Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(25)
Опубликована: Апрель 18, 2024
Abstract
The
evolution
of
two‐dimensional
conjugated
metal–organic
frameworks
(2D
c‐MOFs)
provides
a
significant
prospect
for
researching
the
next
generation
green
and
advanced
energy
storage
systems
(ESSs).
Especially,
conjugation
topology
engineering
serve
as
an
irreplaceable
character
in
adjusting
electrochemical
properties
ESSs.
Herein,
we
proposed
novel
strategy
using
to
demonstrate
application
2D
c‐MOFs
robust
potassium‐ion
batteries
(PIBs)
first
time.
By
comparing
with
rhombus/kagome
structure
well
three/four‐arm
core,
rhombus
(sql‐Cu‐TBA‐MOF)
cathode
PIBs
can
display
impressive
performance,
including
high
specific
discharge
capacity
178.4
mAh
g
−1
(at
0.2
A
)
long‐term
cycle
stability
more
than
9,000
10.0
).
Moreover,
full
(FPIBs)
are
constructed
by
pairing
sql‐Cu‐TBA‐MOF
dipotassium
terephthalate
(KTP)
anode,
which
delivers
reversible
146.6
0.1
great
practical
prospect.
These
findings
provide
reasonable
implications
design
from
perspective
systems.
Advanced Materials,
Год журнала:
2022,
Номер
34(52)
Опубликована: Март 31, 2022
Abstract
As
a
class
of
porous
materials
with
crystal
lattices,
metal–organic
frameworks
(MOFs),
featuring
outstanding
specific
surface
area,
tunable
functionality,
and
versatile
structures,
have
attracted
huge
attention
in
the
past
two
decades.
Since
first
conductive
MOF
is
successfully
synthesized
2009,
considerable
progress
has
been
achieved
for
development
MOFs,
allowing
their
use
diverse
applications
electrochemical
energy
storage.
Among
those
applications,
supercapacitors
received
great
interest
because
high
power
density,
fast
charging
ability,
excellent
cycling
stability.
Here,
efforts
hitherto
devoted
to
synthesis
design
MOFs
auspicious
capacitive
performance
are
summarized.
Using
as
unique
platform
medium,
electronic
molecular
aspects
storage
mechanism
electrodes
discussed,
highlighting
advantages
limitations
inspire
new
ideas
supercapacitors.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(9), С. 5105 - 5113
Опубликована: Фев. 16, 2023
Covalent
organic
framework
(COF)
materials
with
porous
character
and
robust
structure
have
significant
applied
implications
for
K-ion
battery
(KIB)
anodes,
but
they
are
limited
by
the
low
reversible
capacity
inferior
rate
capability.
Here,
based
on
theoretical
calculations,
we
identified
that
a
bulk
COF
featuring
numerous
pyrazines
carbonyls
in
π-conjugated
periodic
skeleton
could
provide
multiple
accessible
redox-active
sites
high-performance
potassium
storage.
Its
surface-dominated
storage
mechanism
enabled
fast
stable
of
K-ions.
insolubility
electrolytes
small
volumetric
change
after
potassiation
ensured
electrode
cycling.
As
KIB
anode,
this
demonstrated
an
unprecedentedly
outstanding
combination
(423
mAh
g-1
at
0.1
C),
capability
(185
10
cyclability.
The
simulation
comprehensive
characterizations
confirmed
active
contributed
C═O,
C═N,
cation-π
effect.
Metal-organic
frameworks
(MOFs)
with
diverse
composition,
tunable
structure,
and
unique
physicochemical
properties
have
emerged
as
promising
materials
in
various
fields.
The
pore
abundant
active
sites,
ultrahigh
specific
surface
area
can
facilitate
mass
transport
provide
outstanding
capacity,
making
MOFs
an
ideal
material
for
electrochemical
energy
storage
conversion.
However,
the
poor
electrical
conductivity
of
pristine
severely
limits
their
applications
electrochemistry.
Developing
conductive
has
proved
to
be
effective
solution
this
problem.
This
review
focuses
on
design
synthesis
MOF
composites
judiciously
chosen
conducting
materials,
MOFs,
assembly
methods,
well
preparation
intrinsically
based
building
2D
π-conjugated
structures,
introducing
mixed-valence
metal
ions/redox-active
ligands,
designing
π-π
stacked
pathways,
constructing
infinite
metal-sulfur
chains
(-M-S-)∞
.
Furthermore,
recent
progress
challenges
conversion
(supercapacitors,
Li-ion
batteries,
Li-S
water
splitting)
are
summarized.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(11)
Опубликована: Янв. 24, 2023
Two-dimensional
conductive
metal-organic
frameworks
(2D-c-MOFs)
have
attracted
extensive
attention
owing
to
their
unique
structures
and
physical-chemical
properties.
However,
the
planarly
extended
structure
of
2D-c-MOFs
usually
limited
accessibility
active
sites.
