JP4417232B2 - Lead acid battery - Google Patents
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- JP4417232B2 JP4417232B2 JP2004343225A JP2004343225A JP4417232B2 JP 4417232 B2 JP4417232 B2 JP 4417232B2 JP 2004343225 A JP2004343225 A JP 2004343225A JP 2004343225 A JP2004343225 A JP 2004343225A JP 4417232 B2 JP4417232 B2 JP 4417232B2
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- 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
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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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Description
本発明は、深い放電が繰り返され、かつガッシングが起き難い条件で使用しても高い電池容量が維持され、かつ長寿命な、特にアイドリングストップや過充電防止システムを採用した自動車に適した鉛蓄電池に関する。 The present invention relates to a lead-acid battery that is suitable for automobiles that employ an idling stop or overcharge prevention system that maintains a high battery capacity even when used under conditions in which deep discharge is repeated and gassing is unlikely to occur. About.
鉛蓄電池では、充放電中、特に深い放電後の充電時に、濃厚な硫酸が沈降して、電解液の比重が電極板の下部に行くほど高くなる成層化現象が起きる。
この成層化現象では、電極下部の電解液比重が高くなるため、充電効率が低下して、正負両極でサルフェーション(粗大硫酸鉛結晶粒の生成)が進行するとともに濃淡電池を形成して自己放電が急速に進行する。その結果、電池寿命は著しく短くなる。
In a lead storage battery, during charging / discharging, particularly during charging after deep discharge, concentrated sulfuric acid settles, and a stratification phenomenon occurs in which the specific gravity of the electrolytic solution increases toward the lower part of the electrode plate.
In this stratification phenomenon, the specific gravity of the electrolyte below the electrode increases, so the charging efficiency decreases, sulfation (generation of coarse lead sulfate crystal grains) proceeds in both positive and negative electrodes, and a self-discharge is formed by forming a concentration cell. Proceeds rapidly. As a result, the battery life is significantly shortened.
前記成層化現象を防止するものとして、柔軟な合成樹脂製肉薄シートのベース面に多数のリブ(条)を垂直方向に設けたリブ付きセパレータが提案された(特許文献1)。このセパレータによれば、電極板下部に滞留する高濃度硫酸が、過充電時の水分解で発生するガスの撹拌(ガッシング)により、リブに邪魔されることなく浮上し成層化現象が解消される。 In order to prevent the stratification phenomenon, a ribbed separator has been proposed in which a large number of ribs (stripes) are provided in the vertical direction on the base surface of a flexible synthetic resin thin sheet (Patent Document 1). According to this separator, the high-concentration sulfuric acid staying at the lower part of the electrode plate floats without being obstructed by the ribs and eliminates the stratification phenomenon due to gas stirring (gassing) generated by water decomposition during overcharge. .
しかしながら、近年、自動車には、省燃費や排ガス削減を目的に、信号などで停車中はエンジンを停止するアイドリングストップが採用された。しかしエンジン停止中は、電力が鉛蓄電池から供給され、発進時には速やかにエンジンを始動するため、鉛蓄電池は従来のSLI用途(始動・照明・イグニション)とは比較にならないほど放電が深くなり、成層化現象が起き易くなった。また過充電の手前で充電を終了して発電機の負荷を軽減する過充電防止システムが採用されているが、この場合は、過充電によるガッシング回数が減り、成層化現象が解消され難くなった。さらにアイドリングストップによる深い放電は、正極活物質の軟化(活物質の結合力の低下)を早めた。このようなことから電池寿命が著しく低下した。 However, in recent years, an idling stop that stops the engine while the vehicle is stopped by a signal or the like has been adopted for automobiles in order to save fuel consumption and reduce exhaust gas. However, when the engine is stopped, power is supplied from the lead-acid battery, and the engine is started quickly when starting. Therefore, the lead-acid battery has a deep discharge that is not comparable to conventional SLI applications (starting, lighting, and ignition). It became easy to occur. Also, an overcharge prevention system that reduces the load on the generator by terminating charging before overcharging is adopted, but in this case, the number of gassing due to overcharging is reduced, making it difficult to eliminate the stratification phenomenon. . Furthermore, deep discharge due to idling stop accelerated softening of the positive electrode active material (decrease in the binding force of the active material). As a result, the battery life was significantly reduced.
