ACS Catalysis,
Journal Year:
2025,
Volume and Issue:
15(3), P. 1477 - 1486
Published: Jan. 9, 2025
Electronic
perturbation
induced
by
the
microenvironment
regulation
adjacent
to
FeN4
sites
anchored
on
metal–N–C
materials
will
accelerate
its
oxygen
reduction
reaction
(ORR)
kinetics.
Herein,
we
report
a
fine-tuning
in
charge
configuration
of
through
defect-rich
N/S-doped
carbon
nest
derived
from
chemically
cross-linked
pyrrole/thiophene
copolymer
(CCPPT)
with
sp3-hybridized
cross-linker.
Compared
(PPT)
without
cross-linker,
CCPPT
knitted
three-dimensional
(3D)
network
delivers
higher
defect
density
and
∼2-fold
sulfur
retention
after
pyrolysis.
The
structural
characterizations
combined
theoretical
calculations
suggest
that
vacancy
defects
(Cvd)
FeN4/S2
moiety
together
induce
redistribution
resultant
CC-Fe1/NSC
CCPPT,
reducing
adsorption
strength
oxygen-containing
intermediates
energy
barrier
ORR.
As
expected,
shows
an
impressive
half-wave
potential
∼0.91
V
vs
reversible
hydrogen
electrode
(RHE),
surpassing
both
PPT-derived
Fe1/NSC
(0.88
V)
commercial
Pt/C
(0.86
V).
This
work
provides
distinctive
path
manipulate
single-atom
catalysts
toward
ORR
or
even
beyond.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(32)
Published: June 3, 2024
Abstract
Directly
coupling
N
2
and
CO
to
synthesize
urea
by
photocatalysis
paves
a
sustainable
route
for
synthesis,
but
its
performance
is
limited
the
competition
of
photogenerated
electrons
between
,
as
well
underutilized
holes.
Herein,
we
report
an
efficient
synthesis
process
involving
holes
in
respectively
converting
over
redox
heterojunction
consisting
WO
3
Ni
single‐atom‐decorated
CdS
(Ni
1
‐CdS/WO
).
For
photocatalytic
from
pure
water,
attained
yield
rate
78
μM
h
−1
apparent
quantum
0.15
%
at
385
nm,
which
ranked
among
best
reported.
Mechanistic
studies
reveal
that
was
converted
into
NO
species
⋅OH
radicals
generated
component,
meanwhile,
transformed
*CO
site
electrons.
The
were
further
coupled
form
*OCNO
intermediate,
then
gradually
urea.
This
work
emphasizes
importance
reasonably
utilizing
reduction
reactions.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(14), P. 4847 - 4870
Published: Jan. 1, 2024
Based
on
the
advancements
in
atomically
dispersed
multi-site
catalysts
for
FZABs,
this
review
discusses
design
methodologies
to
regulate
performance
of
bifunctional
oxygen
electrocatalysts
from
electronic
and
geometric
structures.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(36), P. 24945 - 24955
Published: Aug. 30, 2024
Heterogeneous
dual-atomic-site
catalysts
(DACs)
hold
great
potential
for
diverse
applications.
However,
to
date,
the
synthesis
of
DACs
primarily
relies
on
different
atoms
freely
colliding
support
during
synthesis,
principally
leading
low
yields.
Herein,
we
report
a
general
metal
ion
recognition
(MIR)
strategy
constructing
series
DACs,
including
but
not
limited
Fe1Sn1,
Fe1Co1,
Fe1Ni1,
Fe1Cu1,
Fe1Mn1,
Co1Ni1,
Co1Cu1,
Co2,
and
Cu2.
This
is
achieved
by
coupling
target
inorganometallic
cations
anions
as
pairs,
which
are
sequentially
adsorbed
onto
nitrogen-doped
carbon
substrate
precursor.
Taking
oxygen
reduction
reaction
an
example,
demonstrated
that
Fe1Sn1-DAC
synthesized
through
this
delivers
record
peak
power
density
1.218
W
cm–2
under
2.0
bar
H2–O2
conditions
enhanced
stability
compared
single-atom-site
FeN4.
Further
study
revealed
superior
performance
arises
from
synergistic
effect
Fe1Sn1
dual
vicinal
sites,
effectively
optimizes
adsorption
*OH
alleviates
troublesome
Fenton-like
reaction.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 19, 2025
Abstract
Numerous
in
situ
characterization
studies
have
focused
on
revealing
the
catalytic
mechanisms
of
single‐atom
catalysts
(SACs),
providing
a
theoretical
basis
for
their
rational
design.
Although
research
is
relatively
limited,
stability
SACs
under
long‐term
operating
conditions
equally
important
and
prerequisite
real‐world
energy
applications,
such
as
fuel
cells
water
electrolyzers.
Recently,
there
has
been
rise
destabilization
regeneration
SACs;
however,
timely
comprehensive
summaries
that
provide
catalysis
community
with
valuable
insights
directions
are
still
lacking.
This
review
summarizes
recent
advances
strategies
SACs,
specifically
highlighting
various
state‐of‐the‐art
techniques
employed
studies.
The
factors
induce
identified
by
discussing
failure
active
sites,
coordination
environments,
supports,
reaction
scenarios.
Next,
primary
introduced,
including
redispersion,
surface
poison
desorption,
exposure
subsurface
sites.
Additionally,
advantages
limitations
both
ex
discussed.
Finally,
future
proposed,
aimed
at
constructing
structure–stability
relationships
guiding
design
more
stable
SACs.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(25)
Published: April 3, 2024
Atomic
metal
catalysts
have
unique
electronic,
structural,
and
catalytic
properties,
which
are
widely
used
in
the
field
of
catalysis.
However,
designing
new
simple
synthesis
methods
to
fabricate
atomic
is
a
challenge
applications.
Herein,
one-step
precursor
combustion
strategy
presented
that
starts
directly
from
precursors
salts,
using
spontaneous
process
convert
platinum
nitrate
Pt
sites.
The
sites
with
low
valence
anchored
formed
interface
between
grains
on
vacancy-enriched
CeO
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Jan. 1, 2024
This
review
systematically
provides
various
insights
into
the
pH
effect
on
hydrogen
electrocatalysis,
and
thus
providing
a
reference
for
future
development
of
electrocatalysis
based
these
insights.
