KR100440485B1 - New non-aqueous electrolyte and lithium secondary battery using the same - Google Patents

New non-aqueous electrolyte and lithium secondary battery using the same Download PDF

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KR100440485B1
KR100440485B1 KR10-2002-0000473A KR20020000473A KR100440485B1 KR 100440485 B1 KR100440485 B1 KR 100440485B1 KR 20020000473 A KR20020000473 A KR 20020000473A KR 100440485 B1 KR100440485 B1 KR 100440485B1
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secondary battery
lithium secondary
lithium
carbonate
electrolyte
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KR20030059729A (en
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조정주
김형진
김수진
이연희
배준성
임근영
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주식회사 엘지화학
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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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • 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
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • 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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  • Secondary Cells (AREA)

Abstract

본 발명은 새로운 첨가제를 포함하는 비수전해액 및 이를 이용한 리튬 이차 전지에 관한 것으로, 특히 리튬염 및 전해핵 화합물을 포함하는 리튬 이차 전지용 비수전해액에 있어서, 1,3-디비닐테트라메틸디실록산 0.5 내지 5 중량% 포함하는 비수전해액 및 이를 이용한 리튬 이차 전지에 관한 것이다.The present invention relates to a nonaqueous electrolyte containing a novel additive and a lithium secondary battery using the same, in particular, in a nonaqueous electrolyte for a lithium secondary battery containing a lithium salt and an electrolytic nucleus compound, 1,3-divinyltetramethyldisiloxane 0.5 to It relates to a non-aqueous electrolyte containing 5% by weight and a lithium secondary battery using the same.

본 발명은 말단에 비닐기가 있고 가교 결합을 통해 안정성이 뛰어나 부동태막을 형성할 수 있는 첨가제를 전해액에 사용하여 안정성이 우수하고 전지 수명이 향상된 리튬 이차 전지를 제공할 수 있다.The present invention can provide a lithium secondary battery having excellent stability and improved battery life by using an additive in an electrolyte having a vinyl group at an end thereof and having excellent stability through crosslinking to form a passivation film.

Description

새로운 비수전해액 및 이를 이용한 리튬 이차 전지{NEW NON-AQUEOUS ELECTROLYTE AND LITHIUM SECONDARY BATTERY USING THE SAME}New Non-Aqueous Electrolyte and Lithium Secondary Battery Using the Same

본 발명은 새로운 첨가제를 포함하는 비수전해액 및 이를 이용한 리튬 이차 전지에 관한 것으로, 더욱 상세하게는 전지의 수명과 안정성 등의 전지 성능을 향상시킬 수 있는 새로운 첨가제를 포함하는 비수전해액 및 이를 이용한 리튬 이차 전지에 관한 것이다.The present invention relates to a non-aqueous electrolyte containing a new additive and a lithium secondary battery using the same, and more particularly, to a non-aqueous electrolyte containing a new additive that can improve battery performance, such as battery life and stability, and a lithium secondary using the same It relates to a battery.

리튬 이차 전지는 고용량이면서도 가볍기 때문에 휴대폰이나 컴퓨터 등에 주로 사용되고 있다. 상기 리튬 이차 전지의 성능을 향상시키기 위하여, 여러 가지 첨가제가 개발 시도되고 있는데, 이러한 첨가제들은 전지의 수명향상, 온도특성 향상, 팽윤(Swelling) 방지 등의 목적에 따라 다양하게 개발되고 있다.Lithium secondary batteries are mainly used in mobile phones and computers because of their high capacity and light weight. In order to improve the performance of the lithium secondary battery, various additives have been developed, and these additives have been variously developed according to the purpose of improving battery life, improving temperature characteristics, and preventing swelling.

리튬이온 이차전지용 전해액은 일반적으로 환형 카보네이트(cyclic carbonate)와 선형 카보네이트(linear carbonate)의 조합에 의해 이루어진다. 이에 사용되는 환형 카보네이트는 EC, PC, GBL 등이 있으며, 선형 카보네이트로는 DEC, DMC, EMC 등이 대표적으로 사용되고 있다.The electrolyte solution for a lithium ion secondary battery is generally formed by a combination of a cyclic carbonate and a linear carbonate. The cyclic carbonates used therein are EC, PC, GBL, and the like, and linear carbonates include DEC, DMC, and EMC.

현재 수명향상을 가져오는 대표적인 첨가제로는 VC (vinylene carbonate) 및 VEC (vinylethylene carbonate) 등의 여러 가지 화합물이 알려져 있다.Currently, various compounds such as VC (vinylene carbonate) and VEC (vinylethylene carbonate) are known as representative additives to improve the lifetime.

