Journal of the American Chemical Society,
Год журнала:
2020,
Номер
142(17), С. 7765 - 7775
Опубликована: Апрель 13, 2020
Exploring
efficient
and
low-cost
electrocatalysts
for
hydrogen
evolution
reaction
(HER)
in
alkaline
media
is
critical
developing
anion
exchange
membrane
electrolyzers.
The
key
to
a
rational
catalyst
design
understanding
the
descriptors
that
govern
HER
activity.
Unfortunately,
principles
performance
remain
unclear
are
still
under
debate.
By
studying
at
series
of
NiCu
bimetallic
surfaces,
where
electronic
structure
modulated
by
ligand
effect,
we
demonstrate
activity
can
be
correlated
with
either
calculated
or
experimental-measured
d
band
center
(an
indicator
binding
energy)
via
volcano-type
relationship.
Such
correlation
indicates
descriptor
role
center,
this
hypothesis
further
supported
evidence
combining
Ni
Cu
produces
variety
adsorption
sites,
which
possess
near-optimal
energy.
Our
finding
broadens
applicability
theory
prediction
metal
may
offer
an
insightful
mechanism.
Advanced Materials,
Год журнала:
2021,
Номер
33(31)
Опубликована: Июнь 12, 2021
Abstract
Hydrogen
economy
has
emerged
as
a
very
promising
alternative
to
the
current
hydrocarbon
economy,
which
involves
process
of
harvesting
renewable
energy
split
water
into
hydrogen
and
oxygen
then
further
utilization
clean
fuel.
The
production
by
electrolysis
is
an
essential
prerequisite
with
zero
carbon
emission.
Among
various
technologies,
alkaline
splitting
been
commercialized
for
more
than
100
years,
representing
most
mature
economic
technology.
Here,
historic
development
overviewed,
several
critical
electrochemical
parameters
are
discussed.
After
that,
advanced
nonprecious
metal
electrocatalysts
that
recently
negotiating
evolution
reaction
(OER)
(HER)
discussed,
including
transition
oxides,
(oxy)hydroxides,
chalcogenides,
phosphides,
nitrides
OER,
well
alloys,
carbides
HER.
In
this
section,
particular
attention
paid
catalyst
synthesis,
activity
stability
challenges,
performance
improvement,
industry‐relevant
developments.
Some
recent
works
about
scaled‐up
novel
electrode
designs,
seawater
also
spotlighted.
Finally,
outlook
on
future
challenges
opportunities
offered,
potential
directions
speculated.
Chemical Society Reviews,
Год журнала:
2022,
Номер
51(11), С. 4583 - 4762
Опубликована: Янв. 1, 2022
Replacing
fossil
fuels
with
energy
sources
and
carriers
that
are
sustainable,
environmentally
benign,
affordable
is
amongst
the
most
pressing
challenges
for
future
socio-economic
development.
Journal of the American Chemical Society,
Год журнала:
2020,
Номер
142(27), С. 11901 - 11914
Опубликована: Июнь 15, 2020
The
oxygen
evolution
reaction
(OER)
is
the
performance-limiting
half
of
water
splitting,
which
can
be
used
to
produce
hydrogen
fuel
using
renewable
energies.
Whereas
a
number
transition
metal
oxides
and
oxyhydroxides
have
been
developed
as
promising
OER
catalysts
in
alkaline
medium,
mechanisms
on
these
are
not
well
understood.
Here
we
combine
electrochemical
situ
spectroscopic
methods,
particularly
operando
X-ray
absorption
Raman
spectroscopy,
study
mechanism
cobalt
oxyhydroxide
(CoOOH),
an
archetypical
unary
catalyst.
We
find
dominating
resting
state
catalyst
Co(IV)
species
CoO2.
Through
isotope
exchange
experiments,
discover
superoxide
active
intermediate
OER.
This
formed
concurrently
oxidation
CoOOH
Combing
electrokinetic
data,
identify
rate-determining
step
release
dioxygen
from
intermediate.
work
provides
important
experimental
fingerprints
new
mechanistic
perspectives
for
catalysts.
Chemical Society Reviews,
Год журнала:
2019,
Номер
48(9), С. 2518 - 2534
Опубликована: Янв. 1, 2019
Great
attention
has
been
recently
drawn
to
metal
oxide
electrocatalysts
for
electrocatalysis-based
energy
storage
and
conversion
devices.
To
find
the
optimal
electrocatalyst,
a
prerequisite
is
an
activity
metric
that
reasonably
evaluates
intrinsic
electrocatalytic
of
particular
catalyst.
The
commonly
defined
as
specific
which
current
per
unit
catalyst
surface
area.
