Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Oct. 25, 2024
Abstract
Understanding
the
role
of
adsorbed
intermediates
at
polarized
catalyst‐electrolyte
interface
on
structure
electrical
double
layer
(EDL)
is
essential
for
developing
highly
efficient
electrocatalysts.
Here,
we
prepared
a
series
unconventional
face‐centered‐cubic
(
fcc
)
phase
Ru‐based
catalysts
(i.e.
‐Ru,
‐RuCr,
and
‐RuCrW)
by
rational
tuning
binding
energetics
hydroxyl
intermediate
to
engineer
electrochemical
boost
performance
alkaline
hydrogen
oxidation
reaction
(HOR).
The
introduction
oxyphilic
metals
Cr
W
can
regulate
orbital
occupation
Ru,
promote
adsorption
species,
resulting
in
an
anomalous
behavior
that
HOR
under
media
exceeds
acidic
media.
Experimental
results
theoretical
calculations
unravel
modulated
species
electrode
surface
are
responsible
reconstruction
interfacial
water
dynamic
evolution
free
molecules
from
nearest
above
gap
region
EDL,
thereby
leading
significantly
increased
connectivity
bond
network.
Our
work
reveals
new
understanding
controlling
process
bonding
network
electrocatalysis,
will
guide
design
advanced
electrocatalysts
through
engineering.
Inorganic Chemistry Frontiers,
Journal Year:
2024,
Volume and Issue:
11(14), P. 4080 - 4106
Published: Jan. 1, 2024
This
summary
describes
the
effects
of
wettability,
local
pH,
interfacial
water
structure,
and
electrolyte
composition
on
interface
reactant
compositions,
key
intermediate
adsorption,
reaction
kinetics.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(17)
Published: Feb. 17, 2024
Searching
for
highly
efficient
and
economical
electrocatalysts
alkaline
hydrogen
oxidation
reaction
(HOR)
is
crucial
the
development
of
polymer
membrane
fuel
cells.
Here,
we
report
a
valid
strategy
to
active
pyrite-type
RuS
National Science Review,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 10, 2025
The
electrochemical
CO2
reduction
reaction
(CO2RR)
is
an
important
application
that
can
considerably
mitigate
environmental
and
energy
crises.
However,
the
slow
proton-coupled
electron
transfer
process
continues
to
limit
overall
catalytic
performance.
Fine-tuning
microenvironment
by
accurately
constructing
local
structure
of
catalysts
provides
a
novel
approach
enhancing
kinetics.
Here,
cubic-phase
α-MoC1-x
nanoparticles
were
incorporated
into
carbon
matrix
coupled
with
cobalt
phthalocyanine
molecules
(α-MoC1-x-CoPc@C)
for
co-reduction
H2O,
achieving
impressive
Faradaic
efficiency
CO
close
100%.
Through
combination
in-situ
spectroscopies,
measurements,
theoretical
simulations,
it
demonstrated
CoPc
optimized
configuration
serve
as
active
centers
H2O
activation
reduction,
respectively.
interfacial
water
rearranged,
forming
dense
hydrogen
bond
network
on
catalyst
surface.
This
at
electrode-electrolyte
interface
synergistically
enhanced
dissociation,
accelerated
proton
transfer,
improved
performance
CO2RR.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 28, 2025
Electrocatalytic
dehalogenative
deuteration
is
a
sustainable
method
for
precise
deuteration,
whereas
its
Faradaic
efficiency
(FE)
limited
by
high
overpotential
and
severe
D2
evolution
reaction
(DER).
Here,
Cuδ+
site-adjusted
adsorption
crown
ether-reconfigured
interfacial
D2O
are
reported
to
cooperatively
increase
the
FE
of
up
84%
at
−100
mA
cm–2.
sites
strengthen
aryl
iodides,
promoting
mass
transfer
thus
accelerating
kinetics
toward
deuteration.
The
ethers
disrupt
hydration
effect
K·D2O
reconstruct
hydrogen
bond
with
D2O,
lowering
content
electric
double
layer
hindering
interaction
between
cathode,
inhibiting
competitive
DER.
A
linear
relationship
matched
sizes
alkali
metal
cations
demonstrated
universally
increasing
FEs.
This
also
suitable
various
halides
easily
reducible
functional
group
compatibility
improved
FEs
ACS Nano,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 14, 2025
Common
O-/H-down
orientation
of
H2O
molecules
on
electrocatalysts
brings
favorable
OH/H
delivery;
however,
adverse
H/OH
delivery
in
their
dissociation
process
hampers
the
kinetics
alkaline
hydrogen
evolution
reaction
(HER).
To
overcome
this
challenge,
we
raised
a
synergetic
concept
metal-supported
involving
efficient
OH
from
O-down
to
metal,
timely
proton
relay
metal
H-down
support
through
hydrogen-bond
network,
and
prompt
H
support.
After
theoretically
profiling
that
high
work
function
difference
between
(ΔΦ)
induces
strong
electric
field
at
metal–support
interface
increases
connectivity
promote
relay,
practiced
over
cobalt
phosphide-supported
ruthenium
(Ru/CoP)
catalysts
with
ΔΦ
=
0.4
eV,
achieving
record-high
Ru
utilization
HER
activity
66.1
A
mgRu–1
−0.1
V
vs
RHE.
The
insights
into
mechanism
provide
opportunity
for
design
bicomponent
electrocatalysts.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 15, 2025
The
electric
double
layer
(EDL),
which
is
directly
related
to
ions,
influences
the
electrocatalytic
performance.