前記成層化現象をリテーナマット(AGM)からなるセパレータを用いて防止した密閉式鉛蓄電池が提案されたが、この電池は電解液が少量なため十分な電池容量が得られず、また仮に電解液量が多くてもAGMセパレータは緻密で電解液の拡散性が悪いため、やはり電解液量相応の電池容量は得られなかった。 A sealed lead-acid battery in which the stratification phenomenon is prevented by using a separator made of a retainer mat (AGM) has been proposed. However, since this battery has a small amount of electrolyte, sufficient battery capacity cannot be obtained. Even if the amount is large, since the AGM separator is dense and the diffusibility of the electrolyte is poor, the battery capacity corresponding to the amount of the electrolyte cannot be obtained.
本発明は、深い放電が繰り返され、かつガッシングが起き難い条件で使用しても高い電池容量が維持され、かつ長寿命な、特にアイドリングストップや過充電防止システムを採用した自動車に適した鉛蓄電池の提供を目的とする。 The present invention relates to a lead-acid battery that is suitable for automobiles that employ an idling stop or overcharge prevention system that maintains a high battery capacity even when used under conditions in which deep discharge is repeated and gassing is unlikely to occur. The purpose is to provide.
本発明は、正極板と、袋状セパレータ内に収容された負極板とを、フェルト状セパレータを介して交互に積層してなる極板群が電槽内に挿入された鉛蓄電池において、前記フェルト状セパレータは平均孔径が10〜100μmであり、20kPa加圧時の厚みuと5kPa加圧時の厚みvの比率(u/v)が50%以上であり、前記極板群が電槽内に圧迫度10〜25kPaで挿入されていることを特徴とする鉛蓄電池である。 The present invention relates to a lead-acid battery in which a positive electrode plate and a negative electrode plate accommodated in a bag-like separator are alternately laminated via a felt-like separator, and the electrode plate group is inserted in a battery case. The shape separator has an average pore diameter of 10 to 100 μm, the ratio (u / v) of the thickness u at the time of 20 kPa pressurization and the thickness v at the time of 5 kPa pressurization is 50% or more, and the electrode plate group is in the battery case. It is a lead storage battery characterized by being inserted at a compression degree of 10 to 25 kPa.
本発明の鉛蓄電池は、正極板と、袋状セパレータ内に収容された負極板とを、フェルト状セパレータを介して交互に積層してなる極板群が電槽内に挿入された鉛蓄電池において、前記フェルト状セパレータの平均孔径並びに加圧時の厚み比率、および極板群の電槽内圧迫度を適正に規定したもので、前記フェルト状セパレータは、電解液の保持および拡散を良好に維持しつつ高濃度硫酸の沈降を抑制し、さらに正極活物質の軟化を防止する。そのため、本発明の鉛蓄電池は、電池容量および容量維持率(電池寿命)が優れる。 The lead storage battery of the present invention is a lead storage battery in which a positive electrode plate and a negative electrode plate accommodated in a bag-like separator are alternately laminated via a felt-like separator and inserted into the battery case. The felt-shaped separator appropriately defines the average pore diameter, the thickness ratio at the time of pressurization, and the degree of pressure in the battery case of the electrode plate group, and the felt-shaped separator maintains the retention and diffusion of the electrolyte well. In addition, the sedimentation of high-concentration sulfuric acid is suppressed, and the softening of the positive electrode active material is further prevented. Therefore, the lead storage battery of the present invention is excellent in battery capacity and capacity retention rate (battery life).
本発明において、フェルト状セパレータの平均孔径を10〜100μm、20kPa加圧時の厚みuと5kPa加圧時の厚みvの比率(u/v)を50%以上、前記極板群の圧迫度を10〜25kPaに規定する理由は、前記平均孔径が10μm未満でも、前記厚み比率(u/v)が50%未満でも、電槽内圧迫度が25kPaを超えても、フェルト状セパレータの平均孔径が小さくなって電解液の保持性並びに拡散性が低下し、十分な電池容量が得られなくなるためである。また前記平均孔径が100μmを超えても、前記圧迫度が10kPa未満でも、フェルト状セパレータの平均孔径が大きいため高濃度硫酸が沈降して成層化現象が起き易くなるためである。さらに圧迫度が10kPa未満の場合は正極活物質が軟化し易くなるためである。 In the present invention, the average pore diameter of the felt separator is 10 to 100 μm, the ratio (u / v) of the thickness u when pressing 20 kPa and the thickness v when pressing 5 kPa is 50% or more, and the degree of compression of the electrode plate group is Even if the average pore diameter is less than 10 μm, the thickness ratio (u / v) is less than 50%, or even if the pressure in the battery case exceeds 25 kPa, the average pore diameter of the felt separator is set to 10-25 kPa. This is because it becomes smaller and the retention and diffusibility of the electrolytic solution decrease, and a sufficient battery capacity cannot be obtained. Further, even if the average pore diameter exceeds 100 μm, even if the degree of compression is less than 10 kPa, since the average pore diameter of the felt separator is large, high-concentration sulfuric acid is settled and a stratification phenomenon easily occurs. Further, when the degree of compression is less than 10 kPa, the positive electrode active material is easily softened.
