Spinel
oxides
are
considered
as
promising
low-cost
non-precious
metal
electrocatalysts
for
oxygen
evolution
reaction
(OER)
due
to
their
desirable
catalytic
activities
and
fast
kinetics.
However,
a
result
of
the
structural
complexity
spinel
oxides,
systematic
in-depth
studies
on
enhancing
OER
performance
remain
inadequate.
In
particular,
construction
active
sites
regarding
large
number
unoccupied
octahedral
interstices
has
not
yet
been
explored.
Herein,
more
with
high
constructed
surface
via
cationic
misalignment,
which
is
induced
by
defects
in
oxide
solutions,
i.e.,
MoFe2
O4
CoFe2
nanosheets
supported
an
iron
foam
(MCFO
NS/IF).
With
increased
modified
electronic
structure,
state-of-the-art
electrocatalyst
exhibits
excellent
activity
onset
potential
1.41
V
versus
RHE
overpotential
290
mV
achieve
current
density
500
mA
cm-2
.
Moreover,
such
also
demonstrates
kinetics
Tafel
slope
38
dec-1
superior
durability
maintaining
at
250
1000
h.
Chemical Reviews,
Год журнала:
2022,
Номер
123(9), С. 6039 - 6106
Опубликована: Сен. 1, 2022
Zeolites
with
ordered
microporous
systems,
distinct
framework
topologies,
good
spatial
nanoconfinement
effects,
and
superior
(hydro)thermal
stability
are
an
ideal
scaffold
for
planting
diverse
active
metal
species,
including
single
sites,
clusters,
nanoparticles
in
the
framework-associated
sites
extra-framework
positions,
thus
affording
metal-in-zeolite
catalysts
outstanding
activity,
unique
shape
selectivity,
enhanced
recyclability
processes
of
Brønsted
acid-,
Lewis
metal-catalyzed
reactions.
Especially,
thanks
to
advances
zeolite
synthesis
characterization
techniques
recent
years,
zeolite-confined
(denoted
as
metal@zeolite
composites)
have
experienced
rapid
development
heterogeneous
catalysis,
owing
combination
merits
both
intrinsic
properties.
In
this
review,
we
will
present
developments
strategies
incorporating
tailoring
zeolites
advanced
identification
location,
distribution,
coordination
environment
species
zeolites.
Furthermore,
catalytic
applications
demonstrated,
emphasis
on
composites
hydrogenation,
dehydrogenation,
oxidation
Finally,
point
out
current
challenges
future
perspectives
precise
synthesis,
atomic
level
identification,
practical
application
catalyst
system.
Advanced Materials,
Год журнала:
2021,
Номер
33(51)
Опубликована: Окт. 5, 2021
Abstract
Zeolites
possessing
large
specific
surface
areas,
ordered
micropores,
and
adjustable
acidity/basicity
have
emerged
as
ideal
supports
to
immobilize
metal
species
with
small
sizes
high
dispersities.
In
recent
years,
the
zeolite‐supported
catalysts
been
widely
used
in
diverse
catalytic
processes,
showing
excellent
activity,
superior
thermal/hydrothermal
stability,
unique
shape‐selectivity.
this
review,
a
comprehensive
summary
of
state‐of‐the‐art
achievements
applications
are
presented
for
important
heterogeneous
processes
last
five
mainly
including
1)
hydrogenation
reactions
(e.g.,
CO/CO
2
hydrogenation,
unsaturated
compounds,
nitrogenous
compounds);
2)
dehydrogenation
alkane
chemical
hydrogen
storage
materials);
3)
oxidation
CO
oxidation,
methane
alkene
epoxidation);
4)
other
hydroisomerization
reaction
selective
reduction
NO
x
ammonia
reaction).
Finally,
some
current
limitations
future
perspectives
on
challenge
opportunity
subject
pointed
out.
It
is
believed
that
review
will
inspire
more
innovative
research
synthesis
catalysis
promote
their
developments
meet
emerging
demands
practical
applications.
National Science Review,
Год журнала:
2021,
Номер
8(10)
Опубликована: Янв. 15, 2021
Abstract
Zeolites,
as
efficient
and
stable
catalysts,
are
widely
used
in
the
environmental
catalysis
field.
Typically,
Cu-SSZ-13
with
small-pore
structure
shows
excellent
catalytic
activity
for
selective
reduction
of
NOx
ammonia
(NH3-SCR)
well
high
hydrothermal
stability.
This
review
summarizes
major
advances
applied
to
NH3-SCR
reaction,
including
state
copper
species,
standard
fast
SCR
reaction
mechanism,
deactivation
poisoning
resistance
synthetic
methodology.
