Physical Chemistry Chemical Physics,
Год журнала:
2023,
Номер
26(1), С. 558 - 568
Опубликована: Ноя. 29, 2023
A
series
of
bifunctional
OER/ORR
SACs
supported
on
g-t-C
4
N
3
is
proposed.
It
found
from
DFT
calculations
that
the
d-orbital
structure
can
regulate
catalytic
activity
-based
SACs.
Abstract
Modifying
the
coordination
or
local
environments
of
single‐,
di‐,
tri‐,
and
multi‐metal
atom
(SMA/DMA/TMA/MMA)‐based
materials
is
one
best
strategies
for
increasing
catalytic
activities,
selectivity,
long‐term
durability
these
materials.
Advanced
sheet
supported
by
metal
atom‐based
have
become
a
critical
topic
in
fields
renewable
energy
conversion
systems,
storage
devices,
sensors,
biomedicine
owing
to
maximum
utilization
efficiency,
precisely
located
centers,
specific
electron
configurations,
unique
reactivity,
precise
chemical
tunability.
Several
offer
excellent
support
are
attractive
applications
energy,
medical
research,
such
as
oxygen
reduction,
production,
hydrogen
generation,
fuel
selective
detection,
enzymatic
reactions.
The
strong
metal–metal
metal–carbon
with
metal–heteroatom
(i.e.,
N,
S,
P,
B,
O)
bonds
stabilize
optimize
electronic
structures
atoms
due
interfacial
interactions,
yielding
activities.
These
provide
models
understanding
fundamental
problems
multistep
This
review
summarizes
substrate
structure‐activity
relationship
different
active
sites
based
on
experimental
theoretical
data.
Additionally,
new
synthesis
procedures,
physicochemical
characterizations,
biomedical
discussed.
Finally,
remaining
challenges
developing
efficient
SMA/DMA/TMA/MMA‐based
presented.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 10, 2025
Abstract
Reducing
carbon
dioxide
(CO
2
)to
high‐value
products
using
green
renewable
energy
is
a
promising
approach
for
addressing
and
greenhouse
effect
issues.
Consequently,
electrocatalytic
CO
reduction
reaction
(CO
RR)
technology
has
become
current
research
hotspot.
Since
the
discovery
of
high
activity
selectivity
copper
in
RR,
atomically
dispersed
Cu
catalysts
have
garnered
widespread
attention
due
to
their
efficient
atom
utilization,
unique
electronic
structure,
outstanding
catalytic
performance.
However,
great
challenge
remains
providing
rational
catalyst
design
principles
achieve
regulation
product
distribution.
A
clear
understanding
materials
an
in‐depth
interpretation
mechanism
as
well
elucidation
strategy
progress
toward
different
are
keys
building
solving
above
problem.
Therefore,
this
review
starts
with
introduction
advanced
characterization
techniques
reveal
structure
mechanisms.
Then,
various
optimization
strategies
applications
producing
targeted
summarized
discussed.
Finally,
perspectives
on
RR
field
future
development
offered.
Journal of Energy Chemistry,
Год журнала:
2023,
Номер
88, С. 169 - 182
Опубликована: Сен. 20, 2023
The
electrochemical
CO2
reduction
reaction
(CO2RR)
to
controllable
chemicals
is
considered
as
a
promising
pathway
store
intermittent
renewable
energy.
Herein,
set
of
catalysts
based
on
copper-nitrogen-doped
carbon
xerogel
(Cu-N-C)
are
successfully
developed
varying
the
copper
amount
and
nature
precursor,
for
efficient
CO2RR.
electrocatalytic
performance
Cu-N-C
materials
assessed
by
rotating
ring-disc
electrode
(RRDE),
technique
still
rarely
explored
For
comparison,
products
also
characterized
online
gas
chromatography
in
H-cell.
as-synthesized
found
be
active
highly
CO
selective
at
low
overpotentials
(from
−0.6
−0.8
V
vs.
RHE)
0.1
M
KHCO3,
while
H2
from
competitive
water
appears
larger
(−0.9
RHE).
optimum
acetate-derived
catalyst
containing
Cu-N4
moieties
exhibits
CO2-to-CO
turnover
frequency
997
h−1
−0.9
RHE
with
H2/CO
ratio
1.8.
These
results
demonstrate
that
RRDE
configuration
can
used
feasible
approach
identifying
electrolysis
Abstract
The
electrochemical
reduction
of
CO
2
into
C
2+
products
represents
a
promising
solution
to
completing
the
carbon
cycle,
thereby
fostering
sustainable
energy
supply.
Single‐atom
electrocatalysts
(SAECs)
have
garnered
significant
attention
as
efficient
for
reaction.
Herein,
we
carried
out
first‐principles
study
on
mechanism
C−C
bond
formation
single‐Cu‐atom‐modified
covalent
triazine
frameworks
(Cu‐CTFs),
which
are
platform
SAECs.
Static
density
functional
calculations
indicated
that
dimerization
CO,
is
main
bulk
Cu
metals,
was
not
favorable
Cu‐CTFs
because
lack
adjacent
sites
co‐adsorption
molecules.
Rather
than
dimerization,
reaction
between
adsorbed
*CHO
and
produce
*COCHO
has
relatively
low
barrier.
Constrained
ab
initio
molecular
dynamics
analyses
revealed
bond‐forming
proceeds
via
insertion
at
intermediate,
modest
activation
0.09
eV.
Specifically,
when
molecule
constrained
be
brought
close
*CHO,
occurs
distance
1.8
Å.
This
transition
step
this
formation.