# US 2021/0242470 A1 · Cathode, lithium-air battery including the same, and method of preparing the same

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- Number: US 2021/0242470 A1
- Document ID: US20210242470A1
- Status: Published application
- Kind: A1
- Application number: 17/156,934
- Filed: 2021-01-25
- Published: 2021-08-05
- Earliest claimed: 2020-01-30
- Assignees: Samsung Electronics Co., Ltd.
- Applicants: Samsung Electronics Co., Ltd.
- Inventors: Mokwon KIM; Jungock PARK; Hyunpyo LEE
- Web page: https://patentgrep.com/patent/US20210242470A1

## CPC

- H01M 4/8621: {containing only metallic or ceramic material, e.g. made by sintering or sputtering}
- H01M 4/382: {Lithium (H01M4/405 takes precedence)}
- H01M 4/8605: {Porous electrodes}
- H01M 4/8663: {Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers}
- H01M 4/8673: {Electrically conductive fillers}
- H01M 4/8853: {Electrodeposition}
- H01M 12/08: composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
- H01M 2004/027: {Negative electrodes}
- H01M 2004/8689: {Positive electrodes}
- Y02E 60/10: Energy storage using batteries
- Y02E 60/50: Fuel cells
- 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

A cathode configured to use oxygen as a cathode active material includes: a porous electrically conductive framework substrate; and a coating layer disposed on a surface of the porous electrically conductive framework substrate, wherein the coating layer includes at least one of a lithium-containing metal oxide or a composite including a lithium-containing metal oxide, and wherein a porosity of the porous electrically conductive framework substrate is about 70 percent to about 99 percent, based on a total volume of the cathode, and an areal resistance of the porous electrically conductive framework substrate is about 0.01 milliohms per square centimeter to about 100 milliohms per square centimeter.

## Claims

### Claim 1

A cathode configured to use oxygen as a cathode active material, the cathode comprising:
a porous electrically conductive framework substrate; and
a coating layer disposed on a surface of the porous electrically conductive framework substrate,
wherein the coating layer comprises at least one of a lithium-containing metal oxide or a composite comprising a lithium-containing metal oxide,
wherein a porosity of the porous electrically conductive framework substrate is about 70 percent to about 99 percent, based on a total volume of the cathode, and
wherein an areal resistance of the porous electrically conductive framework substrate is about 0.01 milliohms per square centimeter to about 100 milliohms per square centimeter.

### Claim 2 (depends on 1)

The cathode of claim 1, wherein a thickness of the porous electrically conductive framework substrate is in a range of about 1 micrometer to about 500 micrometers.

### Claim 3 (depends on 1)

The cathode of claim 1, wherein the porous electrically conductive framework substrate comprises a fibrous framework,
wherein the fibrous framework comprises a plurality of fibers, and
wherein an average diameter of a fiber of the fibrous framework is in a range of about 0.1 micrometer to about 10 micrometers.

### Claim 4 (depends on 1)

The cathode of claim 1, wherein the porous electrically conductive framework substrate comprises at least one of a carbon, a metal, or a metal oxide,
wherein the carbon is at least one of a carbon fiber or a carbon tube,
the metal is at least one of Ni, Cu, Ti, V, Cr, Mn, Fe, Co, Zn, Mo, W, Ag, Au, Ru, Pt, Ir, Al, Sn, Bi, Si, Sb, stainless steel, or an alloy thereof, and
the metal oxide is an oxide of a metal comprising at least one of Ru, Sb, Ba, Ga, Ge, Hf, In, La, Ma, Se, Si, Ta, Se, Ti, V, Y, Zn, or Zr.

### Claim 5 (depends on 1)

The cathode of claim 1, wherein the porous electrically conductive framework substrate is at least one of a carbon paper, a carbon woven fabric, a carbon non-woven fabric, a carbon mesh, a carbon foam, a metal mesh, or a metal foam.

### Claim 6 (depends on 3)

The cathode of claim 3, wherein a thickness of the coating layer is in a range of about 50 nanometers to about 3 micrometers,
wherein the thickness of the coating layer is about 30% or less of an average diameter of the fiber of the fibrous framework.

