WO2016088535A1 - 蓄電装置 - Google Patents
蓄電装置 Download PDFInfo
- Publication number
- WO2016088535A1 WO2016088535A1 PCT/JP2015/082018 JP2015082018W WO2016088535A1 WO 2016088535 A1 WO2016088535 A1 WO 2016088535A1 JP 2015082018 W JP2015082018 W JP 2015082018W WO 2016088535 A1 WO2016088535 A1 WO 2016088535A1
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- WIPO (PCT)
- Prior art keywords
- load
- power storage
- negative electrode
- active material
- secondary battery
- Prior art date
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Images
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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
- This invention relates to a power storage device.
- EVs Electric Vehicles
- PHVs Plug Vehicles Hybrid Vehicles
- power storage devices such as lithium ion secondary batteries that store electric power supplied to electric motors.
- a power storage device includes an electrode assembly in which a positive electrode and a negative electrode are stacked in layers while being insulated from each other.
- the negative electrode includes a metal foil and an active material layer covering the surface of the metal foil, and the active material layer of the negative electrode includes a carbon-based material as an active material. It is included. And in patent document 1, it suppresses that the active material layer of a negative electrode expands with charging / discharging by prescribing
- the expansion of the active material layer can be suppressed by applying a load to the electrode assembly. For this reason, it is expected to suppress expansion of the active material layer in consideration of applying a load to the electrode assembly.
- the present invention has been made paying attention to such problems existing in the conventional technology, and an object thereof is to provide a power storage device capable of suppressing the expansion of the active material layer.
- a power storage device that solves the above problems includes an electrode assembly that is layered in a state in which a positive electrode and a negative electrode are insulated from each other, and the positive electrode and the negative electrode that overlap each other in the electrode assembly.
- the density of the carbon-based material in the active material layer is 1.2 g / cm 3 or more, and the (100) plane X-ray diffraction intensities I (100) and (002) plane in the active material layer
- the degree of orientation given by the ratio (I (100) / I (002)) to the X-ray diffraction intensity I (002) of the material is 0.3 or less, and the load applied by the load application mechanism is 0.2 MPa or more.
- a carbon-based material serving as an active material has a crystal structure similar to that of graphite at least partially.
- delamination occurs due to the insertion and removal of lithium from the interlayer, which may cause the negative electrode active material layer to expand.
- the density of the carbon-based material is 1.2 g / cm 3 or more and the degree of orientation is 0.3 or less, so that the direction in which the positive electrode and the negative electrode overlap with each other The expansion and contraction direction can be matched.
- delamination can be suppressed by giving a load of 0.2 MPa or more to the electrode assembly from the direction in which the positive electrode and the negative electrode overlap, and expansion of the active material layer of the negative electrode can be suppressed.
- the load applied by the load applying mechanism is preferably 0.22 MPa or more. According to this configuration, delamination is further suppressed and the active material layer of the negative electrode is suppressed as compared with the case where the load applied from the direction in which the positive electrode and the negative electrode overlap with the electrode assembly is 0.2 MPa or more. Can be further suppressed from expanding.
- the electrode assembly has a laminated structure in which the positive electrodes and the negative electrodes are alternately laminated, and the load application mechanism applies a load that applies a load to the electrode assembly. It is preferable to have a surface. According to this configuration, since the load can be applied to the electrode assembly on the load application surface, the area capable of suppressing the expansion of the active material layer can be increased.
- the electrode assembly includes a porous separator interposed between the positive electrode and the negative electrode and insulating the positive electrode and the negative electrode from each other, and the load application
- the load applied by the mechanism is preferably 4 MPa or less. According to this configuration, it is possible to suppress the function of the separator from being impaired by the load while suppressing the expansion of the active material layer.
- the power storage device includes a case that houses the electrode assembly, and the load applying mechanism is configured to apply a load from the outside of the case.
- the load applying mechanism is provided outside the case, so that the maintenance of the load applying mechanism can be facilitated.
- the said load provision mechanism has a pair of restraint board arrange
- the “elastic member” is not limited to a material that exhibits elasticity even in a state where the entire body is formed as a uniform solid body, such as rubber, and a material that exhibits elasticity in a porous state, such as foamed plastic. means. According to this configuration, the battery performance (capacity maintenance ratio) is reduced by the load applying mechanism as compared with the case where a load is applied to the wall of the case via the pair of restraint plates without the elastic member interposed. This can be suppressed.
