Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
14(8)
Published: Dec. 22, 2023
Abstract
Conversion
of
air
and
water
into
valuable
chemicals
ammonia
(NH
3
)
by
plasma
activation
electrochemical
reduction
is
a
promising
approach
to
achieve
zero
carbon‐emission
synthesis
NH
.
However,
designing
highly
efficient
catalysts
one
the
key
challenges
in
accomplishing
this
strategy.
Herein,
self‐supported
cobalt–tungsten
alloy
supported
on
cobalt
foam
(CoW/CF)
developed
via
simple
method
at
room
temperature.
Surprisingly,
catalyst
exhibits
ultra‐high
partial
current
density
(1559
mA
cm
−2
),
superior
yield
rate
(164.3
mg
h
−1
high
Faradaic
efficiency
(98.1%)
under
condition
0.2
M
nitrate/nitrite,
outperforming
most
reported
values
electrosynthesis
knowledge.
The
introduction
W
makes
Co
atom
surface
electron
deficient,
which
can
enhance
adsorption
NO
x
−
mitigate
excessive
bonding
hydroxyl
radicals
(OH
*
generated
during
nitrite
(NO
2
hydrogenation,
thereby
reducing
energy
barrier
potential‐determining
step.
More
interestingly,
scale‐up
reaction
system
established,
achieving
an
4.771
g
successfully
converting
solution
solid
4
Cl.
aforementioned
progress
significantly
enhances
facilitation
industrialization.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(35), P. 16006 - 16011
Published: July 29, 2022
Formic
acid
(HCOOH)
can
be
exclusively
prepared
through
CO2
electroreduction
at
an
industrial
current
density
(0.5
A
cm–2).
However,
the
global
annual
demand
for
formic
is
only
∼1
million
tons,
far
less
than
emission
scale.
The
exploration
of
economical
and
green
approach
to
upgrading
CO2-derived
significant.
Here,
we
report
electrochemical
process
convert
nitrite
into
high-valued
formamide
over
a
copper
catalyst
under
ambient
conditions,
which
offers
selectivity
from
up
90.0%.
Isotope-labeled
in
situ
attenuated
total
reflection
surface-enhanced
infrared
absorption
spectroscopy
quasi
electron
paramagnetic
resonance
results
reveal
key
C–N
bond
formation
coupling
*CHO
*NH2
intermediates.
This
work
strategy
upgrade
high-value
formamide.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
62(5)
Published: Dec. 5, 2022
We
propose
the
pseudobrookite
Fe2
TiO5
nanofiber
with
abundant
oxygen
vacancies
as
a
new
electrocatalyst
to
ambiently
reduce
nitrate
ammonia.
Such
catalyst
achieves
large
NH3
yield
of
0.73
mmol
h-1
mg-1cat.
and
high
Faradaic
Efficiency
(FE)
87.6
%
in
phosphate
buffer
saline
solution
0.1
M
NaNO3
,
which
is
lifted
1.36
96.06
at
-0.9
V
vs.
RHE
for
nitrite
conversion
ammonia
NaNO2
.
It
also
shows
excellent
electrochemical
durability
structural
stability.
Theoretical
calculation
reveals
enhanced
conductivity
this
an
extremely
low
free
energy
-0.28
eV
adsorption
presence
vacant
oxygen.
ACS Nano,
Journal Year:
2022,
Volume and Issue:
16(10), P. 15512 - 15527
Published: Oct. 14, 2022
Artificial
nitrogen
conversion
reactions,
such
as
the
production
of
ammonia
via
dinitrogen
or
nitrate
reduction
and
synthesis
organonitrogen
compounds
C–N
coupling,
play
a
pivotal
role
in
modern
life.
As
alternatives
to
traditional
industrial
processes
that
are
energy-
carbon-emission-intensive,
electrocatalytic
reactions
under
mild
conditions
have
attracted
significant
research
interests.
However,
electrosynthesis
process
still
suffers
from
low
product
yield
Faradaic
efficiency,
which
highlight
importance
developing
efficient
catalysts.
In
contrast
transition-metal-based
catalysts
been
widely
studied,
p-block-element-based
recently
shown
promising
performance
because
their
intriguing
physiochemical
properties
intrinsically
poor
hydrogen
adsorption
ability.
this
Perspective,
we
summarize
latest
breakthroughs
development
electrocatalysts
toward
applications,
including
N2
urea
using
nitrogen-containing
feedstocks
carbon
dioxide.
The
catalyst
design
strategies
underlying
reaction
mechanisms
discussed.
Finally,
major
challenges
opportunities
future
directions
also
proposed.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(19), P. 13527 - 13535
Published: May 1, 2024
Closing
the
carbon
and
nitrogen
cycles
by
electrochemical
methods
using
renewable
energy
to
convert
abundant
or
harmful
feedstocks
into
high-value
C-
N-containing
chemicals
has
potential
transform
global
landscape.
However,
efficient
conversion
avenues
have
date
been
mostly
realized
for
independent
reduction
of
CO2
NO3–.
The
synthesis
more
complex
C–N
compounds
still
suffers
from
low
efficiency
due
inability
find
effective
catalysts.
To
this
end,
here
we
present
amorphous
bismuth–tin
oxide
nanosheets,
which
effectively
reduce
barrier
catalytic
reaction,
facilitating
highly
selective
urea
production.
With
enhanced
adsorption
activation
on
catalyst,
a
coupling
pathway
based
*CO2
rather
than
traditional
*CO
is
realized.
optimized
orbital
symmetry
(*CO2)
(*NO2)
intermediates
promotes
significant
increase
in
Faraday
production
an
outstanding
value
78.36%
at
−0.4
V
vs
RHE.
In
parallel,
selectivity
formation
also
90.41%
95.39%,
respectively.
results
insights
provide
valuable
reference
further
development
new
catalysts
CO2.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(18)
Published: Feb. 15, 2024
Abstract
Environmentally
friendly
electrocatalytic
coupling
of
CO
2
and
N
for
urea
synthesis
is
a
promising
strategy.
However,
it
still
facing
problems
such
as
low
yield
well
stability.
Here,
new
carbon‐coated
liquid
alloy
catalyst,
Ga
79
Cu
11
Mo
10
@C
designed
efficient
electrochemical
by
activating
active
sites.
During
the
co‐reduction
process,
reaches
28.25
mmol
h
−1
g
,
which
highest
reported
so
far
under
same
conditions,
Faraday
efficiency
(FE)
also
high
60.6
%
at
−0.4
V
vs.
RHE.
In
addition,
catalyst
shows
excellent
stability
100
testing.
Comprehensive
analyses
showed
that
sequential
exposure
density
sites
promoted
adsorption
activation
reactions.
This
reaction
occurs
through
thermodynamic
spontaneous
between
*N=N*
to
form
C−N
bond.
The
deformability
state
facilitates
recovery
enhances
resistance
poisoning.
Moreover,
introduction
stimulates
sites,
successfully
synthesises
*NCON*
intermediate.
energy
barrier
third
proton‐coupled
electron
transfer
process
rate‐determining
step
(RDS)
*NHCONH→*NHCONH
was
lowered,
ensuring
urea.
