Advanced Energy Materials,
Год журнала:
2022,
Номер
12(45)
Опубликована: Сен. 30, 2022
Abstract
The
development
of
graphene
has
readily
accelerated
the
research
progress
on
2D
materials.
As
a
representative
family,
transition
metal
dichalcogenides
are
widely
used
in
realms
energy
storage
and
conversion.
In
particular,
molybdenum
diselenide
(MoSe
2
)
captured
widespread
interests
owing
to
its
unique
physical
chemical
properties
remarkable
potential
applications.
Nevertheless,
typically,
electrochemical
property
pristine
MoSe
does
not
meet
expectations,
which
necessitates
exploration
applications
proper
modification
strategies
achieve
full
potential.
Herein,
several
state‐of‐the‐art
molecular
engineering
summarized,
their
energy‐oriented
described.
Furthermore,
insightful
information
significance
methods
improving
perspectives
future
developments
presented.
It
is
anticipated
that
community
can
use
this
review
improve
targeting
practical
application
scenarios.
Abstract
Electrocatalytic
nitrogen
reduction
reaction
(NRR)
represents
a
promising
sustainable
approach
for
NH
3
synthesis.
However,
the
poor
NRR
performance
of
electrocatalysts
is
great
challenge
at
this
stage,
mainly
owing
to
their
low
activity
and
competitive
hydrogen
evolution
(HER).
Herein,
2D
ferric
covalent
organic
framework/MXene
(COF‐Fe/MXene)
nanosheets
with
controllable
hydrophobic
behaviors
are
successfully
prepared
via
multiple‐in‐one
synthetic
strategy.
The
boosting
hydrophobicity
COF‐Fe/MXene
can
effectively
repel
water
molecules
inhibit
HER
enhanced
performances.
By
virtue
ultrathin
nanostructure,
well‐defined
single
Fe
sites,
enrichment
effect,
high
hydrophobicity,
1H,1H,2H,2H‐perfluorodecanethiol
modified
hybrid
shows
yield
41.8
µg
h
−1
mg
cat.
Faradaic
efficiency
43.1%
−0.5
V
versus
RHE
in
0.1
m
Na
2
SO
4
solution,
which
vastly
superior
known
Fe‐based
catalysts
even
noble
metal
catalysts.
This
work
provides
universal
strategy
design
synthesis
non‐precious
high‐efficiency
N
.
Accounts of Chemical Research,
Год журнала:
2022,
Номер
56(1), С. 52 - 65
Опубликована: Ноя. 15, 2022
ConspectusHexagonal
boron
nitrides
(h-BNs)
are
attractive
two-dimensional
(2D)
nanomaterials
that
consist
of
alternating
B
and
N
atoms
layered
honeycomb-like
structures
similar
to
graphene.
They
have
exhibited
unique
properties
promising
application
potentials
in
the
field
energy
storage
transformation.
Recent
advances
utilizing
h-BN
as
a
metal-free
catalyst
oxidative
dehydrogenation
propane
triggered
broad
interests
exploring
catalysis.
However,
h-BN-based
materials
robust
nanocatalysts
heterogeneous
catalysis
still
underexplored
because
limited
methodologies
capable
affording
with
controllable
crystallinity,
abundant
porosity,
high
purity,
defect
engineering,
which
played
important
roles
tuning
their
catalytic
performance.
In
this
Account,
our
recent
progress
addressing
above
issues
will
be
highlighted,
including
synthesis
high-quality
via
both
bottom-up
top-down
pathways
utilization
catalysts
or
supports
tune
interfacial
electronic
on
metal
nanoparticles
(NPs).
First,
we
focus
large-scale
fabrication
nanosheets
(h-BNNSs)
improved
surface
area,
satisfactory
tunable
defects.
derived
from
traditional
approaches
using
trioxide
urea
starting
generally
contains
carbon/oxygen
impurities
has
low
crystallinity.
Several
new
strategies
were
developed
address
issues.
Using
bulk
precursor
gas
exfoliation
liquid
nitrogen,
single-
few-layered
h-BNNS
defects
could
generated.
Amorphous
precursors
converted
crystallinity
assisted
by
magnesium
metallic
flux
successive
dissolution/precipitation/crystallization
procedure.
The
as-fabricated
featured
purity
well
porosity.
An
ionothermal
metathesis
procedure
was
inorganic
molten
salts
(NaNH2
NaBH4)
precursors.
scaffolds
produced
large
scale
yield,
as-afforded
possessed
Second,
as-prepared
library
hydrogenation
reactions
summarized,
they
enhanced
activity
over
counterparts
previous
method.
Third,
interface
modulation
between
NPs
defects'
support
highlighted.
strong
metal-support
interaction
(SMSI)
constructed
without
involving
reducible
oxides
deploying
specific
salts,
acting
CO
oxidation.
Under
conditions
simulated
for
practical
exhaust
systems,
efficiency
together
thermal
stability
sintering
resistance
achieved.
Across
all
these
examples,
insights
into
structures,
defects,
interfaces
emerge
in-depth
characterization
through
microscopy,
spectroscopy,
diffraction
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.
