Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Июль 3, 2023
Understanding
charge
transfer
dynamics
and
carrier
separation
pathway
is
challenging
due
to
the
lack
of
appropriate
characterization
strategies.
In
this
work,
a
crystalline
triazine/heptazine
carbon
nitride
homojunction
selected
as
model
system
demonstrate
interfacial
electron-transfer
mechanism.
Surface
bimetallic
cocatalysts
are
used
sensitive
probes
during
in
situ
photoemission
for
tracing
S-scheme
photogenerated
electrons
from
triazine
phase
heptazine
phase.
Variation
sample
surface
potential
under
light
on/off
confirms
dynamic
transfer.
Further
theoretical
calculations
an
interesting
reversal
path
light/dark
conditions,
which
also
supports
experimental
evidence
transport.
Benefiting
unique
merit
electron
transfer,
shows
significantly
enhanced
activity
CO2
photoreduction.
Our
work
thus
provides
strategy
probe
mechanisms
design
delicate
material
structures
towards
efficient
Chemical Society Reviews,
Год журнала:
2021,
Номер
50(8), С. 5281 - 5322
Опубликована: Янв. 1, 2021
This
review
presents
the
recent
advances
in
synthetic
strategies,
characterisation,
and
computations
of
carbon-based
single-atom
catalysts,
as
well
their
innovative
applications
mechanisms
advanced
oxidation
technologies.
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).
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(37), С. 17097 - 17109
Опубликована: Сен. 6, 2022
Solar
carbon
dioxide
(CO2)
conversion
is
an
emerging
solution
to
meet
the
challenges
of
sustainable
energy
systems
and
environmental/climate
concerns.
However,
construction
isolated
active
sites
not
only
influences
catalytic
activity
but
also
limits
understanding
structure-catalyst
relationship
CO2
reduction.
Herein,
we
develop
a
universal
synthetic
protocol
fabricate
different
single-atom
metal
(e.g.,
Fe,
Co,
Ni,
Zn,
Cu,
Mn,
Ru)
anchored
on
triazine-based
covalent
organic
framework
(SAS/Tr-COF)
backbone
with
bridging
structure
metal-nitrogen-chlorine
for
high-performance
Remarkably,
as-synthesized
Fe
SAS/Tr-COF
as
representative
catalyst
achieved
impressive
CO
generation
rate
high
980.3
μmol
g-1
h-1
selectivity
96.4%,
over
approximately
26
times
higher
than
that
pristine
Tr-COF
under
visible
light
irradiation.
From
X-ray
absorption
fine
analysis
density
functional
theory
calculations,
superior
photocatalytic
performance
attributed
synergic
effect
atomically
dispersed
host,
decreasing
reaction
barriers
formation
*COOH
intermediates
promoting
adsorption
activation
well
desorption.
This
work
affords
rational
design
state-of-the-art
catalysts
at
molecular
level
provides
in-depth
insights
efficient
conversion.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(4), С. 1861 - 1871
Опубликована: Янв. 20, 2022
Single
clusters
have
attracted
extensive
research
interest
in
the
field
of
catalysis.
However,
achieving
a
highly
uniform
dispersion
single-cluster
catalyst
is
challenging.
In
this
work,
for
first
time,
we
present
versatile
strategy
uniformly
dispersed
polyoxometalates
(POMs)
covalent
organic
frameworks
(COFs)
through
confining
POM
cluster
into
regular
nanopores
COF
by
linkage.
These
COF-POM
composites
combine
properties
light
absorption,
electron
transfer,
and
suitable
catalytic
active
sites;
as
result,
they
exhibit
outstanding
activity
artificial
photosynthesis:
that
is,
CO2
photoreduction
with
H2O
donor.
Among
them,
TCOF-MnMo6
achieved
highest
CO
yield
(37.25
μmol
g-1
h-1
ca.
100%
selectivity)
gas-solid
reaction
system.
Furthermore,
mechanism
study
based
on
density
functional
theory
(DFT)
calculations
demonstrated
photoinduced
transfer
(PET)
process
occurs
from
to
POM,
then
reduction
oxidation
occur
COF,
respectively.
This
work
developed
method
single
which
also
shows
potential
using
materials
photocatalysis.
