Journal of the American Chemical Society,
Год журнала:
2025,
Номер
147(9), С. 7993 - 8003
Опубликована: Фев. 19, 2025
The
structure-dependent
transition
in
reaction
pathways
during
acidic
oxygen
evolution
(OER)
is
pivotal
due
to
the
active
site
oxidation
accompanied
by
coordination
environment
changes.
In
this
work,
charge-polarized
Ir-O-Co
units
are
constructed
alkali
metal
cobalt
oxides
(LiCoO2,
and
Na0.74CoO2)
modify
lower
Hubbard
band.
Benefiting
from
accelerated
delithiation
reconstruction
induced
altered
band
structure,
typical
Ir-LiCoO2
produces
high-valent
Ir
sites
with
unsaturated
through
charge
compensation
OER.
Oxygen
atoms
shared
trimetallic
exhibit
strong
Bro̷nsted
acidity,
promoting
proton
migration
for
dynamically
enhancing
deprotonation.
Furthermore,
stable
environment,
along
electron
donation
Co
sites,
significantly
improves
stability
of
sites.
unique
electrochemical
activation
results
a
low
overpotential
190
mV
at
10
mA
cm-2
OER
delivers
exceptional
1
A
150
h
slight
voltage
degradation
exchange
membrane
electrolyzer.
This
work
provides
in-depth
insights
into
relationship
between
catalyst
mechanisms.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(31)
Опубликована: Июнь 7, 2023
H2
O2
photosynthesis
coupled
with
biomass
valorization
can
not
only
maximize
the
energy
utilization
but
also
realize
production
of
value-added
products.
Here,
a
series
COFs
(i.e.
Cu3
-BT-COF,
-pT-COF
and
TFP-BT-COF)
regulated
redox
molecular
junctions
have
been
prepared
to
study
furfuryl
alcohol
(FFA)
photo-oxidation
furoic
acid
(FA).
The
FA
generation
efficiency
-BT-COF
was
found
be
575
mM
g-1
(conversion
≈100
%
selectivity
>99
%)
rate
reach
up
187
000
μM
,
which
is
much
higher
than
-pT-COF,
TFP-BT-COF
its
monomers.
As
shown
by
theoretical
calculations,
covalent
coupling
Cu
cluster
thiazole
group
promote
charge
transfer,
substrate
activation
FFA
dehydrogenation,
thus
boosting
both
kinetics
increase
efficiency.
This
first
report
about
for
valorization,
might
facilitate
exploration
porous-crystalline
catalysts
in
this
field.
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(11), С. 5626 - 5676
Опубликована: Янв. 1, 2024
Metalation
of
metal-organic
frameworks
(MOFs)
has
been
developed
as
a
prominent
strategy
for
materials
functionalization
pore
chemistry
modulation
and
property
optimization.
By
introducing
exotic
metal
ions/complexes/nanoparticles
onto/into
the
parent
framework,
many
metallized
MOFs
have
exhibited
significantly
improved
performance
in
wide
range
applications.
In
this
review,
we
focus
on
research
progress
metalation
during
last
five
years,
spanning
design
principles,
synthetic
strategies,
potential
Based
crystal
engineering
minor
change
MOF
composition
through
would
lead
to
leveraged
variation
properties.
This
review
starts
from
general
strategies
established
incorporation
species
within
MOFs,
followed
by
principles
graft
desired
functionality
while
maintaining
porosity
frameworks.
Facile
contributed
great
number
bespoke
with
excellent
performance,
summarize
their
applications
gas
adsorption
separation,
heterogeneous
catalysis,
detection
sensing,
energy
storage
conversion.
The
underlying
mechanisms
are
also
investigated
state-of-the-art
techniques
analyzed
gaining
insight
into
structure-property
relationships,
which
turn
facilitate
further
development
principles.
Finally,
current
challenges
opportunities
discussed,
promising
future
directions
customizing
next-generation
advanced
outlined
well.
Biosensors,
Год журнала:
2023,
Номер
13(5), С. 542 - 542
Опубликована: Май 12, 2023
Wide-ranging
research
efforts
have
been
directed
to
prioritize
scientific
and
technological
inventions
for
healthcare
monitoring.
In
recent
years,
the
effective
utilization
of
functional
nanomaterials
in
various
electroanalytical
measurements
realized
a
rapid,
sensitive,
selective
detection
monitoring
wide
range
biomarkers
body
fluids.
Owing
good
biocompatibility,
high
organic
capturing
ability,
strong
electrocatalytic
activity,
robustness,
transition
metal
oxide-derived
nanocomposites
led
enhancements
sensing
performances.
The
aim
present
review
is
describe
key
advancements
oxide
nanocomposites-based
electrochemical
sensors,
along
with
current
challenges
prospects
towards
development
highly
durable
reliable
biomarkers.
