National Science Review,
Год журнала:
2022,
Номер
10(2)
Опубликована: Окт. 4, 2022
ABSTRACT
A
major
impediment
to
industrial
urea
synthesis
is
the
lack
of
catalysts
with
high
selectivity
and
activity,
which
inhibits
efficient
production
urea.
Here,
we
report
a
new
catalyst
system
suitable
for
highly
selective
by
in
situ
growth
graphdiyne
on
surface
cobalt–nickel
mixed
oxides.
Such
multi-heterojunction
interfacial
structure
resulting
obvious
incomplete
charge-transfer
phenomenon
between
metal
oxide
interface
multiple
intermolecular
interactions.
These
intrinsic
characteristics
are
origin
performance
catalyst.
Studies
mechanism
reveal
that
could
effectively
optimize
adsorption/desorption
capacities
intermediate
promote
direct
C–N
coupling
significantly
suppressing
by-product
reactions
toward
formation
H2,
CO,
N2
NH3.
The
can
selectively
synthesize
directly
from
nitrite
carbon
dioxide
water
at
room
temperature
pressure,
exhibits
record-high
Faradaic
efficiency
64.3%,
nitrogen
(Nurea-selectivity)
86.0%,
(Curea-selectivity)
∼100%,
as
well
yield
rates
913.2
μg
h−1
mgcat−1
remarkable
long-term
stability.
Chemical Reviews,
Год журнала:
2022,
Номер
122(11), С. 10087 - 10125
Опубликована: Апрель 21, 2022
Metal–organic
frameworks
(MOFs)
have
recently
emerged
as
ideal
electrode
materials
and
precursors
for
electrochemical
energy
storage
conversion
(EESC)
owing
to
their
large
specific
surface
areas,
highly
tunable
porosities,
abundant
active
sites,
diversified
choices
of
metal
nodes
organic
linkers.
Both
MOF-based
MOF-derived
in
powder
form
been
widely
investigated
relation
synthesis
methods,
structure
morphology
controls,
performance
advantages
targeted
applications.
However,
engage
them
applications,
both
binders
additives
would
be
required
postprocessed
electrodes,
fundamentally
eliminating
some
the
sites
thus
degrading
superior
effects
MOF-based/derived
materials.
The
advancement
freestanding
electrodes
provides
a
new
promising
platform
EESC
thanks
apparent
merits,
including
fast
electron/charge
transmission
seamless
contact
between
current
collectors.
Benefiting
from
synergistic
effect
structures
materials,
outstanding
can
achieved,
stimulating
increasing
enthusiasm
recent
years.
This
review
timely
comprehensive
overview
on
structural
features
fabrication
techniques
electrodes.
Then,
latest
advances
are
summarized
devices
electrocatalysis.
Finally,
insights
into
currently
faced
challenges
further
perspectives
these
feasible
solutions
discussed,
aiming
at
providing
set
guidance
promote
development
scale-up
production
commercial
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(35), С. 19068 - 19073
Опубликована: Июнь 17, 2021
Abstract
Highly
efficient
electrocatalysts
are
essential
for
the
production
of
green
hydrogen
from
water
electrolysis.
Herein,
a
metal‐organic
framework‐assisted
pyrolysis‐replacement‐reorganization
approach
is
developed
to
obtain
ultrafine
Pt‐Co
alloy
nanoparticles
(sub‐10
nm)
attached
on
inner
and
outer
shells
porous
nitrogen‐doped
carbon
nanotubes
(NCNT)
with
closed
ends.
During
thermal
reorganization,
migration
nano‐alloys
both
surfaces
ensures
maximized
exposure
active
sites
while
maintaining
robust
attachment
matrix.
Density
functional
theory
calculations
suggest
nearly
thermodynamically‐neutral
free
energy
adsorption
intermediates
diversified
induced
by
alloying,
thus
resulting
in
great
promotion
intrinsic
activity
towards
evolution
reaction
(HER).
Benefiting
delicate
structural
design
compositional
modulation,
optimized
Pt
3
Co@NCNT
electrocatalyst
manifests
outstanding
HER
superior
stability
acidic
alkaline
media.
Nano-Micro Letters,
Год журнала:
2021,
Номер
13(1)
Опубликована: Июнь 1, 2021
The
core
reactions
for
fuel
cells,
rechargeable
metal-air
batteries,
and
hydrogen
production
are
the
oxygen
reduction
reaction
(ORR),
evolution
(OER),
(HER),
which
heavily
dependent
on
efficiency
of
electrocatalysts.
Enormous
attempts
have
previously
been
devoted
in
non-noble
electrocatalysts
born
out
metal-organic
frameworks
(MOFs)
ORR,
OER,
HER
applications,
due
to
following
advantageous
reasons:
(i)
significant
porosity
eases
electrolyte
diffusion;
(ii)
supreme
catalyst-electrolyte
contact
area
enhances
diffusion
efficiency;
(iii)
electronic
conductivity
can
be
extensively
increased
owing
unique
construction
block
subunits
MOFs-derived
electrocatalysis.
Herein,
recent
progress
including
synthesis
protocols,
design
engineering,
DFT
calculations
roles,
energy
applications
is
discussed
reviewed.
