KR101115913B1 - Copper foil for current collector of lithium secondary battery - Google Patents

Copper foil for current collector of lithium secondary battery Download PDF

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KR101115913B1
KR101115913B1 KR1020090037039A KR20090037039A KR101115913B1 KR 101115913 B1 KR101115913 B1 KR 101115913B1 KR 1020090037039 A KR1020090037039 A KR 1020090037039A KR 20090037039 A KR20090037039 A KR 20090037039A KR 101115913 B1 KR101115913 B1 KR 101115913B1
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copper foil
secondary battery
lithium secondary
current collector
tensile strength
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KR20100118288A (en
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김대영
최승준
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엘에스엠트론 주식회사
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • 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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  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Cell Electrode Carriers And Collectors (AREA)

Abstract

본 발명은 Lab 표색계 기준으로 동박표면의 L값이 85 ~ 90, a값이 12 ~ 18이고, 매트면(Matte Side)의 표면조도(Rzjis)가 1.5㎛ 이하이고, 인장강도가 30~40kgf/㎟이며, 180℃에서 5분 동안 열처리한 이후에 인장강도의 저하율이 10% 이하이고, 연신율이 3~20%이고, 동박두께가 1~35㎛인 것을 특징으로 하는 리튬 이자전지 집전체용 동박을 개시한다.According to the present invention, the L value of the copper foil surface is 85 to 90, the a value is 12 to 18, the surface roughness (R zjis ) of the mat surface is 1.5 µm or less, and the tensile strength is 30 to 40 kgf. / Mm2, and after heat treatment at 180 DEG C for 5 minutes, the decrease in tensile strength is 10% or less, the elongation is 3 to 20%, and the copper foil thickness is 1 to 35 µm. Start copper foil.

집전체, 동박, Lab 표색계, 매트면, 표면조도, 인장강도, 연신율 Current collector, copper foil, Lab colorimeter, mat surface, surface roughness, tensile strength, elongation

Description

리튬 이차전지의 집전체용 동박{COPPER FOIL FOR CURRENT COLLECTOR OF LITHIUM SECONDARY BATTERY}Copper foil for current collector of lithium secondary battery {COPPER FOIL FOR CURRENT COLLECTOR OF LITHIUM SECONDARY BATTERY}

본 발명은 리튬 이차전지의 집전체로 사용되는 동박에 관한 것으로서, 더욱 상세하게는 활물질을 균일하게 코팅할 수 있는 표면 구조를 가진 리튬 이차전지의 집전체용 동박에 관한 것이다.The present invention relates to a copper foil used as a current collector of a lithium secondary battery, and more particularly, to a current collector copper foil of a lithium secondary battery having a surface structure capable of uniformly coating an active material.

리튬 이차전지는 여타의 이차전지에 비해 상대적으로 에너지 밀도가 높고, 작동전압이 높을 뿐만 아니라 우수한 보존 및 수명특성을 보이는 등 많은 장점이 있어 개인용 컴퓨터, 캠코더, 휴대용 전화기, 휴대용 CD 플레이어, PDA 등 각종 휴대용 전자기기에 널리 사용되고 있다.Lithium secondary battery has many advantages such as high energy density, high operating voltage and excellent storage and lifespan characteristics compared to other secondary batteries, which can be used for personal computers, camcorders, portable phones, portable CD players, PDAs, etc. Widely used in portable electronic devices.

일반적으로 리튬 이차전지는 전해질을 사이에 두고 배치된 양극 및 음극과, 상기 양극과 음극에 각각 포함된 양극 활물질 및 음극 활물질과, 상기 양극 활물질과 음극 활물질에 각각 접촉하는 양극 집전체 및 음극 집전체를 구비한 구조를 갖는다.In general, a lithium secondary battery includes a positive electrode and a negative electrode disposed with an electrolyte interposed therebetween, a positive electrode active material and a negative electrode active material included in the positive electrode and the negative electrode, and a positive electrode current collector and a negative electrode current collector in contact with the positive electrode active material and the negative electrode active material, respectively. It has a structure provided with.

