Chemical Science,
Год журнала:
2021,
Номер
12(16), С. 5737 - 5766
Опубликована: Янв. 1, 2021
This
review
summarizes
comprehensively
the
latest
methods
of
synthesizing
MOFs/graphene
and
their
derivatives,
application
in
energy
storage
conversion
with
a
detailed
analysis
structure–property
relationship.
Advanced Functional Materials,
Год журнала:
2021,
Номер
31(20)
Опубликована: Март 10, 2021
Abstract
Efficient
oxygen
reduction
reaction
(ORR)
and
evolution
(OER)
processes
highly
rely
on
the
rational
design
synthesis
of
high‐performance
electrocatalysts.
Herein,
comprehensive
characterizations
density
functional
theory
(DFT)
calculations
are
combined
to
verify
important
roles
crystallinity
vacancy
levels
Co(II)
oxide
(CoO)
ORR
OER
activities.
A
facile
controllable
vacuum‐calcination
strategy
is
utilized
convert
Co(OH)
2
into
oxygen‐defective
amorphous‐crystalline
CoO
(namely
ODAC‐CoO)
nanosheets.
With
carefully
controlled
levels,
optimal
ODAC‐CoO
sample
exhibits
dramatically
enhanced
electrocatalytic
activities
compared
with
pure
crystalline
counterpart.
The
assembled
liquid
quasi‐solid‐state
Zn–air
batteries
as
cathode
material
achieve
remarkable
specific
capacity,
power
density,
excellent
cycling
stability,
outperforming
benchmark
Pt/C
+
IrO
catalysts.
This
study
theoretically
proposes
experimentally
demonstrates
that
simultaneous
introduction
amorphous
structures
vacancies
could
be
an
effective
avenue
towards
OER.
Advanced Materials,
Год журнала:
2022,
Номер
34(16)
Опубликована: Фев. 22, 2022
Electrocatalytic
hydrogen
peroxide
(H2
O2
)
synthesis
via
the
two-electron
oxygen
reduction
reaction
(2e
ORR)
pathway
is
becoming
increasingly
important
due
to
green
production
process.
Here,
cationic
vacancies
on
nickel
phosphide,
as
a
proof-of-concept
regulate
catalyst's
physicochemical
properties,
are
introduced
for
efficient
H2
electrosynthesis.
The
as-fabricated
Ni
(VNi
)-enriched
Ni2-x
P-VNi
electrocatalyst
exhibits
remarkable
2e
ORR
performance
with
molar
fraction
of
>95%
and
Faradaic
efficiencies
>90%
in
all
pH
conditions
under
wide
range
applied
potentials.
Impressively,
as-created
VNi
possesses
superb
long-term
durability
over
50
h,
suppassing
recently
reported
catalysts
Operando
X-ray
absorption
near-edge
spectroscopy
(XANES)
synchrotron
Fourier
transform
infrared
(SR-FTIR)
combining
theoretical
calculations
reveal
that
excellent
catalytic
originates
from
-induced
geometric
electronic
structural
optimization,
thus
promoting
adsorption
favored
"end-on"
configuration.
It
believed
demonstrated
cation
vacancy
engineering
an
effective
strategy
toward
creating
active
heterogeneous
atomic
precision.
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
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 Materials,
Год журнала:
2022,
Номер
34(12)
Опубликована: Янв. 11, 2022
Rational
exploration
of
efficient,
inexpensive,
and
robust
electrocatalysts
is
critical
for
the
efficient
water
splitting.
Conjugated
conductive
metal-organic
frameworks
(cMOFs)
with
multicomponent
layered
double
hydroxides
(LDHs)
to
construct
bifunctional
heterostructure
catalysts
are
considered
as
an
but
complicated
strategy.
Here,
fabrication
a
cMOF/LDH
hetero-nanotree
array
catalyst
(CoNiRu-NT)
coupled
monodispersed
ruthenium
(Ru)
sites
via
controllable
grafted-growth
strategy
reported.
Rich-amino
hexaiminotriphenylene
linkers
coordinate
LDH
nanotrunk
form
cMOF
nanobranches,
providing
numerous
anchoring
precisely
confine
stabilize
RuN4
sites.
Moreover,
reduced
Ru
moieties
facilitate
H2
O
adsorption
dissociation,
heterointerface
between
further
modifies
chemical
electronic
structures.
Optimized
CoNiRu-NT
displays
significant
increase
in
electrochemical
water-splitting
properties
alkaline
media,
affording
low
overpotentials
22
mV
at
10
mA
cm-2
255
20
hydrogen
evolution
reaction
oxygen
reaction,
respectively.
In
actual
system,
drives
overall
splitting
cell
voltage
1.47
V
reach
.
This
performance
comparable
that
pure
noble-metal-based
materials
superior
most
reported
MOF-based
catalysts.
Advanced Functional Materials,
Год журнала:
2021,
Номер
31(22)
Опубликована: Март 21, 2021
Abstract
Electron
transfer
between
metal‐oxides
and
supports
considerably
affects
the
oxidative
desulfurization
(ODS)
performance
of
catalysts,
while
this
is
far
from
being
well
understood.
Herein,
molybdenum
dioxide
with
oxygen
vacancies
(V
O
‐MoO
2
)
catalysts
derived
Mo‐based
metal‐organic
frameworks
are
anchored
on
electron‐rich
nitrogen‐doped
carbon
nanotubes
(NC)
to
obtain
excellent
ODS
activity
reusability.
Results
show
that
either
dibenzothiophene
(DBT)
or
4,6‐dimethyldibenzothiophene
(4,6‐DMDBT)
removed
100%
composite
catalyst
@NC)
within
40
min
reaction
when
cumene
hydroperoxide
chosen
as
an
oxidant.
After
five
cycles
reaction,
DBT
4,6‐DMDBT
removal
still
exceeded
99.5
95.0%,
respectively.
density
functional
theory
calculations
characterizations
confirm
strong
electron‐donating
effect
NC
V
can
promote
dispersion
reduce
bond
energy
MoO
bond,
leading
exposure
active
sites
enrichment
).
Furthermore,
interfacial
electrostatic
interaction
caused
by
electron
leaching
catalyst.
This
study
provides
a
versatile
strategy
constructing
electronic
metal‐oxide
support
via
anchoring
for
design
high‐performance
catalysts.
The
2D
nanosheets
of
metal–organic
frameworks
(MOFs)
have
recently
emerged
as
a
promising
material
that
makes
them
valuable
in
widespread
electrocatalytic
fields
due
to
their
atomic‐level
thickness,
abundant
active
sites,
and
large
surface
area.
Efficient
electrocatalysts
for
hydrogen
evolution
reaction
(HER),
oxygen
(OER),
overall
water
splitting
are
highly
desired
with
low
overpotentials
promote
the
industrial
applications
energy
conversion
devices.
MOF
nanostructures
provide
long‐term
stability
high
electrical
conductivity
enhance
catalyst
activity
durability.
This
review
briefly
summarizes
synthesis
HER/OER/water
splitting.
More
attention
is
focused
on
synthetic
strategies
derivatives.
catalytic
performance
superior
properties
these
materials
highlighted.
outperformance
originates
from
rational
design,
myriad
thickness.
current
future
challenges
this
field
scientific
perspectives
overcome
It
suggested
construction
can
develop
state‐of‐the‐art
electrocatalyst
environmental
division.