Journal of the American Chemical Society,
Год журнала:
2025,
Номер
147(6), С. 5398 - 5407
Опубликована: Янв. 31, 2025
Anion-exchange
membrane
fuel
cell
(AEMFC)
is
a
cost-effective
hydrogen-to-electricity
conversion
technology
under
zero-emission
scenario.
However,
the
sluggish
kinetics
of
anodic
hydrogen
oxidation
reaction
(HOR)
impedes
commercial
implementation
AEMFCs.
Here,
we
develop
Pd
single-atom-embedded
Ni3N
catalyst
(Pd1/Ni3N)
with
unconventional
Pd1Ni2
trimer
sites
to
drive
efficient
and
durable
HOR
in
alkaline
media.
Integrating
theoretical
experimental
analyses,
demonstrate
that
dual
achieve
"*H
on
Pd1Ni2-HV
+
*OH
Pd1Ni2-HN"
adsorption
mode,
effectively
weakening
overstrong
*H
adsorptions
pristine
Ni3N.
Owing
unique
coordination
mode
atomically
dispersed
catalytic
sites,
resulting
Pd1/Ni3N
delivers
high
intrinsic
mass
activity
together
excellent
antioxidation
capability
CO
tolerance.
Specifically,
reaches
7.54
A
mgPd-1
at
overpotential
50
mV.
The
AEMFC
employing
as
anode
displays
power
density
31.7
W
an
ultralow
precious
metal
loading
only
0.023
mgPd
cm-2.
This
study
provides
guidance
for
design
high-performance
atomic
level.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(42)
Опубликована: Сен. 2, 2023
Abstract
Designing
novel
single‐atom
catalysts
(SACs)
supports
to
modulate
the
electronic
structure
is
crucial
optimize
catalytic
activity,
but
rather
challenging.
Herein,
a
general
strategy
proposed
utilize
metalloid
properties
of
trap
and
stabilize
single‐atoms
with
low‐valence
states.
A
series
supported
on
surface
tungsten
carbide
(M‐WC
x
,
M=Ru,
Ir,
Pd)
are
rationally
developed
through
facile
pyrolysis
method.
Benefiting
from
WC
exhibit
weak
coordination
W
C
atoms,
resulting
in
formation
active
centers
similar
metals.
The
unique
metal‐metal
interaction
effectively
stabilizes
single
atoms
improves
orbital
energy
level
distribution
sites.
As
expected,
representative
Ru‐WC
exhibits
superior
mass
activities
7.84
62.52
mg
Ru
−1
for
hydrogen
oxidation
evolution
reactions
(HOR/HER),
respectively.
In‐depth
mechanistic
analysis
demonstrates
that
an
ideal
dual‐sites
cooperative
mechanism
achieves
suitable
adsorption
balance
H
ad
OH
energetically
favorable
Volmer
step.
This
work
offers
new
guidance
precise
construction
highly
SACs.
ACS Applied Nano Materials,
Год журнала:
2023,
Номер
7(1), С. 1138 - 1145
Опубликована: Дек. 20, 2023
Integrating
metal-based
species
with
a
carbon
matrix
is
promising
approach
for
fabricating
inexpensive,
durable,
and
efficient
electrocatalysts.
Herein,
NiSe2-decorated
N-doped
polyhedra
(NC)
are
prepared
as
electrocatalysts
hydrogen
evolution
reaction
(HER)
by
template-assisted
approach.
The
optimal
NC-NiSe2
delivers
extraordinary
catalytic
activities
toward
HER
in
wide
pH
range,
overpotentials
of
127
mV
0.5
M
H2SO4,
226
1
PBS,
205
KOH
to
drive
current
density
10
mA
cm–2.
In
addition,
this
catalyst
undergoes
fast
kinetics
via
Volmer–Heyrovsky
mechanism
exhibits
excelent
long-term
durability
48
h
the
full
media.
During
electrocatalysis,
when
electrons
pass
through
NC
surface
NiSe2
particles,
water
molecules
at
active
sites
reduced,
then
released.
excellent
activity
mainly
benefit
from
hierarchically
porous
architecture
well
synergistic
interaction
nanoparticles
matrix,
which
not
only
significantly
boost
electronic
conductivity
generate
plentiful
but
also
guarantee
chemical
structural
stabilities
species.
This
work
unravels
deep
insights
into
exploration
carbon-supported
metal
chalcogenides
highly
full-pH
values.
Energy & Environmental Science,
Год журнала:
2024,
Номер
17(12), С. 3960 - 4009
Опубликована: Янв. 1, 2024
The
general
principles
in
terms
of
reactivity
and
stability
to
design
efficient
electrocatalysts
for
the
alkaline
hydrogen
oxidation
reaction
are
reviewed.
performance
catalysts
anion-exchange
membrane
fuel
cells
is
further
discussed.