Thus,
precise
assessment
highly
depends
on
reliable
measurement
area,
calls
knowledge
experimental
approaches
determining
areas
electrocatalysts.
This
tutorial
review
aims
summarize
analyze
measuring
evaluating
comparing
their
activities.
We
start
by
popular
metrics
estimation
highlighting
importance
surface-area-normalized
(i.e.
activity)
chemistry
analysis.
Second,
we
provide
some
general
guidelines
experimentally
electrochemically
active
area
(ECSA).
Third,
methods
detailed
procedure
each
method
explicitly
described
step-by-step
manual
guides
researchers
perform
measurement;
rationales
uncertainties
are
discussed
help
readers
justify
Next,
give
our
recommendations
selecting
rational
approach
electrocatalyst.
Lastly,
discuss
future
challenges
ECSA
present
exemplary
novel
technique.
Advanced Materials,
Год журнала:
2021,
Номер
33(20)
Опубликована: Март 25, 2021
Abstract
The
proton
exchange
membrane
(PEM)
water
electrolysis
is
one
of
the
most
promising
hydrogen
production
techniques.
oxygen
evolution
reaction
(OER)
occurring
at
anode
dominates
overall
efficiency.
Developing
active
and
robust
electrocatalysts
for
OER
in
acid
a
longstanding
challenge
PEM
electrolyzers.
Most
catalysts
show
unsatisfied
stability
under
strong
acidic
oxidative
conditions.
Such
also
leads
to
difficulties
better
understanding
mechanisms.
This
review
aims
provide
current
progress
on
mechanisms
acid,
analyze
strategies
enhance
both
activity
stability,
summarize
state‐of‐the‐art
acid.
First,
prevailing
are
reviewed
establish
physicochemical
structure–activity
relationships
guiding
design
highly
efficient
with
stable
performance.
reported
approaches
improve
activity,
from
macroview
microview,
then
discussed.
To
problem
instability,
key
factors
affecting
catalyst
summarized
surface
reconstruction
Various
noble‐metal‐based
non‐noble‐metal‐based
reviewed.
Finally,
challenges
perspectives
development
Nature Communications,
Год журнала:
2020,
Номер
11(1)
Опубликована: Авг. 13, 2020
Abstract
Anodic
oxygen
evolution
reaction
(OER)
is
recognized
as
kinetic
bottleneck
in
water
electrolysis.
Transition
metal
sites
with
high
valence
states
can
accelerate
the
kinetics
to
offer
highly
intrinsic
activity,
but
suffer
from
thermodynamic
formation
barrier.
Here,
we
show
subtle
engineering
of
oxidized
Ni
4+
species
surface
reconstructed
(oxy)hydroxides
on
multicomponent
FeCoCrNi
alloy
film
through
interatomically
electronic
interplay.
Our
spectroscopic
investigations
theoretical
studies
uncover
that
Fe
component
enables
species,
which
energetically
favored
by
multistep
2+
→Ni
3+
.
The
dynamically
constructed
drives
holes
into
ligands
facilitate
intramolecular
coupling,
triggering
lattice
activation
form
Fe-Ni
dual-sites
ultimate
catalytic
center
activity.
As
a
result,
OER
catalyst
delivers
outstanding
mass
activity
and
turnover
frequency
3601
A
g
−1
0.483
s
at
an
overpotential
300
mV
alkaline
electrolyte,
respectively.
Angewandte Chemie International Edition,
Год журнала:
2019,
Номер
59(4), С. 1718 - 1726
Опубликована: Дек. 4, 2019
A
challenging
but
pressing
task
to
design
and
synthesize
novel,
efficient,
robust
pH-universal
hydrogen
evolution
reaction
(HER)
electrocatalysts
for
scalable
sustainable
production
through
electrochemical
water
splitting.
Herein,
we
report
a
facile
method
prepare
an
efficient
Ru-M
(M=Ni,
Mn,
Cu)
bimetal
nanoparticle
carbon
quantum
dot
hybrid
(RuM/CQDs)
HER.
The
RuNi/CQDs
catalysts
exhibit
outstanding
HER
performance
at
all
pH
levels.
unexpected
low
overpotentials
of
13,
58,
18
mV
shown
by
allow
current
density
10
mA
cm-2
in
1
m
KOH,
0.5
H2
SO4
,
PBS,
respectively,
Ru
loading
5.93
μgRu
.
This
is
among
the
best
catalytic
activities
reported
any
platinum-free
electrocatalyst.
Theoretical
studies
reveal
that
Ni
doping
results
moderate
weakening
bonding
energy
nearby
surface
atoms,
which
plays
critical
role
improving
activity.