- the power storage device includes a case that houses the electrode assembly, the load applying mechanism is provided inside the case of a unit power storage unit, and the positive electrode and the negative electrode of the case overlap each other. It may be a thickness adjusting material interposed between the wall in the direction of contact and the electrode assembly.
- the thickness adjusting material is formed of an elastic member such as rubber or foamed plastic. According to this configuration, when the electrode assembly expands, the electrode assembly is pressed against the case wall via the thickness adjusting member interposed between the case wall and the outer surface of the electrode assembly. It is suppressed that an excessive force is applied.
- the power storage device includes a plurality of unit power storage units each including a case and the electrode assembly housed in the case, wherein the unit power storage units are arranged in a line along the overlapping direction, and the load application It is preferable that the mechanism applies a load from both ends of the plurality of unit power storage units in the overlapping direction.
- the carbon-based material is preferably graphite.
- expansion of the active material layer can be suppressed.
- the fragmentary sectional view which shows the secondary battery cell provided with the load provision mechanism of another structure.
- a secondary battery module 10 as a power storage device includes one or a plurality of secondary battery cells 30 as unit power storage units, and a load applying mechanism 50 that applies a load from both ends of the secondary battery cells 30.
- FIG. 1 illustrates a secondary battery module 10 having a plurality of secondary battery cells 30.
- the direction in which the secondary battery cells 30 are arranged is simply referred to as “parallel arrangement direction D1”.
- the secondary battery cell 30 is a lithium ion secondary battery having a rectangular external appearance.
- the secondary battery cell 30 includes a case 11 and an electrode assembly 12 accommodated in the case 11.
- the case 11 includes a bottomed square cylindrical case body 13 having an opening 14 and a square plate-like lid 15 that closes the opening 14.
- the case main body 13 and the lid 15 are made of metal such as stainless steel or aluminum.
- the wall thickness of the case body 13 is set to a thickness that allows elastic deformation.
- the case 11 contains an electrolytic solution as an electrolyte (not shown).
- the electrode assembly 12 includes a positive electrode 16 and a negative electrode 17, and in the electrode assembly 12, the positive electrode 16 and the negative electrode 17 are insulated from each other. It is layered. That is, the electrode assembly 12 has a laminated structure in which the positive electrodes 16 and the negative electrodes 17 are alternately laminated. In the following description, the direction in which the positive electrode 16 and the negative electrode 17 overlap is simply referred to as “stacking direction D2”.
- the electrode assembly 12 includes a porous separator 18 that is interposed between the positive electrode 16 and the negative electrode 17 and insulates the positive electrode 16 and the negative electrode 17 from each other.
- the separator 18 is made of, for example, a resin material such as polypropylene or polyethylene, and has a fine pore structure so that lithium (lithium ions) can pass along with charge and discharge.
- the positive electrode 16 includes a positive electrode metal foil 16a, a positive electrode active material layer 16b covering the positive electrode metal foil 16a, and a positive electrode current collecting tab 16c protruding from the edge in the surface direction of the positive electrode metal foil 16a.
- the positive electrode metal foil 16a is, for example, an aluminum foil or an aluminum alloy foil.
- the positive electrode active material layer 16b includes a positive electrode active material, a binder, and a conductive additive. Examples of the active material for the positive electrode include LiCoO 2 , LiNiO 2 , LiMn 2 O 4 , LiFePO 4 , LiCo 1/3 Ni 1/3 Mn 1/3 O 2 , and the like.
- the binder for the positive electrode is, for example, polyvinylidene fluoride, polytetrafluoroethylene, styrene butadiene rubber or the like.
- the binder for the positive electrode one type may be used, or two or more types may be used in combination.
- the conductive additive for the positive electrode include acetylene black, ketjen black, and flaky graphite.
- the negative electrode 17 has a negative electrode metal foil 17a, a negative electrode active material layer 17b covering the negative electrode metal foil 17a, and a negative electrode current collecting tab 17c protruding from the edge in the surface direction of the negative electrode metal foil 17a.
- the negative electrode metal foil 17a is, for example, a copper foil or a copper alloy foil.
- the negative electrode active material layer 17b includes a negative electrode active material, a binder, and a conductive additive.
- the active material for the negative electrode is a carbon-based material capable of inserting and extracting lithium (lithium ions).
