# US 2019/0173096 A1 · Intermediate-Temperature Fuel Cell Tailored for Efficient Utilization of Methane

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- Number: US 2019/0173096 A1
- Document ID: US20190173096A1
- Status: Published application
- Kind: A1
- Application number: 16/318,246
- Filed: 2017-07-19
- Published: 2019-06-06
- Earliest claimed: 2016-07-19
- Assignees: Georgia Tech Research Corporation; University of Kansas
- Applicants: Georgia Tech Research Corporation; University of Kansas
- Inventors: Meilin Liu; Ik Whang Chang; Yu Chen; Ben M. Deglee; Brian Doyle; Franklin Tao; Lei Zhang
- Web page: https://patentgrep.com/patent/US20190173096A1

## CPC

- H01M 4/8657: {layered}
- H01M 4/8663: {Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers}
- H01M 4/9033: {Complex oxides, optionally doped, of the type M1MeO3, M1 being an alkaline earth metal or a rare earth, Me being a metal, e.g. perovskites}
- H01M 8/0637: Direct internal reforming at the anode of the fuel cell
- H01M 8/1213: characterised by the electrode/electrolyte combination or the supporting material
- H01M 8/1231: with both reactants being gaseous or vaporised
- H01M 8/1253: the electrolyte containing zirconium oxide
- H01M 8/126: the electrolyte containing cerium oxide
- H01M 2008/1293: {Fuel cells with solid oxide electrolytes}
- Y02E 60/50: Fuel cells
- Y02P 70/50: Manufacturing or production processes characterised by the final manufactured product
- 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
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

A solid oxide fuel cell capable of directly utilizing hydrocarbons as a fuel source at operating temperatures between 200° C. and 500° C. The anode, electrolyte, and cathode of the solid oxide fuel cell can include technologies for improved operation at temperatures between 200° C. and 500° C. The anode can include technologies for improved direct utilization of hydrocarbon fuel sources.

## Claims

### Claim 1

A fuel cell comprising:
an anode comprising a doped ceria catalyst;
an electrolyte comprising:
an oxygen ion transporting solid oxide fuel cell (SOFC) electrolyte material; and
a proton transporting SOFC electrolyte material; and
a cathode;
wherein the ratio of oxygen ion transporting SOFC electrolyte material to proton transporting SOFC electrolyte material is approximately 1:10; and
wherein the fuel cell is configured to directly utilize hydrocarbon fuel at temperatures of 500° C. or less.

### Claim 2 (depends on 1)

The fuel cell of claim 1, wherein the anode comprises:
an anode functional layer (AFL);
an anode support layer (ASL); and
anode reforming layer (ARL).

### Claim 3 (depends on 2)

The fuel cell of claim 2, wherein the AFL and ASL layers comprise Ni-based material.

### Claim 4 (depends on 2)

The fuel cell of claim 2, wherein the AFL and ASL layers comprise Ni—BaZr0.1Ce0.7Y0.1Yb0.1O3−δ.

### Claim 5 (depends on 2)

The fuel cell of claim 2, wherein the ARL layer comprises the doped ceria catalyst.

### Claim 6 (depends on 2)

The fuel cell of claim 2, wherein the ASL layer is impregnated with sameria-doped ceria (SDC).

### Claim 7 (depends on 2)

The fuel cell of claim 2, wherein the AFL and ASL layers have a pore structure; and
wherein the AFL layer has a finer pore structure than the ASL layer.

### Claim 8 (depends on 5)

The fuel cell of claim 5, wherein the doped ceria catalyst comprises Ni and Ru doped ceria.

### Claim 9 (depends on 5)

The fuel cell of claim 5, wherein the doped ceria catalyst comprises Ni and Ru supported ceria.

### Claim 10 (depends on 5)

The fuel cell of claim 5, wherein the doped ceria catalyst comprises Ni and Ru doped ceria and Ni and Ru supported ceria.

### Claim 11 (depends on 5)

The fuel cell of claim 5, wherein at least a portion of the dopants are ions dispersed on a surface of the ceria.

### Claim 12 (depends on 5)

The fuel cell of claim 5, wherein the doped ceria comprises nanofibers.

### Claim 13 (depends on 8)

The fuel cell of claim 8, wherein the sum of Ni and Ru by weight is approximately 10% or less.

### Claim 14 (depends on 8)

The fuel cell of claim 8, wherein Ni is present at approximately 5% by weight of the ARL.

### Claim 15 (depends on 8)

The fuel cell of claim 8, wherein Ru is present at approximately 5% by weight of the ARL.

