JACS Au,
Год журнала:
2024,
Номер
4(11), С. 4084 - 4109
Опубликована: Окт. 29, 2024
Propane
dehydrogenation
(PDH)
is
currently
an
approach
for
the
production
of
propylene
with
high
industrial
importance,
especially
in
context
shale
gas
revolution
and
growing
global
demands
downstream
commodity
chemicals.
In
this
Perspective
article,
we
comprehensively
summarize
recent
advances
design
advanced
catalysts
PDH
new
understanding
structure–performance
relationship
supported
metal
catalysts.
Furthermore,
discuss
gaps
between
fundamental
research
practical
applications
catalyst
developments
process.
particular,
overview
some
critical
issues
regarding
regeneration
compatibility
reactor
design.
Finally,
make
perspectives
on
future
directions
research,
including
efforts
toward
achieving
a
unified
relationship,
innovation
engineering,
translation
knowledge
accumulated
studies
to
other
important
alkane
reactions.
Chemical Reviews,
Год журнала:
2023,
Номер
123(8), С. 4855 - 4933
Опубликована: Март 27, 2023
Heterogeneous
bimetallic
catalysts
have
broad
applications
in
industrial
processes,
but
achieving
a
fundamental
understanding
on
the
nature
of
active
sites
at
atomic
and
molecular
level
is
very
challenging
due
to
structural
complexity
catalysts.
Comparing
features
catalytic
performances
different
entities
will
favor
formation
unified
structure-reactivity
relationships
heterogeneous
thereby
facilitate
upgrading
current
In
this
review,
we
discuss
geometric
electronic
structures
three
representative
types
(bimetallic
binuclear
sites,
nanoclusters,
nanoparticles)
then
summarize
synthesis
methodologies
characterization
techniques
for
entities,
with
emphasis
recent
progress
made
past
decade.
The
supported
nanoparticles
series
important
reactions
are
discussed.
Finally,
future
research
directions
catalysis
based
and,
more
generally,
prospective
developments
both
practical
applications.
Science,
Год журнала:
2023,
Номер
383(6678), С. 94 - 101
Опубликована: Дек. 21, 2023
Copper
nanoparticle-based
catalysts
have
been
extensively
applied
in
industry,
but
the
nanoparticles
tend
to
sinter
into
larger
ones
chemical
atmospheres,
which
is
detrimental
catalyst
performance.
In
this
work,
we
used
dealuminated
Beta
zeolite
support
copper
(Cu/Beta-deAl)
and
showed
that
these
particles
become
smaller
methanol
vapor
at
200°C,
decreasing
from
~5.6
~2.4
nanometers
diameter,
opposite
general
sintering
phenomenon.
A
reverse
ripening
process
was
discovered,
whereby
migratable
sites
activated
by
were
trapped
silanol
nests
species
acted
as
new
nucleation
for
formation
of
small
nanoparticles.
This
feature
reversed
channel,
resulting
robust
dimethyl
oxalate
hydrogenation
performed
with
supported
use
industry.
Chemical Reviews,
Год журнала:
2023,
Номер
123(21), С. 12135 - 12169
Опубликована: Окт. 26, 2023
Heterogeneous
catalysts
undergo
thermal-
and/or
adsorbate-induced
dynamic
changes
under
reaction
conditions,
which
consequently
modify
their
catalytic
behavior.
Hence,
it
is
increasingly
crucial
to
characterize
the
properties
of
a
catalyst
conditions
through
so-called
"operando"
approach.
Operando
IR
spectroscopy
probably
one
most
ubiquitous
and
versatile
characterization
methods
in
field
heterogeneous
catalysis,
but
its
potential
identifying
adsorbate-
thermal-induced
phenomena
often
overlooked
favor
other
less
accessible
methods,
such
as
XAS
high-resolution
microscopy.
Without
detracting
from
these
techniques,
while
aware
enormous
value
multitechnique
approach,
purpose
this
Review
show
that
alone
can
provide
relevant
information
field.
This
done
by
discussing
few
selected
case
studies
our
own
research
experience,
belong
categories
both
"single-site"-
nanoparticle-based
catalysts.
JACS Au,
Год журнала:
2024,
Номер
4(2), С. 666 - 679
Опубликована: Фев. 6, 2024
Reactant-induced
structural
evolutions
of
heterogeneous
metal
catalysts
are
frequently
observed
in
numerous
catalytic
systems,
which
can
be
associated
with
the
formation
or
deactivation
active
sites.
In
this
work,
we
will
show
transformation
subnanometer
Pt
clusters
pure-silica
MFI
zeolite
structure
presence
CO,
O2,
and/or
H2O
and
consequences
Pt-zeolite
materials
derived
from
various
treatment
conditions.
By
applying
appropriate
pretreatment
under
a
reactant
atmosphere,
precisely
modulate
size
distribution
species
spanning
single
atoms
to
small
nanoparticles
(1–5
nm)
matrix,
resulting
desirably
stable
for
CO
oxidation.
We
also
incorporation
Fe
into
framework
greatly
promotes
stability
against
undesired
sintering
harsh
conditions
(up
650
°C
moisture).
