Nature Communications,
Journal Year:
2024,
Volume and Issue:
15(1)
Published: March 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.
Chemical Reviews,
Journal Year:
2023,
Volume and Issue:
123(9), P. 6257 - 6358
Published: March 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.
Energy & environment materials,
Journal Year:
2022,
Volume and Issue:
6(5)
Published: May 28, 2022
Electrochemical
water
splitting
represents
one
of
the
most
promising
technologies
to
produce
green
hydrogen,
which
can
help
realize
goal
achieving
carbon
neutrality.
While
substantial
efforts
on
a
laboratory
scale
have
been
made
for
understanding
fundamental
catalysis
and
developing
high‐performance
electrocatalysts
two
half‐reactions
involved
in
electrocatalysis,
much
less
attention
has
paid
doing
relevant
research
larger
scale.
For
example,
few
such
researches
done
an
industrial
Herein,
we
review
very
recent
endeavors
bridge
gaps
between
applications
electrolysis.
We
begin
by
introducing
fundamentals
electrochemical
then
present
comparisons
testing
protocol,
figure
merit,
catalyst
interest,
manufacturing
cost
industry‐based
water‐electrolysis
research.
Special
is
tracking
surface
reconstruction
process
identifying
real
catalytic
species
under
different
conditions,
highlight
significant
distinctions
corresponding
mechanisms.
Advances
designs
industry‐relevant
electrolysis
are
also
summarized,
reveal
progress
moving
practical
forward
accelerating
synergies
material
science
engineering.
Perspectives
challenges
electrocatalyst
design
strategies
proposed
finally
further
lab‐scale
large‐scale
electrocatalysis
applications.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(13), P. 6028 - 6039
Published: March 18, 2022
Water-alkaline
electrolysis
holds
a
great
promise
for
industry-scale
hydrogen
production
but
is
hindered
by
the
lack
of
enabling
evolution
reaction
electrocatalysts
to
operate
at
ampere-level
current
densities
under
low
overpotentials.
Here,
we
report
use
spillover-bridged
water
dissociation/hydrogen
formation
processes
occurring
synergistically
hybridized
Ni3S2/Cr2S3
sites
incapacitate
inhibition
effect
high-current-density-induced
high
coverage
dissociation
site
and
concurrently
promote
Volmer/Tafel
processes.
The
mechanistic
insights
critically
important
enable
density
operation
are
depicted
from
experimental
theoretical
studies.
Volmer
process
drastically
boosted
strong
H2O
adsorption
Cr5c
Cr2S3,
efficient
H2O*
via
heterolytic
cleavage
(Cr5c-H2O*
+
S3c(#)
→
Cr5c-OH*
S3c-H#)
on
Cr5c/S3c
in
rapid
desorption
OH*
Cr2S3via
new
water-assisted
mechanism
(Cr5c-OH*
H2O(aq)
Cr5c-H2O*
OH-(aq)),
while
Tafel
achieved
through
spillover
rapidly
transfer
H#
located
H-rich
(Cr2S3)
H-deficient
(Ni3S2)
with
excellent
activity.
As
result,
electrocatalyst
can
readily
achieve
3.5
A
cm-2
an
overpotential
251
±
3
mV
1.0
M
KOH
electrolyte.
concept
exemplified
this
work
provides
useful
means
address
shortfalls
current-density-tolerant
Hydrogen
(HER)
electrocatalysts.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(16), P. 5652 - 5683
Published: Jan. 1, 2023
This
review
scrutinizes
recent
progress
in
PEMWE
system
including
mechanisms,
the
correlation
among
structure-composition–performance,
manufacturing,
design
and
operation
protocols.
The
challenges
perspectives
for
applications
are
proposed.
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: Feb. 15, 2023
The
poor
stability
of
Ru-based
acidic
oxygen
evolution
(OER)
electrocatalysts
has
greatly
hampered
their
application
in
polymer
electrolyte
membrane
electrolyzers
(PEMWEs).
Traditional
understanding
performance
degradation
centered
on
influence
bias
fails
describing
the
trend,
calling
for
deep
dive
into
essential
origin
inactivation.
Here
we
uncover
decisive
role
reaction
route
(including
catalytic
mechanism
and
intermediates
binding
strength)
operational
catalysts.
