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:
2022,
Volume and Issue:
34(18)
Published: March 12, 2022
Rationally
designed
catalysts
hold
the
key
to
address
sluggish
kinetics
of
oxygen
evolution
reaction
(OER).
However,
engineering
active
sites
such
still
faces
grand
challenges.
This
study
proposes
a
feasible
ligand
modulation
strategy
boost
OER
catalytic
activity
cobalt-iron
oxyhydroxide
((Fe,Co)OOH).
The
2-methylimidazole
(MI)
coordination
on
(Fe,Co)OOH
reduces
orbital
overlap
between
Fe/Co
3d
and
O
2p,
which
weakens
adsorption
oxygen-containing
intermediates
thus
facilitates
unfavorable
O2
desorption.
As
result,
MI
modulated
achieves
an
excellent
performance
with
low
overpotentials
(230/290
mV
at
10/100
mA
cm-2
)
durability
(>155
h).
provides
novel
for
design
catalysts.
Journal of Physics Energy,
Journal Year:
2021,
Volume and Issue:
3(3), P. 034013 - 034013
Published: March 12, 2021
Abstract
Discovery
of
electrocatalytic
materials
for
high-performance
energy
conversion
and
storage
applications
relies
on
the
adequate
characterization
their
intrinsic
activity,
which
is
currently
hindered
by
dearth
a
protocol
consistent
precise
determination
double
layer
capacitance
(
C
DL
).
Herein,
we
propose
seven-step
method
that
aims
to
determine
reliably
scan
rate-dependent
cyclic
voltammetry
considering
aspects
strongly
influence
outcome
analysis,
including
(a)
selection
suitable
measuring
window,
(b)
uncompensated
resistance,
(c)
optimization
settings,
(d)
data
acquisition,
(e)
(f)
extraction
desired
information,
(g)
validation
results.
To
illustrate
proposed
method,
two
systems
were
studied:
resistor–capacitor
electric
circuit,
glassy
carbon
disk
in
an
electrochemical
cell.
With
these
studies,
it
demonstrated
when
any
mentioned
steps
procedure
are
neglected,
substantial
deviations
results
observed
with
misestimations
as
large
61%
case
investigated
system.
Moreover,
allometric
regression
more
model
than
linear
both
ideal
non-ideal
investigated.
We
stress
importance
assessing
accuracy
not
only
highly
specialized
methods,
but
also
those
well-known
commonly
used
voltammetric
methods.
The
herein
limited
,
can
be
effectively
applied
other
analysis
deliver
quantitative
via
crucial
study
kinetic
diffusion
phenomena
systems.
InfoMat,
Journal Year:
2022,
Volume and Issue:
5(1)
Published: Oct. 13, 2022
Abstract
The
hydrogen
energy
generated
by
the
electrocatalytic
water
splitting
reaction
has
been
established
as
a
renewable
and
clean
carrier
with
ultra‐high
density,
which
can
well
make
up
for
shortcomings
of
conventional
sources,
such
geographical
limitations,
climatic
dependence,
wastage.
Notably,
introduction
electrocatalysts
enhance
efficiency
process
to
generate
hydrogen.
Particularly,
heterostructure
constructed
coupling
multiple
components
(or
phases)
have
emerged
most
promising
option
due
well‐known
electronic
synergistic
effects.
existing
reviews
on
interface
engineering
electrocatalyst
design
mostly
focus
relationship
between
heterostructures
specific
reactions.
However,
comprehensive
overview
integration
model
building,
directional
synthesis,
mechanism
rarely
reported.
To
this
end,
in
review,
development
catalysts
is
systematically
introduced
from
perspective
classification,
growth
regulation
performance
based
interfacial
microenvironment
(bonding,
configuration,
lattice
strain,
etc.),
thereby
offering
useful
insights
construction
models.
Besides,
combined
current
applications
strategies,
challenges
future
are
discussed
relevant
solutions
proposed.
Overall,
review
serve
theoretical
reference
mechanism,
further
promote
production
technologies
low
consumption
high
yield.
image
ACS Nano,
Journal Year:
2022,
Volume and Issue:
16(2), P. 3251 - 3263
Published: Jan. 28, 2022
Strain
engineering
in
bimetallic
alloy
structures
is
of
great
interest
electrochemical
CO2
reduction
reactions
(CO2RR),
which
it
simultaneously
improves
electrocatalytic
activity
and
product
selectivity
by
optimizing
the
binding
properties
intermediates.
However,
a
reliable
synthetic
strategy
systematic
understanding
strain
effects
CO2RR
are
still
lacking.
Herein,
we
report
relaxation
used
to
determine
lattice
strains
bimetal
MNi
alloys
(M
=
Pd,
Ag,
Au)
realize
an
outstanding
CO2-to-CO
Faradaic
efficiency
96.6%
show
durability
toward
Zn-CO2
battery.
Molecular
dynamics
(MD)
simulations
predict
that
strained
PdNi
(s-PdNi)
correlated
with
increases
synthesis
temperature,
high
temperature
activation
energy
drives
complete
atomic
mixing
multiple
metal
atoms
allow
for
regulation
strains.
Density
functional
theory
(DFT)
calculations
reveal
effectively
formation
energies
*COOH
*CO
intermediates
on
s-PdNi
surfaces,
as
also
verified
situ
spectroscopic
investigations.
