Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(52)
Опубликована: Ноя. 9, 2023
Developing
novel
synthesis
technologies
is
crucial
to
expanding
bifunctional
electrocatalysts
for
energy-saving
hydrogen
production.
Herein,
we
report
an
ambient
and
controllable
γ-ray
radiation
reduction
synthesize
a
series
of
noble
metal
nanoparticles
anchored
on
defect-rich
manganese
oxides
(M@MnO2-x
,
M=Ru,
Pt,
Pd,
Ir)
glycerol-assisted
H2
evolution.
Benefiting
from
the
strong
penetrability
γ-rays,
defect
supports
are
formed
simultaneously
bridged
by
metal-oxygen
bonds,
guaranteeing
structural
stability
active
site
exposure.
The
special
Ru-O-Mn
bonds
activate
Ru
Mn
sites
in
Ru@MnO2-x
through
interfacial
coordination,
driving
glycerol
electrolysis
at
low
overpotential.
Furthermore,
only
cell
voltage
1.68
V
required
achieve
0.5
A
cm-2
continuous-flow
electrolyzer
system
along
with
excellent
stability.
In
situ
spectroscopic
analysis
reveals
that
coordination
balances
competitive
adsorption
OH*
catalyst
surface.
Theoretical
calculations
further
demonstrate
MnO2
support
promotes
dissociation
O,
while
defect-regulated
promote
deprotonation
desorption,
synergistically
enhancing
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(43), С. 23659 - 23669
Опубликована: Окт. 23, 2023
Designing
stable
single-atom
electrocatalysts
with
lower
energy
barriers
is
urgent
for
the
acidic
oxygen
evolution
reaction.
In
particular,
atomic
catalysts
are
highly
dependent
on
kinetically
sluggish
acid-base
mechanism,
limiting
reaction
paths
of
intermediates.
Herein,
we
successfully
manipulate
steric
localization
Ru
single
atoms
at
Co3O4
surface
to
improve
by
precise
control
anchor
sites.
The
delicate
structure
design
can
switch
mechanism
from
lattice
(LOM)
optimized
adsorbate
(AEM).
embedded
into
cation
vacancies
reveal
an
that
activates
proton
donor-acceptor
function
(PDAM),
demonstrating
a
new
catalytic
pathway
circumvent
classic
scaling
relationship.
Steric
interactions
intermediates
anchored
Ru-O-Co
interface
played
primary
role
in
optimizing
intermediates'
conformation
and
reducing
barrier.
As
comparison,
confined
sites
exhibit
process.
result,
atom
spatial
position
presents
100-fold
increase
mass
activity
36.96
A
gRu(ads)-1
4012.11
gRu(anc)-1
1.50
V.
These
findings
offer
insights
behavior.
Energy & Environmental Science,
Год журнала:
2023,
Номер
17(1), С. 49 - 113
Опубликована: Ноя. 7, 2023
This
perspective
highlights
recent
advancements
in
innovative
strategies
to
provide
valuable
insights
into
the
potential
for
energy-saving
hydrogen
production
through
water
electrolysis.
Advanced Materials,
Год журнала:
2023,
Номер
35(48)
Опубликована: Сен. 6, 2023
The
continuous
oxidation
and
leachability
of
active
sites
in
Ru-based
catalysts
hinder
practical
application
proton-exchange
membrane
water
electrolyzers
(PEMWE).
Herein,
robust
inter-doped
tungsten-ruthenium
oxide
heterostructures
[(Ru-W)Ox
]
fabricated
by
sequential
rapid
metal
thermomigration
processes
are
proposed
to
enhance
the
activity
stability
acidic
oxygen
evolution
reaction
(OER).
introduction
high-valent
W
species
induces
valence
oscillation
Ru
during
OER,
facilitating
cyclic
transition
states
maintaining
operation
sites.
preferential
electronic
gain
heterostructure
significantly
stabilize
RuOx
on
WOx
substrates
beyond
Pourbaix
limit
bare
RuO2
.
Furthermore,
asymmetric
Ru-O-W
units
generated
around
interface
adsorb
intermediates
synergistically,
enhancing
intrinsic
OER
activity.
