• 专利附录
  • 专利说明
  • 权利要求
  • 类似技术
  • 同族专利
  • 引用文献
  • 法律状态
  • 优先权
    • 专利摘要:
    The invention relates to an electrochemical cell (1) of rechargeable lithium-ion battery, comprising a positive electrode (2) comprising a first active material optionally containing initially a quantity Q1 of active lithium, a negative electrode (4) comprising a second active material and on the surface of which a passivation layer SEI is likely to form, and an electrolyte for lithium ions. The positive electrode (2) comprises, facing the negative electrode (4), a perforated lithium sheet (8) having a thickness and a pattern of perforations chosen to constitute a quantity Q2 of lithium, the quantity Q2 of lithium provided by the perforated lithium sheet (8) and the amount Q1 of active lithium provided by the first active material of the positive electrode (2) when said first active material initially comprises active lithium, constituting the necessary amount of lithium and sufficient at the equilibrium of the electrochemical cell (1).
    公开号:CH712499A2
    申请号:CH00488/17
    申请日:2017-04-11
    公开日:2017-11-30
    发明作者:Pitteloud Cédric
    申请人:Belenos Clean Power Holding Ag；
    IPC主号:
    专利说明:

    Description
    FIELD OF THE INVENTION [0001] The invention relates to a rechargeable lithium-ion battery electrochemical cell comprising a positive electrode comprising a first active material optionally initially containing a quantity Q1 of active lithium, a negative electrode comprising a second active material and the surface of which a passivation layer SEI (Solid Electrolyte Interphase) is likely to form, and an electrolyte for lithium ions. The present invention also relates to a method of manufacturing such an electrochemical cell and a rechargeable lithium-ion battery comprising such electrochemical cells.
    BACKGROUND OF THE INVENTION [0002] Such an electrochemical cell is conventionally used for the production of rechargeable lithium-ion batteries. A lithium-ion battery is an electrochemical generator that uses lithium in ionic form. It releases electricity by reversible exchange of lithium ions between a positive electrode and a negative electrode. These positive and negative electrodes include an active material which is an intercalation material capable of inserting / disinbing lithium or forming an alloy therewith. During charging, the lithium ions are deintercalated by oxidation of the positive electrode, generally based on a lithiated oxide, and migrate through the electrolyte, ionic conductor, to the negative electrode, generally based on a carbon material, which is reduced with intercalation of these ions. Simultaneously, the electrons released at the positive electrode join the negative electrode through the external circuit. During the use of the battery, that is to say during the discharge, the reverse phenomena occur spontaneously. This process can be done in a similar way by making an alloy with lithium or by undoing it, for example in the case of the use of silicon as active material of the negative electrode where the alloy is formed during the charging of the drums.
    During the first insertion into the material of the negative electrode or the first formation of the alloy with the material of the negative electrode, a portion of the active lithium content initially in the positive electrode is consumed from irreversibly. This irreversibility is caused essentially by the formation of a passivation layer on the surface of the negative electrode called "Solid Electrolyte Interphase", called SEL. The SEI is an electronically semiconducting, permeable to lithium ions and impervious to other electrolyte components. Although its formation consumes lithium and therefore generates an irreversible capacitance, this protective layer plays a salutary role in the success of the following cycles, in particular by isolating the negative electrode from the electrolytic medium. However the irreversible consumption of lithium by the SEI causes a decrease in the amount of active material available, resulting in a decrease in the amount of current that can be returned by the battery.
    In order to solve this problem, it has been proposed to add lithium electrochemical cells in metallic form to compensate for the loss of lithium consumed by the SEI. This makes it possible to balance the amount of active material again so that the quantities of current released by each of the two oxidation-reduction reactions are similar. This additional lithium can be added for example in the form of an auxiliary electrode incorporated in the cell in contact with the electrolyte but separated from the other two electrodes, as described in US Pat. No. 6,335,115. This method has the disadvantage that it is necessary to remove this third electrode in the final product. This poses construction problems as well as having a distribution of the most homogeneous lithium during lithiation. Another solution is to add stabilized lithium powder, as described in patent application US 2009/0 035 663. However, the lithium powder due to the large surface area of its particles is generally very reactive. To overcome this problem, a protective layer (carbonate, oil) is formed on its surface. After lithiation, this protective layer is still present in the cell adding unwanted and unnecessary elements in the final battery. Another solution is to perform a pre-lithiation of the negative electrode outside the electrochemical cell, as described in the publication WO 96/32 754. This method has the disadvantage of using an electrolyte during this step, which must be washed before assembly of the cell. SUMMARY OF THE INVENTION [0005] One of the objectives of the invention is to overcome these various disadvantages.
