Journal of the American Chemical Society,
Journal Year:
2021,
Volume and Issue:
143(39), P. 16284 - 16292
Published: Sept. 21, 2021
Achieving
more
than
a
two-electron
photochemical
CO2
reduction
process
using
metal-free
system
is
quite
exciting
and
challenging,
as
it
needs
proper
channeling
of
electrons.
In
the
present
study,
we
report
rational
design
synthesis
redox-active
conjugated
microporous
polymer
(CMP),
TPA-PQ,
by
assimilating
an
electron
donor,
tris(4-ethynylphenyl)amine
(TPA),
with
acceptor,
phenanthraquinone
(PQ).
The
TPA-PQ
shows
intramolecular
charge-transfer
(ICT)-assisted
catalytic
activity
for
visible-light-driven
photoreduction
to
CH4
(yield
=
32.2
mmol
g–1)
impressive
rate
(2.15
h–1
high
selectivity
(>97%).
Mechanistic
analysis
based
on
experimental
results,
in
situ
DRIFTS,
computational
studies
reveals
that
potential
catalyzing
was
energetically
driven
photoactivated
ICT
upon
surface
adsorption
CO2,
wherein
adjacent
keto
groups
PQ
unit
play
pivotal
role.
critical
role
stimulating
photocatalysis
further
illustrated
synthesizing
another
CMP
(TEB-PQ),
bearing
triethynylbenzene
(TEB)
PQ,
8-fold
lesser
toward
4.4
compared
TPA-PQ.
results
demonstrate
novel
concept
efficient,
sustainable,
recyclable
robust
organic
photocatalyst.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(34)
Published: March 15, 2023
Single-atom
catalysts
hold
the
potential
to
significantly
impact
chemical
sector,
pushing
boundaries
of
catalysis
in
new,
uncharted
directions.
These
materials,
featuring
isolated
metal
species
ligated
on
solid
supports,
can
exist
many
coordination
environments,
all
which
have
shown
important
functions
specific
transformations.
Their
emergence
has
also
provided
exciting
opportunities
for
mimicking
metalloenzymes
and
bridging
gap
between
homogeneous
heterogeneous
catalysis.
This
Review
outlines
impressive
progress
made
recent
years
regarding
use
single-atom
organic
synthesis.
We
illustrate
knowledge
gaps
search
more
sustainable,
earth-abundant
synthetic
applications.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(21), P. 7602 - 7664
Published: Jan. 1, 2023
Carbon
nitrides,
with
feasibility
of
tailored
band
gap
via
suitable
nanoarchitectonics,
are
deemed
as
best
catalysts
amongst
existing
materials,
especially
for
HER,
OWS,
COR,
NRR,
water
oxidation,
pollutant
removal,
and
organocatalysis.
Deleted Journal,
Journal Year:
2022,
Volume and Issue:
1, P. e9120006 - e9120006
Published: May 12, 2022
Organic
synthesis
driven
by
heterogeneous
catalysis
is
a
central
research
theme
to
both
fundamental
and
industrial
production
of
fine
chemicals.
However,
the
employment
stoichiometric
strong
oxidizing
or
reducing
reagents
(e.g.,
K2Cr2O7
LiAlH4)
harsh
reaction
conditions
high
temperature
pressure)
always
leads
products
overreaction
other
by-product
residues
salt
acid
waste).
Thus
poor
control
product
selectivity
tremendous
energy
consumption
result
in
urgent
demand
develop
novel
technologies
for
catalysis.
Given
current
global
development
CO2
reduction
sustainable
utilization,
one
promising
protocol
photocatalysis.
It
enables
solar-to-chemical
conversion
under
mild
room
temperature,
ambient
pressure,
air
as
oxidant)
offers
unique
pathways
improved
control.
To
accurately
tailor
desired
products,
electronic
structure
positions
valence-band
maximum
conduction-band
minimum),
geometric
nanorod,
nanosheet,
porous
morphology),
surface
chemical
micro-environment
vacancy
sites
co-catalysts)
photocatalysts
require
rational
design
construction.
In
this
review,
we
will
briefly
analyze
some
effective
photocatalytic
systems
with
excellent
regulation
ability
organic
transformations
(mainly
oxidation
types)
visible
light
irradiation,
put
forward
opinions
on
optimal
fabrication
nanostructured
realize
selective
synthesis.
