Battery pack and device including the battery pack

Abstract

A battery pack according to an embodiment of the present invention includes: a pack frame on which a plurality of battery modules are mounted; an internal frame located inside the pack frame and partitioning the plurality of battery modules from each other; and at least one lifting portion located between the internal frame and the upper portion of the pack frame, wherein at least one of the lifting portions is deformed according to the temperature inside the pack frame.

Description

Technical Field

[0001] The present invention relates to a battery pack and a device including the battery pack, and more specifically, to a battery pack capable of maintaining the structure of the battery pack when a thermal runaway or heat propagation phenomenon occurs inside the battery pack, and a device including the battery pack.

Background Art

[0002] Secondary batteries, which are highly applicable to a wide range of products and have electrical characteristics such as high energy density, are widely used not only in portable devices but also in electric vehicles or hybrid vehicles driven by an electric drive source, and power storage devices. Such secondary batteries are attracting attention as a new energy source for environmental friendliness and energy efficiency improvement not only because they can significantly reduce the use of fossil fuels but also because they do not generate any by-products during energy use.

[0003] Currently, commercially available secondary batteries include nickel-cadmium batteries, nickel-metal hydride batteries, nickel-zinc batteries, and lithium secondary batteries. Among them, lithium secondary batteries have attracted attention for their advantages such as almost no memory effect compared to nickel-based secondary batteries, free charge and discharge, very low self-discharge rate, and high energy density.

[0004] Generally, lithium secondary batteries can be classified into cylindrical or square secondary batteries in which an electrode assembly is installed inside a metal can, and pouch-type secondary batteries in which an electrode assembly is installed inside a pouch of an aluminum laminate sheet according to the shape of the exterior material.

[0005] In recent years, with the utilization of secondary batteries as energy storage sources and the increasing demand for large-capacity secondary battery structures, the demand for battery packs with a medium- to large-sized module structure formed by aggregating a number of battery modules connected in series or parallel has been increasing. Such battery modules are formed by connecting a number of battery cells in series or parallel with each other to form a battery cell stack, thereby improving the capacity and output. In addition, a plurality of battery modules can be mounted together with various control and protection systems such as a BMS (Battery Management System) and a cooling system to form a battery pack.

[0006] Since the battery pack is configured with a structure in which a number of battery modules are combined, if some of the battery modules are overvoltage, overcurrent or overheat, the safety and operating efficiency of the battery pack may become a problem. In particular, in order to improve the driving range, the capacity of the battery pack tends to gradually increase, and accordingly, as the energy inside the pack also increases, it is necessary to design a structure that meets the strengthened safety standards and ensures the safety of the vehicle and the driver.

[0007] In connection with this, when a thermal runaway and a heat propagation phenomenon between battery cells occur in the battery pack, deformation of the components of the battery pack may occur due to the high-temperature gas and particles inside the battery pack. In particular, in such a high-temperature environment, the structure of the battery pack may be changed, such as the lead (Lid), which is the upper pack frame of the battery pack, sagging in the direction of gravity, which may cause a problem that the upper vent flow path of the battery pack is clogged. If the upper vent flow path of the battery pack is clogged in this way, there is a problem that the discharge of the high-temperature gas and particles inside the battery pack is delayed, which may lead to an explosion and a fire of the battery pack. Therefore, in order to prevent such a situation, there is a need to develop a battery pack that can prevent the upper ventilation flow path of the battery pack from being clogged and minimize the damage even when a thermal runaway or a heat propagation phenomenon occurs inside the battery pack.

Summary of the Invention

Problems to be Solved by the Invention

[0008] The problem to be solved by the present invention is to provide a battery pack capable of maintaining the structure of the battery pack and a device including the battery pack when a thermal runaway or heat propagation phenomenon occurs inside the battery pack.

[0009] The problem to be solved by the present invention is not limited to the above-described problems, and problems not mentioned should be clearly understood by those having ordinary knowledge in the technical field to which the present invention pertains from this specification and the attached drawings.

Means for Solving the Problem

[0010] A battery pack according to an embodiment of the present invention includes a pack frame on which a plurality of battery modules are mounted; an internal frame located inside the pack frame and partitioning the plurality of battery modules from each other; and at least one lifting portion located between the internal frame and the upper portion of the pack frame, and at least one of the lifting portions is deformed according to the temperature inside the pack frame.

