Advanced Materials,
Год журнала:
2023,
Номер
36(1)
Опубликована: Сен. 24, 2023
Adopting
renewable
electricity
to
produce
"green"
hydrogen
has
been
a
critical
challenge
because
at
high
current
density
the
mass
transfer
capability
of
most
catalytic
electrodes
deteriorates
significantly.
Herein,
unique
lamellar
fern-like
alloy
aerogel
(LFA)
electrode,
showing
dynamically
adaptive
bubbling
and
can
effectively
avoid
stress
concentration
caused
by
bubble
aggregation
is
reported.
The
LFA
electrode
intrinsically
highly
catalytic-active
shows
porous,
resilient,
hierarchically
ordered,
well-percolated
conductive
network.
It
not
only
superior
gas
evacuation
but
also
exhibits
significantly
improved
stability
densities,
record
lowest
oxygen
evolution
reaction
(OER)
overpotential
244
mV
1000
mA
cm
Advanced Materials,
Год журнала:
2021,
Номер
34(16)
Опубликована: Дек. 4, 2021
Abstract
Electrochemical
water
splitting
technology
for
producing
“green
hydrogen”
is
important
the
global
mission
of
carbon
neutrality.
Electrocatalysts
with
decent
performance
at
high
current
densities
play
a
central
role
in
industrial
implementation
this
technology.
This
field
has
advanced
immensely
recent
years,
as
witnessed
by
many
types
catalysts
designed
and
synthesized
toward
industriallyrelevant
(>200
mA
cm
–2
).
By
discussing
advances
field,
several
key
aspects
are
summarized
that
affect
catalytic
high‐current‐density
electrocatalysis,
including
dimensionality
catalysts,
surface
chemistry,
electron
transport
path,
morphology,
catalyst‐electrolyte
interplay.
The
multiscale
design
strategy
considers
these
comprehensively
developing
electrocatalysts
highlighted.
perspectives
on
future
directions
emerging
also
put
forward.
Nanoscale,
Год журнала:
2021,
Номер
13(30), С. 12788 - 12817
Опубликована: Янв. 1, 2021
Current
popular
transition
metal-based
electrocatalysts
developed
for
HER/OER
in
water
splitting
at
high
current
density
are
critically
reviewed
and
discussed.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(7), С. 3039 - 3049
Опубликована: Фев. 3, 2022
Electrochemical
CO2
reduction
is
a
promising
way
to
mitigate
emissions
and
close
the
anthropogenic
carbon
cycle.
Among
products
from
CO2RR,
multicarbon
chemicals,
such
as
ethylene
ethanol
with
high
energy
density,
are
more
valuable.
However,
selectivity
reaction
rate
of
C2
production
unsatisfactory
due
sluggish
thermodynamics
kinetics
C-C
coupling.
The
electric
field
thermal
have
been
studied
utilized
promote
catalytic
reactions,
they
can
regulate
thermodynamic
kinetic
barriers
reactions.
Either
raising
potential
or
heating
electrolyte
enhance
coupling,
but
these
come
at
cost
increasing
side
hydrogen
evolution
reaction.
Here,
we
present
generic
strategy
local
temperature
simultaneously
dramatically
improve
electric-thermal
synergy
desired
in
electrocatalysis.
A
conformal
coating
∼5
nm
polytetrafluoroethylene
significantly
improves
ability
copper
nanoneedles
(∼7-fold
∼40
K
enhancement
tips
compared
bare
experimentally),
resulting
an
improved
Faradaic
efficiency
over
86%
partial
current
density
than
250
mA
cm-2
record-high
turnover
frequency
11.5
±
0.3
s-1
Cu
site-1.
Combined
its
low
scalability,
for
state-of-the-art
catalyst
not
only
offers
new
insight
into
improving
activity
value-added
demonstrated
also
inspires
advances
and/or
other
valuable
electro-/photocatalysis
evolution,
nitrogen
reduction,
peroxide
electrosynthesis.
Advanced Materials,
Год журнала:
2022,
Номер
34(29)
Опубликована: Май 17, 2022
Tuning
the
reactivity
of
lattice
oxygen
is
significance
for
lowering
energy
barriers
and
accelerating
evolution
reaction
(OER).
Herein,
single-atomic
Mo
sites
are
anchored
on
Ni-Fe
oxyhydroxide
nanoarrays
by
a
facile
metal-organic-framework-derived
strategy,
exhibiting
superior
performance
toward
OER
in
alkaline
media.
In
situ
electrochemical
spectroscopy
isotope-labeling
experiments
reveal
involvement
during
cycles.
Combining
theoretical
experimental
investigations
electronic
configuration,
it
comprehensively
confirmed
that
incorporation
enables
higher
oxidation
state
metal
strengthened
metal-oxygen
hybridization,
as
well
formation
oxidized
ligand
holes
above
Fermi
level.
word,
considerable
acceleration
water
achieved
via
enhancing
triggering
activation.
This
work
may
provide
new
insights
designing
ideal
electrocatalysts
tuning
chemical
activating
anions
ligands.
