Angewandte Chemie,
Journal Year:
2023,
Volume and Issue:
135(41)
Published: Aug. 26, 2023
Abstract
Solar‐driven
CO
2
reduction
integrated
with
C−C/C−X
bond‐forming
organic
synthesis
represents
a
substantially
untapped
opportunity
to
simultaneously
tackle
carbon
neutrality
and
create
an
atom‐/redox‐economical
chemical
synthesis.
Herein,
we
demonstrate
the
first
cooperative
photoredox
catalysis
of
efficient
tunable
syngas,
paired
direct
alkylation/arylation
unactivated
allylic
sp
3
C−H
bonds
for
accessing
C−C
products,
over
SiO
‐supported
single
Ni
atoms‐decorated
CdS
quantum
dots
(QDs).
Our
protocol
not
only
bypasses
additional
oxidant/reductant
pre‐functionalization
substrates,
affording
broad
products
moderate
excellent
yields,
but
also
produces
syngas
CO/H
ratios
(1
:
2–5
1).
Such
win‐win
coupling
highlights
high
atom‐,
step‐
redox‐economy,
good
durability,
illuminating
tantalizing
possibility
renewable
sunlight‐driven
feedstocks
manufacturing
industry.
ACS Catalysis,
Journal Year:
2023,
Volume and Issue:
13(6), P. 3971 - 3982
Published: March 8, 2023
The
sun
offers
a
clean
and
renewable
energy
cornucopia,
whereas
how
to
utilize
this
inexhaustible
yet
decentralized
with
the
assistance
of
appropriate
media
is
an
enduring
topic.
Plasmonic
metal-based
nanostructures
(mainly
Au
Ag)
represent
class
fascinating
materials
for
solar
conversion
due
their
exclusive
surface
plasmon
resonance
(SPR)-enabled
light-harvesting
capability.
In
contrast
these
plasmonic
metals
characteristic
SPR
peaks,
modulating
optical
absorption
peaks
nonplasmonic
(e.g.,
small
Pt
nanoparticles)
in
visible
region
but
without
size
alteration
grand
challenge.
Until
recently,
we
demonstrated
near
field
scattering
(NFS)
model
manipulate
nanoparticles
by
adjusting
dielectric
environment,
sowing
seeds
tuning
property
other
metal
even
semiconductor
quantum
dots.
It
purpose
present
Perspective
retrospect
history
NFS
guide
function-oriented
design
NFS-based
artificial
photoredox
transformation.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(41)
Published: Aug. 26, 2023
Solar-driven
CO2
reduction
integrated
with
C-C/C-X
bond-forming
organic
synthesis
represents
a
substantially
untapped
opportunity
to
simultaneously
tackle
carbon
neutrality
and
create
an
atom-/redox-economical
chemical
synthesis.
Herein,
we
demonstrate
the
first
cooperative
photoredox
catalysis
of
efficient
tunable
syngas,
paired
direct
alkylation/arylation
unactivated
allylic
sp3
C-H
bonds
for
accessing
C-C
products,
over
SiO2
-supported
single
Ni
atoms-decorated
CdS
quantum
dots
(QDs).
Our
protocol
not
only
bypasses
additional
oxidant/reductant
pre-functionalization
substrates,
affording
broad
products
moderate
excellent
yields,
but
also
produces
syngas
CO/H2
ratios
(1
:
2-5
1).
Such
win-win
coupling
highlights
high
atom-,
step-
redox-economy,
good
durability,
illuminating
tantalizing
possibility
renewable
sunlight-driven
feedstocks
manufacturing
industry.
ACS Catalysis,
Journal Year:
2023,
Volume and Issue:
13(20), P. 13167 - 13180
Published: Sept. 28, 2023
Covalent–organic
frameworks
(COFs),
as
promising
metal-free
porous
catalysts,
have
become
a
hot
research
topic
in
the
field
of
(photo)catalysis.
Herein,
series
β-ketoenamine
COFs
are
synthesized
using
different
amino
and
aldehyde
monomers,
these
exhibit
diverse
characteristics
terms
crystallinity,
chemical
structure,
microscopic
morphology,
optoelectronic
properties.
TpBD-(CH3)2
from
2,4,6-triformylphloroglucinol
o-tolidine
exhibits
an
extended
π-conjugated
structure
higher
crystallinity
well
more
suitable
redox
potential,
which
greatly
enhances
photocatalytic
activity
benzylamine
oxidation.
Besides,
increased
number
hydroxyl
groups
on
trialdehyde-based
monomer
contributes
to
ketoamines
TpTAB
skeleton,
is
favorable
for
photocatalysis.
Meanwhile,
can
rapidly
increase
their
own
temperature
through
internal
structural
evolution
under
light
irradiation,
thus
boosting
oxidative
coupling
amines
with
high
efficiency.
This
work
could
provide
some
guidance
rational
design
functional
advanced
organic
transformations.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(22)
Published: March 29, 2023
Photocatalytic
epoxide
alcoholysis
through
C-O
bond
cleavage
and
formation
has
emerged
as
an
alternative
to
synthesizing
anti-tumoral
pharmaceuticals
fine
chemicals.
However,
the
lack
of
crucial
evidence
interpret
interaction
between
reactants
photocatalyst
surface
makes
it
challenging
for
photocatalytic
with
both
high
activity
regioselectivity.
In
this
work,
we
report
hierarchical
ZnIn2
S4
@CdS
regioselectivity
nearly
100
%.
Mechanistic
studies
unveil
that
precise
activation
switch
on
exposed
Zn
acid
sites
polarization
a
critical
significance
achieving
efficient
performance.
Furthermore,
establishment
Z-scheme
heterojunction
facilitates
interface
charge
separation
transfer.
Remarkably,
underlying
regioselective
reaction
pathway
been
distinctly
revealed.
