Advanced Functional Materials,
Год журнала:
2023,
Номер
33(28)
Опубликована: Апрель 28, 2023
Abstract
Dielectric
materials
with
higher
energy
storage
and
electromagnetic
(EM)
conversion
are
in
high
demand
to
advance
electronic
devices,
military
stealth,
mitigate
EM
wave
pollution.
Existing
dielectric
for
high‐energy‐storage
electronics
loss
absorbers
studied
toward
realizing
these
goals,
each
aligned
the
current
global
grand
challenges.
Libraries
of
desirable
permittivity,
loss,
and/or
breakdown
strength
potentially
meeting
device
requirements
reviewed
here.
Regardless,
aimed
at
translating
into
oft‐encountered
shortcomings
can
be
caused
by
either
two
confluences:
a)
low
strength;
b)
process
complexity.
Contextualizing
aspects
overarching
objectives
enabling
high‐efficiency
conversion,
recent
advances
by‐design
inorganic–organic
hybrid
here,
a
focus
on
design
approaches,
preparation
methods,
characterization
techniques.
In
light
their
strengths
weaknesses,
potential
strategies
foster
commercial
adoption
critically
interrogated.
Materials Horizons,
Год журнала:
2021,
Номер
8(9), С. 2387 - 2419
Опубликована: Янв. 1, 2021
An
emerging
trend
in
the
application
of
metal–organic
frameworks
is
to
engineer
mobile
devices
possess
chemical
detecting
capabilities
for
environmental
monitoring,
point-of-care
testing,
artificial
intelligence,
food
security
and
defence.
Chemical Reviews,
Год журнала:
2021,
Номер
122(1), С. 442 - 564
Опубликована: Дек. 1, 2021
Synthetic
chemists
have
developed
robust
methods
to
synthesize
discrete
molecules,
linear
and
branched
polymers,
disordered
cross-linked
networks.
However,
two-dimensional
polymers
(2DPs)
prepared
from
designed
monomers
been
long
missing
these
capabilities,
both
as
objects
of
chemical
synthesis
in
nature.
Recently,
new
polymerization
strategies
characterization
enabled
the
unambiguous
realization
covalently
linked
macromolecular
sheets.
Here
we
review
2DPs
2D
methods.
Three
predominant
emerged
date,
which
produce
either
monolayers
or
multilayer
assemblies.
We
discuss
fundamental
understanding
scope
each
approaches,
including:
bond-forming
reactions
used,
synthetic
diversity
prepared,
their
stacking
behaviors,
nanoscale
mesoscale
structures,
macroscale
morphologies.
Additionally,
describe
analytical
tools
currently
available
characterize
various
isolated
forms.
Finally,
emergent
2DP
properties
potential
applications
planar
macromolecules.
Throughout,
highlight
achievements
identify
opportunities
for
continued
study.
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.
ACS Nano,
Год журнала:
2022,
Номер
16(2), С. 1759 - 1780
Опубликована: Янв. 20, 2022
A
highly
effective
electrocatalyst
is
the
central
component
of
advanced
electrochemical
energy
conversion.
Recently,
two-dimensional
conjugated
metal-organic
frameworks
(2D
c-MOFs)
have
emerged
as
a
class
promising
electrocatalysts
because
their
advantages
including
2D
layered
structure
with
high
in-plane
conjugation,
intrinsic
electrical
conductivity,
permanent
pores,
large
surface
area,
chemical
stability,
and
structural
diversity.
In
this
Review,
we
summarize
recent
advances
c-MOF
for
First,
introduce
design
principles
synthetic
strategies
reported
c-MOFs,
well
functional
electrocatalysis.
Subsequently,
present
representative
in
various
reactions,
such
hydrogen/oxygen
evolution,
reduction
reactions
oxygen,
carbon
dioxide,
nitrogen.
We
highlight
property
tuning
to
boost
catalytic
performance,
offer
our
perspectives
regard
challenges
be
overcome.
Journal of the American Chemical Society,
Год журнала:
2021,
Номер
143(47), С. 19992 - 20000
Опубликована: Ноя. 16, 2021
The
electrochemical
N2
reduction
reaction
(NRR)
under
ambient
conditions
is
attractive
in
replacing
the
current
Haber-Bosch
process
toward
sustainable
ammonia
production.
Metal-heteroatom-doped
carbon-rich
materials
have
emerged
as
most
promising
NRR
electrocatalysts.
However,
simultaneously
boosting
their
activity
and
selectivity
remains
a
grand
challenge,
while
principle
for
precisely
tailoring
active
sites
has
been
elusive.
Herein,
we
report
first
case
of
crystalline
two-dimensional
conjugated
covalent
organic
frameworks
(2D
c-COFs)
incorporated
with
M-N4-C
centers
novel,
defined,
effective
catalysts,
achieving
enhanced
electrocatalytic
to
ammonia.
Such
2D
c-COFs
are
synthesized
based
on
metal-phthalocyanine
(M
=
Fe,
Co,
Ni,
Mn,
Zn,
Cu)
pyrene
units
bonded
by
pyrazine
linkages.
Significantly,
Fe-N4-C
center
exhibit
higher
yield
rate
(33.6
μg
h-1
mgcat-1)
Faradaic
efficiency
(FE,
31.9%)
at
-0.1
V
vs
reversible
hydrogen
electrode
than
those
other
centers,
making
them
among
best
electrocatalysts
(yield
>30
mgcat-1
FE
>
30%).
In
situ
X-ray
absorption
spectroscopy,
Raman
spectroelectrochemistry,
theoretical
calculations
unveil
that
act
catalytic
sites.
They
show
unique
electronic
structure
localized
states
Fermi
level,
allowing
stronger
interaction
thus
faster
activation
kinetics
centers.
Our
work
opens
possibility
developing
metal-nitrogen-doped
superior
electrocatalyst
provides
an
atomic
understanding
M-Nx-C
designing
high-performance
catalysts.
Designing
a
functional,
conductive
metal-organic
framework
(cMOF)
is
highly
desired.
Substantial
efforts
have
been
dedicated
to
increasing
the
intralayer
conjugation
of
cMOFs,
while
less
dedication
has
made
tuning
interlayer
charge
transport
nanosheets
for
controllable
dielectric
property.
Here,
we
construct
series
bimetallic
organic
frameworks
(Zn
x
Cu
3-x
)
(hexahydroxytriphenylene)
2
(ZnCu-HHTP)
allow
fine-tuned
spacing
two-dimensional
frameworks,
by
adjusting
ratios
Zn
and
metal
ions.
This
approach
atomistic
design
allows
finely
control
transport,
band
structure,
properties
cMOF.
As
result,
Zn3Cu1-HHTP,
with
an
optimal
property,
exhibits
high-efficiency
absorption
in
gigahertz
microwave
range,
achieving
ultra-strong
reflection
loss
−81.62
decibels.
study
not
only
advances
understanding
microstructure-function
relationships
cMOFs
but
also
offers
generic
nanotechnology–based
MOFs
targeted
applications.
