Advanced Functional Materials,
Год журнала:
2022,
Номер
33(4)
Опубликована: Ноя. 30, 2022
Abstract
Designing
high‐performance
and
cost‐effective
electrocatalysts
for
water
splitting
at
high
current
density
is
pivotal
practical
industrial
applications.
Herein,
it
found
that
atomic‐level
surface
engineering
of
self‐supported
nickel
phosphide
(NiP)
nanoarrays
via
a
facile
cation‐exchange
method
can
substantially
regulate
the
chemical
physical
properties
catalysts
by
introducing
Co
atoms.
Such
surface‐engineered
Ni
x
1–x
P
endows
several
aspects
merits:
i)
rough
nanosheet
array
electrode
structure
accessible
to
diffusion
electrolytes
release
gas
bubbles,
ii)
enriched
vacancies
companied
doping
thus
increased
active
sites,
iii)
synergy
5
4
NiP
2
beneficial
catalytic
activity
enhancement.
By
virtue
finely
controlling
contents,
optimal
0.96
0.04
achieves
remarkable
bifunctional
electrocatalytic
performance
overall
large
1000
mA
cm
−2
,
showing
overpotentials
249.7
mV
hydrogen
evolution
reaction
281.7
oxygen
reaction.
Furthermore,
500
exhibits
an
ultralow
potential
(1.71
V)
ultralong
durability
(500
h)
splitting.
This
study
implies
materials
offers
viable
route
gaining
density.
Advanced Materials,
Год журнала:
2021,
Номер
33(17)
Опубликована: Март 22, 2021
Abstract
Electrochemical
water
splitting
has
attracted
significant
attention
as
a
key
pathway
for
the
development
of
renewable
energy
systems.
Fabricating
efficient
electrocatalysts
these
processes
is
intensely
desired
to
reduce
their
overpotentials
and
facilitate
practical
applications.
Recently,
metal–organic
framework
(MOF)
nanoarchitectures
featuring
ultrahigh
surface
areas,
tunable
nanostructures,
excellent
porosities
have
emerged
promising
materials
highly
active
catalysts
electrochemical
splitting.
Herein,
most
pivotal
advances
in
recent
research
on
engineering
MOF
are
presented.
First,
design
catalytic
centers
MOF‐based/derived
summarized
compared
from
aspects
chemical
composition
optimization
structural
functionalization
at
atomic
molecular
levels.
Subsequently,
fast‐growing
breakthroughs
activities,
identification
sites,
fundamental
mechanisms
thoroughly
discussed.
Finally,
comprehensive
commentary
current
primary
challenges
future
perspectives
its
commercialization
hydrogen
production
provided.
Hereby,
new
insights
into
synthetic
principles
electrocatalysis
designing
utilization
offered,
thus
further
promoting
prosperity
wide
range
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(41), С. 22513 - 22521
Опубликована: Авг. 13, 2021
Abstract
We
synthesized
a
series
of
carbon‐supported
atomic
metal‐N‐C
catalysts
(M‐SACs:
M=Mn,
Fe,
Co,
Ni,
Cu)
with
similar
structural
and
physicochemical
properties
to
uncover
their
catalytic
activity
trends
mechanisms.
The
peroxymonosulfate
(PMS)
are
Fe‐SAC>Co‐SAC>Mn‐SAC>Ni‐SAC>Cu‐SAC,
Fe‐SAC
displays
the
best
single‐site
kinetic
value
(1.65×10
5
min
−1
mol
)
compared
other
species.
First‐principles
calculations
indicate
that
most
reasonable
reaction
pathway
for
1
O
2
production
is
PMS→OH*→O*→
;
M‐SACs
exhibit
moderate
near‐average
Gibbs
free
energies
in
each
step
have
better
activity,
which
key
outstanding
performance
Fe‐SACs.
This
study
gives
atomic‐scale
understanding
fundamental
mechanisms
PMS‐assisted
reactive
oxygen
species
via
M‐SACs,
thus
providing
guidance
developing
organic
pollutant
degradation.
RSC Advances,
Год журнала:
2023,
Номер
13(6), С. 3843 - 3876
Опубликована: Янв. 1, 2023
Electrochemical
splitting
of
water
is
an
appealing
solution
for
energy
storage
and
conversion
to
overcome
the
reliance
on
depleting
fossil
fuel
reserves
prevent
severe
deterioration
global
climate.
Though
there
are
several
cells,
hydrogen
(H
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(41), С. 22276 - 22282
Опубликована: Авг. 24, 2021
Abstract
Designing
definite
metal‐support
interfacial
bond
is
an
effective
strategy
for
optimizing
the
intrinsic
activity
of
noble
metals,
but
rather
challenging.
