Nature Communications,
Год журнала:
2022,
Номер
13(1)
Опубликована: Фев. 10, 2022
Electrochemical
reduction
of
CO2
(CO2ER)
has
received
significant
attention
due
to
its
potential
sustainably
produce
valuable
fuels
and
chemicals.
However,
the
reaction
mechanism
is
still
not
well
understood.
One
vital
debate
whether
rate-limiting
step
(RLS)
dominated
by
availability
protons,
conversion
water
molecules,
or
adsorption
CO2.
This
paper
describes
insights
into
RLS
investigating
pH
dependency
kinetic
isotope
effect
with
respect
rate
expression
CO2ER.
Focusing
on
electrocatalysts
geared
towards
two-electron
transfer
reactions,
we
find
generation
rates
CO
formate
be
invariant
either
deuteration
electrolyte
over
Au,
Ag,
Sn,
In.
We
elucidate
CO2ER
onto
surface
electrocatalysts.
expect
this
finding
provide
guidance
for
improving
activity
through
enhancement
processes
strategies
such
as
modification
catalysts
careful
control
pressure
interfacial
electric
field
within
reactors.
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(38), С. 20627 - 20648
Опубликована: Апрель 17, 2021
Abstract
The
electrochemical
carbon
dioxide
reduction
reaction
(CO
2
RR)
provides
an
attractive
approach
to
convert
renewable
electricity
into
fuels
and
feedstocks
in
the
form
of
chemical
bonds.
Among
different
CO
RR
pathways,
conversion
is
considered
one
most
promising
candidate
reactions
because
its
high
technological
economic
feasibility.
Integrating
catalyst
electrolyte
design
with
understanding
catalytic
mechanism
will
yield
scientific
insights
promote
this
technology
towards
industrial
implementation.
Herein,
we
give
overview
recent
advances
challenges
for
selective
CO.
Multidimensional
engineering
are
also
summarized.
Furthermore,
studies
on
large‐scale
production
highlighted
facilitate
industrialization
.
To
conclude,
remaining
future
directions
application
generate
highlighted.
Advanced Materials,
Год журнала:
2020,
Номер
32(44)
Опубликована: Июль 14, 2020
Abstract
Electrocatalysis
is
at
the
center
of
many
sustainable
energy
conversion
technologies
that
are
being
developed
to
reduce
dependence
on
fossil
fuels.
The
past
decade
has
witnessed
significant
progresses
in
exploitation
advanced
electrocatalysts
for
diverse
electrochemical
reactions
involved
electrolyzers
and
fuel
cells,
such
as
hydrogen
evolution
reaction
(HER),
oxygen
reduction
(ORR),
CO
2
(CO
RR),
nitrogen
(NRR),
(OER).
Herein,
recent
research
advances
made
porous
these
five
important
reviewed.
In
discussions,
an
attempt
highlight
advantages
multiobjective
optimization
surface
active
sites
including
not
only
their
density
accessibility
but
also
intrinsic
activity.
First,
current
knowledge
about
electrocatalytic
briefly
summarized.
Then,
mechanisms
above‐mentioned
(HER,
ORR,
RR,
NRR,
OER),
challenges
faced
by
reactions,
efforts
meet
using
examined.
Finally,
future
directions
synthetic
strategies
leading
materials,
insights
into
sites,
standardized
tests
performance
requirements
discussed.
Energy & Environmental Science,
Год журнала:
2020,
Номер
13(9), С. 2856 - 2863
Опубликована: Янв. 1, 2020
We
discover
that
an
Sb
single
atom
material
consisting
of
Sb–N4
moieties
anchored
on
N-doped
carbon
nanosheets
can
serve
as
a
CO2RR
catalyst
to
produce
formate
with
high
efficiency.
Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
59(50), С. 22465 - 22469
Опубликована: Сен. 2, 2020
Abstract
Main‐group
element
indium
(In)
is
a
promising
electrocatalyst
which
triggers
CO
2
reduction
to
formate,
while
the
high
overpotential
and
low
Faradaic
efficiency
(FE)
hinder
its
practical
application.
