WO2022027823A1 - 一种三电极可修复锂离子电池 - Google Patents

一种三电极可修复锂离子电池 Download PDF

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WO2022027823A1
WO2022027823A1 PCT/CN2020/121002 CN2020121002W WO2022027823A1 WO 2022027823 A1 WO2022027823 A1 WO 2022027823A1 CN 2020121002 W CN2020121002 W CN 2020121002W WO 2022027823 A1 WO2022027823 A1 WO 2022027823A1
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electrode
lithium
battery
repairable
ion battery
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PCT/CN2020/121002
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English (en)
French (fr)
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孙全
司晓影
程传捷
肖莹
徐斌
卢珊珊
刘巍
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双登集团股份有限公司
江苏双登富朗特新能源有限公司
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Publication of WO2022027823A1 publication Critical patent/WO2022027823A1/zh

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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
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • 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
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/4242—Regeneration of electrolyte or reactants
    • 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
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/44—Methods for charging or discharging
    • H01M10/446—Initial charging measures
    • 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

Definitions

  • the invention relates to the technical field of chemical power sources, in particular to a lithium ion battery.
  • Lithium-ion batteries have been developed for 30 years since their introduction in the 1990s. Lithium-ion batteries have the advantages of high energy density, high operating voltage, wide operating temperature range, long cycle life, high safety performance, maintenance-free and no memory effect. In recent years, lithium-ion batteries have been widely used in digital, electric vehicles, energy storage, and military fields.
  • the capacity will gradually decay, because in the interior of lithium-ion batteries, in addition to the normal lithium-ion intercalation and de-intercalation reactions of positive and negative electrodes, there will be many side reactions, such as the formation of SEI film and Factors such as growth, electrolyte decomposition, binder decomposition, rupture of positive and negative active materials, etc., will cause the capacity of lithium-ion batteries to decrease. Although there are many factors that cause the attenuation of lithium-ion batteries, the main reason is the loss of active lithium, which is derived from the positive electrode and is limited in quantity. During the use process, with the formation and destruction of the SEI film, the lithium precipitation of the negative electrode will consume the only Li resources.
  • a method for pre-lithiation of lithium ion batteries is also disclosed.
  • a slurry containing lithium powder is prepared, and then the slurry is directly coated on the negative electrode sheet of the lithium ion battery by a coating method.
  • a lithium ion battery negative electrode sheet with a surface layer rich in lithium ion is obtained on the surface, and is assembled with the positive electrode to make a lithium ion battery.
  • this solution is basically a one-time supplement of lithium to improve the first charge and discharge efficiency of the battery, and it cannot continuously supplement the consumption of active lithium during use, which has serious deficiencies.
  • the present invention provides a three-electrode repairable lithium ion battery, which has the advantages of simple preparation process, easy operation, suitable for large-scale production, etc., and at the same time It can significantly improve the first charge and discharge efficiency of lithium-ion batteries and prolong the service life of the battery.
  • a three-electrode repairable lithium-ion battery comprising a positive electrode, a negative electrode, a diaphragm, an electrolyte, and an outer casing, and is characterized in that it further comprises a third electrode, the active material of the third electrode is lithium metal, and the lithium metal capacity is the battery 10-30% of the total capacity of the positive active material.
  • the current collector used in the positive electrode is porous aluminum foil
  • the current collector used in the negative electrode is porous copper foil.
  • Porous positive and negative electrode current collectors are used to facilitate the free shuttle of lithium ions between the electrodes.
  • the pole group is wrapped with lithium metal foil, or a lithium metal plate is attached to both sides of the pole group, and the lithium metal electrode is made of nickel or copper as the output. terminal as the third pole.
  • the capacity recovery of the three-electrode repairable lithium-ion battery is performed in an empty state.