- the carbon-based material include graphite (natural graphite, artificial graphite), coke, graphite, glassy carbon, fired organic polymer compound, carbon fiber, activated carbon, carbon black, and the like. Is graphite.
- the binder for the negative electrode include polyvinylidene fluoride, polytetrafluoroethylene, and styrene butadiene rubber. One type of binder may be used for the negative electrode, or two or more types may be used in combination.
- the conductive auxiliary for the negative electrode include acetylene black and ketjen black.
- the density (filling density) of the carbon-based material in the negative electrode active material layer is 1.2 g / cm 3 or more.
- the density of the carbon-based material in the negative electrode active material layer is preferably 1.2 g / cm 3 or more and 1.7 g / cm 3 or less, more preferably 1.3 g / cm 3 or more and 1.6 g / cm 3 or less.
- the density of the active material in the negative electrode active material layer exceeds 1.7 g / cm 3 , the density becomes too high and the active materials are easily brought into contact with each other and damaged.
- the ratio (X (100) / I (002)) of the X-ray diffraction intensity I (100) of the (100) plane and the X-ray diffraction intensity I (002) of the (002) plane in the negative electrode active material layer is not more than 0.3, more preferably not more than 0.07.
- the active material particles 27 made of a carbon-based material have a crystal structure similar to that of graphite at least in part, and within the crystal structure of the graphite.
- the ratio in which the direction Da is oriented so as to be along the surface direction of the negative electrode metal foil 17a is increased.
- each active material particle 27 is oriented so that the interlayer direction Db in the graphite crystal structure is perpendicular to the surface of the negative electrode metal foil 17a, that is, along the stacking direction D2.
- lithium is easily expanded and contracted along the interlayer direction Db due to the insertion and removal of lithium with respect to the interlayer during charging and discharging, and the interlayer direction Db is charged and discharged. It becomes the expansion and contraction direction accompanying. That is, in the negative electrode active material layer 17b, the active material particles 27 are oriented so that the expansion / contraction direction of the active material particles 27 is along the stacking direction D2.
- each active material particle 27 is shown in a simplified manner. However, actually, each active material particle 27 is not necessarily uniformly oriented, and It is not necessarily a uniform shape or size.
- the electrode assembly 12 has a positive electrode current collection tab group 19 that protrudes from a surface 12a facing the lid 15 and in which a plurality of positive electrode current collection tabs 16c are stacked in layers.
- the positive electrode current collecting tab group 19 is connected to a positive electrode terminal 20 that exchanges electricity with the electrode assembly 12.
- the positive terminal 20 is fixed to the lid 15 and protrudes outside the case 11.
- the electrode assembly 12 has a negative electrode current collection tab group 21 that protrudes from the facing surface 12a and in which a plurality of negative electrode current collection tabs 17c are stacked in layers.
- the negative electrode current collecting tab group 21 is connected to a negative electrode terminal 22 that exchanges electricity with the electrode assembly 12.
- the negative terminal 22 is fixed to the lid 15 and protrudes outside the case 11.
- the length (thickness) of the electrode assembly 12 along the stacking direction D2 is the same or substantially the same as the distance between the inner wall surfaces of the two walls 13a facing each other in the stacking direction D2 among the walls of the case 11. Is set to For example, an insulating film or a thickness adjusting material may be interposed between the wall of the case 11 and the electrode assembly 12. Therefore, in the secondary battery cell 30, it is possible to apply a load from the stacking direction D2 to the electrode assembly 12 by applying a load from the stacking direction D2 to each wall 13a.
- the secondary battery cells 30 are in a state in which the stacking directions D ⁇ b> 2 in the electrode assemblies 12 included in the secondary battery cells 30 are aligned.
- the secondary battery cells 30 are arranged in a row (parallel arrangement direction D 1), and the electrode assembly included in each secondary battery cell 30. 12, the direction in which the positive electrode 16 and the negative electrode 17 overlap (the stacking direction D2) coincides.
- the load applying mechanism 50 includes a first constraining plate 51 and a second constraining plate 52 as a pair of constraining plates disposed at both ends in the stacking direction D2.
- the first restraining plate 51 is disposed at the first end in the stacking direction D2, and has a load application surface 51a that applies a load by making surface contact with the case 11 of the secondary battery cell 30.
