Abstract
Research
results
about
the
structure,
acid‐base,
redox,
and
adsorption
characteristics
of
zinc(yttrium)‐containing
dealuminated
BEA
zeolites
(Si/Al=1000),
Zn(Y)SiBEA
their
catalytic
properties
in
propane
dehydrogenation
with
CO
2
(CO
‐PDH)
are
presented.
The
catalysts
were
prepared
through
a
two‐step
procedure
involving
complete
dealumination
zeolite
followed
by
introduction
Zn
2+
Y
3+
cations
into
vacant
T‐atom
sites,
impregnation.
samples
obtained
characterized
using
XRD,
XPS,
29
Si
DP
MAS
NMR,
low‐temperature
N
ad/desorption,
TPR‐H
,
C
3
H
8
/C
6
NH
)‐TPD,
FTIR‐Py
techniques.
influence
zinc
content
yttrium
on
functional
surface
activity/selectivity
(Zn
1.0
‐,
2.0
SiBEA)
‐PDH
process
analyzed.
balanced
acid‐base
determine
‐mediated
to
propene.
Propane
conversion
propene
selectivity/yield
over
higher
compared
direct
(without
).
Russian Chemical Reviews,
Год журнала:
2023,
Номер
92(12), С. RCR5104 - RCR5104
Опубликована: Дек. 1, 2023
After
the
appearance
of
green
chemistry
concept,
which
was
introduced
in
vocabulary
early
1990s,
its
main
statements
have
been
continuously
developed
and
modified.
Currently,
there
are
10–12
cornerstones
that
should
form
basis
for
an
ideal
chemical
process.
This
review
analyzes
accumulated
experience
achievements
towards
design
products
processes
reduce
or
eliminate
use
generation
hazardous
substances.
The
presents
views
leading
Russian
scientists
specializing
various
fields
this
subject,
including
homogeneous
heterogeneous
catalysis,
fine
basic
organic
synthesis,
electrochemistry,
polymer
chemistry,
based
on
bio-renewable
feedstocks
energetic
compounds
materials.
A
new
approach
to
quantitative
evaluation
environmental
friendliness
by
authors
is
described.
<br>
bibliography
includes
1761.
ACS Catalysis,
Год журнала:
2022,
Номер
12(18), С. 11239 - 11252
Опубликована: Сен. 1, 2022
In
this
work,
a
series
of
VOx-loaded
In2O3
catalysts
were
prepared,
and
their
catalytic
performance
was
evaluated
for
CO2-assisted
oxidative
dehydrogenation
propane
(CO2-ODHP)
compared
with
alone.
The
optimal
composition
is
obtained
on
3.4V/In2O3
(surface
V
density
3.4V
nm–2),
which
exhibited
not
only
higher
C3H6
selectivity
than
other
V/In
under
isoconversion
conditions
but
also
an
improved
reaction
stability.
To
elucidate
the
catalyst
structure–activity
relationship,
VOx/In2O3
characterized
by
chemisorption
[NH3-temperature-programmed
desorption
(TPD),
NH3-diffuse
reflectance
infrared
Fourier
transform
spectroscopy
(DRIFTS),
CO2-TPD,
CO2-DRIFTS],
H2-temperature-programmed
reduction
(TPR),
in
situ
Raman
spectroscopy,
UV–vis
diffuse
near-ambient
pressure
X-ray
photoelectron
absorption
further
examined
using
functional
theory.
In–O–V
structure
extent
oligomerization,
play
crucial
role
improving
stability,
identified
catalysts.
particular,
presence
surface
VOx
(i)
inhibits
deep
In2O3,
thereby
preserving
activity,
(ii)
neutralizes
excess
basicity
thus
suppressing
dry
reforming
achieving
propylene
selectivity,
(iii)
introduces
additional
redox
sites
that
participate
utilizing
CO2
as
soft
oxidant.
present
work
provides
insights
into
developing
selective,
stable,
robust
metal-oxide
CO2-ODHP
controlling
conversion
reagents
via
desired
pathways
through
interplay
between
acid–base
interactions
properties.
ACS Catalysis,
Год журнала:
2024,
Номер
14(4), С. 2502 - 2521
Опубликована: Фев. 2, 2024
Olefins
are
important
building
blocks
that
have
been
extensively
used
to
produce
diverse
consumer
products
in
petrochemical
industry.