  • the recovery steps are as follows: connect the positive electrode of the discharge machine to the negative electrode of the battery, and connect the negative electrode of the discharge machine to the third electrode of the battery.
  • the method can repair the capacity without disassembling after the battery is used.
  • the discharge current is 0.01C-0.1C, which can be precisely controlled by setting the discharge current 0.01C-0.1C and setting the discharge time. The effect of restored capacity.
  • the negative electrode pre-lithiation treatment is performed before the first charge and discharge of the three-electrode repairable lithium ion battery.
  • the effect of pre-lithiation improves the first charge and discharge efficiency of the battery.
  • the discharge current is 0.01C-0.1C, which reaches the capacity of accurately controlling the restored capacity by setting the discharge current 0.01C-0.1C and setting the discharge time. Effect.
  • the present invention has the following technical advantages compared with the prior art:
  • the present invention provides a scheme for continuously replenishing lithium in a lithium ion battery. Compared with the one-time lithium replenishing scheme, the biggest advantage is that the battery can be repaired in capacity after use.
  • the purpose of one-time lithium supplementation is to improve the first charge and discharge efficiency of lithium-ion batteries, and then increase the energy density of the battery.
  • the present invention can not only improve the first charge and discharge efficiency of the lithium ion battery, but also restore the capacity attenuation caused by the loss of active lithium during the cycle of the battery, thereby greatly reducing the use cost of the lithium ion battery.
  • Porous positive and negative current collectors are used, so that the lithium-ion battery can freely shuttle between electrodes, which can improve the efficiency of lithium-ion battery repair.
  • the invention has good manufacturability and is especially suitable for mass production.
  • Lithium-ion battery is a sealed system, and the lithium metal electrode of the third pole is implanted inside the battery before the battery is packaged. Do not disassemble the battery in the later battery repair, and repair it directly through the external circuit, which is simple and easy to operate.
  • the lithium ion battery production equipment of the present invention is common to the existing lithium ion battery production equipment, and the tooling of individual processes can be adjusted slightly, which is suitable for large-scale production.
  • the positive and negative electrode active materials are coated on porous aluminum and copper foils, dried and cut to obtain positive and negative electrode pieces.
  • the positive and negative electrodes and separators are made into rolling cores by a cylindrical winding process.
  • the positive electrode of the discharger is connected to the negative electrode of the battery
  • the negative electrode of the discharger is connected to the third electrode of the battery, that is, the lithium metal electrode
  • the discharge current is set to 30mA
  • the discharge time is 5h, which can achieve pre-embedded 0.15Ah lithium to the negative electrode , the effect of increasing the first efficiency of the battery by about 4%.
  • the capacity of the battery decays to about 80% during use.
  • the negative electrode can improve the first efficiency of the battery by about 5%.
  • the capacity of the battery decays to about 80% during use.
  • the same method can be used to restore 6-8%.
  • the capacity of the battery decays to about 80% during use. First, connect the positive and negative electrodes of the discharger to the positive and negative electrodes of the battery to empty the battery capacity. Then connect the positive electrode of the discharger to the negative electrode of the battery, and connect the negative electrode of the discharger to the lithium metal electrode of the battery. Set the discharge current to 2500mA and the discharge time to 2h. Add 5Ah of active lithium to the negative electrode, and the capacity of the battery can be recovered by 8-9%. . When the battery capacity decays to 80% again, the same method can be used to restore 6-8%.
  • the positive electrode of the discharger is connected to the negative electrode of the battery, and the negative electrode of the discharger is connected to the third electrode of the battery, that is, the lithium metal electrode.
  • the discharge current is set to 5000mA, and the discharge time is 1.5h, which can achieve pre-embedded 7.5Ah lithium
  • the first efficiency of the battery is increased by about 6%.
  • the capacity of the battery decays to about 80% during use.
  • the capacity of 12.5Ah of active lithium is added to the negative electrode, and the capacity of the battery can be recovered by 10- 11%.
  • the same method can be used to restore 9-10%.