[0011] The lifting portion may include a lifting member that bends in a direction toward the upper portion of the pack frame when the temperature inside the pack frame rises.

[0012] The lifting portion may further include at least one fixing member that fixes the lifting member to the internal frame.

[0013] The fixing member is a bolting member, and the lifting member and the internal frame may be bolted together.

[0014] The lifting member may be configured such that a portion located between portions fixed by the fixing member bends in a direction toward the upper portion of the pack frame.

[0015] The lifting member can extend along the width direction of the battery module.

[0016] The inner frame includes at least one horizontal beam extending along the width direction of the battery module and at least two vertical beams extending along the length direction of the battery module, and at least one of the lifting portions can extend along the same direction as the horizontal beam.

[0017] At least one of the lifting portions includes a pair of lifting portions spaced apart from each other, and the pair of lifting portions can be located between the horizontal beam and one side surface of the lower pack frame facing the horizontal beam.

[0018] At least one of the lifting portions is located on at least two of the vertical beams, and the fixing member can fix the lifting member to each of the at least two vertical beams.

[0019] The lifting member can have a shape in which an upper portion of the lifting member is composed of more material than a lower portion of the lifting member relatively.

[0020] The lifting member can have a cross section of one of a V shape, a U shape, a T shape, an inverted triangle shape, and a semicircle shape.

[0021] The lifting member can be composed of steel.

[0022] A device according to another embodiment of the present invention includes the battery pack described above.

Advantages of the Invention

[0023] According to an embodiment, the battery pack of the present invention and a device including the battery pack include a lifting member between an upper pack frame and an inner frame of the battery pack, and can maintain the structure of the battery pack when a thermal runaway or heat propagation phenomenon occurs inside the battery pack.

[0024] The effects of the present invention are not limited to the effects described above, and the effects not mentioned will be clearly understood by those having ordinary knowledge in the technical field to which the present invention pertains from the present specification and the attached drawings.

Brief Description of the Drawings

[0025]

Figure 1

Figure 2

Figure 3

Figure 4

Figure 5

Figure 6

Figure 7

Modes for Carrying Out the Invention

[0026] Hereinafter, with reference to the accompanying drawings, various embodiments of the present invention will be described in detail so that those having ordinary knowledge in the technical field to which the present invention pertains can easily implement them. The present invention can be implemented in several different forms and is not limited to the embodiments described herein.

[0027] To clearly explain the present invention, parts not related to the explanation are omitted, and the same reference numerals are used for the same or similar components throughout the specification.

[0028] In addition, the sizes and thicknesses of the respective components shown in the drawings are arbitrarily shown for the convenience of explanation, and the present invention is not necessarily limited to what is shown in the drawings. In the drawings, the thickness is enlarged to clearly represent a plurality of layers and regions. And, in the drawings, for the convenience of explanation, the thicknesses of some layers and regions are exaggerated.

[0029] Also, throughout the specification, when a certain part "includes" a certain component, this means that, unless otherwise stated to the contrary, it does not exclude other components, but can further include other components.

[0030] Also, throughout the specification, "on a plane" means when the target part is viewed from above, and "in a cross-section" means when the cross-section obtained by vertically cutting the target part is viewed from the side.

[0031] Hereinafter, a battery pack according to an embodiment of the present invention will be described.

[0032] FIG. 1 is a perspective view showing a battery pack according to an embodiment of the present invention. FIG. 2 is an exploded perspective view of the components included in the battery pack of FIG. 1. FIG. 3 is a perspective view showing the structure of the battery pack of FIG. 1 with the upper pack frame and a plurality of battery modules removed.

[0033] Referring to FIGS. 1 and 2, a battery pack according to an embodiment of the present invention includes pack frames 1100 and 1200 on which a plurality of battery modules are mounted, and an internal frame 1300 located inside the pack frames 1100 and 1200 and partitioning the plurality of battery modules 100 from each other.

[0034] Here, the pack frames 1100 and 1200 can include a lower pack frame 1100 on which a plurality of battery modules 100 are mounted and an upper pack frame 1200 located above the battery modules 100. More specifically, the upper pack frame 1200 can cover the upper part of the lower pack frame 1100 with a plurality of battery modules 100 mounted on the lower pack frame 1100. Here, the lower pack frame 1100 and the upper pack frame 1200 can be joined by a method such as welding or adhesion at the surfaces in contact with each other to seal the inside of the battery pack 1000.

