Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: May 9, 2024
Abstract
Electrochemical
CO
2
reduction
reaction
(CO
RR)
powered
by
renewable
energy
provides
a
promising
route
to
conversion
and
utilization.
However,
the
widely
used
neutral/alkaline
electrolyte
consumes
large
amount
of
produce
(bi)carbonate
byproducts,
leading
significant
challenges
at
device
level,
thereby
impeding
further
deployment
this
reaction.
Conducting
RR
in
acidic
electrolytes
offers
solution
address
“carbonate
issue”;
however,
it
presents
inherent
difficulties
due
competitive
hydrogen
evolution
reaction,
necessitating
concerted
efforts
toward
advanced
catalyst
electrode
designs
achieve
high
selectivity
activity.
This
review
encompasses
recent
developments
RR,
from
mechanism
elucidation
design
engineering.
begins
discussing
mechanistic
understanding
pathway,
laying
foundation
for
RR.
Subsequently,
an
in‐depth
analysis
advancements
catalysts
is
provided,
highlighting
heterogeneous
catalysts,
surface
immobilized
molecular
enhancement.
Furthermore,
progress
made
device‐level
applications
summarized,
aiming
develop
high‐performance
systems.
Finally,
existing
future
directions
are
outlined,
emphasizing
need
improved
selectivity,
activity,
stability,
scalability.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
146(1), P. 263 - 273
Published: Dec. 18, 2023
Dual-atom
catalysts
(DACs)
with
paired
active
sites
can
provide
unique
intrinsic
properties
for
heterogeneous
catalysis,
but
the
synergy
of
centers
remains
to
be
elucidated.
Here,
we
develop
a
high-performance
DAC
Zn
ACS Energy Letters,
Journal Year:
2023,
Volume and Issue:
8(3), P. 1330 - 1335
Published: Feb. 7, 2023
Improved
oxygen
electrocatalysis
is
crucial
for
the
ever-growing
energy
demand.
Metal-nitrogen-carbon
(M-N-C)
materials
are
promising
candidates
catalysts.
Their
activity
tunable
via
varying
electronic
and
geometric
properties,
such
as
porosity.
Because
of
difficulty
in
modeling
porosity,
M-N-Cs
with
variable
surface
curvature
remained
largely
unexplored.
In
this
work,
we
developed
a
realistic
in-pore
dual-atom
site
M-N-C
model
applied
density
functional
theory
to
investigate
effect
on
reduction
evolution
reactions.
We
show
that
curving
tailors
both
scaling
relations
barriers.
Thus,
predict
adjusting
can
improve
catalytic
toward
mono-
bifunctional
electrocatalysis.
Chemical Science,
Journal Year:
2024,
Volume and Issue:
15(14), P. 5082 - 5112
Published: Jan. 1, 2024
This
review
systematically
introduces
how
to
regulate
the
electronic
structure
and
geometric
configuration
of
atomic
catalysts
achieve
high-efficiency
electrocatalysis
performances
by
analyzing
detailed
electrocatalytic
applications
mechanisms.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(46)
Published: Sept. 25, 2023
Electronic
structure
calculations
represent
an
essential
complement
of
experiments
to
characterize
single-atom
catalysts
(SACs),
consisting
isolated
metal
atoms
stabilized
on
a
support,
but
also
predict
new
catalysts.
However,
simulating
SACs
with
quantum
chemistry
approaches
is
not
as
simple
often
assumed.
In
this
work,
the
factors
that
reliable
simulation
activity
are
examined.
The
Perspective
focuses
importance
precise
atomistic
characterization
active
site,
since
even
small
changes
in
atom's
surroundings
can
result
large
reactivity.
dynamical
behavior
and
stability
under
working
conditions,
well
adopting
appropriate
methods
solve
Schrödinger
equation
for
quantitative
evaluation
reaction
energies
addressed.
relevance
model
adopted.
For
electrocatalysis
must
include
effects
solvent,
presence
electrolytes,
pH,
external
potential.
Finally,
it
discussed
how
similarities
between
coordination
compounds
may
intermediates
usually
observed
electrodes.
When
these
aspects
adequately
considered,
predictive
power
electronic
quite
limited.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(22)
Published: March 30, 2023
Iron
phthalocyanine-based
polymers
(PFePc)
are
attractive
noble-metal-free
candidates
for
catalyzing
oxygen
reduction
reaction
(ORR).
However,
the
low
site-exposure
degree
and
poor
electrical
conductivity
of
bulk
PFePc
restricted
their
practical
applications.
Herein,
laminar
nanosheets
covalently
longitudinally
linked
to
graphene
(3D-G-PFePc)
was
prepared.
Such
structural
engineering
qualifies
3D-G-PFePc
with
high
site
utilization
rapid
mass
transfer.
Thence,
demonstrates
efficient
ORR
performance
a
specific
activity
69.31
μA
cm-2
,
81.88
A
g-1
turnover
frequency
0.93
e
s-1
site-1
at
0.90
V
vs.
reversible
hydrogen
electrode
in
O2
-saturated
0.1
M
KOH,
outperforming
lamellar
wrapped
counterpart.
Systematic
electrochemical
analyses
integrating
variable-frequency
square
wave
voltammetry
situ
scanning
microscopy
further
underline
kinetics
towards
ORR.
Nano Letters,
Journal Year:
2024,
Volume and Issue:
24(28), P. 8502 - 8509
Published: July 1, 2024
N2O
is
a
dominant
atmosphere
pollutant,
causing
ozone
depletion
and
global
warming.
Currently,
electrochemical
reduction
of
has
gained
increasing
attention
to
remove
N2O,
but
its
product
worthless
N2.
Here,
we
propose
direct
eight-electron
(8e)
pathway
electrochemically
convert
into
NH3.
As
proof
concept,
using
density
functional
theory
calculation,
an
Fe2
double-atom
catalyst
(DAC)
anchored
by
N-doped
porous
graphene
(Fe2@NG)
was
screened
out
be
the
most
active
selective
for
electroreduction
toward
NH3
via
novel
8e
pathway,
which
benefits
from
unique
bent
adsorption
configuration.
Guided
theoretical
prediction,
Fe2@NG
DAC
fabricated
experimentally,
it
can
achieve
high
N2O-to-NH3
Faradaic
efficiency
77.8%
with
large
yield
rate
2.9
mg
h–1
cm–2
at
−0.6
V
vs
RHE
in
neutral
electrolyte.
Our
study
offers
feasible
strategy
synthesize
pollutant
simultaneous
removal.
