Abstract
Using
electrochemical
water
splitting
to
produce
hydrogen
is
still
a
grand
challenge
due
the
lack
of
economical
and
efficient
Pt‐free
catalysts.
Herein,
single‐atom
Ru
supported
on
MoS
2
(SA‐Ru‐MoS
)
electrocatalyst
for
evolution
reaction
(HER)
reported.
Results
indicate
that
doping
induces
phase
transition
generation
S
vacancies,
which
significantly
improve
performance
inert
2D
HER.
In
particular,
SA‐Ru‐MoS
exhibits
low
overpotential
76
mV
at
10
mA
cm
−2
in
alkaline
media,
superior
most
electrocatalysts
previously
reported
literature.
Combining
experimental
results
with
density
functional
theory
(DFT)
calculations,
it
further
revealed
origin
high
HER
activity
mainly
attributed
synergy
effects
vacancies
local
structure
,
efficiently
tailors
electronic
extremely
reduces
energy
barrier
Volmer
step
adsorption/desorption
H*
intermediate
step.
short,
this
work
provides
strategy
transfer
into
highly
electrocatalysts.
Chemical Reviews,
Год журнала:
2023,
Номер
123(9), С. 6257 - 6358
Опубликована: Март 21, 2023
The
oxygen
evolution
reaction
(OER)
and
reduction
(ORR)
are
core
steps
of
various
energy
conversion
storage
systems.
However,
their
sluggish
kinetics,
i.e.,
the
demanding
multielectron
transfer
processes,
still
render
OER/ORR
catalysts
less
efficient
for
practical
applications.
Moreover,
complexity
catalyst–electrolyte
interface
makes
a
comprehensive
understanding
intrinsic
mechanisms
challenging.
Fortunately,
recent
advances
in
situ/operando
characterization
techniques
have
facilitated
kinetic
monitoring
under
conditions.
Here
we
provide
selected
highlights
mechanistic
studies
with
main
emphasis
placed
on
heterogeneous
systems
(primarily
discussing
first-row
transition
metals
which
operate
basic
conditions),
followed
by
brief
outlook
molecular
catalysts.
Key
sections
this
review
focused
determination
true
active
species,
identification
sites,
reactive
intermediates.
For
in-depth
insights
into
above
factors,
short
overview
metrics
accurate
characterizations
is
provided.
A
combination
obtained
time-resolved
information
reliable
activity
data
will
then
guide
rational
design
new
Strategies
such
as
optimizing
restructuring
process
well
overcoming
adsorption-energy
scaling
relations
be
discussed.
Finally,
pending
current
challenges
prospects
toward
development
homogeneous
presented.
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
Advanced Materials,
Год журнала:
2020,
Номер
32(48)
Опубликована: Окт. 19, 2020
Abstract
Developing
a
scalable
approach
to
construct
efficient
and
multifunctional
electrodes
for
the
hydrogen
evolution
reaction
(HER),
oxygen
(OER),
reduction
(ORR)
is
an
urgent
need
overall
water
splitting
zinc–air
batteries.
In
this
work,
freestanding
3D
heterostructure
film
synthesized
from
Ni‐centered
metal−organic
framework
(MOF)/graphene
oxide.
During
pyrolysis
process,
1D
carbon
nanotubes
formed
MOF
link
with
2D
reduced
graphene
oxide
sheets
stitch
film.
The
results
of
experiments
theoretical
calculations
show
that
synergistic
effect
N‐doped
shell
Ni
nanoparticles
leads
optimized
excellent
electrocatalytic
activity.
Low
overpotentials
95
260
mV
are
merely
needed
HER
OER,
respectively,
reach
current
density
10
mA
cm
−2
.
addition,
high
half‐wave
potential
0.875
V
obtained
ORR,
which
comparable
Pt/RuO
2
ranks
among
top
non‐noble‐metal
catalysts.
use
“all‐in‐one”
as
electrode
performance
homemade
electrolyzer
battery,
indicating
practical
applications.
Abstract
As
a
typical
class
of
single‐atom
catalysts
(SACs)
possessing
prominent
advantages
high
reactivity,
selectivity,
stability,
and
maximized
atomic
utilization,
emerging
metal‐nitrogen‐doped
carbon
(M‐N‐C)
materials,
wherein
dispersive
metal
atoms
are
coordinated
to
nitrogen
doped
in
nanomaterials,
have
presented
promise
replace
the
conventional
or
oxides‐based
catalysts.
In
this
work,
recent
progress
M‐N‐C‐based
materials
achieved
both
theoretical
experimental
investigations
is
summarized
general
principles
for
novel
design
from
electronic
structure
modulating
provided.
Firstly,
applications
mechanisms
on
challenges
variety
sustainable
fuel
generation
bioinspired
reactions,
including
oxygen
reduction
reaction
(ORR),
evolution
(OER),
hydrogen
(HER),
dioxide
(CO
2
RR),
(NRR),
nanozyme
reactions
reviewed.
Then,
strategies
toward
enhancing
catalytic
performance
by
engineering
nature
ion
centers,
coordinative
environment
active
support,
their
synergistic
cooperation,
proposed.
Finally,
prospects
rational
next
high‐performance
outlined.
