Nano Research,
Год журнала:
2021,
Номер
15(4), С. 2773 - 2809
Опубликована: Сен. 4, 2021
Abstract
Engineering
of
defects
in
semiconductors
provides
an
effective
protocol
for
improving
photocatalytic
N
2
conversion
efficiency.
This
review
focuses
on
the
state-of-the-art
progress
defect
engineering
photocatalysts
reduction
toward
ammonia.
The
basic
principles
and
mechanisms
thermal
catalyzed
photon-induced
are
first
concisely
recapped,
including
relevant
properties
molecule,
reaction
pathways,
NH
3
quantification
methods.
Subsequently,
classification,
synthesis
strategies,
identification
techniques
compendiously
summarized.
Advances
situ
characterization
monitoring
state
during
process
also
described.
Especially,
various
surface
strategies
their
critical
roles
photoreduction
performance
highlighted,
vacancies
(i.e.,
anionic
cationic
vacancies),
heteroatom
doping
metal
element
nonmetal
doping),
atomically
defined
sites.
Finally,
future
opportunities
challenges
as
well
perspectives
further
development
defect-engineered
nitrogen
to
ammonia
presented.
It
is
expected
that
this
can
provide
a
profound
guidance
more
specialized
design
catalysts
with
high
activity
stability
photochemical
fixation.
Energy & Environmental Science,
Год журнала:
2022,
Номер
15(2), С. 830 - 842
Опубликована: Янв. 1, 2022
The
g-C
3
N
4
with
dual
defect
sites
exhibits
excellent
photocatalytic
H
2
O
generation
activity
and
selectivity,
the
key
role
of
each
site
in
surface
reaction
mechanism
is
revealed.
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(36), С. 19572 - 19590
Опубликована: Фев. 19, 2021
Abstract
Compared
to
modern
fossil‐fuel‐based
refineries,
the
emerging
electrocatalytic
refinery
(e‐refinery)
is
a
more
sustainable
and
environmentally
benign
strategy
convert
renewable
feedstocks
energy
sources
into
transportable
fuels
value‐added
chemicals.
A
crucial
step
in
conducting
e‐refinery
processes
development
of
appropriate
reactions
optimal
electrocatalysts
for
efficient
cleavage
formation
chemical
bonds.
However,
compared
well‐studied
primary
(e.g.,
O
2
reduction,
water
splitting),
mechanistic
aspects
materials
design
complex
are
yet
be
settled.
To
address
this
challenge,
herein,
we
first
present
fundamentals
heterogeneous
electrocatalysis
some
reactions,
then
implement
these
establish
framework
by
coupling
situ
generated
intermediates
(integrated
reactions)
or
products
(tandem
reactions).
We
also
set
principles
strategies
efficiently
manipulate
reaction
pathways.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(26), С. 11530 - 11535
Опубликована: Июнь 24, 2022
The
electrocatalytic
C-N
coupling
for
one-step
urea
synthesis
under
ambient
conditions
serves
as
the
promising
alternative
to
traditional
synthetic
protocol.
However,
hydrogenation
of
intermediate
species
hinders
efficient
synthesis.
Herein,
oxygen
vacancy-enriched
CeO2
was
demonstrated
electrocatalyst
with
stabilization
crucial
*NO
via
inserting
into
vacant
sites,
which
is
conducive
subsequent
process
rather
than
protonation,
whereas
poor
selectivity
protonation
observed
on
vacancy-deficient
catalyst.
vacancy-mediated
selective
distinguished
and
validated
by
in
situ
sum
frequency
generation
spectroscopy.
introduction
vacancies
tailors
common
catalyst
carrier
an
a
high
yield
rate
943.6
mg
h-1
g-1,
superior
that
partial
noble-metal-based
electrocatalysts.
This
work
provides
novel
insights
design
developments
systems.
Advanced Materials,
Год журнала:
2021,
Номер
34(2)
Опубликована: Окт. 17, 2021
The
electrooxidation
of
5-hydroxymethylfurfural
(HMF)
offers
a
promising
green
route
to
attain
high-value
chemicals
from
biomass.
HMF
reaction
(HMFOR)
is
complicated
process
involving
the
combined
adsorption
and
coupling
organic
molecules
OH-
on
electrode
surface.
An
in-depth
understanding
these
sites
processes
electrocatalysts
fundamentally
important.
Herein,
behavior
,
role
oxygen
vacancy
Co3
O4
are
initially
unraveled.
Correspondingly,
instead
competitive
metal
sites,
it
observed
that
can
fill
into
(Vo)
prior
couple
with
through
lattice
oxidation
process,
which
could
accelerate
rate-determining
step
dehydrogenation
5-hydroxymethyl-2-furancarboxylic
acid
(HMFCA)
intermediates.
With
modulated
as-designed
Vo-Co3
shows
excellent
activity
for
HMFOR
earlier
potential
90
120
mV
at
10
mA
cm-2
in
1
m
KOH
PBS
solution.
This
work
sheds
insight
catalytic
mechanism
vacancy,
benefits
designing
novel
modulate
multi-molecules
behaviors.
Journal of Materials Chemistry A,
Год журнала:
2022,
Номер
10(27), С. 14171 - 14186
Опубликована: Янв. 1, 2022
This
review
about
the
recent
advances
in
oxygen
vacancies
for
catalytic
oxidation
of
volatile
organic
compounds
considers
construction
strategies,
characterization
methods
and
effects
catalysts.
