Electrochimica
Acta
109 (2013) 570–
576
Contents
lists
available
at
ScienceDirect
Electrochimica
Acta
jou
rn
al
hom
ep
age:
www.elsevier.com/locate/elec
tacta
Facile
synthesis
of
palladium–graphene
nanocomposites
and
their
catalysis
for
electro-oxidation
of
methanol
and
ethanol
Yuting
Zhang
a
,
Honghui
Shu
a
,
Gang
Chang
a,∗
,
Kai
Ji
a
,
Munetaka
Oyama
b
,
Xiong
Liu
a
,
Yunbin
He
a,∗
a
Ministry-of-Education
Key
Laboratory
for
the
Green
Preparation
and
Application
of
Functional
Materials,
Faculty
of
Materials
Science
and
Engineering,
Hubei
University,
No.
368
Youyi
Avenue,
Wuchang,
Wuhan
430062,
China
b
Department
of
Material
Chemistry,
Graduate
School
of
Engineering,
Kyoto
University,
Nishikyo-ku,
Kyoto
615-8520,
Japan
a
r
t
i
c
l
e
i
n
f
o
Article
history:
Received
25
April
2013
Received
in
revised
form
25
June
2013
Accepted
10
July
2013
Available online xxx
Keywords:
Graphene
Pd
nanoparticles
Direct
alcohol
fuel
cell
Electro-oxidation
a
b
s
t
r
a
c
t
Well-dispersed
Pd
nanoparticles
(PdNPs)
supported
on
graphene
sheets
were
successfully
prepared
by
a
simple
one-pot
process,
in
which
the
reduction
of
Poly
Vingl
Pyrrolidone-functionalized
graphite
oxide
and
Pd
precursor
was
carried
out
simultaneously
using
ascorbic
acid
as
a
soft
reductant.
The
Pd
nanoparticles
decorated
graphene
composite
(PdNPs/PVP-graphene)
was
characterized
by
X-ray
diffrac-
tion,
transmission
electron
microscopy,
and
X-ray
photoelectron
spectroscopy.
Morphology
and
structure
characterizations
directly
showed
that
Pd
nanoparticles
with
crystallite
size
of
about
8.5
nm
were
evenly
formed
on
graphene.
Catalysis
activity
as
in
fuel
cells
was
investigated
by
further
electrochemical
exper-
iments
including
cyclic
voltammograms
and
chronoamperometric
measurements.
Compared
to
the
commercial
Vulcan
XC-72
supported
Pd
nanoparticles,
PdNPs/PVP-graphene
exhibits
superior
electro-
catalytic
activity
and
stability
toward
electro-oxidation
of
alcohols,
showing
its
potential
use
as
new
electrode
material
for
direct
alcohol
fuel
cells
(DAFCs).
© 2013 Elsevier Ltd. All rights reserved.
1.
Introduction
Due
to
the
continuous
consumption
of
fossil
fuels
and
the
ever-increasing
environmental
problems,
there
has
been
increas-
ing
interest
in
the
development
of
fuel
cell
systems,
especially
the
direct
alcohol
fuel
cells
(DAFCs).
As
a
new
generation
of
power
sources
with
characteristics
of
high
energy
conversion
efficiency,
low
pollutant
emission
and
low
operating
temperature,
fuel
cell
systems
show
great
potential
in
portable
devices
[1–3].
In
recent
years,
Pt-based
catalysts
have
been
widely
studied
as
the
anode
catalysts
for
alcohols
electro-oxidation
in
an
acid
medium.
How-
ever,
the
poisoning
by
CO-like
intermediates
and
the
high
price
of
Pt
hamper
their
extensive
use
in
DAFC
in
the
commercial
mar-
ket
[4–6].
Therefore,
Pd-based
catalysts
have
become
a
hot
topic
of
interest
in
view
of
the
superior
activity,
greater
resistance
to
CO-like
formation
and
lower
cost.
In
order
to
further
maximize
the
catalytic
activity
and
utilization
efficiency
of
Pd,
an
alternative
way
is
to
load
highly
dispersed
Pd
nanostructures
with
controlled
size
and
morphology
on
supporting
materials
having
a
large
specific
surface
area
[7–10].
∗
Corresponding
authors.
Tel.:
+86
27
88661803;
fax:
+86
27
88661803.
E-mail
addresses:
gchanghubei@gmail.com
(G.
Chang),
ybhe@hubu.edu.cn
(Y.
He).
As
supports
for
catalysts
in
DAFC,
various
carbon
materials
have
been
investigated.
The
structure
and
properties
of
the
carbon
sup-
ports
have
significant
effects
on
the
activity
and
stability
of
the
catalysts,
such
as
active
surface
area,
surface
functional
groups
and
the
degree
of
graphitizing
[11,12].
Graphene,
the
two
dimensional
carbon
nanomaterial
with
an
extremely
large
specific
surface
area,
superior
electronic
conductivity,
the
best
mechanical
strength
and
highest
stability
among
carbon
materials,
is
expected
to
be
the
best
candidate
as
the
support
material
[13,14].
And
graphene
supported
metal
or
metal
oxide
nanoparticles
have
demonstrated
high
effi-
ciencies
for
fuel
cell
applications
[2,15].
Therefore,
the
approaches
of
combining
the
graphene
and
Pd
nanoparticles
have
been
stud-
ied
intensively
due
to
their
applicability
to
the
catalysis
of
alcohol
electro-oxidation.
Fundamentally,
graphene
and
metal
nanopar-
ticles
were
prepared
separately
and
then
mixed
in
assistant
of
polymer
or
bridging
agent
[16,17].
But
the
complex
stepwise
proce-
dures
and
use
of
bridging
agents
might
decrease
the
catalysis
ability
of
Pd.
Although
the
reduction
of
metal
ions
and
graphite
oxide
(GO)
could
be
performed
simultaneously
by
some
chemical
reductants,
such
as
hydrazine
and
NaBH
4
,
the
toxicity
of
the
chemical
reagents
and
somewhat
structural
damage
to
the
graphene
support
were
still
a
challenge
[18,19].
In
our
previous
report,
it
was
possible
to
synthesize
Pt
nanopar-
ticles
on
the
graphene
substrate
just
via
reducing
the
platinum
precursor
by
ascorbic
acid,
which
showed
satisfying
attachment
and
high
catalysis
performance
for
the
methanol
oxidation
[19].
0013-4686/$
–
see
front
matter ©
2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.electacta.2013.07.068
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