Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(30)
Published: May 14, 2024
Transition-metal
carbides
with
metallic
properties
have
been
extensively
used
as
electrocatalysts
due
to
their
excellent
conductivity
and
unique
electronic
structures.
Herein,
NbC
nanoparticles
decorated
carbon
nanofibers
(NbC@CNFs)
are
proposed
an
efficient
robust
catalyst
for
electrochemical
synthesis
of
ammonia
from
nitrate/nitrite
reduction,
which
achieves
a
high
Faradaic
efficiency
(FE)
94.4
%
large
yield
30.9
mg
h
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(10), P. 7907 - 7916
Published: May 6, 2024
Electrochemical
nitrate
reduction
(NO3RR)
offers
an
ecofriendly
way
for
ammonia
production.
However,
improving
the
sluggish
kinetics
of
such
a
multistep
reaction
still
remains
challenging.
Herein,
asymmetry
strategy
is
proposed
to
adjust
charge
distribution
active
centers
on
metallene
by
presenting
novel
symmetry-broken
medium-entropy-alloy
(MEA)
via
heteroatom
alloying.
Benefiting
from
maximized
exposure
well-regulated
sites,
proof-of-concept
PdCuCo
MEA
delivers
near
100%
NH3
Faradaic
efficiency
in
both
neutral
and
alkaline
electrolytes,
along
with
record-high
yield
rate
over
532.5
mg
h–1
mgcat–1.
Moreover,
it
enables
99.7%
conversion
industrial
wastewater
level
6200
ppm
drinkable
water
level.
Detailed
studies
further
revealed
that
redistribution
induced
elemental
electronegativity
difference
metallene,
which
will
weaken
N–O
bond
*NO,
thus
reducing
energy
barrier
rate-determining
step.
Meanwhile,
competitive
HER
formation
NO2–
are
also
hindered.
We
believe
our
this
work
shed
light
design
efficient
NO3RR
catalysts
more
practical
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 15, 2024
Abstract
The
underutilization
of
active
sites
limits
the
performance
enhancement
2D
transition
metal
boride
(MBene)
in
electrocatalytic
nitrogen
reduction
reaction
(NRR).
Herein,
a
highly
efficient
NRR
electrocatalyst
with
S
atoms
bridging
Fe
and
Mo
on
surface
MBene
is
successfully
constructed
by
using
an
site
electron
optimization
strategy,
which
increases
charge
density
around
enhances
activation
ability
catalyst
to
N
2
molecules.
It
noteworthy
that
FeS
‐MBene
demonstrates
low
intrinsic
potential
for
(−0.2
V
vs
RHE).
more
favorable
adsorption
comparison
hydrogen
atoms,
thereby
it
can
effectively
inhibit
evolution
(HER).
Under
−0.2
versus
RHE,
ammonia
yield
rate
37.13
±
1.31
µg
h
−1
mg
,
FE
55.97
2.63%.
Density
functional
theory
(DFT)
calculations
demonstrate
serves
as
.
formation
heterostructure
transfer,
resulting
becoming
electron‐rich
state
favor
subsequent
hydrogenation
steps.
This
work
offers
significant
insights
into
design
utilization
MBene‐based
catalysts
NRR.
Nano Letters,
Journal Year:
2024,
Volume and Issue:
24(2), P. 748 - 756
Published: Jan. 3, 2024
The
electrochemical
N2
reduction
reaction
(NRR)
is
a
green
and
energy-saving
sustainable
technology
for
NH3
production.
However,
high
activity
selectivity
can
hardly
be
achieved
in
the
same
catalyst,
which
severely
restricts
development
of
NRR.
In2Se3
with
partially
occupied
p-orbitals
suppress
H2
evolution
(HER),
shows
excellent
presence
VIn
simultaneously
provide
active
sites
confine
Re
clusters
through
strong
charge
transfer.
Additionally,
well-isolated
stabilized
on
by
confinement
effect
result
Re-VIn
maximum
availability.
By
combining
as
dual
spontaneous
adsorption
activation,
NRR
performance
enhanced
significantly.
As
result,
Re-In2Se3-VIn/CC
catalyst
delivers
yield
rate
(26.63
μg
h–1
cm–2)
FEs
(30.8%)
at
−0.5
V
vs
RHE.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(30)
Published: May 14, 2024
Transition-metal
carbides
with
metallic
properties
have
been
extensively
used
as
electrocatalysts
due
to
their
excellent
conductivity
and
unique
electronic
structures.
Herein,
NbC
nanoparticles
decorated
carbon
nanofibers
(NbC@CNFs)
are
proposed
an
efficient
robust
catalyst
for
electrochemical
synthesis
of
ammonia
from
nitrate/nitrite
reduction,
which
achieves
a
high
Faradaic
efficiency
(FE)
94.4
%
large
yield
30.9
mg
h