Abstract

本发明公开了一种三电极可修复锂离子电池，即在锂离子电池制作过程中植入了第三极，达到可持续补充锂离子电池在循环过程中损失的活性锂的效果。本发明采用的第三极锂金属容量为电池正极活性物质总量的10-30%，修复时使用放电机在电池空电状态下做容量恢复，放电电流为0.01C-0.1C，通过设置放电电流和设置放电时间来精确控制恢复的容量的效果。较一次性补锂方案，本发明最大的优势在于电池使用后在不需要拆解情况下可以做容量的修复。

Description

一种三电极可修复锂离子电池 技术领域
本发明涉及化学电源技术领域，具体涉及一种锂离子电池。
背景技术
锂离子电池自上个世纪九十年代问世以来，已经发展了30年。锂离子电池具有能量密度大、工作电压高、工作温度范围宽、循环寿命长、安全性能高等优点，以及免维护和无记忆效应等特点。近年来，锂离子电池已广泛用于数码、电动汽车、储能以及军事等领域。锂离子电池在使用的过程中，容量会逐步衰减，因为在锂离子电池的内部，除了正常的锂离子嵌入和脱嵌正负极的反应，还会存在很多副反应，例如SEI膜的生成和生长，电解液分解，粘结剂分解，正负极活性物质破裂等等因素，都会造成锂离子电池的容量下降。虽然造成锂离子电池衰减的因素很多，但最主要的原因还是活性锂的损失，活性锂来源于正极，数量有限。在使用过程中随着SEI膜的生成、破坏，负极析锂等都会消耗仅有的Li资源。
技术问题
在专利号为201910418237.4的专利中，公开了一种锂离子电池预锂化的方法，其是在惰性气氛条件下，将裸电芯置于电解液中，在两侧分别放置锂金属条，用电源正极与裸电芯的负极连接，电源负极与锂金属条连接，通过对负极充电实现预锂化，最后将裸电芯从电解液中取出封装。这种敞开的是补锂方法，对环境的要求极高，无法规模生产，同时无法做到在使用过程中持续补锂。在专利号为201811607641.8的专利中，同样公开了一种锂离子电池预锂化方法，先制备含锂粉的浆料，再将浆料通过涂覆的方法直接涂覆在锂离子电池的负极片表面得到表层富锂离的锂离子电池负极片，与正极组装制作锂离子电池。此方案与目前公开的专利一样，基本都是一次性的补锂，提高电池的首次充放电效率，对于使用过程中活性锂的消耗无法做到持续补充，存在严重不足。
技术解决方案
为了克服锂离子电池在循环使用过程中活性锂离子损失得不到补充问题问题，本发明提供一种三电极可修复锂离子电池，具有制备工艺简单、易操作、适合大规模生产等优势，同时可以显著提高锂离子电池的首次充放电效率以及延长电池的使用寿命。
为了达到上述发明目的，本发明提供的技术方案如下：
一种三电极可修复锂离子电池，包括正极、负极、隔膜、电解液、外壳，其特征在于还包括第三极，所述第三极的活性物质为锂金属，所述锂金属容量为电池正极活性物质总容量的10-30%。
较佳的，所述正极所用的集流体为多孔铝箔，负极所用的集流体为多孔铜箔，采用多孔正负极集流体，以便于锂离子自由穿梭于电极之间。
较佳的，所述正极、负极与所述隔膜装配成极群后，使用锂金属箔卷绕包裹极群，或用锂金属板贴在极群两侧，锂金属电极用镍或铜做输出端子作为第三极。
较佳的，在三电极可修复锂离子电池在空电状态做容量恢复，其恢复步骤如下：将放电机的正极接电池的负极，放电机的负极接电池的第三极，该电池的恢复方法在电池使用后在不需要拆解情况下就可以做容量的修复。
较佳的，所述三电极可修复锂离子电池在空电状态下做容量恢复步骤中，放电电流为0.01C-0.1C，达到通过设置放电电流0.01C-0.1C和设置放电时间来精确控制恢复的容量的效果。
较佳的，在三电极可修复锂离子电池首次充放电前做负极预锂化处理，其步骤如下：将放电机的正极接电池的负极，放电机的负极接电池的第三极，达到负极预锂化的效果，提高电池首次充放电效率。
较佳的，所述三电极可修复锂离子负极预锂化处理步骤中，放电电流为0.01C-0.1C，达到通过设置放电电流0.01C-0.1C和设置放电时间来精确控制恢复的容量的效果。
有益效果
基于上述技术方案，本发明的与现有技术相比具有如下技术优点：
1. 本发明提供一种锂离子电池持续补锂的方案，较一次性补锂方案最大的优势在于电池使用后可以做容量的修复。一次性补锂目的是提高锂离子电池的首次充放电效率，继而提升电池的能量密度。而本发明不但可以提高锂离子电池的首次充放电效率，而且可以恢复由于电池在循环过程中由于活性锂的损失而造成的容量衰减，极大程度降低了锂离子电池的使用成本。采用了多孔正负极集流体，以便于锂离子电池自由穿梭于电极之间，可提高锂离子电池修复的效率。
