Science,
Journal Year:
2021,
Volume and Issue:
372(6546), P. 1074 - 1078
Published: June 3, 2021
Carbon
dioxide
electroreduction
(CO2R)
is
being
actively
studied
as
a
promising
route
to
convert
carbon
emissions
valuable
chemicals
and
fuels.
However,
the
fraction
of
input
CO2
that
productively
reduced
has
typically
been
very
low,
<2%
for
multicarbon
products;
balance
reacts
with
hydroxide
form
carbonate
in
both
alkaline
neutral
reactors.
Acidic
electrolytes
would
overcome
this
limitation,
but
hydrogen
evolution
hitherto
dominated
under
those
conditions.
We
report
concentrating
potassium
cations
vicinity
electrochemically
active
sites
accelerates
activation
enable
efficient
CO2R
acid.
achieve
on
copper
at
pH
<1
single-pass
utilization
77%,
including
conversion
efficiency
50%
toward
products
(ethylene,
ethanol,
1-propanol)
current
density
1.2
amperes
per
square
centimeter
full-cell
voltage
4.2
volts.
Journal of the American Chemical Society,
Journal Year:
2020,
Volume and Issue:
142(45), P. 19339 - 19345
Published: Oct. 29, 2020
Photocatalytic
reduction
of
CO2
to
value-added
fuels
is
a
promising
route
reduce
global
warming
and
enhance
energy
supply.
However,
poor
selectivity
low
efficiency
catalysts
are
usually
the
limiting
factor
their
applicability.
Herein,
photoinduction
method
was
developed
achieve
formation
Cu
single
atoms
on
UiO-66-NH2
support
(Cu
SAs/UiO-66-NH2)
that
could
significantly
boost
photoreduction
liquid
fuels.
Notably,
SAs/UiO-66-NH2
achieved
solar-driven
conversion
methanol
ethanol
with
an
evolution
rate
5.33
4.22
μmol
h-1
g-1,
respectively.
These
yields
were
much
higher
than
those
pristine
nanoparticles/UiO-66-NH2
composites.
Theoretical
calculations
revealed
introduction
SAs
greatly
facilitates
CHO*
CO*
intermediates,
leading
excellent
toward
ethanol.
This
study
provides
new
insights
for
designing
high-performance
catalyst
photocatalytic
at
atomic
scale.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(36), P. 19572 - 19590
Published: Feb. 19, 2021
Abstract
Compared
to
modern
fossil‐fuel‐based
refineries,
the
emerging
electrocatalytic
refinery
(e‐refinery)
is
a
more
sustainable
and
environmentally
benign
strategy
convert
renewable
feedstocks
energy
sources
into
transportable
fuels
value‐added
chemicals.
A
crucial
step
in
conducting
e‐refinery
processes
development
of
appropriate
reactions
optimal
electrocatalysts
for
efficient
cleavage
formation
chemical
bonds.
However,
compared
well‐studied
primary
(e.g.,
O
2
reduction,
water
splitting),
mechanistic
aspects
materials
design
complex
are
yet
be
settled.
To
address
this
challenge,
herein,
we
first
present
fundamentals
heterogeneous
electrocatalysis
some
reactions,
then
implement
these
establish
framework
by
coupling
situ
generated
intermediates
(integrated
reactions)
or
products
(tandem
reactions).
We
also
set
principles
strategies
efficiently
manipulate
reaction
pathways.
Nature Communications,
Journal Year:
2020,
Volume and Issue:
11(1)
Published: Oct. 16, 2020
Carbonate
formation
is
the
primary
source
of
energy
and
carbon
losses
in
low-temperature
dioxide
electrolysis.
Realigning
research
priorities
to
address
carbonate
problem
essential
if
this
technology
become
a
viable
option
for
renewable
chemical
fuel
production.
Low-temperature
electrolysis
an
attractive
process
sustainable
synthesis,
but
current
systems
suffer
from
low
efficiency.
In
comment,
authors
discuss
limitations
arising
reaction
between
hydroxide,
highlighting
need
new
fundamental
problem.
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(23), P. 12897 - 12914
Published: Jan. 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.
Advanced Powder Materials,
Journal Year:
2021,
Volume and Issue:
1(1), P. 100013 - 100013
Published: Nov. 15, 2021
Various
metal-based
electrocatalysts
from
nanocrystals,
to
clusters
and
single-atoms,
have
been
well-discovered
towards
high-efficient
power
devices
electrocatalytic
conversion.
To
accelerate
energy
transformation
materials
discovery,
developing
high-throughput
DFT
calculations
machine-learning
techniques
is
of
great
necessity.
This
review
comprehensively
outlines
the
latest
progress
theory-guided
design
advanced
materials.
Especially,
we
focus
on
study
single
atoms
in
various
devices,
such
as
fuel
cell
(oxygen
reduction
reaction,
ORR;
acid
oxidation
reaction;
alcohol
reaction),
other
reactions
for
energy-related
conversion
small
molecules,
H2O2
evolution
(2e−
ORR),
water
splitting
(H2
reaction/O2
HER/OER),
N2
reaction
(NRR),
CO2
(CO2RR).
Firstly,
electronic
structure,
interaction
mechanism,
activation
path
are
discussed
provide
an
overall
blueprint
electrocatalysis
batteries
mentioned
above.
Thereafter,
experimental
synthesis
strategies,
structural
recognition,
performance
figured
out.
Finally,
some
viewpoints
into
current
issues
future
concept
provided.