리튬 이차전지에 있어서 음극 집전체의 소재로는 주로 동박이 사용되며, 통상적으로 이 동박에는 카본(Carbon)계 슬러리의 활물질이 코팅된다. 여기서, 동박 은 전기 도금법으로 전해동박을 제조하는 제박공정과 원박에 박리강도(Peel strength) 등을 부여하기 위한 후처리 공정을 통하여 제조된다. 전기도금에 의해 전해동박의 일면에는 상대적으로 조도가 낮아 광택이 나는 샤이니 면(Shiny side)이 형성되고, 타면에는 이른바, 산(Mountain) 구조에 의해 상대적으로 조도가 높으며 광택이 나지 않는 매트면(Matte Side)이 형성된다. 또한, 전해동박은 후처리 공정에서 매트면에 구리 노듈 클러스터(Cu-Nodule Cluster)를 형성하는 표면처리를 거침으로써 집전체로서 적합한 물리적, 화학적 특성이 부여된다.In the lithium secondary battery, copper foil is mainly used as a material of the negative electrode current collector, and typically, the copper foil is coated with an active material of a carbon-based slurry. Here, the copper foil is manufactured through a process for producing an electrolytic copper foil by an electroplating method and a post-treatment process for imparting peel strength to the original foil. The electroplated copper foil has a relatively low roughness on one surface and forms a shiny shiny side. On the other side, a so-called mountain structure has a relatively high roughness and a matt surface that is not glossy. Side is formed. In addition, the electrolytic copper foil undergoes a surface treatment of forming a copper nodule cluster on a mat surface in a post-treatment process to impart physical and chemical properties suitable as a current collector.

리튬 이차전지는 집전체로 사용되는 동박의 표면 상태에 따라 전지특성이 크게 변하므로 수율의 향상을 위해서는 동박의 표면 특성을 개선하는 것이 매우 중요하다.Since the lithium secondary battery greatly changes the battery characteristics depending on the surface state of the copper foil used as the current collector, it is very important to improve the surface characteristics of the copper foil in order to improve the yield.

특히, 동박의 표면조도(Surface Roughness)가 불필요하게 높거나 전기도금공정에서 첨가제가 적정하게 첨가되지 않았을 경우 표면형상의 불균일로 인해 그래파이트(Graphite) 등과 같은 활물질의 코팅이 균일하게 이루어지지 않는다. 동박 표면에 활물질이 불균일하게 코팅되면 충,방전시 단락이 발생하거나 동박으로부터 활물질이 박리되는 현상이 발생하여 수율 저하를 초래하게 된다.In particular, when the surface roughness of the copper foil is unnecessarily high or when the additive is not properly added in the electroplating process, coating of an active material such as graphite is not uniform due to surface irregularities. If the active material is unevenly coated on the surface of the copper foil, a short circuit occurs during charging and discharging, or a phenomenon in which the active material is peeled from the copper foil occurs, resulting in a decrease in yield.

본 발명은 상기와 같은 문제점을 해결하기 위해 창안된 것으로서, 활물질의 균일한 코팅이 가능한 표면구조를 제공하도록 Lab 표색계 범위가 정의된 리튬 이차전지 집전체용 동박을 제공하는 데 그 목적이 있다.The present invention has been made to solve the above problems, an object of the present invention is to provide a copper secondary battery collector copper foil is defined in the range of the lab color system to provide a surface structure capable of uniform coating of the active material.

본 발명의 다른 목적은 집전체로 사용되기에 적합한 물성이 부여되도록 표면조도, 인장강도, 연신율, 두께 등의 인자가 최적화된 리튬 이차전지 집전체용 동박을 제공하는 데 있다.Another object of the present invention to provide a copper foil for a lithium secondary battery current collector is optimized for the factors such as surface roughness, tensile strength, elongation, thickness so as to impart suitable physical properties to be used as the current collector.

