Abstract
The
oxygen
evolution
reaction
(OER)
performance
of
NiCo
LDH
electrocatalysts
can
be
improved
through
fluorine
doping.
roles
Ni
and
Co
active
sites
in
such
catalysts
remain
ambiguous
controversial.
In
addressing
the
issue,
this
study
draws
upon
molecular
orbital
theory
proposes
center
competitive
mechanism
between
Co.
doped
F‐atoms
directly
impact
valence
state
metal
atoms
or
exert
an
indirect
influence
dehydrogenation,
thereby
modulating
center.
As
are
progressively
aggregate,
e
g
orbitals
transition
from
2
to
1
,
subsequently
0
.
corresponding
elevates
+2
+3,
then
+4,
signifying
initial
increase
followed
by
a
subsequent
decrease
electrocatalytic
performance.
Furthermore,
series
F‐NiCo
synthesized
verify
occupancy
analysis,
catalytic
OER
overpotentials
303,
243,
240,
246
mV
at
current
density
10
mA
cm
−2
respectively,
which
coincides
well
with
theoretical
prediction.
This
investigation
not
only
provides
novel
mechanistic
insights
into
competition
but
also
establishes
foundation
for
design
high‐performance
catalysts.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Фев. 15, 2024
Abstract
Cobalt
oxyhydroxide
(CoOOH)
is
a
promising
catalytic
material
for
oxygen
evolution
reaction
(OER).
In
the
traditional
CoOOH
structure,
Co
3+
exhibits
low-spin
state
configuration
(
$${t}_{2{{{{{\rm{g}}}}}}}^{6}{e}_{{{{{{\rm{g}}}}}}}^{0}$$
t2g6e0
),
with
electron
transfer
occurring
in
face-to-face
$${t}_{2{{{{{\rm{g}}}}}}}^{*}$$
*
orbitals.
this
work,
we
report
successful
synthesis
of
high-spin
by
introducing
coordinatively
unsaturated
atoms.
As
compared
to
CoOOH,
occurs
apex-to-apex
$${e}_{{{{{{\rm{g}}}}}}}^{*}$$
orbitals,
which
faster
ability.
result,
performs
superior
OER
activity
an
overpotential
226
mV
at
10
mA
cm
−2
,
148
lower
than
that
CoOOH.
This
work
emphasizes
effect
spin
on
based
electrocatalysts
water
splitting,
and
thus
provides
new
strategy
designing
highly
efficient
electrocatalysts.
Applied Catalysis B Environment and Energy,
Год журнала:
2023,
Номер
343, С. 123584 - 123584
Опубликована: Дек. 1, 2023
The
electrocatalytic
process
of
water
splitting
offers
a
promising
approach
to
produce
sustainable
hydrogen.
However,
the
slow
kinetics
oxygen
evolution
reaction
(OER)
presents
notable
challenge,
especially
in
acidic
environment
proton
exchange
membrane
(PEM)
systems.
Despite
extensive
progress
made
catalyst
development
for
hydrogen
production
through
electrolysis
last
century,
significant
advancements
have
been
accomplished.
quest
OER
catalysts
that
possess
both
high
activity
and
stability,
while
also
being
affordable,
continues
be
challenging.
Currently,
Ru/Ir-based
electrocatalysts
are
only
practical
anode
available.
Therefore,
it
is
crucial
explore
feasible
strategies
enhance
performance
longevity
catalysts.
This
review
comprehensive
assessment
obstacles
prospective
Additionally,
underscores
areas
research
concentration,
providing
valuable
perspectives
future
endeavors
development.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(32)
Опубликована: Март 25, 2024
Abstract
Understanding
of
fundamental
mechanism
and
kinetics
the
oxygen
evolution
reaction
(OER)
is
pivotal
for
designing
efficient
OER
electrocatalysts
owing
to
its
key
role
in
electrochemical
energy
conversion
devices.
In
past
few
years,
lattice
oxidation
(LOM)
arising
from
anodic
redox
chemistry
has
attracted
significant
attention
as
it
involves
a
direct
O─O
coupling
thus
bypasses
thermodynamic
limitations
traditional
adsorbate
(AEM).
Transition
metal‐based
oxyhydroxides
are
generally
acknowledged
real
catalytic
phase
alkaline
media.
particular,
their
low‐dimensional
layered
structures
offer
sufficient
structural
flexibility
trigger
LOM.
Herein,
comprehensive
overview
provided
recent
advances
anion
LOM‐based
electrocatalysts.
Based
on
analyses
electronic
structure
LOM,
strategy
proposed
activate
Possible
identification
techniques
corroboration
also
reviewed.
addition,
reconstruction
process
induced
by
LOM
focused
importance
multiple
situ/operando
characterizations
highlighted
unveil
chemical
origins
To
conclude,
prospect
remaining
challenges
future
opportunities
presented.
