The
proton-coupled
electron
transfer
(PCET)
process
has
garnered
significant
attention
in
photocatalysis
due
to
its
ability
facilitate
challenging
transformations
under
mild
conditions.
By
integrating
PCET
into
heterogeneous
photocatalysts,
substrates
can
be
precisely
activated
through
the
concurrent
of
both
electrons
and
protons
between
catalyst
reaction
medium.
Herein,
we
synthesized
a
novel
type
carbon-nitride-based
photocatalyst,
which
effectively
drive
via
mechanism,
enabling
three-component
synthesis
unsymmetrical
imidazolidines
with
ease.
Chinese Journal of Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 7, 2025
Comprehensive
Summary
The
development
of
sustainable
and
efficient
catalytic
systems
for
the
formation
C—C,
C—N,
C—O
bonds
is
a
fundamental
goal
in
modern
synthetic
chemistry.
We
present
biomass‐derived
Cu/Chitosan‐800
catalyst
that
facilitates
range
carbenoid
insertion
reactions
into
C—H,
N—H,
O—H
bonds.
This
demonstrates
remarkable
activity,
enabling
functionalization
diverse
substrates,
including
late‐stage
modification
drug
molecules
with
up
to
95%
yield
good
recyclability.
Our
findings
highlight
catalyst's
potential
advancing
environmentally
friendly
chemical
transformations,
offering
promising
tool
pharmaceutical
synthesis
organic
synthesis.
ACS Catalysis,
Год журнала:
2025,
Номер
unknown, С. 5601 - 5613
Опубликована: Март 21, 2025
Understanding
charge
transfer
in
light-driven
processes
is
crucial
for
optimizing
the
efficiency
and
performance
of
a
photocatalyst,
as
directly
influences
separation
migration
photogenerated
carriers
determines
overall
reaction
rate
product
formation.
However,
achieving
this
understanding
remains
challenging
context
single-atom
photocatalysis.
This
study
addresses
gap
investigates
an
Ag-based
catalyst
(Ag1@CNx)
photocatalytic
oxidation
benzyl
alcohol
to
benzaldehyde.
Comprehensive
characterization
was
conducted
using
battery
diffractive,
textural,
spectroscopic,
microscopic
methods,
confirming
crystallinity,
porosity,
elemental
composition,
atomic
dispersion
silver
atoms.
material
displayed
efficient
selective
Density
functional
theory
calculations
were
used
rationalize
structure
elucidate
mechanism,
unveiling
role
holes
lowering
energy
barriers.
Time-resolved
transient
spectroscopic
studies
monitor
dynamics
charges
reaction,
revealing
lifetimes
behaviors
excited
states
within
catalyst.
Specifically,
introduction
atoms
led
significant
enhancement
state
lifetime,
which
favors
hole-transfer
presence
alcohol.
indicated
that
photoexcited
effectively
transferred
reactant,
thereby
driving
process
oxygen.
These
mechanistic
insights
are
pivotal
spectroscopically
elucidating
mechanism
can
be
practically
applied
design
photocatalysts
more
rationally,
targeting
materials
combine
both
rapid
reductive
quenching
metal.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 25, 2025
A
novel
Mn-based
single-atom
photocatalyst
is
disclosed
in
this
study,
designed
for
the
dichlorination
of
alkenes
to
achieve
vicinal
dichlorinated
products
using
N-chlorosuccinimide
as
a
mild
chlorinating
agent,
which
have
widespread
applications
pest
controlling
agents,
polymers,
flame
retardants,
and
pharmaceuticals.
In
developing
innovative
catalyst,
we
achieved
atomic
dispersion
Mn
on
aryl-amino-substituted
graphitic
carbon
nitride
(f-C3N4).
This
marks
first
instance
heterogeneous
version,
offering
an
operationally
simple,
sustainable,
efficient
pathway
alkenes,
including
drugs,
bioactive
compounds,
natural
products.
material
was
extensively
characterized
by
techniques
such
UV-vis
spectroscopy,
X-ray
absorption
near-edge
structure
(XANES),
extended
fine
(EXAFS),
high-resolution
transmission
electron
microscopy
(HR-TEM),
photoelectron
spectroscopy
(XPS),
magic-angle
spinning
(MAS),
solid-state
nuclear
magnetic
resonance
(ssNMR)
understand
it
at
level.
Furthermore,
mechanistic
studies
based
multiscale
molecular
modeling,
combining
classical
reactive
dynamics
(RMD)
simulations
quantum
chemistry
(QC)
calculations,
illustrated
that
controlled
formation
Cl
radicals
from
situ
formed
Mn-Cl
bond
responsible
reaction
alkenes.
addition,
gram-scale
reusability
tests
were
also
performed
demonstrate
applicability
approach
industrial
scale.
The
proton-coupled
electron
transfer
(PCET)
process
has
garnered
significant
attention
in
photocatalysis
due
to
its
ability
facilitate
challenging
transformations
under
mild
conditions.
By
integrating
PCET
into
heterogeneous
photocatalysts,
substrates
can
be
precisely
activated
through
the
concurrent
of
both
electrons
and
protons
between
catalyst
reaction
medium.
Herein,
we
synthesized
a
novel
type
carbon-nitride-based
photocatalyst,
which
effectively
drive
via
mechanism,
enabling
three-component
synthesis
unsymmetrical
imidazolidines
with
ease.
