Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
136(32)
Published: May 27, 2024
Abstract
The
practical
application
of
the
electrocatalytic
CO
2
reduction
reaction
(CO
RR)
to
form
formic
acid
fuel
is
hindered
by
limited
activation
molecules
and
lack
universal
feasibility
across
different
pH
levels.
Herein,
we
report
a
doping‐engineered
bismuth
sulfide
pre‐catalyst
(BiS‐1)
that
S
partially
retained
after
electrochemical
reconstruction
into
metallic
Bi
for
RR
formate/formic
with
ultrahigh
performance
wide
range.
best
BiS‐1
maintains
Faraday
efficiency
(FE)
~95
%
at
2000
mA
cm
−2
in
flow
cell
under
neutral
alkaline
solutions.
Furthermore,
catalyst
shows
unprecedentedly
high
FE
(~95
%)
current
densities
from
100
1300
acidic
Notably,
density
can
reach
700
while
maintaining
above
90
membrane
electrode
assembly
electrolyzer
operate
stably
150
h
200
.
In
situ
spectra
functional
theory
calculations
reveals
doping
modulates
electronic
structure
effectively
promotes
formation
HCOO*
intermediate
generation.
This
work
develops
efficient
stable
electrocatalysts
sustainable
production.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
16(11), P. 4714 - 4758
Published: Jan. 1, 2023
This
review
analyzes
advanced
catalysts
and
C
2+
synthesis
mechanisms
based
on
theoretical
explorations
in
situ
/
operando
characterizations.
Triphasic
interface
optimization
is
discussed
for
the
potential
of
industry-compatible
stability.
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
53(5), P. 2693 - 2737
Published: Jan. 1, 2024
Unprecedented
insights
into
electrochemical
surface
dynamics
from
operando
studies
inspire
electronic
and
topographical
strategies,
paving
the
way
for
sustained
electrocatalytic
performance
across
HER,
OER,
ORR,
CO
2
RR
applications.
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: Feb. 10, 2023
Abstract
Exploring
efficient
electrocatalysts
with
fundamental
understanding
of
the
reaction
mechanism
is
imperative
in
CO
2
electroreduction.
However,
impact
sluggish
water
dissociation
as
proton
source
and
surface
species
are
still
unclear.
Herein,
we
report
a
strategy
promoting
protonation
electroreduction
by
implementing
oxygen
vacancy
engineering
on
Bi
O
3
over
which
high
Faradaic
efficiency
formate
(above
90%)
large
partial
current
density
(162
mA
cm
−2
)
achieved.
Systematic
study
reveals
that
production
rate
mainly
hampered
dissociation,
while
introduction
accelerates
kinetics
strengthening
hydroxyl
adsorption
reduces
energetic
span
Moreover,
*
involved
formation
key
clearly
identified
electron
spin
resonance
measurements
designed
situ
Raman
spectroscopy
combined
isotopic
labelling.
Coupled
photovoltaic
device,
solar
to
energy
conversion
reaches
13.3%.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
16(9), P. 3885 - 3898
Published: Jan. 1, 2023
Using
surface-engineered
chemical
composites
to
enhance
the
binding
energy
of
reaction
intermediates
and
conductivity
is
an
attractive
route
achieve
a
high
partial
current
density
increased
yield
target
products.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
16(11), P. 5305 - 5314
Published: Jan. 1, 2023
A
cathodic
electrochemical
CO
2
reduction
to
formate
coupled
anodic
5-hydroxymethylfurfural
electrooxidation
2,5-furandicarboxylic
acid
pair
electrolysis
system
was
developed
for
conversion
and
biomass
valorization
with
low
energy
consumption.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(49)
Published: Oct. 19, 2023
Electrochemical
carbon
dioxide
reduction
reaction
(CO2
RR)
to
produce
valuable
chemicals
is
a
promising
pathway
alleviate
the
energy
crisis
and
global
warming
issues.
However,
simultaneously
achieving
high
Faradaic
efficiency
(FE)
current
densities
of
CO2
RR
in
wide
potential
range
remains
as
huge
challenge
for
practical
implements.
Herein,
we
demonstrate
that
incorporating
bismuth-based
(BH)
catalysts
with
L-histidine,
common
amino
acid
molecule
proteins,
an
effective
strategy
overcome
inherent
trade-off
between
activity
selectivity.
Benefiting
from
significantly
enhanced
adsorption
capability
promoted
electron-rich
nature
by
L-histidine
integrity,
BH
catalyst
exhibits
excellent
FEformate
unprecedented
windows
(>90
%
within
-0.1--1.8
V
>95
-0.2--1.6
versus
reversible
hydrogen
electrode,
RHE).
Excellent
performance
can
still
be
achieved
under
low-concentration
feeding
(e.g.,
20
vol.%).
Besides,
extremely
low
onset
-0.05
VRHE
(close
theoretical
thermodynamic
-0.02
)
was
detected
situ
ultraviolet-visible
(UV-Vis)
measurements,
together
stable
operation
over
50
h
preserved
≈95
partial
density
326.2
mA
cm-2
at
-1.0
.
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
53(12), P. 6295 - 6321
Published: Jan. 1, 2024
Developing
sophisticated
strategies
to
stabilize
oxidative
metal
catalysts
based
on
the
correlation
between
dynamic
oxidation
state
and
product
profile
is
favorable
for
efficient
electrochemical
CO
2
conversion.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(13)
Published: Feb. 2, 2024
Abstract
The
production
of
formic
acid
via
electrochemical
CO
2
reduction
may
serve
as
a
key
link
for
the
carbon
cycle
in
economy,
yet
its
practical
feasibility
is
largely
limited
by
quantity
and
concentration
product.
Here
we
demonstrate
continuous
at
M
an
industrial‐level
current
densities
(i.e.,
200
mA
cm
−2
)
300
h
on
membrane
electrode
assembly
using
scalable
lattice‐distorted
bismuth
catalysts.
optimized
catalysts
also
enable
Faradaic
efficiency
formate
94.2
%
highest
partial
density
1.16
A
,
reaching
rate
21.7
mmol
−1
.
To
assess
practicality
this
system,
perform
comprehensive
techno‐economic
analysis
life
assessment,
showing
that
our
approach
can
potentially
substitute
conventional
methyl
hydrolysis
industrial
production.
Furthermore,
resultant
serves
direct
fuel
air‐breathing
cells,
boasting
power
55
mW
exceptional
thermal
20.1
%.
