# US 12,183,896 B2 · Solid electrolyte membrane and all-solid-state battery comprising same

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- Number: US 12,183,896 B2
- Document ID: US12183896B2
- Status: Granted
- Kind: B2
- Application number: 17/264,051
- Filed: 2020-01-10
- Published: 2021-09-16
- Granted: 2024-12-31
- Earliest claimed: 2019-01-10
- Assignees: LG Energy Solution, Ltd.
- Applicants: LG Chem, Ltd.
- Inventors: Jung-Pil Lee; Eun-Bee Kim; Hyo-Sik Kim; Ji-Hoon Ryu; Seung-He Woo; Suk-Woo Lee
- Web page: https://patentgrep.com/patent/US12183896B2

## CPC

- H01M 10/4235: {Safety or regulating additives or arrangements in electrodes, separators or electrolyte (H01M10/4242 takes precedence)}
- H01M 50/417: Polyolefins
- H01M 4/382: {Lithium (H01M4/405 takes precedence)}
- H01M 10/052: Li-accumulators
- H01M 10/056: characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M 10/0565: Polymeric materials, e.g. gel-type or solid-type
- H01M 50/414: Synthetic resins, e.g. thermoplastics or thermosetting resins
- H01M 50/431: Inorganic material
- H01M 50/446: Composite material consisting of a mixture of organic and inorganic materials
- H01M 2004/027: {Negative electrodes}
- H01M 2300/0071: Oxides
- H01M 2300/0082: Organic polymers
- H01M 2300/0085: Immobilising or gelification of electrolyte
- H01M 2300/0091: in the form of mixtures
- Y02E 60/10: Energy storage using batteries
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

The present disclosure relates to a solid electrolyte membrane for an all-solid-state battery and a battery including the same. The battery may include lithium metal as a negative electrode active material. The solid-electrolyte membrane provides an effect of inhibiting growth of lithium dendrite by ionizing lithium deposited as metal. Therefore, when using lithium metal as a negative electrode in the all-solid-state battery including the solid electrolyte membrane, there is provided an effect of delaying and/or inhibiting growth of lithium dendrite. Thus, it is possible to effectively prevent an electrical short-circuit caused by growth of lithium dendrite.

## Claims

### Claim 1

A solid electrolyte membrane for an all-solid-state battery which is interposed between a negative electrode and a positive electrode, the solid electrolyte membrane comprising a) a polymeric electrolyte material having ion conductivity, b) a dendrite growth-inhibiting material, and c) a plurality of filler particles, wherein the dendrite growth-inhibiting material comprises a metal salt and is mixed with the polymeric electrolyte material, and the metal salt has lower reactivity as compared to lithium metal, and wherein the filler particles are chemically and physically stable against electrochemical reaction and include organic particles and/or inorganic particles,
wherein the metal salt comprises at least one of phosphite or chloride hydrate of Pt(+2), Au or Pt(+4).

### Claim 2 (depends on 1)

The solid electrolyte membrane according to claim 1, wherein the polymeric electrolyte material is present in an amount of 10-95 wt % based on 100 wt % of the solid electrolyte membrane.

### Claim 3 (depends on 1)

The solid electrolyte membrane according to claim 1, wherein the polymeric electrolyte material is an ion conductive composite of a polymer resin with a lithium salt and has an ion conductivity of 1×10−6 S/m or more.

### Claim 4 (depends on 1)

The solid electrolyte membrane according to claim 1, wherein the inorganic particles comprise at least one of a metal oxide or an oxide-based solid electrolyte.

### Claim 5 (depends on 1)

The solid electrolyte membrane according to claim 1, wherein the inorganic particles have a particle diameter of 10 nm to 50 μm.

### Claim 6 (depends on 4)

The solid electrolyte membrane according to claim 4, wherein the metal oxide comprises at least one of BaTiO3, Pb(Zr, Ti)O3 (PZT), Pb1−xLaxZr1−yTiyO3 (PLZT, wherein 0<x<1, 0<y<1), Pb(Mg1/3Nb2/3)O3—PbTiO3(PMN-PT), hafnia (HfO2), SrTiO3, SnO2, CeO2, MgO, NiO, CaO, ZnO, ZrO2, Y2O3, Al2O3, TiO2 or SiC.