本発明において、フェルト状セパレータの加圧時の厚み比率が大きいということは、前記セパレータの圧縮変形抵抗が大きく、従って電極群が高圧迫度で挿入されていても前記セパレータの微細孔は縮径し難いことを意味する。
前記厚み比率が50%以上であれば、圧迫度が25kPaと高くても、また平均孔径が10μmと小さくても、前記セパレータは微細孔が殆ど縮径せず、従って電解液が、セパレータ内に十分な量保持されると同時に、微細孔内を良好に拡散する。
In the present invention, a large thickness ratio during pressurization of the felt-shaped separator means that the separator has a large compressive deformation resistance. Therefore, even if the electrode group is inserted with high pressure, the fine pores of the separator are reduced in diameter. It means that it is difficult to do.
If the thickness ratio is 50% or more, even if the degree of compression is as high as 25 kPa and the average pore diameter is as small as 10 μm, the separator has almost no micropores, so the electrolyte is not contained in the separator. While maintaining a sufficient amount, it diffuses well in the micropores.
本発明において、フェルト状セパレータとは、ガラス繊維、ポリプロピレン繊維などからなる不織布で、微細孔(網目構造)を有し、保水性、通水性、弾力性を備えたマット状のものである。前記フェルト状セパレータは弾力性を有するため活物質を損傷せずに活物質の軟化を防止できる。 In the present invention, the felt-like separator is a non-woven fabric made of glass fiber, polypropylene fiber or the like, has a fine pore (network structure), and has a mat shape having water retention, water permeability and elasticity. Since the felt-shaped separator has elasticity, it can prevent softening of the active material without damaging the active material.
本発明において、負極板は袋状セパレータ内に収容されているので、正極板と接触して短絡事故を起こすことがない。前記袋状セパレータは、例えば、ポリエチレンシートをベースとする合成樹脂製の袋である。 In the present invention, since the negative electrode plate is accommodated in the bag-shaped separator, it does not contact the positive electrode plate to cause a short circuit accident. The bag-like separator is, for example, a synthetic resin bag based on a polyethylene sheet.
Ca0.04質量%、Sn1.0質量%、Al0.015質量%、Ba0.008質量%を含み、残部がPbと不可避不純物からなるPb−Ca系合金を、ブックモールドにより毎分15枚の速度で格子板に鋳造し、次いで前記格子板を120℃で3時間熱処理(時効硬化)して正極基板を作製した。 Pb-Ca alloy containing 0.04 mass% Ca, 1.0 mass% Sn, 0.015 mass% Al, 0.008 mass% Ba, and the balance consisting of Pb and inevitable impurities. Then, the grid plate was heat treated at 120 ° C. for 3 hours (age hardening) to prepare a positive electrode substrate.
次に、公知の方法で調製した正極用ペーストを前記正極基板に充填し、その後温度40℃、湿度95%の雰囲気で24時間熟成し、乾燥して正極未化成板を作製した。
次に、前記正極未化成板に、公知の方法で作製した負極未化成板を、微細なガラス繊維を編組したガラスマット(フェルト状セパレータ)を介して積層し、この積層体の同極板同士をCOS方式で溶接して極板群とした。なお、前記負極未化成板は、厚み0.25mmのポリエチレンシートをベースとする合成樹脂製袋内に収容した。
Next, the positive electrode paste prepared by a known method was filled in the positive electrode substrate, then aged in an atmosphere of a temperature of 40 ° C. and a humidity of 95% for 24 hours, and dried to produce a positive electrode unformed sheet.
Next, the negative electrode non-formed plate produced by a known method is laminated on the positive electrode non-formed plate through a glass mat (felt-shaped separator) braided with fine glass fibers, and the same polar plates of this laminate are combined. Were welded by the COS method to form an electrode plate group. The negative electrode unformed sheet was accommodated in a synthetic resin bag based on a polyethylene sheet having a thickness of 0.25 mm.