그러나, 상기 화합물들을 사용하면 저온 성능이 나빠지거나 전지가 부푸는 등의 문제를 일으켜 바람직하지 못하다.However, the use of such compounds is not preferable because of the problems such as poor low-temperature performance or swelling of the battery.

본 발명은 종래 기술의 문제점을 고려하여, 말단에 비닐기가 있고, 가교결합을 통해 부동태 막의 안정성이 우수하여 전지의 수명을 향상시킬 수 있는 비수전해액 첨가제를 제공하는 것을 목적으로 한다.SUMMARY OF THE INVENTION In view of the problems of the prior art, an object of the present invention is to provide a non-aqueous electrolyte additive which has a vinyl group at the terminal and has excellent stability of the passivation membrane through crosslinking to improve the life of the battery.

본 발명의 다른 목적은 상기 비수전해액 첨가제를 포함하는 리튬 이차 전지를 제공하는 것을 목적으로 한다.Another object of the present invention is to provide a lithium secondary battery comprising the nonaqueous electrolyte additive.

도 1은 본 발명에 따른 실시예 1 내지 3 및 비교예 1에 대한 수명시험 결과를 나타낸 것이다.Figure 1 shows the life test results for Examples 1 to 3 and Comparative Example 1 according to the present invention.

상기 목적을 달성하기 위하여, 본 발명은 리튬염 및 전해핵 화합물을 포함하는 리튬 이차 전지용 비수전해액에 있어서,In order to achieve the above object, the present invention provides a lithium secondary battery non-aqueous electrolyte containing a lithium salt and an electrolytic nucleus compound,

1,3-디비닐테트라메틸디실록산 0.5 내지 5 중량%를 포함하는 비수전해액을 제공한다.It provides a non-aqueous electrolyte containing 0.5 to 5% by weight of 1,3-divinyltetramethyldisiloxane.

또한, 본 발명은 리튬 이차 전지에 있어서,In addition, the present invention is a lithium secondary battery,

a) 리튬이온을 흡장 및 방출할 수 있는 양극;a) a positive electrode capable of occluding and releasing lithium ions;

b) 리튬이온을 흡장 및 방출할 수 있는 음극;b) a negative electrode capable of occluding and releasing lithium ions;

c) 다공성 분리막; 및c) a porous separator; And

d)ⅰ) 리튬 염;d) iii) lithium salts;

ⅱ) 전해액 화합물; 및Ii) electrolyte compounds; And

ⅲ) 1,3-디비닐테트라메틸디실록산Viii) 1,3-divinyltetramethyldisiloxane

을 포함하는 비수전해액Non-aqueous electrolyte solution containing

을 포함하는 리튬 이차 전지를 제공한다.It provides a lithium secondary battery comprising a.

이하에서 본 발명을 상세하게 설명한다.Hereinafter, the present invention will be described in detail.

본 발명은 전지의 수명을 향상시킬 수 있는 첨가제를 포함하는 리튬 이차 전지용 비수전해액 및 이를 포함하는 리튬 이차 전지를 제공하는 것이다.The present invention is to provide a non-aqueous electrolyte for a lithium secondary battery comprising an additive capable of improving the life of the battery and a lithium secondary battery comprising the same.

본 발명의 리튬 이차 전지는 리튬이온을 흡장 방출할 수 있는 양극, 리튬이온을 흡장 방출할 수 있는 음극, 다공성 분리막, 및 전해액을 포함한다.The lithium secondary battery of the present invention includes a positive electrode capable of occluding and releasing lithium ions, a negative electrode capable of occluding and releasing lithium ions, a porous separator, and an electrolyte solution.

특히, 본 발명은 비수전해액에 첨가제로 실록산계열의 화합물을 사용하며, 바람직하게는 1,3-디비닐테트라메틸디실록산을 사용하여 수명향상을 도모하였다.In particular, the present invention uses a siloxane-based compound as an additive to the nonaqueous electrolyte, preferably 1,3-divinyltetramethyldisiloxane to improve the life.

