JP2780480B2 - Non-aqueous electrolyte secondary battery - Google Patents
Non-aqueous electrolyte secondary batteryInfo
- Publication number
- JP2780480B2 JP2780480B2 JP2289150A JP28915090A JP2780480B2 JP 2780480 B2 JP2780480 B2 JP 2780480B2 JP 2289150 A JP2289150 A JP 2289150A JP 28915090 A JP28915090 A JP 28915090A JP 2780480 B2 JP2780480 B2 JP 2780480B2
- Authority
- JP
- Japan
- Prior art keywords
- carbonate
- aqueous electrolyte
- secondary battery
- electrolyte secondary
- battery
- 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 - Lifetime
Links
Classifications
-
- 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
- Secondary Cells (AREA)
Description
【発明の詳細な説明】 産業上の利用分野 本発明は、非水電解液二次電池に関し、特にその低温
特性の改良に関するものである。Description: BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a non-aqueous electrolyte secondary battery, and more particularly to an improvement in its low-temperature characteristics.
従来の技術 従来、この種の非水電解液電池は高電圧、高エネルギ
ー密度を有し、かつ貯蔵性、耐漏液性などの信頼性に優
れるため、広い民生用電子機器の電源に用いられてい
る。また最近ではこの電池を二次電池化する試みが盛ん
である。二次電池の負極としてはリチウムイオンの放出
・吸蔵を繰り返すことのできる合金、炭素材、導電性高
分子、金属リチウムなどが検討されている。また、正極
には負極から溶出したリチウムイオンを収納できる反応
席を持ち、層状あるいはトンネル型の結晶構造を有する
遷移金属の酸化物やカルコゲン化合物が検討されてい
る。また、二次電池の充放電過程でリチウムイオンが電
解液を介して正・負極の間を移動するが、その電解液の
溶媒として一次電池ではプロピレンカーボネートを用い
ることが多い。2. Description of the Related Art Conventionally, this type of non-aqueous electrolyte battery has a high voltage, a high energy density, and has excellent reliability such as storability and leakage resistance. I have. Recently, attempts have been made to convert this battery into a secondary battery. As the negative electrode of the secondary battery, an alloy, a carbon material, a conductive polymer, metallic lithium, and the like, which can repeatedly release and occlude lithium ions, are being studied. Further, transition metal oxides and chalcogen compounds having a layered or tunnel-type crystal structure having a reaction site in the positive electrode capable of storing lithium ions eluted from the negative electrode have been studied. In addition, lithium ions move between the positive electrode and the negative electrode via the electrolyte during the charging and discharging of the secondary battery, and propylene carbonate is often used in the primary battery as a solvent for the electrolyte.
なぜならば、プロピレンカーボネートは支持塩をよく
溶かし、リチウムに対し安定で、しかも放電特性に優れ
るという性質を持っているからである。例えば、リチウ
ム／二酸化マンガン、リチウム／酸化銅電池などの一次
電池で用いられている。This is because propylene carbonate has the property of dissolving the supporting salt well, being stable to lithium, and having excellent discharge characteristics. For example, it is used in primary batteries such as lithium / manganese dioxide and lithium / copper oxide batteries.
発明が解決しようとする課題 このようにプロピレンカーボネートは一次電池におい
て優れた溶媒であるが、一般にプロピレンカーボネート
も含めて環状カーボネートは粘性が高く、二次電池の溶
媒にこれを単独で用いた場合、電解液の電導度が比較的
低くなる。そのため低温での充放電時や高率充放電時に
容量が小さくなるという問題点がある。Problems to be Solved by the Invention As described above, propylene carbonate is an excellent solvent in a primary battery, but generally cyclic carbonate, including propylene carbonate, has a high viscosity, and when used alone as a solvent in a secondary battery, The conductivity of the electrolyte is relatively low. Therefore, there is a problem that the capacity becomes small at the time of charge / discharge at a low temperature or at a high rate.
特にエチレンカーボネートは凝固点が36.4℃と高いた
めに溶質溶解による凝固点降下を考慮しても電解液の凝
固点が高くなる。すなわち、−20℃程度の低温で電解液
が固体状態となり、電池が作動しない。そのため、二次
電池の電解液として単独で用いることは難しい。In particular, since ethylene carbonate has a high freezing point of 36.4 ° C., the freezing point of the electrolytic solution is high even when the freezing point is lowered due to solute dissolution. That is, at a low temperature of about −20 ° C., the electrolyte becomes a solid state, and the battery does not operate. Therefore, it is difficult to use it alone as an electrolyte for a secondary battery.
