WO2017085918A1 - 非水電解質二次電池 - Google Patents
非水電解質二次電池 Download PDFInfo
- Publication number
- WO2017085918A1 WO2017085918A1 PCT/JP2016/004839 JP2016004839W WO2017085918A1 WO 2017085918 A1 WO2017085918 A1 WO 2017085918A1 JP 2016004839 W JP2016004839 W JP 2016004839W WO 2017085918 A1 WO2017085918 A1 WO 2017085918A1
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- WO
- WIPO (PCT)
- Prior art keywords
- negative electrode
- current collector
- silicon
- secondary battery
- electrolyte secondary
- Prior art date
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- 239000011255 nonaqueous electrolyte Substances 0.000 title claims abstract description 51
- 238000004804 winding Methods 0.000 claims abstract description 22
- 238000007789 sealing Methods 0.000 claims abstract description 9
- 239000007773 negative electrode material Substances 0.000 claims description 26
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 claims description 20
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 17
- 229910052751 metal Inorganic materials 0.000 claims description 14
- 239000002184 metal Substances 0.000 claims description 14
- 239000002210 silicon-based material Substances 0.000 claims description 13
- 239000007774 positive electrode material Substances 0.000 claims description 12
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 11
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 10
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 10
- 229910052710 silicon Inorganic materials 0.000 claims description 10
- 239000010703 silicon Substances 0.000 claims description 10
- 229910052759 nickel Inorganic materials 0.000 claims description 9
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 7
- 239000003575 carbonaceous material Substances 0.000 claims description 7
- 229910052814 silicon oxide Inorganic materials 0.000 claims description 7
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 6
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- 229910002804 graphite Inorganic materials 0.000 claims description 6
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- PAZHGORSDKKUPI-UHFFFAOYSA-N lithium metasilicate Chemical compound [Li+].[Li+].[O-][Si]([O-])=O PAZHGORSDKKUPI-UHFFFAOYSA-N 0.000 claims description 6
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- H01M50/543—Terminals
- H01M50/552—Terminals characterised by their shape
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- H01M50/536—Electrode connections inside a battery casing characterised by the method of fixing the leads to the electrodes, e.g. by welding
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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
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- 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
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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
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Definitions
- Patent Document 1 discloses a non-aqueous electrolyte secondary battery in which a plurality of leads are connected to an electrode plate according to the length and width of the electrode plate and the thickness of a current collector.
- Patent Documents 2 and 3 disclose nonaqueous electrolyte secondary batteries in which negative electrode leads are connected to both ends of the negative electrode plate in the length direction.
- both ends in the length direction of the negative electrode plate are electrically connected to the outer can serving as the negative electrode external terminal via the first negative electrode lead or the second negative electrode lead.
- a non-aqueous electrolyte secondary battery having excellent characteristics can be provided. Further, even if the joint between the first negative electrode lead and the second negative electrode lead having relatively weak joint strength is broken, the first negative electrode lead joined to the end of the negative electrode plate on the winding start side is the bottom of the outer can. And the joint is maintained.
- the second negative electrode lead joined to the end of the negative electrode plate on the winding end side loses electrical connection with the outer can, but the second negative electrode current collector provided on the end of the negative electrode plate on the winding end side
- the body exposed portion is in contact with the inner surface of the side wall of the outer can. Therefore, even if the joint between the first negative electrode lead and the second negative electrode lead breaks, electrical connection between both ends of the negative electrode plate and the outer can is ensured. Therefore, according to one embodiment of the present invention, it is possible to provide a nonaqueous electrolyte secondary battery in which a decrease in output characteristics when subjected to external vibration or impact is suppressed.
- a first negative electrode lead 12a and a second negative electrode lead 12b are joined to the first negative electrode current collector exposed portion 11a and the second negative electrode current collector exposed portion 11b, respectively.
- the first and second negative electrode leads 12a and 12b may be bonded to either the front or back of the negative electrode current collector.
- Examples of the joining method of the first and second negative electrode leads 12a and 12b include welding methods such as resistance welding, ultrasonic welding, and laser welding, and a rubbing method.
- the negative electrode current collector is completely exposed at both ends in the length direction of the negative electrode plate 11 in FIG. 2, but the charge / discharge reaction is performed within a range that does not hinder the bonding of the first and second negative electrode leads 12a and 12b.
- a negative electrode active material layer that does not contribute is allowed to adhere to the negative electrode current collector.
- the negative electrode active material a carbon material or a silicon material capable of reversibly occluding and releasing lithium ions can be used.
