Abstract
Ammonia
production
by
electrocatalytic
nitrate
reduction
reaction
(NO
3
RR)
in
water
streams
is
anticipated
as
a
zero‐carbon
route.
Limited
dilute
natural
sewage
and
the
electrostatic
repulsion
between
NO
−
cathode,
RR
can
hardly
be
achieved
energy‐efficiently.
The
hydrophilic
Cu@CuCoO
2
nano‐island
dispersed
on
support
enrich
produce
sensitive
current
response,
followed
electrosynthesis
of
ammonia
through
atomic
hydrogen
(*H)
reported.
accumulated
partially
converted
to
without
external
electric
field
input,
confirming
that
strongly
bind
then
trigger
via
dynamic
evolution
Cu–Co
redox
sites.
Through
identification
intermediates
theoretical
computation.
it
found
N‐side
hydrogenation
*NO
optimal
step,
formation
N─N
dimer
may
prevented.
An
NH
product
selectivity
93.5%,
conversion
96.1%,
an
energy
consumption
0.079
kWh
g
NH3
−1
obtained
48.9
mg‐N
L
naturally
nitrate‐polluted
streams,
which
outperforms
many
works
using
such
influent.
Conclusively,
system
provides
platform
guarantee
self‐sufficiency
agricultural
regions.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(43)
Опубликована: Июнь 25, 2023
Abstract
Ammonia
as
an
irreplaceable
chemical
has
been
widely
demanded
to
keep
the
sustainable
development
of
modern
society.
However,
its
industrial
production
consumes
huge
energy
and
releases
extraordinary
green‐house
gases,
leading
various
environmental
issues.
To
achieve
green
ammonia
is
a
great
challenge
that
extensively
pursued
recently.
In
review,
most
promising
strategy,
electrochemical
nitrate
reduction
reaction
(e‐NO
3
RR)
for
purpose
comprehensively
investigated
give
full
understanding
mechanism
provide
guidance
future
directions.
Particularly,
electrocatalysts
focused
realize
high
yield
rate
Faraday
efficiency
applications.
The
recent‐developed
catalysts,
including
noble
metallic
materials,
alloys,
metal
compounds,
single‐metal‐atom
metal‐free
are
systematically
discussed
review
effects
factors
on
catalytic
performance
in
e‐NO
RR.
Accordingly,
strategies,
defects
engineering,
coordination
environment
modulating,
surface
controlling,
hybridization,
carefully
improve
performance,
such
intrinsic
activity
selectivity.
Finally,
perspectives
challenges
given
out.
This
shall
insightful
advanced
systems
efficiently
industry.
Inorganic Chemistry Frontiers,
Год журнала:
2023,
Номер
10(12), С. 3489 - 3514
Опубликована: Янв. 1, 2023
Ammonia
(NH3)
is
an
essential
raw
material
in
the
production
of
fertilizers
and
a
promising
carbon-free
energy
carrier,
however,
its
synthesis
still
depends
on
energy-
capital-intensive
Haber–Bosch
process.
Recently,
electrochemical
N2
reduction
reaction
has
attracted
significant
interest
as
emerging
method
for
NH3
under
ambient
conditions.
However,
limited
solubility
aqueous
electrolyte
strong
NN
bonds
result
low
yield
rate,
inferior
faradaic
efficiency
unsatisfactory
selectivity,
impeding
further
practical
application.
Considering
high
water
nitrate
(NO3−),
NO3−
(NO3−RR)
become
fascinating
route
achieving
sustainable
NH3,
enormous
progress
been
made
this
field.
As
consequence,
review
discusses
mechanism
systematically
summarizes
recent
development
electrocatalysts
NO3−RR,
including
noble-metal-based
materials,
single-atom
metal
catalysts,
transition-metal-based
catalysts.
Diverse
design
strategies
catalysts
to
boost
NO3−RR
performance,
such
defect
engineering,
rational
structure
design,
strain
engineering
constructing
heterostructures,
are
discussed.
This
followed
by
illustration
how
robust
understanding
optimization
affords
fundamental
insights
into
efficiency,
selectivity
electrocatalysts.
Finally,
we
conclude
with
future
perspectives
critical
issues,
challenges
research
directions
high-efficiency
selective
NH3.
Industrial
ammonia
production
mainly
relies
on
the
conventional
Haber–Bosch
process
accompanied
by
high
energy
consumption
and
plentiful
carbon
dioxide
emissions,
which
triggered
recent
interest
to
explore
more
energy‐efficient
environmentally
benign
alternatives.
Very
recently,
electrochemical
nitrite
reduction
in
an
aqueous
medium
promises
new
opportunities
for
advanced,
energy‐efficient,
sustainable
at
ambient
conditions.
The
formation
rate
Faradic
efficiency
are
strongly
associated
with
adopted
electrocatalysts;
therefore,
striving
high‐efficient
electrocatalysts
is
key
via
reaction.
Herein,
a
critical
overview
of
advances
reaction
presented,
highlighting
latest
innovative
heterogenous
including
noble
metal
catalysts,
transition‐metal‐based
their
compounds.
Meanwhile,
possible
pathway
electroreduction
ammonia,
detection,
catalytic
activity
descriptor
briefly
summarized.
Finally,
perspective
research
challenges
that
convert
outlined,
increasing
contributions
route
realizing
neutral
footprint.
Regulating
electronic
structures
of
the
active
site
by
manipulating
local
coordination
is
one
advantageous
means
to
improve
photocatalytic
hydrogen
evolution
(PHE)
kinetics.