一方、鎖状カーボネートは環状カーボネートに比べ低
粘性であるため、二次電池の溶媒に単独で用いた場合、
電解液の電導度はある程度増加する。しかし、環状カー
ボネートに比べ低誘電率であるため、低温で溶質が析出
する可能性がある。On the other hand, chain carbonate has a lower viscosity than cyclic carbonate, so when used alone in the solvent of the secondary battery,
The conductivity of the electrolyte increases to some extent. However, since the dielectric constant is lower than that of the cyclic carbonate, a solute may be precipitated at a low temperature.
本発明は上記の課題を解決し、低温特性の改良を目的
とするものである。An object of the present invention is to solve the above problems and improve low-temperature characteristics.
課題を解決するための手段 本発明は、正極にリチウム含有化合物を用い、負極に
リチウムイオンを吸蔵・放出できる炭素材を用いた場
合、非水電解液の溶媒として鎖状カーボネートと環状カ
ーボネートを含み、好ましくは鎖状カーボネートを溶媒
成分中に体積比率で30％〜90％含み、より好ましくは50
％〜90％含むこととしたものである。Means for Solving the Problems The present invention uses a lithium-containing compound for the positive electrode, and when a carbon material capable of inserting and extracting lithium ions is used for the negative electrode, includes a chain carbonate and a cyclic carbonate as a solvent of the non-aqueous electrolyte. , Preferably containing 30 to 90% by volume of a linear carbonate in the solvent component, more preferably 50 to 90%.
% To 90%.
作用 本発明により非水電解液の溶媒成分に鎖状カーボネー
トと環状カーボネートを含み、その体積比率（鎖状カー
ボネートの体積÷環状カーボネートの体積）を１以上９
以下とすることにより、電解液の電導度をある程度上
げ、低温での溶質析出を防ぎ、主に低温特性の向上を図
れるものである。According to the present invention, the solvent component of the non-aqueous electrolyte contains a chain carbonate and a cyclic carbonate, and the volume ratio (volume of the chain carbonate ÷ volume of the cyclic carbonate) is 1 to 9
By doing so, the conductivity of the electrolytic solution can be increased to some extent, solute deposition at low temperatures can be prevented, and mainly the low-temperature characteristics can be improved.
実施例 以下、本発明の実施例について説明する。Examples Hereinafter, examples of the present invention will be described.
第１図は実施例に用いたコイン形非水電解液二次電池
の断面図である。図で１は耐食性ステンレス製のケー
ス、２は同じ材質の封口板、３は封口板２の内面にスポ
ット溶接したニッケルのグリッド、４はカーボンを主体
とした負極活物質を缶内成型したものであり、ニッケル
のグリッド３に固着されている。５は三次元的空孔構造
（海綿状）を有するポリオレフィン系（ポリプロピレ
ン、ポリエチレンまたはそれらの共重合体）の微孔性フ
ィルムからなるセパレータである。FIG. 1 is a sectional view of a coin-type non-aqueous electrolyte secondary battery used in Examples. In the figure, 1 is a corrosion-resistant stainless steel case, 2 is a sealing plate of the same material, 3 is a nickel grid spot-welded to the inner surface of the sealing plate 2, and 4 is a carbon-based negative electrode active material molded in a can. And is fixed to a nickel grid 3. Reference numeral 5 denotes a separator made of a polyolefin-based (polypropylene, polyethylene, or a copolymer thereof) microporous film having a three-dimensional pore structure (spongy).
６は正極で、リチウムコバルト複合酸化物（LiCoO2）
を主活物質とする正極合剤を缶内成型したものであり、
チタン製のグリッド７に固着されている。正極６および
負極４に電解液を含浸させた後にセパレータ５を介して
カップリングし、８のポリプロピレン製ガスケットと共
にかしめ、封口した。6 is a positive electrode, a lithium-cobalt composite oxide (LiCoO 2 )
The positive electrode mixture with the main active material is molded in a can,
It is fixed to a grid 7 made of titanium. After the positive electrode 6 and the negative electrode 4 were impregnated with the electrolytic solution, they were coupled via a separator 5, caulked together with a polypropylene gasket 8 and sealed.