It
expected
that
work
will
provide
insights
into
innovation
environmental
technologies.
Advanced Functional Materials,
Год журнала:
2021,
Номер
31(16)
Опубликована: Фев. 17, 2021
Abstract
Electrochemical
water
splitting
is
a
critical
energy
conversion
process
for
producing
clean
and
sustainable
hydrogen;
this
relies
on
low‐cost,
highly
active,
durable
oxygen
evolution
reaction/hydrogen
reaction
electrocatalysts.
Metal
cations
(including
transition
metal
noble
cations),
particularly
high‐valence
that
show
high
catalytic
activity
can
serve
as
the
main
active
sites
in
electrochemical
processes,
have
received
special
attention
developing
advanced
In
review,
heterogenous
electrocatalyst
design
strategies
based
are
presented,
associated
materials
designed
summarized.
discussion,
emphasis
given
to
combined
with
modulation
of
phase/electronic/defect
structure
performance
improvement.
Specifically,
importance
using
situ
operando
techniques
track
real
metal‐based
during
highlighted.
Remaining
challenges
future
research
directions
also
proposed.
It
expected
comprehensive
discussion
electrocatalysts
containing
be
instructive
further
explore
other
energy‐related
reactions.
Advanced Energy Materials,
Год журнала:
2022,
Номер
12(24)
Опубликована: Май 1, 2022
Abstract
Oxygen
evolution
reaction
(OER),
as
a
relevant
half
for
water
splitting
to
address
the
energy
crisis,
has
captured
great
deal
of
attention.
However,
this
technology
always
been
impeded
by
lack
highly
efficient
and
stable
electrocatalyst.
Amorphous
materials,
which
possess
long‐range
disorder
only
short‐range
order
over
few
atoms,
are
often
superior
their
crystalline
counterparts
in
electrocatalysis
owing
more
active
sites,
broader
chemical
composition
range,
structural
flexibility.
This
review
first
introduces
some
assessment
criteria
OER
then
presents
theoretical
modeling
mechanisms
state‐of‐the‐art
amorphous
transition
metal‐based
electrocatalysts,
involving
oxides,
hydroxides,
sulfides,
phosphides,
borides,
composites,
well
practical
applications
OER.
Finally,
recent
development,
existing
challenges,
future
perspectives
electrocatalysts
discussed.
paper
offers
valuable
guidance
designing
applications.
Advanced Materials,
Год журнала:
2021,
Номер
34(11)
Опубликована: Ноя. 30, 2021
Design
and
construction
of
low-cost
electrocatalysts
with
high
catalytic
activity
long-term
stability
is
a
challenging
task
in
the
field
catalysis.
Metal-organic
frameworks
(MOF)
are
promising
candidates
as
precursor
materials
development
highly
efficient
for
energy
conversion
storage
applications.
This
review
starts
summary
basic
concepts
key
evaluation
parameters
involved
electrochemical
water-splitting
reaction.
Then,
different
synthesis
approaches
reported
cobalt-based
Zeolitic
imidazolate
framework
(ZIF-67)
its
derivatives
critically
reviewed.
Additionally,
several
strategies
employed
to
enhance
electrocatalytic
ZIF-67-based
discussed
detail.
The
present
provides
succinct
insight
into
ZIF-67
(oxides,
hydroxides,
sulfides,
selenides,
phosphide,
nitrides,
telluride,
heteroatom/metal-doped
carbon,
noble
metal-supported
derivatives)
oxygen
evolution
reaction
(OER),
hydrogen
(HER),
overall
water
splitting
Finally,
this
concludes
associated
challenges
perspectives
on
developing
best
economic,
durable
materials.
Advanced Energy Materials,
Год журнала:
2020,
Номер
10(41)
Опубликована: Сен. 27, 2020
Abstract
Developing
nonprecious
electrocatalysts
via
a
cost‐effective
methods
to
synergistically
achieve
high
active
sites
exposure
and
optimized
intrinsic
activity
remains
grand
challenge.
Here
low‐cost
scaled‐up
chemical
etching
method
is
developed
for
transforming
nickel
foam
(NF)
into
highly
electrocatalyst
both
the
hydrogen
evolution
reaction
(HER)
oxygen
(OER).
The
synthetic
involves
Na
2
S‐induced
of
NF
in
presence
Fe,
leading
growth
ultrathin
Fe‐doped
Ni
3
S
arrays
on
substrate
(Fe
x
3‐
@
NF).
combined
experimental
theoretical
investigations
reveal
that
incorporated
Fe
cations
significantly
modulate
morphology
surface
electron
density
,
thus
boost
electrochemically
area,
transfer,
optimize
hydrogen/water
absorption
free
energy.
0.9
2.1
requires
overpotentials
only
72
mV
at
10
mA
cm
−2
HER
252
100
OER
1.0
m
KOH,
respectively,
enabling
an
alkaline
electrolyzer
low
cell
voltage
1.51
V
drive
overall
water
splitting.
More
broadly,
this
approach
very
versatile
can
be
used
synthesize
other
metal
sulfides
(e.g.,
Fe–Cu–S,
Fe–Al–S,
Fe–Ti–S).