Proceedings of the National Academy of Sciences,
Год журнала:
2023,
Номер
120(4)
Опубликована: Янв. 17, 2023
Copper
is
distinctive
in
electrocatalyzing
reduction
of
CO
2
into
various
energy-dense
forms,
but
it
often
suffers
from
limited
product
selectivity
including
ethanol
competition
with
ethylene.
Here,
we
describe
systematically
designed,
bimetallic
electrocatalysts
based
on
copper/gold
heterojunctions
a
faradaic
efficiency
toward
60%
at
currents
excess
500
mA
cm
−2
.
In
the
modified
catalyst,
ratio
to
ethylene
enhanced
by
factor
200
compared
copper
catalysts.
Analysis
ATR-IR
measurements
under
operating
conditions,
and
computational
simulations,
suggests
that
heterojunction
dominated
generation
intermediate
OCCOH*.
The
latter
key
contributor
overall,
asymmetrical
electrohydrogenation
giving
rather
than
Chemical Society Reviews,
Год журнала:
2021,
Номер
50(23), С. 12897 - 12914
Опубликована: Янв. 1, 2021
This
tutorial
review
discusses
the
similarities
and
differences
between
electrocatalytic
reduction
of
CO
2
to
C
2+
olefins
oxygenates
over
Cu-based
catalysts.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(32), С. 14936 - 14944
Опубликована: Авг. 4, 2022
An
ampere-level
current
density
of
CO2
electrolysis
is
critical
to
realize
the
industrial
production
multicarbon
(C2+)
fuels.
However,
under
such
a
large
density,
poor
CO
intermediate
(*CO)
coverage
on
catalyst
surface
induces
competitive
hydrogen
evolution
reaction,
which
hinders
reduction
reaction
(CO2RR).
Herein,
we
report
reliable
CO2-to-C2+
by
heteroatom
engineering
Cu
catalysts.
The
Cu-based
compounds
with
(N,
P,
S,
O)
are
electrochemically
reduced
heteroatom-derived
significant
structural
reconstruction
CO2RR
conditions.
It
found
that
N-engineered
(N-Cu)
exhibits
best
productivity
remarkable
Faradaic
efficiency
73.7%
-1100
mA
cm-2
and
an
energy
37.2%
-900
cm-2.
Particularly,
it
achieves
C2+
partial
-909
at
-1.15
V
versus
reversible
electrode,
outperforms
most
reported
In
situ
spectroscopy
indicates
adjusts
*CO
adsorption
alters
local
H
proton
consumption
in
solution.
Density
functional
theory
studies
confirm
high
strength
N-Cu
results
from
depressed
HER
promoted
both
bridge
atop
sites
Cu,
greatly
reduces
barrier
for
C-C
coupling.
Journal of the American Chemical Society,
Год журнала:
2021,
Номер
143(47), С. 19630 - 19642
Опубликована: Ноя. 17, 2021
Given
the
limited
product
variety
of
electrocatalytic
CO2
reduction
reactions
solely
from
and
H2O
as
reactants,
it
is
desirable
to
expand
scope
by
introducing
additional
reactants
that
provide
elemental
diversity.
The
integration
inorganic
heteroatom-containing
into
could,
in
principle,
enable
sustainable
synthesis
valuable
products,
such
organonitrogen
compounds,
which
have
widespread
applications
but
typically
rely
on
NH3
derived
energy-intensive
fossil-fuel-dependent
Haber–Bosch
process
for
their
industrial-scale
production.
In
this
Perspective,
research
progress
toward
building
C–N
bonds
N-integrated
highlighted,
electrosyntheses
urea,
acetamides,
amines
are
examined
standpoints
reactivity,
catalyst
structure,
and,
most
fundamentally,
mechanism.
Mechanistic
discussions
coupling
these
advances
emphasized
critically
evaluated,
with
aim
directing
future
investigations
improving
yield
broadening
reduction.
Accounts of Chemical Research,
Год журнала:
2022,
Номер
55(5), С. 638 - 648
Опубликована: Янв. 18, 2022
ConspectusCarbon
capture,
utilization,
and
sequestration
play
an
essential
role
to
address
CO2
emissions.
Among
all
carbon
utilization
technologies,
electroreduction
has
gained
immense
interest
due
its
potential
for
directly
converting
a
variety
of
valuable
commodity
chemicals
using
clean,
renewable
electricity
as
the
sole
energy
source.
The
research
community
witnessed
rapid
advances
in
electrolysis
technology
recent
years,
including
highly
selective
catalysts,
larger-scale
reactors,
specific
process
modeling,
well
mechanistic
understanding
reduction
reaction.
field
brings
promise
commercial
application
rollout
chemical
manufacturing.This
Account
focuses
on
our
contributions
both
fundamental
applied
electrocatalytic
CO
reactions.
We
first
discuss
(1)
development
novel
electrocatalysts
CO2/CO
enhance
product
selectivity
lower
consumption.
Specifically,
we
synthesized
nanoporous
Ag
homogeneously
mixed
Cu-based
bimetallic
catalysts
enhanced
production
from
multicarbon
products
CO,
respectively.
Then,
review
efforts
(2)
reactor
engineering,
dissolved
H-type
cell,
vapor-fed
three-compartment
flow
membrane
electrode
assembly,
enhancing
reaction
rates
scalability.
Next,
describe
(3)
investigation
mechanisms
situ
operando
techniques,
such
surface-enhanced
vibrational
spectroscopies
electrochemical
mass
spectroscopy.
revealed
participation
bicarbonate
Au
attenuated
total-reflectance
infrared
absorption
spectroscopy,
presence
"oxygenated"
surface
Cu
under
conditions
Raman
origin
oxygen
acetaldehyde
other
electrolyzer
spectrometry.
Lastly,
examine
(4)
technology,
pollutant
effects
developing
techno-economic
analysis.
SO2
NOx
Cu,
Ag,
Sn
catalysts.
also
identify
technical
barriers
that
need
be
overcome
offer
perspective
accelerating
deployment
technology.
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.
Chemical Society Reviews,
Год журнала:
2023,
Номер
52(6), С. 2193 - 2237
Опубликована: Янв. 1, 2023
Electrochemical
C–N
coupling
reaction
by
renewable
electricity
for
the
electrosynthesis
of
organonitrogen
compounds
with
abundant
CO
2
and
nitrogenous
small
molecules
as
carbon
nitrogen
sources,
respectively,
is
a
promising
sustainable
synthetic
strategy.
ACS Energy Letters,
Год журнала:
2023,
Номер
8(4), С. 1992 - 2024
Опубликована: Март 30, 2023
The
study
of
the
electrochemical
CO2
reduction
to
obtain
formate
(HCOO–)
or
formic
acid
(HCOOH)
is
receiving
much
attention
as
a
promising
technology.
Since
continuous–mode
operation
has
become
necessary
for
practical
implementation
reduction,
recent
years
have
seen
rapid
increase
in
number
research
approaches
focusing
on
this
aspect.
This
Focus
Review
provides
unified
discussion
available
studies
continuous
electroreduction
HCOO–/HCOOH,
considering
different
important
features
process
design.
Moreover,
paper
quantitatively
assesses
performance
that
involve
reactors
converting
HCOOH/HCOO–,
comparing
relevant
typically
used
figures
merit,
including
energy
consumption.
Although
some
trade-offs
already
been
achieved,
simultaneous
optimization
all
merit
remains
challenge.
Finally,
concluding
remarks
highlight
detected
trends
and
discuss
aspects
will
be
tackled
by
future
field.
