Chemical Reviews,
Journal Year:
2023,
Volume and Issue:
123(8), P. 4635 - 4662
Published: March 14, 2023
This
review
presents
an
exhaustive
overview
on
the
mechanisms
of
Fe3+
cathodic
reduction
within
context
electro-Fenton
(EF)
process.
Different
strategies
developed
to
improve
rate
are
discussed,
dividing
them
into
two
categories
that
regard
mechanistic
feature
is
promoted:
electron
transfer
control
and
mass
transport
control.
Boosting
conversion
Fe2+
via
includes:
(i)
formation
a
series
active
sites
in
both
carbon-
metal-based
materials
(ii)
use
other
emerging
such
as
single-atom
catalysis
or
confinement
effects.
Concerning
enhancement
regeneration
by
control,
main
routes
involve
application
magnetic
fields,
pulse
electrolysis,
interfacial
Joule
heating
effects,
photoirradiation.
Finally,
challenges
singled
out,
future
prospects
described.
aims
clarify
Fe3+/Fe2+
cycling
process
EF
process,
eventually
providing
essential
ideas
for
smart
design
highly
effective
systems
wastewater
treatment
valorization
at
industrial
scale.
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: Jan. 12, 2023
Direct
hydrogen
peroxide
(H2O2)
electrosynthesis
via
the
two-electron
oxygen
reduction
reaction
is
a
sustainable
alternative
to
traditional
energy-intensive
anthraquinone
technology.
However,
high-performance
and
scalable
electrocatalysts
with
industrial-relevant
production
rates
remain
be
challenging,
partially
due
insufficient
atomic
level
understanding
in
catalyst
design.
Here
we
utilize
theoretical
approaches
identify
transition-metal
single-site
catalysts
for
using
*OOH
binding
energy
as
descriptor.
The
predictions
are
then
used
guidance
synthesize
desired
cobalt
O-modified
Co-(pyrrolic
N)4
configuration
that
can
achieve
current
densities
up
300
mA
cm-2
96-100%
Faradaic
efficiencies
H2O2
at
record
rate
of
11,527
mmol
h-1
gcat-1.
Here,
show
feasibility
versatility
metal
design
various
commercial
carbon
phthalocyanine
starting
materials
high
applicability
acidic,
neutral
alkaline
electrolytes.
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: Aug. 8, 2023
The
two-electron
oxygen
reduction
reaction
in
acid
is
highly
attractive
to
produce
H2O2,
a
commodity
chemical
vital
various
industry
and
household
scenarios,
which
still
hindered
by
the
sluggish
kinetics.
Herein,
both
density
function
theory
calculation
in-situ
characterization
demonstrate
that
dual-atom
CoIn
catalyst,
O-affinitive
In
atom
triggers
favorable
stable
adsorption
of
hydroxyl,
effectively
optimizes
OOH
on
neighboring
Co.
As
result,
Co
atoms
shifts
pathway
for
efficient
H2O2
production
acid.
partial
current
reaches
1.92
mA
cm-2
at
0.65
V
rotating
ring-disk
electrode
test,
while
rate
as
high
9.68
mol
g-1
h-1
three-phase
flow
cell.
Additionally,
CoIn-N-C
presents
excellent
stability
during
long-term
operation,
verifying
practicability
catalyst.
This
work
provides
inspiring
insights
into
rational
design
active
catalysts
other
catalytic
systems.
Nano-Micro Letters,
Journal Year:
2023,
Volume and Issue:
15(1)
Published: May 9, 2023
Abstract
An
environmentally
benign,
sustainable,
and
cost-effective
supply
of
H
2
O
as
a
rapidly
expanding
consumption
raw
material
is
highly
desired
for
chemical
industries,
medical
treatment,
household
disinfection.
The
electrocatalytic
production
route
via
electrochemical
oxygen
reduction
reaction
(ORR)
offers
sustainable
avenue
the
on-site
from
O.
most
crucial
innovative
part
such
technology
lies
in
availability
suitable
electrocatalysts
that
promote
two-electron
(2e
–
)
ORR.
In
recent
years,
tremendous
progress
has
been
achieved
designing
efficient,
robust,
catalyst
materials,
including
noble
metals
their
alloys,
metal-free
carbon-based
single-atom
catalysts,
molecular
catalysts.
Meanwhile,
cell
designs
have
significantly
advanced
applications
at
industrial
level.