Herein,
a
series
quantum‐sized
metal
nanoparticles
(NPs)
anchored
on
nickel
metal–organic
framework
nanohybrids
(M@Ni‐MOF,
M=Ru,
Ir,
Pd)
are
rationally
developed
through
spontaneous
redox
strategy.
The
metal‐oxygen
bonds
between
NPs
and
Ni‐MOF
guarantee
structural
stability
sufficient
exposure
surface
active
sites.
More
importantly,
such
precise
feature
can
effectively
modulate
electronic
structure
hybrids
charge
transfer
formed
Ni‐O‐M
bridge
then
improves
reaction
kinetics.
As
result,
representative
Ru@Ni‐MOF
exhibits
excellent
hydrogen
evolution
(HER)
at
all
pH
values,
even
superior
to
commercial
Pt/C
recent
noble‐metal
catalysts.
Theoretical
calculations
deepen
mechanism
understanding
HER
performance
optimized
adsorption
free
energies
water
due
interfacial‐bond‐induced
electron
redistribution.
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
Advanced Materials,
Год журнала:
2023,
Номер
35(31)
Опубликована: Фев. 23, 2023
Single/dual-metal
atoms
supported
on
carbon
matrix
can
be
modulated
by
coordination
structure
and
neighboring
active
sites.
Precisely
designing
the
geometric
electronic
uncovering
structure-property
relationships
of
single/dual-metal
confront
with
grand
challenges.
Herein,
this
review
summarizes
latest
progress
in
microenvironment
engineering
single/dual-atom
sites
via
a
comprehensive
comparison
single-atom
catalyst
(SACs)
dual-atom
catalysts
(DACs)
term
design
principles,
modulation
strategy,
theoretical
understanding
structure-performance
correlations.
Subsequently,
recent
advances
several
typical
electrocatalysis
process
are
discussed
to
get
general
reaction
mechanisms
finely-tuned
SACs
DACs.
Finally,
full-scaled
summaries
challenges
prospects
given
for
This
will
provide
new
inspiration
development
atomically
dispersed
electrocatalytic
application.
Chemical Reviews,
Год журнала:
2023,
Номер
123(9), С. 5347 - 5420
Опубликована: Апрель 12, 2023
Enzymatic
catalysis
has
fueled
considerable
interest
from
chemists
due
to
its
high
efficiency
and
selectivity.
However,
the
structural
complexity
vulnerability
hamper
application
potentials
of
enzymes.
Driven
by
practical
demand
for
chemical
conversion,
there
is
a
long-sought
quest
bioinspired
catalysts
reproducing
even
surpassing
functions
natural
As
nanoporous
materials
with
surface
areas
crystallinity,
metal-organic
frameworks
(MOFs)
represent
an
exquisite
case
how
enzymes
their
active
sites
are
integrated
into
porous
solids,
affording
heterogeneous
superior
stability
customizable
structures.
In
this
review,
we
comprehensively
summarize
advances
MOFs
catalysis,
discuss
design
principle
various
MOF-based
catalysts,
such
as
MOF-enzyme
composites
embedded
sites,
explore
utility
these
in
different
reactions.
The
advantages
enzyme
mimetics
also
highlighted,
including
confinement,
templating
effects,
functionality,
comparison
homogeneous
supramolecular
catalysts.
A
perspective
provided
potential
solutions
addressing
current
challenges
MOF
catalysis.
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.
Advanced Functional Materials,
Год журнала:
2021,
Номер
31(31)
Опубликована: Май 13, 2021
Abstract
In
human
systems,
reactive
oxygen
species
(ROS)
significantly
affect
different
physiological
activities
and
play
critical
roles
in
diverse
living
processes.
It
is
widely
known
that
excessive
ROS
generation
inflammatory
tissues
can
further
deteriorate
the
localized
tissue
injury
cause
chronic
diseases.
Though
promising
for
reducing
levels,
many
antioxidant
molecules
natural
enzymes
suffer
from
abundant
intrinsic
limitations.
Recently,
a
series
of
biocatalytic
or
nanostructures
have
been
designed
with
distinctive
scavenging
capabilities,
which
show
to
overcome
these
kernel
challenges.
this
timely
review,
most
recent
advances
engineering
are
summarized.
First,
principles
corresponding
methods
testing
various
enzymatic
carefully
concluded.
Subsequently,
rationally
high
efficiencies
comprehensively
discussed,
especially
on
catalytic
activities,
mechanisms,
structure‐function
relationships.
After
that,
representative
applications
biotherapeutics
summarized
detail.
At
last,
primary
challenges
future
perspectives
emerging
research
frontier
also
outlined.
believed
progress
review
will
offer
cutting‐edge
understanding
guidance
high‐performance
broad
biotherapeutic
applications.