Electrochemical Energy Reviews,
Год журнала:
2023,
Номер
6(1)
Опубликована: Июль 27, 2023
Abstract
The
low-temperature
electrolysis
of
CO
2
in
membrane-based
flow
reactors
is
a
promising
technology
for
converting
captured
into
valuable
chemicals
and
fuels.
In
recent
years,
substantial
improvements
reactor
design
have
significantly
improved
the
economic
viability
this
technology;
thus,
field
has
experienced
rapid
increase
research
interest.
Among
factors
related
to
design,
ion
exchange
membrane
(IEM)
plays
prominent
role
energetic
efficiency
conversion
useful
products.
Reactors
utilizing
cation
exchange,
anion
bipolar
membranes
all
been
developed,
each
providing
unique
benefits
challenges
that
must
be
overcome
before
large-scale
commercialization
feasible.
Therefore,
direct
advances
IEM
specific
electrochemical
reduction
reactions
(CO
RRs),
review
serves
first
provide
polymer
scientists
with
general
understanding
RR
membrane-related
shortcomings
encourage
systematic
synthetic
approaches
develop
meet
requirements
RRs.
Second,
provides
researchers
fields
electrocatalysis
RRs
more
detailed
insight
often-overlooked
roles
requirements;
new
methodologies
evaluation
during
may
developed.
By
using
-to-CO/HCOO
−
as
practical
baseline
systems,
clear
conceptualization
merits
different
systems
reasonable
objectives
future
development
are
presented.
Graphical
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Апрель 29, 2024
Electrochemical
carbon
dioxide/carbon
monoxide
reduction
reaction
offers
a
promising
route
to
synthesize
fuels
and
value-added
chemicals,
unfortunately
their
activities
selectivities
remain
unsatisfactory.
Here,
we
present
general
surface
molecular
tuning
strategy
by
modifying
Cu2O
with
pyridine-derivative.
The
modified
nanocubes
4-mercaptopyridine
display
high
Faradaic
efficiency
of
greater
than
60%
in
electrochemical
acetate
current
density
as
large
380
mA/cm2
liquid
electrolyte
flow
cell.
In-situ
attenuated
total
reflectance
surface-enhanced
infrared
absorption
spectroscopy
reveals
stronger
*CO
signal
bridge
configuration
*OCCHO
over
unmodified
during
CO
reduction.
Density
function
theory
calculations
disclose
that
local
can
effectively
regulate
the
electronic
structure
copper
catalyst,
enhancing
*CHO
intermediates
adsorption
stabilization
effect
through
hydrogen
bonding,
which
greatly
promote
asymmetric
*CO-*CHO
coupling
reaction.
iScience,
Год журнала:
2022,
Номер
25(4), С. 104010 - 104010
Опубликована: Март 4, 2022
Tackling
climate
change
is
one
of
the
undoubtedly
most
important
challenges
at
present
time.
This
review
deals
mainly
with
chemical
aspects
current
status
for
converting
greenhouse
gas
CO2
via
electrochemical
reduction
reaction
(CO2RR)
to
multicarbon
alcohols
as
valuable
products.
Feasible
routes
are
presented,
well
catalyst
synthesis
methods
such
electrodeposition,
precipitation,
or
sputtering.
In
addition,
a
comprehensive
overview
currently
achievable
selectivities
in
CO2RR
given.
It
also
outlined
what
extent,
example,
modifications
surfaces
use
bifunctional
compounds
product
distribution
shifted.
influence
varying
electrolyte,
temperature,
and
pressure
described
discussed.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(37), С. 20683 - 20691
Опубликована: Сен. 8, 2023
Metastable
state
is
the
most
active
catalyst
that
dictates
overall
catalytic
performance
and
rules
of
behaviors;
however,
identification
stabilization
metastable
are
still
highly
challenging
due
to
continuous
evolution
sites
during
reaction
process.
In
this
work,
operando119Sn
Mössbauer
measurements
theoretical
simulations
were
performed
track
identify
single-atom
Sn
in
copper
oxide
(Sn1-CuO)
for
selective
CO2
electroreduction
CO.
A
maximum
CO
Faradaic
efficiency
around
98%
at
-0.8
V
(vs.
RHE)
over
Sn1-CuO
was
achieved
an
optimized
loading
5.25
wt.
%.
Operando
spectroscopy
clearly
identified
dynamic
atomically
dispersed
Sn4+
CuO
matrix
enabled
situ
transformation
Sn4+-O4-Cu2+
a
Sn4+-O3-Cu+
under
CO2RR
conditions.
combination
with
quasi
X-ray
photoelectron
spectroscopy,
operando
Raman
attenuated
total
reflectance
surface
enhanced
infrared
absorption
spectroscopies,
promoted
desorption
*CO
Sn4+-O3
stabilized
adjacent
Cu+
site
evidenced.
addition,
density
functional
theory
calculations
further
verified
construction
as
true
altered
path
via
modifying
adsorption
configuration
*COOH
intermediate,
which
effectively
reduced
free
energy
required
hydrogenation
*CO,
thereby
greatly
facilitating
CO2-to-CO
conversion.
This
work
provides
fundamental
insight
into
role
single
atoms
on
tuning
electronic
structure
Cu-based
catalysts,
may
pave
way
development
efficient
catalysts
high-selectivity
electroreduction.
Electrochemical Energy Reviews,
Год журнала:
2023,
Номер
6(1)
Опубликована: Июль 27, 2023
Abstract
The
low-temperature
electrolysis
of
CO
2
in
membrane-based
flow
reactors
is
a
promising
technology
for
converting
captured
into
valuable
chemicals
and
fuels.
In
recent
years,
substantial
improvements
reactor
design
have
significantly
improved
the
economic
viability
this
technology;
thus,
field
has
experienced
rapid
increase
research
interest.
Among
factors
related
to
design,
ion
exchange
membrane
(IEM)
plays
prominent
role
energetic
efficiency
conversion
useful
products.
Reactors
utilizing
cation
exchange,
anion
bipolar
membranes
all
been
developed,
each
providing
unique
benefits
challenges
that
must
be
overcome
before
large-scale
commercialization
feasible.
Therefore,
direct
advances
IEM
specific
electrochemical
reduction
reactions
(CO
RRs),
review
serves
first
provide
polymer
scientists
with
general
understanding
RR
membrane-related
shortcomings
encourage
systematic
synthetic
approaches
develop
meet
requirements
RRs.
Second,
provides
researchers
fields
electrocatalysis
RRs
more
detailed
insight
often-overlooked
roles
requirements;
new
methodologies
evaluation
during
may
developed.
By
using
-to-CO/HCOO
−
as
practical
baseline
systems,
clear
conceptualization
merits
different
systems
reasonable
objectives
future
development
are
presented.
Graphical
