Trends in Microbiology,
Год журнала:
2023,
Номер
32(6), С. 554 - 564
Опубликована: Апрель 13, 2023
The
evolution
of
nitrogen
fixation
undoubtedly
altered
nearly
all
corners
the
biosphere,
given
essential
role
in
synthesis
biomass.
To
date,
there
is
no
unified
view
on
what
planetary
conditions
gave
rise
to
or
how
these
have
sustained
it
evolutionarily.
Intriguingly,
concentrations
metals
that
nitrogenases
require
function
changed
throughout
Earth's
history.
In
this
review,
we
describe
interconnection
metal
and
cycles
with
nitrogenase
importance
ancient
ecology
formation
modern
cycle.
We
argue
exploration
cycle's
deep
past
will
provide
insights
into
humanity's
immediate
environmental
challenges
centered
availability.
Advanced Materials,
Год журнала:
2023,
Номер
35(46)
Опубликована: Июль 25, 2023
The
electrocatalytic
reduction
of
nitrate
(NO3-
)
to
nitrogen
(N2
is
an
environmentally
friendly
approach
for
efficient
N-cycle
management
(toward
a
nitrogen-neutral
cycle).
However,
poor
catalyst
durability
and
the
competitive
hydrogen
evolution
reaction
significantly
impede
its
practical
application.
Interface-chemistry
engineering,
utilizing
close
relationship
between
surface/interface
microenvironment
electron/proton
transfer
process,
has
facilitated
development
catalysts
with
high
intrinsic
activity
physicochemical
durability.
This
study
reports
synthesis
nitrogen-doped
carbon-coated
rice-like
iron
nitride
(RL-Fe2
N@NC)
electrocatalyst
excellent
nitrate-reduction
(high
N2
selectivity
(≈96%)
NO3-
conversion
(≈86%)).
According
detailed
mechanistic
investigations
by
in
situ
tests
theoretical
calculations,
strong
hydrogenation
ability
enhanced
enrichment
system
synergistically
contribute
rapid
nitrogen-containing
species,
increasing
reducing
occurrence
competing
hydrogen-evolution
side
reaction.
Moreover,
RL-Fe2
N@NC
shows
stability,
retaining
good
-to-N2
electrocatalysis
more
than
40
cycles
(one
cycle
per
day).
paper
could
guide
interfacial
design
Fe-based
composite
nanostructures
reduction,
facilitating
shift
toward
neutrality.
Environmental Science & Technology,
Год журнала:
2022,
Номер
56(16), С. 11602 - 11613
Опубликована: Июль 21, 2022
Electrochemically
upcycling
wastewater
nitrogen
such
as
nitrate
(NO3–)
and
nitrite
(NO2–)
into
an
ammonia
fertilizer
is
a
promising
yet
challenging
research
topic
in
resource
recovery
treatment.
This
study
presents
electrified
membrane
made
of
CuO@Cu
foam
polytetrafluoroethylene
(PTFE)
for
reducing
NO3–
to
(NH3)
NH3
(NH4)2SO4,
liquid
ready-use.
A
paired
electrolysis
process
without
external
acid/base
consumption
was
achieved
under
partial
current
density
63.8
±
4.4
mA·cm–2
on
the
cathodic
membrane,
which
removed
99.9%
feed
(150
mM
NO3–)
after
5
h
operation
with
rate
99.5%.
energy
3100
91
g-(NH4)2SO4·m–2·d–1
21.8
3.8
kWh·kg–1-(NH4)2SO4,
respectively,
almost
outcompete
industrial
production
cost
Haber–Bosch
process.
Density
functional
theory
(DFT)
calculations
unraveled
that
situ
electrochemical
conversion
Cu2+
Cu1+
provides
highly
dynamic
active
species
reduction
NH3.
demonstrated
achieve
synergistic
decontamination
nutrient
durable
catalytic
activity
stability.
Advanced Energy Materials,
Год журнала:
2023,
Номер
14(1)
Опубликована: Ноя. 13, 2023
Abstract
The
development
of
industry
and
agriculture
has
been
accompanied
by
an
artificially
imbalanced
nitrogen
cycle,
which
threatens
human
health
ecological
environments.
