Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(37)
Опубликована: Июль 27, 2022
Abstract
The
electrochemical
oxygen
reduction
reaction
(ORR)
provides
a
green
route
for
decentralized
H
2
O
synthesis,
where
structure–selectivity
relationship
is
pivotal
the
control
of
highly
selective
and
active
two‐electron
pathway.
Here,
we
report
fabrication
boron
nitrogen
co‐doped
turbostratic
carbon
catalyst
with
tunable
B−N−C
configurations
(CNB‐ZIL)
by
assistance
zwitterionic
liquid
(ZIL)
hydrogen
peroxide
production.
Combined
spectroscopic
analysis
reveals
fine
tailored
B−N
moiety
in
CNB‐ZIL,
interfacial
species
homogeneous
distribution
tend
to
segregate
into
hexagonal
nitride
domains
at
higher
pyrolysis
temperatures.
Based
on
experimental
observations,
correlation
between
moieties
HO
−
selectivity
established.
CNB‐ZIL
electrocatalysts
optimal
exhibit
high
small
overpotentials
alkaline
media,
giving
yield
≈1787
mmol
g
−1
h
−1.4
V
flow‐cell
reactor.
Shifting
electrochemical
oxygen
reduction
reaction
(ORR)
via
two-electron
pathway
becomes
increasingly
crucial
as
an
alternative/green
method
for
hydrogen
peroxide
(H2
O2
)
generation.
Here,
the
development
of
2e-
ORR
catalysts
in
recent
years
is
reviewed,
aspects
mechanism
exploration,
types
high-performance
catalysts,
factors
to
influence
catalytic
performance,
and
potential
applications
ORR.
Based
on
previous
theoretical
experimental
studies,
underlying
firstly
unveiled,
aspect
pathway,
thermodynamic
free
energy
diagram,
limiting
potential,
volcano
plots.
Then,
various
efficient
producing
H2
are
summarized.
Additionally,
active
sites
catalysts'
such
electronic
structure,
carbon
defect,
functional
groups
(O,
N,
B,
S,
F
etc.),
synergistic
effect,
others
(pH,
pore
steric
hindrance
etc.)
discussed.
The
electrogeneration
also
has
wastewater
treatment,
disinfection,
organics
degradation,
storage.
Finally,
future
directions
prospects
electrochemically
examined.
These
insights
may
help
develop
highly
active/selective
shape
application
this
method.
Advanced Materials,
Год журнала:
2021,
Номер
33(49)
Опубликована: Сен. 24, 2021
Abstract
Hydrogen
peroxide
(H
2
O
)
is
an
environment‐friendly
and
efficient
oxidant
with
a
wide
range
of
applications
in
different
industries.
Recently,
the
production
hydrogen
through
direct
electrosynthesis
has
attracted
widespread
research
attention,
emerged
as
most
promising
method
to
replace
traditional
energy‐intensive
multi‐step
anthraquinone
process.
In
ongoing
efforts
achieve
highly
large‐scale
H
,
carbon‐based
materials
have
been
developed
2e
−
oxygen
reduction
reaction
catalysts,
benefits
low
cost,
abundant
availability,
optimal
performance.
This
review
comprehensively
introduces
strategies
for
optimizing
toward
production,
latest
advances
hybrid
catalysts.
The
active
sites
influence
coordination
heteroatom
doping
on
selectivity
are
extensively
analyzed.
particular,
appropriate
design
functional
groups
understanding
effect
electrolyte
pH
expected
further
improve
selective
efficiency
producing
via
reaction.
Methods
improving
catalytic
activity
by
interface
engineering
kinetics
summarized.
Finally,
challenges
catalysts
face
before
they
can
be
employed
commercial‐scale
identified,
prospects
designing
novel
electrochemical
reactors
proposed.
Advanced Materials,
Год журнала:
2022,
Номер
34(23)
Опубликована: Фев. 8, 2022
Abstract
The
hydrogen
peroxide
(H
2
O
)
generation
via
the
electrochemical
oxygen
reduction
reaction
(ORR)
under
ambient
conditions
is
emerging
as
an
alternative
and
green
strategy
to
traditional
energy‐intensive
anthraquinone
process
unsafe
direct
synthesis
using
H
.
It
enables
on‐site
decentralized
production
air
renewable
electricity
for
various
applications.
Currently,
atomically
dispersed
single
metal
site
catalysts
have
emerged
most
promising
platinum
group
(PGM)‐free
electrocatalysts
ORR.
Further
tuning
their
central
sites,
coordination
environments,
local
structures
can
be
highly
active
selective
2e
−
Herein,
recent
methodologies
achievements
on
developing
are
summarized.
Combined
with
theoretical
computation
advanced
characterization,
a
structure–property
correlation
guide
rational
catalyst
design
favorable
ORR
aimed
provide.
Due
oxidative
nature
of
derived
free
radicals,
stability
effective
solutions
improve
tolerance
emphasized.
Transferring
intrinsic
properties
electrode
performance
viable
applications
always
remains
grand
challenge.
key
metrics
knowledge
during
electrolyzer
development
are,
therefore,
highlighted.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(51)
Опубликована: Окт. 25, 2022
Not
only
high
efficiency
but
also
selectivity
of
the
electrocatalysts
is
crucial
for
high-performance,
low-cost,
and
sustainable
energy
storage
applications.
Herein,
we
systematically
investigate
edge
effect
carbon-supported
single-atom
catalysts
(SACs)
on
oxygen
reduction
reaction
(ORR)
pathways
(two-electron
(2
e-
)
or
four-electron
(4
))
conclude
that
2
-ORR
proceeding
over
edge-hosted
atomic
Co-N4
sites
more
favorable
than
basal-plane-hosted
ones.
As
such,
have
successfully
synthesized
tuned
Co-SACs
with
different
edge-to-bulk
ratios.
The
as-prepared
edge-rich
Co-N/HPC
catalyst
exhibits
excellent
performance
a
remarkable
≈95
%
in
wide
potential
range.
Furthermore,
find
functional
groups
could
saturate
graphitic
carbon
edges
under
ORR
operation
further
promote
electrocatalytic
performance.
These
findings
structure-property
relationship
SACs
offer
promising
direction
large-scale
low-cost
electrochemical
H2
O2
production
via
-ORR.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(23)
Опубликована: Апрель 3, 2024
Abstract
Solar
energy
can
be
utilized
in
photocatalysis
technology
to
realize
light‐driven
hydrogen
peroxide
(H
2
O
)
production,
a
green
chemical
synthesis
route.
Designing
high‐performance
photocatalysts
is
critical
achieving
practical
solar
H
production.
During
the
past
decade,
significant
research
progress
made
photocatalytic
materials
for
Particularly
2D
materials‐based
stand
out
due
their
unique
physical
and
properties.
This
review
highlights
intricate
relationship
between
material
innovation
photochemical
It
starts
with
fundamental
principles
of
generation,
focusing
on
crucial
steps
such
as
photon
absorption,
carrier
dynamics,
surface
reactions,
challenges
that
solve
at
each
step.
Then,
various
production
are
introduced
detail.
Engineering
strategies
optimize
performance
discussed
afterward.
Finally,
future
opportunities
designing
outlined.
expected
inspire
engineering
conversion
other
chemicals.
