THESIS
Investigation
of titanium nitride as catalyst support material and development of durable
electrocatalysts for proton exchange membrane fuel cells
Avasarala, Bharat K., Ph.D., STATE UNIVERSITY OF NEW YORK AT ALBANY,
2011
Abstract:
The impending energy and climatic crisis makes it imperative for human society
to seek non-fossil based alternative sources for our energy needs. Although
many alternative energy technologies are currently being developed, fuel cell
technology provides energy solutions, which satisfy a wide range of
applications. But the current fuel cell technology is far from its target of
large scale commercialization mainly because of its high cost and poor
durability. Considerable work has been done in reducing the cost but its
durability still needs significant improvement. Of the various materials in a
PEM fuel cell, the degradation of electrocatalyst affects its durability the
most, leading to performance loss. Carbon black (C) support corrosion plays a
significant role in the electrocatalyst degradation and its severe affects due
to potential cycling has been identified through my research.
Author introduces titanium nitride nanoparticles (TiN NP) as
alternative catalyst supports replacing carbon black. TiN NP has higher
electrical conductivity and corrosion resistance compared to that of C. The
physical and electrochemical properties of TiN NP were studied and the Pt/TiN
electrocatalyst was synthesized using polyol process. Upon optimizing using
DOE, for desired catalyst particle size and activity, Pt/TiN is shown to have
higher catalytic performance than conventional Pt/C.
TiN NP are significantly influenced by the
electrochemical conditions and show 'active' or 'passive' nature depending on
the temperature and acidic concentration; and a temperature dependence model is
proposed to understand the active/passive nature of TiN NP. A one-to-one
comparison between TiN NP and C electrodes under similar electrochemical conditions
show a superior performance of TiN NP as a catalyst support. The durability of
the Pt/TiN electrocatalyst is also tested and it agrees well with the proposed
model of active/passive nature of the TiN NP. Through theoretical calculation
and spectroscopic characterization, the higher catalytic performance of the
Pt/TiN electrocatalyst is explained. The degradation mechanism and the dominant
pathways are identified for the novel Pt/TiN electrocatalyst. It is shown that,
unlike conventional Pt/C, the novel Pt/TiN degrades predominantly via Pt
particle agglomeration mechanism due to its higher support to Pt particle
ratio.
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