Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 5, 2025
Atomic
defects,
e.g.,
vacancies,
substitutions,
and
dopants,
play
crucial
roles
in
determining
the
functionalities
of
two-dimensional
(2D)
materials,
including
spin
glass,
single-photon
emitters,
energy
storage
conversion,
due
to
introduction
abnormal
charge
states
noncentrosymmetric
distortion.
In
particular,
anti-substitutions
are
regarded
as
promising
topological
defect
types,
which
substitution
occurs
at
opposite
sites,
fundamentally
modifying
atomic
electronic
structures
pristine
lattices.
However,
fabrication
large-scale
remains
challenging
high
formation
energies
complex
reaction
paths.
Here,
we
propose
an
approach
for
synthesizing
atomically
dispersed
Pt
defective
1T'-MoTe2
using
electrochemical
exfoliation-assisted
leaching-redeposition
(EELR)
method.
Atomic-resolution
scanning
transmission
electron
microscopy
(STEM)
imaging
reveals
that
atoms
substitute
Te
forming
unconventional
Mo-Pt
bonds.
A
rich
variety
anti-substitution
configurations
coupling
with
vacancies
have
been
fabricated
by
controlled
conditions.
Density
functional
theory
(DFT)
calculations
suggest
preferentially
occupy
vacancy
sites
coupled
neighboring
stabilizing
configurations.
The
Pt-Te
complexes
exhibit
excellent
hydrogen
evolution
reaction,
overpotential
only
12.9
mV
because
paired
cause
redistribution
regulate
d-band
center
active
suggested
DFT.
These
findings
introduce
effective
engineering
2D
presenting
new
opportunities
precise
design
features
targeted
catalytic
other
advanced
applications.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(37)
Опубликована: Авг. 6, 2023
Abstract
Atomically
precise
composite
site‐based
catalysts
with
new
electrocatalytic
synergistic
mechanisms
and
enhanced
activities
have
emerged
as
a
frontier
in
the
electrocatalysis
community.
This
topical
review
focuses
on
recent
research
advances
of
atomically
metal
sites‐based
electrocatalysts.
work
first
demonstrates
an
overview
configurations
sites,
including
discussion
advanced
methods
employed
for
understanding
sites.
The
then
provides
comprehensive
organization
previously
reported
methodologies
synthesizing
electrocatalysts
Representative
case
studies
are
provided,
starting
from
simple
one‐step
pyrolysis
strategy
to
species‐by‐species
multi‐step
strategy.
Based
preceding
discussions
catalyst
materials,
further
discusses
unique
raised
by
that
different
routine
single
species
systems
mainly
involve
oxygen
reduction
reaction,
evolution
hydrogen
nitrogen
carbon
dioxide
reaction.
themes
this
section
include
true
active
center
determination
sites
various
types
synergy
mechanisms.
Finally,
critical
unanswered
questions
remaining
challenges,
well
promising
underexplored
directions
identified.
ACS Applied Materials & Interfaces,
Год журнала:
2023,
Номер
15(40), С. 47425 - 47433
Опубликована: Сен. 29, 2023
With
the
rapid
development
of
wearable
devices
and
integrated
systems,
protection
against
electromagnetic
waves
is
an
issue.
For
solving
problems
poor
flexibility
a
tendency
to
corrode
traditional
interference
(EMI)
shielding
materials,
two-dimensional
(2D)
nanomaterial
MXene
was
employed
manufacture
next-generation
EMI
materials.
Vacuum-assisted
filtration
combined
with
liquid
nitrogen
prefreezing
strategy
adopted
prepare
flexible
MXene/cellulose
nanofibers
(CNFs)
composite
aerogel
film
unique
cellular
structure.
Here,
CNFs
were
as
reinforcement,
such
structure
design
can
effectively
improve
effectiveness
(SE).
In
particular,
shows
outstanding
SE
54
dB.
Furthermore,
MXene/CNFs
exhibited
prominent
steady
photothermal
conversion
ability,
which
could
obtain
maximum
equilibrium
temperature
89.4
°C
under
808
nm
NIR
laser.
Thus,
our
appealing
construction
holds
great
promise
for
materials
heating
applications
in
cold
complex
practical
environment.
Abstract
The
designing
and
fabricating
highly
active
hydrogen
evolution
reaction
(HER)
electrocatalysts
that
can
superior
to
Pt/C
is
extremely
desirable
but
challenging.
Herein,
the
fabrication
of
Ru/TiO
2
/N‐doped
carbon
(Ru/TiO
/NC)
nanofiber
reported
as
a
novel
HER
electrocatalyst
through
electrospinning
subsequent
pyrolysis
treatment,
in
which
Ru
nanoclusters
are
dispersed
into
TiO
/NC
hybrid
nanofiber.
As
support,
experimental
theoretical
calculation
results
reveal
more
effectively
accelerate
water
dissociation
well
optimize
adsorption
strength
*
H
than
NC,
thus
leading
significantly
enhanced
activity,
merely
requires
an
overpotential
18
mV
reach
10
mA
cm
−2
,
outperforming
alkaline
solution.
electrolytic
cell
composed
NiFe
LDH/NF
generate
500
1000
at
voltages
1.631
1.753
V,
respectively.
Furthermore,
also
exhibits
remarkable
durability
for
least
100
h
200
with
negligible
degradation
activity.
present
work
affords
deep
insight
influence
support
on
activity
strategy
proposed
this
research
be
extended
fabricate
various
other
types
diverse
electrocatalytic
applications.
