrical conductor and serves as a medium that swells and bends the polymeric material. The swelling equilibrium relationship is a state in which the polymer material is swollen by the electrolyte solution and the permeation of the electrolyte solution has reached equilibrium. In order to achieve this swelling equilibrium relationship, the polymeric material is immersed in an electrolyte solution so that the electrolyte solution swells sufficiently and the ionic dissociation of the ionic functional groups reaches equilibrium.
該電解質溶液としては、塩酸、硫酸、リン酸、
水酸化カリウム、水酸化ナトリウム、水酸化アン
モニウム、塩化ナトリウム、臭化ナトリウム、炭
酸カリウム、硫酸カリウム、酢酸ナトリウム、炭
酸カルシウム、塩化マグネシウム、塩化アルミニ
ウム等の電解質物質を、水、またはメタノール、
エタノール、イソプロピルアルコール、エチレン
グリコール、アセトン等の少なくとも１種から成
る有機媒体と水との混合溶媒に溶解されたものが
ある。上記電解質物質は、溶媒に溶解して、電気
伝導体となるものであり、上記のうちの１種また
は２種以上で使用する。また、電解質物質の配合
量は、前記溶媒１中に10-5〜10-1モル含まれて
いることが望ましい。該配合量が、10-5モル未満
の場合には、溶液の電気伝導度が低くなり、曲折
運動の応答性がきわめて低いものとなる。他方、
10-1モルを越える場合には、電極において、イオ
ンが放電し、気体の発生、金属の析出等が生ずる
おそれがある。 The electrolyte solution includes hydrochloric acid, sulfuric acid, phosphoric acid,
Electrolyte substances such as potassium hydroxide, sodium hydroxide, ammonium hydroxide, sodium chloride, sodium bromide, potassium carbonate, potassium sulfate, sodium acetate, calcium carbonate, magnesium chloride, and aluminum chloride are mixed with water, methanol,
Some are dissolved in a mixed solvent of water and an organic medium consisting of at least one of ethanol, isopropyl alcohol, ethylene glycol, and acetone. The electrolyte substance becomes an electrical conductor when dissolved in a solvent, and is used in one or more of the above types. Further, it is desirable that the amount of the electrolyte substance contained in the solvent 1 is 10 -5 to 10 -1 mol. If the amount is less than 10 -5 mol, the electrical conductivity of the solution will be low and the response to bending motion will be extremely low. On the other hand,
If the amount exceeds 10 -1 mol, ions may discharge at the electrode, causing gas generation, metal precipitation, etc.
上記電極としては、電解質溶液中に浸漬しても
酸化溶解を起こさない導電体であり、例えば、白
金、金、ニツケル、マグネシウム、鉄、ステンレ
ススチール、黒鉛、カーボン、カーボン複合材等
を用いる。該電極の形状としては、板状、網状、
メツキ膜状、蒸着膜状ものを用いるものが望まし
い。 The electrode is a conductor that does not undergo oxidative dissolution even when immersed in an electrolyte solution, such as platinum, gold, nickel, magnesium, iron, stainless steel, graphite, carbon, carbon composite material, and the like. The shape of the electrode is plate-like, mesh-like,
It is preferable to use a plated film or a vapor deposited film.
次に、本発明において用いる高分子材料は、イ
オン性の官能基を有する分子構造であることが必
要である。該高分子材料は、電解質溶液中に浸漬
され、膨潤すると、このイオン性の官能基がイオ
ン解離して、溶液と平衡関係になる。この平衡関
係は、電場の印加によりずれ、高分子材料中に浸
透圧差が生じて、高分子材料が曲折させられると
考えられる。 Next, the polymer material used in the present invention needs to have a molecular structure having an ionic functional group. When the polymer material is immersed in an electrolyte solution and swells, the ionic functional groups are ionically dissociated and come into equilibrium with the solution. It is thought that this equilibrium relationship is shifted by the application of an electric field, causing an osmotic pressure difference in the polymer material, causing the polymer material to bend.