### Claim 7 (depends on 4)

The solid electrolyte membrane according to claim 4, wherein the oxide-based solid electrolyte comprises lithium phosphate (Li3PO4), lithium titanium phosphate (LixTiy(PO4)3, 0<x<2, 0<y<3), lithium aluminum titanium phosphate (LixAlyTiz(PO4)3, 0<x<2, 0<y<1, 0<z<3), (LiAlTiP)xOy-type glass (0<x<4, 0<y<13), lithium lanthanum titanate (LixLayTiO3, 0<x<2, 0<y<3), lithium germanium thiophosphate (LixGeyPzSw, 0<x<4, 0<y<1, 0<z<1, 0<w<5), lithium nitride (LixNy, 0<x<4, 0<y<2), SiS2-type glass (LixSiySz, 0<x<3, 0<y<2, 0<z<4), P2S5-type glass (LixPySz, 0<x<3, 0<y<3, 0<z<7), or mixtures thereof.

### Claim 8 (depends on 1)

The solid electrolyte membrane according to claim 1, wherein the organic particles comprise at least one of styrene-butadiene rubber (SBR), polybutadiene rubber, polychloroprene (neoprene), nitrile rubber, acryl rubber, fluoro-rubber (FKM), polyvinyl chloride (PVC), polystyrene, polymethyl methacrylate (PMMA), acrylonitrile-butadiene-styrene (ABS), polyvinylidene fluoride, polyvinyl fluoride, PTFE, polyvinyl acetate, polyvinyl acetate-containing copolymers or polyvinyl acetate-co-ethylene.

### Claim 9 (depends on 1)

An all-solid-state battery comprising a negative electrode, the solid electrolyte membrane of claim 1, and a positive electrode stacked successively, wherein the negative electrode comprises lithium metal as a negative electrode active material.

### Claim 10 (depends on 3)

The solid electrolyte membrane according to claim 3, wherein the polymer resin is at least one of a polyether polymer, polycarbonate polymer, acrylate polymer, polysiloxane polymer, phosphazene polymer, polyethylene derivatives, alkylene oxide derivatives, phosphate polymer, polyagitation lysine, polyester sulfide, polyvinyl alcohol, polyvinylidene fluoride or a polymer containing an ionically dissociable group.

### Claim 11 (depends on 3)

The solid electrolyte membrane according to claim 3, wherein the lithium salt is represented by Li+X−, and the anion (X) is F−, Cl−, Br−, I−, NO3−, N(CN)2−, BF4−, CIO4−, PF6−, (CF3)2PF4−, (CF3)3PF3−, (CF3)4PF2−, (CF3)5PF−, (CF3)6P−, CF3SO3−, CF3CF2SO3−, (CF3SO2)2N−, (FSO2)2N−, CF3CF2(CF3)2CO−, (CF3SO2)2CH−, (SF5)3C−, (CF3SO2)3C−, CF3(CF2)7SO3−, CF3CO2−, CH3CO2−, SCN−, or (CF3CF2SO2)2N−.

### Claim 12 (depends on 3)

The solid electrolyte membrane according to claim 3, wherein the polymeric electrolyte material further includes a polymer gel electrolyte having an ion conductivity of 10−6 S/m or more.

### Claim 13 (depends on 1)

The solid electrolyte membrane according to claim 1, further comprising a crosslinking agent and/or initiator.

### Claim 14 (depends on 1)

The solid electrolyte membrane according to claim 1, having a thickness in a range of 5-500 μm.

### Claim 15 (depends on 1)

The solid electrolyte membrane according to claim 1, wherein the dendrite growth-inhibiting material is dispersed in the electrolyte membrane with uniform distribution.

### Claim 16 (depends on 1)

The solid electrolyte membrane according to claim 1, wherein the dendrite growth-inhibiting material is in an amount of 0.1-90 wt % based on 100 wt % of the solid electrolyte membrane.

### Claim 17 (depends on 1)

The solid electrolyte membrane according to claim 1, wherein the filler particles are in an amount of 5-90 vol % based on 100 vol % of the solid electrolyte membrane.