Nature Communications,
Journal Year:
2025,
Volume and Issue:
16(1)
Published: Feb. 21, 2025
Marvelous
natures
of
alkali
and
alkaline
earth
metal
hydrides
in
catalyzing
chemical
transformations
are
being
discovered.
However,
the
synthesis
(sub)nanostructured
hydrides,
critically
important
to
enhance
their
catalytic
performances,
is
yet
a
very
challenging
task.
Herein,
we
develop
highly
reactive
heterogeneous
catalyst
comprising
atomically
dispersed
barium
on
MgO
support
with
an
ultrahigh
loading
up
20
wt%
via
convenient
preparation
method
involving
liquid-ammonia
impregnation
followed
by
hydrogenation.
The
surface
hydride
species
not
only
exhibits
extraordinary
reactivity
toward
H2
activation
at
room
temperature,
but
also
enables
efficient
hydrogen
isotope
exchange
(HIE)
both
sp3
C–H
sp2
bonds
nonactivated
alkylarenes
using
D2
as
deuterium
source
under
mild
conditions.
deuteration
rate
benzylic
site
two
orders
magnitude
higher
than
that
bulk
BaH2.
This
study
offers
alternative
synthetic
route
for
manufacture
deuterium-labeled
compounds
heterogenous
transition
metal-free
beyond
widely
studied
molecular
complexe
catalysts.
Hydrogen
essential
remains
demonstrates
selective
temperature
hydride.
ACS Nano,
Journal Year:
2023,
Volume and Issue:
17(17), P. 17254 - 17264
Published: Aug. 31, 2023
The
emerging
lattice-oxygen
oxidation
mechanism
(LOM)
presents
attractive
opportunities
for
breaking
the
scaling
relationship
to
boost
oxygen
evolution
reaction
(OER)
with
direct
OLattice-*O
interaction.
However,
currently
LOM-triggering
rationales
are
still
debated,
and
a
streamlined
physicochemical
paradigm
is
extremely
desirable
design
of
LOM-defined
OER
catalysts.
Herein,
Ni
metal-organic
framework/black
phosphorene
(NiMOF/BP)
heterostructure
theoretically
profiled
constructed
as
catalytic
platform
LOM-derived
studies.
It
found
that
p-type
BP
host
can
enlarge
Ni-O
bond
polarizability
NiMOF
through
stretching
valence
declining
synergically.
Such
an
enlarged
will
in
principle
alleviate
lattice
confinement
benefit
LOM
pathway
performance.
As
result,
optimized
NiMOF/BP
catalyst
exhibits
promising
performance
low
overpotential
260
mV
at
10
mA
cm-2
long-term
stability
1
M
KOH
electrolyte.
Both
experiment
calculation
results
suggest
activated
more
balanced
step
barrier
catalyst.
This
research
puts
forward
criterion
LOM-scaled
electrocatalysts
water
oxidation.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(5), P. 3208 - 3217
Published: Feb. 15, 2024
The
design
and
construction
of
highly
efficient
catalytic
active
sites
for
promoting
hydrogen
spillover
are
great
significance
improving
hydrocracking
(HCK)
hydrodesulfurization
(HDS)
performance
in
slurry-phase
hydrogenation
vacuum
residue
(VR)
but
still
challenging.
Herein,
we
report
a
carbon-supported
MoCo
dual-atomic
site
catalyst
(MoCo
DAC/C)
propose
an
oxygen-vacancy-induced
built-in
electric
field
(BIEF)
regulation
mechanism
HCK
HDS.
It
was
found
that
the
coordination
structure
reconstructed
formed
O
vacancies
situ
during
process.
formation
not
only
provided
macromolecular
adsorption
also
broke
electronic
balance
weak
BIEF
between
Mo
Co
atoms.
Meanwhile,
H2
activated
at
to
form
species.
promoted
from
by
Mo–C–Co
bridging
bond,
thus
greatly.