[0035] Referring to FIGS. 1 to 3, the lower pack frame 1100 can include an outer frame 1110 extending from the bottom surface of the pack frames 1100 and 1200 toward the upper pack frame 1200 and a pack bottom 1150 facing the lower surface of the battery module 100. That is, the outer frame 1110 can extend from the pack bottom 1150 toward the upper pack frame 1200.

[0036] In the lower pack frame 1100, the outer frame 1110 and the pack bottom 1150 can be integrated with each other or fixed by a separate fastening method such as welding or adhesion.

[0037] As an example, the outer frame 1110 can be made of a heat insulating member. As another example, the outer frame 1110 can be made of a dissimilar metal bonding material such as clad metal, or can be a structure containing a heat insulating material such as aerogel or EPP (Expanded Polypropylenes) foam. As another example, the outer frame 1110 can be a structure containing materials such as silicon foam, mica, or a glass fiber pad. However, it is not limited thereto, and the outer frame 1110 can be used without limitation as long as it is made of a heat insulating material having a predetermined rigidity.

[0038] Further, the lower pack frame 1100 can be located inside the outer frame 1110 and include an inner frame 1300 extending from the pack bottom 1150 to the upper pack frame 1200. More specifically, the inner frame 1300 includes at least one horizontal beam 1310 and at least two vertical beams 1350.

[0039] The horizontal beam 1310 can extend along the width direction (x-axis direction) of the battery module 100. Also, the vertical beam 1350 is located between one side surface of the outer frame 1110 and the horizontal beam 1310 and can extend along the length direction (y-axis direction) of the battery module 100. Here, one side surface of the outer frame 1110 can mean the side surface of the outer frame 1110 facing the horizontal beam 1310.

[0040] The plurality of battery modules 100 can be partitioned from each other by at least one horizontal beam 1310 and at least two vertical beams 1350. That is, the inner space partitioned by at least one horizontal beam 1310 and at least two vertical beams 1350 can be a module area where the battery modules 100 are respectively mounted, and can be an area where other electrical components are mounted in addition to the battery modules 100.

[0041] However, the configuration of the inner frame 1300 is not limited to this, and any form that can partition and mount the plurality of battery modules 100 from each other can be included in this embodiment. Also, the length, interval, number, etc. of at least one horizontal beam 1310 and at least two vertical beams 1350 can be adjusted according to the size and arrangement form of the battery module 100.

[0042] As an example, the internal frame 1300 can be composed of a heat insulating member. As another example, the internal frame 1300 can be composed of a dissimilar metal joining material such as clad metal, or can be a structure containing a heat insulating material such as aerogel or EPP (Expanded Polypropylenes) foam. As another example, the internal frame 1300 can be a structure containing materials such as silicon foam, mica, or a glass fiber pad. However, it is not limited to this. As long as the internal frame 1300 is composed of a heat insulating material having a predetermined rigidity, it can be used without limitation.

[0043] Accordingly, in the battery pack 1000 according to the present embodiment, the lower pack frame 1100 can be positioned separately because a plurality of battery modules 100 are partitioned from each other by the outer frame 1110 and the inner frame 1300. Even if a fire occurs in some of the plurality of battery modules 100, the heat propagation phenomenon between adjacent battery modules 100 can be effectively prevented.

[0044] Referring to FIG. 2, the battery pack 1000 according to the present embodiment can include a plurality of battery modules 100. Here, the battery module 100 can be mounted on the lower pack frame 1100. More specifically, the plurality of battery modules 100 can be respectively mounted in the regions partitioned by the outer frame 1110 and the inner frame 1300 as shown in FIGS. 2 and 3. However, the arrangement direction of the battery module 100 is not limited to this and can be appropriately changed as needed.

[0045] As an example, the battery module 100 includes a battery cell stack (not shown) in which a plurality of battery cells are stacked, and a module frame (not shown) that houses the battery cell stack (not shown).