However,
effects
of
anions
on
anodic
EDL
and
reaction
kinetics
are
unclear,
especially
in
water-mediated
electrosynthesis.
Here,
ClO4–
discovered
widen
inhibit
competitive
oxygen
evolution
(OER)
for
gram-scale
electrosynthesis
2-chlorocyclohexanol
with
a
90%
Faradaic
efficiency
(FE)
at
100
mA
cm–2.
combined
results
molecular
dynamics
simulations
situ
spectroscopies
provide
solid
evidence
widened
that
originates
from
repulsion
water
molecules
interface
by
ClO4–.
addition
has
negligible
effect
chlorination
because
electrostatic
interaction
between
anode
Cl–
but
obviously
suppresses
anode,
leading
high
FEs
increasing
energy
barrier
undesirable
OER.
In
addition,
this
method
suitable
other
reactions
enhanced
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
147(9), P. 8024 - 8031
Published: Feb. 20, 2025
Electrocatalytically
selective
chlorination
of
olefins
in
Cl--containing
solutions
is
a
sustainable
method
for
synthesizing
chlorohydrin/vicinal
dichloride;
however,
controlling
the
selectivity
challenging.
Here,
aqueous/dimethyl
carbonate
(DMC)
hybrid
electrolytes
with
different
H2O/DMC
ratios
are
designed
to
modulate
·OH
formation
increase
corresponding
selectivities.
The
combined
results
in/ex
situ
spectroscopies
and
molecular
dynamics
simulations
reveal
origin
high
selectivity.
TFSI-
shields
transportation
free
H2O
provide
moderate
synthesis
chlorohydrin.
DMC
reconstructs
hydrogen
bonds
minimize
interaction
between
them
anode,
matching
requirements
vicinal
dichloride
production.
Thus,
these
not
only
achieve
selectivities
80%
76%
chlorohydrin
dichloride,
respectively,
but
also
enable
other
isolated
yields
up
74%.
This
work
provides
facile
strategy
regulate
anodic
via
rational
electrolyte
design.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 4, 2025
Electrocatalysts
can
efficiently
convert
earth-abundant
simple
molecules
into
high-value-added
products.
In
this
context,
heterostructures,
which
are
largely
determined
by
the
interface,
have
emerged
as
a
pivotal
architecture
for
enhancing
activity
of
electrocatalysts.
review,
atomistic
understanding
heterostructured
electrocatalysts
is
considered,
focusing
on
reaction
kinetic
rate
and
electron
configuration,
gained
from
both
empirical
studies
theoretical
models.
We
start
fundamentals
microkinetic
model,
adsorption
energy
theory,
electric
double
layer
model.
The
importance
heterostructures
to
accelerate
electrochemical
processes
via
modulating
configuration
interfacial
reactive
microenvironment
highlighted,
considering
rectification,
space
charge
region,
built-in
field,
synergistic
interactions,
lattice
strain,
geometric
effect.
conclude
review
summarizing
challenges
perspectives
in
field
electrocatalysts,
such
determination
transition
state
energy,
their
dynamic
evolution,
refinement
approaches,
use
machine
learning.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Oct. 25, 2024
Abstract
Understanding
the
role
of
adsorbed
intermediates
at
polarized
catalyst‐electrolyte
interface
on
structure
electrical
double
layer
(EDL)
is
essential
for
developing
highly
efficient
electrocatalysts.
Here,
we
prepared
a
series
unconventional
face‐centered‐cubic
(
fcc
)
phase
Ru‐based
catalysts
(i.e.
‐Ru,
‐RuCr,
and
‐RuCrW)
by
rational
tuning
binding
energetics
hydroxyl
intermediate
to
engineer
electrochemical
boost
performance
alkaline
hydrogen
oxidation
reaction
(HOR).
The
introduction
oxyphilic
metals
Cr
W
can
regulate
orbital
occupation
Ru,
promote
adsorption
species,
resulting
in
an
anomalous
behavior
that
HOR
under
media
exceeds
acidic
media.
Experimental
results
theoretical
calculations
unravel
modulated
species
electrode
surface
are
responsible
reconstruction
interfacial
water
dynamic
evolution
free
molecules
from
nearest
above
gap
region
EDL,
thereby
leading
significantly
increased
connectivity
bond
network.
Our
work
reveals
new
understanding
controlling
process
bonding
network
electrocatalysis,
will
guide
design
advanced
electrocatalysts
through
engineering.
Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
136(17)
Published: Feb. 17, 2024
Abstract
Searching
for
highly
efficient
and
economical
electrocatalysts
alkaline
hydrogen
oxidation
reaction
(HOR)
is
crucial
the
development
of
polymer
membrane
fuel
cells.
Here,
we
report
a
valid
strategy
to
active
pyrite‐type
RuS
2
HOR
electrocatalysis
by
introducing
sulfur
vacancies.
The
obtained
S‐vacancies
modified
2−x
exhibits
outperformed
activity
with
current
density
0.676
mA
cm
−2
mass
1.43
μg
−1
,
which
are
15‐fold
40‐fold
improvement
than
those
Ru
catalyst.
In
situ
Raman
spectra
demonstrate
formation
S−H
bond
during
process,
identifying
S
atom
real
site
catalysis.
Density
functional
theory
calculations
experimental
results
including
in
surface‐enhanced
infrared
absorption
spectroscopy
suggest
introduction
vacancies
can
rationally
modify
p
orbital
atoms,
leading
enhanced
binding
strength
between
sites
H
atoms
on
surface
together
promoted
connectivity
hydrogen‐bonding
network
lowered
water
energy,
contributes
performance.
