Chemistry - A European Journal,
Год журнала:
2024,
Номер
30(20)
Опубликована: Янв. 15, 2024
Abstract
Hydrogen
(H
2
),
produced
by
water
electrolysis
with
the
electricity
from
renewable
sources,
is
an
ideal
energy
carrier
for
achieving
a
carbon‐neutral
and
sustainable
society.
evolution
reaction
(HER)
cathodic
half‐reaction
of
electrolysis,
which
requires
active
robust
electrocatalysts
to
reduce
consumption
H
generation.
Despite
numerous
have
been
reported
academia
HER,
most
them
were
only
tested
under
relatively
small
current
densities
short
period,
cannot
meet
requirements
industrial
electrolysis.
To
bridge
gap
between
industry,
it
crucial
develop
highly
HER
can
operate
at
large
long
time.
In
this
review,
mechanisms
in
acidic
alkaline
electrolytes
are
firstly
introduced.
Then,
design
strategies
towards
high‐performance
large‐current‐density
five
aspects
including
number
sites,
intrinsic
activity
each
site,
charge
transfer,
mass
stability
discussed
via
featured
examples.
Finally,
our
own
insights
about
challenges
future
opportunities
emerging
field
presented.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 12, 2025
The
bifunctional
mechanism,
involving
multiactive
compositions
to
simultaneously
dissociate
water
molecules
and
optimize
intermediate
adsorption,
has
been
widely
used
in
the
design
of
catalysts
boost
electrolysis
for
sustainable
hydrogen
energy
production
but
remains
debatable
due
difficulties
accurately
identifying
reaction
process.
Here,
we
proposed
concept
well-defined
Lewis
pairs
single-atom
catalysts,
with
a
unique
acid-base
nature,
comprehensively
understand
exact
role
an
alkaline
evolution
reaction.
By
facilely
adjusting
active
moieties,
induced
synergistic
effect
between
(M-P/S/Cr
pairs,
M
=
Ru,
Ir,
Pt)
can
significantly
facilitate
cleavage
H-OH
bond
accelerate
removal
intermediates,
thereby
switching
rate-determining
step
from
Volmer
Heyrovsky
step.
Moreover,
representative
Ru-P
deliver
impressive
266
h
durability
at
high
industrial
current
density
2
A
cm-2
without
activity
decay
anion-exchange
membrane
electrolysis,
be
extended
modify
commercial
noble-metal-based
performance
enhancement.
This
work
not
only
sheds
light
on
important
mechanism
scale
also
offers
universal
descriptor
rational
advanced
catalysts.
Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 5, 2025
Abstract
Developing
efficient
and
cost‐effective
electrocatalysts
to
replace
expensive
carbon‐supported
platinum
nanoparticles
for
the
alkaline
hydrogen
evolution
reaction
remains
an
important
challenge.
Recently,
innovative
catalyst,
composed
of
ruthenium
single
atoms
(Ru
1
)
integrated
with
small
Ru
nanoclusters
NC
),
has
attracted
considerable
attention
from
scientific
community.
However,
because
its
complexity,
this
catalyst
a
topic
some
debate.
Here,
method
is
reported
precisely
controlling
ratios
on
nitrogenated
carbon
(NC)‐based
porous
organic
framework
produce
Ru/NC
catalysts,
by
using
different
amounts
(0,
5,
10
wt.%)
reducing
agent.
The
Ru/NC–10
formed
wt.%
agent,
delivered
best
performance
under
conditions,
indicating
that
played
significant
role
in
actual
(HER).
An
anion
exchange
membrane
water
electrolyzer
(AEMWE)
system
required
significantly
lower
operating
voltage
(1.72
V)
than
commercial
Pt/C
(1.95
achieve
500
mA
cm
−2
.
Moreover,
can
be
operated
at
100
without
notable
decay
over
180
h.
Theoretical
calculations
supported
these
experimental
findings
contributed
dissociation
process,
while
more
actively
associated
recombination
process.
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(12), С. 5663 - 5687
Опубликована: Янв. 1, 2023
This
review
summarizes
recent
progress
and
prospects
of
catalysts
containing
metal
single-atom
(M
1
)
nano-aggregates
(MNAs,
particles
or
clusters),
which
promise
to
combine
the
merits
SACs
MNA-based
for
efficient
electrocatalysis.
Angewandte Chemie,
Год журнала:
2023,
Номер
136(7)
Опубликована: Дек. 28, 2023
Abstract
Modulating
the
microenvironment
of
single‐atom
catalysts
(SACs)
is
critical
to
optimizing
catalytic
activity.
