JPH0195470A - Solid polyelectrolyte - Google Patents
Solid polyelectrolyteInfo
- Publication number
- JPH0195470A JPH0195470A JP62251141A JP25114187A JPH0195470A JP H0195470 A JPH0195470 A JP H0195470A JP 62251141 A JP62251141 A JP 62251141A JP 25114187 A JP25114187 A JP 25114187A JP H0195470 A JPH0195470 A JP H0195470A
- Authority
- JP
- Japan
- Prior art keywords
- salt
- polymer
- dielectric constant
- high dielectric
- constant solvent
- 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.)
- Granted
Links
- 239000007787 solid Substances 0.000 title claims abstract description 8
- 229920000867 polyelectrolyte Polymers 0.000 title abstract 3
- 229920000642 polymer Polymers 0.000 claims abstract description 14
- 239000007784 solid electrolyte Substances 0.000 claims abstract description 12
- 150000003839 salts Chemical class 0.000 claims abstract description 11
- 239000002904 solvent Substances 0.000 claims abstract description 9
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 6
- 150000003242 quaternary ammonium salts Chemical class 0.000 claims abstract description 6
- 229920006125 amorphous polymer Polymers 0.000 claims abstract description 3
- 239000002184 metal Substances 0.000 claims abstract 2
- CYSGHNMQYZDMIA-UHFFFAOYSA-N 1,3-Dimethyl-2-imidazolidinon Chemical group CN1CCN(C)C1=O CYSGHNMQYZDMIA-UHFFFAOYSA-N 0.000 claims description 5
- 239000005518 polymer electrolyte Substances 0.000 claims description 4
- 150000001875 compounds Chemical class 0.000 claims description 3
- YBRBMKDOPFTVDT-UHFFFAOYSA-N tert-butylamine Chemical group CC(C)(C)N YBRBMKDOPFTVDT-UHFFFAOYSA-N 0.000 claims description 3
- 230000000717 retained effect Effects 0.000 claims description 2
- 150000002500 ions Chemical class 0.000 abstract description 7
- 229920003171 Poly (ethylene oxide) Polymers 0.000 abstract description 5
- 238000002425 crystallisation Methods 0.000 abstract description 5
- 230000008025 crystallization Effects 0.000 abstract description 5
- 239000000126 substance Substances 0.000 abstract 2
- 150000003863 ammonium salts Chemical class 0.000 abstract 1
- 238000010276 construction Methods 0.000 abstract 1
- 239000010408 film Substances 0.000 description 4
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 3
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 2
- 239000004593 Epoxy Substances 0.000 description 2
- 239000004698 Polyethylene Substances 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 239000011261 inert gas Substances 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 239000005057 Hexamethylene diisocyanate Substances 0.000 description 1
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- GOOHAUXETOMSMM-UHFFFAOYSA-N Propylene oxide Chemical compound CC1CO1 GOOHAUXETOMSMM-UHFFFAOYSA-N 0.000 description 1
- 230000001588 bifunctional effect Effects 0.000 description 1
- ICXXXLGATNSZAV-UHFFFAOYSA-N butylazanium;chloride Chemical compound [Cl-].CCCC[NH3+] ICXXXLGATNSZAV-UHFFFAOYSA-N 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 229920003020 cross-linked polyethylene Polymers 0.000 description 1
- 239000004703 cross-linked polyethylene Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- GYZLOYUZLJXAJU-UHFFFAOYSA-N diglycidyl ether Chemical compound C1OC1COCC1CO1 GYZLOYUZLJXAJU-UHFFFAOYSA-N 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- RRAMGCGOFNQTLD-UHFFFAOYSA-N hexamethylene diisocyanate Chemical compound O=C=NCCCCCCN=C=O RRAMGCGOFNQTLD-UHFFFAOYSA-N 0.000 description 1
- DLDIDQIZPBIVNQ-UHFFFAOYSA-N hydron;2-methylpropan-2-amine;chloride Chemical compound Cl.CC(C)(C)N DLDIDQIZPBIVNQ-UHFFFAOYSA-N 0.000 description 1
- 229910052744 lithium Inorganic materials 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- -1 polyethylene Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 238000001291 vacuum drying Methods 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- Dispersion Chemistry (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Compositions Of Macromolecular Compounds (AREA)
- Polyurethanes Or Polyureas (AREA)
- Secondary Cells (AREA)
Abstract
Description
【発明の詳細な説明】
産業上の利用分野
本発明は、全面体形二次電池の電解質に関するもので、
特に高分子固体電解質の改良に関するものである。[Detailed Description of the Invention] Industrial Application Field The present invention relates to an electrolyte for a full-body secondary battery.