[0046] The battery cell is preferably a pouch-type battery cell. As an example, the battery cell can be manufactured by housing an electrode assembly in a pouch case of a laminate sheet including a resin layer and a middle layer, and then heat-sealing the sealing portion of the pouch case. The battery cell can be formed in a rectangular sheet-like structure. The battery cell can be composed of a plurality of battery cells, and the plurality of battery cells are stacked so as to be electrically connected to each other to form a battery cell stack (not shown). Here, the number of battery cells constituting the battery cell stack (not shown) can be adjusted according to the case.

[0047] The module frame (not shown) can include an upper cover and a U-shaped frame. Here, the U-shaped frame can include a bottom portion and two side portions extending upward from both end portions of the bottom portion. At this time, the bottom portion can cover the lower surface of the battery cell stack (not shown), and the side portions can cover the side surface of the battery cell stack (not shown). The upper cover and the U-shaped frame can be joined by welding or the like in a state where the corner portions corresponding to each other are in contact with each other to form a structure that covers the top, bottom, left, and right of the battery cell stack (not shown). Therefore, the upper cover and the U-shaped frame can be made of a metal material having a predetermined strength.

[0048] However, the structure of the module frame (not shown) is not limited to this. As another example, the module frame (not shown) may have a monoframe structure. Here, the monoframe may be in the form of a metal plate material in which the upper surface, the lower surface, and both side surfaces are integrated. The monoframe can be manufactured by extrusion molding. Also, the structure of the module frame (not shown) may be provided in the form of an L-shaped frame in addition to the monoframe or the U-shaped frame, and may be provided in various structures not described in the above examples.

[0049] In addition, the battery module 100 further includes a bus bar frame positioned on the front and rear surfaces of a battery cell laminate (not shown) and an end plate covering the bus bar frame. Here, a bus bar (not shown) electrically connected to the battery cell laminate (not shown) can be positioned on the bus bar frame. Thereby, the end plate can physically protect the battery cell laminate (not shown) and other electrical components from external impacts.

[0050] Hereinafter, the lifting portion 1400 included in the battery pack 1000 according to an embodiment of the present invention will be mainly described.

[0051] Referring to FIGS. 2 to 3, the battery pack 1000 according to an embodiment of the present invention may include at least one lifting portion 1400 positioned between the internal frame 1300 and the upper portions of the pack frames 1100 and 1200. More specifically, at least one lifting portion 1400 can be positioned between the internal frame 1300 and the upper pack frame 1200. That is, at least one lifting portion 1400 can be positioned in a space where the internal frame 1300 and the upper pack frame 1200 are separated from each other.

[0052] At least one lifting portion 1400 can extend along the width direction (x-axis direction) of the battery module 100. More specifically, at least one lifting portion 1400 can extend along the same direction (x-axis direction) as the horizontal beam 1310. Here, the lifting portion 1400 can extend between one side surface and the other side surface of the outer frames 1110 facing each other of the lower pack frame 1100.

[0053] As an example, at least one lifting part 1400 can include a pair of lifting parts 1400 as shown in FIGS. 2 and 3. Here, the pair of lifting parts 1400 can be located between the horizontal beam 1310 and one side surface of the lower pack frame 1100 facing the horizontal beam 1310. Also, the pair of lifting parts 1400 can be spaced apart from each other.

[0054] However, the number and arrangement of the lifting parts 1400 are not limited thereto, and any number and / or arrangement that can prevent the sagging of the upper pack frame 1200 of the battery pack 1000 when a thermal runaway occurs inside the battery pack 1000 can be included in this embodiment.

[0055] The lifting part 1400 can include a lifting member 1410 that bends in a direction toward the upper part of the pack frames 1100 and 1200 when the temperature inside the pack frames 1100 and 1200 rises. More specifically, the lifting member 1410 may be a material whose length expands when the temperature inside the pack frames 1100 and 1200 rises. Also, as will be described later, by fixing the lifting member 1410 to the internal frame 1300 by the fixing member 1450, the lifting member 1410 can bend toward the upper pack frame 1200 when its length expands.

[0056] As an example, the lifting member 1410 may be a material that expands at a temperature from room temperature to 1500 degrees Celsius or less. Here, the room temperature means a temperature of 15 degrees Celsius to 25 degrees Celsius and can have the same meaning as the generally used room temperature.

[0057] Thereby, in the battery pack 1000 according to this embodiment, within the temperature range from room temperature, which is the usage environment of a general battery pack 1000, to the high temperature environment where a thermal runaway phenomenon occurs inside the battery pack 1000, the upper pack frame 1200 can be supported, and it is possible to prevent the occurrence of a sagging phenomenon due to the structural deformation of the upper pack frame 1200.

