Transition-metal-
and nitrogen-codoped carbide-derived carbon/carbon
nanotube composites (M-N-CDC/CNT) have been prepared, characterized,
and used as cathode catalysts in anion-exchange membrane fuel cells
(AEMFCs). As transition metals, cobalt, iron, and a combination of
both have been investigated. Metal and nitrogen are doped through
a simple high-temperature pyrolysis technique with 1,10-phenanthroline
as the N precursor. The physicochemical characterization shows the
success of metal and nitrogen doping as well as very similar morphologies
and textural properties of all three composite materials. The initial
assessment of the oxygen reduction reaction (ORR) activity, employing
the rotating ring–disk electrode method, indicates that the
M-N-CDC/CNT catalysts exhibit a very good electrocatalytic performance
in alkaline media. We find that the formation of HO
2
–
species in the ORR catalysts depends on the specific
metal composition (Co, Fe, or CoFe). All three materials show excellent
stability with a negligible decline in their performance after 10000
consecutive potential cycles. The very good performance of the M-N-CDC/CNT
catalyst materials is attributed to the presence of M-N
x
and pyridinic-N moieties as well as both micro-
and mesoporous structures. Finally, the catalysts exhibit excellent
performance in in situ tests in H
2
/O
2
AEMFCs,
with the CoFe-N-CDC/CNT reaching a current density close to 500 mA
cm
–2
at 0.75 V and a peak power density (
P
max
) exceeding 1 W cm
–2
. Additional
tests show that
P
max
reaches 0.8 W cm
–2
in an H
2
/CO
2
-free air system
and that the CoFe-N-CDC/CNT material exhibits good stability under
both AEMFC operating conditions.
Cobalt-
and nitrogen-doped carbide-derived carbon/carbon nanotube
(CDC/CNT) composites are prepared and used as oxygen reduction reaction
(ORR) electrocatalysts for an anion exchange membrane fuel cell (AEMFC)
cathode. For the doping, high-temperature pyrolysis is applied using
a cobalt salt and a nitrogen precursor (either dicyandiamide, urea,
or melamine). During the doping, (i) new mesopores are formed as confirmed
by the N2 physisorption results, (ii) atomically dispersed
cobalt is present on the catalysts as detected by scanning transmission
electron microscopy, and (iii) N-pyridinic and Co–N4 are the dominant N-containing species as shown by X-ray photoelectron
spectroscopy. This indicates that using the composite of CDC and CNTs
as well as the cobalt salt and nitrogen precursor is advantageous
for the preparation of electrocatalysts. All three catalyst materials
demonstrate similarly good electrocatalytic activity toward O2 electroreduction in alkaline medium and excellent stability
after 10000 repetitive potential cycles. The Co-N-CDC/CNT catalyst
as the cathode material together with a hexamethyl-p-terphenyl poly(benzimidazolium) (HMT-PMBI) membrane exhibits excellent
AEMFC performance by reaching maximum power density of 577 mW cm–2.
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