- the carbon material and the silicon material can be used alone or in combination. Since the silicon material has a large volume change due to charging / discharging, the second negative electrode current collector exposed portion 11 b arranged on the outermost periphery of the electrode body 16 can reliably contact the inner surface 21 a of the side wall of the outer can 21. Therefore, it is preferable to use a silicon material as the negative electrode active material.
- the positive electrode plate 13 has a positive electrode active material layer formed on a positive electrode current collector.
- the positive electrode active material layer is preferably formed on both surfaces of the positive electrode current collector.
- a positive electrode current collector exposed portion is provided at the center in the length direction of the positive electrode plate 13.
- the positive electrode lead 14 is joined to the exposed portion of the positive electrode current collector. Examples of the joining method include welding methods such as resistance welding, ultrasonic welding, and laser welding, and a rubbing method. By joining the positive electrode lead 14 to the center of the positive electrode plate 13, the current collection efficiency of the positive electrode plate 13 can be increased.
- the positive lead 14 is preferably joined to the central portion of the positive electrode plate 13 in the length direction, but the joining position of the positive lead 14 is not limited to the central portion. It is preferable to apply an insulating tape on the positive electrode lead 14 and on the back surface of the positive electrode current collector to which the positive electrode lead 14 is bonded. Thereby, the internal short circuit resulting from the positive electrode lead 14 can be prevented.
- the electrode body 16 is produced by winding the negative electrode plate 11 and the positive electrode plate 13 with a separator 15 interposed therebetween. As shown in FIG. 3, an annular insulating plate 17 is disposed below the electrode body 16.
- the first negative electrode lead 12a and the second negative electrode lead 12b led out from the electrode body 16 are bent toward the hollow portion 16a of the electrode body 16 to form an overlapping portion 12c.
- the overlapping portion 12 c is joined to the bottom of the outer can 21. Examples of the joining method include resistance welding and laser welding.
- a microporous film mainly composed of polyolefin such as polyethylene (PE) or polypropylene (PP) can be used.
- the microporous membrane can be used singly or as a laminate of two or more layers.
- a layer mainly composed of polyethylene (PE) having a low melting point as an intermediate layer and polypropylene (PP) excellent in oxidation resistance as a surface layer.
- Inorganic particles such as aluminum oxide (Al 2 O 3 ), titanium oxide (TiO 2 ), and silicon oxide (SiO 2 ) can be added to the separator. Such inorganic particles can be carried in the separator and can be applied together with a binder on the separator surface.
- An aramid resin can also be applied to the surface of the separator.
- Examples of cyclic carboxylic acid esters include ⁇ -butyrolactone ( ⁇ -BL) and ⁇ -valerolactone ( ⁇ -VL).
- Examples of chain carboxylic acid esters include methyl pivalate, ethyl pivalate, methyl isobutyrate and methyl Pionate is exemplified.
- the first negative electrode current collector exposed portion 11a and the second negative electrode current collector exposed portion 11b were provided at positions corresponding to both ends in the length direction of the completed negative electrode plate 11, respectively.
- the negative electrode active material layer 11c was compressed with a roller, and the compressed electrode plate was cut into a predetermined size.
- the first negative electrode current collector exposed portion 11a and the second negative electrode current collector exposed portion 11b are respectively connected to the first negative electrode lead 12a and the second negative electrode lead 12b made of a clad material of Ni—Cu—Ni.
- the negative electrode plate 11 shown in FIG. 2 was produced by joining by sonic welding.
- Preparation of positive electrode plate 100 parts by mass of LiNi 0.82 Co 0.15 Al 0.03 O 2 as a positive electrode active material, 1 part by mass of acetylene black as a conductive agent, and 0.9 parts by mass of polyvinylidene fluoride as a binder (PVDF) was mixed. The mixture was put into N-methyl-2-pyrrolidone (NMP) as a dispersion medium and kneaded to prepare a positive electrode mixture slurry. The positive electrode mixture slurry was applied to both surfaces of an aluminum positive electrode current collector having a thickness of 15 ⁇ m by a doctor blade method and dried to form a positive electrode active material layer.
- NMP N-methyl-2-pyrrolidone
- a positive electrode current collector exposed portion was provided at a position corresponding to the central portion of the completed positive electrode plate 13. Subsequently, the positive electrode active material layer was compressed with a roller, and the compressed electrode plate was cut into a predetermined size. Finally, the positive electrode lead 14 made of aluminum was joined to the exposed portion of the positive electrode current collector by ultrasonic welding to produce a positive electrode plate 13.