上記イオン性の官能基を有する分子構造の高分
子としては、ポリアクリル酸、ポリメタクリル
酸、ポリエチレンアクリル酸、ポリマレイン酸、
ポリフマル酸、ポリイタコン酸、ポリ−ｔ−アコ
ニツト酸、ポリエチレンスルホン酸、ポリ−ｐ−
スチレンスルホン酸ナトリウム等の、カルボキシ
ル基またはスルホン基のアニオン性の官能基を有
する架橋高分子、ポリ−２−ビニル−Ｎ−オクチ
ルピリジウムブロミド、ポリ−４−ビニル−Ｎ−
ベンジルピリジウムクロリド、ポリ−４−ビニル
−Ｎ−エチルピリジウムクロリド、ラウリル化ポ
リエチレンイミン、ステアリル化ポリエチレンイ
ミン、ポリ−ｐ−スチレンジブチルスルホニウム
クロリド、ポリ−ｐ−スチレンエチルメチルスル
ホニウムブロミド等の、アンモニウム基またはス
ルホニウム基のカチオン性の官能基を有する架橋
高分子、あるいは上記架橋高分子とポリアクリル
アミド、ポリ−Ｎ−メチロールアクリルアミド、
ポリメタクリル酸メチル、ポリアクリル酸エチ
ル、ポリビニルピロリドン、ポリスチレン等との
共重合体等がある。 Examples of polymers with molecular structures having ionic functional groups include polyacrylic acid, polymethacrylic acid, polyethylene acrylic acid, polymaleic acid,
Polyfumaric acid, polyitaconic acid, poly-t-aconitic acid, polyethylene sulfonic acid, poly-p-
Crosslinked polymers having anionic functional groups such as carboxyl or sulfonic groups such as sodium styrene sulfonate, poly-2-vinyl-N-octylpyridium bromide, poly-4-vinyl-N-
Ammonium chloride, such as benzylpyridium chloride, poly-4-vinyl-N-ethylpyridium chloride, laurated polyethyleneimine, stearylated polyethyleneimine, poly-p-styrene dibutylsulfonium chloride, poly-p-styreneethylmethylsulfonium bromide, etc. or a crosslinked polymer having a cationic functional group such as a group or a sulfonium group, or the above crosslinked polymer and polyacrylamide, poly-N-methylolacrylamide,
Examples include copolymers with polymethyl methacrylate, polyethyl acrylate, polyvinylpyrrolidone, and polystyrene.
また、該高分子材料の形状としては、角柱状、
板状、球状等、特に限定はしないが、種々の用途
に応用するためには、第２図に示すように幅Ｄ、
長さＬの棒状でその長さ方向と電極とが平行にな
るようにした場合に、幅に対する長さの比Ｌ／Ｄ
が５以上の高分子材料を使用するのが望ましい。 In addition, the shape of the polymer material may be prismatic,
Although not particularly limited to plate-shaped, spherical, etc., in order to apply it to various uses, width D, as shown in FIG.
When a rod of length L is made so that its length direction is parallel to the electrode, the ratio of length to width L/D
It is desirable to use a polymeric material having a value of 5 or more.
高分子材料を膨潤させる方法としては、予め、
高分子材料を電解質溶液中に浸漬して膨潤せしめ
た後、正及び負の電極が浸漬されている上記と同
じ電解質溶液中に膨潤した高分子材料を浸漬して
もよく、また、最初から正及び負の電極が浸漬さ
れた電解質溶液中に高分子材料を浸漬して、膨潤
させてもよい。 As a method for swelling a polymer material, in advance,
After the polymeric material is immersed in an electrolyte solution to cause it to swell, the swollen polymeric material may be immersed in the same electrolyte solution as described above in which the positive and negative electrodes are immersed, or the swollen polymeric material may be immersed in the electrolyte solution from the beginning. The polymer material may also be swollen by being immersed in the electrolyte solution in which the negative electrode is immersed.
