The micro direct methanol fuel cell (µDMFC) has been proposed as a candidate to power portable applications. The device can operate at room temperature on inexpensive, energy-dense methanol fuel, and it can be easily "recharged" by fuel refilling. Microfabrication techniques could be one route for the realization of such tiny devices. It is a mature technology, suitable for mass production, where versatile structuring is available at the micro and nano regime. Carbon black supported catalysts synthesized by wet chemistry methods are not readily applicable for standard microfabrication techniques. Atomic layer deposition (ALD), on the other hand, is a highly suitable and still relatively unexplored approach for the synthesis of noble metal catalysts. It is a vapor phase growth method, primarily used to deposit thin lms. ALD is based on self-limiting chemical reactions of alternately injected precursors on the sample surface. Its unique growth characteristic enables conformal and uniform lms of controlled thickness and composition. In certain conditions ALD commences by island growth, resulting in discrete nanoparticle formation, which is generally preferred for catalytic applications. Pt-Ru is the best catalyst toward the methanol oxidation reaction (MOR). In the work described in this PhD dissertation, two series of Pt-Ru ALD catalysts supported on nitrogen-doped multi-walled carbon nanotubes (N-CNTs) have been evaluated toward the CO oxidation and MOR at room temperature in a three-electrode electrochemical cell. The first series was comprised of Pt-Ru ALD catalysts of various Ru compositions, between 0 and 100 at.%. For the compositions investigated, the best catalyst had a Ru composition of 29 at.%. In the second series Ru-decorated Pt catalysts of various Ru loadings, i.e., various Ru ALD cycles (1, 2, 5, 10 and 20), were investigated. The Pt nanoparticles decorated with 2 Ru ALD cycles exhibited highest catalytic activity, which also outperformed the best catalyst of the first series. In addition, a Si-based fuel cell design with ALD catalysts is presented, and its anode was evaluated toward the MOR.
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Thomsen, Erik Vilain, Christensen, Leif H.
Department of Micro- and Nanotechnology, Technical University of Denmark, 2013