Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(37)
Published: May 19, 2024
Abstract
The
conversion
of
carbon
dioxide
(CO
2
)
into
value‐added
chemicals
with
two
or
more
carbons
(C
2+
is
a
promising
strategy
that
cannot
only
mitigate
anthropogenic
CO
emissions
but
also
reduce
the
excessive
dependence
on
fossil
feedstocks.
In
recent
years,
atomically
dispersed
metal
catalysts
(ADCs),
including
single‐atom
(SACs),
dual‐atom
(DACs),
and
single‐cluster
(SCCs),
emerged
as
attractive
candidates
for
fixation
reactions
due
to
their
unique
properties,
such
maximum
utilization
active
sites,
tunable
electronic
structure,
efficient
elucidation
catalytic
mechanism,
etc.
This
review
provides
an
overview
significant
progress
in
synthesis
characterization
ADCs
utilized
photocatalytic,
electrocatalytic,
thermocatalytic
toward
high‐value
C
compounds.
To
provide
insights
designing
chemical
originating
from
,
key
factors
influence
activity
selectivity
are
highlighted.
Finally,
relevant
challenges
opportunities
discussed
inspire
new
ideas
generation
‐based
products
over
ADCs.
Chemical Reviews,
Journal Year:
2024,
Volume and Issue:
124(21), P. 11767 - 11847
Published: July 5, 2024
Anthropogenic
activities
related
to
population
growth,
economic
development,
technological
advances,
and
changes
in
lifestyle
climate
patterns
result
a
continuous
increase
energy
consumption.
At
the
same
time,
rare
metal
elements
frequently
deployed
as
catalysts
processes
are
not
only
costly
view
of
their
low
natural
abundance,
but
availability
is
often
further
limited
due
geopolitical
reasons.
Thus,
electrochemical
storage
conversion
with
earth-abundant
metals,
mainly
form
single-atom
(SACs),
highly
relevant
timely
technologies.
In
this
review
application
SACs
electrocatalytic
chemicals
fuels
or
products
high
content
discussed.
The
oxygen
reduction
reaction
also
appraised,
which
primarily
harnessed
fuel
cell
technologies
metal-air
batteries.
coordination,
active
sites,
mechanistic
aspects
transition
analyzed
for
two-electron
four-electron
pathways.
Further,
water
splitting
toward
green
hydrogen
discussed
terms
evolution
reaction.
Similarly,
production
ammonia
clean
via
nitrogen
portrayed,
highlighting
potential
single
species.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(18)
Published: Jan. 17, 2024
Abstract
Carbon‐based
metal‐free
electrocatalysts
have
been
recognized
as
inexpensive
alternatives
to
afford
excellent
activity
in
oxygen
reduction/evolution
reactions
(ORR/OER).
Nevertheless,
precisely
identifying
the
local
active
sites
and
tailoring
corresponding
electronic
properties
enhance
reaction
kinetics
remain
challenging.
Herein,
a
facile
strategy
create
electrocatalyst
comprised
of
mesoporous
nitrogen‐doped
carbon
matrix
with
phosphorus
incorporation
(NPC)
is
described.
The
as‐prepared
NPC‐950
demonstrates
superior
ORR
under
alkaline
acidic
conditions
half‐wave
potentials
0.88
0.72
V,
respectively,
comparable
commercial
Pt/C
(0.85
0.76
V)
overwhelmingly
other
N‐doped
catalyst
materials.
In
addition,
remarkable
promotion
OER
observed.
Notably,
zinc–air
battery
equipped
this
NCP‐950
exhibits
exceptional
performance
peak
power
density,
specific
capacity,
long‐term
operation
durability.
Theoretical
calculations
uncover
that
NC
material
results
effective
charge
density
redistribution,
thus
modulating
achieve
optimum
adsorption
desorption
intermediates.
work
provides
deep
understanding
heteroatom‐doped
materials
highlights
importance
modulation
bifunctional
electrocatalytic
activity.
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
53(12), P. 6295 - 6321
Published: Jan. 1, 2024
Developing
sophisticated
strategies
to
stabilize
oxidative
metal
catalysts
based
on
the
correlation
between
dynamic
oxidation
state
and
product
profile
is
favorable
for
efficient
electrochemical
CO
2
conversion.