상기 1,3-디비닐테트라메틸디실록산은 이중결합을 갖는 관능기가 양쪽 말단에 있고, 중심에 리튬 이온을 전도할 수 있는 실록산, 에틸렌 옥사이드 등이 있어, 리튬을 잘 전도하고 가교 결합을 통해 안정성이 뛰어나 부동태막을 형성한다. 즉, 첨가제로 사용되는 1,3-디비닐테트라메틸디실록산이 음극 표면위에 부동태 막을 형성하는데 기여하고 이러한 부동태막이 더 이상의 전해액의 분해를 억제한다. 이에 따라, 전지의 제반 성능을 저해하지 않으면서, 전지의 수명을 향상시킬 수 있다.The 1,3-divinyltetramethyldisiloxane has a functional group having a double bond at both ends and siloxane, ethylene oxide, etc. capable of conducting lithium ions at the center thereof, and conducts lithium well and is stable through crosslinking. This is excellent and forms a passive film. That is, 1,3-divinyltetramethyldisiloxane, which is used as an additive, contributes to the formation of a passivation film on the cathode surface, and this passivation film suppresses further decomposition of the electrolyte. Thereby, the lifetime of a battery can be improved, without impairing the overall performance of a battery.

상기 1,3-디비닐테트라메틸디실록산의 함량은 0.5 내지 5 중량%로 사용하는것이 바람직하다. 상기 1,3-디비닐테트라메틸디실록산의 함량이 0.5 중량% 미만이면 첨가제의 효과가 미미한 문제가 있고, 5 중량%를 초과하면 음극의 비가역이 크고 전체적으로 전지의 용량을 작게하는 문제가 있다.The content of 1,3-divinyltetramethyldisiloxane is preferably used in 0.5 to 5% by weight. If the content of the 1,3-divinyltetramethyldisiloxane is less than 0.5% by weight, the effect of the additive is insignificant. If the content of the 1,3-divinyltetramethyldisiloxane is less than 5% by weight, the negative irreversibility of the negative electrode is large and the capacity of the battery is reduced.

또한, 본 발명의 비수전해액은 전해핵 화합물로 환형 카보네이트와 선형 카보네이트를 포함한다. 상기 환형 카보네이트의 예를 들면 에틸렌 카보네이트(EC), 프로필렌 카보네이트(PC), 감마부티로락톤(GBL) 등이 있다. 상기 선형 카보네이트의 예를 들면 디에틸 카보네이트(DEC), 디메틸 카보네이트(DMC), 에틸메틸카보네이트 (EMC), 및 메틸 프로필 카보네이트(MPC)로 이루어진 군으로부터 1 종 이상 선택되는 것이 바람직하다.In addition, the nonaqueous electrolyte of the present invention includes a cyclic carbonate and a linear carbonate as the electrolytic nucleus compound. Examples of the cyclic carbonates include ethylene carbonate (EC), propylene carbonate (PC), gamma butyrolactone (GBL), and the like. For example, the linear carbonate is preferably selected from the group consisting of diethyl carbonate (DEC), dimethyl carbonate (DMC), ethylmethyl carbonate (EMC), and methyl propyl carbonate (MPC).

본 발명의 비수전해액에는 리튬염을 포함하며, 구체적 예를 들면 LiClO4, LiCF3SO3, LiPF6, LiBF4, LiAsF6, 및 LiN(CF3SO2)2로 이루어진 군으로부터 선택되는 것이 바람직하다.The non-aqueous electrolyte of the present invention includes a lithium salt, and specifically selected from the group consisting of LiClO 4 , LiCF 3 SO 3 , LiPF 6 , LiBF 4 , LiAsF 6 , and LiN (CF 3 SO 2 ) 2 . Do.

또한, 본 발명의 리튬 이차 전지에 있어서, 음극의 활물질로는 탄소, 리튬 금속 또는 합금을 사용하는 것이 바람직하다. 기타 리튬을 흡장 및 방출할 수 있고, 리튬에 대한 전위가 2V 미만인 TiO2, SnO2와 같은 금속 산화물도 사용 가능하다.Moreover, in the lithium secondary battery of this invention, it is preferable to use carbon, lithium metal, or an alloy as an active material of a negative electrode. Other metals such as TiO 2 and SnO 2 , which can occlude and release lithium and have a potential for lithium of less than 2 V, can also be used.

본 발명에서는 양극 활물질로 리튬 함유 전이 금속 산화물을 사용하며, 예를 들면 LiCoO2, LiNiO2, LiMn2O4, LiMnO2및 LiNi1-XCoXO2(여기에서, 0＜X＜1)로 이루어진 군으로부터 1종 이상 선택되는 것이 바람직하다. 또한, MnO2와 같은 금속 산화물 혹은 이들의 조합으로 이루어진 양극도 무방하다.In the present invention, a lithium-containing transition metal oxide is used as the positive electrode active material, for example, LiCoO 2 , LiNiO 2 , LiMn 2 O 4 , LiMnO 2, and LiNi 1-X Co X O 2 (where 0 <X <1) It is preferable to select at least one from the group consisting of. In addition, an anode made of a metal oxide such as MnO 2 or a combination thereof may be used.

