ACS Sustainable Chemistry & Engineering,
Год журнала:
2024,
Номер
12(26), С. 9787 - 9794
Опубликована: Июнь 19, 2024
Mitigating
global
CO2
concentrations
from
anthropogenic
sources
through
electrochemical
conversion
to
value-added
chemicals
is
the
need
of
hour.
In
this
work,
fundamental
concept
"Lattice
Charge"
has
been
strategically
manipulated
in
materials
selectively
produce
multi-carbon
products
greenhouse
gas.
To
achieve
this,
a
series
catalysts
within
well-known
ABX2
family
(A
=
Ag,
Cu;
B
In,
Ga,
Fe;
X
S,
Se)
have
explored,
which
exhibit
significant
activity
toward
reduction
reaction
(eCO2RR)
and
results
formation
higher
carbon
including
C3
products,
acetone,
energy-dense
isopropanol
(FE
24.5
±
2.5%).
The
Hirshfeld
charge
analysis
technique
highlighted
structure–activity
correlation
importance
optimized
lattice
distribution
as
crucial
tool
manipulate
eCO2RR
product
electrocatalyst
designs,
real-time
situ
ATR-FTIR
probes
intermediate
species
adsorbed
during
process.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(28)
Опубликована: Май 7, 2024
Alkali
metals
(e.g.
Li,
Na,
and
K)
multivalent
Zn,
Mg,
Ca,
Al)
have
become
star
anodes
for
developing
high-energy-density
rechargeable
batteries
due
to
their
high
theoretical
capacity
excellent
conductivity.
However,
the
inevitable
dendrites
unstable
interfaces
of
metal
pose
challenges
safety
stability
batteries.
To
address
these
issues,
covalent
organic
frameworks
(COFs),
as
emerging
materials,
been
widely
investigated
regular
porous
structure,
flexible
molecular
design,
specific
surface
area.
In
this
minireview,
we
summarize
research
progress
COFs
in
stabilizing
anodes.
First,
present
origins
delve
into
advantages
based
on
physical/chemical
properties
alkali
metals.
Then,
special
attention
has
paid
application
host
design
anodes,
artificial
solid
electrolyte
interfaces,
additives,
solid-state
electrolytes,
separator
modifications.
Finally,
a
new
perspective
is
provided
from
pore
modulation,
synthesis
COFs.
ACS Nano,
Год журнала:
2024,
Номер
18(33), С. 21804 - 21835
Опубликована: Авг. 8, 2024
Covalent
organic
frameworks
(COFs)
are
crystalline
networks
with
extended
backbones
cross-linked
by
covalent
bonds.
Due
to
the
semiconductive
properties
and
variable
metal
coordinating
sites,
along
rapid
development
in
linkage
chemistry,
utilization
of
COFs
photocatalytic
CO2RR
has
attracted
many
scientists'
interests.
In
this
Review,
we
summarize
latest
research
progress
on
for
CO2
reduction.
first
part,
present
COF
linkages
that
have
been
used
CO2RR,
discuss
four
mechanisms
including
as
intrinsic
photocatalysts,
photosensitive
motifs
metalated
semiconductors
heterojunction
photocatalysts.
Then,
principles
structural
designs
functional
building
units
stacking
mode
exchange.
Finally,
outlook
challenges
provided.
This
Review
is
intended
give
some
guidance
design
synthesis
diverse
different
linkages,
various
structures,
divergent
modes
efficient
photoreduction
CO2.
Growing
global
population,
escalating
energy
consumption,
and
climate
change
threaten
future
security.
Fossil
fuel
combustion,
primarily
coal,
oil,
natural
gas,
exacerbates
the
greenhouse
effect
driving
warming
through
CO
Constructing
a
strong
bonded
interface
is
highly
desired
to
build
fast
charge-transfer
channels
and
tune
reactive
sites
for
optimizing
CO2
photoreduction.
In
this
work,
covalent
triazine
framework
(CTF)
combined
with
Bi19S27Br3
heterojunction
designed
using
an
electrostatic
self-assembly
process.
Due
the
oppositely
charged
states
between
two
components
ultrasonic
treatment,
coupled
realized
formation
of
Bi–C/N/O
bonds,
leading
robust
interfacial
polarization.
This
feature
causes
charge
redistribution,
intensifies
interaction
N
CO2,
stabilizes
intermediate
state,
lowers
reaction
energy
barrier.
Meanwhile,
chemically
favors
rapid
electron
migration
from
CTF,
as
proved
by
ultrafast
transient
absorption
spectroscopy
in
situ
irradiation
XPS.
As
result,
CTF/Bi19S27Br3
delivers
superior
photoreduction
performance
yield
CO
(572.2
μmol
g–1
h–1)
pure
water
system,
which
38.6
times
that
Bi19S27Br3,
apparent
quantum
yields
up
7.9
6.2%
at
380
400
nm,
respectively.
coupling
strategy
provides
accessible
pathway
designing
polarized,
high-efficiency
photocatalysts.
