Angewandte Chemie International Edition,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 10, 2025
Relay
catalysis
represents
significant
efficacy
in
alleviating
competition
among
different
reactants
during
coupling
reactions.
However,
a
comprehensive
understanding
of
the
reaction
mechanism
underlying
relay
for
urea
electrosynthesis
remains
challenging.
Herein,
we
have
developed
catalyst
(CuAC-CuSA@NC)
comprising
Cu
atomic
clusters
(CuAC)
with
satellite
Cu─N4
single
atoms
(CuSA)
sites
on
nitrogen-doped
porous
interconnected
carbon
skeleton
(NC),
enabling
elucidation
process
co-reduction
CO2
and
NO3
-.
The
designed
CuAC-CuSA@NC
exhibits
an
approximately
threefold
higher
yield
rate
compared
to
that
CuSA@NC
at
-1.3
V
versus
RHE.
Ex-situ
experimental
results
in-situ
attenuated
total
reflection
surface-enhanced
infrared
absorption
spectroscopy
analysis
reveal
formation
sequence
between
*NH2
*NH2CO
species
increasing
reduction
potential.
combination
theoretical
calculations
further
elucidates
pathway
involves
"CuAC"
facilitating
conversion
*NO3
*NOx,
followed
by
hydrogenation
form
*H
from
water
dissociation
promoted
"CuSA"
sites,
which
subsequently
couples
*CO2
produce
urea.
This
work
provides
novel
insights
into
investigation
reactions,
but
not
limit
to,
synthesis.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Sept. 11, 2024
Abstract
Electrochemical
nitrate
reduction
reaction
(NO
3
RR)
is
a
promising
approach
to
realize
ammonia
generation
and
wastewater
treatment.
However,
the
transformation
from
NO
−
NH
involves
multiple
proton‐coupled
electron
transfer
processes
by‐products
2
,
H
etc.),
making
high
selectivity
challenge.
Herein,
two‐phase
nanoflower
P‐Cu/Co(OH)
electrocatalyst
consisting
of
P‐Cu
clusters
P‐Co(OH)
nanosheets
designed
match
two‐step
tandem
process
)
more
compatible,
avoiding
excessive
accumulation
optimizing
whole
reaction.
Focusing
on
initial
2e
process,
inhibited
*
desorption
Cu
sites
in
gives
rise
appropriate
released
electrolyte.
Subsequently,
exhibits
superior
capacity
for
trapping
transforming
desorbed
during
latter
6e
due
thermodynamic
advantage
contributions
active
hydrogen.
In
1
m
KOH
+
0.1
leads
yield
rate
42.63
mg
h
cm
Faradaic
efficiency
97.04%
at
−0.4
V
versus
reversible
hydrogen
electrode.
Such
well‐matched
achieves
remarkable
synthesis
performance
perspective
catalytic
reaction,
offering
novel
guideline
design
RR
electrocatalysts.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 8, 2025
Abstract
Nitrate
electroreduction
is
promising
for
achieving
effluent
waste‐water
treatment
and
ammonia
production
with
respect
to
the
global
nitrogen
balance.
However,
due
impeded
hydrogenation
process,
high
overpotentials
need
be
surmounted
during
nitrate
electroreduction,
causing
intensive
energy
consumption.
Herein,
a
hydroxide
regulation
strategy
developed
optimize
interfacial
H
2
O
behavior
accelerating
conversion
of
at
ultralow
overpotentials.
The
well‐designed
Ru─Ni(OH)
electrocatalyst
shows
remarkable
efficiency
44.6%
+0.1
V
versus
RHE
nearly
100%
Faradaic
NH
3
synthesis
0
RHE.
In
situ
characterizations
theoretical
calculations
indicate
that
Ni(OH)
can
regulate
structure
promoted
dissociation
process
contribute
spontaneous
hydrogen
spillover
boosting
NO
−
Ru
sites.
Furthermore,
assembled
rechargeable
Zn‐NO
/ethanol
battery
system
exhibits
an
outstanding
long‐term
cycling
stability
charge–discharge
tests
high‐value‐added
ammonium
acetate,
showing
great
potential
simultaneously
removal,
conversion,
chemical
synthesis.