[0058] The lifting member 1410 can extend along the width direction (x-axis direction) of the battery module 100. More specifically, the lifting member 1410 can extend along the same direction (x-axis direction) as the horizontal beam 1310. Here, the lifting member 1410 can extend between one side surface and the other side surface of the outer frame 1110 at positions facing each other of the lower pack frame 1100.

[0059] As shown in FIGS. 2 and 3, the lifting member 1410 can include a pair of lifting members 1410. Here, the pair of lifting members 1410 can be located between the horizontal beam 1310 and one side surface of the lower pack frame 1100 facing the horizontal beam 1310. Also, the pair of lifting members 1410 can be spaced apart from each other.

[0060] However, the number and arrangement of the lifting members 1410 are not limited thereto, and any number and / or arrangement that can prevent the upper pack frame 1200 of the battery pack 1000 from sagging when a thermal runaway occurs inside the battery pack 1000 can be included in this embodiment.

[0061] FIG. 4 is a drawing showing the shape of the lifting member included in the battery pack of FIG. 1. The lifting member 1410 can have a shape in which the upper part of the lifting member 1410 has relatively more material than the lower part. In other words, the lifting member 1410 has a shape in which, with respect to the vertical direction of the lifting member 1410, the upper part of the lifting member 1410 has a relatively larger area than the lower part of the lifting member 1410. As an example, as shown in FIG. 4, the lifting member 1410 can have a cross-section of one of a V shape, a U shape, a T shape, an inverted triangle shape, and a semi-circular shape.

[0062] As a result, the lifting member 1410 can bend towards the portion with relatively more material in the high-temperature environment due to the temperature rise inside the battery pack 1000. In other words, the lifting member 1410 can bend towards the upper part, which is a relatively wide area, with respect to the vertical direction of the lifting member 1410. That is, the lifting member 1410 can bend towards the upper side of the lifting member 1410, that is, the lifting member 1410 can bend in the direction towards the upper pack frame 1200.

[0063] However, the shape of the lifting member 1410 is not limited thereto, and any shape that can bend towards the upper parts of the pack frames 1100 and 1200 in the high-temperature environment due to the temperature rise inside the battery pack 1000 can be included in this embodiment.

[0064] As an example, the lifting member 1410 can be made of steel. However, it is not limited thereto, and any material that has heat resistance and can bend towards the upper parts of the pack frames 1100 and 1200 in the high-temperature environment due to the temperature rise inside the battery pack 1000 can be included in this embodiment.

[0065] FIG. 5 is a drawing showing a part of a cross-section cut along the a-a' axis of FIG. 3.

[0066] Referring to FIGS. 3 to 5, the lifting part 1400 can include at least one fixing member 1450 for fixing the lifting member 1410 to the inner frame 1300. More specifically, at least one fixing member 1450 is disposed at each position where the lifting member 1410 and the inner frame 1300 are in contact with each other, and the lifting member 1410 and the inner frame 1300 can be fixed to each other. As an example, as shown in FIG. 3, at least one lifting member 1410 is located on at least two vertical beams 1350, and at least one fixing member 1450 can fix at least one lifting member 1410 to each of the at least two vertical beams 1350. That is, in the battery pack 1000 according to the present embodiment, the lifting member 1410 may not be fixed to the upper pack frame 1200.

[0067] As an example, the fixing member 1450 is a bolting member, and the lifting member 1410 and the inner frame 1300 can be bolted together. However, the connection method and form of the fixing member 1450 are not limited to this, and any method and form that can fix the lifting member 1410 to the inner frame 1300 can be included in this embodiment.

[0068] FIGS. 6 and 7 are drawings showing a part of a cross section cut along the b-b' axis of FIG. 3.

[0069] Referring to FIGS. 5 and 6, the lifting part 1400 may not undergo structural deformation in the normal state of the battery pack 1000. In contrast, when the temperature inside the pack frames 1100 and 1200 rises, as shown in FIG. 7, the lifting part 1400 can bend in the direction toward the upper parts of the pack frames 1100 and 1200. That is, the lifting part 1400 can bend in the direction toward the upper pack frame 1200.

