Acta Physico-Chimica Sinica,
Год журнала:
2023,
Номер
0(0), С. 2308027 - 2308027
Опубликована: Янв. 1, 2023
The
electrochemical
carbon
dioxide
reduction
reaction
(eCO2RR)
can
convert
CO2
into
valuable
chemicals,
achieving
a
cycle.Copper-based
catalysts
have
demonstrated
unique
ability
to
produce
C2+
products
in
eCO2RR,
which
is
often
limited
by
the
scaling
relationship
of
intermediates,
complex
mechanism
and
competitive
H2
evolution.Organic
functionalization
promising
strategy
for
regulating
activity
selectivity
eCO2RR
toward
products.However,
behind
such
regulation
especially
at
molecular
level,
remains
elusive.In
this
study,
Cu
nanoparticles
were
prepared
functionalized
with
set
amine
derivatives,
including
hexadecylamine
(HDA),
N-methylhexadecylamine
(N-MHDA),
hexadecyldimethylamine
(HDDMA),
palmitamide
(PMM).The
impact
structure
surfactants
on
was
systematically
explored
through
both
experiments
theoretical
calculations.X-ray
photoelectron
spectroscopy
density
functional
theory
calculations
revealed
that
HDA
catalyst
surface
resulted
negative
charge
transfer
from
molecules
Cu.
ECO2RR
examined
1.0
mol•L
-1
KOH
aqueous
electrolyte.HDA
achieved
highest
Faradaic
efficiency
(FE)
73.5%
C2
46.4%
C2H4,
respectively.It
also
provided
partial
current
131.4
mA•cm
-2
-0.9
V
vs.
reversible
hydrogen
electrode
(RHE)
among
these
derivatives
catalysts.In
contrast,
FE
pristine
only
27.0%
50.5
,
respectively.Theoretical
studies
bonding
interactions
intermediates
enriched
CO2,
CO,
other
lowered
kinetic
energy
barrier
CO-CHO
coupling
thereby
promoted
products.Replacing
H
atoms
group
methyl
groups
N-MHDA
HDDMA
dominant
evolution
(HER)
eCO2RR.PMM
Cu-O
bond,
instead
Cu-N
as
HDA,
HDDMA,
preferred
ethanol
production.In
situ
Raman
indicated
CO
adsorption
atop
sites
HDA-capped
catalysts,
bridge
site
clean
surfaces,
possibly
due
former
case.HDA
increased
local
pH
relative
catalysts.The
Cu-HDA-based
rechargeable
Zn-CO2
battery
exhibited
superior
maximum
power
6.48
mW•cm
discharge
16
remarkable
durability
60
h,
outperforming
most
reported
literature.This
work
enhances
CO2-C2
conversion
tuning
Cu-based
materials,
unravels
provides
new
insights
promoting
organic
molecules.
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(32), С. 20990 - 20998
Опубликована: Янв. 1, 2024
This
work
benchmarks
ionomers
for
CO
2
electroreduction
to
multicarbon
products.
Ionomers
with
stronger
hydrophobicity
or
having
bulkier
and
less
hydrated
ionised
side
chains
were
found
favour
*CO
adsorption
product
formation.
Journal of CO2 Utilization,
Год журнала:
2024,
Номер
85, С. 102880 - 102880
Опубликована: Июль 1, 2024
In
the
quest
to
mitigate
excessive
CO2
emissions,
electrochemical
reduction
of
(eCO2R)
into
multi-carbon
fuels
and
vital
chemical
precursors
emerges
as
a
compelling
strategy.
Meticulous
control
C–C
coupling
on
catalyst
surface
is
grand
challenge
in
selective
production
desired
C2+
products.
Ethane
propanol
are
among
most
desirable
products
gas
liquid
phase,
respectively.
Herein,
we
demonstrate
facile
femtosecond
laser-enabled
tuning
Cu
selectivity
towards
ethane
propanol.
The
tailoring
induces
shift
from
C1
This
product
composition
attributed
concurrent
creation
hierarchical
porous
structures,
stabilization
{111},
{200},
{220}
Cu2O
facets,
promotion
Cu1+
oxidation
state.
These
alterations
collectively
enhance
adsorption
strength,
leading
an
increased
propensity
for
C-C
and,
consequently,
elevated
toward
Inorganic Chemistry Frontiers,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
This
paper
reviews
the
progress
of
defective
Cu-based
materials
for
eCO
2
RR,
highlights
design
strategy
defect
structure
and
emphasizes
mechanism
site
on
catalytic
behaviors.
Single
atom
catalyst
(SAC)
show
significant
promise
in
electrocatalytic
carbon
dioxide
reduction
reaction
(eCO2RR)
to
produce
valuable
chemicals,
representing
one
of
the
most
promising
ways
achieve
a
neutral
cycle.
Methane
is
many
products
from
eCO2RR.
Rational
design
SAC
through
deliberate
coordination
regulation
and
controlled
synthesis
at
low
temperatures
toward
methane
production
remains
very
limited.
Herein
this
paper,
Cu
with
four
oxygen
atoms
(Cu-O4)
were
prepared
by
soaking
nanocrystals
on
support
acetic
acid
solution
60
°C
for
12
h.
The
structure
was
revealed
extended
X-ray
absorption
fine
spectrum
photoelectron
spectroscopy.
Cu-O4
demonstrates
excellent
activity
selectivity
towards
production,
Faradaic
efficiency
(FE)
63.0%
partial
current
density
200.5
mA
cm-2.
Theoretical
calculation
indicates
less
positive
charge
center
stronger
delocalization
than
Cu-N4
due
π
bonding
interaction
SAC,
which
stabilizes
intermediates
lowers
potential
determining
step
SAC.
Strong
hydrogen
adsorption
suppresses
evolution
may
favor
hydrogenation
methane.
limiting
that
more
favored
CO,
methanol
formate,
corroborating
high
This
work
highlights
importance
environment
steering
Journal of Materials Chemistry A,
Год журнала:
2023,
Номер
11(23), С. 12121 - 12129
Опубликована: Янв. 1, 2023
A
Cu-BTC-CP
precatalyst
with
asymmetric
building
units,
which
in
situ
reconstructs
to
low-coordinated
Cu
during
the
CO
2
RR,
delivers
an
ethylene
faradaic
efficiency
of
65.2
±
3%
at
350
mA
cm
−2
a
flow
cell.
