Electronic Structure,
Год журнала:
2024,
Номер
6(2), С. 023001 - 023001
Опубликована: Март 7, 2024
Abstract
The
wordwide
energy
demands
and
the
surge
towards
a
net-zero
sustainable
society
let
researchers
set
goal
end
of
carbon
cycle.
This
has
enormously
exaggerated
electrocatalytic
processes
such
as
water
splitting,
CO
2
capture
reduction
nitrogen
reaction
(NRR)
safe
green
alternative
these
involve
utilization
renewable
power.
Interestingly,
NH
3
produced
from
NRR
been
realized
future
fuel
in
terms
safer
H
storage
transportation.
Nevertheless,
to
scale
up
production
electrochemically,
benevolent
catalyst
needs
be
developed.
More
interestingly,
electronic
features
that
actually
contribute
interaction
binding
between
adsorbate
intermediates
should
analyzed
can
tuned
based
on
our
requirements
obtain
desired
high-standard
goals
synthesis.
current
topical
review
aims
provide
an
illustrative
understanding
experimental
theoretical
descriptors
are
likely
influence
structure
catalysts
for
NRR.
We
have
widely
covered
detailed
explanation
regarding
work
function,
d-band
center
effect
structures
catalysts.
While
summarizing
same,
we
there
several
discrepancies
this
field,
which
not
discussed
could
misleading
newcomers
field.
Thus,
briefed
limitations
diverging
explanations
provided
few
directions
looked
upon
overcome
issues.
Abstract
Innovative
advances
in
the
exploitation
of
effective
electrocatalytic
materials
for
reduction
nitrogen
(N
2
)
to
ammonia
(NH
3
are
highly
required
sustainable
production
fertilizers
and
zero‐carbon
emission
fuel.
In
order
achieve
footprints
renewable
NH
production,
electrochemical
N
reaction
(NRR)
provides
a
favorable
energy‐saving
alternative
but
it
requires
more
active,
efficient,
selective
catalysts.
current
work,
sulfur
vacancy
(Sv)‐rich
NiCo
S
4
@MnO
heterostructures
efficaciously
fabricated
via
facile
hydrothermal
approach
followed
by
heat
treatment.
The
urchin‐like
Sv‐NiCo
serve
as
cathodes,
which
demonstrate
an
optimal
yield
57.31
µg
h
−1
mg
cat
Faradaic
efficiency
20.55%
at
−0.2
V
versus
reversible
hydrogen
electrode
(RHE)
basic
electrolyte
owing
synergistic
interactions
between
MnO
.
Density
functional
theory
(DFT)
simulation
further
verifies
that
Co‐sites
beneficial
lowering
energy
threshold
adsorption
successive
protonation.
Distinctive
micro/nano‐architectures
exhibit
high
NRR
activities
might
motivate
researchers
explore
concentrate
on
development
ambient
generation.
ACS Applied Materials & Interfaces,
Год журнала:
2023,
Номер
15(9), С. 11812 - 11826
Опубликована: Фев. 21, 2023
TM-Nx
is
becoming
a
comforting
catalytic
center
for
sustainable
and
green
ammonia
synthesis
under
ambient
conditions,
resulting
in
increasing
interest
single-atom
catalysts
(SACs)
the
electrochemical
nitrogen
reduction
reaction
(NRR).
However,
given
poor
activity
unsatisfactory
selectivity
of
existing
catalysts,
it
remains
long-standing
challenge
to
design
efficient
fixation.
Currently,
two-dimensional
(2D)
graphitic
carbon-nitride
substrate
provides
abundant
evenly
distributed
holes
stably
supporting
transition-metal
atoms,
which
presents
fascinating
prospect
overcoming
this
promoting
NRR.
An
emerging
holey
skeleton
with
C10N3
stoichiometric
ratio
(g-C10N3)
from
supercell
graphene
constructed,
outstanding
electric
conductivity
achieving
high-efficiency
NRR
due
Dirac
band
dispersion.
Herein,
high-throughput
first-principles
calculation
carried
out
evaluate
feasibility
π-d
conjugated
SACs
single
TM
atom
anchored
on
g-C10N3
(TM
=
Sc-Au)
We
find
that
W
metal
embedded
(W@g-C10N3)
can
compromise
ability
adsorb
key
target
species
(N2H
NH2),
hence
acquiring
an
optimal
behavior
among
27
TM-candidates.
Our
calculations
demonstrate
W@g-C10N3
shows
well-suppressed
HER
and,
impressively,
low
energy
cost
-0.46
V.