### Claim 7 (depends on 1)

The cathode of claim 1, wherein a size of the lithium-containing metal oxide in the coating layer is in a range of about 10 nanometers to about 500 nanometers,
wherein a loading level of the coating layer is in a range of about 0.1 milligrams per square centimeter to about 50 milligrams per square centimeter, and
a porosity of the cathode is about 70% or more.

### Claim 8 (depends on 1)

The cathode of claim 1, wherein the lithium-containing metal oxide is at least one of a crystalline lithium-ion conductor, a crystalline electron conductor, or a mixed conductor.

### Claim 9 (depends on 1)

The cathode of claim 1, wherein the lithium-containing metal oxide, has an electronic conductivity of equal to or greater than about 1×10−6 Siemens per centimeter and an ion conductivity of equal to or greater than about 2×10−7 Siemens per centimeter, at a temperature of 25° C.

### Claim 10 (depends on 1)

The cathode of claim 1, wherein the lithium-containing metal oxide comprises at least one of a perovskite compound or a spinel compound.

### Claim 11 (depends on 1)

The cathode of claim 1, wherein the lithium-containing metal oxide comprises a perovskite compound represented by Formula 1:
LixAyGzO3−δ Formula 1
wherein, in Formula 1,
A and G are each independently at least one of a Group 2 to Group 16 element; and
0<x<1, 0<y<1, 0<(x+y)≤1, 0<z≤1.5, and 0≤δ≤1.5.

### Claim 12 (depends on 11)

The cathode of claim 11, wherein A is at least one of H, Na, K, Rb, Cs, Ca, Sr, Ba, Y, La, Ce, Pr, Nd, Pm, Sm, Gd, Tb, Dy, Ho, or Er;
G is at least one of Ti, Pd, Pb, Fe, Ir, Co, Rh, Mn, Cr, Ru, Re, Sn, V, Ge, W, Zr, Ti, Mo, Hf, U, Nb, Th, Ta, Bi, Li, H, Na, K, Rb, Cs, Ca, Sr, Ba, Y, La, Ce, Pr, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Mg, Al, Si, Sc, Zn, Ga, Rb, Ag, Cd, In, Sb, Pt, Au, or Pb; and
0.2<x≤0.7, 0<y≤0.7, 0<(x+y)<1, 0<z≤1.2, and 0≤δ≤1.2.

### Claim 13 (depends on 1)

The cathode of claim 1, wherein the lithium-containing metal oxide comprises a spinel compound represented by at least one of Formula 2 or Formula 3:
Li1±xM2±yO4−δ1, Formula 2
Li4±aM5±bO12−δ2 Formula 3
wherein, in Formulae 2 and 3,
M is each independently at least one of a Group 2 to Group 16 element; and
0<x<1, 0<y<1, 0≤δ1≤1, 0<a<2, 0.3<b<5, and 0≤δ2≤3.

### Claim 14 (depends on 13)

The cathode of claim 13, wherein
M is at least one of Ni, Pd, Pb, Fe, Ir, Co, Rh, Mn, Cr, Ru, Re, Sn, V, Ge, W, Zr, Ti, Mo, Hf, U, Nb, Th, Ta, Bi, Li, H, Na, K, Rb, Cs, Ca, Sr, Ba, Y, La, Ce, Pr, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Mg, Al, Si, Sc, Zn, Ga, Rb, Ag, Cd, In, Sb, Pt, Au, or Pb; and
0<x<1, 0<y<1, 0≤δ1≤1, 0<a<2, 0.3<b<5, and 0≤δ2≤3.

### Claim 15 (depends on 13)

The cathode of claim 13, wherein the spinel compound is represented by Formula 4:
Li4±aTi5-bM′cO12−δ Formula 4
wherein, in Formula 4,
M′ is at least one of Cr, Mg, Ca, Sr, Sc, Y, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Zr, Hf, V, Nb, Ta, Mo, W, Mn, Tc, Re, Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Pt, Cu, Ag, Au, Zn, Cd, Hg, Al, Ga, In, TI, Ge, Sn, Pb, Sb, Bi, Po, As, Se, or Te; and
0.3<a<2, 0.3<b<2, 0.3<c<2, and 0≤δ≤3.

### Claim 16 (depends on 1)

The cathode of claim 1, wherein the lithium-containing metal oxide comprises at least one of a layered compound, a garnet compound, a NASICON compound, a LISICON compound, a phosphate compound, a tavorite compound, a triplite compound, an anti-perovskite compound, a silicate compound, or a borate compound.