前記電解質溶液を容器等に導入し、該電解質溶
液中に正及び負の電極を浸漬し、更にその正及び
負の電極間に高分子材料を電解質溶液と膨潤平衡
関係になるように配置する。膨潤平衡関係に達し
ない状態で電圧を印加すると、可逆的な変化が得
られないおそれがある。なお、応答性向上の面か
ら、高分子材料を電解質溶液中に完全に浸漬した
状態に配置するのがよい。また、大きな曲折運動
を得るためには、高分子材料の長軸方向が電極と
平行となるように配置するのがよい。また、電極
間が狭い場合、高分子材料の側面が電極に接触す
ることがある。それ故、高分子材料の中央部近傍
をピン等で固定してもよい。 The electrolyte solution is introduced into a container or the like, positive and negative electrodes are immersed in the electrolyte solution, and a polymeric material is placed between the positive and negative electrodes so as to have a swelling equilibrium relationship with the electrolyte solution. If a voltage is applied in a state where the swelling equilibrium relationship has not been reached, there is a possibility that no reversible change will be obtained. In addition, from the viewpoint of improving responsiveness, it is preferable to arrange the polymer material in a state where it is completely immersed in the electrolyte solution. Further, in order to obtain a large bending motion, it is preferable to arrange the polymer material so that its long axis direction is parallel to the electrode. Furthermore, when the distance between the electrodes is narrow, the side surfaces of the polymer material may come into contact with the electrodes. Therefore, the vicinity of the center of the polymer material may be fixed with a pin or the like.
容器中に電解質溶液を導入する場合、該容器と
しては、電解質溶液に侵食されない物質で形成さ
れたものがよい。例えば、塩化ビニル等のプラス
チツク、ガラス、塗料で被覆された金属等が挙げ
られる。 When introducing the electrolyte solution into a container, the container is preferably made of a material that is not corroded by the electrolyte solution. Examples include plastics such as vinyl chloride, glass, and metals coated with paint.
このような状態に高分子材料を配置すると共
に、上記正及び負の電極の電極を直流電源により
接続し、直流電圧を印加する。 While placing the polymer material in such a state, the positive and negative electrodes are connected by a DC power source and a DC voltage is applied.
この直流電圧の印加により、高分子材料の解離
したイオンと電解質溶液中のイオンとが、正ある
いは負の電極に向かつて移動し、高分子材料の内
部に浸透圧差を発生させ、高分子材料を曲折させ
る。 By applying this DC voltage, the dissociated ions of the polymer material and the ions in the electrolyte solution move toward the positive or negative electrode, creating an osmotic pressure difference inside the polymer material, and causing the polymer material to bend.
その曲折は、例えば、棒状体の高分子材料を電
極と平行に配置する場合、その棒状体の両端が正
又は負の電極側へ同一方向に曲折する。曲折方向
は、高分子材料の種類、イオン性の官能基、電解
質溶液の種類またはその濃度により異なるが、そ
れらを制御することにより正電極側、負電極側ど
ちらへも変化する。 For example, when a rod-shaped polymer material is arranged parallel to an electrode, both ends of the rod-shaped body are bent in the same direction toward the positive or negative electrode. The bending direction varies depending on the type of polymer material, ionic functional group, type of electrolyte solution, or its concentration, but by controlling these, it can change to either the positive electrode side or the negative electrode side.