Additionally,
all-around
descriptors
are
proposed
uncover
fundamental
mechanism
activity,
3D
volcano
plot
(limiting
potential,
screening
strategy,
electron
origin)
uncovers
trend,
quick
prescreening
numerous
candidates.
Overall,
strategy
structure-
activity-based
TM-Nx-containing
unit
will
offer
useful
insight
further
theoretical
experimental
attempts.
Nano-Micro Letters,
Год журнала:
2024,
Номер
16(1)
Опубликована: Янв. 16, 2024
Abstract
Renewable
energy
driven
N
2
electroreduction
with
air
as
nitrogen
source
holds
great
promise
for
realizing
scalable
green
ammonia
production.
However,
relevant
out-lab
research
is
still
in
its
infancy.
Herein,
a
novel
Sn-based
MXene/MAX
hybrid
abundant
Sn
vacancies,
Sn@Ti
CT
X
/Ti
SnC–V,
was
synthesized
by
controlled
etching
SnC
MAX
phase
and
demonstrated
an
efficient
electrocatalyst
electrocatalytic
reduction.
Due
to
the
synergistic
effect
of
heterostructure,
existence
vacancies
highly
dispersed
active
sites,
obtained
SnC–V
exhibits
optimal
NH
3
yield
28.4
µg
h
−1
mg
cat
excellent
FE
15.57%
at
−
0.4
V
versus
reversible
hydrogen
electrode
0.1
M
Na
SO
4
,
well
ultra-long
durability.
Noticeably,
this
catalyst
represents
satisfactory
rate
10.53
home-made
simulation
device,
where
commercial
electrochemical
photovoltaic
cell
employed
power
source,
ultrapure
water
feed
stock.
The
as-proposed
strategy
potential
toward
production
terms
financial
cost
according
systematic
technical
economic
analysis.
This
work
significance
large-scale
Abstract
Ammonia
serves
as
a
crucial
chemical
raw
material
and
hydrogen
energy
carrier.
Aqueous
electrocatalytic
nitrogen
reduction
reaction
(NRR),
powered
by
renewable
energy,
has
attracted
tremendous
interest
during
the
past
few
years.
Although
some
achievements
have
been
revealed
in
aqueous
NRR,
significant
challenges
also
identified.
The
activity
selectivity
are
fundamentally
limited
activation
competitive
evolution.
This
review
focuses
on
hurdles
of
delves
into
complementary
strategies,
including
materials
design
system
optimization
(reactor,
electrolyte,
mediator).
Then,
it
introduces
advanced
interdisciplinary
technologies
that
recently
emerged
for
using
high‐energy
physics
such
plasma
triboelectrification.
With
better
understanding
corresponding
mechanisms
coming
years,
these
potential
to
be
extended
further
applications.
provides
insight
stability
different
systems.
We
then
recommend
rigorous
detailed
protocol
investigating
NRR
performance
highlight
several
research
directions
this
exciting
field,
coupling
with
applications,
situ/operando
characterizations,
theoretical
calculations.
Nano Letters,
Год журнала:
2024,
Номер
24(2), С. 748 - 756
Опубликована: Янв. 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.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 10, 2025
Abstract
Electrocatalytic
nitrogen
reduction
reaction
(NRR)
is
a
potential
strategy
for
green
synthesis
of
ammonia.
However,
the
lack
efficient
catalysts
with
both
high
activity
and
selectivity
restricts
development
electrocatalytic
NRR.
In
this
study,
simple
water‐based
redox
method
used
to
synthesize
core–shell
nanoparticle
catalyst
2D
Mn
3
O
4
as
shell
core.
The
rich
interface
low‐coordination
helps
provide
more
active
sites
At
same
time,
nucleus
gives
electrons
shell,
jointly
promotes
adsorption
activation
nitrogen,
well
enhancement
NRR
activity.
Moreover,
designed
hydrophobicity,
which
effectively
reduces
side
hydrogen
evolution
H
proton
generated
from
water
dissociation,
improved.
0.1
m
Na
2
SO
,
ammonia
yield
In@Mn
89.44
µg
h
−1
mg
cat
(−0.9
V
vs
RHE)
maximum
Faradaic
efficiency
27.01%
at
−0.7
(vs
RHE),
superior
most
reported
catalysts.
unique
structure
design
low
coordination
insights
regulation
nitrogen–water
environment
rational
advanced
electrocatalysts.