또한, 본 발명은 리튬 이차 전지의 제조시 다공성 분리막을 사용하며, 예를 들면 폴리올레핀계 다공성 분리막을 사용할 수 있다.In addition, the present invention uses a porous separator in the manufacture of a lithium secondary battery, for example, a polyolefin-based porous separator can be used.

본 발명의 리튬 이온 2차 전지는 통상적인 방법으로 음극과 양극 사이에 다공성의 분리막을 넣고, 상기한 LiPF6등의 리튬염과 첨가제를 포함하는 비수전해액을 투입하여 제조하게 된다.The lithium ion secondary battery of the present invention is prepared by inserting a porous separator between the negative electrode and the positive electrode in a conventional manner, by adding a non-aqueous electrolyte containing a lithium salt and additives, such as LiPF 6 described above.

본 발명에 따른 리튬 이차 전지의 외형은 캔으로 된 원통형 또는 각형인 것이 바람직하다. 또한, 상기 전지는 파우치형 전지를 포함할 수 있다.It is preferable that the external shape of the lithium secondary battery according to the present invention is cylindrical or rectangular in shape of a can. In addition, the battery may include a pouch-type battery.

이하의 실시예를 통하여 본 발명을 더욱 상세하게 설명한다. 단 실시예는 본 발명을 예시하기 위한 것이지 본 발명을 한정하는 것은 아니다.The present invention will be described in more detail with reference to the following examples. However, the examples are only for illustrating the present invention and not for limiting the present invention.

[실시예]EXAMPLE

실시예 1 내지 3Examples 1 to 3

전해액으로 EC: EMC = 1: 2의 조성을 가지는 1M LiPF6용액을 사용하였고, 상기 전해액에 각각 1, 2, 및 3 중량%(실시예 1, 2, 3)의 1,3-디비닐테트라메틸디실록산을 첨가하여 사용하였다. 사용된 음극은 인조흑연을 사용하였고, 양극은 LiCoO2를 사용하였다. 이후, 통상적인 방법으로 각형 전지를 제조하여 수명시험을 수행하였다.As an electrolyte solution, a 1M LiPF 6 solution having a composition of EC: EMC = 1: 2 was used, and 1, 2, and 3 wt% (Examples 1, 2, and 3) of 1,3-divinyltetramethyl were respectively added to the electrolyte. Disiloxane was added and used. The negative electrode used was artificial graphite, and the positive electrode was LiCoO 2 . Thereafter, a rectangular battery was manufactured by a conventional method to perform a life test.

비교예 1Comparative Example 1

상기 실시예 1과 동일한 방법으로 제조하되, 1,3-디비닐테트라메틸디실록산을 첨가하지 않은 전해액을 사용하였다.An electrolyte solution prepared in the same manner as in Example 1 but without addition of 1,3-divinyltetramethyldisiloxane was used.

(수명시험)(Life test)

상기 실시예 1 내지 3 및 비교예 1에 대한 수명시험 결과를 도 1에 나타내었다. 도 1에서 보면, 실시예 1 내지 3의 경우 비교예 1 보다 수명이 우수함을 알 수 있다.The life test results of Examples 1 to 3 and Comparative Example 1 are shown in FIG. 1. 1, it can be seen that in Examples 1 to 3, the lifespan is superior to that of Comparative Example 1.

첨가량에 따른 효과는 실시예 1(1 중량% 포함) 및 실시예 2(2 중량% 포함)의 경우 동일하게 나타났으며, 실시예 3의 경우(3 중량% 포함)의 경우 실시예 1과 2 보다는 약간 떨어지나 비교예 1보다는 수명이 우수하였다.The effect of the added amount was the same in Example 1 (including 1% by weight) and Example 2 (including 2% by weight), and in the case of Example 3 (including 3% by weight) Examples 1 and 2 Although slightly dropped, the service life was superior to Comparative Example 1.

이상에서 설명한 바와 같이, 본 발명은 말단에 비닐기가 있고 가교 결합을 통해 안정성이 뛰어나 부동태막을 형성할 수 있는 첨가제를 전해액에 사용하여 안정성이 우수하고 전지 수명이 향상된 리튬 이차 전지를 제공할 수 있다.As described above, the present invention can provide a lithium secondary battery having excellent stability and improved battery life by using an additive in an electrolyte having a vinyl group at an end thereof and having excellent stability through crosslinking to form a passivation film.