次に前記極板群をポリプロピレン製の電槽に挿入し、ヒートシールにより蓋をし、前記蓋の液口から電解液(25℃の比重が1.200の希硫酸に、20g/リットルの硫酸アルミニウムを添加したもの)を注入し、次いで液注入後の電槽を40℃の水槽に入れて電槽化成を行い、5時間率容量が50AhのD23サイズの12V鉛蓄電池を製造した。
電解液比重は1.28(20℃)であった。
Next, the electrode plate group is inserted into a battery case made of polypropylene, covered with heat seal, and an electrolyte solution (a dilute sulfuric acid having a specific gravity of 1.200 at 25 ° C. is added to a 20 g / liter sulfuric acid from a liquid port of the lid). Then, the battery case after the liquid injection was put into a 40 ° C. water tank to form a battery case, and a D23 size 12V lead acid battery having a 5-hour rate capacity of 50 Ah was manufactured.
The electrolyte specific gravity was 1.28 (20 ° C.).
前記ガラスマットの平均孔径および厚み比率(u/v)は本発明規定値内で種々に変化させた。また前記極板群の圧迫度は、極板群端部と電槽内面との間にスペーサーを差し込んで10〜25kPaの範囲内で種々に変化させた。
前記ガラスマットの平均孔径は、前記ガラスマットの任意の横断面を顕微鏡観察して、1mm四方に存在する各微細孔の最大径と最小径を計測し、それらを平均して求めた。
The average pore diameter and thickness ratio (u / v) of the glass mat were variously changed within the specified values of the present invention. The degree of compression of the electrode plate group was variously changed within a range of 10 to 25 kPa by inserting a spacer between the end of the electrode plate group and the inner surface of the battery case.
The average pore diameter of the glass mat was obtained by observing an arbitrary cross section of the glass mat with a microscope, measuring the maximum diameter and the minimum diameter of each micropore present in 1 mm square, and averaging them.
得られた各々の鉛蓄電池について、5時間率容量(初期容量)Y1を常法により測定した。5時間率容量が45Ah以上を良好、45Ah未満を不良と判定した。 The obtained each lead-acid battery, 5-hour rate capacity (initial capacity) and the Y 1 is measured by a conventional method. The 5-hour rate capacity was determined to be good when it was 45 Ah or more, and poor when it was less than 45 Ah.
次に、前記鉛蓄電池について、JIS重負荷試験を40℃の温度で150サイクル行った後、5時間率容量Y2を測定し、容量維持率[(Y2/Y1)×100%]を求めた。容量維持率が65%以上を良好(長寿命)、65%未満を不良と判定した。 Next, the lead storage battery was subjected to a JIS heavy load test for 150 cycles at a temperature of 40 ° C., then the 5-hour rate capacity Y 2 was measured, and the capacity retention rate [(Y 2 / Y 1 ) × 100%] Asked. A capacity maintenance ratio of 65% or more was judged good (long life), and less than 65% was judged bad.
別途得られた各々の鉛蓄電池について、充放電とも電流50Aを6分間流すサイクル試験を200回繰り返した後、セル内の上部と下部の電解液を採取し、比重差を測定して成層化の程度を調べた。
比重差が0.04以下を良好(成層化現象が僅少)、0.04を超えたら不良と判定した。
このサイクル試験では過充電には至らず、ガッシングは起きなかった。
For each lead-acid battery obtained separately, a cycle test in which a current of 50 A was passed for 6 minutes for both charging and discharging was repeated 200 times, and then the upper and lower electrolytes in the cell were collected, and the specific gravity difference was measured to determine stratification. I examined the degree.
A specific gravity difference of 0.04 or less was good (strategy phenomenon was slight), and when it exceeded 0.04, it was judged as defective.
This cycle test did not lead to overcharging, and no gassing occurred.
[比較例1]フェルト状セパレータの平均孔径を本発明規定値外とした他は、実施例1と同じ方法により鉛蓄電池を製造し、実施例1と同じ調査を行った。 [Comparative Example 1] A lead storage battery was manufactured in the same manner as in Example 1 except that the average pore diameter of the felt separator was outside the specified range of the present invention, and the same investigation as in Example 1 was performed.
[比較例2]フェルト状セパレータの厚み比率(u/v)を本発明規定値外とした他は、実施例1と同じ方法により鉛蓄電池を製造し、実施例1と同じ調査を行った。 [Comparative Example 2] A lead storage battery was manufactured by the same method as in Example 1 except that the thickness ratio (u / v) of the felt separator was outside the specified value of the present invention, and the same investigation as in Example 1 was performed.
[比較例3]極板群の圧迫度を本発明規定値外とした他は、実施例1と同じ方法により鉛蓄電池を製造し、実施例1と同じ調査を行った。 [Comparative Example 3] A lead-acid battery was manufactured by the same method as in Example 1 except that the degree of compression of the electrode group was outside the specified value of the present invention, and the same investigation as in Example 1 was performed.