상기와 같은 목적을 달성하기 위해 본 발명에 따른 리튬 이차전지 집전체용 동박은, Lab 표색계 기준으로 동박표면의 L값이 85 ~ 90, a값이 12 ~ 18인 것을 특징으로 한다.In order to achieve the above object, the copper foil for a lithium secondary battery current collector according to the present invention is characterized in that the L value of the copper foil surface is 85 to 90 and the a value is 12 to 18 based on a lab colorimeter.

상기 동박의 매트면(Matte Side)의 표면조도(Rzjis)는 1.5㎛ 이하인 것이 바람직하다.It is preferable that the surface roughness Rzjis of the mat side of the said copper foil is 1.5 micrometers or less.

인장강도가 30~40kgf/㎟이며, 180℃에서 5분 동안 열처리한 이후에 인장강도의 저하율이 10% 이하인 것이 바람직하다.It is preferable that the tensile strength is 30-40 kgf / mm 2, and the rate of decrease of the tensile strength is 10% or less after heat treatment at 180 ° C. for 5 minutes.

상기 동박의 연신율은 3~20%인 것이 바람직하다.It is preferable that the elongation of the said copper foil is 3 to 20%.

상기 동박의 두께는 1~35㎛인 것이 바람직하다.It is preferable that the thickness of the said copper foil is 1-35 micrometers.

본 발명에 따르면 활물질의 코팅 시 균일한 코팅면이 형성될 수 있는 표면 구조를 가진 리튬 이차전지 집전체용 동박이 제공된다. 따라서, 리튬 이차전지의 충,방전 시 단락의 발생을 방지할 수 있으며, 활물질과의 접촉 시 밀착력이 충분히 확보되어 박리강도가 우수하므로 리튬 이차전지의 용량을 안정적으로 유지할 수 있다.According to the invention there is provided a copper foil for a lithium secondary battery current collector having a surface structure capable of forming a uniform coating surface when coating the active material. Therefore, the occurrence of a short circuit during charging and discharging of the lithium secondary battery can be prevented, and the adhesion strength is sufficiently secured upon contact with the active material, so that the peeling strength is excellent, so that the capacity of the lithium secondary battery can be stably maintained.

이하, 첨부된 도면을 참조하여 본 발명의 바람직한 실시예를 상세히 설명하기로 한다. 이에 앞서, 본 명세서 및 청구범위에 사용된 용어나 단어는 통상적이거나 사전적인 의미로 한정해서 해석되어서는 아니되며, 발명자는 그 자신의 발명을 가장 최선의 방법으로 설명하기 위해 용어의 개념을 적절하게 정의할 수 있다는 원칙에 입각하여 본 발명의 기술적 사상에 부합하는 의미와 개념으로 해석되어야만 한다. 따라서, 본 명세서에 기재된 실시예와 도면에 도시된 구성은 본 발명의 가장 바람직한 일 실시예에 불과할 뿐이고 본 발명의 기술적 사상을 모두 대변하는 것은 아니므로, 본 출원시점에 있어서 이들을 대체할 수 있는 다양한 균등물과 변형예들이 있을 수 있음을 이해하여야 한다.Hereinafter, exemplary embodiments of the present invention will be described in detail with reference to the accompanying drawings. Prior to this, terms or words used in the specification and claims should not be construed as having a conventional or dictionary meaning, and the inventors should properly explain the concept of terms in order to best explain their own invention. Based on the principle that can be defined, it should be interpreted as meaning and concept corresponding to the technical idea of the present invention. Therefore, the embodiments described in the specification and the drawings shown in the drawings are only the most preferred embodiment of the present invention and do not represent all of the technical idea of the present invention, various modifications that can be replaced at the time of the present application It should be understood that there may be equivalents and variations.