ACS Catalysis,
Год журнала:
2021,
Номер
11(15), С. 9569 - 9577
Опубликована: Июль 16, 2021
Transition
metal
catalysts
are
known
to
activate
persulfate,
but
the
properties
that
govern
intrinsic
activity
of
these
still
unknown.
Here,
we
developed
a
series
with
transition
metals
anchored
on
carbon
nanotubes
(denoted
M–N–CNTs,
where
M
=
Co,
Fe,
Mn,
or
Ni)
containing
single-atom
M–N
moieties,
peroxymonosulfate
for
efficient
nonradical
oxidation
sulfamethoxazole.
The
spin
state
M–N–CNTs
strongly
determined
their
catalytic
activity.
A
large
effective
magnetic
moment
high
(e.g.,
Co–N)
favored
overlap
d
orbitals
oxygen-containing
adsorbates
(such
as
peroxo
species)
active
sites
and
promoted
electron
transfer,
which
facilitated
adsorption
enhanced
capacity
reactive
species.
These
findings
advance
mechanistic
understanding
metal-mediated
persulfate
activation
inform
development
spintronic
environmental
applications.
ACS Catalysis,
Год журнала:
2021,
Номер
11(8), С. 4739 - 4769
Опубликована: Апрель 5, 2021
The
effective
separation
of
photogenerated
carriers
plays
a
vital
role
in
photocatalytic
reactions.
In
addition
to
the
intrinsic
driving
force
photocatalysis,
an
external
field
generating
enhancement
effect
can
provide
extra
energy
system,
acting
as
additional
impetus
separate
charges
and
thus
improving
overall
catalytic
efficiency.
Under
favorable
noncontact
conditions,
exploring
field,
different
from
pure
photocatalysis
or
photoelectrocatalysis,
could
widen
applications
technology.
this
review,
four
typical
fields
(i.e.,
thermal,
magnetic,
microwave,
ultrasonic
fields)
their
coupling
effects
on
are
summarized.
Specifically,
review
focuses
mechanism
characteristics
each
field's
synergistic
performance
system.
charge
forces
provided
by
traditional
one
distinguished
defined
for
first
time.
challenges
future
prospects
external-field-driven
discussed.
We
hope
that
will
reference
research
development
external-field-assisted
give
insights
in-depth
study
external-field-coupling-enhanced
toward
improvement
Accounts of Materials Research,
Год журнала:
2021,
Номер
2(5), С. 327 - 339
Опубликована: Фев. 26, 2021
ConspectusThe
fine
design
and
regulation
of
catalysts
play
critical
roles
in
the
development
catalysis.
The
microenvironment,
which
gives
rise
to
unique
spatial
structures
electronic
properties
around
catalytic
sites,
has
been
proven
dramatically
regulate
behavior
enzymes
homogeneous
However,
understanding
microenvironment
modulation
(MEM)
sites
remains
challenging
very
limited
heterogeneous
catalysis
mainly
due
lack
structural
precision
and/or
tailorability
traditional
solid
catalysts.
Among
diverse
materials,
metal–organic
frameworks
(MOFs),
a
class
porous
crystalline
solids,
have
intensively
studied
as
recent
years.
atomically
precise
well
tunable
MOFs
make
them
an
ideal
platform
for
rationally
regulating
surrounding
sites.
Accordingly,
their
well-defined
hold
great
promise
elucidating
how
affects
resulting
performance.
Nevertheless,
investigations
accurate
control
over
modulated
are
still
limited.
Therefore,
it
is
importance
summarize
related
results
provide
in-depth
insights
into
MOF-based
catalysis,
accelerating
future
this
emerging
research
topic.In
Account,
we
presented
summary
our
attempts
optimize
performance
materials
via
modulation.
In
view
component
advantages
MOFs,
deliver
general
fundamentals
rational
Initially,
opportunities
brought
about
by
engineering,
including
origin
abundant
active
flexible
strategies,
structure,
introduced
detail.
next
section,
focus
on
specific
strategies
dominate
molecular/electron-transfer
process
intrinsic
activity
Meanwhile,
chemical
basis
underlying
structure–property
relationship
behind
enhanced
will
be
highlighted.
Finally,
major
challenges
outlooks
further
discussed.
It
expected
that
Account
would
afford
significant
inspiration
toward
engineering