In
VR,
DAC/C
demonstrates
remarkable
activity
with
TOFT
calculated
total
metals
up
0.77
s–1
(two
times
enhancement
than
single
atoms
(SAs)/C),
per
pass
conversion
VR
76
wt
%,
liquid
product
yield
92
coke
content
0.55
%.
shows
robust
HDS
dibenzothiophene
(DBT)
70
Density
functional
theory
reveals
leads
discrepancy
Bader
charge
atoms,
resulting
local
can
favor
diffusion
positively
charged
(+0.10
e−)
H
atom.
This
work
proposes
atomic
scale
enhancing
reaction
process
spillover,
which
novel
insights
development
high-performance
catalysts.
Nature Communications,
Journal Year:
2024,
Volume and Issue:
15(1)
Published: June 7, 2024
Abstract
For
di-nitroaromatics
hydrogenation,
it
is
a
challenge
to
achieve
the
multi-step
hydrogenation
with
high
activity
and
selectivity
due
complexity
of
process
involving
two
nitro
groups.
Consequently,
many
precious
metal
catalysts
suffer
from
low
for
this
reaction.
Herein,
we
employ
fully
exposed
Pt
clusters
catalyst
consisting
an
average
four
atoms
on
nanodiamond@graphene
(Pt
n
/ND@G),
demonstrating
excellent
catalytic
performance
2,4-dinitrotoluene.
The
TOF
(40647
h
−1
)
/ND@G
significantly
superior
that
single
catalyst,
nanoparticles
even
all
known
catalysts.
Density
functional
theory
calculations
absorption
experiments
reveal
synergetic
interaction
between
multiple
active
sites
facilitate
co-adsorption/activation
reactants
H
2
,
as
well
desorption
intermediates/products,
which
key
higher
than
catalyst.
Small,
Journal Year:
2023,
Volume and Issue:
19(42)
Published: June 15, 2023
Abstract
Dual‐Active‐Sites
Single‐Atom
catalysts
(DASs
SACs)
are
not
only
the
improvement
of
SACs
but
also
expansion
dual‐atom
catalysts.
The
DASs
contains
dual
active
sites,
one
which
is
a
single
atomic
site,
and
other
site
can
be
atom
or
type
endowing
with
excellent
catalytic
performance
wide
range
applications.
categorized
into
seven
types,
including
neighboring
mono
metallic
SACs,
bonded
non‐bonded
bridged
asymmetric
metal
nonmetal
combined
space
separated
SACs.
Based
on
above
classification,
general
methods
for
preparation
comprehensively
described,
especially
their
structural
characteristics
discussed
in
detail.
Meanwhile,
in‐depth
assessments
variety
applications
electrocatalysis,
thermocatalysis
photocatalysis
provided,
as
well
unique
mechanism
addressed.
Moreover,
prospects
challenges
related
highlighted.
authors
believe
great
expectations
this
review
will
provide
novel
conceptual
methodological
perspectives
exciting
opportunities
further
development
application
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(18), P. 13800 - 13813
Published: Sept. 3, 2024
Hydrodeoxygenation
of
lignin-derived
guaiacol
to
aromatic
products
under
mild
conditions
was
achieved
using
an
interesting
Pt/TiO2-D
catalyst.
The
defects
in
TiO2-D
played
a
pivotal
role
H2
dissociation
and
exhibited
unique
capability
for
the
migration
active
H
species
on
surface
within
bulk
phase
TiO2-D,
resulting
formation
"H
reservoir"
adjacent
Pt
sites.
Consequently,
superb
activity
cleavage
C–O
bond
extremely
low
hydrogen
concentration
(1
atm
10%
H2/Ar).
Moreover,
H−migration
into
induced
new
Ti3O5
crystalline
phase,
creating
additional
defects,
which
turn
accelerated
activation,
Pt-H
species,
reservoir,
account
satisfactory
ability
adsorption
conditions.
