Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(36), С. 19797 - 19803
Опубликована: Май 27, 2021
Abstract
Covalent
organic
frameworks
(COFs)
have
emerged
as
an
important
class
of
semiconductors
and
photocatalysts
for
the
hydrogen
evolution
reaction
(HER)from
water.
To
optimize
their
photocatalytic
activity,
typically
moieties
constituting
are
considered
most
suitable
combinations
them
searched
for.
However,
effect
covalent
linkage
between
these
on
performance
has
rarely
been
studied.
Herein,
we
demonstrate
that
donor‐acceptor
(D‐A)
type
imine‐linked
COFs
can
produce
with
a
rate
high
20.7
mmol
g
−1
h
under
visible
light
irradiation,
upon
protonation
imine
linkages.
A
significant
red‐shift
in
absorbance,
largely
improved
charge
separation
efficiency,
increase
hydrophilicity
triggered
by
Schiff‐base
COFs,
responsible
performance.
Journal of the American Chemical Society,
Год журнала:
2020,
Номер
142(49), С. 20763 - 20771
Опубликована: Ноя. 23, 2020
Excitonic
effects
caused
by
Coulomb
interactions
between
electrons
and
holes
play
subtle
significant
roles
on
photocatalysis,
yet
have
been
long
ignored.
Herein,
porphyrinic
covalent
organic
frameworks
(COFs,
specifically
DhaTph-M),
in
the
absence
or
presence
of
different
metals
porphyrin
centers,
shown
as
ideal
models
to
regulate
excitonic
effects.
Remarkably,
incorporation
Zn2+
COF
facilitates
conversion
singlet
triplet
excitons,
whereas
Ni2+
introduction
promotes
dissociation
excitons
hot
carriers
under
photoexcitation.
Accordingly,
discriminative
behavior
DhaTph-Zn
DhaTph-Ni
enables
activation
O2
1O2
O2•–,
respectively,
visible
light
irradiation,
resulting
distinctly
activity
selectivity
photocatalytic
terpinene
oxidation.
Benefiting
from
these
results,
exhibits
excellent
O2•–-engaged
hydroxylation
boronic
acid,
while
possesses
superior
performance
1O2-mediated
selective
oxidation
sulfides.
This
work
provides
in-depth
insights
into
molecular
oxygen
opens
an
avenue
regulation
based
COFs.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(6), С. 1887 - 1931
Опубликована: Янв. 1, 2020
This
article
provides
a
comprehensive
review
of
the
latest
progress,
challenges
and
recommended
future
research
related
to
metal-free
photocatalysts
for
hydrogen
productionviawater-splitting.
Chemical Reviews,
Год журнала:
2020,
Номер
120(21), С. 11810 - 11899
Опубликована: Авг. 13, 2020
Atomically
dispersed
metal
catalysts
(ADCs),
as
an
emerging
class
of
heterogeneous
catalysts,
have
been
widely
investigated
during
the
past
two
decades.
The
atomic
dispersion
nature
catalytic
centers
makes
them
ideal
system
for
bridging
homogeneous
and
catalysts.
recent
rapid
development
new
synthetic
strategies
has
led
to
explosive
growth
ADCs
with
a
wide
spectrum
atoms
on
supports
different
chemical
compositions
natures.
availability
diverse
creates
powerful
materials
platform
investigating
mechanisms
complicated
catalysis
at
levels.
Considering
most
are
coordinated
by
donors
from
supports,
this
review
will
demonstrate
how
surface
coordination
chemistry
plays
important
role
in
determining
performance
ADCs.
This
start
link
between
catalysis.
After
brief
description
advantages
limitations
common
structure
characterization
methods
ADCs,
types
be
discussed.
We
mainly
illustrate
local
vicinal
species
support
systems
act
together
center
determine
activity,
selectivity,
stability
dynamic
change
highlighted.
At
end
review,
personal
perspectives
further
field
provided.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(12), С. 3920 - 3951
Опубликована: Янв. 1, 2020
This
review
highlights
the
state-of-the-art
progress
achieved
in
two-dimensional
covalent
organic
frameworks
(COFs)
with
hierarchical
porosity,
an
emerging
class
of
COFs
constructed
by
integrating
different
types
pores
into
one
framework.
Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
59(33), С. 13722 - 13733
Опубликована: Апрель 9, 2020
Abstract
Many
sophisticated
chemical
and
physical
properties
of
porous
materials
strongly
rely
on
the
presence
metal
ions
within
structures.
Whereas
homogeneous
distribution
metals
is
conveniently
realized
in
metal–organic
frameworks
(MOFs),
limited
stability
potentially
restricts
their
practical
implementation.
From
that
perspective,
development
metal–covalent
organic
(MCOFs)
may
address
these
shortcomings
by
incorporating
active
species
atop
highly
stable
COF
backbones.
This
Minireview
highlights
examples
MCOFs
tackle
important
issues
from
design,
synthesis,
characterization
to
cutting‐edge
applications.
Chemical Society Reviews,
Год журнала:
2021,
Номер
50(4), С. 2540 - 2581
Опубликована: Янв. 1, 2021
The
recent
progress
made
on
porphyrin-based
frameworks
and
their
applications
in
energy-related
conversion
technologies
(e.g.,
ORR,
OER
CO2RR)
storage
Zn–air
batteries).
Nature,
Год журнала:
2022,
Номер
604(7904), С. 72 - 79
Опубликована: Апрель 6, 2022
Abstract
Covalent
organic
frameworks
(COFs)
are
distinguished
from
other
polymers
by
their
crystallinity
1–3
,
but
it
remains
challenging
to
obtain
robust,
highly
crystalline
COFs
because
the
framework-forming
reactions
poorly
reversible
4,5
.
More
chemistry
can
improve
6–9
this
typically
yields
with
poor
physicochemical
stability
and
limited
application
scope
5
Here
we
report
a
general
scalable
protocol
prepare
imine
COFs,
based
on
an
unexpected
framework
reconstruction.
In
contrast
standard
approaches
in
which
monomers
initially
randomly
aligned,
our
method
involves
pre-organization
of
using
removable
covalent
tether,
followed
confined
polymerization.
This
reconstruction
route
produces
reconstructed
greatly
enhanced
much
higher
porosity
means
simple
vacuum-free
synthetic
procedure.
The
increased
improves
charge
carrier
transport,
leading
sacrificial
photocatalytic
hydrogen
evolution
rates
up
27.98
mmol
h
−1
g
nanoconfinement-assisted
strategy
is
step
towards
programming
function
materials
through
atomistic
structural
control.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(17), С. 6248 - 6272
Опубликована: Янв. 1, 2020
Owing
to
the
unique
structural
features
and
facile
tunability
of
subcomponents
channels,
chiral
COFs
show
great
potential
in
heterogeneous
catalysis,
enantioselective
separation,
recognition.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(3), С. 839 - 864
Опубликована: Янв. 1, 2020
This
review
highlights
the
luminescent
and
unique
photophysical
properties
of
covalent
organic
frameworks.
Their
potential
use
in
applications
related
to
chemical
sensing,
photocatalysis,
optoelectronics
are
discussed.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(8), С. 2291 - 2302
Опубликована: Янв. 1, 2020
Covalent
organic
frameworks
are
crystalline
porous
materials
with
2-
or
3-dimensional
structures
designed
modularly
from
their
molecular
precursors.
Using
bottom-up
top-down
strategies,
single-
few-layer
can
be
obtained
them.