In particular, it relates to improvements in solid polymer electrolytes.
従来技術とその問題点
リチウムのイオン導電性固体電解質として−ＬｉＯＩ０
４等のＬ１堆を溶解させたポリエチレンオキシド（ＰＥ
Ｏ）に代表される高分子固体電解質がある。このものは
薄膜への加工が容易である二と、強度が大でしかも柔軟
性があること等の長所を有する。Prior art and its problems As an ion conductive solid electrolyte for lithium - LiOI0
Polyethylene oxide (PE
There are polymer solid electrolytes represented by O). This material has the advantages of being easy to process into a thin film, and having high strength and flexibility.
しかしながら、従来のＰＥＯにおいては、直鎖形（二官
能）を用いてＬ１塩を溶解させる段階でＰＥＯの結晶化
が起こり、イオンの移動度が低下する。このために、高
い導電率が得られないという欠点があった。However, in conventional PEO, crystallization of PEO occurs at the stage of dissolving the L1 salt using a linear form (bifunctional), resulting in a decrease in ion mobility. For this reason, there was a drawback that high conductivity could not be obtained.
この改良として、三官能性ボリエーテｐをインシアナー
ト化合物等で架橋した三次元架橋体が提案されている。As an improvement on this, a three-dimensionally crosslinked product in which trifunctional polyate p is crosslinked with an incyanate compound or the like has been proposed.
これは、ポリマーの結晶化が抑制されているために、従
来より高いイオン導電性が得られた。しかしながら、こ
れらのイオン導電性は室温で１０ ８ｍ であり、電
池が一般に使用される室温において、充分な性能が発揮
できないという欠点があった。This is because the crystallization of the polymer is suppressed, resulting in higher ionic conductivity than before. However, their ionic conductivity was 10 8 m at room temperature, and they had the drawback that they could not exhibit sufficient performance at room temperature, where batteries are generally used.
又、ポリ弗化ビニリデンやエポキシといつた高分子を支
持体とし、樵を溶解しているプロピレンカーボネートや
ポリエチレングリス−μといった高誘電率溶媒を支持体
中に物理的にとり込ませることにより、固体状態であり
ながら高いイオン伝導性を得ようとする相互侵入型高分
子網目が知られているが、これでも充分な性能が発揮で
きない程度のイオン伝導性であった。In addition, by using a polymer such as polyvinylidene fluoride or epoxy as a support and physically incorporating a high dielectric constant solvent such as propylene carbonate or polyethylene grease-μ in which wood is dissolved into the support, solid Although an interpenetrating polymer network is known that attempts to obtain high ion conductivity while remaining in the state, the ion conductivity was still at a level where sufficient performance could not be achieved.
発明の目的
本発明は上記従来の欠点に鑑みなされたものであり、イ
オン導電性の高い１高分子固体電解質を提供することを
目的とする。OBJECTS OF THE INVENTION The present invention was made in view of the above-mentioned conventional drawbacks, and an object of the present invention is to provide a monopolymer solid electrolyte with high ionic conductivity.
発明の構成
本発明は上記目的を達成するべく、無定形ポリマーを架
橋した高分子化合物に金ｊＩ塩を溶解した固体電解質に
おいて、架橋構造中に高誘電率溶媒とりわけ１．３−ジ
メチルイミダゾリジノンを共存していることを特徴とす
る高分子固体電解質である。SUMMARY OF THE INVENTION In order to achieve the above object, the present invention provides a solid electrolyte in which a gold jI salt is dissolved in a polymer compound crosslinked with an amorphous polymer, in which a high dielectric constant solvent, particularly 1,3-dimethylimidazolidinone, is added to the crosslinked structure. It is a polymer solid electrolyte characterized by the coexistence of
又、上記固体電解質中に四級アンモニウム塩を添加した
高分子固体電解質である・
又、上記四級アンモニウム塩がｔ−ブチルアン砥ニウム
塩である高分子固体電解質である・即ち、支持体自体が
高いイオン伝導性をもつ、ポリエチレンオキシド架橋体
−塊鎖体を用い、ジメチルイミダゾリジノンに代表され
る高誘電率溶媒を用いたものが極めて高いイオン伝導性
を与えることを見い出した。Also, it is a polymer solid electrolyte in which a quaternary ammonium salt is added to the solid electrolyte. Also, it is a polymer solid electrolyte in which the quaternary ammonium salt is t-butylammonium salt. In other words, the support itself is We have found that extremely high ionic conductivity can be achieved by using a polyethylene oxide cross-linked mass chain, which has high ionic conductivity, and a high dielectric constant solvent such as dimethylimidazolidinone.
