Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(27)
Published: April 21, 2023
Competition
from
hydrogen/oxygen
evolution
reactions
and
low
solubility
of
N2
in
aqueous
systems
limited
the
selectivity
activity
on
nitrogen
fixation
reaction.
Herein,
we
design
an
aerobic-hydrophobic
Janus
structure
by
introducing
fluorinated
modification
porous
carbon
nanofibers
embedded
with
partially
carbonized
iron
heterojunctions
(Fe3
C/Fe@PCNF-F).
The
simulations
prove
that
can
keep
internal
Fe3
C/Fe@PCNF-F
away
water
infiltration
endow
a
molecular-concentrating
effect,
suppressing
competing
overcoming
mass-transfer
limitations
to
build
robust
"quasi-solid-gas"
state
micro-domain
around
catalyst
surface.
In
this
proof-of-concept
system,
exhibits
excellent
electrocatalytic
performance
for
(NH3
yield
rate
up
29.2
μg
h-1
mg-1cat.
Faraday
efficiency
(FE)
27.8
%
reduction
reaction;
NO3-
15.7
FE
3.4
oxidation
reaction).
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(11), P. 6410 - 6419
Published: March 13, 2023
Sustainable
conversion
of
plastic
waste
to
mitigate
environmental
threats
and
reclaim
value
is
important.
Ambient-condition
photoreforming
practically
attractive
convert
hydrogen
(H2);
however,
it
has
poor
performance
because
mutual
constraint
between
proton
reduction
substrate
oxidation.
Here,
we
realize
a
cooperative
photoredox
using
defect-rich
chalcogenide
nanosheet-coupled
photocatalysts,
e.g.,
d-NiPS3/CdS,
give
an
ultrahigh
H2
evolution
∼40
mmol
gcat-1
h-1
organic
acid
yield
up
78
μmol
within
9
h,
together
with
excellent
stability
beyond
100
h
in
commercial
poly(lactic
acid)
poly(ethylene
terephthalate).
Significantly,
these
metrics
represent
one
the
most
efficient
reported.
In
situ
ultrafast
spectroscopic
studies
confirm
charge
transfer-mediated
reaction
mechanism
which
d-NiPS3
rapidly
extracts
electrons
from
CdS
boost
evolution,
favoring
hole-dominated
oxidation
improve
overall
efficiency.
This
work
opens
practical
avenues
for
converting
into
fuels
chemicals.
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
13(11)
Published: Jan. 29, 2023
Abstract
Recent
years
have
witnessed
an
upsurge
of
interest
in
exploiting
advanced
photo‐/electrocatalysts
for
efficient
energy
conversion
and
environmental
remediation.
Constructing
internal
electric
fields
has
been
highlighted
as
a
rising
star
to
help
facilitate
various
catalytic
processes,
with
the
merits
promoting
charge
transfer/separation,
optimizing
redox
potential
creating
effective
active/adsorption
sites.
Internal
are
usually
formed
by
polarization
uneven
distributions
between
different
constituent
layers,
which
widely
exist
piezoelectrics,
polar
surface
terminations,
heterostructure
materials.
Herein,
groundbreaking
interdisciplinary
overview
latest
advances
construction
improve
photo(electro)catalytic
electrocatalytic
activity
is
provided.
This
critical
review
begins
encyclopedic
summary
classification,
advantages,
synthesis
strategies
fields.
Subsequently,
identification
methods
thoroughly
discussed
based
on
characterization
techniques,
experiments,
theoretical
calculations,
can
provide
profound
guidance
in‐depth
study
To
elaborate
theory–structure–activity
relationships
fields,
corresponding
reaction
mechanisms,
modification
strategies,
performance
jointly
discussed,
along
discussion
their
practical
applications.