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(6), С. 2771 - 2807
Опубликована: Янв. 1, 2024
This
review
presents
the
basics
of
electrochemical
water
electrolysis,
discusses
progress
in
computational
methods,
models,
and
descriptors,
evaluates
remaining
challenges
this
field.
Advanced Energy Materials,
Год журнала:
2023,
Номер
14(2)
Опубликована: Ноя. 21, 2023
Abstract
Electrocatalytic
biomass
valorization
coupled
with
hydrogen
production
provides
an
efficient
and
economical
way
to
achieve
a
zero‐carbon
economy.
Ni‐based
electrocatalysts
are
promising
candidates
due
their
intrinsic
redox
capabilities,
but
the
rational
design
of
active
Ni
site
coordination
is
still
huge
challenge.
Herein,
combined
strategies
surface
reconstruction
heteroatom
doping
adopted
modify
3
S
2
pre‐catalysts
obtained
bimetallic
catalyst
exhibits
superior
electrocatalytic
performance
toward
5‐hydroxymethylfurfural
(HMF)
oxidation
2,5‐furanedicarboxylic
acid
(FDCA).
Specifically,
oxysulfide‐coordinated
amorphous
NiOOH
(NiOOH‐SO
x
)
phase
in
situ
constructed
following
anionic
regulation
mechanism,
which
endows
numerous
defects
unsaturated
sites
for
anodic
HMF
oxidation.
Cu
further
modulates
electronic
structure
abundant
Lewis
acidic
sites,
offering
advanced
capability
adsorption.
Several
operando
characterization
techniques
(in
Raman,
infrared,
electrochemical
impedance
spectroscopies)
performed
disclose
reaction
pathway
structure‐activity‐potential
relationship.
Theoretical
results
demonstrate
that
oxyanionic
effectively
modulate
local
environment
correspondingly
tailor
intermediate
adsorption
behavior
then
promote
kinetics.
Moreover,
two‐electrode
system
assembled
pair
cathode
production,
demonstrating
better
energy
conversion
efficiency.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(37)
Опубликована: Май 6, 2024
Abstract
The
exploitation
of
highly
activity
oxygen
evolution
reaction
(OER)
electrocatalysts
is
critical
for
the
application
electrocatalytic
water
splitting.
Triggering
lattice
mechanism
(LOM)
expected
to
provide
a
promising
pathway
overcome
sluggish
OER
kinetics,
however,
effectively
enhancing
involvement
remains
challenging.
In
this
study,
fabrication
B,
Fe
co‐doped
CoP
(B,
Fe─CoP)
nanofibers
reported,
which
serve
as
efficient
electrocatalyst
through
phosphorization
and
boronation
treatment
Fe‐doped
Co
3
O
4
nanofibers.
Experimental
results
combined
with
theoretical
calculations
reveal
that
simultaneous
incorporation
both
B
can
more
trigger
participation
in
CoFe
oxyhydroxides
reconstructed
from
Fe─CoP
compared
incorporating
only
or
Fe.
Therefore,
optimized
exhibit
superb
low
overpotentials
361
376
mV
at
1000
mA
cm
−2
alkaline
freshwater
natural
seawater,
respectively.
present
work
provides
significant
guidelines
innovative
design
concepts
development
following
LOM
pathway.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июнь 13, 2024
Single-atom
electrocatalysts
(SACs)
are
a
class
of
promising
materials
for
driving
electrochemical
energy
conversion
reactions
due
to
their
intrinsic
advantages,
including
maximum
metal
utilization,
well-defined
active
structures,
and
strong
interface
effects.
However,
SACs
have
not
reached
full
commercialization
broad
industrial
applications.
This
review
summarizes
recent
research
achievements
in
the
design
crucial
electrocatalytic
on
sites,
coordination,
substrates,
as
well
synthesis
methods.
The
key
challenges
facing
activity,
selectivity,
stability,
scalability,
highlighted.
Furthermore,
it
is
pointed
out
new
strategies
address
these
increasing
activity
enhancing
utilization
improving
optimizing
local
environment,
developing
fabrication
techniques,
leveraging
insights
from
theoretical
studies,
expanding
potential
Finally,
views
offered
future
direction
single-atom
electrocatalysis
toward
commercialization.
Chemical Reviews,
Год журнала:
2024,
Номер
124(15), С. 9136 - 9223
Опубликована: Июль 22, 2024
The
electrocatalytic
oxygen
evolution
reaction
(OER)
supplies
the
protons
and
electrons
needed
to
transform
renewable
electricity
into
chemicals
fuels.
However,
OER
is
kinetically
sluggish;
it
operates
at
significant
rates
only
when
applied
potential
far
exceeds
reversible
voltage.
origin
of
this
overpotential
hidden
in
a
complex
mechanism
involving
multiple
electron
transfers
chemical
bond
making/breaking
steps.
Our
desire
improve
catalytic
performance
has
then
made
mechanistic
studies
an
area
major
scientific
inquiry,
though
complexity
understanding
difficult.
While
historically,
have
relied
solely
on
experiment
phenomenological
models,
over
past
twenty
years