Materials Horizons,
Год журнала:
2024,
Номер
11(18), С. 4239 - 4255
Опубликована: Янв. 1, 2024
This
review
summarizes
the
design
strategies
of
MXene-based
catalysts
for
HER,
OER,
ORR
and
NRR,
including
surface
modification,
MXene
lattice
substitution,
morphology,
defect
heterostructure
engineering.
ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
16(11), С. 13828 - 13838
Опубликована: Март 6, 2024
Alluaudite
sodium
iron
sulfate
(NFS)
exhibits
great
potential
for
use
in
sodium-ion
battery
cathodes
due
to
its
elevated
operating
and
abundant
element
reserves.
However,
conventional
solid-state
methods
demonstrate
a
low
heating/cooling
rate
sluggish
reaction
kinetics,
requiring
long
thermal
treatment
effectively
fabricate
NFS
cathodes.
Herein,
we
propose
shock
(TS)
strategy
synthesize
alluaudite
using
either
hydrous
or
anhydrous
raw
materials.
The
analysis
of
the
phase
formation
process
reveals
that
TS
can
significantly
facilitate
removal
crystal
water
decomposition
intermediate
Na2Fe(SO4)2
precursor.
In
case
precursor,
kinetics
combination
between
Na2SO4
FeSO4
be
also
accelerated
by
treatment.
Consequently,
pure
completed
after
substantially
shorter
time
post-sintering,
thereby
saving
significant
energy.
TS-treated
cathode
derived
from
precursor
higher
retention
200
cycles
at
1C
better
capability
than
counterpart
prepared
long-term
tube
furnace
sintering,
demonstrating
this
novel
strategy.
ACS Materials Letters,
Год журнала:
2024,
Номер
6(5), С. 1711 - 1721
Опубликована: Март 28, 2024
Single-atom
catalysts
(SACs)
have
improved
the
performance
of
NO
electroreduction
to
NH3
(NORR)
a
high
level.
However,
influence
low-nuclearity
clusters,
which
exist
in
SACs
as
well,
on
catalytic
is
always
overlooked.
Herein,
via
density
functional
theory,
we
not
only
designed
9
single
TMs,
namely,
Sc,
Ti,
V,
Cr,
Mn,
Fe,
Co,
Ni,
and
Cu,
anchored
three
Ti3C2O2-based
models
(Ti3C2O2-V0,
Ti3C2O2-O1,
Ti3C2O2-Ti1)
for
NORR
but
also
further
evaluated
impact
clusters
optimal
SAC.
Our
results
identified
Cu/Ti3C2O2-V0
Ni/Ti3C2O2-Ti1
promising
ultrahigh
NORR.
Furthermore,
activity
both
diminished
with
formation
cluster,
especially
Ni
Ti3C2O2-Ti1.
From
atoms
projected
states
increases
significantly
near
Fermi
level,
leading
stronger
interactions
between
reaction
intermediates,
thereby
hindering
hydrogenation
steps
greatly
slowing
down
cluster.
Meanwhile,
pH-dependent
analysis
revealed
that
rate-determining
step
changed
pH
increased
Ni/Ti3C2O2-Ti1,
an
acidic
environment
facilitates
effective
NO-to-NH3
conversion
Cu/Ti3C2O2-V0.
Therefore,
this
work
predicts
highly
efficient
catalyst
reveals
weakening
mechanism
would
guide
future
experimental
research
metal
Abstract
The
restacking
and
oxidizable
nature
of
vanadium‐based
carbon/nitride
(V
2
C‐MXene)
poses
a
significant
challenge.
Herein,
tellurium
(Te)‐doped
V
C/V
O
3
electrocatalyst
is
constructed
via
mild
H
oxidation
calcination
treatments.
Especially,
this
work
rationally
exploits
the
inherent
easy
characteristic
associated
with
MXene
to
alter
interfacial
information,
thereby
obtaining
stable
self‐generated
heterointerfaces.
Meanwhile,
microetching
effect
creates
numerous
pores
address
issues.
Besides,
Te
element
doping
settles
issue
awkward
levels
absorption/desorption
ability
intermediates.
obtains
an
unparalleled
hydrogen
evolution
reaction
oxygen
overpotential
83.5
279.8
mV
at
−10
10
mA
cm
−2
,
respectively.
In
addition,
overall
water‐splitting
device
demonstrates
low
cell
voltage
1.41
obtain
.
Overall,
drawbacks
can
be
turned
into
benefits
based
on
planning
strategy
create
these
electrocatalysts
desirable
kinetics.
Abstract
Electrocatalytic
hydrogen
evolution
reaction
(HER)
is
a
promising
strategy
to
solve
and
mitigate
the
coming
energy
shortage
global
environmental
pollution.
Searching
for
efficient
electrocatalysts
HER
remains
challenging
through
traditional
trial‐and‐error
methods
from
numerous
potential
material
candidates.
Theoretical
high
throughput
calculation
assisted
by
machine
learning
possible
method
screen
excellent
effectively.
This
will
pave
way
high‐efficiency
low‐price
electrocatalyst
findings.
In
this
review,
we
comprehensively
introduce
workflow
standard
models
reduction
reactions.
mainly
illustrates
how
used
in
catalyst
filtration
descriptor
exploration.
Subsequently,
several
applications,
including
surface
electrocatalysts,
two‐dimensional
(2D)
single/dual
atom
using
electrocatalytic
HER,
are
highlighted
introduced.
Finally,
corresponding
challenge
perspective
reactions
concluded.
We
hope
critical
review
can
provide
comprehensive
understanding
of
design
guide
future
theoretical
experimental
investigation
