Angewandte Chemie,
Год журнала:
2023,
Номер
136(5)
Опубликована: Дек. 13, 2023
Abstract
Covalent
organic
frameworks
(COFs)
have
been
utilized
for
catalyzing
the
reduction
of
carbon
dioxide
(CO2RR)
due
to
their
atomic
metal
centers
and
controllable
pore
channels,
which
are
facilitated
by
different
covalent
bonds.
However,
exploration
boron‐based
linkages
in
these
catalytic
COFs
has
limited
owing
potential
instability.
Herein,
we
present
construction
boronic
ester‐linked
through
nucleophilic
substitution
reactions
order
catalyze
CO
2
RR.
The
inclusion
abundant
fluorine
atoms
within
enhances
hydrophobicity
subsequently
improves
water
tolerance
chemical
stability
COFs.
content
boron
COF
was
carefully
controlled,
with
featuring
a
higher
density
exhibiting
increased
electronic
conductivity,
enhanced
reductive
ability,
stronger
binding
affinity
towards
.
Consequently,
demonstrate
improved
activity
selectivity.
optimized
achieve
highest
activity,
achieving
turnover
frequency
1695.3
h
−1
selectivity
95.0
%
at
−0.9
V.
Operando
synchrotron
radiation
measurements
confirm
Co
(II)
as
catalytically
active
sites.
By
successfully
constructing
COFs,
not
only
address
instability
concerns
but
also
exceptional
performance
Nano-Micro Letters,
Год журнала:
2024,
Номер
16(1)
Опубликована: Фев. 29, 2024
Abstract
The
exploration
of
sustainable
energy
utilization
requires
the
implementation
advanced
electrochemical
devices
for
efficient
conversion
and
storage,
which
are
enabled
by
usage
cost-effective,
high-performance
electrocatalysts.
Currently,
heterogeneous
atomically
dispersed
catalysts
considered
as
potential
candidates
a
wide
range
applications.
Compared
to
conventional
catalysts,
metal
atoms
in
carbon-based
have
more
unsaturated
coordination
sites,
quantum
size
effect,
strong
metal–support
interactions,
resulting
exceptional
catalytic
activity.
Of
these,
dual-atomic
(DACs)
attracted
extensive
attention
due
additional
synergistic
effect
between
two
adjacent
atoms.
DACs
advantages
full
active
site
exposure,
high
selectivity,
theoretical
100%
atom
utilization,
ability
break
scaling
relationship
adsorption
free
on
sites.
In
this
review,
we
summarize
recent
research
advancement
DACs,
includes
(1)
comprehensive
understanding
synergy
atomic
pairs;
(2)
synthesis
DACs;
(3)
characterization
methods,
especially
aberration-corrected
scanning
transmission
electron
microscopy
synchrotron
spectroscopy;
(4)
energy-related
last
part
focuses
great
catalysis
small
molecules,
such
oxygen
reduction
reaction,
CO
2
hydrogen
evolution
N
reaction.
future
challenges
opportunities
also
raised
prospective
section.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(36)
Опубликована: Март 18, 2024
Abstract
Recently,
a
diverse
array
of
novel
metal‐nitrogen‐carbon
(M‐N‐C)
single‐atom
catalysts
(SACs)
have
rapidly
evolve,
particularly
in
the
realm
oxygen
reduction
reaction
(ORR).
Despite
plethora
proposed
design
and
improvement
strategies
for
SACs,
comprehensive
review
systematically
compiling
components
M‐N‐C
from
unified
perspective
is
notably
absent.
For
first
time,
thorough
examination
each
component
conducted,
focusing
on
entropy
increase
active
sites
SACs.
single
M‐N
4
whole
system,
an
implies
elevated
degree
disorder
chaos.
Broadly,
entropy‐increasing
modification
M
(single
mental
sites)
guest
groups
entails
augmentation
chaos,
with
most
effective
co‐catalytic
synergy
achieved
by
establishing
multiple
through
“cocktail
effect”.
Concerning
N
(nitrogen
other
heteroatoms)
C
(carbon
supports),
induces
heightened
disorder,
symmetry
breaking
more
likely
to
drive
toward
adsorbing
molecules
attain
equilibrium
symmetric
structure.
All
these
innovative
led
remarkable
ORR
activity
stability
offer
guiding
criterion
future
preparation
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
63(5)
Опубликована: Дек. 13, 2023
Covalent
organic
frameworks
(COFs)
have
been
utilized
for
catalyzing
the
reduction
of
carbon
dioxide
(CO2RR)
due
to
their
atomic
metal
centers
and
controllable
pore
channels,
which
are
facilitated
by
different
covalent
bonds.
However,
exploration
boron-based
linkages
in
these
catalytic
COFs
has
limited
owing
potential
instability.
Herein,
we
present
construction
boronic
ester-linked
through
nucleophilic
substitution
reactions
order
catalyze
CO
Journal of Materials Chemistry A,
Год журнала:
2023,
Номер
12(1), С. 87 - 112
Опубликована: Ноя. 27, 2023
This
review
surveys
Fe-based
dual-atom
catalysts
for
oxygen
reduction
reactions
in
next-generation
energy
devices,
including
challenges
with
single-atom
catalysts,
synthetic
methods,
catalytic
performance,
and
future
research
directions.
Advanced Materials,
Год журнала:
2024,
Номер
36(41)
Опубликована: Авг. 17, 2024
Dual-atom
catalysts
(DACs)
with
atomically
dispersed
dual-sites,
as
an
extension
of
single-atom
(SACs),
have
recently
become
a
new
hot
topic
in
heterogeneous
catalysis
due
to
their
maximized
atom
efficiency
and
dual-site
diverse
synergy,
because
the
synergistic
diversity
dual-sites
achieved
by
asymmetric
microenvironment
tailoring
can
efficiently
boost
catalytic
activity
optimizing
electronic
structure
DACs.
Here,
this
work
first
summarizes
frequently-used
experimental
synthesis
characterization
methods
Then,
four
mechanisms
(cascade
mechanism,
assistance
co-adsorption
mechanism
bifunction
mechanism)
key
modulating
(active
site
strategy,
transverse/axial-modification
engineering,
distance
engineering
strain
engineering)
are
elaborated
comprehensively.
The
emphasis
is
placed
on
effects
DACs
oxygen/carbon
dioxide
reduction
reaction.
Finally,
some
perspectives
outlooks
also
addressed.
In
short,
review
useful
strategy
speed
up
high-performance
electrocatalysts
for
different
reactions.