Electrocatalytic
systems
have
emerged
as
a
sustainable
way
converting
nitrogen‐containing
molecules
into
high
value‐added
chemicals.
However,
the
construction
high‐performance
electrocatalysts
remains
challenging.
oxygen
vacancy
engineering
strategy
promoted
more
research
efforts
to
explore
structure‐activity
relationship
between
catalytic
activity
vacancies.
This
review
systematically
summarizes
recent
vacancies‐rich
metal
oxides
for
electro‐catalyzing
cycling
systems,
involving
electrocatalytic
nitrate
reduction
reaction,
nitric
oxide
C─N
coupling,
urea
oxidation
reaction.
First,
methods
characterization
vacancies
are
summarized.
Then,
effect
on
is
discussed
in
terms
regulating
electronic
structures
electrocatalysts,
improving
electroconductivity
catalysts,
lowing
energy
barrier,
strengthening
adsorption
activation
intermediate
species.
Finally,
future
directions
cycle
anticipated.
ACS Catalysis,
Год журнала:
2023,
Номер
13(8), С. 5375 - 5396
Опубликована: Апрель 6, 2023
Carbon
and
nitrogen
fixation
strategies
are
regarded
as
alternative
routes
to
produce
valuable
chemicals
used
energy
carriers
fertilizers
that
traditionally
obtained
from
unsustainable
energy-intensive
coal
gasification
(CO
CH4),
Fischer–Tropsch
(C2H4),
Haber–Bosch
(NH3)
processes.
Recently,
the
electrocatalytic
CO2
reduction
reaction
(CO2RR)
N2
(NRR)
have
received
tremendous
attention,
with
merits
of
being
both
efficient
store
renewable
electricity
while
providing
preparation
fossil-fuel-driven
reactions.
To
date,
development
CO2RR
NRR
processes
is
primarily
hindered
by
competitive
hydrogen
evolution
(HER);
however,
corresponding
for
inhibiting
this
undesired
side
still
quite
limited.
Considering
such
complex
reactions
involve
three
gas–liquid–solid
phases
successive
proton-coupled
electron
transfers,
it
appears
meaningful
review
current
improving
product
selectivity
in
light
their
respective
mechanisms,
kinetics,
thermodynamics.
By
examining
developments
understanding
catalyst
design,
electrolyte
engineering,
three-phase
interface
modulation,
we
discuss
key
NRR:
(i)
targeting
molecularly
defined
active
sites,
(ii)
increasing
local
reactant
concentration
at
(iii)
stabilizing
confining
intermediates.
Advanced Materials,
Год журнала:
2024,
Номер
36(18)
Опубликована: Янв. 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.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(21)
Опубликована: Янв. 31, 2024
Abstract
Electrochemical
conversion
of
nitrate
offers
an
efficient
solution
to
pollution
and
a
sustainable
strategy
for
ammonia
generation.
Cu
Fe
bimetallic
electrocatalysts
exhibit
excellent
electrochemical
reduction
(NO
3
RR)
reactivity
but
the
conventional
preparation
is
complex
time‐consuming
this
reaction
still
suffers
from
unsatisfied
kinetic
unidentified
mechanisms.
Herein,
in
situ
electrodeposition
employed
induce
modify
active
sites
iron‐based
N‐doping
carbon
nanofiber
electrode
(Fe/Fe
C@NCNFs)
during
NO
RR
Cu‐contained
solution.
Benefiting
synergistic
effect
between
Cu─Fe/Fe
C@NCNFs
electrode,
superior
activity
rate‐determining
(*NO
*NO
2
)
reduced
energy
barriers
following
deoxidation
hydrogenation
steps
are
achieved.
Compared
with
Fe/Fe
C@NCNFs‐500,
pseudo‐first‐order
(PFO)
rate
constant
by
demonstrates
nearly
two‐fold
improvement
high
current
efficiencies
over
wide
pH
voltage
range.
Furthermore,
maximum
─N
removal
capacity
N
selectivity
reach
15593.8
mg
g
−1
ca.
92%
after
twenty
cycles.
This
work
avenue
highly
design,
paving
more
insights
into
interactions
site
construction
performance.