Consequently,
(Ru-W)Ox
not
only
demonstrate
an
overpotential
170
mV
at
10
mA
cm-2
excellent
300
h
electrolytes
but
also
exhibit
potential
for
applications,
as
evidenced
stable
0.5
A
PEMWE.
Advanced Materials,
Год журнала:
2023,
Номер
36(4)
Опубликована: Окт. 10, 2023
Abstract
As
one
of
the
most
promising
approaches
to
producing
high‐purity
hydrogen
(H
2
),
electrochemical
water
splitting
powered
by
renewable
energy
sources
such
as
solar,
wind,
and
hydroelectric
power
has
attracted
considerable
interest
over
past
decade.
However,
electrolysis
process
is
seriously
hampered
sluggish
electrode
reaction
kinetics,
especially
four‐electron
oxygen
evolution
at
anode
side,
which
induces
a
high
overpotential.
Currently,
emerging
hybrid
strategy
proposed
integrating
thermodynamically
favorable
electro–oxidation
reactions
with
cathode,
providing
new
opportunity
for
energy–efficient
H2
production.
To
achieve
highly
efficient
cost–effective
toward
large–scale
practical
H
production,
much
work
been
continuously
done
exploit
alternative
anodic
oxidation
cutting–edge
electrocatalysts.
This
review
will
focus
on
recent
developments
production
coupled
reactions,
including
choice
substrates,
investigation
electrocatalytic
materials,
deep
understanding
underlying
mechanisms.
Finally,
some
insights
into
scientific
challenges
now
standing
in
way
future
advancement
technique
are
shared,
hope
inspiring
further
innovative
efforts
this
rapidly
growing
field.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(21)
Опубликована: Фев. 2, 2024
Abstract
Metal–support
interaction
(MSI)
is
witnessed
as
an
essential
manner
to
stabilize
active
metals
and
tune
catalytic
activity
for
heterogonous
water
splitting.
Kinetically
driving
the
electrolysis
(WE)
appeals
a
rational
MSI
system
with
coupled
electron‐donating/accepting
(e‐D/A)
characters
hydrogen/oxygen
evolution
reactions
(HER/OER).
However,
metal
stabilization
effect
by
will
in
turn
restrict
deblocking
of
e‐D/A
properties
challenge
full
electrocatalytic
optimization.
This
study
profiles
heterostructure
featuring
metastable
Ru
clusters
on
defective
NiFe
hydroxide
(Ru/d‐NiFe
LDH)
support
low‐precious
(≈2
wt%)
platform
efficient
WE.
It
indicated
that
interfacial
oxygen
vacancies
can
deviate
stable
4d
5
orbit
2+δ
state,
regulate
d‐band
center
levels
toward
facilitated
HER/OER
processes.
Resultantly,
Ru/d‐NiFe
LDH
attains
ultralow
overpotentials
at
10
mA
cm
−2
Pt‐beyond
alkaline
HER
(18
mV)
OER
(220
fast
kinetics
durability.
The
symmetrical
electrolyzer
delivers
promising
voltage
1.49
V
1
m
KOH
seawater
splitting
performance.
work
carries
interesting
opportunities
rationalizing
sophisticated
metal‐support
electrocatalysts
through
metal‐site
metastabilization
engineering.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Март 29, 2024
Abstract
Establishing
appropriate
metal-support
interactions
is
imperative
for
acquiring
efficient
and
corrosion-resistant
catalysts
water
splitting.
Herein,
the
interaction
mechanism
between
Ru
nanoparticles
a
series
of
titanium
oxides,
including
TiO,
Ti
4
O
7
TiO
2,
designed
via
facile
non-stoichiometric
engineering
systematically
studied.
7,
with
unique
band
structure,
high
conductivity
chemical
stability,
endows
ingenious
through
interfacial
Ti–O–Ru
units,
which
stabilizes
species
during
OER
triggers
hydrogen
spillover
to
accelerate
HER
kinetics.
As
expected,
Ru/Ti
displays
ultralow
overpotentials
8
mV
150
long
operation
500
h
at
10
mA
cm
−2
in
acidic
media,
expanded
pH-universal
environments.