ACS Catalysis,
Journal Year:
2022,
Volume and Issue:
12(9), P. 5605 - 5660
Published: April 26, 2022
As
a
group
of
large-surface-area
nonmetal
materials,
polymeric
carbon
nitride
(CxNy)
and
its
hybrid
structures
are
nowadays
ever-increasing
interest
for
use
in
energy
devices
involved
conversion
storage,
offering
low
expenses
facile
production
processes.
With
the
growing
requirement
clean
renewable
generation
storage
systems,
progress
replacement
expensive
noble-metal
catalysts
with
CxNy-based
materials
as
efficient
electrocatalysts
has
expanded
considerably,
demand
these
increased.
The
modified
CxNy
architectures
beneficial
to
electrocatalytic
applications,
improving
their
moderate
electrical
conductivities
capacity
loss.
present
review
strives
highlight
recent
advances
research
on
aforementioned
identities
CxNy-derived
structurally
polymorphs.
This
also
discusses
fuel
cells,
metal–air
batteries,
water
splitting
supercapacitor
applications.
Herein,
we
deal
oxidation
reduction
reactions
such
hydrogen
evolution,
oxygen
reduction,
CO2
nitrogen
etc.
Each
device
been
studied
clearer
understanding
patent
relevant
experiments
reviewed
separately.
Additionally,
role
some
general
redox
capable
being
exploited
any
is
included.
ACS Catalysis,
Journal Year:
2021,
Volume and Issue:
11(17), P. 11109 - 11116
Published: Aug. 20, 2021
Organic
π-conjugated
polymers
are
promising
heterogeneous
photocatalysts
that
involve
photoredox
or
energy
transfer
processes.
In
such
settings,
the
materials
usually
applied
in
form
of
dispersion
liquid
medium,
which
is
bound
to
certain
technological
limits
applicability.
Herein,
we
present
an
innovative
approach
using
carbon
nitride
thin
films
prepared
via
chemical
vapor
deposition
at
different
vessel
walls
and
them
as
batch
microfluidic
photoreactors.
This
allows
us
not
only
fabricate
technologically
relevant
reusable
devices
but
also
improve
photophysical
properties
nitride,
singlet–triplet
gap
lifetime
triplet
excited
states,
when
material
assembled
films.
These
morphological
changes
employed
maximize
performance
photocatalytic
reactions,
show
least
1
order
magnitude
higher
activity
per
area
unit
compared
photocatalysis
suspended
particles.
ACS Nano,
Journal Year:
2021,
Volume and Issue:
15(10), P. 16106 - 16117
Published: Sept. 20, 2021
In
this
work,
we
discover
a
piezoelectrocatalytic
system
composed
of
ferroelectric
heterostructure
BaTiO3
(BTO)@MoSe2
nanosheets,
which
exhibit
piezoelectric
potential
(piezopotential)
coupling
with
electrocatalyzed
effects
by
strain-induced
piezopotential
to
provide
an
internal
bias
the
catalysts'
surface;
subsequently,
catalytic
properties
are
substantially
altered
enable
formation
activity
states.
The
H2
production
rate
BTO@MoSe2
for
generation
is
4533
μmol
h–1
g–1,
206%
that
TiO2@MoSe2
piezophototronic
(referred
as
piezophotocatalytic
process)
(∼2195.6
g–1).
presents
long-term
21.2
mmol
g–1
within
8
h,
highest
recorded
value
under
piezocatalytic
conditions.
theoretical
and
experimental
results
indicate
BTO
acts
electric
field
generator
while
few-layered
MoSe2
facilitating
redox
reactions
on
its
active
sites.
This
promising
method
environmental
remediation
clean
energy
development.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(43)
Published: Sept. 8, 2022
Carbon
nitride
(CN)
is
a
heterogeneous
photocatalyst
that
combines
good
structural
properties
and
broad
scope.
The
photocatalytic
efficiency
of
CN
associated
with
the
presence
defective
radical
species.
An
accurate
description
states-both
at
local
extended
level-is
key
to
develop
thorough
mechanistic
understanding
photophysics
CN.
In
turn,
this
will
maximise
generation
usage
photogenerated
charge
carriers
minimise
wasteful
recombination.
Here
influence
morphology
light-excitation
on
number
chemical
nature
defects
assessed.
By
exploiting
magnetic
dipole-dipole
coupling,
spatial
distribution
native
radicals
in
derived
high
precision.
From
analysis
an
average
distance
range
1.99-2.34
nm
determined,
which
corresponds
pairs
located
approximately
four
tri-s-triazine
units
apart.