### Claim 16 (depends on 8)

The fuel cell of claim 8, wherein the doped ceria includes an oxygen vacancy near one of the Ni or Ru dopants dispersed as ions on the surface of the ceria.

### Claim at position 17

-18. (canceled)

### Claim 19 (depends on 1)

The fuel cell of claim 1, wherein the oxygen ion transporting SOFC electrolyte material comprises sameria-doped ceria; and
wherein the proton transporting SOFC electrolyte material comprises barium yttrium zirconate.

### Claim 20

(canceled)

### Claim 21 (depends on 1)

The fuel cell of claim 1, wherein the electrolyte comprises alternating layers of the oxygen ion transporting SOFC electrolyte material and the proton transporting SOFC electrolyte material.

### Claim 22 (depends on 21)

The fuel cell of claim 21, wherein grain boundaries between the oxygen ion transporting SOFC electrolyte material and the proton transporting SOFC electrolyte material are substantially vertical.

### Claim 23 (depends on 1)

The fuel cell of claim 1, wherein the cathode comprises hollow oxide nanofibers.

### Claim 24 (depends on 23)

The fuel cell of claim 23, wherein the nanofibers have an average outer diameter between 200 nm and 400 nm and an average inner diameter between 50 nm and 150 nm.

### Claim 25 (depends on 23)

The fuel cell of claim 23, wherein the nanofibers comprise one or more materials selected from the group consisting of PrBa0.5Sr0.5Co1.5Fe0.5O5+δ, La0.6Sr0.4Co0.2Fe0.8O3, PrBa0.5Sr0.5Co2O6, and Sm0.5Sr0.5CoO3.

### Claim 26 (depends on 23)

The fuel cell of claim 23 further comprising nanoparticles residing on an outer surface of the hollow oxide nanofibers.

### Claim 27 (depends on 26)

The fuel cell of claim 26, wherein the nanoparticles comprise one or more materials selected from the group consisting of PrOx, sameria-doped ceria (SDC), gadolinia-doped ceria (GDC), and Pr0.1Ce0.9O2, Pr2Ni0.5Mn0.5O4.

### Claim 28

A fuel cell comprising:
an anode comprising a doped ceria catalyst;
an electrolyte; and
a cathode;
wherein the fuel cell is configured to directly utilize hydrocarbon fuel while operating with a current density of at least 200 mA/cm2 and an open circuit voltage of 0.75 V at temperatures of 500° C. or less for two hours or more without deactivation.

### Claim 29 (depends on 1)

The fuel cell of claim 1, wherein the fuel cell is configured to directly utilize hydrocarbon fuel and yield a peak power density of 0.368 W/cm2 at temperatures of 500° C. or less.

### Claim at position 29

-33. (canceled)

### Claim 34 (depends on 28)

The fuel cell of claim 28, wherein the fuel cell is configured to directly utilize hydrocarbon fuel and yield a peak power density of 0.368 W/cm2 at temperatures of 500° C. or less.

### Claim 35 (depends on 1)

The fuel cell of claim 1, wherein the doped ceria catalyst is active for wet and dry reforming of methane.

### Claim at position 32

-60. (canceled)

### Claim 61 (depends on 1)

The fuel cell of claim 1, wherein the cathode is formed by the process of:
electrospinning an oxide material;
calcining the electrospun oxide material, resulting in a mat of hollow oxide nanofibers;
flooding the mat of hollow oxide nanofibers with a mixture containing a binder and a solvent;
drying the mat of hollow oxide nanofibers; and
bonding the mat of hollow oxide nanofibers to an electrolyte layer.

### Claim 62 (depends on 2)

The fuel cell of claim 2, wherein the cathode comprises a cathode layer, the fuel cell formed by a process comprising:
forming the anode support layer (ASL);
forming the anode functional layer (AFL) on a top of the ASL;
forming an electrode layer on a top of the AFL layer;
co-firing the ASL, AFL, and electrode layers;
forming the cathode layer on a top of the electrode layer;
co-firing the ASL, AFL, electrode, and cathode layers;
forming the anode reforming layer (ARL) on a bottom of the ASL; and
co-firing the ASL, AFL, electrode, cathode, and ARL layers.

### Claim 63 (depends on 62)

The process of claim 62 further comprising contacting a buffer layer material with a top of the electrode layer.

### Claim 64 (depends on 62)

The process of claim 62 further comprising impregnating the ASL layer with Sm0.52CeO1.9.