2. 本发明工艺性好，尤其适合批量生产。锂离子电池是一个密封的体系，第三极的锂金属电极在电池封装前被植入到电池内部。后期的电池修复不要拆解电池，直接通过外电路修复，简单易操作。此外本发明的锂离子电池生产设备与现有锂离子电池生产设备通用，个别工序的工装稍微做调整即可，适合大规模生产。
本发明的最佳实施方式
下面结合实施例对本发明作进一步的解释说明。
实施例1
以3Ah三电极可修复锂离子电池为例。
1. 将正极、负极活性物质涂覆到多孔的铝和铜箔上，烘干分切获得正极、负极极片。采用圆柱型卷绕的工艺将正负极和隔膜制成卷芯。
2. 用0.3Ah的锂箔包裹卷芯，用镍带汇流连接到盖板第三极端子上，封装注液后制成3Ah圆柱型锂离子电池。
3. 在电池化成充电前，用放电机的正极接电池的负极，放电机的负极接电池的第三极即锂金属电极，设置放电电流30mA，放电时间5h，可达到预嵌0.15Ah的锂到负极，将电池的首次效率提升4%左右的效果。
4. 电池在使用过程中容量衰减至80%左右，首先用放电机正负极连接电池正负极将电池容量放空。再用放电机的正极接电池的负极，放电机的负极接电池的锂金属电极，设置放电电流30mA，放电时间5h，将0.15Ah的容量活性锂补充到负极，电池的容量可以恢复4-5%。
本发明的实施方式
实施例2
以10Ah三电极可修复锂离子电池为例。
1 、将正极、负极活性物质涂覆到多孔的铝和铜箔上，烘干分切获得正极、负极极片。采用方形卷绕的工艺将正负极和隔膜制成卷芯。
2 、用2.0Ah的锂箔包裹卷芯，用镍带汇流连接到盖板第三极端子上，封装注液后制成10Ah方形铝壳锂离子电池。
3 、在电池化成充电前，用放电机的正极接电池的负极，放电机的负极接电池的第三极即锂金属电极，设置放电电流200mA，放电时间3h，可达到预嵌0.60Ah的锂到负极，将电池的首次效率提升5%左右的效果。
4 、电池在使用过程中容量衰减至80%左右，首先用放电机正负极连接电池正负极将电池容量放空。再用放电机的正极接电池的负极，放电机的负极接电池的锂金属电极，设置放电电流200mA，放电时间5h，将1Ah的容量活性锂补充到负极，电池的容量可以恢复8-9%。当电池容量再次衰减至80%，采用同样的方法可以恢复6-8%。
实施例3 ：
以50Ah三电极可修复锂离子电池为例。
1 、将正极、负极活性物质涂覆到多孔的铝和铜箔上，烘干分切获得正极、负极极片。采用软包叠片的工艺将正负极和隔膜制成极群。
2 、用两片总容量12.5Ah的锂片夹住极群，用铜带汇流连接到第三极极耳上，封装注液后制成50Ah软包叠片锂离子电池。
3 、在电池化成充电前，用放电机的正极接电池的负极，放电机的负极接电池的锂金属电极，设置放电电流1000mA，放电时间2.5h，达到预嵌2.5Ah的锂到负极，将电池的首次效率提升4%左右的效果。
4 、电池在使用过程中容量衰减至80%左右，首先用放电机正负极连接电池正负极将电池容量放空。再用放电机的正极接电池的负极，放电机的负极接电池的锂金属电极，设置放电电流2500mA，放电时间2h，将5Ah的容量活性锂补充到负极，电池的容量可以恢复8-9%。当电池容量再次衰减至80%，采用同样的方法可以恢复6-8%。
实施例4
以100Ah三电极可修复锂离子电池为例。
1 、将正极、负极活性物质涂覆到多孔的铝和铜箔上，烘干分切获得正极、负极极片。采用方形卷绕的工艺将正负极和隔膜制成卷芯。
2 、用两片总容量30Ah的锂片夹住极群，用镍带汇流连接到盖板第三极端子上，封装注液后制成100Ah方形铝壳锂离子电池。
3 、在电池化成充电前，用放电机的正极接电池的负极，放电机的负极接电池的第三极即锂金属电极，设置放电电流5000mA，放电时间1.5h，可达到预嵌7.5Ah的锂到负极，将电池的首次效率提升6%左右的效果。
4 、电池在使用过程中容量衰减至80%左右，首先用放电机正负极连接电池正负极将电池容量放空。再用放电机的正极接电池的负极，放电机的负极接电池的锂金属电极，设置放电电流5000mA，放电时间2.5h，将12.5Ah的容量活性锂补充到负极，电池的容量可以恢复10-11%。当电池容量再次衰减至80%，采用同样的方法可以恢复9-10%。
上述内容为本发明的示例及说明，但不意味着本发明可取得的优点受此限制，凡是本发明实践过程中可能对结构的简单变换、和/或一些实施方式中实现的优点的其中一个或多个均在本申请的保护范围内。