印加する電圧は10ボルト以上とするのが望まし
い。10ボルト未満の電圧を印加してもわずかに高
分子材料は曲折するものの、曲折運動、応答速度
が小さく、スイツチ素子等に実用化することはむ
ずかしい。また、印加電圧が大きいほど、曲折変
位量、応答速度は大きくなるが、非常に大きな電
圧の場合、高分子材料に変質等の悪影響を与える
こともあり、好ましくはその上限は1000ボルトと
するのがよい。 It is desirable that the applied voltage be 10 volts or more. Although the polymer material bends slightly when a voltage of less than 10 volts is applied, the bending motion and response speed are small, making it difficult to put it to practical use in switch elements and the like. Additionally, the larger the applied voltage, the greater the amount of bending displacement and response speed; however, in the case of a very large voltage, it may have an adverse effect such as deterioration of the polymer material, so the upper limit should preferably be 1000 volts. Good.
上記のように、電圧を印加して、高分子材料を
曲折させた後、電圧の印加を停止すると、高分子
材料は元の状態に戻りうる。すなわち、可逆性が
ある。なお、電極の正・負を逆にすることによ
り、より速く元の状態に戻ることができる。 As described above, after applying a voltage to cause the polymeric material to bend, the polymeric material may return to its original state when the voltage application is stopped. That is, it is reversible. Note that by reversing the positive and negative electrodes, the original state can be returned to the original state more quickly.
本発明によれば、電圧の印加により、イオン性
の官能基を有する分子構造の高分子材料を迅速か
つ大きく曲折させることができる。しかもその曲
折運動は可逆的である。
According to the present invention, a polymeric material having a molecular structure having an ionic functional group can be quickly and largely bent by applying a voltage. Moreover, the bending motion is reversible.
このような曲折運動が得られるのは、次のよう
な現象が生じているためであると考えられる。 The reason why such a bending motion is obtained is considered to be due to the occurrence of the following phenomenon.
すなわち、高分子材料が電解質溶液中で膨潤す
ることにより、該高分子中のイオン性の官能基が
イオン解離を行ない、電解質溶液中で解離平衡に
達する。この状態で電圧が印加されると、電解質
溶液中の高分子の解離イオン及び電解質イオンと
が電極に向かつて移動される。 That is, when the polymer material swells in the electrolyte solution, the ionic functional groups in the polymer undergo ionic dissociation and reach a dissociation equilibrium in the electrolyte solution. When a voltage is applied in this state, the dissociated ions of the polymer and the electrolyte ions in the electrolyte solution are moved toward the electrode.
上記の移動するイオンの速度差により高分子材
料の正極側と負極側とで浸透圧差ができ、電極の
法線方向へ曲折すると考えられる。 It is thought that the difference in speed of the moving ions creates a difference in osmotic pressure between the positive and negative electrode sides of the polymer material, causing the ions to bend in the normal direction of the electrode.
また、電圧の印加を停止、あるいは正・負極を
逆にすることにより、すみやかに高分子材料は元
の状態に戻り、あるいは更に逆の方向へその両端
が曲折することができる。 Furthermore, by stopping the application of voltage or reversing the positive and negative electrodes, the polymer material can quickly return to its original state, or both ends can be bent in the opposite direction.
本発明方法を利用して、高分子の種類、イオン
性の官能基の解離度、電解質の種類や濃度、及び
電圧の大きさによつて制御することにより、高分
子材料をスイツチ素子、人工筋肉などの医用材
料、ロボツトの触手等へ実用化することが可能で
ある。 By using the method of the present invention and controlling the type of polymer, the degree of dissociation of ionic functional groups, the type and concentration of electrolyte, and the magnitude of voltage, polymer materials can be used to create switch elements and artificial muscles. It can be put to practical use in medical materials such as robot tentacles, etc.
以下、本発明の実施例を説明する。 Examples of the present invention will be described below.
実施例 １
第１図に本実施例を概略的に説明する図を示
す。Example 1 FIG. 1 shows a diagram schematically explaining this example.
