ChemPhysChem,
Journal Year:
2024,
Volume and Issue:
25(7)
Published: Feb. 7, 2024
Abstract
Using
functionalized
supporting
materials
for
the
immobilization
of
molecular
catalysts
is
an
appealing
strategy
to
improve
efficiency
electrocatalysis.
Herein,
we
report
covalent
tethering
cobalt
porphyrins
on
phenolic
resins
(
PR
)
improved
electrocatalytic
oxygen
reduction
reaction
(ORR)
and
evolution
(OER).
A
porphyrin
bearing
alkyl
bromide
substituent
was
covalently
tethered
resins,
through
substitution
bromides
with
hydroxyl
groups,
afford
molecule‐engineered
Co‐PR
).
The
resulted
efficient
ORR
OER
by
displaying
half‐wave
potential
E
1/2
=0.78
V
versus
RHE
overpotential
420
mV
get
10
mA/cm
2
current
density.
We
propose
that
many
residual
groups
will
surround
Co
play
critical
roles
in
facilitating
proton
electron
transfers.
Importantly,
outperformed
unmodified
loaded
simple
physical
adsorption
(termed
Co@PR
zinc‐air
battery
assembled
using
displayed
a
performance
comparable
Pt/C+Ir/C.
This
work
significant
present
as
material
support
electrocatalysts
demonstrate
electrocatalysis
use
resin
residues.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(31)
Published: Feb. 23, 2023
Single/dual-metal
atoms
supported
on
carbon
matrix
can
be
modulated
by
coordination
structure
and
neighboring
active
sites.
Precisely
designing
the
geometric
electronic
uncovering
structure-property
relationships
of
single/dual-metal
confront
with
grand
challenges.
Herein,
this
review
summarizes
latest
progress
in
microenvironment
engineering
single/dual-atom
sites
via
a
comprehensive
comparison
single-atom
catalyst
(SACs)
dual-atom
catalysts
(DACs)
term
design
principles,
modulation
strategy,
theoretical
understanding
structure-performance
correlations.
Subsequently,
recent
advances
several
typical
electrocatalysis
process
are
discussed
to
get
general
reaction
mechanisms
finely-tuned
SACs
DACs.
Finally,
full-scaled
summaries
challenges
prospects
given
for
This
will
provide
new
inspiration
development
atomically
dispersed
electrocatalytic
application.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(9), P. 5330 - 5341
Published: Feb. 23, 2023
Personalized
tumor
vaccines
have
become
a
promising
modality
for
cancer
immunotherapy.
However,
in
situ
personalized
generated
from
immunogenic
cell
death
(ICD)
and
adjuvants
are
mired
by
toxic
side
effects
unsatisfactory
efficiency.
Herein,
functionalizing
the
reticular
structure
to
optimize
catalytic
activity
of
materials,
series
biocompatible
covalent
organic
framework
(COF)-based
catalysts
been
designed
screened
establishing
bioorthogonal-activated
vaccine
an
efficient
safe
way.
Especially,
pro-doxorubicin
(pro-DOX)
could
be
bioorthogonally
activated
COF-based
Fe(II)
catalysts,
which
elicited
ICD
released
tumor-associated
antigens
(TAAs).
This
prodrug
activation
strategy
minimize
drug
maximize
treatment
effects.
More
importantly,
system
also
catalytically
activate
pro-imiquimod
(pro-IMQ,
TLR7/8
immune
agonist),
served
as
adjuvant
amplify
antitumor
immunity.
Notably,
this
not
only
facilitated
strong
response
but
prevented
dose-dependent
chemotherapeutic
drugs,
including
systemic
inflammation
caused
random
distribution
adjuvants.
To
best
our
knowledge,
it
is
first
time
devise
platform
generating
vaccine,
would
provide
paradigm
achieving
secure
robust
Advanced Functional Materials,
Journal Year:
2022,
Volume and Issue:
32(40)
Published: July 22, 2022
Abstract
The
oxygen
evolution
reaction
(OER)
remains
a
bottleneck
for
the
overall
water
splitting.
Electrocatalysts
with
superior
activity
and
stability
are
still
highly
desired.
