Energy & Fuels,
Год журнала:
2021,
Номер
35(8), С. 6504 - 6526
Опубликована: Апрель 5, 2021
Graphitic
carbon
nitride
(g-C3N4),
a
polymeric
semiconductor,
has
become
rising
star
for
photocatalytic
energy
conversion
because
of
its
facile
accessibility,
metal-free
nature,
low
cost,
and
environmentally
benign
properties.
This
work
reviews
the
latest
progress
g-C3N4-based
materials
in
visible-light-driven
water
splitting
to
hydrogen.
It
begins
with
brief
history
g-C3N4,
followed
by
various
engineering
strategies
such
as
elemental
doping,
copolymerization,
crystalline
tailoring,
surface
engineering,
single-atom
modification,
elevated
decomposition.
In
addition,
synthesis
g-C3N4
different
dimensions
(0D,
1D,
2D,
3D)
configurations
series
heterojunctions
(type
II,
Z-scheme,
S-scheme,
g-C3N4/metal,
g-C3N4/carbon
heterojunctions)
were
also
discussed
their
improvement
hydrogen
production.
Lastly,
challenges
opportunities
nanomaterials
are
provided.
is
anticipated
that
this
review
will
promote
further
development
emerging
more
efficiency
Environmental Science & Technology,
Год журнала:
2022,
Номер
56(16), С. 11635 - 11645
Опубликована: Июль 11, 2022
Single-atom
catalysts
(SACs)-based
peroxymonosulfate
(PMS)
systems
are
highly
selective
to
the
type
of
organic
pollutants
while
mechanisms
remain
ambiguous.
In
this
work,
we
carried
out
experimental
and
theoretical
investigations
reveal
origins
selectivity
radical
nonradical
pathways
in
a
designated
Co–N4–C/PMS
system.
Two
typical
[bisphenol
A
(BPA)
metronidazole
(MNZ)]
with
different
molecular
structures
were
employed
for
comparison.
We
found
that
oxidation
(SO4•–
HO•)
electron-transfer
pathway
(ETP)
co-existed
Pollutants
(e.g.,
MNZ)
high
redox
potential
degraded
primarily
by
free
radicals
rather
than
ETP,
oxidization
low-redox
BPA)
was
dominated
ETP
at
surface
region
Co–N4–C
which
overwhelmed
contributions
homogeneous
phase.
Intriguingly,
could
be
manipulated
PMS
loading,
simultaneously
increased
population
elevated
Co–N4–C-PMS*
complexes
ETP.
Findings
from
work
will
unravel
mysterious
behavior
SACs/PMS
micropollutants.
ACS Catalysis,
Год журнала:
2021,
Номер
11(15), С. 9569 - 9577
Опубликована: Июль 16, 2021
Transition
metal
catalysts
are
known
to
activate
persulfate,
but
the
properties
that
govern
intrinsic
activity
of
these
still
unknown.
Here,
we
developed
a
series
with
transition
metals
anchored
on
carbon
nanotubes
(denoted
M–N–CNTs,
where
M
=
Co,
Fe,
Mn,
or
Ni)
containing
single-atom
M–N
moieties,
peroxymonosulfate
for
efficient
nonradical
oxidation
sulfamethoxazole.
The
spin
state
M–N–CNTs
strongly
determined
their
catalytic
activity.
A
large
effective
magnetic
moment
high
(e.g.,
Co–N)
favored
overlap
d
orbitals
oxygen-containing
adsorbates
(such
as
peroxo
species)
active
sites
and
promoted
electron
transfer,
which
facilitated
adsorption
enhanced
capacity
reactive
species.
These
findings
advance
mechanistic
understanding
metal-mediated
persulfate
activation
inform
development
spintronic
environmental
applications.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(29)
Опубликована: Май 6, 2022
Abstract
Simultaneous
regulation
of
the
coordination
environment
single‐atom
catalysts
(SACs)
and
engineering
architectures
with
efficient
exposed
active
sites
are
strategies
for
boosting
peroxymonosulfate
(PMS)
activation.
We
isolated
cobalt
atoms
dual
nitrogen
oxygen
(Co−N
3
O
1
)
on
oxygen‐doped
tubular
carbon
nitride
(TCN)
by
pyrolyzing
a
hydrogen‐bonded
cyanuric
acid
melamine–cobalt
acetate
precursor.
The
theoretically
constructed
Co−N
moiety
TCN
exhibited
an
impressive
mass
activity
7.61×10
5
min
−1
mol
high
2
selectivity.
Theoretical
calculations
revealed
that
single
occupied
environment,
PMS
adsorption
was
promoted
energy
barriers
reduced
key
*O
intermediate
produced
.
were
attached
to
widely
used
poly(vinylidene
fluoride)
microfiltration
membrane
deliver
antibiotic
wastewater
treatment
system
97.5
%
ciprofloxacin
rejection
over
10
hours,
thereby
revealing
suitability
industrial
applications.
Proceedings of the National Academy of Sciences,
Год журнала:
2022,
Номер
119(31)
Опубликована: Июль 25, 2022
Nonradical
Fenton-like
catalysis
offers
opportunities
to
overcome
the
low
efficiency
and
secondary
pollution
limitations
of
existing
advanced
oxidation
decontamination
technologies,
but
realizing
this
on
transition
metal
spinel
oxide
catalysts
remains
challenging
due
insufficient
understanding
their
catalytic
mechanisms.
Here,
we
explore
origins
selectivity
Fe-Mn
identify
electron
delocalization
surface
active
site
as
key
driver
its
nonradical
catalysis.
Through
fine-tuning
crystal
geometry
trigger
superexchange
interaction
at
octahedra,
ZnFeMnO4
with
high-degree
Mn-O
unit
was
created
enable
near
100%
activation
peroxymonosulfate
(PMS)
unprecedented
utilization
efficiency.
The
resulting
surface-bound
PMS*
complex
can
efficiently
oxidize
electron-rich
pollutants
extraordinary
degradation
activity,
selectivity,
good
environmental
robustness
favor
water
applications.
Our
work
provides
a
molecule-level
bimetallic
interactions
oxides,
which
may
guide
design
low-cost
oxides
for
more
selective
efficient