The
gives
a
valuable
summary
new
insights
into
matching
between
catalyst
design
principles
characteristics
Cu2+-exchanged
zeolitic
highlighting
significant
opportunity
presented
by
zeolite-based
catalysts.
Principles
designing
zeolites
performance
stability
proposed.
On
basis
these
principles,
more
hydrothermally
Cu-AEI
Cu-LTA
elaborated
other
alternative
NH3-SCR.
Finally,
we
call
attention
challenges
facing
Cu-based
that
still
need
be
addressed.
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(13), С. 7197 - 7204
Опубликована: Янв. 6, 2021
Abstract
Cu‐CHA
is
the
state‐of‐the‐art
catalyst
for
Selective
Catalytic
Reduction
(SCR)
of
NOx
in
vehicle
applications.
Although
extensively
studied,
diverse
mechanistic
proposals
still
stand
terms
nature
active
Cu‐ions
and
reaction
pathways
SCR
working
conditions.
Herein
we
address
redox
mechanism
underlying
Low‐Temperature
(LT)
on
by
an
integration
chemical‐trapping
techniques,
transient‐response
methods,
operando
UV/Vis‐NIR
spectroscopy
with
modelling
tools
based
transient
kinetic
analysis
density
functional
theory
calculations.
We
show
that
rates
Half‐Cycle
(RHC)
LT‐SCR
display
a
quadratic
dependence
Cu
II
,
thus
questioning
mechanisms
isolated
‐ions.
propose,
instead,
‐pair
mediated
LT‐RHC
pathway,
which
NO
oxidative
activation
to
mobile
nitrite‐precursor
intermediates
accounts
reduction.
These
results
highlight
role
dinuclear
complexes
not
only
oxidation
part
LT‐SCR,
but
also
RHC
cascade.
Advanced Materials,
Год журнала:
2023,
Номер
35(40)
Опубликована: Июнь 26, 2023
Artificial
photosynthetic
diluted
CO2
reduction
directly
driven
by
natural
sunlight
is
a
challenging,
but
promising
way
to
realize
carbon-resources
recycling
utilization.
Herein,
three-in-one
photocatalytic
system
of
enrichment,
and
H2
O
oxidation
sites
designed
for
reduction.
A
Zn-Salen-based
covalent
organic
framework
(Zn-S-COF)
with
reductive
synthesized;
then,
ionic
liquids
(ILs)
are
loaded
into
the
pores.
As
result,
[Emim]BF4
@Zn-S-COF
shows
visible-light-driven
-to-CO
conversion
rate
105.88
µmol
g-1
h-1
under
(15%)
atmosphere,
even
superior
than
most
photocatalysts
in
high
concentrations
.
Moreover,
also
reaches
126.51
5
h.
Further
experiments
theoretical
calculations
reveal
that
triazine
ring
Zn-S-COF
promotes
activity
sites,
ILs
provide
an
enriched
realizing
efficient
Nature Communications,
Год журнала:
2022,
Номер
13(1)
Опубликована: Авг. 8, 2022
Commercial
Cu-exchanged
small-pore
SSZ-13
(Cu-SSZ-13)
zeolite
catalysts
are
highly
active
for
the
standard
selective
catalytic
reduction
(SCR)
of
NO
with
NH
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
146(1), С. 289 - 297
Опубликована: Дек. 22, 2023
Copper
(Cu),
with
the
advantage
of
producing
a
deep
reduction
product,
is
unique
catalyst
for
electrochemical
CO2
(CO2RR).
Designing
Cu-based
to
trigger
CO2RR
multicarbon
product
and
understanding
accurate
structure–activity
relationship
elucidating
reaction
mechanisms
still
remain
challenge.
Herein,
we
demonstrate
rational
design
core–shell
structured
silica-copper
(p-Cu@m-SiO2)
through
Cu–Si
direct
bonding
efficient
selective
CO2RR.
The
interface
fulfills
inversion
in
selectivity.
ratio
C2H4/CH4
changes
from
0.6
14.4
after
silica
modification,
current
density
reaches
high
up
450
mA
cm–2.
kinetic
isotopic
effect,
situ
attenuated
total
reflection
Fourier-transform
infrared
spectra,
functional
theory
were
applied
elucidate
mechanism.
SiO2
shell
stabilizes
*H
intermediate
by
forming
Si–O–H
inhibits
hydrogen
evolution
effectively.
Moreover,
direct-bonded
makes
bare
Cu
sites
larger
charge
density.
Such
stabilized
*CHO
activated
*CO,
promoting
coupling
*CO
intermediates
form
C2H4.
This
work
provides
promising
strategy
designing
catalysts
C2H4
catalytic
activity.