Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
63(3)
Published: Dec. 7, 2023
Abstract
Electrocatalytic
C−N
coupling
process
is
indeed
a
sustainable
alternative
for
direct
urea
synthesis
and
co‐upgrading
of
carbon
dioxide
nitrate
wastes.
However,
the
main
challenge
lies
in
unactivated
process.
Here,
we
proposed
strategy
intermediate
assembly
with
alkali
metal
cations
to
activate
at
electrode/electrolyte
interface.
Urea
activity
follows
trend
Li
+
<Na
<Cs
<K
.
In
presence
K
,
world‐record
performance
was
achieved
yield
rate
212.8±10.6
mmol
h
−1
g
on
single‐atom
Co
supported
TiO
2
catalyst
−0.80
V
versus
reversible
hydrogen
electrode.
Theoretical
calculations
operando
synchrotron‐radiation
Fourier
transform
infrared
measurements
revealed
that
energy
barriers
were
significantly
decreased
via
mediated
assembly.
By
applying
this
various
catalysts,
demonstrate
interface
universal
approach
boost
synthesis.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(28)
Published: Jan. 28, 2024
Abstract
Electrocatalytic
C‐N
coupling
reaction
is
regarded
as
a
promising
strategy
for
achieving
clean
and
sustainable
urea
production
by
coreducing
CO
2
nitrogen
species,
thus
contributing
to
carbon
neutrality
the
artificial
cycle.
However,
restricted
sluggish
adsorption
of
reactants,
competitive
side
reactions,
multistep
pathways,
electrochemical
suffers
from
low
yield
rate
selectivity
so
far.
In
order
comprehensively
improve
synthesis
performance,
it
crucial
develop
highly
efficient
catalysts
coupling.
this
article,
catalyst‐designing
strategies,
mechanisms,
fundamental
research
methods
are
reviewed.
For
coreduction
different
several
prevailing
mechanisms
discussed.
With
aim
establishing
standard
system,
fundamentals
electrocatalytic
introduced.
The
most
important
strategies
boosting
discussed,
including
heteroatom
doping,
vacancy
engineering,
crystal
facet
regulation,
atom‐scale
modulation,
alloying
heterostructure
construction.
Finally,
challenges
perspectives
proposed
future
industrial
applications
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(23)
Published: April 6, 2024
Abstract
The
development
of
a
methodology
for
synthesizing
value‐added
urea
(CO(NH
2
)
via
renewable
electricity‐driven
C−N
coupling
reaction
under
mild
conditions
is
highly
anticipated.
However,
the
complex
catalytic
active
sites
that
act
on
carbon
and
nitrogen
species
make
mechanism
unclear,
resulting
in
low
efficiency
from
co‐reduction
dioxide
(CO
nitrate
(NO
3
−
).
Herein,
we
propose
novel
tandem
catalyst
Mo‐PCN‐222(Co),
which
Mo
serve
to
facilitate
reduction
*NH
intermediate,
while
Co
enhance
CO
carbonic
oxide
(CO),
thus
synergistically
promoting
coupling.
synthesized
Mo‐PCN‐222(Co)
exhibited
noteworthy
yield
rate
844.11
mg
h
−1
g
,
alongside
corresponding
Faradaic
33.90
%
at
−0.4
V
vs.
reversible
hydrogen
electrode
(RHE).
By
combining
situ
spectroscopic
techniques
with
density
functional
theory
calculations,
demonstrate
efficient
attributed
system
*CO
intermediates
produced
by
stabilize
formation
*CONH
intermediate.
This
study
provides
an
effective
avenue
design
synthesis
catalysts
electrocatalytic
synthesis.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(18)
Published: Jan. 25, 2024
The
artificial
disturbance
in
the
nitrogen
cycle
has
necessitated
an
urgent
need
for
nitric
oxide
(NO)
removal.
Electrochemical
technologies
NO
conversion
have
gained
increasing
attention
recent
years.