Herein,
ZnIn2
S4
/Mo2
TiC2
Schottky
junctions
are
designed
be
constructed
through
interfacial
In3+
with
electronegative
O
terminal
group
on
Mo2
based
different
work
functions.
Kelvin
probe
force
microscopy
and
charge
density
difference
reveal
that
an
unidirectional
transport
channel
across
interface
from
established
formed
nucleophilic/electrophilic
region.
The
increased
electron
inhibits
backflow
electrons,
boosts
transfer
separation,
optimizes
adsorption
energy.
Therefore,
photocatalyst
exhibits
a
superior
PHE
rate
3.12
mmol
g-1
h-1
under
visible
light,
reaching
3.03
times
pristine
.
This
provides
some
insights
inspiration
for
preparing
MXene-based
catalysts
accelerate
Ammonia
(NH3
)
is
an
indispensable
feedstock
for
fertilizer
production
and
one
of
the
most
ideal
green
hydrogen
rich
fuel.
Electrochemical
nitrate
(NO3-
reduction
reaction
RR)
being
explored
as
a
promising
strategy
to
synthesize
industrial-scale
NH3
,
which
has
nonetheless
involved
complex
multi-reaction
process.
This
work
presents
Pd-doped
Co3
O4
nanoarray
on
titanium
mesh
(Pd-Co3
/TM)
electrode
highly
efficient
selective
electrocatalytic
NO3-
RR
at
low
onset
potential.
The
well-designed
Pd-Co3
/TM
delivers
large
yield
745.6
µmol
h-1
cm-2
extremely
high
Faradaic
efficiency
(FE)
98.7%
-0.3
V
with
strong
stability.
These
calculations
further
indicate
that
doping
Pd
improves
adsorption
characteristic
optimizes
free
energies
intermediates,
thereby
facilitating
kinetics
reaction.
Furthermore,
assembling
this
catalyst
in
Zn-NO3-
battery
realizes
power
density
3.9
mW
excellent
FE
98.8%
.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(50)
Опубликована: Авг. 27, 2023
Abstract
Single‐atom
catalysts
(SACs)
are
desirable
in
environmental
catalysis
due
to
friendliness,
structural
stability,
and
maximum
utilization
of
active
metal
sites.
Extensive
research
has
compared
the
catalytic
performance
between
SACs
with
different
single‐atom
metals.
However,
their
is
also
highly
dependent
on
supports,
which
play
an
important
role
modulating
local
coordination
environment
SACs.
Unfortunately,
a
comprehensive
review
that
systematically
discusses
relationship
supports
environment,
as
well
combined
effects
scare.
In
this
review,
three
widely
investigated
applications
including
advanced
oxidation
processes
(AOPs),
mainly
Fenton
Fenton‐like
reactions,
nitrate
reduction
reaction
(NO
3
RR)
focused.
By
correlating
characterization
results,
performances,
computational
environments
reactivity
examined
detail,
from
origin
pathways
AOPs
NO
RR
attempted
reveal.
Finally
look
forward
for
potential
opportunities
challenges
on‐demand
applications,
provided.
Advanced Materials,
Год журнала:
2024,
Номер
36(29)
Опубликована: Апрель 29, 2024
Abstract
The
development
of
high‐performance
electrocatalysts
for
energy
conversion
reactions
is
crucial
advancing
global
sustainability.
design
catalysts
based
on
their
electronic
properties
(e.g.,
work
function)
has
gained
significant
attention
recently.
Although
numerous
reviews
electrocatalysis
have
been
provided,
no
such
reports
function‐guided
electrocatalyst
are
available.
Herein,
a
comprehensive
summary
the
latest
advancements
in
diverse
electrochemical
applications
provided.
This
includes
function‐based
catalytic
activity
descriptors,
and
both
monolithic
heterostructural
catalysts.
measurement
function
first
discussed
descriptors
various
fully
analyzed.
Subsequently,
function‐regulated
material‐electrolyte
interfacial
electron
transfer
(IET)
employed
catalyst
design,
methods
regulating
optimizing
performance
discussed.
In
addition,
key
strategies
tuning
function‐governed
material‐material
IET
examined.
Finally,
perspectives
determination,
put
forward
to
guide
future
research.
paves
way
rational
efficient
sustainable
applications.
Advanced Materials,
Год журнала:
2024,
Номер
36(25)
Опубликована: Апрель 2, 2024
Abstract
Renewable
electricity‐powered
nitrate/carbon
dioxide
co‐reduction
reaction
toward
urea
production
paves
an
attractive
alternative
to
industrial
processes
and
offers
a
clean
on‐site
approach
closing
the
global
nitrogen
cycle.
However,
its
large‐scale
implantation
is
severely
impeded
by
challenging
C–N
coupling
requires
electrocatalysts
with
high
activity/selectivity.
Here,
cobalt‐nanoparticles
anchored
on
carbon
nanosheet
(Co
NPs@C)
are
proposed
as
catalyst
electrode
boost
yield
Faradaic
efficiency
(FE)
electrosynthesis
enhanced
coupling.
Such
Co
NPs@C
renders
superb
urea‐producing
activity
FE
reaching
54.3%
of
2217.5
µg
h
−1
mg
cat.
,
much
superior
NPs
C
counterparts,
meanwhile
shows
strong
stability.
The
affords
rich
catalytically
active
sites,
fast
reactant
diffusion,
sufficient
catalytic
surfaces‐electrolyte
contacts
favored
charge
ion
transfer
efficiencies.
theoretical
calculations
reveal
that
high‐rate
formation
*CO
*NH
2
intermediates
crucial
for
facilitating
synthesis.
