Cell Reports Physical Science,
Journal Year:
2022,
Volume and Issue:
3(4), P. 100825 - 100825
Published: March 25, 2022
The
electrochemical
reduction
of
CO2
from
flue
gas
or
direct
air
capture
to
relevant
syngas
mixtures
is
a
promising
route
toward
mitigation
environmental
pollution
and
production
bulk
chemicals
fuels.
Among
the
different
cell
types,
gas-fed
zero-gap
electrolyzers
are
as
energy-efficient
scalable
devices.
We
herein
investigate
influence
operational
parameters
related
cathode
water
management,
such
orientation,
humidification,
compression
onto
CO2R.
By
stepwise
optimization
our
not
yet
fully
optimized
electrolyzer,
stability
could
be
improved
by
factor
3
up
10
h
at
V
300
mA
cm−2.
Faradic
efficiency
for
CO
after
2
electrolysis
was
increased
14%
over
60%.
Controlling
management
key
parameter
high
input
leads
flooding
electrodes,
whereas
lower
values
decrease
performance
anion
exchange
membrane
reduce
catalyst
wetting.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(13), P. 6028 - 6039
Published: March 18, 2022
Water-alkaline
electrolysis
holds
a
great
promise
for
industry-scale
hydrogen
production
but
is
hindered
by
the
lack
of
enabling
evolution
reaction
electrocatalysts
to
operate
at
ampere-level
current
densities
under
low
overpotentials.
Here,
we
report
use
spillover-bridged
water
dissociation/hydrogen
formation
processes
occurring
synergistically
hybridized
Ni3S2/Cr2S3
sites
incapacitate
inhibition
effect
high-current-density-induced
high
coverage
dissociation
site
and
concurrently
promote
Volmer/Tafel
processes.
The
mechanistic
insights
critically
important
enable
density
operation
are
depicted
from
experimental
theoretical
studies.
Volmer
process
drastically
boosted
strong
H2O
adsorption
Cr5c
Cr2S3,
efficient
H2O*
via
heterolytic
cleavage
(Cr5c-H2O*
+
S3c(#)
→
Cr5c-OH*
S3c-H#)
on
Cr5c/S3c
in
rapid
desorption
OH*
Cr2S3via
new
water-assisted
mechanism
(Cr5c-OH*
H2O(aq)
Cr5c-H2O*
OH-(aq)),
while
Tafel
achieved
through
spillover
rapidly
transfer
H#
located
H-rich
(Cr2S3)
H-deficient
(Ni3S2)
with
excellent
activity.
As
result,
electrocatalyst
can
readily
achieve
3.5
A
cm-2
an
overpotential
251
±
3
mV
1.0
M
KOH
electrolyte.
concept
exemplified
this
work
provides
useful
means
address
shortfalls
current-density-tolerant
Hydrogen
(HER)
electrocatalysts.
ACS Energy Letters,
Journal Year:
2023,
Volume and Issue:
8(3), P. 1502 - 1509
Published: Feb. 26, 2023
Hydrogen
is
poised
to
play
a
key
role
in
the
energy
transition
by
decarbonizing
hard-to-electrify
sectors
and
enabling
storage,
transport,
trade
of
renewable
energy.
Recent
forecasts
project
thousand-fold
expansion
global
water
electrolysis
capacity
as
early
2030.
In
this
context,
several
technologies
are
likely
coexist
market,
each
catering
different
applications
geographies.
They
face
common
challenge
decreasing
cost
hydrogen
produced,
for
which
efficiency
major
but
not
only
factor.
Perspective,
we
dispel
misconceptions─rooted
outdated
designs─around
alkaline
offer
an
overview
main
technical
pathways
reduce
from
modern
systems
already
under
commercialization.
By
identifying
research
needs,
aim
motivate
work
into
overlooked
areas
that
both
interesting
scientific
questions
can
contribute
gigawatt-scale
production
green
short-
medium-term.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(24)
Published: March 31, 2022
Integrating
molecular
catalysts
into
designed
frameworks
often
enables
improved
catalysis.
Compared
with
porphyrin-based
frameworks,
metal-corrole-based
have
been
rarely
developed,
although
monomeric
metal
corroles
are
usually
more
efficient
than
porphyrin
counterparts
for
the
electrocatalytic
oxygen
reduction
reaction
(ORR)
and
evolution
(OER).
