# US 11,909,052 B2 · Fabrication of membrane electrode assembly with filament extension atomizer spray

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- Number: US 11,909,052 B2
- Document ID: US11909052B2
- Status: Granted
- Kind: B2
- Application number: 17/364,163
- Filed: 2021-06-30
- Published: 2023-01-05
- Granted: 2024-02-20
- Earliest claimed: 2021-06-30
- Assignees: Xerox Corporation
- Applicants: Palo Alto Research Center Incorporated
- Inventors: Elif Karatay; Kathryn F. Murphy
- Web page: https://patentgrep.com/patent/US11909052B2

## CPC

- H01M 4/8825: {Methods for deposition of the catalytic active composition}
- B05B 3/04: driven by the liquid or other fluent material discharged, e.g. the liquid actuating a motor before passing to the outlet
- H01M 4/8642: {Gradient in composition}
- H01M 4/8807: {Gas diffusion layers}
- H01M 4/881: {Electrolytic membranes}
- H01M 8/1004: characterised by membrane-electrode assemblies [MEA] (H01M8/12 takes precedence)
- H01M 8/1081: starting from solutions, dispersions or slurries exclusively of polymers
- H01M 4/886: {Powder spraying, e.g. wet or dry powder spraying, plasma spraying}
- H01M 2008/1095: {Fuel cells with polymeric electrolytes}
- Y02E 60/50: Fuel cells
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- B05B: SPRAYING APPARATUS; ATOMISING APPARATUS; NOZZLES (spray-mixers with nozzles B01F25/72; processes for applying liquids or other fluent materials to surfaces by spraying B05D)
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

A method and apparatus are described for forming a multilayer assembly. The method includes adhering first and second catalyst layers to opposed sides of a polymer membrane. At least one of the first catalyst layer, the second catalyst layer, and the polymer membrane is formed by filament extension atomization of a fluid material to form atomized droplets that are sprayed to form the respective membrane or layer.

## Claims

### Claim 1

A method for forming a multilayer assembly comprising:
providing a first catalyst layer in contact with a first side of a polymer membrane, the first catalyst layer being formed from a first layer-forming material comprising a polymer and catalyst particles, dispersed in the polymer, the first layer-forming material further comprising at least one solvent, wherein a total solvent is no more than 10 wt. % of the first layer-forming material;
providing a second catalyst layer in contact with an opposed second side of the polymer membrane, the second catalyst layer being formed from the first layer-forming material or from a second layer-forming material comprising a polymer and catalyst particles, dispersed in the polymer;
wherein at least one of the first catalyst layer, the second catalyst layer, and the polymer membrane is formed by filament extension atomization of a fluid material to form atomized droplets that are sprayed to form the respective membrane or layer.

### Claim 2 (depends on 1)

The method of claim 1, wherein the total solvent is no more than 5 wt. % of the first layer-forming material.

### Claim 3 (depends on 1)

The method of claim 1, wherein the first layer-forming material is sprayed onto one of the membrane and a microporous layer.

### Claim 4 (depends on 1)

The method of claim 1, wherein the first catalyst layer comprises at least two sub-layers of a controllable thickness, a first of the sublayers having a higher concentration of the catalyst particles than a second of the sublayers.

### Claim 5 (depends on 1)

The method of claim 1, further comprising varying a concentration of catalyst particles in the first catalyst layer in a direction parallel to a thickness of the membrane.

### Claim 6 (depends on 1)

The method of claim 1, further comprising varying a concentration of catalyst particles in the first catalyst layer in a direction perpendicular to a thickness of the membrane.

### Claim 7

A method for forming a multilayer assembly comprising:
providing a first catalyst layer in contact with a first side of a polymer membrane, the first catalyst layer being formed from a first layer-forming material comprising a polymer and catalyst particles, dispersed in the polymer;
providing a second catalyst layer in contact with an opposed second side of the polymer membrane, the second catalyst layer being formed from the first layer-forming material or from a second layer-forming material comprising a polymer and catalyst particles, dispersed in the polymer;
wherein the polymer membrane is formed by filament extension atomization of a membrane-forming material to form atomized droplets that are sprayed on at least one of the first and second catalyst layers, the membrane-forming material comprising a molten thermoset polymer.

### Claim 8 (depends on 1)

The method of claim 1, wherein an interface between the first catalyst layer and the membrane is non-planar.

### Claim 9 (depends on 1)

The method of claim 1, further comprising adhering the first catalyst layer to a first microporous layer and adhering the second catalyst layer to a second microporous layer.

### Claim 10 (depends on 9)

The method of claim 9, further comprising coating the first microporous layer with a fluoropolymer layer formed by filament extension atomization of a fluid fluoropolymer material prior to adhering the first catalyst layer to a first microporous layer.

### Claim 11 (depends on 1)

The method of claim 1, wherein the polymer membrane is proton-permeable.

### Claim 12 (depends on 1)

The method of claim 1, further comprising incorporating the multilayer assembly into a membrane electrode assembly, the membrane electrode assembly comprising first and second electrodes spaced by the multilayer assembly.

### Claim 13 (depends on 1)

The method of claim 1, wherein:
the filament extension atomization of the first catalyst layer forming material is performed with a first filament extension atomizer which generates an aerosol from the first catalyst layer forming material in fluid form, by stretching the fluid material in a nip defined between rotating rollers; and
forming the first catalyst layer with a first applying station which receives the aerosol, the first applying station including outlets which deposit droplets of the aerosol on a substrate to form the first catalyst layer, the substrate comprising one of a microporous layer and the polymer membrane;
the first applying station, or a second applying station, applying the other of the microporous layer and the polymer membrane to the first catalyst layer.

### Claim 14 (depends on 1)

The method of claim 1, wherein:
the polymer and catalyst particles comprise at least 20 wt. % of the first catalyst layer material;
the method further comprising:
adhering a first microporous layer to the first catalyst layer; and
curing the first catalyst layer material.

### Claim 15

A method for forming a multilayer assembly the multilayer comprising first and second microporous layers, a polymer membrane, a first catalyst layer in contact with a first side of the polymer membrane and a second catalyst layer in contact with a second side of the polymer membrane, the method comprising:
spraying atomized droplets formed by filament extension atomization of a first layer-forming material to form a first catalyst layer on one of the first microporous layer and the first side of the polymer membrane, the first layer-forming material comprising a polymer and catalyst particles, dispersed in the polymer, the first layer-forming material comprising no more than 10 wt. % of solvent; and
spraying atomized droplets formed by filament extension atomization of a second layer-forming material to form the second catalyst layer on one of the second microporous layer and the second side of a polymer membrane, the second layer-forming material comprising a polymer and catalyst particles, dispersed in the polymer, the second layer-forming material comprising no more than 10 wt. % of solvent.