Using
MRuOx
(M
=
Ce4+,
Sn4+,
Ru4+,
Cr4+)
solid
solution
as
structure
model,
find
route,
thereby
stability,
can
be
customized
by
controlling
Ru
charge.
screened
SnRuOx
thus
exhibits
orders
magnitude
lifespan
extension.
A
scalable
PEMWE
single
cell
using
anode
conveys
an
ever-smallest
rate
53
μV
h-1
during
a
1300
h
operation
at
1
cm-2.
Advanced Energy Materials,
Journal Year:
2022,
Volume and Issue:
12(14)
Published: Feb. 17, 2022
Abstract
Proton
exchange
membrane
water
electrolyzer
(PEMWE)
technology
is
of
interest
in
the
context
electrocatalytic
hydrogen
generation
from
renewable
energies.
It
has
benefits
immediate
response,
higher
proton
conductivity,
lower
ohmic
losses,
and
gas
crossover
rate.
One
key
step
toward
to
large‐scale
application,
development
highly
efficient,
durable,
compatible
anodic
oxygen
evolution
electrocatalysts
acidic
media
decrease
usage
expensive
scarce
precious
metals.
Within
this
scenario,
an
in‐depth
understanding
reaction
mechanisms
including
adsorption
mechanism
lattice
first
provided
aid
innovative
materials
elucidate
origin
catalyst
degradation.
Second,
recent
progress
acid
reviewed
with
emphasis
on
underlying
structure–performance
relationships.
Third,
current
application
status
research
PEMWEs
along
representative
examples
are
discussed.
Last,
remaining
challenges
promising
insights
proposed
inspire
future
studies
production
energy.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(22)
Published: March 24, 2023
Nickel-based
catalysts
have
been
regarded
as
one
of
the
most
promising
electrocatalysts
for
urea
oxidation
reaction
(UOR),
however,
their
activity
is
largely
limited
by
inevitable
self-oxidation
Ni
species
(NSOR)
during
UOR.
Here,
we
proposed
an
interface
chemistry
modulation
strategy
to
trigger
occurrence
UOR
before
NSOR
via
constructing
a
2D/2D
heterostructure
that
consists
ultrathin
NiO
anchored
Ru-Co
dual-atom
support
(Ru-Co
DAS/NiO).
Operando
spectroscopic
characterizations
confirm
this
unique
triggering
mechanism
on
surface
DAS/NiO.
Consequently,
fabricated
catalyst
exhibits
outstanding
with
low
potential
1.288
V
at
10
mA
cm-2
and
remarkable
long-term
durability
more
than
330
h
operation.
DFT
calculations
demonstrate
favorable
electronic
structure
induced
heterointerface
endows
energetically
NSOR.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
16(6), P. 2611 - 2620
Published: Jan. 1, 2023
The
grain
boundary
defect
engineered
Ni
nanoparticles
has
been
explored
for
boosting
selective
nitrate
electroreduction
to
ammonia,
and
its
NH
3
generation
rate
is
much
higher
than
those
of
the
reported
copper
or
noble
metal-based
catalysts.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
62(11)
Published: Dec. 22, 2022
Abstract
Polymer
electrolyte
membrane
water
electrolysis
(PEMWE)
has
been
regarded
as
a
promising
technology
for
renewable
hydrogen
production.
However,
acidic
oxygen
evolution
reaction
(OER)
catalysts
with
long‐term
stability
impose
grand
challenge
in
its
large‐scale
industrialization.
In
this
review,
critical
factors
that
may
lead
to
catalyst's
instability
couple
potential
solutions
are
comprehensively
discussed,
including
mechanical
peeling,
substrate
corrosion,
active‐site
over‐oxidation/dissolution,
reconstruction,
oxide
crystal
structure
collapse
through
the
lattice
oxygen‐participated
pathway,
etc.
Last
but
not
least,
personal
prospects
provided
terms
of
rigorous
evaluation
criteria,
situ
/
operando
characterizations,
economic
feasibility
and
practical
electrolyzer
consideration,
highlighting
ternary
relationship
evolution,
industrial‐relevant
activity
serve
roadmap
towards
ultimate
application
PEMWE.