    More specifically, an object of the invention is to provide a rechargeable lithium-ion battery electrochemical cell whose balance is preserved during its operation.
    Another object of the invention is to provide a rechargeable lithium-ion battery electrochemical cell for using as active material of the positive electrode, a material that does not initially contain a sufficient amount of lithium to ensure the equilibrium of the electrochemical cell, or even a material initially totally devoid of lithium.
    For this purpose, the present invention relates to a rechargeable lithium-ion battery electrochemical cell, comprising a positive electrode comprising a first active material optionally optionally containing a quantity Q1 of active lithium, a negative electrode comprising a second active material and the surface of which a passivation layer SEI (Solid Electrolyte Interphase) is likely to form, and an electrolyte for lithium ions.
    According to the invention, the positive electrode comprises, opposite the negative electrode, a perforated lithium sheet having a thickness and a pattern of perforations chosen to constitute a quantity Q2 of lithium, the quantity Q2 of lithium supplied by the perforated lithium sheet and the quantity Q1 of active lithium initially supplied by the first active material of the positive electrode when said first active material initially comprises active lithium, constituting the amount of lithium necessary and sufficient for the equilibrium of the cell.
    The present invention also comprises a method of manufacturing an electrochemical cell as defined above, comprising: a step of calculating the quantity Q2 of lithium to be supplied by the perforated lithium sheet according to the capacity blocked in the SEI, the capacity of the second active material of the negative electrode and the capacity of the active lithium optionally initially contained in the first active material of the positive electrode, - a step of determining the thickness and the pattern perforations of the lithium sheet to be perforated as a function of the calculated quantity Q2; a step of producing the lithium sheet according to the determined thickness and a step of forming the perforations according to the determined pattern of perforations; assembly of the perforated lithium sheet made at the positive electrode, and a step of mounting the positive electrode and its perforated lithium sheet with the negative electrode and the electrolyte to form the cell.
    The present invention also comprises a rechargeable lithium-ion battery comprising electrochemical cells as defined above.
    The use of a perforated lithium sheet having a predetermined thickness and a pattern of perforations makes it possible to obtain a balanced electrochemical cell, comprising the quantity of lithium which is sufficient, but not excessively, after the first cycle, in order to guarantee a optimal operation of said electrochemical cell. The presence of a perforated lithium sheet having a thickness and a pattern of perforations determined also makes it possible to use, as active material of the positive electrode, a material which does not initially contain a sufficient quantity of lithium to ensure the equilibrium of the electrochemical cell, or even a material initially totally free of lithium, which could not be used optimally so far in an electrochemical cell of a rechargeable lithium-ion battery.
    BRIEF DESCRIPTION OF THE DRAWINGS [0013] Other characteristics and advantages of the invention will appear more clearly on reading the following description of an embodiment of the invention, given as a simple illustrative and nonlimiting example, and annexed figures, among which: FIG. 1 is a diagrammatic sectional view of an electrochemical cell according to the invention prepared with a view to producing a lithium-ion battery by stacking FIGS. 2 and 3 show a diagrammatic plan view of different lithium sheet perforation patterns used according to the invention, FIGS. 4 and 5 show a detail view of the perforations of the perforation patterns corresponding to FIGS. 2 and 3 respectively, and FIG. 6 shows the evolution of the capacity of an electrochemical cell according to the invention as a function of the number of charge-discharge cycles, at a current level of 0.5C between 2 and 4V.
    Detailed Description of a Preferred Embodiment [0014] Referring to FIG. 1, there is shown a schematic sectional view of an electrochemical cell 1 according to the invention. In the embodiment shown, the electrochemical cell is prepared for the production of a battery stack, which can be in the form of pocket, called "pouch" or button cell. It is obvious that the present invention also applies to the construction of cylindrical batteries, in which the electrodes are wound to form cylindrical cells.
