The
atomic
dispersed
heterogeneous
catalysts
are
attracting
much
research
interests.
Recently,
multiple
active
sites
(two,
three
or
even
more)
exhibits
all-round
characters
for
regulation
of
intrinsic
sites.
However,
depth
exploration
in
persulfate
activation
etc
fenton-like
advanced
oxidation
process
is
still
its
infancy.
Herein,
binary
anchored
visible-light-responsive
carbon
nitride
Co-Mn/CN
catalyst
was
designed
representatively.
characterization
and
theory
calculation
clarified
the
coordination
environment
metallic
center
atoms
confirms
CoN4-MnN2
moiety.
unique
coordinated
geometry
on
one
hand
highlights
synergy
effect
between
photocatalysis
peroxymonosulfate
(PMS)
activation,
other
promotes
form
metastable
metal-PMS
complex
subsequent
process.
Furthermore,
present
efficient
application
to
purify
oil
spill
pollutes
water
considering
quality,
pH
durability
etc.
This
work
sheds
light
rational
diatomic
photo-Fenton-like
catalysts.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Окт. 10, 2024
Abstract
Microplastic
pollution,
an
emerging
environmental
issue,
poses
significant
threats
to
aquatic
ecosystems
and
human
health.
In
tackling
microplastic
pollution
advancing
green
hydrogen
production,
this
study
reveals
a
tandem
catalytic
degradation-hydrogen
evolution
reaction
(MPD-HER)
process
using
hierarchical
porous
carbon
nitride-supported
single-atom
iron
catalysts
(FeSA-hCN).
Through
hydrothermal-assisted
Fenton-like
reactions,
we
accomplish
near-total
ultrahigh-molecular-weight-polyethylene
degradation
into
C
3
-C
20
organics
with
64%
selectivity
of
carboxylic
acid
under
neutral
pH,
leap
beyond
current
capabilities
in
efficiency,
selectivity,
eco-friendliness,
stability
over
six
cycles.
The
system
demonstrates
versatility
by
degrading
various
daily-use
plastics
across
different
settings.
mixture
FeSA-hCN
plastic
products
further
achieves
42
μmol
h
‒1
illumination,
outperforming
most
existing
photoreforming
methods.
This
MPD-HER
not
only
provides
scalable
economically
feasible
strategy
combat
but
also
contributes
the
economy,
far-reaching
implications
for
global
sustainability
initiatives.
Chemical Society Reviews,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
Catalytic
active
sites
and
mechanisms
of
various
dimensional
carbonaceous
materials
in
activation
oxidants
towards
advanced
oxidant
processes
for
wastewater/water
treatment
were
reviewed.
ACS Catalysis,
Год журнала:
2023,
Номер
13(17), С. 11711 - 11722
Опубликована: Авг. 21, 2023
Ammonia
(NH3)
splitting
to
hydrogen
(H2)
is
a
promising
route
for
on-site
production
of
green
energy;
however,
the
application
limited
due
high-cost
noble-metal-based
catalysts
and
high
operating
temperature
endothermic
nature.
Herein,
we
develop
series
macroporous
carbon
nitride-supported
single-atom
transition
metal
(TMs-MCN,
TMs:
Co,
Mn,
Fe,
Ni,
Cu)
catalyst
panels
solar
light-driven
photocatalytic
gaseous
NH3
splitting.
Under
ambient
reaction
conditions,
optimized
Ni-MCN
shows
an
H2
rate
35.6
μmol
g–1
h–1,
much
superior
that
MCN
other
TMs-MCN.
Such
enhanced
photoactivity
attributed
presence
Ni–N4
sites,
which
improve
optical
properties,
accelerate
charge
carrier
separation/transfer,
boost
kinetics
catalysts.
Density
functional
theory
calculations
further
reveal
sites
can
effectively
modify
electronic
structure
nitride.
Compared
with
site
possesses
moderate
binding
strength
lowest
energy
barrier
facilitate
formation
key
intermediates
*NH
+
*H.
These
findings
provide
valuable
guidelines
rational
design
toward
energy-
cost-effective
production.
Accounts of Chemical Research,
Год журнала:
2024,
Номер
57(16), С. 2303 - 2315
Опубликована: Авг. 6, 2024
ConspectusGraphitic
carbon
nitride-based
materials
have
emerged
as
promising
photocatalysts
for
a
variety
of
energy
and
environmental
applications
owing
to
their
"earth-abundant"
nature,
structural
versatility,
tunable
electronic
optical
properties,
chemical
stability.
Optimizing
nitride's
physicochemical
properties
encompasses
approaches,
including
the
regulation
inherent
defects,
morphology
control,
heterostructure
construction,
heteroatom
metal-atom
doping.
These
strategies
are
pivotal
in
ultimately
enhancing
photocatalytic
activities.
Previous
reviews
with
extensive
examples
mainly
focused
on
synthesis,
modification,
application
photocatalysis.
However,
there
has
been
lack
straightforward
in-depth
discussion
understand
characteristics
functions
various
engineered
nitrides
well
precise
tailoring
explain
regularity
specificity
improved
performance
targeted
systems.
In
past
ten
years,
our
group
conducted
investigations
studies
demonstrate
close
yet
intricate
relationship
between
structure
nitride
reactivity.
Understanding
nitride,
different
engineering
strategies,
is
essential
improvement
processes
from
fundamental
study
practical
applications.To
this
end,
Account,
we
first
delve
into
nature
highlighting
structures,
band
structure,
density
states,
molecular
orbitals,
center,
its
functions,
such
charge
distribution,
internal
electric
field,
external
force.
Subsequently,
based
recent
research
group,
present
detailed
strategic
modifications
consequential
impacts
particularly
intrinsic
characteristics,
performance.
categorized
follows:
(i)
component
changing,
which
involves
intralayer
interface
heterojunctions
homojunctions,
modulate
band-edge
potentials
reactivity
photoinduced
electrons
holes
toward
surface
redox
reactions;
(ii)
dimensional
tuning,
engineers
influence
electron
transfer
direction;
(iii)
defect
introduces
symmetry
break
framework,
promote
redistribution
altering
structure;
(iv)
anchoring
single-atom
metals
facilitate
orbital
hybridization
enhancement
through
unique
metal-N
coordination
configurations.
Finally,
propose
an
appraisal
prospects
challenges
manipulation
characterization
nitride.
The
integration
Chemical Reviews,
Год журнала:
2024,
Номер
124(20), С. 11348 - 11434
Опубликована: Окт. 9, 2024
Environmental
catalysis
has
emerged
as
a
scientific
frontier
in
mitigating
water
pollution
and
advancing
circular
chemistry
reaction
microenvironment
significantly
influences
the
catalytic
performance
efficiency.
This
review
delves
into
engineering
within
liquid-phase
environmental
catalysis,
categorizing
microenvironments
four
scales:
atom/molecule-level
modulation,
nano/microscale-confined
structures,
interface
surface
regulation,
external
field
effects.
Each
category
is
analyzed
for
its
unique
characteristics
merits,
emphasizing
potential
to
enhance
efficiency
selectivity.
Following
this
overview,
we
introduced
recent
advancements
advanced
material
system
design
promote
(e.g.,
purification,
transformation
value-added
products,
green
synthesis),
leveraging
state-of-the-art
technologies.
These
discussions
showcase
was
applied
different
reactions
fine-tune
regimes
improve
from
both
thermodynamics
kinetics
perspectives.
Lastly,
discussed
challenges
future
directions
engineering.
underscores
of
intelligent
materials
drive
development
more
effective
sustainable
solutions
decontamination.