- the negative electrode plate 11 and the positive electrode plate 13 were wound through a separator 15 made of a polyethylene microporous film to produce an electrode body 16.
- the first negative electrode current collector exposed portion 11a was arranged on the winding start side, and the second negative electrode current collector exposed portion 11b was arranged on the winding end side.
- the winding core was removed from the electrode body 16, whereby a hollow portion 16 a was formed at a position corresponding to the winding axis of the electrode body 16.
- the end of winding of the electrode body 16 was fixed with a winding tape.
- a bottomed cylindrical outer can 21 was produced by drawing a plate member plated with nickel.
- the arithmetic average roughness (Ra) of the inner surface 21a of the side wall of the outer can 21 was 1.4 ⁇ m.
- the arithmetic average roughness (Ra) was measured by a method based on JIS B 0601-2001.
- the insulating plate 18 was disposed on the upper portion of the electrode body 16, and a rotating disk was pressed against the outer side surface of the outer can 21 to form a groove portion.
- a gasket 19 was disposed on the grooved portion, and a sealing body 20 was connected to the positive electrode lead 14.
- a nonaqueous electrolyte is injected into the inside of the outer can 21, and the sealing body 20 is caulked and fixed to the groove portion of the outer can 21 via the gasket 19, whereby the cylindrical nonaqueous electrolyte secondary battery shown in FIG. 10 was produced.
- Examples 2 and 3 The nonaqueous electrolyte secondary battery according to Examples 2 and 3 in the same manner as in Example 1 except that the arithmetic average roughness (Ra) of the inner surface 21a of the side wall of the outer can 21 was changed to the value described in Table 1. 10 was produced.
- Nonaqueous electrolyte secondary batteries 10 according to Examples 4 to 7 were produced in the same manner as in Example 3 except that a mixture of graphite and SiO produced as described above was used as the negative electrode active material.
- Table 1 shows the content of SiO in the negative electrode active materials of Examples 4 to 7. The SiO content shown in Table 1 is expressed as a percentage of SiO with respect to the total mass of graphite and SiO.
- the internal resistance (IR) of each battery was measured before and after the vibration test, and the increase amount ( ⁇ IR) of the internal resistance by the vibration test was calculated.
- Table 1 shows the test results.
- the amount of increase in internal resistance ( ⁇ IR) shown in Table 1 is an average value of five batteries measured for each example and comparative example.
- Example 1 to 7 and Comparative Example 1 the current value during resistance welding was set to 1.4 kA, but the increase in internal resistance due to the vibration test was suppressed by setting the current value to 2.1 kA. This is shown by the result of 2. However, if the current value during resistance welding is excessively increased, production problems such as generation of spatter and damage to the bottom of the outer can occur. That is, as shown in Examples 1 to 7, according to one embodiment of the present invention, the current value at the time of resistance welding can be reduced, so that a non-aqueous electrolyte secondary battery having excellent load characteristics can be produced. Can be avoided.
- Comparison of Examples 3 to 7 shows that the increase in internal resistance is suppressed as the content of SiO in the negative electrode active material is increased. If the content of SiO is 4% by mass or more, the internal resistance is not increased. From the viewpoint of suppressing the increase in internal resistance, the larger the SiO content, the better. However, considering the balance with battery characteristics such as cycle characteristics, the SiO content is preferably 20% by mass or less. Therefore, the preferable range of the SiO content is 4% by mass or more and 20% by mass or less.