マレイン酸0.30モルをメチレンビスアクリルア
ミド0.01モルで架橋した高分子材料５ｇを電解質
溶液としての0.04規定水酸化カリウム（KOH）
水溶液500ml中に24時間浸漬して、該高分子材料
を膨潤せしめた。該膨潤した高分子材料を大きさ
５×５×50mmの直線状角柱に切り出した。次に、
テフロンから成る容器１に電解質溶液２としての
上記KOH水溶液10mlを満たし、該KOH水溶液に
表面を絶縁被覆した白金から成る正電極板３及び
負電極板３′を電極間距離３cmで対向するように
浸漬し、更に前記角柱の高分子材料４を上記正・
負電極板３，３′の間に浸漬した。この場合、
正・負電極板３，３′の中央部に両電極板と平行
に高分子材料４を配置し、また、この高分子材料
４の中心部をピン５で固定し、高分子材料が完全
に浸漬するようにした。 0.04 N potassium hydroxide (KOH) as an electrolyte solution containing 5 g of a polymer material in which 0.30 mol of maleic acid is cross-linked with 0.01 mol of methylenebisacrylamide.
The polymer material was swollen by immersion in 500 ml of an aqueous solution for 24 hours. The swollen polymer material was cut into a rectilinear prism with a size of 5 x 5 x 50 mm. next,
A container 1 made of Teflon was filled with 10 ml of the above KOH aqueous solution as an electrolyte solution 2, and a positive electrode plate 3 and a negative electrode plate 3' made of platinum whose surfaces were coated with insulation were placed in the KOH aqueous solution so that they faced each other with a distance of 3 cm between the electrodes. The prismatic polymer material 4 is immersed in the prismatic polymer material 4.
It was immersed between the negative electrode plates 3 and 3'. in this case,
A polymer material 4 is placed in the center of the positive and negative electrode plates 3, 3' in parallel with both electrode plates, and the center of this polymer material 4 is fixed with a pin 5 to ensure that the polymer material is completely covered. I decided to soak it.
次に、正・負電極を直流電圧源６により接続
し、30ボルトの直流電圧を４分間印加した。その
結果、第３図に示すように、高分子材料４は、そ
の両端４１，４２が負極側へ曲折した。その変位
量Ａは、10mmであつた。その後、直流電圧の印加
を停止したところ、高分子材料の両端は元の状態
に向つて移動し、約10分後元の直線状角柱に回復
した。 Next, the positive and negative electrodes were connected by a DC voltage source 6, and a DC voltage of 30 volts was applied for 4 minutes. As a result, as shown in FIG. 3, both ends 41 and 42 of the polymer material 4 were bent toward the negative electrode side. The amount of displacement A was 10 mm. Thereafter, when the application of the DC voltage was stopped, both ends of the polymer material moved toward their original state, and after about 10 minutes, they recovered to their original straight prismatic shape.
実施例 ２
アクリル酸0.1モルとアクリルアミド0.2モルを
メチレンビスアクリルアミド0.01モルで架橋した
高分子材料５ｇを電解質溶液としての0.01規定の
水酸化ナトリウム（NaOH）水溶液500ml中に20
時間浸漬して、該高分子材料を膨潤平衡状態に達
しめた。電解質溶液として0.01規定のNaOH水溶
液を使用した以外は、実施例１と同様にして、上
記高分子材料を配置し、これに30ボルトの直流電
圧を３分間印加した。Example 2 5 g of a polymeric material in which 0.1 mol of acrylic acid and 0.2 mol of acrylamide were cross-linked with 0.01 mol of methylenebisacrylamide was added to 500 ml of a 0.01 N sodium hydroxide (NaOH) aqueous solution as an electrolyte solution.
The polymeric material was allowed to reach swelling equilibrium by soaking for a period of time. The above polymer material was placed in the same manner as in Example 1, except that a 0.01N NaOH aqueous solution was used as the electrolyte solution, and a DC voltage of 30 volts was applied thereto for 3 minutes.
