ACS Catalysis,
Journal Year:
2022,
Volume and Issue:
12(3), P. 1919 - 1929
Published: Jan. 20, 2022
Solar-driven
catalytic
oxidation
of
5-hydroxymethylfurfural
(HMF)
into
2,5-diformylfuran
(DFF)
coupled
with
H2
evolution
has
been
considered
a
promising
approach.
The
exploration
an
active
and
stable
photocatalyst
still
remains
challenging
work.
Herein,
we
found
that
the
flexible
ultrathin
graphitic
carbon
nitride
(UCNT)
could
be
ideal
candidate.
UCNT
exhibits
photocatalytic
performance
in
selective
HMF
DFF
activities
95.0
92.0
μmol
g–1
h–1
under
visible
light
irradiation.
Importantly,
also
demonstrates
high
selectivity
(95%)
good
cycling
stability.
activity
may
ascribed
to
strong
specific
interaction
between
UCNT.
Solid-state
nuclear
magnetic
resonance
(NMR)
density
functional
theory
(DFT)
results
reveal
twisted
structure
molecules
form
UCNT,
reducing
dehydrogenation
energy
barrier
for
oxidation.
In
addition,
mechanistic
studies
•C6H4O3
is
key
radical
intermediate
during
process
by
situ
electron
spin
(ESR)
trapping
test.
Our
work
clarifies
complex
biomass
on
catalyst
surface
provides
views
further
development
heterogeneous
conversion.
ACS Catalysis,
Journal Year:
2020,
Volume and Issue:
10(17), P. 10253 - 10315
Published: Aug. 27, 2020
The
use
of
solar
energy
to
catalyze
the
photo-driven
processes
has
attracted
tremendous
attention
from
scientific
community
because
its
great
potential
address
and
environmental
issues.
In
this
regard,
several
attempts
have
been
made
by
researchers
design
develop
different
materials
with
enhanced
photocatalytic
efficiencies.
This
Review
comprehensively
summarizes
recent
reports
on
perovskite
oxide
based
photocatalysts
for
organic
pollutant
degradation,
water
splitting,
carbon
dioxide
conversion,
nitrogen
fixation
along
basic
understanding
involved
mechanisms,
current
trends
advances
in
field.
design,
synthesis,
development
strategies
discussed
detail
provide
a
comprehensive
view
materials'
fabrication
that
influences
their
properties.
Subsequently,
insights
materials,
including
simple
oxides,
mixed
layered
are
provided
above-mentioned
applications
detailed
manner.
Finally,
summary
perspective
future
research
direction
discussed.
Based
progress
field,
it
is
highly
anticipated
systems,
comprising
groundbreaking
technologies
large-scale
realization
these
processes,
can
be
established
near
environment-oriented
challenges.
Nature Communications,
Journal Year:
2021,
Volume and Issue:
12(1)
Published: Jan. 20, 2021
Abstract
Artificial
photosynthesis
of
H
2
O
from
and
,
as
a
spotless
method,
has
aroused
widespread
interest.
Up
to
date,
most
photocatalysts
still
suffer
serious
salt-deactivated
effects
with
huge
consumption
photogenerated
charges,
which
severely
limit
their
wide
application.
Herein,
by
using
phenolic
condensation
approach,
carbon
dots,
organic
dye
molecule
procyanidins
4-methoxybenzaldehyde
are
composed
into
metal-free
photocatalyst
for
the
photosynthetic
production
in
seawater.
This
catalyst
exhibits
high
photocatalytic
ability
produce
yield
1776
μmol
g
−1
h
(
λ
≥
420
nm;
34.8
mW
cm
−2
)
real
seawater,
about
4.8
times
higher
than
pure
polymer.
Combining
in-situ
photoelectrochemical
transient
photovoltage
analysis,
active
site
catalytic
mechanism
this
composite
seawater
also
clearly
clarified.
work
opens
up
an
avenue
highly
efficient
practical,
available
photoproduction
ACS Catalysis,
Journal Year:
2021,
Volume and Issue:
11(14), P. 8510 - 8520
Published: June 29, 2021
One
of
the
research
hotspots
in
solar
energy
conversion
is
developing
photocatalysts
for
visible-light-driven
H2
production.
In
this
study,
a
ternary
CdS@Au/MXene
composite
was
elaborately
constructed
by
facile
situ
self-assembly
strategy,
where
ultrathin
Ti3–xC2Ty
nanosheets
with
characteristic
Ti
vacancies
were
employed
as
support
core–shell
structured
CdS@Au
nanojunctions.
presence
1.0
wt
%
MXene,
merely
0.1
Au
helped
composites
achieve
high
H2-production
rate
5371
μmol·g–1·h–1
under
visible-light
irradiation,
more
than
26.6
times
higher
that
bare
CdS.