Advanced Functional Materials,
Год журнала:
2021,
Номер
31(20)
Опубликована: Март 12, 2021
Abstract
Polymeric
g‐C
3
N
4
is
a
promising
visible‐light‐responsive
photocatalyst;
however,
the
fast
recombination
of
charge
carriers
and
moderate
oxidation
ability
remarkably
restrict
its
photocatalytic
efficiency
towards
organic
pollutants.
To
overcome
these
drawbacks,
self‐modification
strategy
one‐step
formaldehyde‐assisted
thermal
polycondensation
molten
urea
to
prepare
carbon‐deficient
oxygen‐doped
(V
C
‐OCN)
developed,
carbon
vacancy
concentration
well‐controlled
by
changing
formaldehyde
dosage.
The
V
‐OCN
catalysts
exhibit
interesting
concentration‐dependent
removal
p
‐nitrophenol
(PNP)
atrazine
(ATN),
in
which
15
with
appropriate
displays
significantly
higher
pollutant
than
bulk
.
apparent
first‐order
rate
constant
for
PNP
ATN
4.4
5.2
times
that
A
combination
experimental
results
theoretic
calculations
confirm
synergetic
effect
vacancies
oxygen
doping
sites
can
not
only
delay
but
also
facilitate
adsorption
molecules
on
vacancies,
leads
generation
plentiful
active
species
including
superoxide
anion
radicals
indirectly
formed
hydroxyl
singlet
oxygen.
These
play
dominant
role
target
Advanced Functional Materials,
Год журнала:
2021,
Номер
32(6)
Опубликована: Окт. 27, 2021
Abstract
Electrochemical
water
splitting
powered
by
renewable
energy
sources
has
been
considered
as
an
attractive
hydrogen
generation
technology
with
high‐purity
product
and
zero
carbon
emission.
However,
the
efficient
realization
of
large‐scale
is
severely
hampered
sluggish
hydrogen/oxygen
evolution
reaction
(HER/OER).
As
important
class
functional
materials,
complex
hollow
electrocatalysts
provide
promising
solutions
to
accelerate
HER/OER
kinetics
owing
their
advantageous
features,
such
abundant
exposed
active
sites,
increased
contact
area
between
catalysts
electrolyte,
shortened
mass/charge
transport
length.
Herein,
recent
advances
in
development
outstanding
performances
are
summarized.
Beginning
introduction
mechanisms
design
principles,
achievements
engineering
highlighted
focus
on
structural
modulation,
composition
control,
electrocatalytic
evaluation.
Finally,
some
present
challenges
future
perspectives
for
advanced
toward
further
discussed.
Advanced Powder Materials,
Год журнала:
2022,
Номер
1(3), С. 100030 - 100030
Опубликована: Янв. 10, 2022
Water
splitting
has
been
regarded
as
a
sustainable
and
environmentally-friendly
technique
to
realize
green
hydrogen
generation,
while
more
energy
is
consumed
due
the
high
overpotentials
required
for
anode
oxygen
evolution
reaction.
Urea
electrooxidation,
an
ideal
substitute,
thus
received
increasing
attention
in
assisting
water-splitting
reactions.
Note
that
highly
efficient
catalysts
are
still
drive
urea
oxidation,
facile
generation
of
valence
state
species
significant
reaction
based
on
electrochemical-chemical
mechanisms.
The
cost
rareness
make
noble
metal
impossible
further
consideration
large-scale
application.
Ni-based
very
promising
their
cheap
price,
structure
tuning,
good
compatibility,
easy
active
phase
formation.
In
light
advances
made
recently,
herein,
we
reviewed
recent
powder
oxidation
fundamental
firstly
presented
clarify
mechanism
urea-assisted
water
splitting,
then
prevailing
evaluation
indicators
briefly
expressed
electrochemical
measurements.
catalyst
design
principle
including
synergistic
effect,
electronic
defect
construction
surface
reconstruction
well
main
fabrication
approaches
various
assisted
summarized
discussed.
problems
challenges
also
concluded
fabrication,
performance
evaluation,
Considering
key
influencing
factors
catalytic
process
application,
should
be
given
structure−property
relationship
deciphering,
novel
development
real
device;
specifically,
effort
directed
with
multi-functions
simultaneously
promote
steps
anti-corrosion
ability
by
revealing
local
integration
practical
We
believe
current
summarization
will
instructive
helpful
understanding
action
via
technique.
Abstract
High‐entropy
alloys
(HEAs)
are
expected
to
function
well
as
electrocatalytic
materials,
owing
their
widely
adjustable
composition
and
unique
physical
chemical
properties.
Recently,
HEA
catalysts
extensively
studied
in
the
field
of
electrocatalysis;
this
motivated
authors
investigate
relationship
between
structure
HEAs
performance.
In
review,
latest
advances
electrocatalysts
systematically
summarized,
with
special
focus
on
nitrogen
fixation,
carbon
cycle,
water
splitting,
fuel
cells;
addition,
by
combining
characterization
analysis
microstructures,
rational
design
strategies
for
optimizing
electrocatalysts,
including
controllable
preparation,
component
regulation,
strain
engineering,
defect
theoretical
prediction
proposed.
Moreover,
existing
issues
future
trends
predicted,
which
will
help
further
develop
these
high‐entropy
materials.
