Method for pre-lithiation of negative electrode for lithium secondary battery and lithium metal laminate used therefor

1. A method for pre-lithiation of a negative electrode, comprising the steps of:

producing a lithium metal laminate which comprises i) lithium metal foil having a thickness of 150 μm to 300 μm; and ii) a buffer layer comprising inorganic compound particles, and at least one of carbonaceous material particles or polymer compound particles, said buffer layer having a first surface and a second surface opposite the first surface, wherein the first surface of the buffer layer is coated directly on one surface of the lithium metal foil, and wherein the buffer layer has a thickness of 5 μm to 15 μm,

wherein the inorganic compound particles are Li 4 Ti 5 O 12 ;

producing a negative electrode comprising a negative electrode current collector, and a negative electrode active material layer formed on at least one surface of the negative electrode current collector;

wetting the negative electrode with an electrolyte solution composition, before laminating the lithium metal laminate with the negative electrode, and wherein, laminating the lithium metal laminate with the negative electrode is performed in the electrolyte solution composition;

laminating the lithium metal laminate with the negative electrode in such a manner that the second surface of the buffer layer of the lithium metal laminate is in direct contact with the negative electrode active material layer; and

removing the lithium metal laminate from the negative electrode to obtain the pre-lithiated negative electrode.

2. The method for pre-lithiation of a negative electrode according to claim 1 , wherein the particles of the buffer layer have a closely packed or densely packed structure so that they are in surface contact with each other, and an interstitial volume defined by the surface contact of the particles function as pores.

3. The method for pre-lithiation of a negative electrode according to claim 1 , which further comprises a step of pressurizing the laminate of the lithium metal laminate and the negative electrode with a force of 0.1 kgf-50 kgf per 1.5 cm 2 , after laminating the lithium metal laminate with the negative electrode.

4. The method for pre-lithiation of a negative electrode according to claim 1 , wherein the lithium metal laminate is formed by a method comprising: coating polymer compound particles dispersed in a dispersion medium on a surface of the lithium metal foil.

5. The method for pre-lithiation of a negative electrode according to claim 1 , wherein the lithium metal laminate is formed by a method comprising: coating carbonaceous material and/or inorganic compound particles on a surface of the lithium metal foil.

6. The method for pre-lithiation of a negative electrode according to claim 1 , wherein the polymer compound is present in the buffer layer as a binder polymer, and wherein the carbonaceous material particles and/or the inorganic compound particles are bound by the binder polymer.

7. The method for pre-lithiation of a negative electrode according to claim 1 , wherein the polymer compound particles are present and comprise a binder polymer, which is at least one selected from the group consisting of polyvinylidene fluoride (PVDF), polyacrylic acid (PAA), polyvinyl alcohol (PVA), carboxymethyl cellulose, hydroxypropylene cellulose, diacetylene cellulose, polyvinyl chloride, polyvinyl pyrrolidone, polytetrafluoroethylene (PTFE), polyethylene and polypropylene.

8. A lithium metal laminate for pre-lithiation of a negative electrode which comprises: i) lithium metal foil having a thickness of 150 μm to 300 μm; and ii) a buffer layer including inorganic compound particles, and at least one of carbonaceous material particles or polymer compound particles, and coated directly on one surface of the lithium metal foil, wherein the buffer layer has a thickness of 5 μm to 15 μm,

wherein the inorganic compound particles are Li 4 Ti 5 O 12 ,

wherein the carbonaceous material particles are selected from the group consisting of amorphous carbon, carbon nanotubes and graphene,

wherein the carbonaceous material particles or the inorganic compound particles are bound by a binder polymer, and

wherein the binder polymer is used in an amount from 1 to 20 wt. %.

9. The lithium metal laminate for pre-lithiation of the negative electrode according to claim 8 , wherein the particles of the buffer layer have a closely packed or densely packed structure so that they may be in surface contact with each other, and an interstitial volume defined by the surface contact of the particles function as pores.

10. The lithium metal laminate for pre-lithiation of the negative electrode according to claim 8 , wherein the polymer compound particles are present and comprise the binder polymer, which is at least one selected from the group consisting of polyvinylidene fluoride (PVDF), polyacrylic acid (PAA), polyvinyl alcohol (PVA), carboxymethyl cellulose, hydroxypropylene cellulose, diacetylene cellulose, polyvinyl chloride, polyvinyl pyrrolidone, polytetrafluoroethylene (PTFE), polyethylene and polypropylene.

11. A lithium secondary battery comprising the pre-lithiated negative electrode obtained from the method as defined in claim 1 .