Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(42)
Published: Sept. 1, 2023
Solvent
effect
plays
an
important
role
in
catalytic
reaction,
but
there
is
little
research
and
attention
on
it
electrochemical
CO2
reduction
reaction
(eCO2
RR).
Herein,
we
report
a
stable
covalent-organic
framework
(denoted
as
PcNi-im)
with
imidazole
groups
new
electrocatalyst
for
eCO2
RR
to
CO.
Interestingly,
compared
neutral
conditions,
PcNi-im
not
only
showed
high
Faraday
efficiency
of
CO
product
(≈100
%)
under
acidic
conditions
(pH
≈
1),
also
the
partial
current
density
was
increased
from
258
320
mA
cm-2
.
No
obvious
degradation
observed
over
10
hours
continuous
operation
at
250
The
mechanism
study
shows
that
group
can
be
protonated
form
cation
media,
hence
reducing
surface
work
function
charge
active
metal
center.
As
result,
poisoning
weakened
key
intermediate
*COOH
stabilized,
thus
accelerating
rate.
Chemical Society Reviews,
Journal Year:
2022,
Volume and Issue:
51(15), P. 6307 - 6416
Published: Jan. 1, 2022
This
review
highlights
the
recent
advances
of
metalated
covalent
organic
frameworks,
including
synthetic
strategies
and
applications,
discusses
current
challenges
future
directions.
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.
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: June 24, 2023
Developing
highly
efficient,
selective
and
low-overpotential
electrocatalysts
for
carbon
dioxide
(CO2)
reduction
is
crucial.
This
study
reports
an
efficient
Ni
single-atom
catalyst
coordinated
with
pyrrolic
nitrogen
pyridinic
CO2
to
monoxide
(CO).
In
flow
cell
experiments,
the
achieves
a
CO
partial
current
density
of
20.1
mA
cmgeo-2
at
-0.15
V
vs.
reversible
hydrogen
electrode
(VRHE).
It
exhibits
high
turnover
frequency
over
274,000
site-1
h-1
-1.0
VRHE
maintains
Faradaic
efficiency
(FECO)
exceeding
90%
within
-0.9
VRHE.
Operando
synchrotron-based
infrared
X-ray
absorption
spectra,
theoretical
calculations
reveal
that
mono
CO-adsorbed
single
sites
formed
during
electrochemical
processes
contribute
balance
between
key
intermediates
formation
desorption,
providing
insights
into
catalyst's
origin
catalytic
activity.
Overall,
this
work
presents
good
selectivity
activity
while
shedding
light
on
its
underlying
mechanism.
Energy & Environmental Science,
Journal Year:
2022,
Volume and Issue:
16(1), P. 201 - 209
Published: Nov. 23, 2022
A
novel
2D
nickel
porphyrin-based
covalent
organic
framework
is
fabricated
as
an
efficient
nitrate
reduction
electrocatalyst
that
shows
a
great
selectivity
of
∼90%
under
mild
overpotential
with
remarkable
production
rate
and
turnover
frequency.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(26)
Published: March 14, 2023
Non‐noble
iron‐nitrogen‐carbon
(Fe‐N‐C)
catalysts
have
been
explored
as
one
type
of
the
most
promising
alternatives
precious
platinum
(Pt)
in
catalyzing
oxygen
reduction
reaction
(ORR).
However,
their
catalytic
ORR
activity
and
stability
still
cannot
meet
requirement
practical
applications.
Active
sites
such
are
key
factors
determining
performance.
This
review
gives
a
critical
overview
on
identification
understanding
active
sties
non‐pyrolytic
pyrolytic
Fe‐N‐C
terms
design
strategies,
synthesis,
characterization,
functional
mechanisms
performance
validation.
The
diversity
complexity
that
greatly
dominate
progress
include
Fe‐containing
(Fe‐based
nanoparticles
single‐atom
Fe‐species)
metal‐free
(heteroatoms
doping
defects).
Meanwhile,
synergistic
effects
also
discussed
this
with
emphasis
interaction
among
multiple
sites.
Although
substantial
endeavors
devoted
to
develop
efficient
catalysts,
some
challenges
remain.
To
facilitate
further
research
toward
applications,
perspectives
prospected
aspects
innovative
synthesis
methods,
active‐sites
modulation
high‐resolution
ex
situ/in
situ/operando
characterization
techniques,
theoretical
calculations,
so
on.
may
provide
guideline
for
identifying
developing
high‐performance
catalysts.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(8), P. 5622 - 5633
Published: Feb. 19, 2024
Ethylene
glycol
is
an
essential
commodity
chemical
with
high
demand,
which
conventionally
produced
via
thermocatalytic
oxidation
of
ethylene
huge
fossil
fuel
consumption
and
CO2
emission.
The
one-step
electrochemical
approach
offers
a
sustainable
route
but
suffers
from
reliance
on
noble
metal
catalysts,
low
activity,
mediocre
selectivity.
Herein,
we
report
to
over
earth-abundant
metal-based
molecular
catalyst,
cobalt
phthalocyanine
supported
carbon
nanotube
(CoPc/CNT).
catalyst
delivers
100%
selectivity
1.78
min–1
turnover
frequency
at
room
temperature
ambient
pressure,
more
competitive
than
those
obtained
palladium
catalysts.
Experimental
data
demonstrate
that
the
orchestrates
multiple
tasks
in
sequence,
involving
water
activation
generate
high-valence
Co-oxo
species,
epoxidation
afford
oxide
intermediate
oxygen
transfer,
eventually
ring-opening
facilitated
by
situ
formed
Lewis
acid
site.
This
work
great
opportunity
for
chemicals
synthesis
based
one-step,
metal-catalyzed,
renewable
electricity-driven
route.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(4), P. 1540 - 1548
Published: Jan. 1, 2024
Electronic
structure
optimization
of
two-dimensional
metal
phthalocyanine
through
confined
atomic
Ru
species
eliminates
electrocatalytic
kinetic
differences
for
all-pH
hydrogen
evolution.
