Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 10, 2025
Abstract
Electrochemical
converting
CO
2
to
via
single
atom
catalyst
is
an
effective
strategy
for
reducing
concentration
in
the
atmosphere
and
achieving
a
carbon‐neutral
cycle.
However,
relatively
low
industrial
processes
large
energy
barriers
activating
severely
obstruct
actual
application.
Reasonably
modulating
coordination
shell
of
active
center
enhance
activity
catalysts.
Herein,
well‐designed
single‐atom
electrocatalyst
Ni‐N
3
S
1
developed
large‐scale
synthesis
strategy.
The
constructed
S‐C
exhibits
superior
catalytic
than
4
‐C
conversion
H‐type
cells,
industrial‐level
current
density
with
excellent
durability
at
wide
pH
range
can
be
achieved
gas‐diffusion
flow
cells.
Experimental
results
functional
theory
(DFT)
calculation
demonstrate
that
introducing
electronegative
significantly
regulate
electronic
structure
site,
promoting
adsorption
capacity
decreasing
barrier
*COOH
formation,
thus
larger
size
flexibility
sulfur
mitigate
nickel
agglomeration
stability
catalyst.
This
work
provides
designing
highly
catalysts
electrocatalysis
reactive
sites.
Advanced Materials,
Год журнала:
2023,
Номер
36(1)
Опубликована: Апрель 20, 2023
This
topical
review
focuses
on
the
distinct
role
of
carbon
support
coordination
environment
single-atom
catalysts
(SACs)
for
electrocatalysis.
The
article
begins
with
an
overview
atomic
configurations
in
SACs,
including
a
discussion
advanced
characterization
techniques
and
simulation
used
understanding
active
sites.
A
summary
key
electrocatalysis
applications
is
then
provided.
These
processes
are
oxygen
reduction
reaction
(ORR),
evolution
(OER),
hydrogen
(HER),
nitrogen
(NRR),
dioxide
(CO
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(45)
Опубликована: Окт. 6, 2023
Coordination
assembly
offers
a
versatile
means
to
developing
advanced
materials
for
various
applications.
However,
current
strategies
assembling
metal-organic
networks
into
nanoparticles
(NPs)
often
face
challenges
such
as
the
use
of
toxic
organic
solvents,
cytotoxicity
because
synthetic
ligands,
and
complex
synthesis
procedures.
Herein,
we
directly
assemble
NPs
using
metal
ions
polyphenols
(i.e.,
metal-phenolic
(MPNs))
in
aqueous
solutions
without
templating
or
seeding
agents.
We
demonstrate
role
buffers
(e.g.,
phosphate
buffer)
governing
NP
formation
engineering
physicochemical
properties
tunable
sizes
from
50
270
nm)
by
altering
conditions.
A
library
MPN
is
prepared
natural
ions.
Diverse
functional
cargos,
including
anticancer
drugs
proteins
with
different
molecular
weights
isoelectric
points,
are
readily
loaded
within
applications
biocatalysis,
therapeutic
delivery)
direct
mixing,
surface
modification,
owing
strong
affinity
guest
molecules.
This
study
provides
insights
mechanism
complexes
simple
strategy
engineer
nanosized
desired
diverse
biotechnological
Advanced Materials,
Год журнала:
2023,
Номер
36(4)
Опубликована: Авг. 31, 2023
Manipulating
the
coordination
environment
of
individual
active
sites
in
a
precise
manner
remains
an
important
challenge
electrocatalytic
reactions.
Herein,
inspired
by
theoretical
predictions,
facile
procedure
to
synthesize
series
symmetry-breaking
zinc
metal-organic
framework
(Zn-MOF)
catalysts
with
well-defined
structures
is
presented.
Benefiting
from
optimized
microenvironment
regulated
symmetry-breaking,
Zn-N
Nanoscale,
Год журнала:
2023,
Номер
15(39), С. 16056 - 16067
Опубликована: Янв. 1, 2023
Tailoring
the
coordination
environment
is
an
effective
strategy
to
modulate
electronic
structure
and
catalytic
activity
of
atomically
dispersed
transition-metal
(TM)
catalysts,
which
has
been
widely
investigated
for
single-atom
catalysts
but
received
less
attention
emerging
double-atom
(DACs).
Herein,
based
on
first-principles
calculations,
taking
commonly
studied
N-coordinated
graphene-based
DACs
as
references,
we
explored
effect
engineering
behaviors
towards
electrocatalytic
nitrogen
reduction
reaction
(NRR),
realized
through
replacing
one
N
atom
by
B
or
O
form
B,
O,
co-coordinated
DACs.
We
found
that
co-coordination
could
significantly
strengthen
N2
adsorption
alter
pattern
TM
dimer
active
center,
greatly
facilitates
activation.
Moreover,
DACs,
linear
scaling
relationship
between
binding
strengths
key
intermediates
can
be
attenuated.
Consequently,
Mn2
exhibiting
ultralow
limiting
potential
-0.27
V,
climb
peak
volcano.
In
addition,
experimental
feasibility
this
DAC
system
was
also
identified.
Overall,
benefiting
from
effect,
chemical
performance
NRR
boosted.
This
phenomena
understood
adjusted
center
due
changes
its
microenvironment,
affects
strength
(pattern)
pathways,
leading
enhanced
selectivity.
work
highlights
importance
in
developing
other
important
reactions.
Progress in Materials Science,
Год журнала:
2024,
Номер
145, С. 101299 - 101299
Опубликована: Апрель 16, 2024
Electrochemistry-driven
techniques
for
advanced
energy
storage/conversion
and
environmental
protection
play
a
crucial
role
in
achieving
sustainable
development
goals.
As
an
indispensable
component
diverse
electrochemical
systems,
electroactive
materials
gain
soaring
interest
terms
of
rational
design
synthesis.
Notably,
mechanochemistry-based
green
powerful
synthesis
has
been
widely
employed
to
fabricate
materials,
given
their
scalability
tunability.
Recently,
mechanochemically
synthesized
have
applied
various
fields,
leading
significant
progress.
However,
systematic
analysis
these
advancements
is
still
missing.
Herein,
we
comprehensively
discuss
recent
achievements
mechanosynthesized
applications.
The
mechanochemical
introduced,
along
with
different
types
materials.
Subsequently,
the
review
delves
into
applications
conversion/storage
systems
remediation.
structure-performance
correlation
are
illustrated
by
discussing
effects
process
on
internal
external
properties
performance.
Lastly,
key
perspectives
this
field
discussed,
including
monitoring,
field-assisted
synthesis,
material
performance
optimization,
practical
applications,
mechanochemistry-driven
fuels/chemicals
By
illustrating
current
advances
related
aims
shed
some
light
upcoming
research
synthesis-driven
sustainability.