Moreover,
preparation
nanomaterials,
electrode
fabrication,
mechanism,
electrode-bio
interface,
performance
oxides
nanocomposite-based
sensor
platforms
will
be
described.
ACS Nano,
Год журнала:
2023,
Номер
17(16), С. 15605 - 15614
Опубликована: Июль 28, 2023
Immunotherapy
is
an
advanced
therapeutic
strategy
of
cancer
treatment
but
suffers
from
the
issues
off-target
adverse
effects,
lack
real-time
monitoring
techniques,
and
unsustainable
response.
Herein,
ultrasmall
Au
nanocluster
(NC)-based
theranostic
probe
designed
for
second
near-infrared
window
(NIR-II)
photoluminescence
(PL)
imaging-guided
phototherapies
photoactivatable
immunotherapy.
The
(Au44MBA26-NLG
short)
composed
atomically
precise
NIR-II
emitting
Au44MBA26
NCs
(here
MBA
denotes
water-soluble
4-mercaptobenzoic
acid)
conjugated
with
immune
checkpoint
inhibitor
1-cyclohexyl-2-(5H-imidazo[5,1-a]isoindol-5-yl)ethanol
(NLG919)
via
a
singlet
oxygen
(1O2)-cleavable
linker.
Upon
NIR
photoirradiation,
Au44MBA26-NLG
not
only
enables
PL
imaging
tumors
in
deep
tissues
guiding
tumor
therapy
also
allows
leverage
photothermal
property
(PTT)
photogenerated
1O2
photodynamic
(PDT)
releasing
NLG919
Such
multiple
effect
modulated
by
prompts
proliferation
activation
effector
T
cells,
upshifts
systemic
antitumor
T-lymphocyte
(T
cell)
immunity,
finally
suppresses
growth
both
primary
distant
living
mice.
Overall,
this
study
may
provide
promising
nanoplatform
toward
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(17)
Опубликована: Фев. 26, 2024
Atomically
precise
metal
nanoclusters
(NCs)
with
unique
optical
properties
and
abundant
catalytic
sites
are
promising
in
photocatalysis.
However,
their
light-induced
instability
the
difficulty
of
utilizing
photogenerated
carriers
for
photocatalysis
pose
significant
challenges.
Here,
MAg
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Фев. 28, 2024
Abstract
The
development
of
facile
tailoring
approach
to
adjust
the
intrinsic
activity
and
stability
atomically-precise
metal
nanoclusters
catalysts
is
great
interest
but
remians
challenging.
Herein,
well-defined
Au
8
modified
by
single-atom
sites
are
rationally
synthesized
via
a
co-eletropolymerization
strategy,
in
which
uniformly
dispersed
nanocluster
co-entrenched
on
poly-carbazole
matrix.
Systematic
characterization
theoretical
modeling
reveal
that
functionalizing
single-atoms
enable
altering
electronic
structures
clusters,
amplifies
their
electrocatalytic
reduction
CO
2
~18.07
fold
compared
isolated
clusters.
rearrangements
structure
not
only
strengthen
adsorption
key
intermediates
*COOH,
also
establish
favorable
reaction
pathway
for
reaction.
Moreover,
this
strategy
fixing
cross-linked
polymer
networks
efficiently
deduce
performance
deactivation
caused
agglomeration
during
catalytic
process.
This
work
contribute
explore
improvement
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(13), С. 9026 - 9035
Опубликована: Март 5, 2024
The
introduction
of
single
or
multiple
heterometal
atoms
into
metal
nanoparticles
is
a
well-known
strategy
for
altering
their
structures
(compositions)
and
properties.
However,
surface
nonmetal
atom
doping
challenging
rarely
reported.
For
the
first
time,
we
have
developed
synthetic
methods,
realizing
"surgery"-like,
successive
doping,
replacement,
addition
ultrasmall
(metal
nanoclusters,
NCs),
successfully
synthesized
characterized
three
novel
bcc
NCs
Au38I(S-Adm)19,
Au38S(S-Adm)20,
Au38IS(S-Adm)19
(S-Adm:
1-adamantanethiolate).
influences
replacement
on
NC
structure
optical
properties
(including
absorption
photoluminescence)
were
carefully
investigated,
providing
insights
(composition)–property
correlation.
Furthermore,
bottom-up
method
was
employed
to
construct
metal–organic
framework
(MOF)
surface,
which
did
not
essentially
alter
but
led
partial
release
ligands
stimulated
activity
catalyzing
p-nitrophenol
reduction.
MOF
construction
enhanced
stability
water
solubility,
another
dimension
tunning
catalytic
by
modifying
functional
groups.
