Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(34), С. 24033 - 24041
Опубликована: Авг. 15, 2024
Palladium
(Pd)-based
single-atom
catalysts
(SACs)
have
shown
outstanding
selectivity
for
semihydrogenation
of
alkynes,
but
most
Pd
single
sites
coordinated
with
highly
electronegative
atoms
(such
as
N,
O,
and
S)
supports
will
result
in
a
decrease
the
electron
density
sites,
thereby
weakening
adsorption
reactants
reducing
catalytic
performance.
Constructing
rich
outer-shell
environment
by
changing
coordination
structure
offers
novel
opportunity
to
enhance
efficiency
excellent
alkene
selectivity.
Therefore,
this
work,
we
first
propose
situ
preparation
isolated
encapsulated
within
Al/Si-rich
ZSM-5
using
one-pot
seed-assisted
growth
method.
Organic Letters,
Год журнала:
2025,
Номер
27(4), С. 1024 - 1029
Опубликована: Янв. 21, 2025
Developed
Co-MgO/TiO2
was
applicable
to
C-N
bond
formation
by
direct
amination
of
primary
and
secondary
alcohols
with
NH3
via
a
borrowing
hydrogen
protocol.
Selective
synthesis
primary,
secondary,
tertiary
amines
achieved
controlling
the
reaction
conditions.
Asymmetric
can
be
synthesized
coupling
amines.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 5, 2025
Single-atom
catalysts
exhibit
the
excellent
catalytic
activity
and
selectivity,
making
them
widely
applicable
in
fields
of
advanced
materials,
environmental
science,
chemical
synthesis.
However,
understanding
mechanism
single-atom
reactions,
such
as
hydrogen
generation
reaction,
is
still
challenging,
which
notably
hampers
optimization
precise
control
reaction.
Here,
we
immobilize
a
single-metal
atom
model
catalyst
into
single-molecule
electrical
detection
platform
for
situ
monitoring
process
at
single-event
level.
In
combination
with
theoretical
experimental
studies,
mechanisms
especially
selection
center
through
charge,
spin,
orbital
quantum
control,
are
elucidated.
addition,
via
spin-induced
catalysis
observed,
turnover
frequency
increases
by
about
65
times
magnetic
field
50
mT.
This
study
provides
valuable
insights
intrinsic
opens
up
unique
avenues
their
thus
offering
useful
strategy
efficiently
developing
clean
energy.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 13, 2025
Abstract
Tuning
transition
metal
spin
states
potentially
offers
a
powerful
means
to
control
electrocatalyst
activity.
However,
implementing
such
strategy
in
electrochemical
CO
2
reduction
(CO
R)
is
challenging
since
rational
design
rules
have
yet
be
elucidated.
Here
we
show
how
the
addition
of
P
dopants
ferromagnetic
element
(Fe,
Co,
and
Ni)
single‐atom
catalyst
(SAC)
can
shift
its
state.
For
instance,
with
Fe
SAC,
enable
switch
from
low
state
(
d
x2‐
y2
0
,
z2
xz
yz
1
xy
)
Fe‐N
4
high
x2‐y2
3
‐P.
This
studied
using
suite
characterization
efforts,
including
X‐ray
absorption
spectroscopy
(XAS),
electron
resonance
(ESR)
spectroscopy,
superconducting
quantum
interference
device
(SQUID)
measurements.
When
used
for
R,
SAC
‐P
active
sites
yields
>
90%
Faradaic
efficiency
over
wide
potential
window
≈530
mV
maximum
partial
current
density
≈600
mA
cm
−2
.
Density
functional
theory
calculations
reveal
that
3+
exhibits
enhanced
back
donation
via
/
‐π*
bond,
which
enhances
*
COOH
adsorption
promotes
formation.
Taken
together,
results
intentionally
tuned
boost
R
performance.
Single-atom
catalysts
(SACs)
have
garnered
considerable
attention
owing
to
their
profound
potential
in
promoting
the
efficient
utilization
of
metal
resources
and
attaining
atomic-level
economy.
Fe,
Co,
Ni
SACs
demonstrated
broad
application
prospects
electrocatalysis
due
tunable
composition
structure,
as
well
unique
electronic
properties.
Firstly,
various
preparation
methods
for
are
outlined
this
review,
including
high-temperature
pyrolysis,
impregnation,
chemical
vapor
deposition,
atomic
layer
deposition.
These
not
only
enhance
efficiency
atoms
but
also
ensure
stability
catalysts.
Subsequently,
review
summarizes
recent
progress
applications
electrocatalysis,
with
a
particular
focus
on
efficacy
hydrogen
evolution
reaction,
oxygen
reduction
carbon
dioxide
nitrogen
reaction.
Despite
remarkable
advancements,
still
face
challenges
related
large-scale
production,
enhancement,
comprehensive
characterization,
mechanistic
exploration.
Finally,
discusses
these
proposes
strategies
address
them
order
fully
realize
high-performance
ACS Omega,
Год журнала:
2025,
Номер
10(9), С. 9649 - 9660
Опубликована: Фев. 24, 2025
Construction
of
a
C-C
bond
via
alkylation
ketones
with
alcohol
as
the
alkylating
source
by
employing
hydrogen-borrowing
strategy
is
attracting
significant
attention
and
highly
appealing
due
to
its
simplicity,
cost-effectiveness,
environmental
benefits,
fact
that
water
only
byproduct.
The
development
heterogeneous
catalysts
based
on
nonprecious
base
metals
progressing
rapidly.
Our
newly
disclosed
manganese-doped
cerium
oxide
nanocomposite
(10
wt
%
Mn@CeO2)
stands
out
cost-efficient
air-stable
catalyst,
synthesized
through
straightforward
coprecipitation
method
employed
for
α-alkylation
primary
alcohols
strategy.
X-ray
diffraction
(XRD)
analysis
confirms
high
crystallinity
CeO2,
while
field
emission
scanning
electron
microscopy
(FE-SEM)
high-resolution
transmission
(HR-TEM)
images
reveal
MnO2
nanoparticles,
measuring
19
nm
in
size,
uniformly
decorated
rod-shaped
CeO2
which
have
size
33
nm.
photoelectron
spectroscopy
(XPS)
uncovers
presence
Mn4+
species
embedded
nanorods.
Electron
paramagnetic
resonance
(EPR)
further
indicates
surface
defects
contribute
impressive
catalytic
yield,
ranges
from
70
98%
α-alkylated
ketones.
Thermogravimetric
(TGA)
demonstrates
remarkable
thermal
stability
maintaining
up
800
°C.
Additionally,
inductively
coupled
plasma
mass
spectrometry
(ICP-MS)
no
leaching
Mn
ions,
emphasizing
heterogeneity
catalyst.
Remarkably,
10
Mn@CeO2
recycled
six
cycles
loss
activity.
This
study
underscores
synergistic
effect
between
metal
redox
pair
key
exceptional
activity
reactions,
making
promising
catalyst
sustainable
efficient
formation.
Inorganic Chemistry,
Год журнала:
2025,
Номер
64(10), С. 4784 - 4790
Опубликована: Март 5, 2025
A
novel
magnetic
hollowed
CoFe@C-650
prism
catalyst
has
been
successfully
prepared
and
applied
in
the
N-alkylation
of
alcohols
amines
through
a
hydrogen
borrowing
strategy.
The
demonstrates
good
to
excellent
activities
reaction
with
broad
substrate
scope
afford
up
99%
yield
target
products.
preliminary
mechanistic
study
reveals
that
high
valent
Co
species
may
promote
adsorption
conversion
alcohols,
while
Fe
assists
hydrogenating
imine
intermediates.
