Document Type

Dissertation

Degree

Doctor of Philosophy (PhD)

Major/Program

Materials Science and Engineering

First Advisor's Name

W. Kinzy Jones

First Advisor's Committee Title

Committee Chair

Second Advisor's Name

Norman D. H. Munroe

Third Advisor's Name

Chenzhong Li

Fourth Advisor's Name

Chunlei Wang

Date of Defense

3-26-2009

Abstract

Miniature direct methanol fuel cells (DMFCs) are promising micro power sources for portable application. Low temperature cofired ceramic (LTCC), a competitive technology for current MEMS based fabrication, provides cost-effective mass manufacturing route for miniature DMFCs. Porous silver tape is adapted as electrodes to replace the traditional porous carbon electrodes due to its compatibility to LTCC processing and other electrochemical advantages. Electrochemical evaluation of silver under DMFCs operating conditions demonstrated that silver is a good electrode for DMFCs because of its reasonable corrosion resistance, low passivating current, and enhanced catalytic effect. Two catalyst loading methods (cofiring and postfiring) of the platinum and ruthenium catalysts are evaluated for LTCC based processing. The electrochemical analysis exhibits that the cofired path out-performs the postfiring path both at the anode and cathode. The reason is the formation of high surface area precipitated whiskers.

Self-constraint sintering is utilized to overcome the difficulties of the large difference of coefficient of thermal expansion (CTE) between silver and LTCC (Dupont 951) tape during cofiring. The graphite sheet employed as a cavity fugitive insert guarantees cavity dimension conservation.

Finally, performance of the membrane electrode assembly (MEA) with the porous silver electrode in the regular graphite electrode based cell and the integrated cofired cell is measured under passive fuel feeding condition. The MEA of the regular cell performs better as the electrode porosity and temperature increased. The power density of 10 mWcm'2 was obtained at ambient conditions with 1M methanol and it increased to 16 mWcm'2 at 50 °C from an open circuit voltage of 0.58V. For the integrated prototype cell, the best performance, which depends on the balance methanol crossover and mass transfer at different temperatures and methanol concentrations, reaches 1.13 mWcm'2 at 2M methanol solution at ambient pressure. The porous media pore structure increases the methanol crossover resistance. As temperature increased to 60 °C, the device increases to 2.14 mWcm'2.

Identifier

FI15101497

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