Synlett,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 26, 2025
Abstract
In
this
account,
we
summarize
our
recent
progress
on
the
structural
regulation
and
selective
catalysis
of
biomass-derived
carbon-based
non-precious
nanocatalysts
(Fe,
Co,
Ni,
Cu)
in
organic
reactions
that
include
hydrogenation
functional
nitro
compounds
to
amines,
oxidation
alkenes,
coupling
reactions,
unsaturated
aldehydes.
1
Introduction
2
Fe-Based
Catalysts
3
Co-Based
4
Ni-Based
5
Cu-Based
6
Conclusions
Proceedings of the National Academy of Sciences,
Journal Year:
2025,
Volume and Issue:
122(2)
Published: Jan. 9, 2025
Despite
the
broad
catalytic
relevance
of
metal–support
interfaces,
controlling
their
chemical
nature,
interfacial
contact
perimeter
(exposed
to
reactants),
and
consequently,
contributions
overall
reactivity,
remains
challenging,
as
nanoparticle
support
characteristics
are
interdependent
when
catalysts
prepared
by
impregnation.
Here,
we
decoupled
both
using
a
raspberry-colloid-templating
strategy
that
yields
partially
embedded
PdAu
nanoparticles
within
well-defined
SiO
2
or
TiO
supports,
thereby
increasing
compared
nonembedded
attaching
same
onto
surfaces.
Between
PdAu/SiO
PdAu/TiO
,
identified
effect
resulting
in
1.4-fold
higher
activity
than
for
benzaldehyde
hydrogenation.
Notably,
partial
embedding
raspberry-colloid-templated
increased
number
Au/TiO
sites
5.4-fold,
which
further
enhanced
an
additional
4.1-fold.
Theoretical
calculations
situ
surface-sensitive
desorption
analyses
reveal
facile
binding
at
interface
Pd
ensembles
on
surface,
explaining
connection
between
(via
perimeter)
activity.
Our
results
demonstrate
synthetic
produce
thermocatalytically
stable
increase
catalytically
active
augment
arising
from
interfaces.
The Journal of Physical Chemistry Letters,
Journal Year:
2025,
Volume and Issue:
unknown, P. 924 - 931
Published: Jan. 20, 2025
Understanding
the
mechanism
of
nitrogen
reduction
reaction
(NRR)
is
essential
for
designing
highly
efficient
catalysts.
In
this
study,
we
investigated
effects
metal–support
interaction
(MSI)
on
NRR
using
density
functional
theory.
The
simulations
revealed
that
MSI
weak
in
Au13/BiOCl
system,
with
charge
accumulation
and
depletion
primarily
occurring
within
Au13
cluster.
By
replacement
one
Au
atom
either
a
Ag
or
Pt
atom,
becomes
stronger
compared
to
system.
because
doping
breaks
symmetry
cluster,
leading
at
interface.
Specifically,
enhanced
reduces
energy
barriers
rate-determining
step
from
1.07
eV
system
0.91
Au12Ag/BiOCl
0.87
Au12Pt/BiOCl,
respectively.
Our
study
uncovers
critical
role
activity
NRR,
providing
theoretical
insights
development
Metal–support
interactions
(MSI)
play
a
crucial
role
in
enhancing
the
catalytic
activity
and
stability
of
metal
catalysts
by
establishing
stable
metal-oxide
interface.
However,
precisely
controlling
MSI
at
atomic
scale
remains
significant
challenge,
as
how
to
construct
an
optimal
is
still
not
fully
understood:
Both
insufficient
excessive
showed
inferior
performance.
In
this
study,
we
propose
finely
tuning
using
temporal-precise
transient
high-temperature
pulse
heating.
Using
Pt/CeO2
model
system,
systematically
investigate
variations
duration
atmosphere
influence
reconstruction
metal–support
interface
MSIs.
This
leads
formation
two
distinct
types
MSI:
(1)
strong
(SMSI,
Pt@CeO2)
(2)
reactive
(RMSI,
Pt5Ce@CeO2),
each
with
unique
compositions,
structures,
electrochemical
behaviors.
Notably,
Pt5Ce@CeO2
RMSI
exhibits
remarkable
performance
alkaline
hydrogen
evolution,
showing
overpotential
−29
mV
operation
for
over
300
h
−10
mA·cm–2.
Theoretical
studies
reveal
that
alloying
Pt
Ce
form
Pt5Ce
modifies
electronic
structure
Pt,
shifting
d-band
center
optimize
adsorption
dissociation
intermediates,
thereby
reducing
reaction
energy
barrier.
Moreover,
intimate
interaction
CeO2
further
improves
stability.
Our
strategy
enables
precise,
stepwise,
controllable
regulation
MSIs,
providing
insights
development
highly
efficient
durable
heterostructured
wide
range
applications.
Chemistry,
Journal Year:
2025,
Volume and Issue:
7(1), P. 26 - 26
Published: Feb. 19, 2025
This
study
was
aimed
at
elucidating
the
role
of
carboneous
component
in
Co–carbon-containing
catalysts
for
hydrogenation
organic
compounds.
A
Co-C/SiO2
catalyst
synthesized
via
pyrolysis
a
Co(II)
complex
with
1,2-diaminobenzene
on
silica
and
subsequently
irradiated
2.3
MeV
electrons,
producing
Co-C/SiO2*.
comprehensive
characterization
using
XRD,
TEM,
IR,
Raman
spectroscopy
indicated
minimal
structural
changes
cobalt
nanoparticles
materials.
However,
analysis
revealed
slight
decrease
defect
content
upon
irradiation,
which
could
occur
due
to
healing.
The
catalytic
tests,
including
26
compounds,
demonstrated
an
enhanced
performance
17
cases.
improvement
attributed
modification
material.
It
be
concluded
that
components
Co-C
composites
contributed
their
performance,
probably
by
modifying
electronic
structure
Co
nanoparticles.
In
turn,
results
provide
arguments
against
supposition
occurs
defects
Small,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 21, 2025
Abstract
Ruthenium
(Ru)
–based
catalysts
have
been
considered
a
promising
candidate
for
efficient
sustainable
hydrogen
and
chlor‐alkali
co‐production.
Theoretical
calculations
disclosed
that
the
hollow
sites
on
Ru
surface
strong
adsorption
energies
of
H
Cl
species,
which
inevitably
leads
to
poor
activity
cathodic
evolution
reaction
(HER)
anodic
chlorine
(CER),
respectively.
Furthermore,
it
confirmed
anchoring
Lewis
acid
oxide
nanoparticles
such
as
MgO
can
induce
formation
onion‐like
charge
distribution
atoms
around
nanoparticles,
thereby
exposing
Ru‐bridge
at
interface
excellent
accelerate
both
HER
CER.
Under
guidance
theoretical
calculations,
novel
dispersed
(MgO
x
‐Ru)
electrocatalyst
is
successfully
prepared.
In
strongly
alkaline
saline
media,
‐Ru
recorded
CER
electrocatalytic
with
very
low
overpotential
19
mV
74
current
density
10
mA
cm
−2
,
More
stirringly,
electrochemical
test
electrodes
under
simulated
electrolysis
conditions
demonstrated
superior
performance
industrial
commercial
20
wt%
Pt/C
dimensionally
stable
anode
(DSA).