- Nonaqueous electrolyte secondary battery 11 negative electrode plate 11a first negative electrode current collector exposed portion 11b second negative electrode current collector exposed portion 11c negative electrode active material layer 12a first negative electrode lead 12b second negative electrode lead 12c overlapping portion 13 positive electrode plate 14 Positive electrode lead 15
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Abstract
Description
(負極板の作製)
負極活物質としての97質量部の黒鉛と、増粘剤としての1.5質量部のカルボキシメチルセルロース(CMC)と、結着剤としての1.5質量部のスチレンブタジエンゴムを混合した。その混合物を分散媒としての水へ投入し、混練して負極合剤スラリーを作製した。その負極合剤スラリーを、厚み8μmの銅製の負極集電体の両面にドクターブレード法により塗布し、乾燥して負極活物質層11cを形成した。このとき、完成した負極板11の長さ方向の両端部に対応するそれぞれの位置に第1負極集電体露出部11aと第2負極集電体露出部11bを設けた。次いで、負極活物質層11cをローラーで圧縮し、圧縮された極板を所定サイズに切断した。最後に、第1負極集電体露出部11a及び第2負極集電体露出部11bにそれぞれNi-Cu-Niの三層のクラッド材からなる第1負極リード12a及び第2負極リード12bを超音波溶接で接合して図2に示す負極板11を作製した。
正極活物質として100質量部のLiNi0.82Co0.15Al0.03O2と、導電剤としての1質量部のアセチレンブラックと、結着剤としての0.9質量部のポリフッ化ビニリデン(PVDF)を混合した。その混合物を分散媒としてのN-メチル-2-ピロリドン(NMP)に投入し、混練して正極合剤スラリーを調製した。その正極合剤スラリーをドクターブレード法により厚みが15μmのアルミニウム製の正極集電体の両面に塗布し、乾燥して正極活物質層を形成した。このとき、完成した正極板13の中央部に対応する位置に正極集電体露出部を設けた。次いで、正極活物質層をローラーにより圧縮し、圧縮された極板を所定サイズに切断した。最後に、正極集電体露出部にアルミニウム製の正極リード14を超音波溶接で接合して正極板13を作製した。
負極板11及び正極板13を、ポリエチレン製微多孔膜からなるセパレータ15を介して巻回して電極体16を作製した。電極体の作製の際、第1負極集電体露出部11aを巻き始め側に、第2負極集電体露出部11bを巻き終り側に配置した。電極体16の作製後、巻芯を電極体16から取り除くことにより電極体16の巻回軸に対応する位置に中空部16aが形成された。電極体16の巻き終り端部は巻き止めテープで固定した。
エチレンカーボネート(EC)と、エチルメチルカーボネート(EMC)と、ジメチルカーボネート(DMC)を25:5:70の体積比(1気圧、25℃)で混合して非水溶媒を調製した。その非水溶媒に電解質塩としてのヘキサフルオロリン酸リチウム(LiPF6)を1.4mol/Lの濃度に溶解して非水電解質を調製した。
ニッケルめっきされた板状部材を絞り加工することによって有底筒状の外装缶21を作製した。外装缶21の側壁の内面21aの算術平均粗さ(Ra)は1.4μmであった。算術平均粗さ(Ra)はJIS B 0601-2001に準拠した方法で測定した。
電極体16の中空部16aの近傍から突出する第1負極リード12aを環状の絶縁板17の開口部に挿入して絶縁板17を電極体16の下部に貼り付けた。そして、電極体16の外周部から導出している第2負極リード12bを電極体16の中空部16aに向けて折り曲げた。次いで、第1負極リード12aを電極体16の中空部16aに向けて折り曲げて、図3に示す重なり部12cを形成した。その電極体16を外装缶21へ挿入した後、次のように重なり部12cを外装缶21の底部に接合した。まず、電極体16の中空部16aから電極棒を挿入して電極棒を重なり部12cに当接させた。次いで、その電極棒と対極になる電極板を外部から外装缶21の底部に当接させた。その電極棒と電極板との間に1.4kAの電流を流すことにより重なり部12cと外装缶21の底部を抵抗溶接した。これにより、第1負極リード12aの一方の面が外装缶21の底部に接合され、第1負極リード12aの他方の面が第2負極リード12bに接合された。
外装缶21の側壁の内面21aの算術平均粗さ(Ra)を表1に記載された値に変更したこと以外は実施例1と同様にして実施例2及び3に係る非水電解質二次電池10を作製した。外装缶21の側壁の内面21aの算術平均粗さ(Ra)を変更するために、外装缶21の作製の際にニッケルめっきされた鉄製の板状部材の絞り回数や絞り加工に用いる治具を調整した。