- the second constraining plate 52 is disposed at a second end opposite to the first end in the stacking direction D2, and a load applying surface 52a that applies a load by being in surface contact with the case 11 of the secondary battery cell 30. have.
- the load application surfaces 51 a and 52 a are in contact with the single secondary battery cell 30.
- the load application surface 51 a of the first restraint plate 51 contacts the secondary battery cell 30 disposed at the first end, and the second restraint cell 51.
- the load application surface 52a of the plate 52 is in contact with the secondary battery cell 30 disposed at the second end.
- the load application mechanism 50 is configured to apply a load to the electrode assembly 12 from the outside of the case 11.
- the load applied by the load applying mechanism 50 is 0.20 MPa or more, preferably 0.22 MPa or more, and more preferably 0.25 MPa or more. Further, the load applied by the load applying mechanism 50 is, for example, 4 MPa or less. By setting the load applied by the load applying mechanism 50 to 4 MPa or less, the pore structure of the separator 18 can be suppressed from being blocked. In the load application mechanism 50, the load applied to the secondary battery cell 30 can be appropriately changed by adjusting the degree of screwing of the nut 54.
- the stacking direction D2 and the expansion / contraction direction of the active material particles 27 in the negative electrode active material layer 17b of the negative electrode 17 are matched. That is, in the secondary battery module 10, the negative electrode active material layer 17b is included in the negative electrode active material layer 17b by applying a load to the secondary battery cell 30 (electrode assembly 12) from the stacking direction D2. A load can be applied from the direction of expansion and contraction of the active material particles 27. Therefore, the active material particles 27 can be efficiently prevented from being unwound due to charge / discharge without excessively increasing the load applied by the load applying mechanism 50.
- the density of the carbon-based material is 1.2 g / cm 3 or more and the degree of orientation is 0.3 or less, so that the stacking direction D2 and the expansion / contraction direction of the active material particles 27 are reduced. And can be in a consistent state. Then, delamination is suppressed by applying a load of 0.20 MPa or more, preferably 0.22 MPa or more to the electrode assembly 12 from the stacking direction D2, and the negative electrode active material layer 17b of the negative electrode 17 expands. This can be suppressed.
- the load applying mechanism 50 includes a secondary battery cell 30 disposed at the first end among the secondary battery cells 30 as the plurality of unit power storage units disposed in the parallel direction D ⁇ b> 1.
- a plate-like elastic member 60 is interposed between the first constraining plate 51, between the secondary battery cell 30 disposed at the second end and the second constraining plate 52, and between adjacent secondary battery cells 30. ing.
- the elastic member 60 is formed in a size that covers the entire surface of the wall 13a and the end surface of the lid 15 that face each other in the juxtaposition direction D1 among the walls of the case body 13 of the case 11 of the secondary battery cell 30. Elastic rubber is used as the elastic member 60.
- the secondary battery cell 30 is not in direct contact with the first restraint plate 51, the second restraint plate 52, or the adjacent secondary battery cell 30, and the elastic member 60 is interposed therebetween. Therefore, when a load is applied by the load applying mechanism 50, a force is easily applied uniformly to the wall 13a of the case body 13, and the load is applied uniformly to the electrode assembly 12 from the stacking direction D2, so that the electrolyte on the electrode surface Unevenness of the holding amount is suppressed, leading to an improvement in the life of the secondary battery cell 30.
- the elastic member 60 is interposed as compared with the case where the load applied to the secondary battery cell 30 by the load applying mechanism 50 is adjusted only by the degree of screwing of the nut 54 to the through bolt 53. It becomes easy to adjust the magnitude of the load to a target value.
- the following effects can be obtained in addition to the effects basically the same as (1) to (5) of the first embodiment. .
- the load applying mechanism 50 includes the secondary battery cell 30 and the first restraining plate arranged at the first end among the secondary battery cells 30 as the plurality of unit power storage units arranged in the juxtaposed direction D1. 51, a plate-like elastic member 60 is interposed between the secondary battery cell 30 disposed at the second end and the second restraining plate 52, and between the adjacent secondary battery cells 30. . Therefore, compared to a configuration in which the plate-like elastic member 60 is not interposed, unevenness in the amount of electrolyte solution retained in the secondary battery cell 30 can be suppressed, leading to an improvement in the life of the secondary battery cell 30.
- the embodiment is not limited to the above, and may be embodied as follows, for example.
- the secondary battery module 10 may include a single or a plurality of secondary battery cells 30 over a plurality of rows.