[0070] That is, the lifting member 1410 can expand in the length direction in a high-temperature environment due to the temperature rise inside the battery pack 1000. Here, since a part of the lifting member 1410 is fixed to the inner frame 1300 by the fixing member 1450, the lifting member 1410 can bend toward the upper pack frame 1200 by expanding in the length direction.

[0071] More specifically, in the lifting member 1410, the portion located between the portions fixed by the fixing member 1450 can bend in the direction toward the upper parts of the pack frames 1100 and 1200. That is, in the lifting member 1410, the portion located between the portions fixed by the fixing member 1450 can bend in the direction toward the upper pack frame 1200.

[0072] Thereby, in the battery pack 1000 according to the present embodiment, the direction in which the lifting part 1400 bends is induced in the direction toward the upper pack frame 1200, the lifting part 1400 can support the upper pack frame 1200, and the structural rigidity of the battery pack 1000 can be increased.

[0073] At the same time, the lifting part 1400 prevents the occurrence of a sagging phenomenon due to the structural deformation of the upper pack frame 1200, and the lifting part 1400 can prevent the gas venting flow path formed between the upper pack frame 1200 and the plurality of battery modules 100 from being blocked. That is, in the battery pack 1000 according to the present embodiment, even when a thermal runaway phenomenon occurs inside the battery pack 1000, the gas generated inside the battery pack 1000 can be easily discharged to the outside, and additional heat propagation or explosion situations can be prevented or delayed.

[0074] A device according to another embodiment of the present invention includes the battery pack described above. Such a device is applicable to transportation means such as electric bicycles, electric vehicles, and hybrid vehicles, but the present invention is not limited thereto, and is applicable to various devices that can use the battery module and the battery pack including the battery pack, which also belongs to the scope of the present invention.

[0075] As described above, the preferred embodiments of the present invention have been described in detail. However, the scope of the present invention is not limited thereto, and various modifications and improvements by those skilled in the art using the basic concept of the present invention defined in the claims also belong to the scope of the present invention.

Description of Reference Numerals

[0076] 100 Battery Module 1000 Battery Pack 1100 Lower Pack Frame 1200 Upper Pack Frame 1300 Inner Frame 1400 Lifting Portion 1410 Lifting Member 1450 Fixing Member

Claims

1. A pack frame with a plurality of battery modules mounted thereon; An internal frame located inside the pack frame and partitioning the plurality of battery modules from each other; and At least one lifting portion located between the internal frame and the upper portion of the pack frame, wherein at least one of the lifting portions is a battery pack that is deformed according to the temperature inside the pack frame.

2. The battery pack according to claim 1, wherein the lifting portion includes a lifting member that bends in a direction toward the upper portion of the pack frame when the temperature inside the pack frame rises.

3. The battery pack according to claim 2, wherein the lifting portion further includes at least one fixing member for fixing the lifting member to the internal frame.

4. The fixing member is a fastening member, and the battery pack according to claim 3, wherein the lifting member and the internal frame are fastened and coupled.

5. The battery pack according to claim 3, wherein the lifting member is configured such that a portion located between portions fixed by the fixing member bends in a direction toward the upper portion of the pack frame.

6. The battery pack according to claim 3, wherein the lifting member extends along the width direction of the battery module.

7. The internal frame includes at least one horizontal beam extending along the width direction of the battery module and at least two vertical beams extending along the length direction of the battery module, and the battery pack according to claim 6, wherein at least one of the lifting portions extends along the same direction as the horizontal beam.

8. At least one of the lifting portions includes a pair of lifting portions spaced apart from each other, and the battery pack according to claim 7, wherein the pair of lifting portions is located between the horizontal beam and one side surface of the lower pack frame facing the horizontal beam.

9. At least one of the lifting portions is located on at least two of the vertical beams, and the battery pack according to claim 7, wherein the fixing member fixes the lifting member to each of the at least two vertical beams.

10. The battery pack according to claim 1, wherein the lifting member has a shape in which an upper portion of the lifting member is composed of more material than a lower portion of the lifting member relatively.

11. The battery pack according to claim 10, wherein the lifting member has a cross section of one of a V shape, a U shape, a T shape, an inverted triangle shape, and a semicircle shape.

12. The battery pack according to claim 1, wherein the lifting member is made of steel.

13. A device including the battery pack according to any one of claims 1 to 12.

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