Accounts of Chemical Research,
Journal Year:
2022,
Volume and Issue:
55(5), P. 638 - 648
Published: Jan. 18, 2022
ConspectusCarbon
capture,
utilization,
and
sequestration
play
an
essential
role
to
address
CO2
emissions.
Among
all
carbon
utilization
technologies,
electroreduction
has
gained
immense
interest
due
its
potential
for
directly
converting
a
variety
of
valuable
commodity
chemicals
using
clean,
renewable
electricity
as
the
sole
energy
source.
The
research
community
witnessed
rapid
advances
in
electrolysis
technology
recent
years,
including
highly
selective
catalysts,
larger-scale
reactors,
specific
process
modeling,
well
mechanistic
understanding
reduction
reaction.
field
brings
promise
commercial
application
rollout
chemical
manufacturing.This
Account
focuses
on
our
contributions
both
fundamental
applied
electrocatalytic
CO
reactions.
We
first
discuss
(1)
development
novel
electrocatalysts
CO2/CO
enhance
product
selectivity
lower
consumption.
Specifically,
we
synthesized
nanoporous
Ag
homogeneously
mixed
Cu-based
bimetallic
catalysts
enhanced
production
from
multicarbon
products
CO,
respectively.
Then,
review
efforts
(2)
reactor
engineering,
dissolved
H-type
cell,
vapor-fed
three-compartment
flow
membrane
electrode
assembly,
enhancing
reaction
rates
scalability.
Next,
describe
(3)
investigation
mechanisms
situ
operando
techniques,
such
surface-enhanced
vibrational
spectroscopies
electrochemical
mass
spectroscopy.
revealed
participation
bicarbonate
Au
attenuated
total-reflectance
infrared
absorption
spectroscopy,
presence
"oxygenated"
surface
Cu
under
conditions
Raman
origin
oxygen
acetaldehyde
other
electrolyzer
spectrometry.
Lastly,
examine
(4)
technology,
pollutant
effects
developing
techno-economic
analysis.
SO2
NOx
Cu,
Ag,
Sn
catalysts.
also
identify
technical
barriers
that
need
be
overcome
offer
perspective
accelerating
deployment
technology.
Nature Communications,
Journal Year:
2022,
Volume and Issue:
13(1)
Published: March 2, 2022
Electrocatalytic
recycling
of
waste
nitrate
(NO3-)
to
valuable
ammonia
(NH3)
at
ambient
conditions
is
a
green
and
appealing
alternative
the
Haber-Bosch
process.
However,
reaction
requires
multi-step
electron
proton
transfer,
making
it
grand
challenge
drive
high-rate
NH3
synthesis
in
an
energy-efficient
way.
Herein,
we
present
design
concept
tandem
catalysts,
which
involves
coupling
intermediate
phases
different
transition
metals,
existing
low
applied
overpotentials,
as
cooperative
active
sites
that
enable
cascade
NO3--to-NH3
conversion,
turn
avoiding
generally
encountered
scaling
relations.
We
implement
by
electrochemical
transformation
Cu-Co
binary
sulfides
into
potential-dependent
core-shell
Cu/CuOx
Co/CoO
phases.
Electrochemical
evaluation,
kinetic
studies,
in-situ
Raman
spectra
reveal
inner
preferentially
catalyze
NO3-
reduction
NO2-,
rapidly
reduced
nearby
shell.
This
unique
catalyst
system
leads
Faradaic
efficiency
93.3
±
2.1%
wide
range
concentrations
pH
13,
high
yield
rate
1.17
mmol
cm-2
h-1
0.1
M
-0.175
V
vs.
RHE,
half-cell
energy
~36%,
surpassing
most
previous
reports.
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(4), P. 2540 - 2581
Published: Jan. 1, 2021
The
recent
progress
made
on
porphyrin-based
frameworks
and
their
applications
in
energy-related
conversion
technologies
(e.g.,
ORR,
OER
CO2RR)
storage
Zn–air
batteries).
Chemical Society Reviews,
Journal Year:
2020,
Volume and Issue:
49(18), P. 6632 - 6665
Published: Jan. 1, 2020
The
electrochemical
reduction
of
CO2
stores
intermittent
renewable
energy
in
valuable
raw
materials,
such
as
chemicals
and
transportation
fuels,
while
minimizing
carbon
emissions
promoting
carbon-neutral
cycles.
Recent
technoeconomic
reports
suggested
economically
feasible
target
products
electroreduction
the
relative
influence
key
performance
parameters
faradaic
efficiency
(FE),
current
density,
overpotential
practical
industrial-scale
applications.
Furthermore,
fundamental
factors,
available
reaction
pathways,
shared
intermediates,
competing
hydrogen
evolution
reaction,
scaling
relations
intermediate
binding
energies,
mass
transport
limitations,
should
be
considered
relation
to
performance.
Intensive
research
efforts
have
been
devoted
designing
developing
advanced
electrocatalysts
improving
mechanistic
understanding.
More
recently,
focus
was
extended
catalyst
environment,
because
interfacial
region
can
delicately
modulate
catalytic
activity
provide
effective
solutions
challenges
that
were
not
fully
addressed
material
development
studies.
Herein,
we
discuss
importance
catalyst-electrolyte
interfaces
operational
based
on
kinetic
equations.
extensively
review
previous
studies
controlling
organic
modulators,
electrolyte
ions,
electrode
structures,
well
three-phase
boundary
at
interface.
modulates
electrocatalytic
properties
via
electronic
modification,
stabilization,
proton
delivery
regulation,
structure
reactant
concentration
control,
regulation.
We
understanding
interface
its
effect
activity.