본 발명에 따른 리튬 이차전지 집전체용 동박은 Lab 표색계, 표면조도, 인장강도, 연신율 등의 인자가 최적화되어 집전체로 사용되기에 적합한 표면특성과 인장 특성이 부여된다.Copper foil for a lithium secondary battery current collector according to the present invention is optimized by the factors such as Lab color system, surface roughness, tensile strength, elongation is given a surface property and tensile properties suitable for use as a current collector.

바람직하게, 본 발명에 따른 리튬 이차전지 집전체용 동박은 황산동을 전해액으로 하고, 도금 표면에 광택이 나도록 하는 Brighter나 도금 범위를 넓혀주는 Leveler, 도금이 고르게 진행되도록 하는 Suppresser 등과 같은 첨가제를 첨가하여 30 ~ 80ASD(A/dm2)의 전류밀도로 제박기의 드럼 표면에 구리를 전착하여 원박을 제조하고, 방청처리를 위해 동박 표면을 크로메이트(Chromate) 처리하는 공정을 거쳐 제조된다.Preferably, the copper foil for the current collector of the lithium secondary battery according to the present invention, by using copper sulfate as an electrolyte, by adding additives such as a brighter to shine on the surface of the plating, a leveler to broaden the plating range, and a suppresser to evenly proceed the plating. A copper foil is prepared by electrodepositing copper on a drum machine's drum surface with a current density of 30 to 80 ASD (A / dm 2 ), and is manufactured through a process of chromate treating the copper foil surface for rust prevention treatment.

동박의 표면은 통상의 Lab 표색계 기준으로 명도 지수 L값이 85 ~ 90, 색도 지수 a값이 12 ~ 18인 조건을 만족해야 한다. Lab 표색계는 Hunter의 광전색도계로 측정되는 L, a, b 값을 좌표로 하는 등색차 표색계이다. Lab 표색계를 기준으로 할 때, 동박 표면의 L값이 100이면 흰색(White)을 띠게 되며, 0이면 검은색(Black)을 띠게 된다. 또한, a값이 양(+)의 방향으로 증가할수록 점차 적색(Red)을 띠게 되며, b값이 양(+)의 방향으로 증가할수록 점차 노란색(Yellow)을 띠게 된다. 전기도금공정에서 첨가제가 적정하게 첨가되지 않거나, 지나치게 높은 조도를 갖는 첨가제가 첨가된 동박의 경우에는 상기 L값 및 a값 범위를 벗어나는 Lab 표색계 분포 특성을 보이게 된다.The surface of the copper foil must satisfy the condition that the brightness index L value is 85 to 90 and the chromaticity index a value is 12 to 18 based on a standard Lab colorimeter. Lab colorimetric is an isochromatic colorimetric system that uses the L, a, and b values as measured by Hunter's photochromic system. Based on Lab color system, if the L value of the copper foil surface is 100, it will be white, and if it is 0, it will be black. In addition, as the value a increases in the positive direction, the color becomes red gradually, and the value b gradually becomes yellow as the value b increases in the positive direction. In the electroplating process, the additive is not added properly, or in the case of the copper foil to which the additive having an excessively high roughness is added, the Lab colorimetric distribution characteristic is out of the L value and a value range.

동박에 있어서 매트면의 표면조도(Rzjis)는 1.5㎛ 이하의 조건을 만족해야 한다. 이러한 조건을 만족할 경우 보다 균일한 표면구조가 제공되어 음극 활물질의 코팅이 균일하게 이루어질 수 있으며, 리튬 이차전지의 충,방전 시 단락의 발생을 방지할 수 있다.In copper foil, the surface roughness (R zjis ) of the mat surface should satisfy the condition of 1.5 µm or less. If this condition is satisfied, a more uniform surface structure may be provided to uniformly coat the negative electrode active material, and may prevent occurrence of a short circuit during charging and discharging of the lithium secondary battery.