Herein,
we
designed
a
triptycene-based
2D
vertically
MOF
(2D-vc-MOF)
by
coordinating
2,3,6,7,14,15-hexahydroxyltriptycene
(HHTC)
with
Cu2+
.
The
2D-vc-MOF(Cu)
possesses
weak
interlayer
interaction,
which
leads
facile
exfoliation
nanosheet.
Compared
classical
structures,
exhibits
100
%
increased
catalytic
activity
in
terms
turnover
number
two-fold
selectivity.
Density
functional
theory
(DFT)
calculations
further
revealed
that
higher
originated
from
lower
energy
barriers
during
CO2
reduction
reaction
process.
Crystal Growth & Design,
Год журнала:
2024,
Номер
24(5), С. 2235 - 2265
Опубликована: Фев. 26, 2024
Metal-organic
frameworks
(MOFs),
formed
by
the
combination
of
both
inorganic
and
organic
components,
have
attracted
special
attention
for
their
tunable
porous
structures,
chemical
functional
diversities,
enormous
applications
in
gas
storage,
catalysis,
sensing,
etc.
Recently,
electronic
MOFs
like
electrocatalysis,
supercapacitors,
batteries,
electrochemical
etc.,
become
a
major
research
topic
MOF
chemistry.
However,
low
electrical
conductivity
most
represents
handicap
development
these
emerging
applications.
To
overcome
limitations,
different
strategies
been
developed
to
enhance
implementation
devices.
In
this
review,
we
outline
all
employed
increase
conduction
intrinsically
(framework-modulated)
extrinsically
(guests-modulated)
conducting
MOFs.
eScience,
Год журнала:
2023,
Номер
3(2), С. 100094 - 100094
Опубликована: Янв. 13, 2023
Sn-based
materials
are
promising
candidates
for
lithium
storage
but
suffer
generally
from
huge
volume
change
during
the
(de)lithiation
processes.
Sn-organic
with
monodispersed
Sn
centers
surrounded
by
active
ligands
can
alleviate
of
anode
based
on
reversible
However,
structural
factors
governing
kinetics
and
utilization
efficiency
sites
not
well
understood
to
date.
Herein,
we
report
three
two-dimensional
enhanced
performance
manipulation
π-aromatic
conjugation
ligands.
The
increasing
plays
a
key
role
in
promoting
efficient
storage,
expansion
reaction
is
suppressed
these
materials.
This
work
reveals
that
ligand
crucial
improving
metal-organic
minimised
expansion.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(21)
Опубликована: Март 10, 2023
Abstract
Organic
redox‐active
materials
are
promising
electrode
candidates
for
lithium‐ion
batteries
by
virtue
of
their
designable
structure
and
cost‐effectiveness.
However,
poor
electrical
conductivity
high
solubility
in
organic
electrolytes
limit
the
device's
performance
practical
applications.
Herein,
π‐conjugated
nitrogen‐containing
heteroaromatic
molecule
hexaazatriphenylene
(HATN)
is
strategically
embedded
with
centers
skeleton
a
Cu‐based
2D
conductive
metal–organic
framework
(2D
c
‐MOF)
to
optimize
lithium
(Li)
storage
electrodes,
which
delivers
improved
specific
capacity
(763
mAh
g
−1
at
300
mA
),
long‐term
cycling
stability
(≈90%
retention
after
600
cycles
excellent
rate
performance.
The
correlation
experimental
computational
results
confirms
that
this
Li
derives
from
maximum
number
active
sites
(CN
HATN
unit
CO
CuO
4
unit),
favorable
conductivity,
efficient
mass
transfer
channels.
This
strategy
integrating
multiple
moieties
into
‐MOF
opens
up
new
avenue
design
high‐performance
materials.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(10), С. 6753 - 6762
Опубликована: Фев. 27, 2024
High-temperature
rechargeable
batteries
are
essential
for
energy
storage
in
elevated-temperature
situations.
Due
to
the
resource
abundance
of
potassium,
high-temperature
K-ion
drawing
increasing
research
interest.
However,
raising
working
temperature
would
aggravate
chemical
and
mechanical
instability
KIB
anode,
resulting
very
fast
capacity
fading,
especially
when
high
is
pursued.
Here,
we
demonstrated
that
a
porous
conductive
metal–organic
framework
(MOF),
which
constructed
by
N-rich
aromatic
molecules
CuO4
units
via
π–d
conjugation,
could
provide
multiple
accessible
redox-active
sites
promised
robust
structure
stability
efficient
potassium
at
temperatures.
Even
60
°C,
this
MOF
anode
deliver
initial
(455
mAh
g–1),
impressive
rate,
extraordinary
cyclability
(96.7%
retention
1600
cycles),
much
better
than
those
reported
anodes.
The
mechanistic
study
revealed
C═N
groups
contributed
abundant
sites;
synergistic
effect
conjugated
character
reticular
architecture
facilitated
K+/e–
transport
ensured
an
insoluble
electrode
with
small
volume
deformation,
thus
achieving
stable
high-capacity
storage.