Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(30)
Published: May 31, 2023
Abstract
The
conversion
of
industrial
exhaust
gases
nitrogen
oxides
into
high‐value
products
is
significantly
meaningful
for
global
environment
and
human
health.
And
green
synthesis
amino
acids
vital
biomedical
research
sustainable
development
mankind.
Herein,
we
demonstrate
an
innovative
approach
converting
nitric
oxide
(NO)
to
a
series
α‐amino
(over
13
kinds)
through
electrosynthesis
with
α‐keto
over
self‐standing
carbon
fiber
membrane
CoFe
alloy.
essential
leucine
exhibits
high
yield
115.4
μmol
h
−1
corresponding
Faradaic
efficiency
32.4
%,
gram
can
be
obtained
within
24
hours
in
lab
as
well
ultra‐long
stability
(>240
h)
the
catalyst,
which
could
convert
NO
NH
2
OH
rapidly
attacking
acid
subsequent
hydrogenation
form
acid.
In
addition,
this
method
also
suitable
other
sources
including
gaseous
or
liquidus
3
−
.
Therefore,
work
not
only
presents
promising
prospects
from
gas
nitrate‐laden
waste
water
products,
but
has
significant
implications
synthetizing
catalytic
science.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(45)
Published: Sept. 20, 2023
Pyridine
oximes
produced
from
aldehyde
or
ketone
with
hydroxylamine
(NH2
OH)
have
been
widely
applied
in
pharmaceutics,
enzymatic
and
sterilization.
However,
the
important
raw
material
NH2
OH
exhibits
corrosive
unstable
properties,
leading
to
substantial
energy
consumption
during
storage
transportation.
Herein,
this
work
presents
a
novel
method
for
directly
synthesizing
highly
valuable
pyridine
using
situ
generated
electrocatalytic
NO
reduction
well-design
nanofiber
membranes
(Al-NFM)
derived
-MIL-53(Al).
Particularly,
2-pyridinealdoxime,
precursor
of
antidote
pralidoxime
(2-PAM)
nerve
agents
suffering
scarcity
high
cost,
was
achieved
Faraday
efficiency
up
49.8
%
yield
92.1
%,
attributing
selectivity
production
on
Al-NFM,
further
easily
reacted
iodomethane
produce
2-PAM.
This
study
proposes
creative
approach,
having
wide
universality
other
range
functional
groups,
which
not
only
facilitates
conversion
exhaust
gas
(NO)
waste
water
(NO2-
)
into
chemicals
especially
utilization
through
electrochemistry,
but
also
holds
significant
potential
synthesis
neuro
detoxifying
drugs
humanity
security.
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.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(5), P. 3287 - 3297
Published: Feb. 15, 2024
Cyclohexanone
oxime
is
an
important
precursor
for
Nylon-6
and
typically
synthesized
via
the
nucleophilic
addition–elimination
of
hydroxylamine
with
cyclohexanone.
Current
technologies
production
are,
however,
not
environment-friendly
due
to
requirement
harsh
reaction
conditions.
Here,
we
report
electrochemical
method
one-pot
synthesis
cyclohexanone
under
ambient
conditions
aqueous
nitrate
as
nitrogen
source.
A
series
Zn–Cu
alloy
catalysts
are
developed
drive
reduction
nitrate,
where
intermediate
formed
in
electroreduction
process
can
undergo
a
chemical
present
electrolyte
produce
corresponding
oxime.
The
best
performance
achieved
on
Zn93Cu7
electrocatalyst
97%
yield
27%
Faradaic
efficiency
at
100
mA/cm2.
By
analyzing
catalytic
activities/selectivities
different
alloys
conducting
in-depth
mechanistic
studies
situ
Raman
spectroscopy
theoretical
calculations,
demonstrate
that
adsorption
species
plays
central
role
performance.
Overall,
this
work
provides
attractive
strategy
build
C–N
bond
organic
through
reduction,
while
highlighting
importance
controlling
surface
product
selectivity
electrosynthesis.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(15), P. 10573 - 10580
Published: April 3, 2024
Atomic
thick
two-dimensional
(2D)
materials
with
exciting
physical,
chemical,
and
electronic
properties
are
gaining
increasing
attention
in
next-generation
science
technology,
showing
great
promise
catalysis
energy
science.
However,
the
precise
design
synthesis
of
efficient
catalytic
systems
based
on
such
still
face
many
difficulties,
especially
how
to
control
preparation
structurally
determined,
highly
active,
atomic-scale
distribution
material
systems.
Here,
we
report
that
a
active
zerovalent
osmium
single-atom-layer
thickness
single
atom
size
has
been
successfully
controllably
self-organized
surface
2D
graphdiyne
(GDY)
material.
Detailed
characterizations
showed
incomplete
charge
transfer
effect
between
Os
atoms
GDY
not
only
stabilized
system
but
also
improved
intrinsic
activity,
making
Gibbs
free
reach
best
resulting
remarkable
performance
small
overpotential
49
mV
at
500
mA
cm–2,
large
specific
j0
18.6
turnover
frequency
3.89
H2
s–1
50
mV.
In
addition,
formation
sp-C–Os
bonds
guarantees
high
long-term
stability
800
h
current
density
cm–2
alkaline
simulated
seawater.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(15)
Published: Jan. 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.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(20), P. 13974 - 13982
Published: May 9, 2024
It
has
been
reported
that
it
was
selective
to
produce
ammonia
on
metallic
cobalt
in
the
electrocatalytic
nitric
oxide
reduction
reaction
(eNORR),
where
hexagonal
close-packed
(hcp)
outperforms
face-centered
cubic
(fcc)
cobalt.
However,
hydroxylamine
is
more
selectively
produced
a
single-atom
catalyst
(Co-SAC).
Herein,
we
uncover
structural
sensitivity
over
hcp-Co,
fcc-Co,
and
Co-SAC
eNORR
by
employing
recently
developed
constant
potential
simulation
method
microkinetic
modeling.
found
superior
activity
for
production
hcp-Co
can
be
attributed
its
facile
electron
proton
transfer
stronger
lateral
suppression
effect
from
NO*
fcc-Co.
The
exceptional
selectivity
due
modified
electronic
structure,
namely,
positively
charged
active
center.
favorable
NOH*
while
HNO*
preferable
Co-SAC,
which
are
firmly
correlated
with
vertical
strong
NO
adsorption
former
moderate
latter.
In
other
words,
key
factor
control
first
step
of
protonation.
Therefore,
local
structure
catalysts
critical
regulating
eNORR.