National Science Review,
Год журнала:
2024,
Номер
11(10)
Опубликована: Июнь 3, 2024
Proton
activity
at
the
electrified
interface
is
central
to
kinetics
of
proton-coupled
electron
transfer
(PCET)
reactions
in
electrocatalytic
oxygen
reduction
reaction
(ORR).
Here,
we
construct
an
efficient
Fe
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 10, 2025
Abstract
Anion
exchange
membrane
fuel
cells
(AEMFCs)
are
among
the
most
promising
sustainable
electrochemical
technologies
to
help
solve
energy
challenges.
Compared
proton
(PEMFCs),
AEMFCs
offer
a
broader
choice
of
catalyst
materials
and
less
corrosive
operating
environment
for
bipolar
plates
membrane.
This
can
lead
potentially
lower
costs
longer
operational
life
than
PEMFCs.
These
significant
advantages
have
made
highly
competitive
in
future
cell
market,
particularly
after
advancements
developing
non‐platinum‐group‐metal
anode
electrocatalysts,
anion
membranes
ionomers,
understanding
relationships
between
conditions
mass
transport
AEMFCs.
review
aims
compile
recent
literature
provide
comprehensive
three
key
areas:
i)
mechanisms
hydrogen
oxidation
reaction
(HOR)
oxygen
reduction
(ORR)
alkaline
media;
ii)
synthesis
routes
structure‐property
cutting‐edge
HOR
ORR
as
well
ionomers;
iii)
conditions,
including
water
management
impact
CO
2
.
Finally,
based
on
these
aspects,
development
perspectives
proposed.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(31), С. 17485 - 17494
Опубликована: Авг. 1, 2023
Converting
hydrogen
chemical
energy
into
electrical
by
fuel
cells
offers
high
efficiencies
and
environmental
advantages,
but
ultrapure
(over
99.97%)
is
required;
otherwise,
the
electrode
catalysts,
typically
platinum
on
carbon
(Pt/C),
will
be
poisoned
impurity
gases
such
as
ammonia
(NH3).
Here
we
demonstrate
remarkable
NH3
resistivity
over
a
nickel-molybdenum
alloy
(MoNi4)
modulated
chromium
(Cr)
dopants.
The
resultant
Cr-MoNi4
exhibits
activity
toward
alkaline
oxidation
can
undergo
10,000
cycles
without
apparent
decay
in
presence
of
2
ppm
NH3.
Furthermore,
cell
assembled
with
this
catalyst
retains
95%
initial
peak
power
density
even
when
(10
ppm)/H2
was
fed,
whereas
output
reduces
to
61%
value
for
Pt/C
catalyst.
Experimental
theoretical
studies
reveal
that
Cr
modifier
not
only
creates
electron-rich
states
restrain
lone-pair
electron
donation
also
downshifts
d-band
center
suppress
d-electron
back-donation,
synergistically
weakening
adsorption.
Angewandte Chemie,
Год журнала:
2023,
Номер
135(42)
Опубликована: Сен. 2, 2023
Abstract
Designing
novel
single‐atom
catalysts
(SACs)
supports
to
modulate
the
electronic
structure
is
crucial
optimize
catalytic
activity,
but
rather
challenging.
Herein,
a
general
strategy
proposed
utilize
metalloid
properties
of
trap
and
stabilize
single‐atoms
with
low‐valence
states.
A
series
supported
on
surface
tungsten
carbide
(M‐WC
x
,
M=Ru,
Ir,
Pd)
are
rationally
developed
through
facile
pyrolysis
method.
Benefiting
from
WC
exhibit
weak
coordination
W
C
atoms,
resulting
in
formation
active
centers
similar
metals.
The
unique
metal‐metal
interaction
effectively
stabilizes
single
atoms
improves
orbital
energy
level
distribution
sites.
As
expected,
representative
Ru‐WC
exhibits
superior
mass
activities
7.84
62.52
mg
Ru
−1
for
hydrogen
oxidation
evolution
reactions
(HOR/HER),
respectively.
In‐depth
mechanistic
analysis
demonstrates
that
an
ideal
dual‐sites
cooperative
mechanism
achieves
suitable
adsorption
balance
H
ad
OH
energetically
favorable
Volmer
step.
This
work
offers
new
guidance
precise
construction
highly
SACs.
Advanced Materials,
Год журнала:
2024,
Номер
36(38)
Опубликована: Июль 24, 2024
Constructing
well-defined
active
multisites
is
an
effective
strategy
to
break
linear
scaling
relationships
develop
high-efficiency
catalysts
toward
multiple-intermediate
reactions.
Here,
dual-intermetallic
heterostructure
composed
of
tungsten-bridged
Co
Inorganic Chemistry Frontiers,
Год журнала:
2024,
Номер
11(7), С. 2029 - 2038
Опубликована: Янв. 1, 2024
Benefiting
from
d–d
electron
interaction
within
the
constituent
metals,
as-prepared
FeCoNiMoW
HEAs
exhibit
optimized
adsorption
energy
for
critical
intermediates,
and
attain
improved
catalytic
ability
inoxidizability
alkaline
HOR.