동박의 인장강도는 30~40kgf/㎟의 범위에 속하고, 180℃의 고온에서 5분 동안 열처리한 이후에 인장강도의 저하율이 10% 이하인 조건을 만족해야 한다. 또한, 동박의 연신율은 3~20%, 두께는 1~35㎛의 조건을 만족해야 한다. 이와 같은 범위를 벗어나는 경우 동박 표면에 물성 편차가 발생하여 활물질의 코팅이 균일하게 이루어지지 않으며 집전체의 물성이 불균일해지는 문제가 발생하게 된다.Tensile strength of the copper foil is in the range of 30 ~ 40kgf / ㎜, and after the heat treatment for 5 minutes at a high temperature of 180 ℃ must satisfy the condition that the decrease rate of the tensile strength is 10% or less. Moreover, the elongation of copper foil should satisfy | fill the conditions of 3 to 20% and thickness of 1 to 35 micrometers. If it is out of such a range, the physical property variation occurs on the surface of the copper foil, the coating of the active material is not made uniformly, a problem that the physical properties of the current collector is uneven.

도 1은 본 발명의 실시예 1 내지 3에 따른 리튬 이차전지 집전체용 동박의 물성을 종래기술(비교예 1 내지 3)과 비교하여 나타낸 테이블이다. 도 1에서 L값은 X-lite사의 색차계(SP-62)를 이용하여 측정하였으며, 매트면의 표면조도는 동박 시편별로 10 포인트(Point)를 선정하여 조도를 측정한 후 평균화하는 과정을 통해 산 출하였다. 상온 인장강도는 UTM(Universal Testing Machine)을 이용하여 측정하였는데, 이때 표점거리(Gauge Length)는 5㎝로 설정하였다. 또한, 고온인장강도는 동박 시편을 180℃에서 5분 동안 열처리한 후에 UTM을 이용하여 측정하였다.1 is a table showing the physical properties of the copper foil for lithium secondary battery current collector according to Examples 1 to 3 of the present invention in comparison with the prior art (Comparative Examples 1 to 3). In FIG. 1, the L value was measured using a color difference meter (SP-62) of X-lite, and the surface roughness of the mat surface was selected by averaging 10 points (Points) for each copper foil specimen and measuring the roughness. Calculated. Tensile strength at room temperature was measured using a universal testing machine (UTM), where the gauge length was set to 5 cm. In addition, the high temperature tensile strength was measured by using a UTM after heat-treated the copper foil specimen at 180 ℃ for 5 minutes.

본 발명의 실시예 1 내지 3에 따른 동박은 상술한 Lab 표색계 범위, 표면조도, 인장강도, 연신율, 동박두께의 조건을 바람직하게 모두 만족함으로써 균일한 활물질 코팅 특성을 제공한다. 반면에, 비교예 1 내지 3에 따른 동박은 활물질이 불균일하게 코팅되거나, 동박 표면과 활물질 간에 밀착성이 떨어져서 리튬 이차전지의 집전체로 사용되기에 부적합한 특성을 보이게 된다.Copper foil according to Examples 1 to 3 of the present invention provides uniform active material coating properties by preferably satisfying all of the above-described Lab colorimeter range, surface roughness, tensile strength, elongation, copper foil thickness. On the other hand, the copper foils according to Comparative Examples 1 to 3 are unevenly coated with the active material or have poor adhesion between the surface of the copper foil and the active material, thereby exhibiting unsuitable characteristics for use as a current collector of a lithium secondary battery.

이상에서 본 발명은 비록 한정된 실시예와 도면에 의해 설명되었으나, 본 발명은 이것에 의해 한정되지 않으며 본 발명이 속하는 기술분야에서 통상의 지식을 가진 자에 의해 본 발명의 기술사상과 아래에 기재될 특허청구범위의 균등범위 내에서 다양한 수정 및 변형이 가능함은 물론이다.Although the present invention has been described above by means of limited embodiments and drawings, the present invention is not limited thereto and will be described below by the person skilled in the art to which the present invention pertains. Of course, various modifications and variations are possible within the scope of the claims.

