Chemical Reviews,
Journal Year:
2020,
Volume and Issue:
121(2), P. 1007 - 1048
Published: Dec. 22, 2020
The
unprecedented
ability
of
computations
to
probe
atomic-level
details
catalytic
systems
holds
immense
promise
for
the
fundamentals-based
bottom-up
design
novel
heterogeneous
catalysts,
which
are
at
heart
chemical
and
energy
sectors
industry.
Here,
we
critically
analyze
recent
advances
in
computational
catalysis.
First,
will
survey
progress
electronic
structure
methods
atomistic
catalyst
models
employed,
have
enabled
catalysis
community
build
increasingly
intricate,
realistic,
accurate
active
sites
supported
transition-metal
catalysts.
We
then
review
developments
microkinetic
modeling,
specifically
mean-field
kinetic
Monte
Carlo
simulations,
bridge
gap
between
nanoscale
insights
macroscale
experimental
kinetics
data
with
increasing
fidelity.
finally
advancements
theoretical
accelerating
discovery.
Throughout
review,
provide
ample
examples
applications,
discuss
remaining
challenges,
our
outlook
near
future.
ACS Energy Letters,
Journal Year:
2018,
Volume and Issue:
4(1), P. 317 - 324
Published: Dec. 14, 2018
Significant
advances
have
been
made
in
recent
years
discovering
new
electrocatalysts
and
developing
a
fundamental
understanding
of
electrochemical
CO2
reduction
processes.
This
field
has
progressed
to
the
point
that
efforts
can
now
focus
on
translating
this
knowledge
toward
development
practical
electrolyzers,
which
potential
replace
conventional
petrochemical
processes
as
sustainable
route
produce
fuels
chemicals.
In
Perspective,
we
take
critical
look
at
progress
incorporating
catalysts
into
device
architectures
operate
using
vapor-phase
reactants,
thereby
overcoming
intrinsic
limitations
aqueous-based
systems.
Performance
comparison
is
between
state-of-the-art
electrolyzers
commercial
H2O
electrolyzers—a
well-established
technology
provides
realistic
performance
targets.
Beyond
just
higher
rates,
vapor-fed
reactors
represent
paradigms
for
unprecedented
control
local
reaction
conditions,
provide
perspective
challenges
opportunities
generating
achieving
technological
electrolyzers.
ACS Energy Letters,
Journal Year:
2020,
Volume and Issue:
5(2), P. 486 - 519
Published: Jan. 8, 2020
The
conversion
of
carbon
dioxide
(CO2)
into
fuels
and
value-added
products
is
one
the
most
significant
inventions
to
address
global
warming
energy
needs.
Photoelectrochemical
(PEC)
CO2
can
be
considered
as
an
artificial
photosynthesis
technique
that
produces
formate,
formaldehyde,
formic
acid,
methane,
methanol,
ethanol,
etc.
Recent
advances
in
electrode
materials,
mechanisms,
kinetics,
thermodynamics,
reactor
designs
PEC
have
been
comprehensively
reviewed
this
article.
adsorption
activation
CO2/intermediates
at
surface
are
key
steps
for
improving
kinetics
conversion.
efficiency
could
upgraded
through
utilization
2D/3D
plasmonic
metals,
carbon-based
catalysts,
porous
nanostructures,
metal–organic
frameworks,
molecular
biological
molecules.
defect
engineered
(by
cation/anion
vacancy,
crystal
distortion,
pits,
creation
oxygen
vacancies)
Z-scheme
heterojunctions,
bioelectrodes,
tandem
photovoltaic–PEC
reactors
suitable
options
enhance
low
external
bias.
Journal of the American Chemical Society,
Journal Year:
2019,
Volume and Issue:
141(6), P. 2490 - 2499
Published: Jan. 18, 2019
Understanding
the
structural
and
compositional
sensitivities
of
electrochemical
CO2
reduction
reaction
(CO2RR)
is
fundamentally
important
for
developing
highly
efficient
selective
electrocatalysts.
Here,
we
use
Ag/Cu
nanocrystals
to
uncover
key
role
played
by
interface
in
promoting
CO2RR.
Nanodimers
including
two
constituent
metals
as
segregated
domains
sharing
a
tunable
are
obtained
seeded
growth
synthesis,
wherein
preformed
Ag
nanoparticles
used
nucleation
seeds
Cu
domain.
We
find
that
type
metal
precursor
strength
reducing
agent
play
achieving
desired
chemical
control.
show
tandem
catalysis
electronic
effects,
both
enabled
addition
form
nanodomain
within
same
catalyst,
synergistically
account
an
enhancement
Faradaic
efficiency
C2H4
3.4-fold
partial
current
density
2-fold
compared
with
pure
counterpart.
The
insights
gained
from
this
work
may
be
beneficial
designing
multicomponent
catalysts
reduction.
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 Materials,
Journal Year:
2018,
Volume and Issue:
30(49)
Published: Oct. 10, 2018
Abstract
Electrochemical
reduction
of
carbon
dioxide
(CO
2
)
is
an
appealing
approach
toward
tackling
climate
change
associated
with
atmospheric
CO
emissions.
This
uses
as
the
feedstock
to
produce
value‐added
chemicals,
resulting
in
a
carbon‐neutral
(or
even
carbon‐negative)
process
for
chemical
production.
Many
efforts
have
been
devoted
development
electrolysis
devices
that
can
be
operated
at
industrially
relevant
rates;
however,
limited
progress
has
made,
especially
valuable
C
2+
products.
Herein,
nanoporous
copper
catalyst
synthesized
and
integrated
into
microfluidic
flow
cell
electrolyzer.
The
electrolyzer
exhibits
current
density
653
mA
cm
−2
product
selectivity
≈62%
applied
potential
−0.67
V
(vs
reversible
hydrogen
electrode).
highly
porous
electrode
structure
facilitates
rapid
gas
transport
across
electrode–electrolyte
interface
high
densities.
Further
investigations
on
electrolyte
effects
reveal
surface
pH
value
substantially
different
from
bulk
electrolyte,
nonbuffering
near‐neutral
electrolytes
when
operating
currents.
ACS Catalysis,
Journal Year:
2019,
Volume and Issue:
10(3), P. 1754 - 1768
Published: Dec. 30, 2019
In
the
recent
years,
significant
progress
has
been
made
toward
designing
active
and
selective
catalysts
for
electrochemical
CO2
reduction,
with
particular
interest
focused
on
two
major
C2
products—ethylene
ethanol.
Numerous
efforts
have
to
enhance
understanding
of
heterogeneous
copper-based
reduction
mechanisms
by
computational
studies.
Here
we
provide
a
critical
assessment
various
proposed
scenarios
initial
post
C–C
coupling
steps
that
result
in
either
ethylene
or
silico
rationalization
parameters
controlling
product
selectivity,
such
as
catalyst
structure
composition
(Cu
facets,
presence
defective
sites
and/or
subsurface
oxygen
atoms,
interplay
second
metal)
reaction
conditions
(pH,
applied
potential,
electrolyte),
is
provided.
A
comprehensive
scheme
combining
pathways
derived,
issues
are
still
under
debate
require
further
investigations
highlighted.