ACS ES&T Engineering,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 15, 2024
Livestock
and
poultry
industries
are
pivotal
for
meat
production,
but
produced
wastewater
with
heavy
pollution
challenges
environmental
sustainability
public
health.
The
electro-Fenton
(EF)
process,
capable
of
in
situ
production
activation
hydrogen
peroxide,
is
promising
decontaminating
recalcitrant
pollutants,
yet
fabricating
a
highly
active
bifunctional
cathode
catalyst
across
broad
pH
range
remains
bottleneck.
Guided
by
green
chemistry
principles,
we
synthesized
dual-site
from
biological
waste
to
facilitate
hydroxyl
radical
production.
Combined
experimental
theoretical
investigations
unveiled
that
the
Fe2O3
sites
facilitated
H2O2
generation
via
catalyzing
oxygen
reduction
reaction,
whereas
Fe3N
promoted
into
radicals.
This
electrocatalyst,
integrated
gas
diffusion
electrode,
achieved
stable,
aeration-free
mineralization
antibiotic
contaminants
at
neutral
low
energy
consumption
just
0.94
kWh/g
removed
total
organic
carbon.
further
development
tandem
system
coupled
anammox
bioprocess
EF
process
exhibited
exceptional
efficiency
both
nitrogen
removal
tertiary
purification
actual
livestock
wastewater,
obviating
need
adjustments
or
Fenton
reagent
additives.
These
findings
underscore
potential
scalability
application
our
proposed
approach
promoting
sustainable
management
practices.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Окт. 25, 2024
Supramolecular
polymers
possess
great
potential
in
catalysis
owing
to
their
distinctive
molecular
recognition
and
dynamic
crosslinking
features.
However,
investigating
supramolecular
electrocatalysts
with
high
efficiency
oxygen
reduction
reaction
hydrogen
peroxide
(ORHP)
remains
an
unexplored
frontier.
Herein,
we
present
organic
for
ORHP
by
introducing
cyclodextrin-containing
noncovalent
building
blocks,
affording
these
supramolecules
abundant
bonds.
The
electronic
states
kinetics
are
further
well-modulated
via
a
host-guest
strategy,
resulting
appropriate
regional
electron
binding
force
controllable
chemical
activity.
Notably,
integrating
units
into
phenyl
group-containing
model
covalent
polymer
achieves
production
rate
of
9.14
mol
g
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 5, 2025
Abstract
Limited
by
the
activity‐selectivity
trade‐off
relationship,
electrochemical
activation
of
small
molecules
(like
O
2
,
N
2,
and
CO
)
rapidly
diminishes
Faradaic
efficiencies
with
elevated
current
densities
(particularly
at
ampere
levels).
Nevertheless,
some
catalysts
can
circumvent
this
restriction
in
a
two‐electron
oxygen
reduction
reaction
(2e
−
ORR),
sustainable
pathway
for
activating
to
hydrogen
peroxide
(H
).
Here
we
report
2e
ORR
expedited
fluorine‐bridged
copper
metal–organic
framework
catalyst,
arising
from
water
spillover
effect.
Through
operando
spectroscopies,
kinetic
theoretical
characterizations,
it
demonstrates
that
under
neutral
conditions,
plays
dual
role
accelerating
dissociation
stabilizing
key
*
OOH
intermediate.
Benefiting
spillover,
catalyst
expedite
density
range
0.1–2.0
A
cm
−2
both
high
(99–84.9%)
H
yield
rates
(63.17–1082.26
mg
h
−1
Further,
feasibility
present
system
has
been
demonstrated
scaling
up
unit
module
cell
25
combination
techno‐economics
simulations
showing
production
cost
strongly
dependent
on
densities,
giving
lowest
price
$0.50
kg
2.0
.
This
work
is
expected
provide
an
additional
dimension
leverage
systems
independent
oftraditional
rules.
Deleted Journal,
Год журнала:
2024,
Номер
1(2), С. 181 - 206
Опубликована: Авг. 4, 2024
Abstract
Metal–organic
frameworks
(MOFs)
have
emerged
as
promising
materials
in
the
realm
of
electrocatalysis
due
to
their
high
surface
area,
tunable
porosity,
and
versatile
chemical
functionality.
However,
practical
application
has
been
hampered
by
inherent
limitations
such
low
electrical
conductivity
a
limited
number
active
metal
sites.
Researchers
addressed
these
challenges
through
various
strategies,
including
enhancing
incorporating
conductive
nanoparticles,
modifying
structure
composition
MOFs
replacing
nodes
functionalizing
linkers,
preparing
catalysts
thermal
processes
decarburization
conversion
into
oxides,
phosphides
(MPs),
sulfides
(MSs).
This
review
provided
comprehensive
summary
strategies
that
were
employed
enhance
electroactivity
for
improved
electrocatalytic
performance
recent
years.