Claims (8)

리튬염 및 전해핵 화합물을 포함하는 리튬 이차 전지용 비수전해액에 있어서,In the nonaqueous electrolyte solution for lithium secondary batteries containing a lithium salt and an electrolytic nucleus compound, 1,3-디비닐테트라메틸디실록산 0.5 내지 5 중량%를 포함하는 비수전해액.A non-aqueous electrolyte comprising 0.5 to 5% by weight of 1,3-divinyltetramethyldisiloxane. 리튬 이차 전지에 있어서,In a lithium secondary battery, a) 리튬이온을 흡장 및 방출할 수 있는 양극;a) a positive electrode capable of occluding and releasing lithium ions; b) 리튬이온을 흡장 및 방출할 수 있는 음극;b) a negative electrode capable of occluding and releasing lithium ions; c) 다공성 분리막; 및c) a porous separator; And d)ⅰ) 리튬 염;d) iii) lithium salts; ⅱ) 전해액 화합물; 및Ii) electrolyte compounds; And ⅲ) 1,3-디비닐테트라메틸디실록산Viii) 1,3-divinyltetramethyldisiloxane 을 포함하는 비수전해액Non-aqueous electrolyte solution containing 을 포함하는 리튬 이차 전지.Lithium secondary battery comprising a. 제 2 항에 있어서,The method of claim 2, 상기 d)ⅲ)의 1,3-디비닐테트라메틸디실록산의 함량이 전해액에 대하여 0.5 내지 5 중량%인 리튬 이차 전지.The lithium secondary battery having a content of 1,3-divinyltetramethyldisiloxane of d) iii) is 0.5 to 5% by weight based on the electrolyte. 제 2 항에 있어서,The method of claim 2, 상기 a)의 양극의 활물질이 LiCoO2, LiNiO2, LiMn2O4, LiMnO2및 LiNi1-XCoXO2(여기에서, 0＜X＜1)로 이루어진 군으로부터 1종 이상 선택되는 리튬 전이금속 산화물인 리튬 이차 전지.Lithium selected from the group consisting of LiCoO 2 , LiNiO 2 , LiMn 2 O 4 , LiMnO 2 and LiNi 1-X Co X O 2 (here, 0 <X <1), wherein the active material of the positive electrode of a) Lithium secondary battery which is a transition metal oxide. 제 2 항에 있어서,The method of claim 2, 상기 b)의 음극의 활물질이 탄소, 리튬 금속 또는 합금인 리튬 이차 전지.The lithium secondary battery, wherein the active material of the negative electrode of b) is carbon, lithium metal or alloy. 제 2 항에 있어서,The method of claim 2, 상기 d)ⅰ)의 리튬염이 LiClO4, LiCF3SO3, LiPF6, LiBF4, LiAsF6, 및 LiN(CF3SO2)2로 이루어진 군으로부터 1종 이상 선택되는 리튬 이차 전지.The lithium secondary battery of d) iii) is at least one selected from the group consisting of LiClO 4 , LiCF 3 SO 3 , LiPF 6 , LiBF 4 , LiAsF 6 , and LiN (CF 3 SO 2 ) 2 . 제 2 항에 있어서,The method of claim 2, 상기 d)ⅱ)의 전해액 화합물이 에틸렌 카보네이트(EC), 프로필렌 카보네이트(PC), 및 감마부티로락톤(GBL)로 이루어진 군으로부터 1 종 이상 선택되는 환형 카보네이트; 및 디에틸 카보네이트(DEC), 디메틸 카보네이트(DMC), 에틸메틸카보네이트 (EMC), 및 메틸 프로필 카보네이트(MPC)로 이루어진 군으로부터 1 종 이상 선택되는 선형 카보네이트를 포함하는 리튬 이차 전지.The cyclic carbonate wherein the electrolyte compound of d) ii) is selected from the group consisting of ethylene carbonate (EC), propylene carbonate (PC), and gamma butyrolactone (GBL); And a linear carbonate selected from the group consisting of diethyl carbonate (DEC), dimethyl carbonate (DMC), ethylmethyl carbonate (EMC), and methyl propyl carbonate (MPC). 제 2 항에 있어서,The method of claim 2, 상기 리튬 이차 전지는 캔으로 된 원통형 또는 각형, 또는 파우치형인 리튬 이차 전지.The lithium secondary battery is a cylindrical or angular or pouch type lithium secondary battery made of cans.
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