Finally,
insightful
analysis
challenges
future
prospects
field‐based
catalysts
discussed.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(10)
Published: Jan. 18, 2023
Electroreduction
of
nitrate
into
ammonia
(NRA)
provides
a
sustainable
route
to
convert
the
widespread
pollutants
high-value-added
products
under
ambient
conditions,
which
unfortunately
suffers
from
unsatisfactory
selectivity
due
competitive
hydrogen
evolution
reaction
(HER).
Previous
strategies
modifying
metal
sites
catalysts
often
met
dilemma
for
simultaneously
promoting
activity
and
toward
NRA.
Here,
general
strategy
is
reported
enable
an
efficient
selective
NRA
process
through
coordination
modulation
single-atom
tailor
local
proton
concentration
at
catalyst
surface.
By
contrast,
two
analogous
Ni-single-atom
enriched
conjugated
polymers
(NiO4
-CCP
NiN4
-CCP)
with
different
motifs
are
investigated
proof-of-concept
study.
The
NiO4
exhibits
yield
rate
as
high
1.83
mmol
h-1
mg-1
Faradaic
efficiency
94.7%
current
density
125
mA
cm-2
,
outperforming
catalyst.
These
experimental
theoretical
studies
both
suggest
that
can
not
only
accelerate
by
adjusting
adsorption
energies
intermediates
on
but
also
inhibit
HER
regulating
migration
contributions
metal-hydrated
cations
adsorbed
surface,
thus
achieving
simultaneous
enhancement
activity.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(8), P. 5779 - 5787
Published: April 1, 2024
Photocatalytic
dinitrogen
(N2)
fixation
is
regarded
as
an
achievable
technology
for
ammonia
(NH3)
production.
However,
the
poor
separation
efficiency
of
photoinduced
carriers
and
ineffective
N2
activation
remain
grand
obstacles
to
high-performance
NH3
photosynthesis.
Designing
advanced
heterostructured
systems
accelerate
charge
activate
molecule
a
feasible
strategy
optimize
photocatalytic
activity.
Herein,
direct
Z-scheme
configuration
established
between
BiOBr
Bi4O5Br2
through
facile
one-step
solvothermal
reaction.
This
enables
effective
spatial
electron–hole
pairs
preserves
robust
redox
ability
carriers,
concurrently
promoting
N≡N
bond
diminishing
energy
barrier
rate-determining
step.
The
formation
BiOBr/Bi4O5Br2
heterojunctions
mostly
attributed
similarities
in
their
lattice
structures
crystal
growth
conditions.
As
result,
heterojunction
exhibits
high
yield
66.87
μmol
g–1
h–1
without
using
sacrificing
reagents,
surpassing
that
pristine
by
approximately
3.3
5.6
times,
respectively.
study
provides
approach
construct
implementing
under
mild
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(42)
Published: June 16, 2023
Abstract
The
rational
design
of
a
step‐scheme
(S‐scheme)
heterojunctions
in
hybrid
semiconductors
by
avoiding
unwanted
charge
transport
paths
is
considered
as
an
attractive
way
to
achieve
high
photocatalytic
activity
hydrogen
evolution
reaction
(HER).
Here,
dual
S‐scheme
heterojunction
formed
the
lychee‐shaped
W
18
O
49
/CdWO
4
/CdS
nanostructures
proposed
for
improving
performance
HER
under
visible
light
irradiation.
remarkable
attributed
unique
structure
and
effective
separation
photoinduced
defect‐transit
mechanism
strong
internal
electric
field.
measurements
X‐ray
photoelectron
spectroscopy
(XPS),
femtosecond
transient
absorption
(fs‐TA)
spectroscopy,
electron
paramagnetic
resonance
(EPR)
further
confirm
carrier
transfer
pathways
following
mechanism.
This
research
can
provide
new
strategy
designing
improve
through
defect
band
engineering.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
36(5)
Published: Aug. 28, 2023
Piezo-photocatalysis
is
a
frontier
technology
for
converting
mechanical
and
solar
energies
into
crucial
chemical
substances
has
emerged
as
promising
sustainable
strategy
N