上記電解液の溶媒をエチレンカーボネート（以下ECで
示す）とジエチルカーボネート（以下DECで示す）の混
合溶媒とし、その混合体積比をEC:DEC＝70:30（電池
とする）、60:40（）、50:50（）、40:60（）、3
0:70（）、20:80（）、10:90（）、0:100（）
の８種類として電池を各20個ずつ作成した。電解液の溶
質は過塩素酸リチウムを用い、１モル／の濃度になる
ように調整した。The solvent of the electrolytic solution is a mixed solvent of ethylene carbonate (hereinafter referred to as EC) and diethyl carbonate (hereinafter referred to as DEC), and the mixing volume ratio is EC: DEC = 70: 30 (referred to as a battery), 60:40 (referred to as a battery). ), 50:50 (), 40:60 (), 3
0:70 (), 20:80 (), 10:90 (), 0: 100 ()
20 batteries were prepared for each of the eight types. The solute of the electrolyte was lithium perchlorate and adjusted to a concentration of 1 mol /.
試験条件は1mAの定電流で充電終始電圧を4.2V、放電
終始電圧を3.0Vとし、充放電を100サイクルくり返し
た。The test conditions were a constant current of 1 mA, a charge-start voltage of 4.2 V and a discharge end voltage of 3.0 V, and charging and discharging were repeated 100 cycles.
試験温度は各10個を終始20℃で、残りの10個を初期20
℃、10サイクル以降−20℃で行うこととした。The test temperature was 20 ° C for all 10 test pieces, and the initial 10
After 10 cycles at -20 ° C.
それぞれの温度での50サイクルめの放電容量を試験後
10個の平均により求め、各電池系についてプロットした
グラフを第２図に示す。第２図より20℃での放電容量は
DECの占める割合が増加するにつれて大きくなるが、こ
れは電解液の電導度の増加にともなって電池の分極が減
少したためと考えられる。電池の分極が小さくなると電
池電圧（放電時）が上がり、結果的に放電容量は大きく
なる。また、−20℃での放電容量は又はの混合比の
付近で極大値を湿す山型のカーブとなっている。と
の電池が低容量を示すのはECの組成比が大きいために電
導度が低く、電池の分極が大きいためであると考えられ
る。〜ではDECの増加につれて電解液の電導度が上
がり、それに伴って容量も増えている。〜で容量が
減少するが、これは電解液中の溶質が析出し、電池の内
部抵抗が上がり、電池の分極が増加したことが原因と考
えられる。After testing the 50th cycle discharge capacity at each temperature
FIG. 2 shows a graph obtained by averaging 10 batteries and plotting the results for each battery system. From Fig. 2, the discharge capacity at 20 ° C is
The ratio increases as the proportion of DEC increases. This is considered to be because the polarization of the battery decreases with an increase in the conductivity of the electrolyte. As the polarization of the battery decreases, the battery voltage (during discharge) increases, and as a result, the discharge capacity increases. In addition, the discharge capacity at −20 ° C. has a peak-shaped curve in which the maximum value is wetted near the mixing ratio of or. It is considered that the reason why the battery having low capacity exhibited a low capacity was that the conductivity was low due to the large composition ratio of EC, and the polarization of the battery was large. In ~, the conductivity of the electrolyte increases as the DEC increases, and the capacity also increases accordingly. The decrease in the capacity is considered to be caused by the precipitation of the solute in the electrolytic solution, the increase in the internal resistance of the battery, and the increase in the polarization of the battery.
以上の結果から本発明により非水電解液の溶媒成分の
環状カーボネートと鎖状カーボネートを含み、好ましく
は鎖状カーボネートを溶媒成分中に体積比率で30％〜90
％含み、より好ましくは50％〜90％含むこととすること
が低温特性の向上に大きな効果を持つことがわかった。
なお、実施例では正極活物質にリチウムコバルト複合酸
化物を用いたが、他のたとえばリチウムマンガン複合酸
化物などのリチウム含有化合物であってもよい。From the above results, according to the present invention, the nonaqueous electrolyte solution contains cyclic carbonate and chain carbonate as solvent components, and preferably contains 30% to 90% by volume of chain carbonate in the solvent component.
%, More preferably 50% to 90%, has a significant effect on improving low-temperature characteristics.