ACS Nano,
Journal Year:
2024,
Volume and Issue:
18(14), P. 9823 - 9851
Published: March 28, 2024
With
the
increasingly
serious
greenhouse
effect,
electrochemical
carbon
dioxide
reduction
reaction
(CO2RR)
has
garnered
widespread
attention
as
it
is
capable
of
leveraging
renewable
energy
to
convert
CO2
into
value-added
chemicals
and
fuels.
However,
performance
CO2RR
can
hardly
meet
expectations
because
diverse
intermediates
complicated
processes,
necessitating
exploitation
highly
efficient
catalysts.
In
recent
years,
with
advanced
characterization
technologies
theoretical
simulations,
exploration
catalytic
mechanisms
gradually
deepened
electronic
structure
catalysts
their
interactions
intermediates,
which
serve
a
bridge
facilitate
deeper
comprehension
structure-performance
relationships.
Transition
metal-based
(TMCs),
extensively
applied
in
CO2RR,
demonstrate
substantial
potential
for
further
modulation,
given
abundance
d
electrons.
Herein,
we
discuss
representative
feasible
strategies
modulate
catalysts,
including
doping,
vacancy,
alloying,
heterostructure,
strain,
phase
engineering.
These
approaches
profoundly
alter
inherent
properties
TMCs
interaction
thereby
greatly
affecting
rate
pathway
CO2RR.
It
believed
that
rational
design
modulation
fundamentally
provide
viable
directions
development
toward
conversion
many
other
small
molecules.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(29)
Published: March 17, 2024
Abstract
The
oxygen
reduction
reaction
(ORR)
plays
a
fundamental
role
in
sustainable
energy
technologies.
However,
the
creation
of
non‐precious
metal
electrocatalysts
with
high
ORR
activity
and
durability
under
all
pH
conditions
is
great
significance
but
remains
challenging.
Herein,
aim
to
overcome
this
challenge
by
creating
Fe
single
atom
catalyst
on
2D
defect‐containing
nitrogen‐doped
carbon
support
(Fe
1
/DNC)
via
microenvironment
engineering
strategy.
Microkinetic
modeling
reveals
that
FeN
4
(OH)
moieties
are
real
active
sites
conditions.
Due
synergistic
promotion
effect
denser
accessible
defect‐induced
electronic
properties,
/DNC
achieves
extraordinary
alkaline,
acidic,
neutral
conditions,
half‐wave
potentials
0.95,
0.82,
0.70
V,
respectively.
Moreover,
negligible
performance
decay
observed
stability
methanol
tolerance
tests.
Zn‐air
battery
employing
delivers
remarkable
peak
power
density
long‐term
operational
durability.
Theoretical
analysis
provides
compelling
evidence
defects
adjacent
can
endow
an
inductive
reshape
properties
balance
OOH*
formation
OH*
reduction.
This
work
offers
insight
into
regulation
asymmetric
coordination
structure
for
boosting
electrocatalytic
stability.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(14), P. 5039 - 5047
Published: Jan. 1, 2024
This
work
is
the
first
to
introduce
photocontrolled
catalysts
into
CO
2
RR,
and
further
RE
single
atom
catalysts,
aiming
optimize
photocatalytic
performance
by
utilizing
synergistic
effect
of
composites.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(22)
Published: March 26, 2024
Abstract
Single
atomic
catalysts
(SACs)
offer
a
superior
platform
for
studying
the
structure–activity
relationships
during
electrocatalytic
CO
2
reduction
reaction
(CO
RR).
Yet
challenges
still
exist
to
obtain
well‐defined
and
novel
site
configuration
owing
uncertainty
of
functional
framework‐derived
SACs
through
calcination.
Herein,
Bi−N
O
supported
on
(1
1
0)
plane
hydrogen‐bonded
organic
framework
(HOF)
is
reported
directly
RR.
In
flow
cell,
target
catalyst
Bi1‐HOF
maintains
faradaic
efficiency
(FE)
HCOOH
over
90
%
at
wide
potential
window
1.4
V.
The
corresponding
partial
current
density
ranges
from
113.3
747.0
mA
cm
−2
.
And,
exhibits
long‐term
stability
30
h
under
successive
potential‐step
test
with
100–400
Density
function
theory
(DFT)
calculations
illustrate
that
HOF
effectively
induces
oriented
electron
transfer
Bi
center
molecule,
reaching
an
enhanced
activation
reduction.
Besides,
this
study
offers
versatile
method
reach
series
M−N
sites
regulable
metal
centers
via
same
intercalation
mechanism,
broadening