We
herein
report
on
porous
organic
polymers
(POPs)
as
ORR
OER
electrocatalysts.
M-POPs
(M=Mn,
Fe,
Co,
Cu)
were
synthesized
by
coupling
10-phenyl-5,15-(4-iodophenyl)corrole
tetrakis(4-ethynylphenyl)methane.
corrole
monomers,
displayed
significantly
enhanced
catalytic
activity
stability.
Co-POP
outperformed
other
achieving
four-electron
a
half-wave
potential
of
0.87
V
vs.
RHE
reaching
10
mA
cm-2
current
density
at
340
mV
overpotential.
This
work
is
unparalleled
to
develop
explore
POPs
ACS Catalysis,
Journal Year:
2022,
Volume and Issue:
12(9), P. 5605 - 5660
Published: April 26, 2022
As
a
group
of
large-surface-area
nonmetal
materials,
polymeric
carbon
nitride
(CxNy)
and
its
hybrid
structures
are
nowadays
ever-increasing
interest
for
use
in
energy
devices
involved
conversion
storage,
offering
low
expenses
facile
production
processes.
With
the
growing
requirement
clean
renewable
generation
storage
systems,
progress
replacement
expensive
noble-metal
catalysts
with
CxNy-based
materials
as
efficient
electrocatalysts
has
expanded
considerably,
demand
these
increased.
The
modified
CxNy
architectures
beneficial
to
electrocatalytic
applications,
improving
their
moderate
electrical
conductivities
capacity
loss.
present
review
strives
highlight
recent
advances
research
on
aforementioned
identities
CxNy-derived
structurally
polymorphs.
This
also
discusses
fuel
cells,
metal–air
batteries,
water
splitting
supercapacitor
applications.
Herein,
we
deal
oxidation
reduction
reactions
such
hydrogen
evolution,
oxygen
reduction,
CO2
nitrogen
etc.
Each
device
been
studied
clearer
understanding
patent
relevant
experiments
reviewed
separately.
Additionally,
role
some
general
redox
capable
being
exploited
any
is
included.
iScience,
Journal Year:
2022,
Volume and Issue:
25(4), P. 104011 - 104011
Published: March 4, 2022
For
the
efficient
electrochemical
conversion
of
CO2
into
valuable
chemical
feedstocks,
a
well-coordinated
interaction
all
electrolyzer
compartments
is
required.
In
addition
to
catalyst,
whose
role
described
in
detail
part
"Electrochemical
Reduction
toward
Multicarbon
Alcohols
-
The
Microscopic
World
Catalysts
&
Process
Conditions"
this
divided
review,
general
cell
setups,
design
and
manufacture
electrodes,
membranes
used,
process
parameters
must
be
optimally
matched.
authors'
goal
provide
comprehensive
review
current
literature
on
how
these
aspects
affect
overall
performance
electrolysis.
To
economically
competitive
as
an
process,
framework
conditions,
i.e.,
supply
reaction
product
treatment
also
considered.
If
key
indicators
for
density,
selectivity,
voltage,
lifetime
mentioned
techno-economic
consideration
are
met,
reduction
can
make
contribution
creation
closed
carbon
cycles
sustainable
energy
economy.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
61(9)
Published: Dec. 16, 2021
Abstract
Proton
transfer
is
vital
for
many
biological
and
chemical
reactions.
Hydrogen‐bonded
water‐containing
networks
are
often
found
in
enzymes
to
assist
proton
transfer,
but
similar
strategy
has
been
rarely
presented
by
synthetic
catalysts.
We
herein
report
the
Co
corrole
1
with
an
appended
crown
ether
unit
its
boosted
activity
hydrogen
evolution
reaction
(HER).
Crystallographic
H
NMR
studies
proved
that
of
can
grab
water
via
bonds.
By
using
protic
acids
as
sources,
HER
was
largely
added
water,
while
crown‐ether‐free
analogues
showed
very
small
enhancement.
Inhibition
adding
1)
external
18‐crown‐6‐ether
extract
molecules
2)
potassium
ion
or
N
‐benzyl‐n‐butylamine
block
further
confirmed
critical
role
assisting
grabbed
molecules.
This
work
presents
a
example
boost
through
networks.