Photocatalytic
conversion
of
carbon
dioxide
(CO2)
to
fuel
provides
an
ideal
pathway
achieving
neutrality.
One
significant
hindrance
in
the
reduction
CO2
higher
energy
density
multicarbon
products
(C2+)
was
difficulty
coupling
C–C
bonds
efficiently.
Copper
(Cu)
is
considered
most
suitable
metal
catalyst
for
form
C2+
reaction
(CO2RR),
but
it
encounters
challenges
such
as
low
product
selectivity
and
slow
catalytic
efficiency.
Herein,
we
constructed
a
defect
on
Cu-doped
nitride
(Cu–CvN),
efficient
photocatalytic
CO2RR.
The
optimized
(Cu–CvN-550)
with
shows
high
activity
ethanol,
ethanol
production
rate
122.6
μmol
g–1
h–1
93.7%.
yield
4.5
times
than
that
Cu–CN-550
without
defect.
ratio
Cu+/Cu0
Cu
species
changes
regularly
calcination
temperature,
which
linearly
correlated
liquid
DFT
calculations
combined
experimental
results
revealed
doping
promoted
activation,
followed
by
enhanced
*CO
adsorption
weakened
hydrogenation
desorption.
Carbon
defects
lower
free
greatly
accelerate
transfer
process
promoting
formation
six-membered
ring
intermediate
state,
serving
intramolecular
dimerization.
Synergistic
thermodynamic
kinetic
interactions
were
realized
through
introduction
defects,
thereby
enhancing
performance
production.
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 7, 2025
Abstract
Photocatalytic
CO
2
reduction
into
high‐value
C
2+
products
such
as
H
6
is
of
great
importance
but
challenging
due
to
their
multi‐electron
steps
and
high
energy
barrier
C─C
coupling.
Moreover,
improving
its
solar‐to‐chemical
(STC)
conversion
efficiency
in
pure
water
beyond
the
current
1%
empirical
value
also
a
significant
challenge.
Herein,
graphite
carbon
nitride
(g‐C
3
N
4
)
nanosheets
with
controllable
(C)
doping
nitrogen
(N)
vacancies
(PCCN‐x)
are
designed
through
biochar‐tailored
protocol
for
efficiently
selectively
photo‐converting
.
The
optimal
PCCN‐10
photocatalyst
enables
achievement
an
exceptional
activity
99.14
µmol
g
−1
h
selectivity
80.33%
over
20
water.
A
record
STC
≈1.13%
solar
fuel
production
from
O
vapor
achieved
without
any
other
inputs.
Outdoor
tests
demonstrated
impressive
‐to‐C
photo‐conversion
rate
43.17
water,
stable
50
period.
Critically,
experimental
theoretical
calculations
further
confirm
pivotal
role
bridged
sites
activating
molecules
promoting
formation
coupling
intermediate
(
*
OCCO),
which
very
beneficial
performance
this
work
photocatalytic
fuels
paves
way
large‐scale
broader
sustainable
applications.
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Jan. 1, 2024
Metal
oxides,
metal
sulfides,
MXenes,
and
metal–organic
frameworks
act
as
catalysts,
while
covalent
organic
frameworks,
carbon
nitrides,
phosphides,
graphene
oxides
serve
cocatalysts
for
CO
2
photoreduction
to
multicarbon
products.
Inorganic Chemistry,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 9, 2025
The
production
of
high-energy-density
liquid
fuels
through
the
photoconversion
CO2
offers
a
highly
efficient
method
for
storing
sustainable
solar
energy
future
use.
Bi4Ti3O12
(BTO)
nanorods
loaded
with
Cu–Pd
nanoalloys
were
designed
selective
photoreduction
to
ethyl
alcohol,
using
H2O
as
proton
source.
A
tandem
synergistic
catalysis
mechanism
was
proposed
this
process.
Initially,
*CO
intermediates
are
produced
at
BTO
nanorod,
then
transfer
neighboring
Cu
atoms,
where
they
convert
into
alcohol
via
C–C
bond
formation
on
Pd
atoms.
Adjusting
ratio
can
modify
binding
strength
catalyst
surface
and
reaction
kinetics
reduction,
thus
optimizing
efficiency
selectivity
products.
With
substitution
TiO2,
CeO2,
SiO2
nanorod
in
similar
systems,
only
CO
or
CH4
produced,
highlighting
essential
role
present
photoconversion.
Additionally,
thermal-assisted
photocatalysis
also
tested
lower
free
barrier
*OCCO
intermediate,
crucial
production,
enhance
charge
separation
BTO,
leading
2.7-fold
improvement
compared
that
under
light
illumination
alone.
photocatalytic
reduction
device
well
area
25
cm
×
cm,
providing
potential
model
large-scale
from
CO2.
This
research
may
pave
way
utilizing
effects
metal
active
sites
photocatalyst
substrates
generation
multicarbon
species
reduction.