It
also
explored
future
directions
potential
innovations
design
synthesis
MOF‐based
electrocatalysts,
offering
valuable
insights
advancing
sustainable
energy
technologies.
Angewandte Chemie International Edition,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 11, 2025
Abstract
To
advance
electrochemical
H
2
O
production
and
unravel
catalytic
mechanisms,
the
precise
structural
coordination
of
single‐atomic
M‐N‐C
electrocatalysts
is
urgently
required.
Herein,
Co─N
5
site
with
an
asymmetric
electronic
configuration
constructed
to
boost
two‐electron
oxygen
reduction
reaction
(2e
−
ORR)
compared
symmetric
4
,
effectively
overcoming
trade‐off
between
activity
selectivity
in
production.
Both
experimental
theoretical
analyses
demonstrate
that
breaking
symmetry
sites
promotes
activation
molecules
moderates
adsorption
key
*OOH
intermediate
by
disrupting
linear
scaling
relationship
for
intermediates
adsorption.
This
modulation
enables
efficient
H₂O₂
its
effective
retention
subsequent
applications.
As
a
proof
concept,
achieves
rate
as
high
16.1
mol
g
cat
−1
h
flow
cell,
outperforming
most
recently
reported
counterparts.
Furthermore,
coupling
2e
ORR
oxidation
cellulose‐derived
carbohydrates
accomplishes
formic
acid
yields
(84.1%
from
glucose
62.0%–92.1%
other
substrates),
underpinning
sustainable
electro‐refinery
biomass
valorization
at
ambient
conditions.
By
elucidating
intrinsic
2e⁻
asymmetry
sites,
this
work
paves
way
high‐performance
electrosynthesis.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 14, 2025
Abstract
Two‐electron
oxygen
reduction
reaction
(2e
−
ORR)
in
acidic
media
is
a
promising
route
for
the
decentralized
and
on‐site
hydrogen
peroxide
(H
2
O
)
generation.
Nevertheless,
strong
interaction
between
active
sites
*
OOH
intermediates
usually
induces
O─O
bond
cleavage
to
convert
2e
pathway
into
sluggish
4e
ORR.
Therefore,
it
highly
necessary
optimize
electronic
structure
of
ORR
electrocatalysts
regulation
adsorption
energy.
Herein,
we
propose
utilization
atomically
dispersed
Co/Mo
anchored
on
mesoporous
carbon
hollow
spheres
(Co/Mo‐MCHS)
via
template‐engaged
strategy
selective
H
acid.
Benefitting
from
electron‐donating
effect
Mo
atoms,
an
enriched
electron
density
around
Co
center
Co/Mo‐MCHS
observed,
resulting
optimal
key
approach
apex
volcano
plot.
Moreover,
introduction
species
simultaneously
suppresses
electroreduction
as‐obtained
sites.
As
consequence,
delivers
high
selectivity
90–95%
The
flow
cell
based
catalyst
achieves
remarkable
yield
2102
mg
150
h.
this
can
be
extended
other
early
transition
metal
elements
with
similar
modifier
effects.
ACS Nano,
Год журнала:
2024,
Номер
18(33), С. 21836 - 21854
Опубликована: Авг. 7, 2024
Single
metal
atom
catalysts
(SACs)
have
garnered
considerable
attention
as
promising
agents
for
catalyzing
important
industrial
reactions,
particularly
the
electrochemical
synthesis
of
hydrogen
peroxide
(H
Advanced Materials,
Год журнала:
2024,
Номер
36(41)
Опубликована: Авг. 16, 2024
Abstract
Heterogeneous
single‐metal‐site
catalysts
(SMSCs),
often
referred
to
as
single‐atom
(SACs),
demonstrate
promising
catalytic
activity,
selectivity,
and
stability
across
a
wide
spectrum
of
reactions
due
their
rationally
designed
microenvironments
encompassing
coordination
geometry,
binding
ligands,
electronic
configurations.
However,
the
inherent
disorderliness
SMSCs
at
both
atomic
scale
nanoscale
poses
challenges
in
deciphering
working
principles
establishing
correlations
between
performances
SMSCs.
The
rearrangement
randomly
dispersed
single
metals
into
homogeneous
atomic‐precisely
structured
periodic
single‐metal
site
(PSMSCs)
not
only
simplifies
chaos
systems
but
also
unveils
new
opportunities
for
manipulating
performance
gaining
profound
insights
reaction
mechanisms.
Moreover,
synergistic
effects
adjacent
integration
arrangement
further
broaden
industrial
application
scope
This
perspective
offers
comprehensive
overview
recent
advancements
outlines
prospective
avenues
research
design
characterizations
PSMSCs,
while
acknowledging
formidable
encountered
prospects
that
lie
ahead.