ACS Catalysis,
Год журнала:
2022,
Номер
12(22), С. 13813 - 13830
Опубликована: Окт. 27, 2022
X-ray
absorption
spectroscopy
(XAS)
[extended
fine
structure
(EXAFS)
and
near-edge
(XANES)]
is
a
key
technique
within
the
heterogeneous
catalysis
community
to
probe
properties
of
active
site(s)
for
diverse
range
catalytic
materials.
However,
interpretation
raw
experimental
data
derive
an
atomistic
picture
catalyst
requires
modeling
analysis;
EXAFS
are
compared
model,
goodness
fit
parameter
used
judge
best
fit.
This
can
often
be
nontrivial
time-consuming;
overcoming
or
improving
these
limitations
remains
central
challenge
community.
Considering
limitations,
this
Perspective
highlights
how
recent
developments
in
analysis
software,
increased
availability
reliable
computational
models,
application
science
tools
improve
speed,
accuracy,
reliability
interpretation.
In
particular,
we
emphasize
advantages
combining
theory
as
unified
that
should
treated
standard
(when
applicable)
identify
sites
not
two
separate
complementary
methods.
Building
on
trends
community,
also
present
community-driven
approach
adopt
FAIR
Guiding
Principles
collection,
analysis,
dissemination,
storage
XAS
data.
Written
with
both
audience
mind,
provide
roadmap
foster
collaborations
between
communities.
ACS Catalysis,
Год журнала:
2024,
Номер
14(3), С. 1232 - 1242
Опубликована: Янв. 10, 2024
Machine
learning
(ML),
when
used
synergistically
with
atomistic
simulations,
has
recently
emerged
as
a
powerful
tool
for
accelerated
catalyst
discovery.
However,
the
application
of
these
techniques
been
limited
by
lack
interpretable
and
transferable
ML
models.
In
this
work,
we
propose
curriculum-based
training
(CBT)
philosophy
to
systematically
develop
reactive
machine
potentials
(rMLPs)
high-throughput
screening
zeolite
catalysts.
Our
CBT
approach
combines
several
different
types
calculations
gradually
teach
model
about
relevant
regions
potential
energy
surface.
The
resulting
rMLPs
are
accurate,
transferable,
interpretable.
We
further
demonstrate
effectiveness
exhaustively
thousands
[CuOCu]2+
sites
across
hundreds
Cu-zeolites
industrially
methane
activation
reaction.
Specifically,
large-scale
analysis
entire
International
Zeolite
Association
(IZA)
database
identifies
set
previously
unexplored
zeolites
(i.e.,
MEI,
ATN,
EWO,
CAS)
that
show
highest
ensemble-averaged
rates
[CuOCu]2+-catalyzed
activation.
believe
can
be
generally
applied
other
zeolite-catalyzed
reactions
and,
subsequently,
heterogeneous
Thus,
represents
an
important
step
toward
overcoming
long-standing
barriers
within
computational
catalysis
community.
ACS Nano,
Год журнала:
2024,
Номер
18(8), С. 6638 - 6649
Опубликована: Фев. 13, 2024
Strong
metal–support
interactions
(SMSIs)
are
well-known
in
the
field
of
heterogeneous
catalysis
to
induce
encapsulation
platinum
(Pt)
group
metals
by
oxide
supports
through
high
temperature
H2
reduction.
However,
demonstrations
SMSI
overlayers
have
largely
been
limited
reducible
oxides,
such
as
TiO2
and
Nb2O5.
Here,
we
show
that
amorphous
native
surface
plasmonic
aluminum
nanocrystals
(AlNCs)
exhibits
SMSI-induced
Pt
following
reduction
a
structure
dependent
manner.
Reductive
treatment
at
300
°C
induces
formation
an
AlOx
overlayer
on
clusters,
leaving
single-atom
sites
(Ptiso)
exposed
available
for
catalysis.
The
remaining
Ptiso
species
possess
more
uniform
local
coordination
environment
than
has
observed
other
forms
Al2O3,
suggesting
AlNCs
presents
well-defined
anchoring
individual
atoms.
This
observation
extends
our
understanding
SMSIs
providing
evidence
H2-induced
can
occur
wider
variety
materials
should
stimulate
expanded
studies
this
effect
include
nonreducible
oxides
with
oxygen
defects
presence
disorder.
It
also
suggests
created
manner,
when
combined
properties
Al
nanocrystal
core,
may
allow
site-specific
photocatalysis,
dynamic
control
over
light-driven
reactivity
these
systems.
JACS Au,
Год журнала:
2023,
Номер
3(11), С. 3213 - 3226
Опубликована: Ноя. 2, 2023
Zeolite-encapsulated
subnanometer
metal
catalysts
are
an
emerging
class
of
solid
with
superior
performances
in
comparison
to
supported
on
open-structure
carriers.
Currently,
there
is
no
general
synthesis
methodology
for
the
encapsulation
different
zeolite
structures.
In
this
work,
we
will
show
a
method
clusters
(Pt,
Pd,
and
Rh)
within
various
silicoaluminate
zeolites
topologies
(MFI,
CHA,
TON,
MOR).
The
successful
generation
species
relies
introduction
Sn,
which
can
suppress
migration
during
high-temperature
oxidation–reduction
treatments
according
advanced
electron
microscopy
spectroscopy
characterizations.
advantage
encapsulated
Pt
reflected
direct
coupling
ethane
benzene
production
ethylbenzene,
acid
sites
work
synergistic
way.