    The cell 1 comprises a positive electrode 2 comprising a first current collector and a first active material optionally initially containing a quantity Q1 of active lithium, said first active material being applied to both sides of the first current collector. The cell 1 also comprises a negative electrode 4 comprising a second current collector and a second active material, said second active material being applied to both sides of the second current collector. The cell 1 also comprises a separator 6 disposed between the positive electrode 2 and the negative electrode 4. The cell 1 also contains an electrolyte for the lithium ions.
    The first active material of the positive electrode 2 comprises a lithium intercalation material, that is to say, capable of reversibly inserting / disinserting lithium or forming an alloy reversibly with that -this.
    The first active material of the positive electrode 2 may initially contain lithium or is capable of being lithiated during the first discharge of the cell. Preferably, the first active material of the positive electrode may be selected from the group comprising transition metal oxides and their lithiated compounds. The transition metal oxides are based for example on cobalt, manganese, molybdenum, or vanadium. The lithiated compounds preferably comprise LiMP04 where M = Ni, Co, Mn, Fe and their mixtures, LixHyV308 where x is between 0 and 4.5 and y is between 0 and 6.5, LiMn204, LiMn1i5Ni0.5O4, LiNiMnCo02 where the ratio between Ni, Mn and Co can vary between 0 and 1, LiNiCoAI02 where the ratio between Ni, Co and Al can vary between 0 and 1, Li2FePO4F, V205, S, Lh_xV0P04, Li3V2 (PO4) 3. It is obvious that any active material known to those skilled in the art suitable for the positive electrode can be used.
    The first active material may be conventionally combined with a conductive agent, for example a carbon compound, and a binder, for example a polymeric binder.
    The second active material of the negative electrode 4 comprises a lithium intercalation material, that is to say, capable of reversibly inserting / disinserting lithium or forming an alloy reversibly with that -this. It comprises an intercalation or alloy composition in which the lithium can be interposed or form an alloy during charging. Preferably, the second active material comprises a carbon-based intercalation composition, such as graphite, or a silicon, aluminum, or lithium alloy composition, such as Li 4 Ti 5 O 12, as well as the intermetallic alloys. base of Fe, Sn, Sb, Mn, Cu, Ni and other metals known to those skilled in the art to form suitable alloys with lithium.
    During the first charge, a passivation layer SEI is formed on the surface of the negative electrode 4. This phenomenon is known and does not require detailed description here.
    The electrolyte makes it possible to transport the Li + ions from one electrode to the other. For example, a liquid electrolyte generally consisting of a lithium salt dissolved in an organic solvent is chosen. The lithium salt is, for example, lithium hexafluorophosphate (LiPF 6), or LiClO 4, LiFSI, LiTFSI, LiBOB, LiDFOB. The electrolyte may also be in solid form, or be composed of ionic liquids.
    These various components of the electrochemical cell are known to those skilled in the art and do not require detailed description here.
    According to the invention, the positive electrode 2 comprises, opposite the negative electrode 4, between the positive electrode 2 and the associated separator 6, a perforated lithium sheet 8 having a thickness and a pattern of perforations. chosen to constitute a quantity Q2 of lithium, the quantity Q2 of lithium supplied by the perforated lithium sheet 8 and the quantity Q1 of active lithium supplied by the first active material of the positive electrode 2 when said first active material initially comprises lithium active, constituting the amount of lithium necessary and sufficient for the equilibrium of cell 1.
    A balanced cell is a cell in which the amount of lithium is sufficient, and without excess after the first cycle, to obtain a cell whose operation is optimal. This quantity of lithium supplied at the level of the positive electrode must therefore be sufficient to cover the formation of the SEI as well as to completely quench the second active material of the negative electrode 4. The quantity of active material is related to the amount of current released, and therefore to the capacity of the active material. At the level of the negative electrode, a capacitance greater than 2% to 10%, preferably from 2% to 5%, is generally expected to the theoretical capacity of the second active material of the negative electrode, in particular in order to avoid the formation of dendrites.
    As a result, the thickness and perforation pattern of the perforated lithium sheet 8 are chosen so that the quantity Q2 of lithium supplied by the perforated lithium sheet 8 makes it possible to have a lithium capacity provided by the perforated lithium sheet 8 such that: lithium capacity provided by the perforated lithium sheet + capacity of the active lithium possibly initially contained in the first active material of the positive electrode = capacity blocked in the SEI + (1 + z) x capacity the second active material of the negative electrode, z being between 0.02 and 0.1, and preferably between 0.02 and 0.5.
