# US 2025/0096237 A1 · Multi-layer cathode for rechargeable batteries and method for making same

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- Number: US 2025/0096237 A1
- Document ID: US20250096237A1
- Status: Published application
- Kind: A1
- Application number: 18/370,091
- Filed: 2023-09-19
- Published: 2025-03-20
- Earliest claimed: 2023-09-19
- Assignees: International Business Machines Corporation; Sidus Energy, Inc.
- Applicants: International Business Machines Corporation; Sidus Energy, Inc.
- Inventors: Phillip Medina; Maxwell Giammona; Linda Karin Sundberg; Han Zhen
- Web page: https://patentgrep.com/patent/US20250096237A1

## CPC

- H01M 4/366: {as layered products}
- H01M 4/0404: {by coating on electrode collectors}
- H01M 4/136: Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
- H01M 4/1397: of electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
- H01M 4/382: {Lithium (H01M4/405 takes precedence)}
- H01M 4/582: {Halogenides}
- H01M 4/622: {being polymers}
- H01M 4/625: {Carbon or graphite}
- H01M 4/661: {Metal or alloys, e.g. alloy coatings (H01M4/669 take precedence)}
- H01M 4/663: {containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres}
- H01M 4/667: {in the form of layers, e.g. coatings}
- H01M 4/668: {Composites of electroconductive material and synthetic resins}
- H01M 10/0568: characterised by the solutes
- H01M 10/0569: characterised by the solvents
- H01M 2004/028: {Positive electrodes}
- H01M 2300/0037: Mixture of solvents
- 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

A rechargeable battery with a multi-layer cathode has high active material loading, high-rate capability, high specific capacity, and low cell impedance. The multi-layer cathode has a first electrode layer with at least one adhesion promoting binder and at least one first conductive additive with an electrochemical surface area ≥800 m2/gm, which is prepared as a slurry and is applied to a cathode current collector; and a second binder with at least one polymeric binder that participates in a complexation interaction with at least halogen or at last one metal halide active material and at least one second conductive additive with a conductivity ≥5 S/cm, which is prepared as a slurry and is coated over the first electrode layer. The at least one halogen or metal halide active material, which is dissolved in water or alcohol for application, may be dosed into either the first or second electrode layer slurry. Additional electrode layers may have the same or a different formulation as the second electrode layer, with or without the active material.

## Claims

### Claim 1

A rechargeable battery comprising:
an anode;
a cathode current collector;
a multi-layer cathode comprising (i) at least one halogen or metal halide active material, (ii) a first electrode layer in contact with the cathode current collector, wherein the first electrode layer comprises at least one adhesion promoting binder and at least one first conductive additive with an electrochemical surface area ≥800 m2/gm, and (iii) a second electrode layer coated over the first electrode layer, wherein the second electrode layer comprises at least one polymeric binder that participates in a complexation interaction with the at least one halogen or metal halide active material and at least one second conductive additive with a conductivity ≥5 S/cm; and
an electrolyte in contact with the anode and the cathode.

### Claim 2 (depends on 1)

The battery of claim 1, wherein the at least one adhesion promoting binder of the first electrode layer is selected from the group consisting of sodium carboxymethylcellulose (CMC), styrene-butadiene rubber (SBR), polyvinylidene difluoride (PVDF), polyamide-imide (PAI) resin, and combinations thereof.

### Claim 3 (depends on 1)

The battery of claim 1, wherein the at least one first conductive additive of first electrode layer is selected from the group consisting of graphene, conductive carbon black, carbide-derived carbon, Ketjen black, and combinations thereof.

### Claim 4 (depends on 1)

The battery of claim 1, wherein the at least one polymeric binder of the second electrode layer is selected from the group consisting of amylose, amylopectin, cellulose, xylan, chitin, chitosan, alginic acid, glycogen, poly(vinyl) acetate (PVAc), poly(vinyl) alcohol (PVA), poly(vinyl) pyrrolidone (PVP), nylon, polyaniline (PANI), polypyrrole (PPy), poly(vinyl) pyridine, polyacrylonitrile (PAN), polyacetylene (PA), poly phenylacetylene (PPA), polyphenylene vinylene (PPV), polythiophene (PT), alpha-cyclodextrin, beta-cyclodextrin, poly(3,4-ethyenedioxythiophene) polystyrene sulfonate (PEDOT: PSS), poly(2-dimethylamino)ethyl methacrylate) methyl chloride quaternary salt (MADQUAT), poly(diallyl dimethylammonium chloride) (PDADMAC), and combinations thereof.

### Claim 5 (depends on 1)

The battery of claim 1, wherein the at least one second conductive additive of the second electrode layer is selected from the group consisting of conductive carbon black, single-walled carbon nanotubes, graphite, graphene, carbon black, activated carbon, carbon fibers, carbide-derived carbon, Ketjen black, and combinations thereof.

### Claim 6 (depends on 1)

The battery of claim 1, wherein the at least one halogen or metal halide active material is incorporated into the first electrode layer.

### Claim 7 (depends on 1)

The battery of claim 1, wherein the at least one halogen or metal halide active material is incorporated into the second electrode layer.