- the secondary battery module 10 may include a load applying mechanism 50 inside the case 11 of the secondary battery cell 30.
- a configuration in which a plurality of electrode assemblies 12 are arranged in parallel in the stacking direction D2 inside one case may be employed.
- the load applied to the electrode assembly 12 may be adjusted by, for example, a thickness adjusting member 70 interposed between the electrode assembly 12 and the wall 13a of the case body 13 as shown in FIG.
- the thickness adjusting material 70 corresponds to the load applying mechanism 50.
- the thickness adjusting member 70 is formed of an elastic member such as rubber or foamed plastic to have a predetermined thickness, and one or a plurality of thickness adjusting members 70 are provided corresponding to the distance between the electrode assembly 12 and the wall 13a of the case body 13. .
- the thickness adjusting members 70 may be provided separately on both sides of the electrode assembly 12 or may be provided only on one side of the electrode assembly 12.
- the load applying mechanism 50 may be configured to apply a load by an actuator.
- the load applying mechanism 50 includes a second end between the secondary battery cell 30 disposed at the first end and the first restraining plate 51 among the plurality of secondary battery cells 30 disposed in the parallel direction D1.
- the elastic member 60 may be interposed between at least one location between the secondary battery cell 30 and the second restraining plate 52 disposed between the secondary battery cell 30 and the adjacent secondary battery cell 30.
- the elastic member is provided only between the secondary battery cell 30 disposed at the first end and the first restraint plate 51 and between the secondary battery cell 30 disposed at the second end and the second restraint plate 52.
- a configuration in which the elastic member 60 is interposed only between the adjacent secondary battery cells 30 may be employed.
- the load applying mechanism 50 is provided between the secondary battery cell 30 and the first restraining plate 51 arranged at the first end, and between the secondary battery cell 30 and the first restraining plate 51 arranged at the second end.
- the plate-like elastic member 60 is interposed between the adjacent secondary battery cells 30 and between the adjacent secondary battery cells 30, unevenness in the amount of electrolyte retained in the secondary battery cells 30 can be further suppressed, leading to an improvement in life.
- the electrode assembly 12 may be a wound electrode assembly wound in a state where a strip-shaped separator is interposed between the strip-shaped positive electrode and the strip-shaped negative electrode.
- the electrode assembly 12 may be formed to have a flat surface that faces the wall 13a of the case 11 respectively.
- the case 11 constituting the secondary battery cell 30 may be in a shape capable of applying a load from the stacking direction D2 in the electrode assembly 12, and may not be rectangular.
- the secondary battery module 10 may be mounted on a passenger car or an industrial vehicle as a vehicle, or may be applied as a stationary power storage device.
- the secondary battery module 10 may be embodied as a power storage module including a plurality of capacitors such as an electric double layer capacitor and a lithium ion capacitor.
- D50 is the median diameter.
- the active material paste was applied to an aluminum foil having a thickness of 15 ⁇ m, further dried, and then cut into a sheet shape.
- the basis weight of the active material layer 18.3 mg / cm 2
- the active material in the positive electrode active material layer A positive electrode having a density of 3.13 g / cm 3 was obtained.
- a load applying mechanism is assembled to the obtained single secondary battery cell so that a load of 0.25 MPa is applied to the secondary battery cell 30 (electrode assembly 12). Got.
- the secondary battery modules of Samples 2 to 5 are the same as the secondary battery module of Sample 1 although the density of the active material in the negative electrode active material layer, the degree of orientation, and the load due to the load applying mechanism are different. Therefore, detailed description is omitted.
- the secondary battery module of Sample 6 is the secondary battery module of the second embodiment, that is, between the secondary battery cell arranged at the first end of the plurality of secondary battery cells and the first restraining plate.
- Capacity maintenance rate (%) (Charge capacity after specified cycle / Charge capacity after first cycle) x 100
- the density of the active material (carbon-based material) in the negative electrode active material layer is 1.2 g / cm 3 or more, the degree of orientation is 0.3 or less, and the load applied by the load application mechanism is 0.1.
- Samples 2, 3, 5, 6, and 7 having a pressure of 22 MPa or more a result in which the capacity retention rate was higher than those of Sample 1 and Sample 4 was obtained.