    When the first active material of the positive electrode 2 initially contains lithium, the capacity of the active lithium then initially contained in the first active material of the positive electrode is known, and is for example provided by the manufacturer. Similarly, the capacity of the second active material of the negative electrode is known, and is for example provided by the manufacturer. Blocked capacity in the SEI is also known and is determined by experience. The SEI is calculated as the difference in charge between the first and second cycles of a "second active material / metallic lithium" half-battery system, the metallic lithium constituting the negative electrode of the system.
    Once the capacity of the lithium to provide the calculated perforated lithium sheet, the thickness of the lithium sheet and the pattern of perforations are determined to obtain said capacity, and therefore the amount of lithium Q2.
    In particular, the perforation pattern of the lithium sheet forms perforations whose dimensions, shapes, arrangements, spacings, opening ratios, are chosen in combination with the thickness of said perforated lithium sheet. to supply the amount of lithium Q2.
    Preferably, the dimensions of the perforations are such that the distance between the center of the perforation and the edge of the perforation is less than 2 mm, and preferably less than 1.5 mm.
    Fig. 2 is a schematic top view of a pattern of perforations of a perforated lithium sheet 8 in the form of circular perforations and FIG. 4 represents the detail of a perforation.
    The distance x between the center of the perforation and the edge of the perforation is less than 2 mm, and preferably less than 1.5 mm. For example, a perforated R3T4 lithium plate comprising 3 mm diameter round holes staggered at 60 ° with a center distance of 4 mm can be used, giving a void percentage of 51.02%.
    FIG. 3 is a schematic top view of a pattern of perforations of a perforated lithium sheet 8 in the form of trapezoidal perforations and FIG. 5 represents the detail of a perforation. The distance x between the center of the perforation and the edge of the perforation is less than 2 mm, and preferably less than 1.5 mm.
    It is obvious that any other form of perforations can be used.
    The perforations are made in the lithium sheet by any method known to those skilled in the art, for example by successive and regular tearing with dots and stretching of the material.
    The thickness of the lithium sheet may be between 30 μm and 200 μm.
    The invention makes it possible to use lithium sheets whose thickness is still sufficiently large to allow easy use of a process for producing lithium sheets by rolling, but without excess lithium, in order to obtain a balanced cell. The addition of lithium by the perforated lithium sheet allows to use for the positive electrode, active materials low in lithium or lithium, which could not be used until now in the known electrochemical cells.
    The present invention relates to a method of manufacturing an electrochemical cell as defined above, and comprising: - a step of calculating the quantity Q2 of lithium to be supplied by the perforated lithium sheet, determined as has seen above from the capacity of lithium to provide, itself calculated from the capacity blocked in the SEI, the capacity of the second active material of the negative electrode and the capacity of the active lithium possibly content initially in the first active material of the positive electrode, - a step of determining the pattern of perforations and the thickness of the lithium sheet to be perforated as a function of the amount Q2 calculated, - a step of producing the sheet of lithium according to the determined thickness and a step of forming the perforations according to the perforation pattern determined, - a step of assembling the perforated lithium sheet e performed at the positive electrode, and - a step of mounting the positive electrode and its perforated lithium foil with the negative electrode and the electrolyte to form the cell.
    Once made, the perforated lithium sheet 8 can be connected to the positive electrode 2 opposite the negative electrode 4, between the positive electrode 2 and the associated separator 6, by rolling or any other appropriate method. . Then the other elements of the cell are assembled in a manner known to those skilled in the art. Everything is impregnated with electrolyte.
    The present invention also relates to a rechargeable lithium-ion battery comprising electrochemical cells as defined above.
    The following example illustrates the present invention without limiting the scope thereof.
    Example: Cells are made using for each cell: - a positive electrode comprising an active layer containing as active material U0.5I-L.5V3O8, conductive carbon compounds and a binder, the active layer being deposited on each face of a current collector - R3T4 perforated lithium sheets of 50 μm thickness, laminated on each side of the positive electrode - a carbon-based negative electrode - a polyethylene-based separator disposed between the electrode Positive coated with its perforated lithium sheet and the negative electrode.
    A battery is made by stacking these cells, adding the electrolyte, and sealing by vacuum sealing.