しかし、これら高誘電率溶媒が保持されたポリエチレン
オキシド架橋体は、塩の溶解度が大かくなく、結晶化を
起こしやすい。このために、室°温付近においては、充
分なイオン伝導性が発揮されないばかりか、逆にイオン
伝導性を低下させるという問題があった。However, these crosslinked polyethylene oxides in which a high dielectric constant solvent is retained do not have a high solubility of salt, and are likely to crystallize. For this reason, there is a problem that not only sufficient ionic conductivity is not exhibited at around room temperature, but also the ionic conductivity is decreased.
この問題を解決する手段として、相間移動剤として四級
アンモニウム塩な添加することにより、塩の溶解度を上
げることができる。これにより塩の結晶化を防ぎ、室温
付近のイオン伝導度を上昇させることができることが判
った。As a means to solve this problem, the solubility of the salt can be increased by adding a quaternary ammonium salt as a phase transfer agent. It was found that this could prevent salt crystallization and increase ionic conductivity near room temperature.
四級アンモニウム塩の種類として、ｔ−ブチルアンモニ
ウム塩、セチ〃トリメチ〃アン壁ニウム塩等を挙げるこ
とが出来るが、これに限定されるものではない。Types of quaternary ammonium salts include t-butylammonium salts, cetitrimethyammonium salts, and the like, but are not limited thereto.
実施例 以下、本発明の詳細について実施例により説明する。Example Hereinafter, the details of the present invention will be explained with reference to Examples.
実施例１
９ｗｔ％の過塩素酸リチウム及び１ｗｔ％の１−ブチル
アン屹ニウムクロリドを溶解させたトリ＃−＊型Ｅ官ａ
性ボｙ ｘ −Ｔ ＩＶ （分子ｆｆ１３．ｏｏｏ）５
部を準備し、次に予め７ｖｔ％の過塩素酸リチウム及び
０．５ｖｔ％のｔ−グチルアンモニウムクロリドを溶解
させた１、３−ジメチルイミダゾリジノン１部を調製し
、加える。Example 1 Tri#-*Type E-type a in which 9wt% lithium perchlorate and 1wt% 1-butylampanium chloride were dissolved
sex boy x -T IV (molecule ff13.ooo)5
Next, prepare and add 1 part of 1,3-dimethylimidazolidinone in which 7 vt% lithium perchlorate and 0.5 vt% t-glylammonium chloride are dissolved in advance.
当ｔのへキサメチレンジイソシアナート及び微量のＤｉ
−ｎ−ブチ／Ｉ／銅がアセテートを加え、充分混合した
後ガラスシャーレ上に流延し、８０℃の不活性ガス雰囲
気で放置し、反応させて架橋体フィルムを得る。Hexamethylene diisocyanate and a trace amount of Di
-N-buty/I/copper is added with acetate, thoroughly mixed, and then cast onto a glass petri dish, left to stand in an inert gas atmosphere at 80°C, and reacted to obtain a crosslinked film.
このフィルムを真空乾燥した後、ペレット状に打抜き白
金板ではさみ、交流インピーダンス法によりイオン伝導
度を測定した０その結果を第１図の本発明１として示し
た。After drying this film in vacuum, it was sandwiched between punched platinum plates in the form of pellets, and the ionic conductivity was measured by an alternating current impedance method.The results are shown as Invention 1 in FIG.
１．３−ジメチルイミダゾリジノン及びｔ−ブチルアン
叱ニウムクロリドを添加しない系を従来品とした。A conventional product was a system in which 1.3-dimethylimidazolidinone and t-butylaminium chloride were not added.
実施例２
予め７ｖｔ％の過塩素酸リチウム及びｏ、ｓｖｔ％のｔ
−ブチルアン叱ニウムクロリドを溶解させた１、３−ジ
メチルイミダゾリジノン１部にエポキシとしてビスフェ
ノ−〃ムーデロビレンオキシド２１１１０４ｒ付加体の
ジグリシジ〃エーテ／Ｉ１５部、当量のプロピレンオキ
シドトリアミンを加え、充分混合する。その後、ガラス
シャーレ上に流延し８０℃の不活性ガス雰囲気で放置し
、反応させて架橋体フィルムを得た。このフィルムを真
空乾燥した後、実施例１と同様にイオン伝導度を測定し
た。その結果を第１図の本発明２として示した。Example 2 Preliminary 7vt% lithium perchlorate and o, svt% t
-To 1 part of 1,3-dimethylimidazolidinone in which butylaminium chloride has been dissolved, add 15 parts of diglycidyl ether/I of bispheno-mudelobylene oxide 211104r adduct as epoxy and an equivalent amount of propylene oxide triamine, and mix thoroughly. do. Thereafter, it was cast onto a glass Petri dish and left in an inert gas atmosphere at 80°C to react, thereby obtaining a crosslinked film. After vacuum drying this film, the ionic conductivity was measured in the same manner as in Example 1. The results are shown as invention 2 in FIG.