In the example, the lithium-cobalt composite oxide was used as the positive electrode active material. However, another lithium-containing compound such as a lithium-manganese composite oxide may be used.
また、電解液の溶媒成分である環状カーボネートとし
てエチレンカーボネートを例に挙げたが、他の環状カー
ボネート、たとえばプロピレンカーボネート、ブチレン
カーボネートなどでも良く、二種以上の混合物としても
よい。また、鎖状カーボネートとしてジエチルカーボネ
ートを例に挙げたが、ジプロピルカーボネートやメチル
エチルカーボネートなどでも良く、二種以上の混合物と
してもよい。また、環状カーボネートと鎖状カーボネー
トと他の溶媒、たとえばγ−ブチロラクトン等のラクト
ン類、１、２−ジメトキシエタンなどのエーテル類、等
一種以上との混合溶媒としてもよい。Further, ethylene carbonate has been described as an example of the cyclic carbonate which is a solvent component of the electrolytic solution. However, other cyclic carbonates such as propylene carbonate and butylene carbonate may be used, or a mixture of two or more kinds may be used. In addition, diethyl carbonate has been described as an example of the chain carbonate, but dipropyl carbonate, methyl ethyl carbonate, or the like may be used, or a mixture of two or more kinds may be used. Also, a mixed solvent of a cyclic carbonate, a chain carbonate, and one or more other solvents such as lactones such as γ-butyrolactone, ethers such as 1,2-dimethoxyethane, and the like may be used.
発明の効果 このように本発明では低温特性に優れた非水電解液二
次電池を提供することができるものである。As described above, the present invention can provide a non-aqueous electrolyte secondary battery having excellent low-temperature characteristics.
第１図は本発明におけるコイン形電池の代表的な構造を
示す断面図、第２図は20℃、−20℃における50サイクル
めの放電容量を各電池系について示した図である。 １……正極ケース、２……負極封口板、３……負極集電
体、４……負極、５……セパレータ、６……正極、７…
…正極集電体、８……ガスケット。FIG. 1 is a cross-sectional view showing a typical structure of a coin-type battery according to the present invention, and FIG. 2 is a view showing the discharge capacity at the 50th cycle at 20 ° C. and −20 ° C. for each battery system. DESCRIPTION OF SYMBOLS 1 ... Positive electrode case, 2 ... Negative electrode sealing plate, 3 ... Negative electrode current collector, 4 ... Negative electrode, 5 ... Separator, 6 ... Positive electrode, 7 ...
... Positive electrode current collector, 8 ... Gasket.
───────────────────────────────────────────────────── フロントページの続き (56)参考文献 特開 昭62−121260（ＪＰ，Ａ) 特開 平２−172163（ＪＰ，Ａ) 吉沢四郎監修 「電池ハンドブック」 （昭和51年11月18日 特許庁資料館受 け入れ） 電気書院 第３−162〜３− 164頁 (58)調査した分野(Int.Cl.6，ＤＢ名) H01M 10/40────────────────────────────────────────────────── ─── Continuation of the front page (56) References JP-A-62-121260 (JP, A) JP-A-2-172163 (JP, A) Shiro Yoshizawa, supervised by "Battery Handbook" (November 18, 1976 Patent (Received by the Agency Archives) Denki Shoin Pages 3-162 to 3-164 (58) Field surveyed (Int. Cl. 6 , DB name) H01M 10/40
Claims (5)
からなる負極と、非水電解液と、リチウム含有化合物か
らなる正極とを備え、上記非水電解液は溶媒に環状カー
ボネートと鎖状カーボネートを含むことを特徴とする非
水電解液二次電池。1. A negative electrode comprising a carbon material capable of inserting and extracting lithium ions, a non-aqueous electrolyte, and a positive electrode comprising a lithium-containing compound, wherein the non-aqueous electrolyte comprises cyclic carbonate and chain carbonate as a solvent. Non-aqueous electrolyte secondary battery characterized by including.
にエチレンカーボネートを含んでいる特許請求の範囲第
１項記載の非水電解液二次電池。2. The non-aqueous electrolyte secondary battery according to claim 1, wherein the cyclic carbonate, which is a solvent component of the electrolyte, contains ethylene carbonate.
に、ジメチルカーボネート、ジエチルカーボネート、エ
チルメチルカーボネートのうち、少なくとも一つを含む
特許請求の範囲第１項記載の非水電解液二次電池。3. The non-aqueous electrolyte secondary battery according to claim 1, wherein the chain carbonate as a solvent component of the electrolyte contains at least one of dimethyl carbonate, diethyl carbonate, and ethyl methyl carbonate. .