(負極活物質の作製)
SiO(一般式SiOxのx=1に対応)の組成を有する酸化ケイ素を炭化水素系のガスを含むアルゴン雰囲気下で加熱し、炭化水素系のガスを熱分化させる化学蒸着(CVD)法によりSiOの表面を炭素で被覆した。炭素の被覆量はSiOの質量に対して10質量%とした。次に、炭素で被覆されたSiO粒子をアルゴン雰囲気下において1000℃での不均化反応によりSiO粒子中に微細にSi相とSiO2相を形成して、所定の粒度に分級して負極活物質に用いるSiOを作製した。
電極体36から導出している第1及び第2負極リード32a,32bを電極体36の中空部に向けて折り曲げる際に、第1負極リード32aを折り曲げた後に第2負極リード32bを折り曲げたこと以外は実施例1と同様にして比較例1に係る非水電解質二次電池を作製した。比較例1に係る非水電解質二次電池においては、図4に示すように第2負極リード32bの一方の面が外装缶41の底部に接合され、第2負極リード32bの他方の面が第1負極リード32aに接合されている。さらに、抵抗溶接時の電流値を2.1kAとしたこと以外は比較例1と同様にして比較例2に係る非水電解質二次電池を作製した。
実施例及び比較例に係る各電池について、次の条件に基づいて振動試験を行った。各電池を巻回軸が水平方向になるように振動試験装置に固定した後、振動数が15分間で7Hz→200Hz→7Hzと変化するように正弦波形の振動を対数掃引して各電池に振動を与えた。その振動サイクルを各電池のX軸方向、Y軸方向、及びZ軸方向のそれぞれの振動方向に対して4サイクル行うことにより、各電池に合計12サイクルの振動を与えた。なお、X軸、Y軸、及びZ軸は互いに直交する3つの空間軸に対応し、そのうち一つは電極体の巻回軸に対応する。振動試験前後に各電池の内部抵抗(IR)を測定し、振動試験による内部抵抗の増加量(ΔIR)を算出した。表1に試験結果を示す。なお、表1に示した内部抵抗の増加量(ΔIR)は各実施例及び比較例について測定した5個の電池の平均値である。
11 負極板
11a 第1負極集電体露出部
11b 第2負極集電体露出部
11c 負極活物質層
12a 第1負極リード
12b 第2負極リード
12c 重なり部
13 正極板
14 正極リード
15 セパレータ
16 電極体
16a 中空部
17 絶縁板
18 絶縁板
19 ガスケット
20 封口体
21 外装缶
21a 外装缶の側壁の内面
Claims (8)
- 負極集電体に負極活物質層が形成された負極板及び正極集電体上に正極活物質層が
形成された正極板がセパレータを介して巻回された電極体と、
非水電解質と、
前記電極体及び前記非水電解質を収容する有底筒状の外装缶と、
前記外装缶の開口部を封止する封口体と、を備え、
前記負極板が巻き始め側の端部及び巻き終り側の端部にそれぞれ負極活物質層が形成されていない第1負極集電体露出部及び第2負極集電体露出部を有し、
前記第2負極集電体の少なくとも一部が前記外装缶の側壁の内面に接触し、
前記第1負極集電体露出部及び前記第2負極集電体露出部に、それぞれ第1負極リード及び第2負極リードが接合され、
前記第1負極リード及び前記第2負極リードが前記電極体の一方の端面から前記外装缶の底部に向けて導出しており、
前記第1負極リードが前記外装缶の底部に接合され、前記第2負極リードが前記第1負極リードに接合されている、
非水電解質二次電池。 - 前記負極活物質層が黒鉛とケイ素材料を含む、請求項1に記載の非水電解質二次電池。
- 前記ケイ素材料がケイ素、酸化ケイ素、ケイ素合金、ケイ酸リチウム、及びケイ素複合体からなる群から選ばれる少なくとも一つである、請求項2に記載の非水電解質二次電池。
- 前記酸化ケイ素が一般式SiOx(0.5≦x<1.6)で表される請求項3に記載の非水電解質二次電池。
- 前記ケイ素合金がニッケル、鉄、銅、チタン、タングステン、及び、モリブデンからなる群から選ばれる少なくとも一つの金属元素とケイ素との合金である請求項3に記載の非水電解質二次電池。
- 前記ケイ素複合体が炭素材料及びケイ酸リチウムの少なくとも一方と、ケイ素からなる請求項3に記載の非水電解質二次電池。
- 前記ケイ素材料は前記負極活物質層中に前記黒鉛と前記ケイ素材料の合計質量に対して4質量%以上20質量%以下含まれる請求項2から6のいずれかに記載の非水電解質二次電池。
- 前記外装缶の側壁の内面の表面粗さRaが0μm以上1.4μm以下である請求項1から7のいずれかに記載の非水電解質二次電池。
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US10468655B2 (en) | 2019-11-05 |
CN108352491B (zh) | 2021-01-08 |
US20180323419A1 (en) | 2018-11-08 |
JP6879214B2 (ja) | 2021-06-02 |
CN108352491A (zh) | 2018-07-31 |
JPWO2017085918A1 (ja) | 2018-09-06 |
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