Herein,
stepwise
electrochemical
strategy
is
developed
to
prepare
Co(OH)
2
/NiP
x
nanosheet
arrays
intimate
abundant
heterostructures.
nanosheets,
which
first
electrodeposited
on
blank
carbon
cloth
electrode,
serve
as
substrate
nucleation
growth
of
NiP
.
resultant
heterointerfaces
well
regulated
by
altering
loading
heterostructured
optimal
demonstrate
significantly
enhanced
conductivity
hydrophilicity,
greatly
facilitate
electron
mass
transfer.
In
addition,
strong
electronic
interaction
between
observed,
favoring
generation
high‐valence
cobalt
center,
thus
electrocatalytic
performances
toward
OER
remarkably
improved.
nanosheets
achieve
current
density
10
mA
cm
−2
at
an
overpotential
236
mV,
while
corresponding
values
benchmark
Ir/C
292
262
respectively.
This
study
provides
facile
effective
fabricate
transition
metal
hydroxide/phosphide
composite
nanomaterials
heterostructures,
conductivity,
improved
wettability,
opens
new
direction
design
active
electrocatalysts.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
62(1)
Published: Nov. 8, 2022
Synthesizing
large-area
free-standing
covalent
organic
framework
(COF)
films
is
of
vital
importance
for
their
applications
but
still
a
big
challenge.
Herein,
we
reported
the
synthesis
large
metalloporphyrin-based
COF
and
oxygen
electrocatalysis.
The
reaction
meso-benzohydrazide-substituted
metal
porphyrins
with
tris-aldehyde
linkers
afforded
at
liquid-air
interface.
These
can
be
scaled
up
to
3000
cm2
area
display
great
mechanical
stability
structural
integrity.
Importantly,
Co-porphyrin-based
are
efficient
electrocatalytic
O2
reduction
evolution
reactions.
A
flexible,
all-solid-state
Zn-air
battery
was
assembled
using
showed
high
performance
charge-discharge
voltage
gap
0.88
V
1
mA
cm-2
under
bent
conditions
(0°
180°).
This
work
thus
presents
strategy
synthesize
functionalized
quality
uses
in
flexible
electronics.
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
53(3), P. 1447 - 1494
Published: Jan. 1, 2024
A
comprehensive
overview
on
organic
polymers
as
electrocatalysts
is
summarized.
By
presenting
the
engineering
strategies,
insightful
understandings,
challenges,
and
perspectives,
we
hope
this
review
can
provide
valuable
references
for
readers.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(38)
Published: Aug. 8, 2023
Abstract
The
nucleophilic
attack
of
water
or
hydroxide
on
metal‐oxo
units
forms
an
O−O
bond
in
the
oxygen
evolution
reaction
(OER).
Coordination
tuning
to
improve
this
is
intriguing
but
has
been
rarely
realized.
We
herein
report
improved
OER
catalysis
by
metal
porphyrin
1‐M
(M=Co,
Fe)
with
a
coordinatively
unsaturated
ion.
designed
and
synthesized
sterically
blocking
one
side
tethered
tetraazacyclododecane
unit.
With
protection,
species
generated
can
maintain
unoccupied
trans
axial
site.
Importantly,
displays
higher
activity
alkaline
solutions
than
analogues
lacking
such
protection
decreasing
up
150‐mV
overpotential
achieve
10
mA/cm
2
current
density.
Theoretical
studies
suggest
that
site,
unit
becomes
more
positively
charged
thus
favoured
for
as
compared
bearing
ligands.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(51)
Published: Nov. 3, 2023
Abstract
In
nature,
cytochrome
c
oxidases
catalyze
the
4e
−
oxygen
reduction
reaction
(ORR)
at
heme/Cu
site,
in
which
Cu
I
is
used
to
assist
O
2
activation.
Because
of
thermodynamic
barrier
generate
,
synthetic
Fe‐porphyrin/Cu
complexes
usually
show
moderate
electrocatalytic
ORR
activity.
We
herein
report
on
a
Co‐corrole/Co
complex
1‐Co
for
energy‐efficient
ORR.
By
hanging
Co
II
ion
over
corrole,
realizes
with
half‐wave
potential
0.89
V
versus
RHE,
outstanding
among
corrole‐based
electrocatalysts.
Notably,
outperforms
corrole
hanged
or
Zn
.
revealed
that
can
provide
an
electron
improve
binding
thermodynamically
and
dynamically,
function
represented
by
biological
site.
This
work
significant
present
remarkable
electrocatalyst
vital
role
second‐sphere
redox‐active
metal
promoting