Claims (7)

  1. 一种三电极可修复锂离子电池，包括正极、负极、隔膜、电解液、外壳，其特征在于,还包括第三极，所述第三极的活性物质为锂金属，所述锂金属容量为电池正极活性物质总容量的10-30%，即所述第三极为锂金属电极。
  2. 根据权利要求1所述的三电极可修复锂离子电池，其特征在于,所述正极所用的集流体为多孔铝箔，负极所用的集流体为多孔铜箔。
  3. 根据权利要求1所述的三电极可修复锂离子电池，其特征在于,所述正极、负极与所述隔膜装配成极群后，使用锂金属箔卷绕包裹极群，或用锂金属板贴在所述极群的两侧，锂金属电极用镍或铜做输出端子作为第三极。
  4. 根据权利要求1-3中任意一项所述的三电极可修复锂离子电池，其特征在于,在三电极可修复锂离子电池在空电状态下做容量恢复，其恢复步骤如下：将放电机的正极接电池的负极，放电机的负极接电池的第三极。
  5. 根据权利要求4所述的三电极可修复锂离子电池，其特征在于,在所述三电极可修复锂离子电池在空电状态下做容量恢复步骤中，放电电流为0.01C-0.1C。
  6. 根据权利要求1-3中任意一项所述的三电极可修复锂离子电池，其特征在于,在三电极可修复锂离子电池首次充放电前做负极预锂化处理，其步骤如下：将放电机的正极接电池的负极，放电机的负极接电池的第三极。
  7. 根据权利要求6所述的三电极可修复锂离子电池，其特征在于,在所述三电极可修复锂离子负极预锂化处理步骤中，放电电流为0.01C-0.1C。
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