- the active material particles in the negative electrode active material layer are not sufficiently oriented so that the interlayer direction Db in the crystal structure is along the stacking direction D2, and delamination occurs due to the load applied by the load applying mechanism. It is considered that the capacity retention rate was lowered as a result.
- the load applying mechanism has a configuration in which an elastic member is interposed between the secondary battery cell and the first restraining plate, between the secondary battery cell and the second restraining plate, and between adjacent secondary battery cells. From the evaluation results of the sample 6 and the sample 7 used, a result in which the capacity retention rate was higher than that of the corresponding sample 3 and sample 5 not using the elastic member was obtained.
- Fig. 8 shows the relationship between the number of cycles and the capacity retention rate for Samples 1-7. From FIG. 8, it can be seen that the capacity retention rate is higher in samples 2, 3 and 5 than in samples 1 and 4, and the capacity retention rate is higher in samples 6 and 7 than in samples 2, 3, and 5. I understand clearly.
- the density of the active material in the negative electrode active material layer is preferably 1.2 g / cm 3 or more, the degree of orientation is 0.3 or less, and the load by the load applying mechanism is preferably 0.22 MPa or more. It was done.
- D2 ... stacking direction, Da ... inner layer direction, Db ... interlayer direction, 10 ... secondary battery module (power storage device), 11 ... case, 12 ... electrode assembly, 16 ... positive electrode, 17 ... negative electrode, 17a ... negative electrode Metal foil (metal foil), 17b ... negative electrode active material layer (active material layer), 18 ... separator, 27 ... active material particles (carbon-based material), 30 ... secondary battery cell (unit power storage unit), 50 ... load application Mechanism: 51 ... first restraint plate, 51a ... load application surface, 52 ... second restraint plate, 52a ... load application surface, 60 ... elastic member, 70 ... thickness adjusting material.
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Abstract
Description
以下、本実施形態の二次電池モジュールについて説明する。
図1に示すように、蓄電装置としての二次電池モジュール10は、単位蓄電部としての単数又は複数の二次電池セル30と、二次電池セル30の両端から荷重を付与する荷重付与機構50とを備えている。なお、図1には、複数の二次電池セル30を有する二次電池モジュール10が例示されている。以下の説明では、複数の二次電池セル30を有する場合において、二次電池セル30が並ぶ方向を単に「並設方向D1」と示す。