It
concluded
that
elevated
performances
attributed
an
advantageously
well-designed
high-porosity
structure,
surface
area,
plentiful
active
centers.
Furthermore,
perspectives
MOF-derived
presented.
Advanced Functional Materials,
Год журнала:
2021,
Номер
31(42)
Опубликована: Июль 20, 2021
Abstract
The
great
interest
in
rechargeable
Zn–air
batteries
(ZABs)
arouses
extensive
research
on
low‐cost,
high‐active,
and
durable
bifunctional
electrocatalysts
to
boost
the
sluggish
oxygen
reduction
reaction
(ORR)
evolution
(OER).
It
remains
a
challenge
simultaneously
host
high‐active
independent
ORR
OER
sites
single
catalyst.
Herein
dual‐phasic
carbon
nanoarchitecture
consisting
of
single‐atom
phase
for
nanosized
is
proposed.
Specifically,
Co
atoms
supported
nanotubes
(single‐atom
phase)
encapsulated
zeolitic‐imidazole‐framework‐derived
polyhedron
(nanosized
are
integrated
together
via
nanotube
bridges.
obtained
catalyst
shows
small
overpotential
difference
0.74
V
between
potential
at
10
mA
cm
−2
half‐wave
potential.
ZAB
based
demonstrates
large
power
density
172
mW
.
Furthermore,
it
charge‐discharge
gap
0.51
5
outstanding
discharge‐charge
cycling
durability.
This
study
provides
feasible
design
concept
achieve
multifunctional
catalysts
promotes
development
ZABs.
Rechargeable
zinc-air
batteries
call
for
high-performance
bifunctional
oxygen
electrocatalysts.
Transition
metal
single-atom
catalysts
constitute
a
promising
candidate
considering
their
maximum
atom
efficiency
and
high
intrinsic
activity.
However,
the
fabrication
of
atomically
dispersed
transition
sites
is
highly
challenging,
creating
need
new
design
strategies
synthesis
methods.
Here,
clicking
confinement
strategy
proposed
to
efficiently
predisperse
transitional
atoms
in
precursor
directed
by
click
chemistry
ensure
successful
construction
abundant
sites.
Concretely,
cobalt-coordinated
porphyrin
units
are
covalently
clicked
on
substrate
cobalt
affording
Co-N-C
electrocatalyst.
The
electrocatalyst
exhibits
impressive
electrocatalytic
performances
with
an
activity
indicator
Δ
E
0.79
V.
This
work
extends
approach
prepare
efficient
electrocatalysis
inspires
methodology
precise
catalytic
materials.
Chemical Reviews,
Год журнала:
2022,
Номер
122(24), С. 17241 - 17338
Опубликована: Ноя. 1, 2022
Current
energy
and
environmental
challenges
demand
the
development
design
of
multifunctional
porous
materials
with
tunable
properties
for
catalysis,
water
purification,
conversion
storage.
Because
their
amenability
to
de
novo
reticular
chemistry,
metal-organic
frameworks
(MOFs)
have
become
key
in
this
area.
However,
usefulness
is
often
limited
by
low
chemical
stability,
conductivity
inappropriate
pore
sizes.
Conductive
two-dimensional
(2D)
robust
structural
skeletons
and/or
functionalized
surfaces
can
form
stabilizing
interactions
MOF
components,
enabling
fabrication
nanocomposites
characteristics.
Graphene
its
functional
derivatives
are
largest
class
2D
possess
remarkable
compositional
versatility,
diversity,
controllable
surface
chemistry.
Here,
we
critically
review
current
knowledge
concerning
growth,
structure,
graphene
derivatives,
MOFs,
graphene@MOF
composites
as
well
associated
structure-property-performance
relationships.
Synthetic
strategies
preparing
tuning
also
comprehensively
reviewed
together
applications
gas
storage/separation,
catalysis
(organo-,
electro-,
photocatalysis),
electrochemical
storage
conversion.
hybrids
practical
addressed,
revealing
areas
future
investigation.
We
hope
that
will
inspire
further
exploration
new
energy,
electronic,
biomedical,
photocatalysis
studies
on
previously
unreported
known
reveal
potential
"diamonds
rough".
eScience,
Год журнала:
2023,
Номер
3(2), С. 100092 - 100092
Опубликована: Янв. 10, 2023
Micro/nano
metal–organic
frameworks
(MOFs)
have
attracted
significant
attention
in
recent
years
due
to
their
numerous
unique
properties,
with
many
synthetic
methods
and
strategies
being
reported
for
constructing
MOFs
specific
micro/nano
structures.
In
addition,
the
design
of
energy
storage
conversion
applications
study
structure–activity
relationship
also
become
research
hotspots.
Herein,
a
comprehensive
overview
progress
on
is
presented.
We
begin
brief
introduction
various
synthesis
controlling
morphology
MOFs.
Subsequently,
structure-dependent
properties
as
electrode
materials
or
catalysts
terms
batteries,
supercapacitors,
catalysis
are
discussed.
Finally,
remaining
challenges
future
perspectives
this
field
Overall,
review
expected
inspire
advanced
efficient
technologies.