Benefitting
from
excellent
bifunctional
performance,
proton
exchange
membrane
anion
electrolyzer
assembled
achieves
superior
performance
robust
operation.
The
work
paves
way
energy
conversion
devices.
Advanced Materials,
Год журнала:
2023,
Номер
36(7)
Опубликована: Окт. 26, 2023
Abstract
Neutral
oxygen
evolution
reaction
(OER)
with
unique
reactive
environments
exhibits
extremely
slow
kinetics,
posing
significant
challenges
in
the
design
of
catalysts.
Herein,
a
built‐in
electric
field
between
tungstate
(Ni‐FeWO
4
)
adjustable
work
function
and
Lewis
acid
WO
3
is
elaborately
constructed
to
regulate
asymmetric
interfacial
electron
distribution,
which
promotes
accumulation
Fe
sites
tungstate.
This
decelerates
rapid
dissolution
under
OER
potentials,
thereby
retaining
active
hydroxyl
oxide
optimized
pathway.
Meanwhile,
enhances
adsorption
near
electrode
surface
improve
mass
transfer.
As
expected,
Ni‐FeWO
@WO
/NF
self‐supporting
achieves
low
overpotential
235
mV
at
10
mA
cm
−2
neutral
media
maintains
stable
operation
for
200
h.
Furthermore,
membrane
assembly
by
such
robust
stability
250
h
during
seawater
electrolysis.
deepens
understanding
reconstruction
catalysts
paves
way
development
energy
conversion
technologies.
ACS Energy Letters,
Год журнала:
2024,
Номер
9(3), С. 853 - 879
Опубликована: Фев. 7, 2024
Hydrogen
production
via
electrocatalytic
water
splitting
is
hampered
by
the
slow
kinetics
of
anodic
oxygen
evolution
reaction
(OER).
To
address
this
limitation,
electrochemical
hydrogen
(HER)
can
be
boosted
with
more
favorable
oxidation
small
organic
molecules
ideally
driven
renewable
energies,
producing
valuable
chemicals.
In
context,
coupling
methanol
(MOR)
simultaneous
formate
has
garnered
significant
interest.
Such
a
cost-effective
process,
meeting
growing
demand
for
energy
storage
and
fuel
production,
requires
developing
cheap
efficient
electrocatalysts.
Given
knowledge
gap
between
precious
nonprecious
metal
electrocatalysts,
exemplified
nickel
its
derived
compounds,
review
focuses
on
MOR
from
fundamental
electrochemistry,
materials
design
synthesis,
activity-composition/structure
relations.
Despite
advances,
we
still
face
formidable
challenges
in
deciphering
intricate
catalytic
mechanism,
elevating
activity
selectivity
to
new
heights,
pioneering
development
scalable
prototypes.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июнь 10, 2024
Abstract
Electrocatalytic
water
splitting
driven
by
sustainable
energy
is
a
clean
and
promising
water‐chemical
fuel
conversion
technology
for
the
production
of
high‐purity
green
hydrogen.
However,
sluggish
kinetics
anodic
oxygen
evolution
reaction
(OER)
pose
challenges
large‐scale
hydrogen
production,
limiting
its
efficiency
safety.
Recently,
OER
has
been
replaced
nucleophilic
oxidation
(NOR)
with
biomass
as
substrate
coupled
(HER),
which
attracted
great
interest.
Anode
NOR
offers
faster
kinetics,
generates
high‐value
products,
reduces
consumption.
By
coupling
reaction,
can
be
enhanced
while
yielding
products
or
degrading
pollutants.
Therefore,
NOR‐coupled
HER
another
new
electrolytic
strategy
after
significance
realizing
development
global
decarbonization.
This
review
explores
potential
reactions
an
alternative
to
delves
into
mechanisms,
guiding
future
research
in
production.
It
assesses
different
methods,
analyzing
pathways
catalyst
effects.
Furthermore,
it
evaluates
role
electrolyzers
industrialized
discusses
prospects
challenges.
comprehensive
aims
advance
efficient
economical