[比較例4]フェルト状セパレータを用いなかった他は、実施例1と同じ方法により鉛蓄電池を製造し、実施例1と同じ調査を行った。
実施例1および比較例1〜4の調査結果を表1に示す。
[Comparative Example 4] A lead-acid battery was manufactured by the same method as in Example 1 except that no felt separator was used, and the same investigation as in Example 1 was performed.
The investigation results of Example 1 and Comparative Examples 1 to 4 are shown in Table 1.
表1から明らかなように、本発明例の鉛蓄電池(実施例1、No.1〜9)は、いずれも初期容量が45Ah以上、上下比重差が0.03以下、容量維持率が70%以上と優れた特性を示した。これはガラスマット(フェルト状セパレータ)の平均孔径並びに厚み比率、および極板群の電槽内圧迫度を適正に規定したため、電解液がガラスマット内に十分保持され、また電解液がガラスマットの微細孔内を良好に拡散し、かつ高濃度硫酸の沈降および正極活物質の軟化が抑制されたことによる。さらに負極板を合成樹脂製の袋に入れたので短絡事故も起きなかった。 As is clear from Table 1, all of the lead storage batteries of the present invention (Example 1, Nos. 1 to 9) have an initial capacity of 45 Ah or more, an upper / lower specific gravity difference of 0.03 or less, and a capacity maintenance ratio of 70%. Excellent characteristics were shown as above. This is because the average pore diameter and thickness ratio of the glass mat (felt-shaped separator) and the pressure in the battery case of the electrode plate group are properly defined, so that the electrolyte is sufficiently retained in the glass mat, and the electrolyte is This is because the inside of the fine pores diffuses satisfactorily, and sedimentation of high concentration sulfuric acid and softening of the positive electrode active material are suppressed. Furthermore, since the negative electrode plate was placed in a synthetic resin bag, no short circuit accident occurred.
これに対し、No.10はもともとガラスマットの平均孔径が小さいため、No.12はガラスマットの厚み比率(圧縮変形抵抗)が小さいため、No.14は極板群の圧迫度が大きいため、いずれも電解液が、ガラスマット内に十分保持されず、また電解液が十分拡散しなかったため初期容量が低下した。 In contrast, no. No. 10 originally has a small average pore size of the glass mat, so No. 12 has a small thickness ratio (compression deformation resistance) of the glass mat. In No. 14, since the degree of compression of the electrode plate group was large, the electrolyte was not sufficiently retained in the glass mat, and the initial capacity was reduced because the electrolyte did not sufficiently diffuse.
No.11はガラスマットの平均孔径がもともと大きかったため、No.13は圧迫度が小さかったため、いずれも高濃度硫酸が沈降して成層化現象が起き、容量維持率が低下した。No.15はガラスマットを使用しなかったため、成層化現象に加え、正極活物質が軟化し、容量維持率が著しく低下した。
No. No. 11 was because the average pore size of the glass mat was originally large. Since No. 13 had a low degree of compression, high concentration sulfuric acid settled, causing a stratification phenomenon, and the capacity retention rate decreased. No. Since No. 15 did not use a glass mat, in addition to the stratification phenomenon, the positive electrode active material was softened, and the capacity retention rate was significantly reduced.
Claims (1)
In a lead-acid battery in which an electrode plate group in which a positive electrode plate and a negative electrode plate accommodated in a bag-like separator are alternately laminated via a felt-like separator is inserted into a battery case, the felt-like separator is an average The pore diameter is 10 to 100 μm, the ratio (u / v) of the thickness u at the time of 20 kPa pressurization and the thickness v at the time of 5 kPa pressurization is 50% or more. A lead-acid battery, which is inserted at 25 kPa.
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CN103283080B (en) | 2011-03-08 | 2016-01-20 | 株式会社杰士汤浅国际 | Liquid formula lead accumulator and battery system |
JP2013145663A (en) * | 2012-01-13 | 2013-07-25 | Panasonic Corp | Valve regulated lead-acid |
JP2016513861A (en) * | 2013-03-07 | 2016-05-16 | ダラミック エルエルシー | Oxidation-resistant laminated separator |
JP6164266B2 (en) * | 2015-09-18 | 2017-07-19 | 株式会社Gsユアサ | Lead acid battery |
JP6750378B2 (en) * | 2016-07-29 | 2020-09-02 | 株式会社Gsユアサ | Lead acid battery |
JP7084381B2 (en) | 2017-04-28 | 2022-06-14 | エンテックアジア株式会社 | Separator for lead-acid battery |
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