ACS Nano,
Год журнала:
2021,
Номер
16(1), С. 1013 - 1024
Опубликована: Дек. 17, 2021
Tip-induced
dendrites
on
metallic
zinc
anodes
(MZAs)
fundamentally
deteriorate
the
rechargeability
of
aqueous
Zn
metal
batteries
(ZMBs).
Herein,
an
intriguing
ion
sieve
(IS)
consisting
3D
intertwined
bacterial
cellulose,
deposited
surface
MZAs
(Zn@IS)
through
in
situ
self-assembly
route,
is
first
presented
to
be
effective
inhibiting
dendrite-growth
MZAs.
Experimental
analyses
together
with
theoretical
calculations
suggested
that
IS
coating
can
facilitate
desolvation
[Zn(H2O)6]2+
clusters
via
a
strong
interplay
ions,
weaken
hydrogen
evolution
reaction
MZAs,
and
homogenize
flux
abundant
nanopores
serving
as
tunnels,
synergistically
enabling
dendrite-free
deposition
Zn@IS
anodes.
Consequently,
lifespan
up
3000
h
at
cutoff
capacity
0.25
mA
cm–2
was
observed
Zn@IS∥Zn@IS
symmetric
cell.
In
terms
application,
pairing
carbon-nanotube@MnO2
cathode
example,
full
ZMBs
acquired
enhanced
much
higher
retention
over
73.3%
after
cycles
compared
counterpart
pristine
MZA
(21%).
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(23), С. 12759 - 12764
Опубликована: Март 1, 2021
Abstract
Nitrogen‐doped
graphene
could
catalyze
the
electrochemical
reduction
and
evolution
of
oxygen,
but
unfortunately
suffers
from
sluggish
catalytic
kinetics.
Herein,
for
first
time,
we
report
an
onion‐like
carbon
coated
Co,
N‐doped
(OLC/Co‐N‐C)
material,
which
possesses
multilayers
highly
curved
nanostructures
that
form
mesoporous
architectures.
These
unique
nanospheres
are
produced
when
surfactant
micelles
introduced
to
synthesis
precursors.
Owing
combined
electronic
effect
nanostructuring
effect,
our
OLC/Co‐N‐C
materials
exhibit
high
bifunctional
oxygen
reduction/evolution
reaction
(ORR/OER)
activity,
showing
a
promising
application
in
rechargeable
Zn‐air
batteries.
Experimental
results
rationalized
by
theoretical
calculations,
curvature
graphitic
plays
vital
role
promoting
activities
meta‐carbon
atoms
near
N
ortho/meta
close
pyridinic
N.
Abstract
Electron
density
modulation
is
of
great
importance
in
an
attempt
to
achieve
highly
active
electrocatalysts
for
the
oxygen
evolution
reaction
(OER).
Here,
successful
construction
CuO@CoOOH
p‐n
heterojunction
(i.e.,
p‐type
CuO
and
n‐type
CoOOH)
nanoarray
electrocatalyst
through
situ
anodic
oxidation
CuO@CoS
x
on
copper
foam
reported.
The
can
remarkably
modify
electronic
properties
space‐charge
region
facilitate
electron
transfer.
Moreover,
Raman
study
reveals
generation
SO
4
2−
from
CoS
oxidation,
cloud
distribution
functional
theory
calculation
suggest
that
surface‐adsorbed
OER
process
by
enhancing
adsorption
OH
−
.
positively
charged
CoOOH
significantly
enhance
activity.
As
a
result,
shows
enhanced
performance
with
low
overpotential
186
mV
afford
current
10
mA
cm
−2
preparation
large
scale
(14
×
25
2
)
sample
demonstrates
possibility
promoting
catalyst
industrial‐scale
production.
This
offers
new
insights
into
design
fabrication
non‐noble
metal‐based
as
effective
catalytic
materials
energy
storage
conversion.
Advanced Materials,
Год журнала:
2021,
Номер
34(9)
Опубликована: Дек. 30, 2021
Alkaline
water
electrolysis
is
commercially
desirable
to
realize
large-scale
hydrogen
production.
Although
nonprecious
catalysts
exhibit
high
electrocatalytic
activity
at
low
current
density
(10-50
mA
cm-2
),
it
still
challenging
achieve
industrially
required
over
500
due
inefficient
electron
transport
and
competitive
adsorption
between
hydroxyl
water.
Herein,
the
authors
design
a
novel
metallic
heterostructure
based
on
nickel
nitride
monoclinic
molybdenum
disulfide
(Ni3
N@2M-MoS2
)
for
extraordinary
electrolysis.
The
Ni3
composite
with
heterointerface
provides
two
kinds
of
separated
reaction
sites
overcome
steric
hindrance
hydroxyl/water
adsorption.
kinetically
decoupled
adsorption/dissociation
conductivity
enable
production
from
N
oxygen
evolution
large
density.
proved
be
imperative
stabilization
activation
,
which
can
efficiently
regulate
active
electronic
states
Ni/N
atoms
around
Fermi-level
through
charge
transfer
MoMo
bonds
2M-MoS2
boost
overall
splitting.
incorporated
electrolyzer
requires
ultralow
cell
voltage
1.644
V@1000
≈100%
retention
300
h,
far
exceeding
commercial
Pt/C║RuO2
(2.41
100
58.2%).