### Claim 8 (depends on 1)

The battery of claim 1, wherein the multi-layer cathode includes one or more additional electrode layers having a composition similar to the second electrode layer.

### Claim 9 (depends on 1)

The battery of claim 1, further comprising an oxidizing gas in contact with the anode, the cathode, and the electrolyte.

### Claim 10 (depends on 9)

The battery of claim 9, wherein the oxidizing gas is selected from the group consisting of oxygen, air, nitric oxide, nitrogen dioxide, and combinations thereof.

### Claim 11 (depends on 1)

The battery of claim 1, wherein the active material is a metal halide with a mono-iodide or poly-iodide salt.

### Claim 12 (depends on 1)

The battery of claim 1, wherein the electrolyte is a liquid electrolyte comprising at least one organic solvent and at least one ionic salt.

### Claim 13 (depends on 10)

The battery of claim 10, wherein the at least one organic solvent is selected from the group consisting of 1,2-dimethoxyethane (DME), tetraglyme (G4), 1,3-dioxolane (DOL), tetrahydrofuran (THF), ethyl acetate, acetonitrile, dimethylformamide (DMF), dimethyl sulfoxide (DMSO), acetone, hexamethylphosphoric triamide (HMPA), and combinations thereof.

### Claim 14 (depends on 10)

The battery of claim 10, wherein the ionic salt is selected from the group consisting of lithium nitrate (LiNO3), lithium bix (oxalate)-borate (LiBOB), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), lithium bis(fluorosulfonyl)imide (LiFSI), lithium hexafluorophosphate (LiPF6), and combinations thereof.

### Claim 15 (depends on 1)

The battery of claim 1, wherein the anode comprises a material selected from the group consisting of carbon, graphite, silicon, lithium (Li), sodium (Na), potassium (K), calcium (Ca), zinc (Zn), aluminum (Al), vanadium (V), iron (Fe), and combinations thereof.

### Claim 16 (depends on 1)

The battery of claim 1, wherein the cathode current collector comprises a material selected from the group consisting of aluminum (Al), copper (Cu), nickel (Ni), titanium (Ti), stainless steel, and combinations thereof.

### Claim 17

A rechargeable battery comprising:
a lithium-containing anode;
a stainless-steel cathode current collector;
a two-layer cathode comprising (i) lithium iodide as an active cathode material, (ii) a first electrode layer in contact with the cathode current collector, wherein the first electrode layer comprises at least two adhesion promoting binders and at least two first conductive additives with an electrochemical surface area ≥800 m2/gm, and (iii) a second electrode layer coated over the first electrode layer, wherein the second electrode layer comprises at least one polymeric binder that participates in a complexation interaction with the lithium iodide active material and at least one second conductive additive with a conductivity ≥5 S/cm; and an electrolyte in contact with the anode and the cathode;
a liquid electrolyte comprising at least one organic solvent and at least one ionic salt in contact with the anode and the cathode; and
an oxidizing gas in contact with the anode, the cathode, and the liquid electrolyte.

### Claim 18 (depends on 15)

The battery of claim 15, wherein the at least two adhesion promoting binders of the first electrode layer are sodium carboxymethylcellulose and styrene-butadiene rubber.

### Claim 19 (depends on 15)

The battery of claim 15, wherein the at least two first conductive additives of first electrode layer are graphene and Ketjen black.

### Claim 20 (depends on 15)

The battery of claim 15, wherein the at least one polymeric binder of the second electrode layer is poly(vinyl) pyrrolidone (PVP).

### Claim 21 (depends on 15)

The battery of claim 15, wherein the at least one second conductive additive of the second electrode layer is Ketjen black.

### Claim 22 (depends on 15)

The battery of claim 15, wherein the lithium iodide active cathode material is incorporated into the first electrode layer.

### Claim 23 (depends on 15)

The battery of claim 15, wherein the lithium iodide active cathode material is incorporated into the second electrode layer.

### Claim 24

A method of fabricating a multi-layer cathode for a rechargeable battery comprising:
preparing a first slurry comprising at least one adhesion promoting binder and at least one first conductive additive with an electrochemical surface area ≥800 m2/gm;
dosing at least one halogen or metal halide active material solubilized in water or alcohol into the first slurry;
applying the first slurry with the active material to a cathode current collector to form a first electrode layer of a multi-layer cathode;
preparing a second slurry comprising at least one polymeric binder and at least one second conductive additive with a conductivity ≥5 S/cm; and
coating the second slurry over the first electrode layer to form a second electrode layer of the multi-layer cathode.

### Claim 25

A method of fabricating a multi-layer cathode for a rechargeable battery comprising:
preparing a first slurry comprising at least one adhesion promoting binder and at least one first conductive additive with an electrochemical surface area ≥800 m2/gm;
applying the first slurry to a cathode current collector to form a first electrode layer of a multi-layer cathode;
preparing a second slurry comprising at least one polymeric binder, at least one second conductive additive with a conductivity ≥5 S/cm, and at least one halogen or metal halide active material solubilized in water or alcohol; and
coating the second slurry over the first electrode layer to form a second electrode layer of the multi-layer cathode.
