Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(14), С. 10044 - 10051
Опубликована: Апрель 1, 2024
The
electrochemical
NO
reduction
reaction
(NORR)
is
a
promising
approach
for
both
nitrogen
cycle
regulation
and
ammonia
synthesis.
Due
to
the
relatively
low
concentration
of
source
poor
solubility
in
solution,
mass
transfer
limitation
serious
but
easily
overlooked
issue.
In
this
work,
porous
carbon-supported
ultrafine
Cu
clusters
grown
on
nanowire
arrays
(defined
as
Cu@Cu/C
NWAs)
are
prepared
low-concentration
NORR.
A
high
Faradaic
efficiency
(93.0%)
yield
rate
(1180.5
μg
h–1
cm–2)
realized
NWAs
at
−0.1
V
vs
reversible
hydrogen
electrode
(RHE),
which
far
superior
those
other
reported
performances
under
similar
conditions.
construction
carbon
support
can
effectively
decrease
diffusion
kinetics
promote
coverage
subsequent
highly
effective
conversion.
Moreover,
favorable
metal–support
interaction
between
enhances
adsorption
decreases
barrier
*HNO
formation
comparison
with
that
pure
NWAs.
Overall,
whole
NORR
be
fully
strengthened
concentrations.
ACS Nano,
Год журнала:
2022,
Номер
16(10), С. 15512 - 15527
Опубликована: Окт. 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.
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(4), С. 1590 - 1596
Опубликована: Янв. 1, 2023
Herein,
we
demonstrate
cobaloximes
as
a
bioinspired
molecular
platform
for
exclusive
ammonia
synthesis
via
electrocatalytic
NO
2
−
reduction
(eNO
RR),
which
attained
98.5%
faradaic
efficiency
(FE)
under
close-to-neutral
conditions.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(10), С. 6409 - 6421
Опубликована: Фев. 27, 2024
Green
ammonia
(NH3),
made
by
using
renewable
electricity
to
split
nearly
limitless
nitrogen
(N2)
molecules,
is
a
vital
platform
molecule
and
an
ideal
fuel
drive
the
sustainable
development
of
human
society
without
carbon
dioxide
emission.
The
NH3
electrosynthesis
field
currently
faces
dilemma
low
yield
rate
efficiency;
however,
decoupling
overlapping
issues
this
area
providing
guidelines
for
its
directions
are
not
trivial
because
it
involves
complex
reaction
process
multidisciplinary
entries
(for
example,
electrochemistry,
catalysis,
interfaces,
processes,
etc.).
In
Perspective,
we
introduce
classification
scheme
based
on
process,
namely,
direct
(N2
reduction
reaction)
indirect
(Li-mediated/plasma-enabled
electrosynthesis).
This
categorization
allows
us
finely
decouple
complicated
pathways
identify
specific
rate-determining
steps/bottleneck
each
synthesis
approach
such
as
N2
activation,
H2
evolution
side
reaction,
solid-electrolyte
interphase
engineering,
plasma
etc.
We
then
present
detailed
overview
latest
progresses
solving
these
core
in
terms
whole
electrochemical
system
covering
electrocatalysts,
electrodes,
electrolytes,
electrolyzers,
Finally,
discuss
research
focuses
promising
strategies
future
with
multiscale
perspective
atomistic
mechanisms,
nanoscale
microscale
electrodes/interfaces,
macroscale
electrolyzers/processes.
It
expected
that
Perspective
will
provide
readers
in-depth
understanding
bottleneck
insightful
guidance
designing
efficient
systems.
Abstract
Ammonia,
a
vital
component
in
the
synthesis
of
fertilizers,
plastics,
and
explosives,
is
traditionally
produced
via
energy‐intensive
environmentally
detrimental
Haber–Bosch
process.
Given
its
considerable
energy
consumption
significant
greenhouse
gas
emissions,
there
growing
shift
toward
electrocatalytic
ammonia
as
an
eco‐friendly
alternative.
However,
developing
efficient
electrocatalysts
capable
achieving
high
selectivity,
Faraday
efficiency,
yield
under
ambient
conditions
remains
challenge.
This
review
delves
into
decades‐long
research
synthesis,
highlighting
evolution
fundamental
principles,
theoretical
descriptors,
reaction
mechanisms.
An
in‐depth
analysis
nitrogen
reduction
(NRR)
nitrate
(NitRR)
provided,
with
focus
on
their
electrocatalysts.
Additionally,
theories
behind
electrocatalyst
design
for
are
examined,
including
Gibbs
free
approach,
Sabatier
principle,
d
‐band
center
theory,
orbital
spin
states.
The
culminates
comprehensive
overview
current
challenges
prospective
future
directions
development
NRR
NitRR,
paving
way
more
sustainable
methods
production.
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(14), С. 7455 - 7488
Опубликована: Янв. 1, 2024
Seawater
electrolysis
for
the
production
of
fuels
and
chemicals
involved
in
onshore
offshore
plants
powered
by
renewable
energies
offers
a
promising
avenue
unique
advantages
energy
environmental
sustainability.
Nevertheless,
seawater
presents
long-term
challenges
issues,
such
as
complex
composition,
potential
side
reactions,
deposition
poisoning
microorganisms
metal
ions,
well
corrosion,
thus
hindering
rapid
development
technology.
This
review
focuses
on
value-added
(hydrogen
beyond)
fine
through
electrolysis,
step
towards
sustainable
carbon
neutrality.
The
principle
related
are
first
introduced,
redox
reaction
mechanisms
summarized.
Strategies
operating
anodes
cathodes
including
application
chloride-
impurity-resistant
electrocatalysts/membranes
reviewed.
We
comprehensively
summarize
(hydrogen,
monoxide,
sulfur,
ammonia,
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(32)
Опубликована: Май 29, 2024
Abstract
Electrochemical
nitrate
reduction
reaction
(NO
3
RR)
is
a
promising
approach
to
achieve
remediation
of
nitrate‐polluted
wastewater
and
sustainable
production
ammonia.
However,
it
still
restricted
by
the
low
activity,
selectivity
Faraday
efficiency
for
ammonia
synthesis.
Herein,
we
propose
an
effective
strategy
modulate
electrolyte
microenvironment
in
electrical
double
layer
(EDL)
mediating
alkali
metal
cations
enhance
NO
RR
performance.
Taking
bulk
Cu
as
model
catalyst,
experimental
study
reveals
that
−
‐to‐NH
performance
different
electrolytes
follows
trend
Li
+
<Cs
<Na
<K
.
Theoretical
studies
illustrate
proton
transport
rate
activity
rate‐determining
step
2
)
increase
order
The
cation
effects
are
also
general
two
typical
nanostructured
catalysts
including
copper/cuprous
oxide
nickel
phosphides,
achieving
near‐100
%
Faradaic
over
99
conversion
NH
Furthermore,
demonstrate
can
be
converted
high‐purity
4
Cl
catalyst
K
‐containing
electrolyte.