This
review
summarizes
fundamental
basics
advances
2e
-ORR,
design,
mechanistic
explorations,
theoretical
computations,
experimental
evaluations,
designs.
Perspectives
on
addressing
remaining
challenges
are
also
presented
with
an
emphasis
large-scale
synthesis
route.
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
13(36)
Published: Aug. 6, 2023
Abstract
Hydrogen
peroxide
is
an
essential
chemical
that
attracting
strong
attention
for
energy
and
environmental
applications.
However,
the
struggle
between
growing
market
demand
unsustainability
of
conventional
anthraquinone
method
motivates
exploration
alternative
H
2
O
production
processes.
Although
several
new
processes
have
been
proposed,
environmental‐friendly
solar‐driven
attracts
most
because
only
inputs
water,
oxygen,
light
energy.
The
rational
design
functional
photo‐responsive
catalysts
promotes
in
photocatalytic
photoelectrocatalytic
approaches.
These
are,
general,
achieved
by
facilitating
preferential
adsorption
key
intermediates
OOH*/OH*/O*,
enhancing
absorption,
promoting
charge
separation,
accelerating
surface
transfer
with
selective
number
involved
charges.
This
review
systematically
summarizes
strategies
photo(electro)catalysts
toward
via
both
water
oxidation
oxygen
reduction
pathways.
Though
route
perceived
as
more
popular
community,
emerging
a
convincing
alternative.
Furthermore,
prevailing
hypotheses,
state‐of‐the‐art
catalysts,
critical
challenges,
perspectives
are
discussed
depth.
aims
to
enhance
comprehension
this
research
field
promote
interest
sustainable
production.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(15)
Published: Feb. 28, 2023
Abstract
Oxygen
reduction
reaction
via
the
two‐electron
route
(2e
−
ORR)
provides
a
green
method
for
direct
production
of
hydrogen
peroxide
(H
2
O
)
along
with
in
situ
utilization.
The
effective
catalysts
high
ORR
activity,
2e
selectivity,
and
stability
are
essential
application
this
technology.
Single‐atom
(SACs)
have
attracted
intensively
attention
H
electrosynthesis
owing
to
unique
geometric
electronic
configurations.
In
review,
mechanism
theoretical
predictions
over
SACs
first
introduced.
Then,
recent
advances
various
documented.
And
correlation
between
central
atom,
coordination
atoms,
environment
corresponding
electrocatalytic
performance
including
emphatically
analyzed
summarized.
Finally,
major
challenges
opportunities
regarding
future
design
pointed
out.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(14)
Published: Feb. 10, 2023
Proton
transfer
is
crucial
for
electrocatalysis.
Accumulating
cations
at
electrochemical
interfaces
can
alter
the
proton
rate
and
then
tune
electrocatalytic
performance.
However,
mechanism
regulating
remains
ambiguous.
Here,
we
quantify
cation
effect
on
diffusion
in
solution
by
hydrogen
evolution
microelectrodes,
revealing
be
suppressed
more
than
10
times.
Different
from
prevalent
opinions
that
transport
slowed
down
modified
electric
field,
found
water
structure
imposes
a
evident
kinetics.
FTIR
test
path
integral
molecular
dynamics
simulation
indicate
prefers
to
wander
within
hydration
shell
of
rather
hop
rapidly
along
wires.
Low
connectivity
networks
disrupted
corrupts
fast-moving
bulk
water.
This
study
highlights
promising
way
kinetics
via
structure.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(13), P. 9434 - 9443
Published: March 20, 2024
Electrocatalytic
synthesis
of
hydrogen
peroxide
(H2O2)
in
acidic
media
is
an
efficient
and
eco-friendly
approach
to
produce
inherently
stable
H2O2,
but
limited
by
the
lack
selective
catalysts
under
industrial-relevant
current
densities.
Herein,
we
report
a
diatomic
cobalt
catalyst
for
two-electron
oxygen
reduction
efficiently
H2O2
at
50–400
mA
cm–2
acid.
Electrode
kinetics
study
shows
>95%
selectivity
on
sites.
In
flow
cell
device,
record-high
production
rate
11.72
mol
gcat–1
h–1
exceptional
long-term
stability
(100
h)
are
realized
high
situ
spectroscopic
studies
theoretical
calculations
reveal
that
introducing
second
metal
into
coordination
sphere
site
can
optimize
binding
strength
key
intermediates
due
downshifted
d-band
center
cobalt.
We
also
demonstrate
feasibility
processing
municipal
plastic
wastes
through
decentralized
production.
