Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Sept. 6, 2024
Abstract
Electrochemical
nitrate
reduction
reaction
(NO
3
RR)
is
emerging
as
a
promising
strategy
for
removal
and
ammonia
(NH
)
production
using
renewable
electricity.
Although
great
progresses
have
been
achieved,
the
crystal
phase
effect
of
electrocatalysts
on
NO
RR
remains
rarely
explored.
Here,
epitaxial
growth
unconventional
2H
Cu
hexagonal
close‐packed
(
hcp
IrNi
template,
resulting
in
formation
three
IrNiCu@Cu
nanostructures,
reported.
IrNiCu@Cu‐20
shows
superior
catalytic
performance,
with
NH
Faradaic
efficiency
(FE)
86%
at
−0.1
(vs
reversible
hydrogen
electrode
[RHE])
yield
rate
687.3
mmol
g
−1
h
,
far
better
than
common
face‐centered
cubic
Cu.
In
sharp
contrast,
IrNiCu@Cu‐30
IrNiCu@Cu‐50
covered
by
shell
display
high
selectivity
toward
nitrite
2
−
),
FE
above
60%
0.1
RHE).
Theoretical
calculations
demonstrated
that
has
optimal
electronic
structures
due
to
highest
d‐band
center
strongest
trend
lowest
energy
barriers.
The
electroactivity
originates
from
abundant
low
coordination
sites
surface,
which
guarantees
fast
electron
transfer
accelerate
intermediate
conversions.
This
work
provides
feasible
tactic
regulate
product
distribution
engineering
electrocatalysts.
Proceedings of the National Academy of Sciences,
Journal Year:
2023,
Volume and Issue:
120(50)
Published: Dec. 8, 2023
Zinc-nitrate
batteries
can
integrate
energy
supply,
ammonia
electrosynthesis,
and
sewage
disposal
into
one
electrochemical
device.
However,
current
zinc-nitrate
still
severely
suffer
from
the
limited
density
poor
rechargeability.
Here,
we
report
synthesis
of
tetraphenylporphyrin
(tpp)-modified
heterophase
(amorphous/crystalline)
rhodium-copper
alloy
metallenes
(RhCu
M-tpp).
Using
RhCu
M-tpp
as
a
bifunctional
catalyst
for
nitrate
reduction
reaction
(NO
ACS Nano,
Journal Year:
2023,
Volume and Issue:
17(3), P. 2992 - 3006
Published: Jan. 27, 2023
Rationally
combining
designed
supports
and
metal-based
nanomaterials
is
effective
to
synergize
their
respective
physicochemical
electrochemical
properties
for
developing
highly
active
stable/durable
electrocatalysts.
Accordingly,
in
this
work,
sub-5
nm
monodispersed
nanodots
(NDs)
with
the
special
nanostructure
of
an
ultrafine
Cu1Au1
core
a
2-3-atomic-layer
Cu1Pd3
shell
are
synthesized
by
facile
solvothermal
method,
which
further
evenly
firmly
anchored
onto
3D
porous
N-doped
graphene
nanosheets
(NGS)
via
simple
annealing
(A)
process.
The
as-obtained
Cu1Au1@Cu1Pd3
NDs/NGS-A
exhibits
exceptional
electrocatalytic
activity
noble-metal
utilization
toward
alkaline
oxygen
reduction,
methanol
oxidation,
ethanol
oxidation
reactions,
showing
dozens-fold
enhancements
compared
commercial
Pd/C
Pt/C.
Besides,
it
also
has
excellent
long-term
stability
durability.
Advanced
comprehensive
experimental
theoretical
analyses
unveil
synthetic
mechanism
core@shell
reveal
origins
significantly
enhanced
performance:
(1)
prominent
structural
NGS,
(2)
ultrasmall
size
as
well
uniform
morphology
NDs-A,
(3)
Cu-Au-Pd
alloy
subnanometer
shell,
(4)
strong
metal-support
interaction.
This
work
not
only
develops
method
fabricating
ultrafine-core@ultrathin-shell
but
proposes
practical
design
paradigm
comprehensively
rationally
considering
both
realizing
high-performance
multifunctional
electrocatalysts,
can
be
expanded
other
energy-conversion
or
environmental
(electro)catalytic
applications.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(21)
Published: Feb. 19, 2024
Abstract
The
inefficiency
of
Pt
and
Pd
benchmark
catalysts
in
achieving
complete
ethanol
oxidation,
coupled
with
their
inherent
susceptibility
to
poisoning,
poses
a
significant
obstacle
the
advancement
direct
fuel
cells.
