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PNNL-13501 - Pacific Northwest National Laboratory

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Study Control Number: PN00089/1496<br />

Ultrathin Solid Oxide Fuel Cell Fabrication<br />

Peter M. Martin, Dean W. Matson, Kerry Meinhardt<br />

The development of ultrathin electrolyte layers for use in solid oxide fuel cells may allow both a significant reduction in<br />

operating temperature and improvement in power output compared with cells produced using conventional ceramic<br />

processing methods.<br />

Project Description<br />

The purpose of this project was to demonstrate the<br />

production and application of a vapor-deposited ultrathin<br />

electrolyte layer for solid oxide fuel cells. Ultrathin<br />

electrolyte layers are predicted to allow operation of solid<br />

oxide fuel cell units at lower temperatures than are<br />

possible using the thicker elecrolyte layers produced<br />

using conventional ceramic processed technology. Thin<br />

(1 to10 micrometer) yttria-stabilized zirconia (YSZ)<br />

coatings were deposited onto nickel-zirconia cermet<br />

electrodes using reactive sputtering from metal alloy<br />

targets. We have shown that, despite irregular surfaces on<br />

the underlying cermet substrates, dense, defect-free yttriastabilized<br />

zirconia electrolyte layers can be produced.<br />

The microstructure and crystallographic phase of the<br />

yttria-stabilized zirconia electrolyte were related to the<br />

sputtering parameters used to produce the coatings.<br />

Introduction<br />

Solid oxide fuel cells provide a highly efficient means to<br />

convert fossil fuels to electricity. This is produced by<br />

migration of oxygen ions from a porous airside electrode<br />

through a solid gas impermeable electrolyte to a porous<br />

fuel-side electrode. The maximum power of these<br />

devices is limited by the resistance of the electrolyte to<br />

oxygen ion permeation and electrode/electrolyte<br />

interfacial reaction kinetics. In most solid oxide fuel cell<br />

designs, the electrolyte layer ranges in thickness from 40<br />

to 200 microns. The maximum power is less than<br />

400 milliwatts per square centimeter when operated at<br />

1000°C. Recent work has shown that solid oxide fuel<br />

cells made with thin electrolyte layers (~10 microns) that<br />

were produced using colloidal processing methods may<br />

allow both a reduction in operating temperature and an<br />

increase in power to greater than 1 watt per square<br />

centimeter. Further reduction in the thickness of the<br />

electrolyte layers that were produced using colloidal<br />

processes is considered impractical without introducing<br />

pinholes and other defects detrimental to solid oxide fuel<br />

cells operation. Vapor deposition methods available at<br />

330 FY 2000 <strong>Laboratory</strong> Directed Research and Development Annual Report<br />

<strong>PNNL</strong> allow the production of very thin (micrometer<br />

scale) electrolyte layers that will permit solid oxide fuel<br />

cells operating temperatures to be lowered by hundreds of<br />

degrees while maintaining high power outputs.<br />

Approach<br />

This project focused on the production of thin yttriastabilized<br />

zirconia electrolyte layers using reactive<br />

magnetron sputtering. The process involves removal of<br />

atomic species from an yttrium/zirconium metal alloy<br />

target by bombarding it with ionized argon atoms in the<br />

presence of a background oxygen concentration. The<br />

oxygen atoms combine with the atomized metal to<br />

produce oxide coatings on substrates placed in the path of<br />

the sputtered material. To produce yttria-stabilized<br />

zirconia that is stable at temperatures required to operate<br />

fuel cells, the yttria-stabilized zirconia deposit was made<br />

with an yttrium doping at an elevated temperature. The<br />

yttria-stabilized zirconia thin film electrodes formed in<br />

this study were produced from yttrium/zirconium targets<br />

containing either 7 or 12 atom percent yttrium and with<br />

the substrates heated to temperatures of up to 600°C<br />

during the deposits.<br />

The substrates used for the yttria-stabilized zirconia<br />

electrolyte deposit were thin wafers of a porous<br />

nickel/zirconia cermet that was produced using<br />

conventional tape casting methods. The cermet layer<br />

acted both as a support for the yttria-stabilized zirconia<br />

electrolyte layer and as the fuel-side electrode for the fuel<br />

cell. The anodes were pre-sintered in air at 1350°C for<br />

1 hour. The porous air-side electrode of strontium-doped<br />

lanthanum manganite was applied to the exposed face of<br />

the yttria-stabilized zirconia electrolyte using a<br />

conventional ceramic screen-printing process after the<br />

electrolyte deposition was completed. The cathode was<br />

sintered on at 1200°C. A platinum grid was screen<br />

printed and sintered on each electrode as a current<br />

collector. Platinum meshes with attached current and<br />

voltage leads were sintered to the platinum current<br />

collectors.

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