This
work
not
only
provide
guidance
in
extensive
reactions
but
also
inspire
design
novel
hybrid
flow
multiple
functions.
Nature Communications,
Journal Year:
2025,
Volume and Issue:
16(1)
Published: Jan. 21, 2025
Renewable
energy-driven
electrocatalytic
nitrate
reduction
reaction
presents
a
low-carbon
and
sustainable
route
for
ammonia
synthesis
under
mild
conditions.
Yet,
the
practical
application
of
this
process
is
currently
hindered
by
unsatisfactory
activity
long-term
stability.
Herein
we
achieve
high-rate
electrosynthesis
using
stable
amorphous/crystalline
dual-phase
Cu
catalyst.
The
partial
current
density
formation
rate
reach
3.33
±
0.005
A
cm-2
15.5
0.02
mmol
h-1
at
low
cell
voltage
2.6
0.01
V,
respectively.
Remarkably,
catalyst
can
maintain
production
with
Faradaic
efficiency
around
90%
high
1.5
up
to
300
h.
scale-up
demonstration
an
electrode
size
100
cm2
achieves
as
11.9
0.5
g
total
160
A.
impressive
performance
ascribed
presence
amorphous
domains
which
promote
adsorption
hydrogenation
nitrogen-containing
intermediates,
thus
improving
kinetics
formation.
This
work
underscores
importance
stabilizing
metastable
structures
reactivity
Nature Communications,
Journal Year:
2025,
Volume and Issue:
16(1)
Published: Feb. 22, 2025
The
concept
of
precatalyst
is
widely
accepted
in
electrochemical
water
splitting,
but
the
role
activation
and
resulted
changes
electrolyte
composition
often
overlooked.
Here,
we
elucidate
impact
potential-dependent
for
both
using
Co2Mo3O8
as
a
model
system.
Potential-dependent
reconstruction
results
an
electrochemically
stable
Co(OH)2@Co2Mo3O8
catalyst
additional
Mo
dissolved
MoO42−
into
electrolyte.
Co(OH)2/Co2Mo3O8
interface
accelerates
Volmer
reaction
negative
potentials
induced
Mo2O72−
(from
MoO42−)
further
enhances
proton
adsorption
H2
desorption.
Leveraging
these
insights,
well-designed
MoO42−/Mo2O72−
modified
achieves
Faradaic
efficiency
99.9%
yield
1.85
mol
h−1
at
−0.4
V
versus
reversible
hydrogen
electrode
(RHE)
generation.
Moreover,
it
maintains
over
one
month
approximately
100
mA
cm−2,
highlighting
its
industrial
suitability.
This
work
underscores
significance
understanding
on
evolution
design.
properties
electrocatalysis
crucial
authors
report
efficient
transition
metal
production
by
manipulating
composition.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
147(9), P. 8012 - 8023
Published: Feb. 18, 2025
The
electrocatalytic
nitrite
reduction
(NO2RR)
converts
nitrogen-containing
pollutants
to
high-value
ammonia
(NH3)
under
ambient
conditions.
However,
its
multiple
intermediates
and
multielectron
coupled
proton
transfer
process
lead
low
activity
NH3
selectivity
for
the
existing
electrocatalysts.
Herein,
we
synthesize
a
solid-solution
copper-zinc
cyanamide
(Cu0.8Zn0.2NCN)
with
localized
structure
distortion
tailored
surface
electrostatic
potential,
allowing
asymmetric
binding
of
NO2-.
It
exhibits
outstanding
NO2RR
performance
Faradaic
efficiency
∼100%
an
yield
22
mg
h-1
cm-2,
among
best
such
process.
Theoretical
calculations
in
situ
spectroscopic
measurements
demonstrate
that
Cu-Zn
sites
coordinated
linear
polarized
[NCN]2-
could
transform
symmetric
[Cu-O-N-O-Cu]
CuNCN-NO2-
[Cu-N-O-Zn]
configuration
Cu0.8Zn0.2NCN-NO2-,
thus
enhancing
adsorption
bond
cleavage.