Herein,
we
innovatively
propose
a
strategy
improve
local
reaction
environment
Ru
single
atoms
by
precisely
switching
crystallinity
support
from
high
crystalline
and
low
crystalline,
which
significantly
improves
hydrogen
evolution
(HER)
The
catalyst
anchored
on
low‐crystalline
nickel
hydroxide
(Ru−LC−Ni(OH)
2
)
reconstructs
distribution
balance
interfacial
ions
due
activation
effect
metal
dangling
bonds
support.
Single‐site
with
oxidation
state
induces
aggregation
hydronium
(H
3
O
+
),
leading
formation
acidic
in
alkaline
media,
breaking
pH‐dependent
HER
As
comparison,
high‐crystalline
(Ru−HC−Ni(OH)
exhibits
sluggish
Volmer
step
conventional
environment.
expected,
Ru−LC−Ni(OH)
requires
overpotentials
9
136
mV
at
10
1000
mA
cm
−2
conditions
operates
stably
500
for
h
an
seawater
anion
exchange
membrane
(AEM)
electrolyzer.
This
study
provides
new
perspective
constructing
highly
active
electrocatalysts.
Nano-Micro Letters,
Год журнала:
2024,
Номер
16(1)
Опубликована: Май 23, 2024
Single-atom
(SA)
catalysts
with
nearly
100%
atom
utilization
have
been
widely
employed
in
electrolysis
for
decades,
due
to
the
outperforming
catalytic
activity
and
selectivity.
However,
most
of
reported
SA
are
fixed
through
strong
bonding
between
dispersed
single
metallic
atoms
nonmetallic
substrates,
which
greatly
limits
controllable
regulation
electrocatalytic
catalysts.
In
this
work,
Pt-Ni
bonded
Pt
catalyst
adjustable
electronic
states
was
successfully
constructed
a
electrochemical
reduction
on
coordination
unsaturated
amorphous
Ni(OH)
ACS Catalysis,
Год журнала:
2024,
Номер
14(11), С. 8238 - 8251
Опубликована: Май 13, 2024
Currently,
the
construction
of
an
acid-like
catalyst
surface
in
a
high-pH
electrolyte
is
advocated
as
one
most
pioneering
strategies
for
significantly
improving
catalytic
activity
alkaline
hydrogen
evolution
reaction.
However,
proton
transfer
kinetics
that
determines
proton-coupled
electron
reaction
largely
dependent
on
usage
extensive
noble-metal
bulk
phase.
Herein,
well-designed
dynamic
system
constructed
by
metallic
WO2
matrix
and
supported
Ru
single
atoms
(0.89
wt
%)
grown
nickel
foam
(Ru
SAC@WO2/NF).
The
as-prepared
SAC@WO2/NF
free-standing
exhibits
superior
activities
with
delivering
current
densities
10,
50,
200
mA/cm2
only
requiring
overpotentials
∼0,
40,
84
mV,
respectively,
ultralow
Tafel
slope
(38
mV/dec)
1.0
M
KOH
electrolyte.
Moreover,
our
deliberately
prepared
composite
also
shows
long-term
stability
negligible
decay
after
continuous
generation
at
more
than
50
h.
Comprehensive
spectroscopy
characterizations
combined
density
function
theory
calculations
reveal
improved
can
be
understood
two
reasons:
(i)
contributes
to
environment
through
formation
weak-acid
tungsten
bronze
(HxWOy)
intermediates
solid–liquid
interface
electrolyte;
(ii)
unlike
weak
electronic
interaction
between
nanoparticles
HxWOy
intermediates,
are
evidenced
efficiently
tailor
acidity
accelerated
deprotonation
kinetics,
thus
resulting
regeneration
active
sites
next
cycle.
Such
interesting
concept
design
driven
basic
chemical
theories
will
benefit
exploration
but
higher
added-values
water
electrolysis
beyond.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Авг. 8, 2024
The
development
of
highly
efficient
and
durable
alkaline
hydrogen
evolution
reaction
(HER)
catalysts
is
crucial
for
achieving
high-performance
practical
anion
exchange
membrane
water
electrolyzer
(AEMWE)
at
ampere-level
current
density.
Herein,
we
report
a
design
concept
by
employing
Ga
single
atoms
as
an
electronic
bridge
to
stabilize
the
Ru
clusters
boosting
HER
performance
in
AEMWE.
Experimental
theoretical
results
collectively
reveal
that
bridged
sites
trigger
strong
metal-support
interaction
homogeneous
distribution
with
high
density,
well
optimize
Ru-H
bond
strength
due
electron
transfer
between
enhanced
intrinsic
activity.
Moreover,
oxophilic
near
tend
adsorb
hydroxyl
species
accelerate
dissociation
sufficient
proton
supplement
medium.
Ru-Ga