In
this
study,
development
self‐supported
ultrathin
RhCuBi
trimetallenes,
demonstrating
exceptional
performance
electrooxidation
through
segregation
interface
engineering
is
presented.
distinctive
RhBi‐rich
crystalline/RhCu‐rich
amorphous
heterostructure
trimetallenes
creates
wealth
highly
active
interfacial
sites
for
oxidation
reaction
(EOR).
This
results
an
impressive
43.3%
Faradaic
efficiency
C1
pathway
peak
mass
activity
1.11
A
mg
Rh
−1
at
0.68
V
versus
reversible
hydrogen
electrode.
Moreover,
retain
60%
initial
after
8.5
h
constant
potential
electrolysis,
outperforming
commercial
(<3%).
In/ex
situ
infrared
spectroscopy
directly
reveals
generated
products
key
CH
3
CO*
intermediates
EOR
on
trimetallenes.
Theoretical
calculations
confirm
that
RhBi
alloy,
particularly
lattice‐stretched
crystalline/amorphous
sites,
facilitates
adsorption/activation
dehydrogenation
toward
EOR.
breakthrough
offers
promising
prospects
enhancing
stability
cell
applications.
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 9, 2025
Abstract
Multi‐metallic
catalysts
with
specific
structures
play
a
crucial
role
in
enhancing
the
selectivity
and
activity
of
chemical
reactions.
However,
challenges
such
as
unfavorable
alcohol
adsorption
on
catalysts,
CO
poisoning,
high
free
energy
barriers
during
oxidation
processes
pose
significant
obstacles
to
catalysts'
ability
cleave
C─C
bonds
for
complete
oxidation.
Here,
series
PdCuCo
metalene
electrocatalysts
is
reported,
wherein
varying
intermetallic
interactions
among
Pd,
Cu,
Co
effectively
modulate
pathway.
Notably,
catalyst
Pd
0.15
Cu
0.35
2
,
synthesized
by
galvanic
replacement
metallic
surface,
delivers
remarkably
electrocatalytic
ethylene
glycol
glycerol
alkaline
electrolytes
(9.7
10.9
A
mg
−1
respectively),
both
which
are
much
better
than
reported
broadly
applicable
various
alcohols.
High
performance
assigned
structural
advantages
material
synergistic
effects
multiple
metals.
This
synergy
not
merely
enhances
surface
electronics,
fostering
creation
exclusive
active
sites,
but
also
facilitates
oxidative
cleavage
stable
bond
efficient
ACS Materials Letters,
Journal Year:
2022,
Volume and Issue:
4(11), P. 2058 - 2079
Published: Sept. 26, 2022
The
electrocatalytic
carbon
dioxide
reduction
reaction
(CO2RR)
holds
great
potential
in
promoting
neutral
through
effectively
converting
CO2
molecules
to
useful
chemicals
and
fuels.
high-efficiency
electrochemical
conversion
of
single-carbon
products
has
been
well
realized,
while
more
efforts
are
needed
for
the
generation
high-value
multicarbon
products.
Metal–organic
frameworks
(MOFs),
featuring
porous
structures,
high
chemical
tunability,
ultralarge
surface
area,
have
attracted
increasing
attention
CO2RR.
Herein,
we
review
recent
progress
CO2RR
on
MOF-based
materials
toward
First,
structure
MOFs
is
briefly
introduced.
Then,
performance
corresponding
catalytic
mechanism
pristine
(classified
according
kind
organic
ligands/linkers)
MOF-derived
(including
metal
nanomaterials,
single-atom
catalysts
nanocomposites)
product
systematically
discussed.
Finally,
critical
challenges
opportunities
highlighted
inspire
rational
design
targeted
synthesis
advanced
high-performance
Advanced Science,
Journal Year:
2022,
Volume and Issue:
10(1)
Published: Nov. 18, 2022
Electro-organic
synthesis
has
attracted
a
lot
of
attention
in
pharmaceutical
science,
medicinal
chemistry,
and
future
industrial
applications
energy
storage
conversion.
To
date,
there
not
been
detailed
review
on
electro-organic
with
the
strategy
heterogeneous
catalysis.
In
this
review,
most
recent
advances
synthesizing
value-added
chemicals
by
catalysis
are
summarized.
An
overview
electrocatalytic
oxidation
reduction
processes
as
well
paired
electrocatalysis
is
provided,
anodic
alcohols
(monohydric
polyhydric),
aldehydes,
amines
discussed.
This
also
provides
in-depth
insight
into
cathodic
carboxylates,
carbon
dioxide,
CC,
C≡C,
reductive
coupling
reactions.
Moreover,
electro-synthesis
methods,
including
parallel
paired,
sequential
divergent
convergent
electrolysis,
Additionally,
strategies
developed
to
achieve
high
electrosynthesis
efficiency
associated
challenges
addressed.
It
believed
that
promising
direction
organic
electrochemistry,
offering
numerous
opportunities
develop
new
reaction
methods.