図2に示すように、二次電池セル30は、外観が角型であるリチウムイオン二次電池である。二次電池セル30は、ケース11と、該ケース11に収容されている電極組立体12と、を備えている。ケース11は、開口部14を有する有底四角筒状のケース本体13と、開口部14を塞ぐ四角板状の蓋15と、を有する。ケース本体13及び蓋15は、例えばステンレスやアルミニウムなどの金属製である。ケース本体13の壁の肉厚は、弾性変形可能な程度の厚さに設定されている。また、ケース11には、図示しない電解質として、電解液が収容されている。
荷重付与機構50は、積層方向D2の両端に配置されている一対の拘束板として、第1拘束板51と第2拘束板52とを有している。第1拘束板51は、積層方向D2における第1端に配置されており、二次電池セル30のケース11と面接触することで荷重を付与する荷重付与面51aを有している。第2拘束板52は、積層方向D2における第1端とは反対側の第2端に配置されており、二次電池セル30のケース11と面接触することで荷重を付与する荷重付与面52aを有している。
(1)本実施形態では、炭素系材料の密度が1.2g/cm3以上であって、且つ配向度が0.3以下であることで、積層方向D2と活物質粒子27の膨張収縮方向とを整合させた状態にできる。そして、電極組立体12に対して、積層方向D2から0.20MPa以上、好ましくは0.22MPa以上の荷重を付与することにより層間剥離を抑制し、負極電極17の負極活物質層17bが膨張することを抑制できる。
(3)荷重付与機構50が付与する荷重を4MPa以下とすることで、負極活物質層17bの膨張を抑制しつつも、荷重によってセパレータ18の機能を損なってしまうことを抑制できる。
(5)負極活物質層における活物質粒子の解れを抑制し、充放電が繰り返されることによる容量維持率の低下を抑制できる。即ち、二次電池モジュール10としての寿命が短くなることを抑制できる。
次に、第2の実施形態の二次電池モジュールについて説明する。なお、この実施形態は、第1の実施形態において、荷重付与機構の構成を変更した点が異なり、他の構成は同様であるため、同様の部分についてはその詳細な説明を省略する。
二次電池モジュール10は、単数又は複数の二次電池セル30を、複数列にわたって備えていてもよい。
荷重付与機構50は、並設方向D1に配置された複数の二次電池セル30のうちの、第1端に配置された二次電池セル30と第1拘束板51との間、第2端に配置された二次電池セル30と第2拘束板52との間、及び隣合う二次電池セル30との間の少なくとも1箇所に弾性部材60が介在している構成としてもよい。例えば、第1端に配置された二次電池セル30と第1拘束板51との間、及び第2端に配置された二次電池セル30と第2拘束板52との間にのみ弾性部材60が介在している構成や、隣合う二次電池セル30の間のみに弾性部材60が介在している構成としてもよい。しかし、荷重付与機構50は、第1端に配置された二次電池セル30と第1拘束板51との間、第2端に配置された二次電池セル30と第1拘束板51との間、及び隣合う二次電池セル30間の全てに板状の弾性部材60が介在している方が、二次電池セル30における電解液保持量のムラをより抑制でき、寿命向上に繋がる。
二次電池モジュール10は、車両としての乗用車や産業用車両に搭載してもよく、定置用の蓄電装置として適用してもよい。
<試料の作製>
(試料1)
[正極電極の作製]
正極用の活物質としてLiNi0.5Co0.2Mn0.3O2(D50=6μm,比表面積=0.5m2/g,タップ密度=2.2g/cm3)と、導電助剤として鱗片状黒鉛と、バインダとしてポリフッ化ビニリデンとをN-メチル-2-ピロリドン(NMP)に懸濁させ、正極用の活物質ペーストを得た。なお、D50は、メジアン径である。続けて、厚さ15μmのアルミニウム箔に対して活物質ペーストを塗布し、さらに乾燥させた後にシート状に切り出し、活物質層の目付け量=18.3mg/cm2、正極活物質層における活物質の密度=3.13g/cm3である正極電極を得た。
負極用の活物質として黒鉛(D50=20μm,比表面積=3.7m2/g,タップ密度=0.98g/cm3)と、増粘剤としてカルボキシメチルセルロース(CMC)と、バインダとしてスチレンブタジエンゴム(SBR)とを水に懸濁させ、負極用の活物質ペーストを得た。続けて、厚さ10μmの銅箔に対して活物質ペーストを塗布し、さらに乾燥及びプレスしたのちにシート状に切り出し、活物質層の目付け量=11.1mg/cm2、負極活物質層における活物質の密度=1.0g/cm3、配向度=0.48である負極電極を得た。
作製した正極電極と負極電極とを間にセパレータを介在させた状態で交互に積層し、電極組立体を作製するとともに、該電極組立体をケースに収容したのち、電解液をケースに充填して二次電池セルを得た。なお、電解液としては、エチレンカーボネートとメチルエチルカーボネートとジメチルカーボネートとを体積比3:3:4で混合した混合溶媒に、ヘキサフルオロリン酸リチウムを1Mの濃度となるように溶解させたものを用いた。
得られた単一の二次電池セルに対して荷重付与機構を組み付け、0.25MPaの荷重が二次電池セル30(電極組立体12)に付与された状態とし、試料1の二次電池モジュールを得た。
