Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(21)
Опубликована: Март 23, 2023
Hydrogen
peroxide
(H2
O2
)
is
an
indispensable
basic
reagent
in
various
industries,
such
as
textile
bleach,
chemical
synthesis,
and
environmental
protection.
However,
it
challenging
to
prepare
H2
a
green,
safe,
simple
efficient
way
under
ambient
conditions.
Here,
we
found
that
could
be
synthesized
using
catalytic
pathway
only
by
contact
charging
two-phase
interface
at
room
temperature
normal
pressure.
Particularly,
the
action
of
mechanical
force,
electron
transfer
occurs
during
physical
between
polytetrafluoroethylene
particles
deionized
water/O2
interfaces,
inducing
generation
reactive
free
radicals
(⋅OH
⋅O2-
),
react
form
,
yielding
high
313
μmol
L-1
h-1
.
In
addition,
new
reaction
device
show
long-term
stable
production.
This
work
provides
novel
method
for
preparation
which
may
also
stimulate
further
explorations
on
contact-electrification-induced
chemistry
process.
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.
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 Energy Materials,
Год журнала:
2020,
Номер
11(15)
Опубликована: Дек. 18, 2020
Abstract
Hydrogen
peroxide
(H
2
O
)
is
an
environmentally
friendly
oxidant,
finding
widespread
use
across
the
chemical
industry,
in
sanitation
and
environmental
remediation.
Currently,
H
manufactured
via
anthraquinone
process
which
has
a
number
of
disadvantages
including
nondistributed
production,
high‐energy
consumption,
substantial
organic
by‐product
waste,
need
to
transport
obtained
point‐of‐use.
Accordingly,
electrochemical
synthesis
now
attracting
lot
interest
as
alternative,
cost‐effective,
small‐scale,
distributed
technology
for
manufacture.
This
review
summarizes
recent
advancements
development
Homogeneous
Heterogeneous
catalysts
electrocatalytic
reduction
reaction
(ORR)
.
The
basic
principles
ORR,
methodologies
investigating
ORR
are
first
introduced.
Next,
production
over
discussed,
with
focus
on
mechanisms
factors
that
influence
activity,
selectivity,
kinetics.
Subsequently,
breakthroughs
catalysts,
nonnoble
metal‐based
nanomaterials,
carbon
materials,
single‐atom
described.
latter
given
special
attention,
since
they
serve
bridge
between
catalysis
catalysis,
while
also
offering
excellent
performance.
Finally,
challenges
opportunities
critically
discussed.
Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
60(19), С. 10469 - 10480
Опубликована: Сен. 16, 2020
Abstract
Hydrogen
peroxide
(H
2
O
),
as
a
green
fuel
and
oxidant,
has
drawn
increasing
attention
in
the
energy
environmental
research.
Compared
with
traditional
anthraquinone
process,
electrochemical
(EC)
photoelectrochemical
(PEC)
syntheses
of
H
are
cost‐effective
environmentally
friendly.
In
order
to
construct
membraneless
EC/PEC
devices
for
full
synthesis,
anodic
production
by
water
oxidation,
which
is
less
developed
than
cathodic
generation,
highly
desirable.
Here,
we
review
recent
developments
including
fundamental
aspects,
benchmarking
activity
evaluation,
material/catalyst
selection,
strategies
selectivity,
efficiency,
accumulation.
Furthermore,
discuss
challenges
outlook
oxidation
production,
especially
device‐level
development,
accumulation
stability,
industrial
applications.
Our
intended
stimulate
studies
further
improving
production.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(12)
Опубликована: Янв. 19, 2022
The
in-depth
understanding
of
local
atomic
environment-property
relationships
p-block
metal
single-atom
catalysts
toward
the
2
e-
oxygen
reduction
reaction
(ORR)
has
rarely
been
reported.
Here,
guided
by
first-principles
calculations,
we
develop
a
heteroatom-modified
In-based
metal-organic
framework-assisted
approach
to
accurately
synthesize
an
optimal
catalyst,
in
which
single
In
atoms
are
anchored
combined
N,S-dual
first
coordination
and
B
second
supported
hollow
carbon
rods
(In
SAs/NSBC).
SAs/NSBC
catalyst
exhibits
high
H2
O2
selectivity
above
95
%
wide
range
pH.
Furthermore,
SAs/NSBC-modified
natural
air
diffusion
electrode
unprecedented
production
rate
6.49
mol
peroxide
gcatalyst-1
h-1
0.1
M
KOH
electrolyte
6.71
PBS
electrolyte.
This
strategy
enables
design
next-generation
high-performance
materials,
provides
practical
guidance
for
electrosynthesis.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Янв. 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.