    The open circuit of the cell shows a negative potential of -0.3 V when the negative electrode is carbon. The battery is then charged to 4V and different cycles are performed. Fig. 6 represents the evolution of the capacity of the battery of the invention as a function of the number of discharge-charge cycles, at a current level of 0.5C between 2 and 4V. The results show that the battery comprising a perforated lithium sheet according to the invention can be operational over several cycles even if the active material of the positive electrode does not initially contain a sufficient quantity of lithium which would ensure the balance of cells.
    权利要求:
    Claims (11)
    [1]
    claims
    An electrochemical cell (1) for a rechargeable lithium-ion battery, comprising a positive electrode (2) comprising a first active material optionally initially containing a quantity Q1 of active lithium, a negative electrode (4) comprising a second active material and at the surface of which a passivation layer SEI (Solid Electrolyte Interphase) is likely to form, and an electrolyte for lithium ions, characterized in that the positive electrode (2) comprises, opposite the negative electrode (4) a perforated lithium sheet (8) having a thickness and pattern of perforations selected to constitute a quantity Q2 of lithium, the quantity Q2 of lithium provided by the perforated lithium sheet (8) and the quantity Q1 of active lithium supplied by the first active material of the positive electrode (2) when said first active material initially comprises active lithium, constituting the quantity of lithium required and sufficient to the equilibrium of the electrochemical cell (1).
    [2]
    2. Cell according to claim 1, characterized in that the thickness and perforation pattern of the perforated lithium sheet (8) are chosen so that the quantity Q2 of lithium supplied by the perforated lithium sheet (8) allows to have a lithium capacity provided by the perforated lithium sheet (8) such that: lithium capacity provided by the perforated lithium sheet + capacity of the active lithium possibly initially contained in the first active material of the positive electrode = capacity blocked in the SEI + (1 + z) x capacity of the second active material of the negative electrode, z being between 0.02 and 0.1.
    [3]
    3. Cell according to one of the preceding claims, characterized in that the perforation pattern of the lithium sheet (8) forms perforations whose dimensions, shapes, arrangements, spacings, opening ratios, are selected in combination with the thickness of said perforated lithium sheet (8) to provide the amount of lithium Q2.
    [4]
    4. Cell according to the preceding claim, characterized in that the dimensions of the perforations are such that the distance between the center of the perforation and the edge of the perforation is less than 2 mm, and preferably less than 1.5 mm.
    [5]
    5. Cell according to one of the preceding claims, characterized in that the first active material of the positive electrode (2) comprises a first lithium intercalation material.
    [6]
    6. Cell according to the preceding claim, characterized in that the first active material of the positive electrode (2) is selected from the group comprising transition metal oxides and their lithiated compounds.
    [7]
    7. Cell according to one of the preceding claims, characterized in that the second active material of the negative electrode (4) is an intercalation composition or lithium alloy.
    [8]
    8. Cell according to the preceding claim, characterized in that the second active material of the negative electrode (4) comprises a second lithium intercalation material.
    [9]
    9. A method of manufacturing an electrochemical cell according to one of claims 1 to 8, characterized in that it comprises: - a step of calculating the quantity Q2 of lithium to be supplied by the perforated lithium sheet (8) depending on the capacity blocked in the SEI, the capacity of the second active material of the negative electrode (4) and the capacity of the active lithium optionally initially contained in the first active material of the positive electrode (2), a step of determining the pattern of perforations and the thickness of the lithium sheet (8) to be perforated as a function of the calculated quantity Q2, - a step of producing the perforated lithium sheet (8) according to the determined thickness and a step of forming the perforations according to the perforation pattern determined, - a step of assembling the perforated lithium sheet (8) made at the positive electrode, and - a step of assembling the elec positive trode (2) and its perforated lithium sheet (8) with the negative electrode (4) and the electrolyte to form the cell.
    [10]
    10. The method of claim 9, characterized in that the perforated lithium sheet (8) is assembled to the positive electrode (2) facing the negative electrode (4) by rolling.
    [11]
    11. Rechargeable lithium-ion battery comprising electrochemical cells according to one of claims 1 to 8.
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    引用文献:
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    法律状态:
    优先权:
    申请号 | 申请日 | 专利标题
    EP16171588.3A|EP3249718B1|2016-05-26|2016-05-26|Electrochemical cell for rechargeable lithium-ion battery|
    EP16199128.6A|EP3249719B1|2016-05-26|2016-11-16|Electrochemical cell for rechargeable lithium-ion battery|
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