試料2の二次電池モジュールは、負極活物質層における活物質の密度=1.2g/cm3、配向度=0.3、荷重付与機構による荷重=0.25MPaとなるように作製した。なお、試料2~5の二次電池モジュールは、負極活物質層における活物質の密度、配向度、及び荷重付与機構による荷重が異なるものの、作製手順は試料1の二次電池モジュールと同様であるので詳細な説明を省略する。
試料3の二次電池モジュールは、負極活物質層における活物質の密度=1.5g/cm3、配向度=0.07、荷重付与機構50による荷重=0.25MPaとなるように作製した。
試料4の二次電池モジュールは、負極活物質層における活物質の密度=1.2g/cm3、配向度=0.3、荷重付与機構50による荷重=0.1MPaとなるように作製した。
試料5の二次電池モジュールは、負極活物質層における活物質の密度=1.2g/cm3、配向度=0.3、荷重付与機構50による荷重=0.22MPaとなるように作製した。
試料6の二次電池モジュールは、第2の実施形態の二次電池モジュール、即ち複数の二次電池セルのうちの、第1端に配置された二次電池セルと第1拘束板との間、第2端に配置された二次電池セルと第2拘束板との間、及び隣合う二次電池セル間に板状の弾性部材が介在している二次電池モジュールである。そして、負極活物質層における活物質の密度=1.5g/cm3、配向度=0.07、荷重付与機構50による荷重=0.25MPaとなるように作製した。
試料7の二次電池モジュールも、第2の実施形態の二次電池モジュールと同じ構成の二次電池モジュールにおいて、負極活物質層における活物質の密度=1.2g/cm3、配向度=0.3、荷重付与機構50による荷重=0.22MPaとなるように作製した。
得られた試料1~7について、60℃の環境温度のもと、電圧範囲3.48V~3.93Vにおいて、1Cの電流レートによる放電及び充電を1回とするサイクルを規定サイクル行った。そして、初回サイクルにおける充電容量と規定サイクル後の充電容量とに基づき、下記式により与えられる容量維持率(%)を算出した。その結果を表1に示す。
規定サイクルとして600回の放電及び充電を行った試料1~7について、放電後に分解して負極電極を取り出し、ジメチルカーボネートで洗浄したのちに乾燥させてから、負極電極の膜厚を測定した。測定の結果、負極電極の膜厚が増加した試料については、活物質粒子の解れが生じたものと判定した。その結果を表2に示す。
Claims (9)
- 正極電極と負極電極とが相互に絶縁された状態で層状に重なっている電極組立体と、
前記電極組立体において前記正極電極及び前記負極電極が重なる方向から前記電極組立体に荷重を付与する荷重付与機構と、を備え、
前記負極電極は、金属箔と、該金属箔の少なくとも一部を覆い且つ活物質として炭素系材料を含む活物質層と、を有しており、
前記活物質層における前記炭素系材料の密度は1.2g/cm3以上であり、
前記活物質層における(100)面のX線の回折強度I(100)と(002)面のX線の回折強度I(002)との比(I(100)/I(002))によって与えられる配向度は0.3以下であり、
前記荷重付与機構が付与する荷重は0.2MPa以上である蓄電装置。 - 前記荷重付与機構が付与する荷重は0.22MPa以上である請求項1に記載の蓄電装置。
- 前記電極組立体は、前記正極電極と前記負極電極とが交互に積層された積層構造を有しており、
前記荷重付与機構は、前記電極組立体に荷重を付与する荷重付与面を有する請求項1又は請求項2に記載の蓄電装置。 - 前記電極組立体は、前記正極電極と前記負極電極との間に介在し、前記正極電極と前記負極電極とを相互に絶縁している多孔質のセパレータを備え、
前記荷重付与機構が付与する荷重は4MPa以下である請求項1~請求項3の何れか1項に記載の蓄電装置。 - 前記電極組立体を収容しているケースを備え、
前記荷重付与機構は、前記ケースの外部から荷重を付与するように構成されている請求項1~請求項4の何れか1項に記載の蓄電装置。 - 前記荷重付与機構は、複数の単位蓄電部の、前記ケースの前記正極電極と前記負極電極とが重なっている方向の両端に配置されている一対の拘束板を有し、
前記単位蓄電部と前記拘束板との間、及び隣合う前記単位蓄電部との間の少なくとも1箇所に板状の弾性部材が介在している請求項5に記載の蓄電装置。 - 前記電極組立体を収容しているケースを備え、
前記荷重付与機構は、単位蓄電部の前記ケースの内部に設けられ、前記ケースの前記正極電極と前記負極電極とが重なっている方向の壁と、前記電極組立体との間に介在する厚み調節材である請求項1~請求項4の何れか1項に記載の蓄電装置。 - ケースと該ケースに収容された前記電極組立体とを有する複数の単位蓄電部を備え、前記単位蓄電部は、前記重なる方向に沿って列状に並んでおり、前記荷重付与機構は、前記重なる方向における前記複数の単位蓄電部の両端から荷重を付与する請求項1~請求項4の何れか1項に記載の蓄電装置。
- 前記炭素系材料は、黒鉛である請求項1~請求項8の何れか1項に記載の蓄電装置。
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JP2018129132A (ja) * | 2017-02-06 | 2018-08-16 | トヨタ自動車株式会社 | 組電池 |
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WO2020134747A1 (zh) * | 2018-12-29 | 2020-07-02 | 宁德时代新能源科技股份有限公司 | 电池模组以及电池包 |
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