その結果、高分子材料は、その両端は正極側へ
14mm曲折した。その後、直流電圧の印加を停止す
ると、高分子材料の両端は元の状態に向つて移動
し、約11分後元の直線状角柱に回復した。 As a result, both ends of the polymer material move toward the positive electrode.
Bent 14mm. After that, when the application of the DC voltage was stopped, both ends of the polymer material moved toward their original state, and after about 11 minutes, they recovered to their original straight prismatic shape.
実施例 ３
電解質溶液として0.05規定のNaOH水溶液を用
いた以外は、実施例２と同様な高分子材料、条件
で、該高分子材料を配置し、これに60ボルトの直
流電圧を２分間印加した。Example 3 Except for using a 0.05N NaOH aqueous solution as the electrolyte solution, the polymer material was placed under the same conditions as in Example 2, and a DC voltage of 60 volts was applied for 2 minutes. .
その結果、高分子材料は、その両端が負極側へ
18mm曲折した。その後、直流電圧の印加を停止す
ると、高分子材料の両端は元の状態に向つて移動
し、約９分後元の直線状角柱に回復した。 As a result, both ends of the polymer material move toward the negative electrode.
Bent 18mm. Thereafter, when the application of the DC voltage was stopped, both ends of the polymer material moved toward their original state, and after about 9 minutes, they recovered to their original straight prismatic shape.
実施例 ４
ｐ−スチレンスルホン酸ナトリウム0.1モルと
スチレン0.2モルをジビニルベンゼン0.01モルで
架橋した高分子材料５ｇを電解質溶液としての
0.02規定の塩化ナトリウム（NaCl）水溶液500ml
中に24時間浸漬し、該高分子材料を膨潤平衡状態
に達しめた。電解質溶液として0.02規定のNaCl
水溶液を使用した以外は、実施例１と同様にし
て、上記高分子材料を配置し、これに30ボルトの
直流電圧を30秒印加した。Example 4 5 g of a polymeric material obtained by crosslinking 0.1 mol of sodium p-styrene sulfonate and 0.2 mol of styrene with 0.01 mol of divinylbenzene was used as an electrolyte solution.
500ml of 0.02N sodium chloride (NaCl) aqueous solution
for 24 hours to allow the polymeric material to reach a swelling equilibrium state. 0.02N NaCl as electrolyte solution
The above polymer material was placed in the same manner as in Example 1 except that an aqueous solution was used, and a DC voltage of 30 volts was applied thereto for 30 seconds.
その結果、高分子材料は、その両端が負極側へ
15mm曲折した。その後、直流電圧を−30ボルトに
すると、高分子材料の両端は元の状態に向つて移
動し、30秒後元の直線状角柱に回復した。 As a result, both ends of the polymer material move toward the negative electrode.
Bent by 15mm. Then, when the DC voltage was set to -30 volts, both ends of the polymer material moved toward their original state, and after 30 seconds, they recovered to their original straight prismatic shape.
実施例 ５
４−ビニルピリジン0.3モルをジビニルベンゼ
ン0.01モルで架橋し、その後、塩化ベンジルで窒
素原子を４級化して、アンモニウムイオンを導入
した高分子材料５ｇを、電解質溶液としての臭化
ナトリウム（NaBr）を0.01モル／溶解させた
水・メタノール混合溶液（水80％、メタノール20
％）500ml中に24時間浸漬し、該高分子材料を膨
潤平衡状態に達しめた。電解質溶液として上記
NaBr溶液を使用した以外は、実施例１と同様に
して、上記高分子材料を配置し、これに90ボルト
の直流電圧を１分間印加した。Example 5 0.3 mol of 4-vinylpyridine was cross-linked with 0.01 mol of divinylbenzene, and then 5 g of a polymer material into which ammonium ions were introduced by quaternizing nitrogen atoms with benzyl chloride was added to sodium bromide (as an electrolyte solution). A mixed solution of water and methanol (80% water, 20% methanol) dissolved in 0.01 mol/NaBr)
%) for 24 hours to reach a swelling equilibrium state. Above as electrolyte solution
The above polymer material was placed in the same manner as in Example 1 except that the NaBr solution was used, and a DC voltage of 90 volts was applied thereto for 1 minute.