Angewandte Chemie,
Год журнала:
2024,
Номер
136(28)
Опубликована: Май 7, 2024
Abstract
Alkali
metals
(e.g.
Li,
Na,
and
K)
multivalent
Zn,
Mg,
Ca,
Al)
have
become
star
anodes
for
developing
high‐energy‐density
rechargeable
batteries
due
to
their
high
theoretical
capacity
excellent
conductivity.
However,
the
inevitable
dendrites
unstable
interfaces
of
metal
pose
challenges
safety
stability
batteries.
To
address
these
issues,
covalent
organic
frameworks
(COFs),
as
emerging
materials,
been
widely
investigated
regular
porous
structure,
flexible
molecular
design,
specific
surface
area.
In
this
minireview,
we
summarize
research
progress
COFs
in
stabilizing
anodes.
First,
present
origins
delve
into
advantages
based
on
physical/chemical
properties
alkali
metals.
Then,
special
attention
has
paid
application
host
design
anodes,
artificial
solid
electrolyte
interfaces,
additives,
solid‐state
electrolytes,
separator
modifications.
Finally,
a
new
perspective
is
provided
from
pore
modulation,
synthesis
COFs.
Chemistry of Materials,
Год журнала:
2024,
Номер
36(15), С. 7362 - 7369
Опубликована: Июль 26, 2024
Covalent
organic
frameworks
(COFs)
linked
by
imine
bonds
have
attracted
significant
attention,
primarily
due
to
the
accessibility
of
monomers
and
facile
synthesis
highly
crystalline
materials.
However,
reversible
nature
raises
stability
concerns
for
these
materials
in
practical
applications.
Therefore,
there
is
a
pressing
need
development
imine-linked
COFs
that
can
combine
high
crystallinity,
good
stability,
functionality.
Here,
adopting
two-in-one
molecular
design
strategy,
we
designed
an
building
block
containing
both
acetal
amino
connecting
groups,
featuring
pyridine
functional
site,
with
side
chains
consisting
alkoxyl
groups.
Following
synthesis,
elements
were
combined
confined
channel
(0.85
nm),
leading
two-dimensional
(2D)
(COF-LIFM4
COF-LIFM5)
crystallinity
strong
acid
base
conditions.
Moreover,
COF-LIFM5
exhibited
favorable
CO2
affinity
appropriate
hydrophobicity,
making
it
promising
modifier
improving
mass
transfer
reduction
reaction
(CO2RR).
As
result,
Cu/COF-LIFM5
showcased
enhanced
C2+
product
selectivity
CO2RR,
Faradaic
efficiency
exceeding
80%
at
current
density
500
mA
cm–2
flow
cell.
Science China Materials,
Год журнала:
2024,
Номер
68(1), С. 21 - 38
Опубликована: Ноя. 8, 2024
Abstract
The
conversion
of
carbon
dioxide
(CO
2
)
to
the
reduced
chemical
compounds
offers
substantial
environmental
benefits
through
minimizing
emission
greenhouse
gas
and
fostering
sustainable
practices.
Recently,
unique
properties
metal-organic
frameworks
(MOFs)
make
them
attractive
candidates
for
electrocatalytic
CO
reduction
reaction
RR),
providing
many
opportunities
develop
efficient,
selective,
environmentally
processes
mitigating
emissions
utilizing
as
a
valuable
raw
material
synthesis
fuels
chemicals.
Here,
recent
advances
in
MOFs
efficient
catalysts
RR
are
summarized.
detailed
characteristics,
mechanisms,
practical
approaches
improving
efficiency,
selectivity,
durability
under
realistic
conditions
also
clarified.
Furthermore,
outlooks
on
prospects
MOF-based
electrocatalysts
provided.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
unknown
Опубликована: Июнь 27, 2024
Abstract
The
multiple
mortise‐and‐tenon
joint
parts
are
the
core
factors
to
provide
structural
stability
and
diversity
of
Chinese
Luban
locks;
however,
constructing
such
structures
is
very
challenging.
Herein,
single
crystals
a
covalent
organic
nanoribbon
(named
CityU‐27
)
prepared
through
assembly
hexahydroxytriphenylene
(HHTP),
4,4′‐vinylenedipyridine
(BYE),
phenylboronic
acid
(BA)
together
dative
boron←nitrogen
(B←N)
bonds.
single‐crystal
X‐ray
diffraction
analysis
indicates
that
has
structure,
where
each
forms
tight
π–π
interactions
with
four
neighboring
others
generate
lock‐like
configuration.
been
demonstrated
be
an
efficient
photocatalyst
in
one‐pot
tandem
reaction
hydrogen
evolution
(HER)
semi‐hydrogenation
alkynes
series
produce
olefins
without
any
additional
photosensitizers
co‐catalysts
(metal‐free).