Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(44), P. 24230 - 24239
Published: Oct. 27, 2023
Developing
an
electrocatalyst
platform
that
can
control
the
interplay
among
activity,
selectivity,
and
stability
at
atomic
precision
remains
a
grand
challenge.
Here,
we
have
synthesized
highly
crystalline
polymetallophthalocyanines
(pMPcs,
M
=
Fe,
Co,
Ni,
Cu)
through
annulation
of
tetracyanobenzene
in
presence
transition
metals.
The
conjugated,
conductive,
stable
backbones
with
precisely
installed
metal
sites
render
pMPcs
unique
electrochemical
catalysis,
where
tunability
emerges
from
long-range
interactions.
construction
pCoNiPc
Co
Ni
dual-site
integrates
advantageous
features
pCoPc
pNiPc
electrocatalytic
CO2
reduction
electronic
communication
unprecedented
long
separation
≥14
chemical
bonds.
This
integration
provides
excellent
activity
(current
density,
j
-16.0
-100
mA
cm-2
H-type
flow
cell,
respectively),
selectivity
(CO
Faraday
efficiency,
FECO
94%),
(>10
h),
making
it
one
best-performing
reticular
materials.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
34(4)
Published: Nov. 2, 2021
Exploiting
effective
electrocatalysts
based
on
elaborate
heterostructures
for
the
oxygen
evolution
reaction
(OER)
has
been
considered
as
a
promising
strategy
boosting
water
splitting
efficiency
to
produce
clean
energy-hydrogen.
However,
constructing
catalytically
active
with
novel
composition
and
architecture
remains
poorly
developed
due
synthetic
challenge.
In
this
work,
it
is
demonstrated
that
unique
Ni(CN)2
/NiSe2
heterostructures,
composed
of
single-crystalline
nanoplates
surrounded
by
crystallographically
aligned
NiSe2
nanosatellites,
can
be
created
from
nickel-based
Hofmann-type
coordination
polymers
through
stepwise
topochemical
pathways.
When
employed
OER
electrocatalyst,
show
enhanced
performance,
which
could
attributed
optimized
geometric
electronic
structures
catalytic
sites
endowed
synergy
between
two
components.
This
work
demonstrates
rational
route
creating
Ni-based
electrocatalyst
possesses
nanoscale
heterostructure,
whose
composition,
spatial
organization,
interface
configuration
finely
manipulated.
Chemical Reviews,
Journal Year:
2023,
Volume and Issue:
123(8), P. 4972 - 5019
Published: March 27, 2023
Scanning
electrochemical
probe
microscopy
(SEPM)
techniques
can
disclose
the
local
reactivity
of
interfaces
in
single-entity
and
sub-entity
studies.
Operando
SEPM
measurements
consist
using
a
tip
to
investigate
performance
electrocatalysts,
while
interface
is
simultaneously
modulated.
This
powerful
combination
correlate
activity
with
changes
surface
properties,
e.g.,
topography
structure,
as
well
provide
insight
into
reaction
mechanisms.
The
focus
this
review
reveal
recent
progress
catalytic
toward
reduction
evolution
O2
H2
conversion
CO2.
capabilities
SEPMs
are
showcased,
possibility
coupling
other
presented.
Emphasis
given
scanning
(SECM),
ion
conductance
(SICM),
tunneling
(EC-STM),
cell
(SECCM).
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(51)
Published: April 24, 2023
Metal
alloys-structured
electrocatalysts
(MAECs)
have
made
essential
contributions
to
accelerating
the
practical
applications
of
electrocatalytic
devices
in
renewable
energy
systems.
However,
due
complex
atomic
structures,
varied
electronic
states,
and
abundant
supports,
precisely
decoding
metal-metal
interactions
structure-activity
relationships
MAECs
still
confronts
great
challenges,
which
is
critical
direct
future
engineering
optimization
MAECs.
Here,
this
timely
review
comprehensively
summarizes
latest
advances
creating
MAECs,
including
interactions,
coordination
microenvironments,
relationships.
First,
fundamental
classification,
design,
characterization,
structural
reconstruction
are
outlined.
Then,
merits
modulation
strategies
recent
breakthroughs
for
noble
non-noble
metal-structured
thoroughly
discussed,
such
as
solid
solution
alloys,
intermetallic
single-atom
alloys.
Particularly,
unique
insights
into
bond
theoretical
understanding,
operando
techniques
mechanism
disclosure
given.
Thereafter,
current
states
diverse
with
a
focus
on
property-reactivity
relationships,
reaction
pathways,
performance
comparisons
discussed.
Finally,
challenges
perspectives
systematically
It
believed
that
comprehensive
can
offer
substantial
impact
stimulating
widespread
utilization
metal
materials
electrocatalysis.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(49)
Published: Oct. 21, 2023
The
electrolyte
cations-dependent
kinetics
have
been
widely
observed
in
many
fields
of
electrocatalysis,
however,
the
exact
mechanism
influence
on
catalytic
performance
is
still
a
controversial
topic
considerable
discussion.
Herein,
combined
with
operando
X-ray
diffraction
(XRD)
and
high-resolution
transmission
electron
microscopy
(HRTEM),
we
verify
that
cations
could
intercalate
into
layer
pristine
CoOOH
catalyst
during
oxygen
evolution
reaction
(OER)
process,
while
bigger
lead
to
enlarged
interlayer
spacing
increased
OER
activity,
following
order
Cs+
>K+
>Na+
>Li+
.
absorption
spectroscopy
(XAS),
situ
Raman,
Ultraviolet-visible
(UV/Vis)
spectroscopy,
XAS
cyclic
voltammetry
(CV),
theoretical
calculations
reveal
intercalation
efficiently
modify
oxidation
states
Co
by
enlarging
Co-O
bonds,
which
turn
enhance
d-band
center
Co,
optimize
adsorption
strength
intermediates,
facilitate
formation
active
Co(IV)
species,
reduce
energy
barrier
rate-determing
step
(RDS),
thereby
enhancing
activity.
This
work
not
only
provides
an
informative
picture
understand
complicated
dependence
cations,
but
also
sheds
light
understanding
other
cation-targeted
electrocatalysis.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(44), P. 24230 - 24239
Published: Oct. 27, 2023
Developing
an
electrocatalyst
platform
that
can
control
the
interplay
among
activity,
selectivity,
and
stability
at
atomic
precision
remains
a
grand
challenge.
Here,
we
have
synthesized
highly
crystalline
polymetallophthalocyanines
(pMPcs,
M
=
Fe,
Co,
Ni,
Cu)
through
annulation
of
tetracyanobenzene
in
presence
transition
metals.
The
conjugated,
conductive,
stable
backbones
with
precisely
installed
metal
sites
render
pMPcs
unique
electrochemical
catalysis,
where
tunability
emerges
from
long-range
interactions.
construction
pCoNiPc
Co
Ni
dual-site
integrates
advantageous
features
pCoPc
pNiPc
electrocatalytic
CO2
reduction
electronic
communication
unprecedented
long
separation
≥14
chemical
bonds.
This
integration
provides
excellent
activity
(current
density,
j
-16.0
-100
mA
cm-2
H-type
flow
cell,
respectively),
selectivity
(CO
Faraday
efficiency,
FECO
94%),
(>10
h),
making
it
one
best-performing
reticular
materials.