This
approach
provides
promising
catalyst
design,
enabling
independent
optimization
reaction
improve
catalytic
simultaneously.
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(20), P. 11293 - 11380
Published: Jan. 1, 2021
In
view
of
their
unique
characteristics
and
properties,
silver
nanomaterials
(Ag
NMs)
have
been
used
not
only
in
the
field
nanomedicine
but
also
for
diverse
advanced
catalytic
technologies.
this
comprehensive
review,
light
is
shed
on
general
synthetic
approaches
encompassing
chemical
reduction,
sonochemical,
microwave,
thermal
treatment
among
preparative
methods
syntheses
Ag-based
NMs
applications.
Additionally,
some
latest
innovative
such
as
continuous
flow
integrated
with
MW
other
benign
emphasized
that
ultimately
pave
way
sustainability.
Moreover,
potential
applications
emerging
Ag
NMs,
including
sub
single
atoms,
liquid-phase
catalysis,
photocatalysis,
electrocatalysis
well
a
positive
role
reactions
are
meticulously
summarized.
The
scientific
interest
synthesis
lies
benefits
activity,
selectivity,
stability,
recovery.
Therefore,
rise
journey
NM-based
catalysts
will
inspire
new
generation
chemists
to
tailor
design
robust
can
effectively
tackle
major
environmental
challenges
help
replace
noble
metals
This
overview
concludes
by
providing
future
perspectives
research
into
arena
photocatalysis.
Advanced Energy Materials,
Journal Year:
2022,
Volume and Issue:
12(26)
Published: June 1, 2022
Abstract
Achieving
efficient
efficiency
and
selectivity
for
the
electroreduction
of
CO
2
to
value‐added
feedstocks
has
been
challenging,
due
thermodynamic
stability
molecules
competing
hydrogen
evolution
reaction.
Herein,
a
dual‐single‐atom
catalyst
consisting
atomically
dispersed
CuN
4
NiN
bimetal
sites
is
synthesized
with
electrospun
carbon
nanofibers
(CuNi‐DSA/CNFs).
Theoretical
experimental
studies
reveal
strong
electron
interactions
induced
by
electronegativity
offset
between
Cu
Ni
atoms.
The
delicately
averaged
compensated
electronic
structures
result
in
an
effect
that
optimizes
adsorption
strength
*COOH
intermediate
boosts
reduction
reaction
(CO
RR)
kinetics,
notably
promoting
intrinsic
activity
catalyst.
CuNi‐DSA/CNFs
exhibits
outstanding
FE
99.6%
across
broad
potential
window
−0.78–
−1.18
V
(vs
reversible
electrode),
high
turnover
frequency
2870
h
–1
,
excellent
durability
(25
h).
Furthermore,
aqueous
Zn‐CO
battery
power
conversion
constructed.
This
atomic‐level
dual‐atom
provides
appealing
direction
develop
advanced
electrocatalysts
RR.
Nano Letters,
Journal Year:
2022,
Volume and Issue:
22(4), P. 1656 - 1664
Published: Feb. 4, 2022
Heterostructure
engineering
plays
a
vital
role
in
regulating
the
material
interface,
thus
boosting
electron
transportation
pathway
advanced
catalysis.
Herein,
novel
Bi2O3/BiO2
heterojunction
catalyst
was
synthesized
via
molten
alkali-assisted
dealumination
strategy
and
exhibited
rich
structural
dynamics
for
an
electrocatalytic
CO2
reduction
reaction
(ECO2RR).
By
coupling
situ
X-ray
diffraction
Raman
spectroscopy
measurements,
we
found
that
as-synthesized
heterostructure
can
be
transformed
into
Bi/BiO2
Mott–Schottky
heterostructure,
leading
to
enhanced
adsorption
performance
*OCHO
intermediates.
Consequently,
high
selectivity
toward
formate
larger
than
95%
rendered
wide
potential
window
along
with
optimum
partial
current
density
of
−111.42
mA
cm–2
benchmarked
state-of-the-art
Bi-based
ECO2RR
catalysts.
This
work
reports
construction
fruitful
dynamic
insights
electrocatalyst
ECO2RR,
which
paves
way
rational
design
efficient
electrocatalysts
beyond.
JACS Au,
Journal Year:
2021,
Volume and Issue:
1(5), P. 527 - 535
Published: April 12, 2021
The
growing
societal
and
political
focus
on
the
use
of
environmentally
friendly
technologies
has
led
to
an
ever-increasing
interest
in
electrolysis
scientific
communities.
This
development
is
reflected
by
plethora
candidate
catalysts
for
hydrogen
oxygen
evolution
reactions,
as
well
CO2
reduction
reaction,
reported
literature.
However,
almost
none
them
entered
stage
application
yet.
Likewise,
reports
process
engineering
inadequately
address
utilization
these
catalysts,
electrode
cell
concepts,
that
might
be
suitable
market.
Evidently,
a
closer
collaboration
between
chemists
engineers
from
industry
academia
desirable
speed
up
disruptive
technologies.
Herein,
we
elucidate
critical
parameters
highlight
necessary
aspects
accelerate
industrially
relevant
capable
fulfilling
forthcoming
challenges
related
energy
conversion
storage.
aim
this
Perspective,
composed
industrial
academic
partners,
critically
question
current
undertakings
encourage
researchers
strike
interdisciplinary
research
pathways.