A
paired
electro-refinery
Cu0.8Zn0.2NCN
cathode
reaches
2000
mA
cm-2
at
2.36
V
remains
fully
operational
industrial-level
400
>140
h
production
rate
∼30
mgNH3
cm-2.
Our
work
opens
new
avenue
tailoring
potentials
using
strategy
advanced
electrocatalysis.
Advanced Science,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 17, 2025
Abstract
Electrochemical
nitrate
reduction
reaction
(NO
3
−
RR)
has
emerged
as
an
alternative
strategy
for
wastewater
treatment
and
ammonia
production
in
neutral
low‐concentration
nitrate.
However,
the
electrocatalyst
faces
challenge
of
limited
NO
distribution
deficient
active
hydrogen
(H
ads
)
on
catalyst
surface
resulting
from
low
concentration
difficulty
water
splitting
under
conditions.
Here,
a
Cu‐Co
dual
sites
tandem
synergistic
catalysis
mechanism
been
proposed
by
doping
Cu
into
CoP
to
facilitate
adsorption
conversion
accelerate
leading
significantly
high
RR
performance.
The
designed
Cu‐CoP
exhibits
yield
7.65
mg
h
−1
cm
−2
Faraday
efficiency
85.1%
at
−1.0
V
(10
m
M
),
which
is
highest
reported
data.
In
situ
characterization
theoretical
calculations
confirm
effect,
site
favors
activation
form
2
,
concurrently
modulates
electronic
structure
Co
with
optimized
H
enhanced
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 28, 2025
Electrochemical
nitrate
reduction
reaction
(eNO3-RR)
to
ammonia
(NH3)
holds
great
promise
for
the
green
treatment
of
NO3-
and
ambient
NH3
synthesis.
Although
Fe-based
electrocatalysts
have
emerged
as
promising
alternatives,
their
excellent
eNO3-RR-to-NH3
activity
is
usually
limited
harsh
alkaline
electrolytes
or
alloying
noble
metals
with
Fe
in
sustainable
neutral
electrolytes.
Herein,
we
demonstrate
an
unusual
self-triggering
localized
alkalinity
Co4Fe6
electrocatalyst
efficient
media,
which
breaks
down
conventional
pH-dependent
kinetics
restrictions
shows
a
98.6%
Faradaic
efficiency
(FE)
99.9%
selectivity
at
-0.69
V
vs
RHE.
The
synergetic
Co-Fe
dual
sites
were
demonstrated
enable
optimal
free
energies
species
balance
water
dissociation
protonation
adsorbed
NO2-.
Notably,
can
attain
high
current
density
100
mA
cm-2
FE
surpassing
96%
long-term
stability
over
500
h
membrane
electrode
assembly
(MEA)
electrolyzer.
This
work
provides
insight
into
tailoring
self-reinforced
local-alkalinity
on
alloy
thus
avoids
practical
upcycling
technology.
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 7, 2025
Abstract
The
NiFe‐based
layered
double
hydroxides
(LDH)
undergo
surface
reconstruction,
generating
metal
hydroxyl
oxides
that
act
as
active
species
during
the
alkaline
oxygen
evolution
reaction
(OER).
However,
sluggish
reconstruction
process
and
excessive
oxidation
at
higher
anodic
potentials
frustrate
OER
activity
stability.
Herein,
a
cation–anion
collaborative
coordination
strategy
is
harnessed
to
build
(Ni,
Fe)─S─Zn
structures
in
NiFe
LDH
on
nickel
foam
(S‐NiFeZn
LDH/NF),
which
lowers
energy
barrier
aids
forming
highly
β‐NiOOH
process.
Meanwhile,
also
optimize
adsorption
of
oxygen‐containing
intermediates,
enhancing
kinetics.
As
result,
S‐NiFeZn
LDH/NF
achieves
low
overpotentials
201
mV
10
mA
cm
−2
293
500
1.0
m
KOH.
Moreover,
cell
assembled
with
anode
commercial
NiMo
cathode
demonstrates
excellent
overall
water
splitting
activity,
voltages
1.62
1.81
V
KOH,
exhibits
ultralong‐term
durability
over
h
,
even
operating
stably
for
200
an
electrolyzer
under
industrial
conditions
(30%
KOH
80
°C).