This
comprehensive
review
presents
advancements
selective
electrocatalytic
of
to
high
value-added
chemicals,
with
specific
emphasis
on
catalyst
design,
electrolyte
composition,
mass
diffusion,
and
adsorption
energies
key
intermediate
species.
Furthermore,
explores
synergistic
electrochemical
co-electrolysis
carbon
source
molecules,
enabling
synthesis
a
range
valuable
chemicals
C─N
bonds.
It
also
provides
in-depth
insights
into
intricate
reaction
pathways
underlying
mechanisms,
offering
perspectives
challenges
prospects
electrolysis.
By
advancing
comprehension
fostering
awareness
balance,
this
contributes
development
efficient
sustainable
systems
from
NO.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(5), P. 1950 - 1960
Published: Jan. 1, 2024
An
oxygen-coordinated
cobalt
single-atom
catalyst
was
successfully
fabricated,
exhibiting
exceptional
electrocatalytic
activity
toward
urea
and
H
2
O
production.
Subsequently,
the
value-added
peroxide
efficiently
synthesized.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(28)
Published: Feb. 21, 2024
Abstract
Electrocatalytic
C−N
couplings
are
promising
alternatives
to
construct
bonds
and
synthesize
vital
chemicals,
including
amine,
amide,
amino
acid,
oxime,
imine,
nitrile,
under
ambient
conditions.
In
recent
years,
the
electrocatalytic
coupling
has
attracted
a
wide
range
of
research
interest
achieved
considerable
developments.
Here,
is
systematically
reviewed
aiming
at
reductive
cathode
oxidative
anode.
cathodic
part,
reaction
systems,
corresponding
design
principles
electrocatalysts
for
different
mechanism
studies
from
experimental
theoretical
aspects,
application‐oriented
devices
summarized.
Anodic
offers
potential
approach
replace
conventional
energy‐demand
synthesis
protocols,
an
indispensable
part
green
controllable
construction
unsaturated
C
=
N
C≡N
bonds.
According
principle
that
electron
transfer
crucial
point
in
anodic
coupling,
reactions
sorted
out
based
on
direct
indirect
paths,
respectively.
Finally,
challenges
outlooks
this
field
proposed.
appealing
topic
electrochemistry
possesses
infinite
possibilities
future.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(32)
Published: June 3, 2024
Abstract
Directly
coupling
N
2
and
CO
to
synthesize
urea
by
photocatalysis
paves
a
sustainable
route
for
synthesis,
but
its
performance
is
limited
the
competition
of
photogenerated
electrons
between
,
as
well
underutilized
holes.
Herein,
we
report
an
efficient
synthesis
process
involving
holes
in
respectively
converting
over
redox
heterojunction
consisting
WO
3
Ni
single‐atom‐decorated
CdS
(Ni
1
‐CdS/WO
).
For
photocatalytic
from
pure
water,
attained
yield
rate
78
μM
h
−1
apparent
quantum
0.15
%
at
385
nm,
which
ranked
among
best
reported.
Mechanistic
studies
reveal
that
was
converted
into
NO
species
⋅OH
radicals
generated
component,
meanwhile,
transformed
*CO
site
electrons.
The
were
further
coupled
form
*OCNO
intermediate,
then
gradually
urea.
This
work
emphasizes
importance
reasonably
utilizing
reduction
reactions.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(11), P. 3739 - 3752
Published: Jan. 1, 2024
The
minireview
highlights
recent
developments
in
designing
electrocatalysts
for
the
co-reduction
of
CO
2
and
nitrates
into
urea.
It
also
discusses
advanced
detection
methods
intermediates
final
products,
as
well
future
research
prospects.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(14), P. 5183 - 5190
Published: Jan. 1, 2024
A
novel
Ru–Cu
9
Bi/CNT
multi-site
alloy
is
synthesised
for
electrocatalytic
C–N
coupling
to
generate
urea
across
a
broad
range
of
NO
3
−
concentrations.
By
improving
the
coverage
key
intermediate
*NHO,
ensure
subsequent
electrosynthesis
urea.