Herein,
we
rationally
design
new
In
single‐atom
catalyst
containing
exclusive
isolated
δ+
–N
4
atomic
interface
sites
for
electroreduction
formate
with
efficiency.
This
exhibits
an
extremely
large
turnover
frequency
(TOF)
up
12500
h
−1
at
−0.95
V
versus
reversible
hydrogen
electrode
(RHE),
FE
of
96
%
current
density
8.87
mA
cm
−2
potential
−0.65
RHE.
Our
findings
present
feasible
strategy
accurate
regulation
main‐group
catalysts
scale.
ACS Nano,
Год журнала:
2022,
Номер
16(12), С. 19959 - 19979
Опубликована: Дек. 15, 2022
To
utilize
intermittent
renewable
energy
as
well
achieve
the
goals
of
peak
carbon
dioxide
emissions
and
neutrality,
various
electrocatalytic
devices
have
been
developed.
However,
reactions,
e.g.,
hydrogen
evolution
reaction/oxygen
reaction
in
overall
water
splitting,
polysulfide
conversion
lithium–sulfur
batteries,
formation/decomposition
lithium
peroxide
lithium–oxygen
nitrate
reduction
to
degrade
sewage,
suffer
from
sluggish
kinetics
caused
by
multielectron
transfer
processes.
Owing
merits
accelerated
charge
transport,
optimized
adsorption/desorption
intermediates,
raised
conductivity,
regulation
microenvironment,
ease
combine
with
geometric
characteristics,
built-in
electric
field
(BIEF)
is
expected
overcome
above
problems.
Here,
we
give
a
Review
about
very
recent
progress
BIEF
for
efficient
electrocatalysis.
First,
construction
strategies
characterization
methods
(qualitative
quantitative
analysis)
are
summarized.
Then,
up-to-date
overviews
engineering
electrocatalysis,
attention
on
electron
structure
optimization
microenvironment
modulation,
analyzed
discussed
detail.
In
end,
challenges
perspectives
proposed.
This
gives
deep
understanding
design
electrocatalysts
next-generation
storage
devices.
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(20), С. 11487 - 11493
Опубликована: Март 8, 2021
Abstract
Electrochemical
carbon
dioxide
(CO
2
)
reduction
reaction
RR)
is
an
attractive
approach
to
deal
with
the
emission
of
CO
and
produce
valuable
fuels
chemicals
in
a
carbon‐neutral
way.
Many
efforts
have
been
devoted
boost
activity
selectivity
high‐value
multicarbon
products
(C
2+
on
Cu‐based
electrocatalysts.
However,
RR
electrocatalysts
suffer
from
poor
catalytic
stability
mainly
due
structural
degradation
loss
active
species
under
condition.
To
date,
most
reported
present
stabilities
over
dozens
hours,
which
limits
advance
for
RR.
Herein,
porous
chlorine‐doped
Cu
electrocatalyst
exhibits
high
C
Faradaic
efficiency
(FE)
53.8
%
at
−1.00
V
versus
reversible
hydrogen
electrode
(V
RHE
).
Importantly,
catalyst
exhibited
outstanding
long‐term
electrocatalysis
240
h.
Experimental
results
show
that
chlorine‐induced
stable
cationic
0
/Cu
+
well‐preserved
structure
abundant
sites
are
critical
FE
run
electrochemical
reduction.
Energy & Environmental Science,
Год журнала:
2021,
Номер
14(3), С. 1247 - 1285
Опубликована: Янв. 1, 2021
This
review
provides
an
overview
of
advances
on
constructing
heterogeneous
nanostructured
and
single
atom
catalysts
for
CO2hydrogenation
to
formic
acid/formate.
The
main
focus
is
placed
structure–activity
correlations
mechanistic
insights.
Energy & Environmental Science,
Год журнала:
2022,
Номер
15(9), С. 3603 - 3629
Опубликована: Янв. 1, 2022
The
review
summarizes
the
recent
strategies
to
improve
energy
efficiency
of
CO
2
electroreduction,
a
guiding
metric
for
industrial
application
and
economic
feasibility,
with
emphasis
on
designing
remarkable
catalyst
advanced
electrolysis
system.