Angewandte Chemie,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 24, 2024
Abstract
The
thermodynamically
and
kinetically
sluggish
electrocatalytic
C−N
coupling
from
CO
2
NO
3
−
is
inert
to
initially
take
place
while
typically
occurring
after
protonation,
which
severely
dwindles
urea
efficiency
carbon
atom
economy.
Herein,
we
report
a
single
O‐philic
adsorption
strategy
facilitate
initial
of
*OCO
subsequent
protonation
over
dual‐metal
hetero‐single‐atoms
in
N
−Fe−(N−B)
−Cu−N
coordination
mode
(FeN
4
/B
CuN
@NC),
greatly
inhibits
the
formation
C‐containing
byproducts
facilitates
electrosynthesis
an
unprecedented
C‐selectivity
97.1
%
with
yield
2072.5
μg
h
−1
mg
cat.
71.9
Faradaic
efficiency,
outperforming
state‐of‐the‐art
electrodes.
carbon‐directed
antibonding
interaction
Cu−B
elaborated
benefit
rather
than
conventional
C‐end
or
bridging
O,O‐end
modes,
can
accelerate
kinetics
initiated
protonation.
Theoretical
results
indicate
that
O‐monodentate
pathway
benefits
thermodynamics
*NO
rate‐determining
step,
markedly
direct
This
oriented
manipulating
reactant
patterns
initiate
specific
step
universal
moderate
oxophilic
transition
metals
offers
kinetic‐enhanced
path
for
multiple
conversion
processes.
Chemical Society Reviews,
Год журнала:
2024,
Номер
unknown
Опубликована: Янв. 1, 2024
This
review
focuses
on
the
synthesis
and
characterization
of
defective
electrocatalysts,
internal
correlation
between
defects
catalytic
activity,
development
application
electrocatalysts
in
various
fields.
ACS Energy Letters,
Год журнала:
2024,
Номер
9(9), С. 4624 - 4632
Опубликована: Авг. 30, 2024
Urea
electrosynthesis
by
coelectrolysis
of
NO3–
and
CO2
(UENC)
represents
a
promising
method
to
enable
efficient
sustainable
urea
production.
In
this
work,
isolated
Cu
alloyed
Ru
(Cu1Ru)
is
developed
as
highly
active
selective
UENC
catalyst.
Combined
theoretical
computations
in
situ
spectroscopic
measurements
reveal
the
synergistic
effect
Cu1–Ru
site
Ru–Ru
on
Cu1Ru
promote
via
tandem
catalysis
pathway,
which
drives
*NO2/CO2
coupling
followed
*CO2NO2-to-*CO2NH
step.
The
formed
*CO2NH
then
migrates
from
adjacent
promotes
*CO2NH⃗*CO2NH2
→
*COOHNH2
steps
toward
generation.
Impressively,
achieves
high
performance
flow
cell,
exhibiting
yield
rate
21.04
mmol
h–1
gcat–1
Faradaic
efficiency
51.27%
at
−0.6
V,
outperforming
most
reported
catalysts.
Abstract
The
escalating
accumulation
of
plastic
waste
has
been
developed
into
a
formidable
global
environmental
challenge.
Traditional
disposal
methods
such
as
landfilling
and
incineration
not
only
exacerbate
degradation
by
releasing
harmful
chemicals
greenhouse
gases,
but
also
squander
finite
resources
that
could
otherwise
be
recycled
or
repurposed.
Upcycling
is
kind
recycling
technology
converts
high‐value
helps
to
avoid
resource
pollution.
Electrocatalytic
upcycling
emerges
novel
distinguished
its
mild
operational
conditions,
high
transformation
efficiency
product
selectivity.
This
review
commences
with
an
overview
the
employed
in
management
respective
advantages
inherent
limitations
are
delineated.
different
types
upcycled
electrocatalytic
strategy
then
discussed
process
examined
together
mechanisms
underlying
upcycling.
Furthermore,
structure‐activity
relationships
between
electrocatalysts
performance
elucidated.
aims
furnish
readers
comprehensive
understanding
techniques
for
provide
guidance
design
towards
efficient
transformation.
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.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(26)
Опубликована: Апрель 10, 2024
Oxime
ethers
are
attractive
compounds
in
medicinal
scaffolds
due
to
the
biological
and
pharmaceutical
properties,
however,
crucial
widespread
step
of
industrial
oxime
formation
using
explosive
hydroxylamine
(NH
ACS Nano,
Год журнала:
2024,
Номер
18(35), С. 23894 - 23911
Опубликована: Авг. 20, 2024
The
C-N
coupling
reaction
demonstrates
broad
application
in
the
fabrication
of
a
wide
range
high
value-added
organonitrogen
molecules
including
fertilizers
(e.g.,
urea),
chemical
feedstocks
amines,
amides),
and
biomolecules
amino
acids).
electrocatalytic
pathways
from
waste
resources
like
CO
Achieving
a
precise
understanding
and
accurate
design
of
heterogeneous
catalysts
based
on
bioinspired
principles
is
challenging
yet
crucial
to
digging
out
optimal
materials
for
artificial
catalysis.
Here,
an
ADH-mimicking
dual-site
photocatalyst
(YCuCdS)
developed,
demonstrates
the
powerful
effects
atomic
site
configuration
proton
transfer
environments
alcohol-amine
coupling.
Mechanism
studies
reveal
that
alcohol
substrate
effectively
dehydrogenated
at
Y
sites,
forming
carbonyl
intermediates
rapidly
experience
condensation
with
amine.
Meanwhile,
released
hydrogen
species
(Hads)
migrate
from
adjacent
Cu
sites
active
S
atoms,
promoting
H2
production
hindering
over-hydrogenation
imine.
As
result,
high
imine
yield
92%
achieved,
along
rate
7400
µmol
g-1
h-1.
This
work
showcases
effective
strategy
bioinspiration.