Owing
the
requirement
of
low-carbon-footprint
processes
and
increasing
use
light
alkanes
sourced
from
shale
gas,
an
environmentally
friendly
economic
route
alternative
state-of-the-art
steam
cracking
crude
oil
has
investigated
for
olefin
production.
The
oxidative
dehydrogenation
(ODH)
olefins
attracted
wide
attention
due
absence
thermodynamic
limitations
coke
formation.
However,
excessive
oxidation
is
prone
occur
this
process.
Developing
a
suitable
ODH
catalyst
with
high
performance,
particularly
enhanced
selectivity,
more
urgent
but
still
remains
challenge.
In
Review,
we
talk
about
representative
currently
developed
isolation
strategies
optimize
selectivity
via
process,
conversion
ethane
ethylene,
which
include
dispersion
regulation
metal
oxide,
nonmetal
sites,
construction
dual
functional
sites
isolate
steps,
adoption
selective
oxygen
species
promotion
soft
oxidants
as
reactants.
Furthermore,
mechanistic
aspects
activation
participation
tailoring
then
classified
discussed
detail.
Finally,
perspectives
emerging
technologies
process
listed
evaluated.
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(22), С. 13510 - 13519
Опубликована: Янв. 1, 2024
Due
to
multiple
reaction
steps
and
a
lack
of
efficient
catalysts,
the
synthesis
ethane
from
CO
2
electroreduction
(ECO
RR)
is
particularly
challenging.
A
Zn(OH)
/Cu
2+1
O/CF
catalyst
was
applied
in
electrocatalytic
reduction
ethane,
which
offers
high
selectivity
at
low
overpotentials.
Abstract
The
carbon
dioxide
reduction
reaction
(CO
2
RR)
for
the
synthesis
of
high‐energy‐density
and
high‐value
multi‐carbon
(C
2+
)
products
has
demonstrated
considerable
potential
practical
applications.
In
this
work,
we
design
a
novel
copper
oxide
foam
(OD‐Cu
foam)
catalyst
through
high‐temperature
calcination
process,
characterized
by
substantial
specific
surface
area.
distinctive
three‐dimensional
structure
OD‐Cu
metal
particles
covered
on
its
provide
abundant
active
sites.
total
Faradaic
efficiency
57.3%
C
over
is
achieved
at
−0.85
V
versus
reversible
hydrogen
electrode
(RHE).
Furthermore,
partial
current
density
reaches
44.1
mA
cm
−2
−0.95
RHE,
surpassing
significantly
that
both
Cu
(3.4
foil
foil)
(1.6
).
addition,
integrated
foam,
which
does
not
require
complex
preparation
processes,
facilitates
application
in
CO
RR.
These
results
underscore
significance
high
area,
emphasizing
effective
sustainable
conversion.
ACS Catalysis,
Год журнала:
2024,
Номер
14(13), С. 10376 - 10391
Опубликована: Июнь 25, 2024
The
CO2
oxidative
dehydrogenation
of
propane
(CO2–ODHP)
is
a
highly
important
reaction
for
not
only
producing
large
amounts
propylene
but
also
consuming
the
resource.
GaN/zeolite
catalysts
deliver
preferable
activity
in
reaction.
However,
similar
to
Pt-
and
Cr-based
catalysts,
there
are
shortcomings
such
as
poor
stability
coke
accumulation,
especially
when
operated
at
temperatures
higher
than
550
°C.
Generally,
carbon
deposition
one
main
reasons
catalyst
deactivation.
limited
mass
transfer
greatly
aggravates
deposited
formation,
since
precursors
could
be
removed
time.
In
present
work,
we
modified
zeolites
with
short
b-axis
hierarchical
pores,
which
offer
shorter
diffusion
distance
pore-rich
structure
enhance
transfer.
Thanks
this
enhancement,
offers
an
initial
conversion
68.0%
yield
39.4%
propylene,
surpassing
other
reported
data.
Importantly,
showed
low
loss
rate
amount
carbon,
was
easily
regenerated
compared
those
without
or
pores.
Density
functional
theory
(DFT)
calculations
situ
diffuse
reflectance
infrared
Fourier
transform
spectroscopy
(DRIFTS)
confirmed
that
involves
coupling
direct
reduction
via
reverse
water–gas
shift
reaction,
participates
work
sheds
light
on
designing
efficient
CO2–ODHP
transfer-boosted
strategy
and,
importantly,
expected
provide
inspiration
constructing
zeolite