第１図に示した如く、本発明は全温度領域において従来
品より優れたイオン導電性である。As shown in FIG. 1, the present invention has superior ionic conductivity over the conventional product over the entire temperature range.
発明の効果
上述した如く、本発明はイオン導電性の高い高分子固体
電解質を提供することが出来るので、その工業的価値は
極めて大である。Effects of the Invention As described above, the present invention can provide a solid polymer electrolyte with high ionic conductivity, and therefore has extremely great industrial value.
第１図は本発明の高分子固体電解質と従来品とのイオン
導電率を比較した図である。FIG. 1 is a diagram comparing the ionic conductivity of the polymer solid electrolyte of the present invention and a conventional product.
Claims (4)
を溶解した固体電解質において、該高分子網目中に相間
移動剤を媒体として高誘電率溶媒を保持することを特徴
とする高分子固体電解質。(1) A solid electrolyte in which a metal salt is dissolved in a polymer compound crosslinked with an amorphous polymer, characterized in that a high dielectric constant solvent is retained in the polymer network using a phase transfer agent as a medium. .
ノンである特許請求の範囲第１項記載の高分子固体電解
質。(2) The solid polymer electrolyte according to claim 1, wherein the high dielectric constant solvent is 1,3-dimethylimidazolidinone.
の範囲第１〜２項記載の高分子固体電解質。(3) The polymer solid electrolyte according to claims 1 to 2, wherein the phase transfer agent is a quaternary ammonium salt.
許請求の範囲第１〜２項記載の高分子固体電解質。(4) The solid polymer electrolyte according to any one of claims 1 to 2, wherein the phase transfer agent is a t-butylammonium salt.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62251141A JPH0834770B2 (en) | 1987-10-05 | 1987-10-05 | Polymer solid electrolyte |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62251141A JPH0834770B2 (en) | 1987-10-05 | 1987-10-05 | Polymer solid electrolyte |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH0195470A true JPH0195470A (en) | 1989-04-13 |
| JPH0834770B2 JPH0834770B2 (en) | 1996-03-29 |
Family
ID=17218283
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP62251141A Expired - Lifetime JPH0834770B2 (en) | 1987-10-05 | 1987-10-05 | Polymer solid electrolyte |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0834770B2 (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH025370A (en) * | 1987-12-01 | 1990-01-10 | Ricoh Co Ltd | Polymer solid electrolyte |
| JP2005174798A (en) * | 2003-12-12 | 2005-06-30 | Sony Corp | Electrolyte and battery using the same |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS60148003A (en) * | 1984-01-13 | 1985-08-05 | 第一工業製薬株式会社 | Ion conductive organic solid electrolyte |
| JPS60163373A (en) * | 1984-02-02 | 1985-08-26 | Mitsubishi Petrochem Co Ltd | Semisolid organic electrolyte |
| JPS60262852A (en) * | 1984-05-29 | 1985-12-26 | ソシエテ・ナシオナル・エルフ・アキテーヌ | Ion conductive high molecular material for manufacturing electrolyte or electrode |
-
1987
- 1987-10-05 JP JP62251141A patent/JPH0834770B2/en not_active Expired - Lifetime
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS60148003A (en) * | 1984-01-13 | 1985-08-05 | 第一工業製薬株式会社 | Ion conductive organic solid electrolyte |
| JPS60163373A (en) * | 1984-02-02 | 1985-08-26 | Mitsubishi Petrochem Co Ltd | Semisolid organic electrolyte |
| JPS60262852A (en) * | 1984-05-29 | 1985-12-26 | ソシエテ・ナシオナル・エルフ・アキテーヌ | Ion conductive high molecular material for manufacturing electrolyte or electrode |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH025370A (en) * | 1987-12-01 | 1990-01-10 | Ricoh Co Ltd | Polymer solid electrolyte |
| JP2005174798A (en) * | 2003-12-12 | 2005-06-30 | Sony Corp | Electrolyte and battery using the same |
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0834770B2 (en) | 1996-03-29 |
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