Chemical Science,
Год журнала:
2024,
Номер
unknown
Опубликована: Янв. 1, 2024
The
utilization
of
earth-abundant
photosensitizers
with
visible
light
absorption
to
enable
sustainable
photocatalysis
is
a
long-standing
challenge.
Overcoming
such
challenge,
in
this
work,
two
lanthanide
(Ln
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(19), С. 10451 - 10457
Опубликована: Апрель 6, 2023
Molecule-based
heterogeneous
photocatalysts
without
noble
metals
are
one
of
the
most
attractive
systems
for
visible-light-driven
CO2
reduction.
However,
reports
on
this
class
still
limited,
and
their
activities
quite
low
compared
to
those
containing
metals.
Herein,
we
report
an
iron-complex-based
photocatalyst
reduction
with
high
activity.
The
key
our
success
is
use
a
supramolecular
framework
composed
iron
porphyrin
complexes
bearing
pyrene
moieties
at
meso
positions.
catalyst
exhibited
activity
under
visible-light
irradiation
(29100
μmol
g-1
h-1
CO
production,
selectivity
99.9%),
which
highest
among
relevant
systems.
performance
also
excellent
in
terms
apparent
quantum
yield
production
(0.298%
400
nm)
stability
(up
96
h).
This
study
provides
facile
strategy
create
highly
active,
selective,
stable
utilizing
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(39)
Опубликована: Июль 29, 2024
Abstract
Electrocatalytic
CO
2
reduction
(ECR)
powered
by
renewable
electricity
is
a
promising
technology
to
mitigate
carbon
emissions
and
lessen
the
dependence
on
fossil
fuels
toward
carbon‐neutral
energy
cycle.
Metal–organic
frameworks
(MOFs)
their
derivatives,
due
excellent
intrinsic
activity,
have
emerged
as
materials
for
ECR
high‐demand
products.
However,
challenges
such
unsatisfactory
efficiency,
selectivity,
relatively
low
production
rates
hinder
industrial
scalability.
Here,
comprehensive
critical
review
presented
that
summarizes
state‐of‐the‐art
progress
in
MOF‐based
MOF‐derived
electroreduction
catalysts
from
design
functionality
perspectives.
The
fundamentals
of
reaction
(CO
RR)
over
heterogeneous
catalysts,
mechanisms,
key
faced
are
described
first
establish
solid
foundation
forthcoming
in‐depth
analyses.
MOF's
building
blocks,
properties,
shortcomings
pertinent
including
conductivity
stability,
systematically
discussed.
Moreover,
discussions
provided
design,
fabrication,
characterization,
RR
activity
pinpoint
intricate
structure‐property‐performance
relationship.
Finally,
recommendations
put
forward
enhancing
MOF
electrocatalysts
durability.
This
work
may
serve
guideline
developing
high‐performance
MOF‐related
RR,
benefiting
researchers
working
this
growing
potentially
game‐changing
area.
Chemical Communications,
Год журнала:
2023,
Номер
59(12), С. 1569 - 1588
Опубликована: Янв. 1, 2023
Metal-organic
frameworks
(MOFs,
also
known
as
porous
coordination
polymers
or
PCPs)
are
a
novel
class
of
crystalline
material.
The
tailorable
structure,
in
terms
size,
geometry
and
function,
has
attracted
the
attention
researchers
across
all
disciplines
materials
science.
One
many
exciting
aspects
MOFs
is
that
through
directional
reversible
bonding,
organic
linkers
(chromophores
with
metal-coordinating
functional
groups)
metal
ions
(and
clusters)
can
be
spatially
organized
preconceived
geometry.
well-defined
spatial
metals
very
advantageous
for
optoelectronic
functions
(solar
cells,
light-emitting
diodes,
photocatalysts)
materials.
This
feature
article
evaluates
scope
charge
transfer
(CT)
interactions
MOFs,
involving
ion
cluster
components.
Irrespective
type
(size,
shape,
electronic
property)
chromophores
involved,
provide
an
insightful
path
to
design
make
CT
process
efficient.
selected
examples
characteristics
do
not
only
illustrate
principles
but
render
pathway
towards
understanding
complex
photophysical
processes
implementing
those
future
catalytic
applications.
Green Chemistry,
Год журнала:
2023,
Номер
26(3), С. 1041 - 1061
Опубликована: Дек. 7, 2023
For
more
than
one
century,
the
synthesis
of
ammonia
(NH
3
)
through
Haber–Bosch
route
has
allowed
industrial-scale
production
fertilizers
and
other
nitrogen-containing
compounds.
ACS Catalysis,
Год журнала:
2023,
Номер
13(18), С. 12391 - 12402
Опубликована: Сен. 6, 2023
Artificial
photosynthesis
is
a
viable
approach
for
transforming
carbon
dioxide
(CO2)
into
value-added
chemicals
driven
by
renewable
solar
energy.
Studies
on
photocatalytic
CO2
reduction
(CO2R)
have
thus
been
expedited
in
recent
years.
Cadmium
sulfide
quantum
dots
(CdS
QDs)
regarded
as
one
of
the
most
promising
photocatalysts,
offering
myriad
advantages
CO2R,
such
narrow
band
gap,
confinement
effect,
and
tunable
redox
potential.
However,
CdS
QDs
usually
suffer
from
photo,
thermal,
oxidative
instability.
In
this
work,
we
demonstrate
an
effective
method
to
endow
assembling
them
with
amphiphilic
metallopolymers
enhance
their
stability
synergistically
increase
catalytic
activity.
The
were
synthesized
via
precise
radical
polymerization
between
1-ethyl-3-vinylimidazolium
bromide
rhenium(I)-N-(3-((4′-methoxy-[2,2′-bipyridin]-4-yl)oxy)propyl)acrylamide
compounds.
resultant
positively
charged
rhenium
complex-containing
metallopolymer
(P(Re-IL))
underwent
spontaneous
assembly
negatively
thioglycolate-capped
electrostatic
interaction,
forming
highly
active
stable
CdS/P(Re-IL)
hybrids.
ultimate
interfacial
interaction
two
components
facilitated
photoinduced
electron
transfer
(PET)
vicinal
bipyridyl
ReI(CO)3Cl
derivatives,
promoting
CO
high
production
rate
selectivity
25
mL-DMF/water
(4:1
v/v)
solution
under
LED
370
nm
irradiation.
For
example,
CdS/P(5%
Re-IL)
was
optimum
catalyst
our
system,
showing
highest
38.3
mmol
g–1
h–1
93.8%
within
2
h
no
induction
period,
which
ranked
among
top
state-of-the-art
CO2R
photocatalysts
mixed
organic-water
media.