# US 2021/0242513 A1 · Multi-domained sulfur electrodes, and manufacturing therefor

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- Number: US 2021/0242513 A1
- Document ID: US20210242513A1
- Status: Published application
- Kind: A1
- Application number: 17/236,614
- Filed: 2021-04-21
- Published: 2021-08-05
- Earliest claimed: 2016-01-20
- Assignees: Cornell University
- Applicants: Cornell University
- Inventors: Yong Lak Joo; Jaehyuk Lee
- Web page: https://patentgrep.com/patent/US20210242513A1

## CPC

- H01M 10/52: Removing gases inside the secondary cell, e.g. by absorption (vent plugs or other mechanical arrangements for facilitating escape of gases H01M50/30)
- H01M 4/0419: {involving spraying}
- H01M 4/134: Electrodes based on metals, Si or alloys
- 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 4/366: {as layered products}
- H01M 4/38: of elements or alloys
- H01M 4/5815: {Sulfides}
- H01M 4/625: {Carbon or graphite}
- H01M 4/663: {containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres}
- H01M 4/808: {Foamed, spongy materials}
- 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

Provided herein are positive electrodes for lithium batteries, particularly lithium sulfur batteries, and the manufacture thereof. Particularly, such electrodes have good performance characteristics, such as capacity and capacity retention, even at very high loading of sulfur (e.g., >5 mg/cm2), as well as flexibility. Exemplary manufacturing techniques include the electrospraying of sulfur (e.g., electrode active sulfur compounds), and an optional additive (e.g., a nanostructured conductive additive), onto a porous, conductive substrate (e.g., a porous carbon substrate, such as comprising multiple layers and/or domains).

## Claims

### Claim at position 1

-61. (canceled)

### Claim 62

A process for producing an electrode, the process comprising:
(a) injecting a first electrostatically charged fluid stock into a gas stream to form a first plume comprising a plurality of first particles, the first electrostatically charged fluid stock comprising a first liquid, sulfur, and a first additive, the first additive comprising a plurality of first carbonaceous inclusions, and
(b) collecting the plurality of the first particles onto a porous carbon substrate to form a porous substrate.

### Claim 63 (depends on 62)

The process of claim 62, wherein the first additive comprises graphene, graphene oxide, reduced graphene oxide, carbon nanotubes, graphene nanoribbons, carbon nanofibers, mesoporous carbon nanostructures, or any combination thereof.

### Claim 64 (depends on 62)

The process of claim 62, wherein the first additive comprises graphene or a graphene analog.

### Claim 65 (depends on 64)

The process of claim 64, wherein the graphene analog is graphene oxide, reduced graphene oxide, or a combination thereof.

### Claim 66 (depends on 62)

The process of claim 62, further comprising:
(c) injecting a second electrostatically charged fluid stock into a second gas stream to form a second plume, the second plume comprising a plurality of second particles, the second electrostatically charged fluid stock comprising a second liquid, a second additive and/or optionally sulfur, the second additive comprising a plurality of the second carbonaceous inclusions, and
(d) collecting the plurality of the second particles onto the porous substrate.

### Claim 67 (depends on 62)

The process of claim 62, wherein the porous substrate comprises at least two layers or domains, wherein a first layer or domain is a course porous layer or domain, and the second layer or domain is a dense porous layer or domain.

### Claim 68 (depends on 62)

The process of claim 62, wherein the electrode is binder free.

### Claim 69 (depends on 62)

The process of claim 62, wherein the electrode comprises a sulfur loading of at least 5 mg/cm2.

### Claim 70 (depends on 62)

The process of claim 62, wherein the electrode comprises a sulfur loading of 10 to 30 mg/cm2.

### Claim 71 (depends on 62)

The process of claim 62, wherein the porous substrate is a macroporous substrate comprising a macroporous domain and a mesoporous and/or microporous domain, wherein the mesoporous and/or microporous domain are formed by at least partially filling the macroporous substrate with the additive.

### Claim 72 (depends on 62)

The process of claim 62, further comprising collecting a first deposition and a second deposition on the porous carbon substrate.

### Claim 73 (depends on 62)

The process of claim 62, further comprising infusing the sulfur into the porous carbon substrate or allowing the sulfur of the sulfur deposition to infuse into the porous carbon substrate.

### Claim 74 (depends on 62)

The process of claim 62, wherein the sulfur is uniformed deposited on the surface of the carbon substrate wherein the standard deviation of the concentration of the sulfur and/or additive on the surface is less than 100% of the average concentration.

### Claim 75 (depends on 73)

The process of claim 73, wherein the standard deviation of the concentration of the sulfur and/or additive on the surface is less than 30% of the average concentration.

### Claim 76 (depends on 62)

The process of claim 62, wherein the electrode comprises a first surface and a second surface and a sulfur is disposed on at least one of the first and second surface.

### Claim 77 (depends on 62)

The process of claim 62, wherein porous substrate is an asymmetric porous substrate comprising a course porous layer with less density, larger and/or more pores and a dense porous layer with higher density, fewer and/or smaller pores.

### Claim 78 (depends on 77)

The process of claim 77, wherein the course porous layer is configured to facilitate higher sulfur loading than the dense porous layer, and the dense porous layer is configured to facilitate capacity retention including the electrolyte soluble polysulfides that are formed during cell cycling of the electrode.

### Claim 79 (depends on 62)

The process of claim 62, wherein the electrode comprising a multilayered substrate comprises a sulfur infused asymmetric carbon substrate, and wherein the carbon substrate comprising multiple layers or domains.

### Claim 80 (depends on 62)

The process of claim 62, wherein the plume comprises a plurality of particles and/or droplets having an average dimension of less than 1 micron.

### Claim 81

A process for producing an electrode, the process comprising:
producing a first plume from a first fluid stock and disposed the first plume on a porous carbon substrate;
producing a second plume from a second fluid stock and disposed the second plume on the porous carbon substrate;
wherein the first fluid stock comprising a sulfur compound, a carbonaceous, or conductive additive; and the second fluid stock comprising a sulfur compound, a carbonaceous or conductive additive; and
wherein the first fluid stock is different from the second fluid stock and wherein at least one of the first and second fluid stock comprising a sulfur compound.