体積比率で30％〜90％含む特許請求の範囲第１項記載の
非水電解液二次電池。4. The non-aqueous electrolyte secondary battery according to claim 1, wherein a chain carbonate is contained in the solvent component of the electrolyte in a volume ratio of 30% to 90%.
体積比率で50％〜90％含む特許請求の範囲第１項記載の
非水電解液二次電池。5. The non-aqueous electrolyte secondary battery according to claim 1, wherein a chain carbonate is contained in the solvent component of the electrolyte in a volume ratio of 50% to 90%.
Priority Applications (5)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2289150A JP2780480B2 (en) | 1990-10-25 | 1990-10-25 | Non-aqueous electrolyte secondary battery |
| EP91107009A EP0482287B2 (en) | 1990-10-25 | 1991-04-30 | A non-aqueous secondary electrochemical battery |
| DE1991627251 DE69127251T3 (en) | 1990-10-25 | 1991-04-30 | Non-aqueous electrochemical secondary battery |
| US08/060,252 US5521027A (en) | 1990-10-25 | 1993-05-12 | Non-aqueous secondary electrochemical battery |
| US08/077,327 US5525443A (en) | 1990-10-25 | 1993-06-14 | Non-aqueous secondary electrochemical battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2289150A JP2780480B2 (en) | 1990-10-25 | 1990-10-25 | Non-aqueous electrolyte secondary battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH04162370A JPH04162370A (en) | 1992-06-05 |
| JP2780480B2 true JP2780480B2 (en) | 1998-07-30 |
Family
ID=17739412
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP2289150A Expired - Lifetime JP2780480B2 (en) | 1990-10-25 | 1990-10-25 | Non-aqueous electrolyte secondary battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2780480B2 (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US7745058B2 (en) | 2006-02-02 | 2010-06-29 | Sony Corporation | Non-aqueous solvent, non-aqueous electrolyte compositions, and non-aqueous electrolyte secondary battery |
| US11637323B2 (en) | 2018-10-15 | 2023-04-25 | Samsung Electronics Co., Ltd. | Lithium battery |
Families Citing this family (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2845069B2 (en) * | 1992-01-13 | 1999-01-13 | 日本電池株式会社 | Organic electrolyte secondary battery |
| US5714280A (en) * | 1994-11-09 | 1998-02-03 | Furukawa Denchi Kabushiki Kaisha | Lithium secondary battery |
| JP3482591B2 (en) * | 1998-07-31 | 2003-12-22 | 日本電池株式会社 | Non-aqueous electrolyte battery |
| JP2000156244A (en) * | 1998-11-18 | 2000-06-06 | Japan Storage Battery Co Ltd | Nonaqueous electrolyte secondary battery |
| JP3956384B2 (en) | 1999-09-20 | 2007-08-08 | ソニー株式会社 | Secondary battery |
| KR101148644B1 (en) * | 2003-11-13 | 2012-05-23 | 우베 고산 가부시키가이샤 | Nonaqueous electrolyte solution and lithium secondary battery |
| JP6939636B2 (en) | 2018-02-22 | 2021-09-22 | トヨタ自動車株式会社 | Electrolyte and lithium-ion battery |
| JP7020208B2 (en) | 2018-03-16 | 2022-02-16 | トヨタ自動車株式会社 | Electrolyte and lithium-ion battery |
-
1990
- 1990-10-25 JP JP2289150A patent/JP2780480B2/en not_active Expired - Lifetime
Non-Patent Citations (1)
| Title |
|---|
| 吉沢四郎監修 「電池ハンドブック」 （昭和５１年１１月１８日 特許庁資料館受け入れ） 電気書院 第３−１６２〜３−１６４頁 |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US7745058B2 (en) | 2006-02-02 | 2010-06-29 | Sony Corporation | Non-aqueous solvent, non-aqueous electrolyte compositions, and non-aqueous electrolyte secondary battery |
| US11637323B2 (en) | 2018-10-15 | 2023-04-25 | Samsung Electronics Co., Ltd. | Lithium battery |
Also Published As
| Publication number | Publication date |
|---|---|
| JPH04162370A (en) | 1992-06-05 |
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