その結果、高分子材料は、その両端が正極側へ
12mm曲折した。その後、直流電圧を−90ボルトに
すると高分子材料の両端は元の状態に向つて移動
し、１分後元の直線状角柱に回復した。 As a result, both ends of the polymer material are directed toward the positive electrode.
Bent by 12mm. Thereafter, when the DC voltage was set to -90 volts, both ends of the polymer material moved toward their original state, and after 1 minute, they recovered to their original straight prismatic shape.
第１図は、本実施例の概略説明図、第２図は本
発明に使用する棒状の高分子材料を示す斜視図、
第３図は本実施例による高分子材料の曲折運動を
示す図である。
１：容器、２：電解質溶液、３：正電極板、
３′：負電極板、４：高分子材料、５：ピン、
６：直流電圧源。
FIG. 1 is a schematic explanatory diagram of this embodiment, and FIG. 2 is a perspective view showing a rod-shaped polymer material used in the present invention.
FIG. 3 is a diagram showing the bending motion of the polymer material according to this example. 1: container, 2: electrolyte solution, 3: positive electrode plate,
3': negative electrode plate, 4: polymer material, 5: pin,
6: DC voltage source.
Claims (1)
間に、イオン性の官能基を有する分子構造の高分
子材料を前記電解質溶液と膨潤平衡関係になるよ
うに配置すると共に、前記正及び負の電極間に直
流電圧を印加することを特徴とする高分子材料の
曲折方法。 ２ 上記イオン性の官能基は、カルボキシル基、
スルホン基、アンモニウム基、スルホニウム基で
ある特許請求の範囲第１項記載の高分子材料の曲
折方法。 ３ 上記直流電圧は、10ボルト以上である特許請
求の範囲第１項記載の高分子材料の曲折方法。[Claims] 1. A polymeric material having a molecular structure having an ionic functional group is arranged between a positive electrode and a negative electrode immersed in an electrolyte solution so as to have a swelling equilibrium relationship with the electrolyte solution, and . A method for bending a polymeric material, characterized in that a DC voltage is applied between the positive and negative electrodes. 2 The ionic functional group is a carboxyl group,
The method for bending a polymeric material according to claim 1, wherein the bending method is a sulfone group, an ammonium group, or a sulfonium group. 3. The method of bending a polymeric material according to claim 1, wherein the DC voltage is 10 volts or more.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP12416384A JPS614731A (en) | 1984-06-16 | 1984-06-16 | Bending of polymeric material |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP12416384A JPS614731A (en) | 1984-06-16 | 1984-06-16 | Bending of polymeric material |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS614731A JPS614731A (en) | 1986-01-10 |
| JPH0218688B2 true JPH0218688B2 (en) | 1990-04-26 |
Family
ID=14878500
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP12416384A Granted JPS614731A (en) | 1984-06-16 | 1984-06-16 | Bending of polymeric material |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS614731A (en) |
Families Citing this family (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS63106245A (en) * | 1986-10-22 | 1988-05-11 | Fuji Photo Film Co Ltd | Autofeeder for photosensitive plate |
| JPH0641530B2 (en) * | 1989-09-02 | 1994-06-01 | 株式会社豊田中央研究所 | Material with variable elastic modulus |
| DE59209254D1 (en) * | 1992-01-30 | 1998-04-30 | Ferag Ag | Method and device for lifting printed matter from a stack |
| WO1994017538A2 (en) * | 1993-01-21 | 1994-08-04 | Mayo Foundation For Medical Education And Research | Microparticle switching devices |
-
1984
- 1984-06-16 JP JP12416384A patent/JPS614731A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS614731A (en) | 1986-01-10 |
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