Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 10, 2025
The
electrocatalytic
utilization
of
oxidized
nitrogen
waste
for
C-N
coupling
chemistry
is
an
exciting
research
area
with
great
potential
to
be
adopted
as
a
sustainable
method
generation
organonitrogen
molecules.
most
widely
used
reaction
reductive
amination.
In
this
work,
we
develop
alternative
electrochemical
amination
that
can
proceed
in
neutral
aqueous
electrolyte
nitrite
the
nitrogenous
reactant
and
via
oxime
intermediate.
We
selection
criterion
reduction
electrocatalysts
suited
electrosynthesis
and,
doing
so,
find
Pd
highly
efficient
catalyst
reaction,
reaching
Faradaic
efficiency
82%
at
-0.21
V
vs
reversible
hydrogen
electrode.
aliphatic
or
aromatic
structure
carbonyl
impacts
efficacy
catalyst,
substrates
leading
suppressed
formation
detrimental
alcohol.
developed
Pb/PbO
electrocatalyst
selectively
performs
electrolyte.
With
acetone
model
substrate,
demonstrate
one-pot,
two-step
conversion
isopropyl
amine
85%
yield
50%
global
efficiency.
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 16, 2024
Abstract
Urea
electrosynthesis
from
co‐electrolysis
of
CO
2
and
NO
3
−
(UECN)
offers
an
innovative
route
for
converting
waste
/NO
into
valuable
urea.
Herein,
Zn
single
atoms
anchored
on
oxygen
vacancy
(OV)‐rich
In
O
3‐x
(Zn
1
/In
)
are
developed
as
a
highly
active
selective
UECN
catalyst,
delivering
the
highest
urea
yield
rate
41.6
mmol
h
−1
g
urea‐Faradaic
efficiency
55.8%
at
−0.7
V
in
flow
cell,
superior
to
most
previously
reported
catalysts.
situ
spectroscopic
measurements
theoretical
calculations
unveil
synergy
In/Zn
sites
OVs
promoting
process
via
tandem
catalysis
mechanism,
where
‐OV
site
activates
form
*
NH
while
In‐OV
CO.
The
formed
spontaneously
migrates
nearby
then
couples
with
generate
CONH
which
is
ultimately
converted
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(28)
Опубликована: Янв. 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,
Год журнала:
2024,
Номер
63(15)
Опубликована: Янв. 16, 2024
Abstract
Chemical
manufacturing
utilizing
renewable
sources
and
energy
emerges
as
a
promising
path
towards
sustainability
carbon
neutrality.
The
electrocatalytic
reactions
involving
nitrogen
oxides
(NO
x
)
offered
potential
strategy
for
synthesizing
various
nitrogenous
chemicals.
However,
it
is
currently
hindered
by
low
selectivity/efficiency
limited
reaction
pathways,
mainly
due
to
the
difficulties
in
controllable
generation
utilization
of
intermediates.
In
this
minireview,
focusing
on
intermediates
NO
‐involved
reactions,
we
discuss
newly
developed
methodologies
studying
controlling
generation,
conversion,
intermediates,
which
enable
recent
developments
that
yield
products,
including
ammonia
(NH
3
),
organonitrogen
molecules,
compounds
exhibiting
unconventional
oxidation
states.
Furthermore,
also
make
an
outlook
highlight
future
directions
emerging
field
reactions.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(28)
Опубликована: Фев. 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.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(43)
Опубликована: Авг. 16, 2024
Abstract
Urea
electrosynthesis
from
co‐electrolysis
of
NO
3
−
and
CO
2
(UENC)
under
ambient
conditions
is
recognized
as
an
appealing
approach
for
effective
sustainable
urea
production,
while
it
requires
high‐efficiency
UENC
electrocatalysts
to
promote
the
C─N
coupling
hydrogenation
processes.
Herein,
single‐atom
Cu
anchored
on
MoS
(Cu
1
‐MoS
)
explored
a
highly
active
selective
catalyst.
Theoretical
calculations
operando
spectroscopic
characterizations
unveil
synergistic
tandem
catalysis
UENC,
where
single
atoms
trigger
early
coupling,
‐edges
key
step
*
NH
COOHNH
generation.
Strikingly,
equipped
in
flow
cell
achieves
excellent
performance
with
maximum
urea‐Faradaic
efficiency
57.02%
at
−0.6
V
corresponding
yield
rate
23.3
mmol
h
−1
g
,
surpassing
nearly
all
previously
reported
catalysts.
