Nature Communications,
Год журнала:
2019,
Номер
10(1)
Опубликована: Июнь 26, 2019
Abstract
Formic
acid
(or
formate)
is
suggested
to
be
one
of
the
most
economically
viable
products
from
electrochemical
carbon
dioxide
reduction.
However,
its
commercial
viability
hinges
on
development
highly
active
and
selective
electrocatalysts.
Here
we
report
that
structural
defects
have
a
profound
positive
impact
electrocatalytic
performance
bismuth.
Bismuth
oxide
double-walled
nanotubes
with
fragmented
surface
are
prepared
as
template,
cathodically
converted
defective
bismuth
nanotubes.
This
electrocatalyst
enables
reduction
formate
excellent
activity,
selectivity
stability.
Most
significantly,
current
density
reaches
~288
mA
cm
−2
at
−0.61
V
versus
reversible
hydrogen
electrode
within
flow
cell
reactor
under
ambient
conditions.
Using
functional
theory
calculations,
activity
rationalized
outcome
abundant
sites
stabilize
*OCHO
intermediate.
Furthermore,
this
coupled
silicon
photocathodes
achieves
high-performance
photoelectrochemical
Journal of the American Chemical Society,
Год журнала:
2020,
Номер
142(12), С. 5702 - 5708
Опубликована: Март 2, 2020
Electrochemical
conversion
of
nitrate
(NO3–)
into
ammonia
(NH3)
recycles
nitrogen
and
offers
a
route
to
the
production
NH3,
which
is
more
valuable
than
dinitrogen
gas.
However,
today's
development
NO3–
electroreduction
remains
hindered
by
lack
mechanistic
picture
how
catalyst
structure
may
be
tuned
enhance
catalytic
activity.
Here
we
demonstrate
enhanced
reduction
reaction
(NO3–RR)
performance
on
Cu50Ni50
alloy
catalysts,
including
0.12
V
upshift
in
half-wave
potential
6-fold
increase
activity
compared
those
obtained
with
pure
Cu
at
0
vs
reversible
hydrogen
electrode
(RHE).
Ni
alloying
enables
tuning
d-band
center
modulates
adsorption
energies
intermediates
such
as
*NO3–,
*NO2,
*NH2.
Using
density
functional
theory
calculations,
identify
NO3–RR-to-NH3
pathway
offer
an
energy–activity
relationship
for
CuNi
system.
This
correlation
between
electronic
NO3–RR
design
platform
further
catalysts.
Journal of the American Chemical Society,
Год журнала:
2019,
Номер
141(19), С. 7646 - 7659
Опубликована: Апрель 15, 2019
Electrochemical
reduction
of
CO2
to
high-energy-density
oxygenates
and
hydrocarbons
beyond
CO
is
important
for
long-term
large-scale
renewable
energy
storage.
However,
the
key
step
C-C
bond
formation
needed
generation
C2
products
induces
an
additional
barrier
on
reaction.
This
inevitably
creates
larger
overpotentials
greater
variety
as
compared
conversion
C1
products.
Therefore,
in-depth
understanding
catalytic
mechanism
required
advancing
design
efficient
electrocatalysts
control
reaction
pathway
desired
Herein,
we
present
a
critical
appraisal
focusing
connection
between
fundamentals
electrocatalysts.
An
discussion
mechanistic
aspects
various
pathways
copper-based
catalysts
presented
together
with
consideration
practical
factors
under
electrocatalytic
operating
conditions.
By
providing
some
typical
examples
illustrating
benefit
merging
theoretical
calculations,
surface
characterization,
electrochemical
measurements,
try
address
issues
ongoing
debate
toward
better
at
atomic
level
envisioning
roadmap
generation.
Energy & Environmental Science,
Год журнала:
2019,
Номер
12(5), С. 1442 - 1453
Опубликована: Янв. 1, 2019
The
substantial
implications
of
high
current
densities
on
the
local
reaction
environment
and
design
catalysts
for
electrochemical
CO2
reduction
are
addressed.
presented
perspectives
also
reflect
practices
within
field
offer
new
opportunities
both
future
catalyst
system-focused
research
efforts.
Science,
Год журнала:
2021,
Номер
372(6546), С. 1074 - 1078
Опубликована: Июнь 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.
Chemical Reviews,
Год журнала:
2019,
Номер
120(2), С. 1184 - 1249
Опубликована: Окт. 3, 2019
The
surface
and
interfaces
of
heterogeneous
catalysts
are
essential
to
their
performance
as
they
often
considered
be
active
sites
for
catalytic
reactions.
With
the
development
nanoscience,
ability
tune
interface
nanostructures
has
provided
a
versatile
tool
optimization
catalyst.
In
this
Review,
we
present
control
nanoparticle
in
context
oxygen
reduction
reaction
(ORR),
electrochemical
CO2
(CO2
RR),
tandem
catalysis
three
sections.
first
section,
start
with
activity
ORR
on
nanoscale
then
focus
approaches
optimize
Pt-based
catalyst
including
using
alloying,
core-shell
structure,
high
area
open
structures.
section
RR,
where
composition
plays
dominant
role,
cover
its
fundamentals
different
nanosized
metal
catalysts.
For
catalysis,
adjacent
single
nanostructure
catalyze
sequential
reactions,
describe
concept
principle,
synthesis
methodology,
application
