Role of two carbon phases in oxygen reduction
reaction on the CoePPyeC catalyst
Hoon T. Chung, Gang Wu, Qing Li, Piotr Zelenay
*
Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, NM 87545, USA
article info
Article history:
Available online 21 June 2014
Keywords:
Polymer electrolyte fuel cell (PEFC)
Oxygen reduction reaction
Non-precious metal catalyst
Carbon
Polypyrrole
abstract
In spite of a significant progress in their performance in recent years, the heat-treated
metal-nitrogenecarbon (M-NeC) non-precious metal catalysts for oxygen reduction reac-
tion (ORR) at the cathode of polymer electrolyte fuel cells (PEFCs) are in need of further
improvement to match the activity and, especially, the stability of Pt-based nanoparticle
catalysts of oxygen reduction. A better understanding of the role of individual components
in M-NeC catalysts is vital for the development of more advanced formulations. In this
work, using a cobalt-polypyrrole-carbon catalyst system as an example, we demonstrate
that carbon originating from the organic nitrogen precursor (ONP) has different properties
than the carbon support. Unlike the carbon originating from polypyrrole, the support
carbon helps to enhance ORR performance but negatively impacts the stability. To the best
of our knowledge, this may be the first time that the properties of the ONP-derived carbon
are being differentiated from the properties of carbon in the carbon support, emphasizing
the potential importance of carbon phases in ORR electrocatalysis on heat-treated M-NeC
catalysts.
Copyright © 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights
reserved.
Introduction
Although the polymer electrolyte fuel cell (PEFC) has long been
recognized as a potential power source for zero-emission ve-
hicles, it still remains economically uncompetitive with the
internal combustion engine. Among other major PEFC com-
ponents, the platinum (Pt) catalyst in the cathode and anode
are the most expensive single cell constituent, accounting for
almost a half of the stack cost. The necessary cost reduction
can be achieved by either lowering platinum content in fuel
cell electrodes or eliminating altogether eliminating Pt. This is
especially important for the cathode where the intrinsically
sluggish oxygen reduction reaction (ORR) requires
substantially higher Pt loading than the much faster hydrogen
oxidation reaction (HOR) at the anode.
The potential use of non-precious metal materials to Pt
replacement in the PEFC cathode has attracted much atten-
tion in recent years. The most promising catalysts are metal-
nitrogenecarbon (M-NeC) formulations obtained by heat-
treating precursors of transition metals (mainly Fe and Co),
nitrogen, and carbon [1e6]. Though the exact nature of the
active site(s) developed during heat treatment still remains
the subject of intense research, all components of M-NeC
catalysts (transition metal, nitrogen functionalities, and spe-
cific carbons) have been reported to affect the ORR activity of
such catalysts. The role of metal in M-NeC catalysts is
controversial, with some groups viewing the transition metal
* Corresponding author. Tel.: þ1 505 667 0197; fax: þ1 505 605 4292.
E-mail address: zelenay@lanl.gov (P. Zelenay).
Available online at www.sciencedirect.com
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journal homepage: www.elsevier.com/locate/he
international journal of hydrogen energy 39 (2014) 15887 e15893
http://dx.doi.org/10.1016/j.ijhydene.2014.05.137
0360-3199/Copyright © 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.