Abstract
Efficient
and
sustainable
energy
development
is
a
powerful
tool
for
addressing
the
environmental
crises.
Single‐atom
catalysts
(SACs)
have
received
high
attention
their
extremely
atom
utilization
efficiency
excellent
catalytic
activity,
broad
application
prospects
in
chemical
production.
M‐N
4
an
active
center
model
with
clear
but
its
properties
such
as
selectivity,
durability
need
to
be
further
improved.
Adjustment
of
coordination
environment
central
metal
by
incorporating
heteroatoms
(e.g.,
sulfur)
effective
feasible
modification
method.
This
paper
describes
precise
synthetic
methods
introducing
sulfur
atoms
into
controlling
whether
they
are
directly
coordinated
form
specific
configuration,
sulfur‐doped
carbon‐based
single‐atom
electrocatalytic
reactions
ORR,
CO
2
RR,
HER,
OER,
other
reaction
systematically
reviewed.
Meanwhile,
effect
tuning
electronic
structure
ligand
configuration
parameters
due
doped
improvement
performance
introduced
combining
different
characterization
testing
methods.
Finally,
several
opinions
on
SACs
put
forward.
Chemical Society Reviews,
Год журнала:
2023,
Номер
52(23), С. 8319 - 8373
Опубликована: Янв. 1, 2023
In
this
review,
we
provide
a
comprehensive
summary
of
recent
advances
in
the
synthesis
strategies,
design
principles,
and
characterization
technologies
high
entropy
alloys,
their
applications
various
electrocatalytic
conversion
reactions.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
63(3)
Опубликована: Ноя. 24, 2023
Abstract
Modulating
the
surface
and
spatial
structure
of
host
is
associated
with
reactivity
active
site,
also
enhances
mass
transfer
effect
CO
2
electroreduction
process
(CO
RR).
Herein,
we
describe
development
two‐step
ligand
etch–pyrolysis
to
access
an
asymmetric
dual‐atomic‐site
catalyst
(DASC)
composed
a
yolk–shell
carbon
framework
(Zn
1
Mn
‐SNC)
derived
from
S,N‐coordinated
Zn−Mn
dimers
anchored
on
metal–organic
(MOF).
In
Zn
‐SNC,
electronic
effects
S/N−Zn−Mn−S/N
configuration
are
tailored
by
strong
interactions
between
dual
sites
co‐coordination
S/N
atoms,
rendering
structural
stability
atomic
distribution.
H‐cell,
‐SNC
DASC
shows
low
onset
overpotential
50
mV
high
Faraday
efficiency
97
%
applied
343
mV,
thus
outperforming
counterparts,
in
flow
cell,
it
reaches
current
density
500
mA
cm
−2
at
−0.85
V,
benefitting
accessibility
sites.
DFT
simulations
showed
that
diatomic
site
optimal
adsorption
strength
COOH*
lowers
reaction
energy
barrier,
boosting
intrinsic
RR
activity
DASC.
The
structure‐property
correlation
found
this
study
suggests
new
ideas
for
highly
accessible
catalysts.
Advanced Materials,
Год журнала:
2023,
Номер
35(51)
Опубликована: Авг. 9, 2023
Electrochemical
nitrogen
reduction
reaction
(NRR)
is
a
burgeoning
field
for
green
and
sustainable
ammonia
production,
in
which
numerous
potential
catalysts
emerge
endlessly.
However,
satisfactory
performances
are
still
not
realized
under
practical
applications
due
to
the
limited
solubility
sluggish
diffusion
of
at
interface.
Herein,
molecular
imprinting
technology
adopted
construct
an
adlayer
with
abundant
imprints
on
electrocatalyst,
capable
selectively
recognizing
proactively
aggregating
high-concentrated
interface
while
hindering
access
overwhelming
water
simultaneously.
With
this
favorable
microenvironment,
can
preferentially
occupy
active
surface,
NRR
equilibrium
be
positively
shifted
facilitate
kinetics.
Approximately
threefold
improvements
both
production
rate
(185.7
µg
h-1
mg-1
)
Faradaic
efficiency
(72.9%)
achieved
by
metal-free
catalyst
compared
bare
one.
It
believed
that
strategy
should
general
method
find
further
applicability
or
even
other
reactions
facing
similar
challenges.
Abstract
Electrocatalytic
nitrogen
reduction
technology
seamlessly
aligns
with
the
principles
of
environmentally
friendly
chemical
production.
In
this
paper,
a
comprehensive
review
recent
advancements
in
electrocatalytic
NH
3
synthesis
utilizing
single‐atom
catalysts
(SACs)
is
offered.
Into
research
and
applications
three
categories
SACs:
noble
metals
(Ru,
Au,
Rh,
Ag),
transition
(Fe,
Mo,
Cr,
Co,
Sn,
Y,
Nb),
nonmetallic
(B)
context
ammonia
delved.
In‐depth
insights
into
material
preparation
methods,
coordination
patterns,
characteristics
reaction
(NRR)
are
provided.
The
systematic
comparison
capabilities
various
SAC
types
offers
framework
for
their
integration
NRR.
Additionally,
challenges,
potential
solutions,
future
prospects
incorporating
SACs
endeavors
discussed.
The Innovation Materials,
Год журнала:
2024,
Номер
2(1), С. 100060 - 100060
Опубликована: Янв. 1, 2024
<p>Inorganic,
organic,
and
hybrid
two-dimensional
(2D)
materials
are
being
developed
for
ever-expanding
numbers
of
applications,
though
energy
catalysis
remain
the
main
drivers
their
development.
We
present
overviews
bottom-up
top-down
synthetic
strategies
such
examine
manufacturing
scalability
issues.
Mechanical,
electrical,
thermal
properties
modulation
highlighted
because
they
fundamental
to
above-mentioned
drivers.
The
burgeoning
importance
heterostructures
in
materials,
particularly
electrode
design
function
is
stressed.
Detailed
attention
given
applications
2D
electrocatalysis
reactions:
oxygen
reduction,
evolution,
hydrogen
carbon
dioxide
nitrogen
reduction.
Water
splitting,
reduction
by
photocatalysis
also
examined.
A
perspective
expected
advances
expansion
types
with
a
focus
on
heterostructure
development,
presented
conclusion.</p>
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(24)
Опубликована: Фев. 5, 2024
Abstract
Photoelectrochemical
(PEC)
technology
offers
new
opportunities
for
pushing
the
renewable
energy‐driven
ammonia
synthesis
toward
a
practical
level,
while
still
facing
unsatisfactory
efficiency
due
to
obstacle
of
dissociating
inert
nitrogen
triple‐bonds.
Herein,
novel
donor‐site‐acceptor
system
is
constructed
in
covalent
organic
frameworks
tackle
this
challenge
highly
efficient
PEC
synthesis.
Highly
active
boron
site
elaborately
embedded
between
donor
and
acceptor
units,
which
can
be
effectively
activated
with
continuous
electron
flow
upon
photoexcitation.
With
assistance
solar
irradiation,
stubborn
dissociation
successfully
changed
from
passive
endothermic
reaction
spontaneous
exothermic
process,
completely
eliminating
energy
barrier
rate‐determining
step
facilitating
overall
kinetics.
The
proof‐of‐concept
achieved
an
excellent
NRR
performance
remarkable
Faradaic
91.6%,
reaching
target
set
by
U.S.
Department
Energy
(90%).