### Claim 17 (depends on 1)

The cathode of claim 1, wherein the lithium-containing metal oxide comprises at least one of a layered compound represented by Formula 5, a NASICON compound represented by Formula 6, a LISICON compound represented by Formula 7, a garnet compound represented by Formula 8, a phosphate compound represented by at least one of Formulae 9 or 10, a tavorite compound or a triplite compound represented by Formula 11, an anti-perovskite compound represented by Formula 12, a silicate compound represented by Formula 13, or a borate compound represented by Formula 14:
Li1±xM1±yO2±δ Formula 5
wherein, in Formula 5,
M is at least one of a Group 2 to Group 16 element; and
0<x<0.5, 0<y<1, and 0≤δ≤1,
Li1+xAxM2−x(XO4)3 Formula 6
wherein, in Formula 6,
A and M are each independently at least one of a Group 2 to Group 16 element;
X is As, P, Mo, or S; and
0<x<1.0,
Li8−cAaB′bO4 Formula 7
wherein, in Formula 7,
A and B′ are each independently at least one of a Group 2 to Group 16 element;
c=ma+nb, wherein m is an oxidation number of A, and n is an oxidation number of B′; and
0<x<8, 0<a≤1, and 0≤b≤1,
LixA3B′2O12 Formula 8
wherein, in Formula 8,
A and B′ are each independently at least one of a Group 2 to Group 16 element; and
3.0≤x≤7.0,
Li1±xMPO4 Formula 9
Li2MP2O7 Formula 10
wherein, in Formulae 9 and 10,
M is each independently at least one of a Group 2 to Group 16 element; and
0≤x≤1.0
Li1±xM(TO4)X Formula 11
wherein, in Formula 11,
M is at least one of a Group 2 to Group 16 element;
T is P or S,
X is F, O, or OH; and
LixMyOA Formula 12
wherein, in Formula 12,
M is at least one of a Group 2 to Group 16 element;
A is F, Cl, Br, I, S, Se, or Te; and
2.0≤x≤3.0 and 0≤y≤1.0,
Li2±xMSiO4 Formula 13
wherein, in Formula 13,
M is at least one of a Group 2 to Group 16 element; and
0≤x≤1.0,
Li1±xMBO3 Formula 14
wherein, in Formula 14,
M is at least one of a Group 2 to Group 16 element; and
0≤x≤1.0.

### Claim 18 (depends on 1)

A lithium-air battery comprising:
the cathode of claim 1;
an anode comprising lithium; and
an electrolyte disposed between the cathode and the anode.

### Claim 19 (depends on 18)

The lithium-air battery of claim 18, wherein the electrolyte comprises a solid electrolyte,
wherein the solid electrolyte is a compound having a crystalline structure or a composition different from that of the lithium-containing metal oxide.

### Claim 20

A method of preparing a cathode, the method comprising:
providing a suspension comprising a lithium-containing metal oxide particle; and
electrophoretically depositing the lithium-containing metal oxide particle on a porous electrically conductive framework substrate to prepare the cathode,
wherein an areal resistance of the porous electrically conductive framework substrate is about 0.01 milliohms per square centimeter to about 100 milliohms per square centimeter.

### Claim 21

A cathode configured to use oxygen as a cathode active material, the cathode comprising:
a porous electrically conductive framework substrate; and
a coating layer disposed on a surface of the porous electrically conductive framework substrate,
wherein the coating layer comprises at least one of a perovskite compound represented by Formula 1, a spinel compound represented by Formula 2, or a spinel compound represented by Formula 3:
LixAyGzO3−δ Formula 1
wherein, in Formula 1,
A and G are each independently at least one of a Group 2 to Group 16 element; and
0<x<1, 0<y<1, 0<(x+y)≤1, 0<z≤1.5, and 0≤δ≤1.5,
Li1±xM2±yO4−δ1 Formula 2
Li4±aM5±bO12−δ2 Formula 3
wherein, in Formulae 2 and 3,
each M is independently selected and is at least one of a Group 2 to Group 16 element; and
0<x<1, 0<y<1, 0≤δ1≤1, 0<a<2, 0.3<b<5, and 0≤δ2≤3.