Such
an
enhancement
predominantly
attributed
to
"dual
Schottky
barriers"
formed
at
interface
CdS@Au/MXene,
which
evidenced
systematic
characterizations
including
X-ray
photoelectron
spectroscopy
and
Kelvin
probe
measurements,
conjunction
density
functional
theory
(DFT)
calculations.
This
work
not
only
highlights
significant
role
MXene
reducing
dosage
noble
metal
cocatalysts
photocatalysis,
but
also
opens
avenues
fabricate
MXene-based
beyond.
Advanced Functional Materials,
Journal Year:
2021,
Volume and Issue:
31(28)
Published: April 25, 2021
Abstract
It
is
a
well‐known
fact
that
the
pronounced
photogenerated
charge
recombination
and
poor
light
absorption
are
main
bottlenecks
of
photocatalysis
applications.
The
conventional
approaches
to
address
these
problems
involve
bandgap
engineering
suppression
after
irradiation,
which
results
in
an
enhancement
photocatalytic
performance
materials.
However,
most
essential
aspect
surface
modification
engineer
active
sites
on
catalyst
generally
not
given
much
importance.
Contrary
this,
defect
another
approach
by
optical,
separation,
properties
materials
can
be
tuned.
In
this
review
article,
effect
introduction
vacancies
selected
semiconductor
materials,
viz.,
metal
oxides,
perovskite
sulfides,
oxyhalides,
nitrides
comprehensively
summarized.
only
improves
their
optical
transfer
but
also
affects
properties,
helpful
adsorption
reactants
surface.
Herein,
hydrogen
evolution
nitrogen
fixation
applications
vacancy
engineered
discussed
detail
along
with
current
trends,
scalability
requirements,
rigorous
experimental
protocols.
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.
ACS Catalysis,
Journal Year:
2020,
Volume and Issue:
11(2), P. 650 - 658
Published: Dec. 30, 2020
Designation
and
optimization
of
facets
photocatalysts
is
an
effective
strategy
to
address
the
issue
facet-dependent
photocatalytic
reactions.
However,
studies
regarding
facet
effect
metal–organic
frameworks
(MOFs)
on
process
are
in
infancy.
In
this
study,
NH2-MIL-125(Ti)
with
different
ratios
{001}
{111}
was
exactly
controlled
synthesized,
it
found
that
activity
photoreduction
CO2
enhanced
gradually
increasing
exposed
proportion
facets.
The
exhibit
maximal
CO
CH4
yields
8.25
1.01
μmol
g–1
h–1,
which
9
5
times
higher
than
those
facets,
respectively.
Also,
give
highest
quantum
0.14
0.07%
for
production,
Steady-state
time-resolved
fluorescence
spectra
reveal
importance
inhibiting
recombination
photoinduced
electrons
holes
sample
Besides,
TiIII
formed
during
reaction
exhibits
strong
reducibility
CO2.
Starting
from
NH2-MIL-125(Ti),
performance
can
be
by
regulating
This
work
not
only
provides
a
further
enhancing
tuning
active
MOFs,
but
also
deep
understanding
factors
improving
reduction
ACS Catalysis,
Journal Year:
2021,
Volume and Issue:
11(21), P. 13266 - 13279
Published: Oct. 18, 2021
It
is
of
great
importance
to
explore
and
achieve
a
more
effective
approach
toward
the
controllable
synthesis
single-atom-based
photocatalysts
with
high
metal
content
long-term
durability.
Herein,
single-atom
platinum
(Pt)
loading
anchored
on
pore
walls
two-dimensional
β-ketoenamine-linked
covalent
organic
frameworks
(TpPa-1-COF)
presented.
Aided
by
advanced
characterization
techniques
aberration-corrected
high-angle
annular
dark-field
scanning
transmission
electron
microscopy
(AC
HAADF-STEM)
X-ray
absorption
fine
structure
(XAFS)
spectroscopy,
it
has
been
demonstrated
that
atomically
dispersed
Pt
formed
TpPa-1-COF
support
through
six-coordinated
C3N–Pt–Cl2
species.
The
optimized
Pt1@TpPa-1
catalyst
exhibits
photocatalytic
H2
evolution
rate
719
μmol
g–1
h–1
under
visible-light
irradiation,
actual
0.72
wt
%,
large
turnover
frequency
(TOF)
19.5
h–1,
activity
equivalent
3.9
48
times
higher
than
those
nanoparticles/TpPa-1
bare
TpPa-1,
respectively.
improved
performance
for
ascribed
photogenerated
charge
separation
migration
well-dispersed
active
sites
Pt.
Moreover,
density
functional
theory
(DFT)
calculations
further
reveal
role
single
atoms
in
enhanced
evolution.
Overall,
this
work
provides
some
inspiration
designing
outstanding
stability
efficiency
using
COFs
as
support.