본 명세서에 첨부되는 다음의 도면은 본 발명의 바람직한 실시예를 예시하는 것이며, 상술한 발명의 상세한 설명과 함께 본 발명의 기술사상을 더욱 이해시키는 역할을 하는 것이므로, 본 발명은 그러한 도면에 기재된 사항에만 한정되어 해석되어서는 아니된다.The following drawings, which are attached to this specification, illustrate exemplary embodiments of the present invention, and together with the detailed description of the present invention, serve to further understand the technical spirit of the present invention. It should not be construed as limited to.

도 1은 본 발명의 실시예 1 내지 3에 따른 리튬 이차전지 집전체용 동박의 물성을 종래기술과 비교하여 나타낸 테이블이다.1 is a table showing the physical properties of the copper foil for a lithium secondary battery current collector according to Examples 1 to 3 of the present invention in comparison with the prior art.

Claims (6)

리튬 이자전지의 집전체로 사용되는 동박에 있어서,In the copper foil used as an electrical power collector of a lithium rechargeable battery, Lab 표색계 기준으로 동박표면의 L값이 85 ~ 90, a값이 12 ~ 18이고,Based on Lab colorimeter, L value of copper foil surface is 85 ~ 90, a value is 12 ~ 18, 매트면(Matte Side)의 표면조도(Rzjis)가 1.5㎛ 이하인 것을 특징으로 하는 리튬 이차전지의 집전체용 동박.Surface roughness (R zjis ) of the mat side (Matte Side) is copper foil for the current collector of the lithium secondary battery, characterized in that less than 1.5㎛ . 삭제delete 제1항에 있어서,The method of claim 1, 인장강도가 30~40kgf/㎟이며, 180℃에서 5분 동안 열처리한 이후에 인장강도의 저하율이 10% 이하인 것을 특징으로 하는 리튬 이차전지의 집전체용 동박.Tensile strength of 30 ~ 40kgf / ㎠, copper foil for a current collector of a lithium secondary battery, characterized in that the rate of decrease in tensile strength is 10% or less after heat treatment at 180 ℃ for 5 minutes. 제1항에 있어서,The method of claim 1, 연신율이 3~20%인 것을 특징으로 하는 리튬 이차전지의 집전체용 동박.Copper foil for the electrical power collector of the lithium secondary battery characterized by the elongation being 3 to 20%. 제1항에 있어서,The method of claim 1, 동박두께가 1~35㎛인 것을 특징으로 하는 리튬 이차전지의 집전체용 동박.Copper foil thickness is 1-35 micrometers, The copper foil for electrical power collectors of the lithium secondary battery characterized by the above-mentioned. 리튬 이자전지의 집전체로 사용되는 동박에 있어서,In the copper foil used as an electrical power collector of a lithium rechargeable battery, Lab 표색계 기준으로 동박표면의 L값이 85 ~ 90, a값이 12 ~ 18이고,Based on Lab colorimeter, L value of copper foil surface is 85 ~ 90, a value is 12 ~ 18, 매트면(Matte Side)의 표면조도(Rzjis)가 1.5㎛ 이하이고,The surface roughness (R zjis ) of the mat side is 1.5 μm or less, 인장강도가 30~40kgf/㎟이며, 180℃에서 5분 동안 열처리한 이후에 인장강도의 저하율이 10% 이하이고,Tensile strength is 30 ~ 40kgf / ㎜, and after the heat treatment for 5 minutes at 180 ℃ the rate of decrease in tensile strength is 10% or less, 연신율이 3~20%이고,Elongation is 3-20%, 동박두께가 1~35㎛인 것을 특징으로 하는 리튬 이차전지의 집전체용 동박.Copper foil thickness is 1-35 micrometers, The copper foil for electrical power collectors of the lithium secondary battery characterized by the above-mentioned.
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