Angewandte Chemie,
Год журнала:
2023,
Номер
136(1)
Опубликована: Окт. 24, 2023
Abstract
Electrochemical
CO
2
reduction
(CO
RR)
on
copper
(Cu)
shows
promise
for
higher‐value
products
beyond
CO.
However,
challenges
such
as
the
limited
solubility,
high
overpotentials,
and
competing
hydrogen
evolution
reaction
(HER)
in
aqueous
electrolytes
hinder
practical
realization.
We
propose
a
functionalized
ionic
liquid
(IL)
which
generates
ion‐CO
adducts
bond
donor
(HBD)
upon
absorption
to
modulate
RR
Cu
non‐aqueous
electrolyte.
As
revealed
by
transient
voltammetry,
electrochemical
impedance
spectroscopy
(EIS),
situ
surface‐enhanced
Raman
(SERS)
complemented
with
image
charge
augmented
quantum‐mechanical/molecular
mechanics
(IC‐QM/MM)
computations,
unique
microenvironment
is
constructed.
In
this
microenvironment,
catalytic
activity
primarily
governed
IL
HBD
concentrations;
former
controlling
double
layer
thickness
latter
modulating
local
proton
availability.
This
translates
ample
availability,
reduced
overpotential,
suppressed
HER
where
C
4
are
obtained.
study
deepens
understanding
of
electrolyte
effects
role
ions
towards
electrocatalytic
design.
Chemical Science,
Год журнала:
2024,
Номер
15(26), С. 9949 - 9976
Опубликована: Янв. 1, 2024
Electrocatalysis
stands
out
as
a
promising
avenue
for
synthesizing
high-value
products
with
minimal
environmental
footprint,
aligning
the
imperative
sustainable
energy
solutions.
Deep
eutectic
solvents
(DESs),
renowned
their
eco-friendly,
safe,
and
cost-effective
nature,
present
myriad
advantages,
including
extensive
opportunities
material
innovation
utilization
reaction
media
in
electrocatalysis.
This
review
initiates
an
exposition
on
distinctive
features
of
DESs,
progressing
to
explore
applications
electrocatalyst
synthesis
Additionally,
it
offers
insightful
analysis
challenges
prospects
inherent
electrocatalysis
within
DESs.
By
delving
into
these
aspects
comprehensively,
this
aims
furnish
nuanced
understanding
thus
broadening
horizons
realm
facilitating
expanded
application.
Environmental Science & Technology,
Год журнала:
2025,
Номер
59(6), С. 3263 - 3275
Опубликована: Янв. 6, 2025
Electrocatalytic
nitrate
reduction
reaction
(NO3RR)
to
harmless
nitrogen
(N2)
presents
a
viable
approach
for
purifying
NO3–-contaminated
wastewater,
yet
most
current
electrocatalysts
predominantly
produce
ammonium/ammonia
(NH4+/NH3)
due
challenges
in
facilitating
N–N
coupling.
This
study
focuses
on
identifying
metal
catalysts
that
preferentially
generate
N2
and
elucidating
the
mechanistic
origins
of
their
high
selectivity.
Our
evaluation
16
commercially
available
metals
reveals
only
Pb,
Sn,
In
demonstrated
substantial
selectivity
(79.3,
70.0,
57.0%,
respectively,
under
conditions
6
h
electrolysis,
density
10
mA/cm2,
an
initial
NO3–-N
concentration
100
mg/L),
while
others
largely
favored
NH4+
production.
Comprehensive
experimental
theoretical
analyses
indicate
NH4+-selective
(e.g.,
Co)
exhibited
water
activity
enhances
•H
coverage,
thereby
promoting
hydrogenation
NO3–
through
hydrogen
atom
transfer
mechanism.
contrast,
N2-selective
catalysts,
with
lower
activity,
promoted
formation
N-containing
intermediates,
which
likely
undergo
dimerization
form
via
proton-coupled
electron
Enhancing
adsorption
was
beneficial
improve
by
competitively
reducing
coverage.
findings
highlight
crucial
role
NO3RR
performance
offer
rational
design
enhanced
Advanced Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 5, 2025
Abstract
Electrocatalytic
CO
2
reduction
(CO
RR)
is
rapidly
emerging
as
a
promising
sustainable
strategy
for
transforming
into
valuable
fuels
and
chemical
feedstocks,
crucial
step
toward
carbon‐neutral
society.
The
efficiency,
selectivity,
stability
of
RR
are
heavily
influenced
by
the
chosen
catalyst
operating
conditions
used.
Despite
substantial
advances
in
development
catalysts,
there
scarcity
comprehensive
reviews
focusing
on
influence
different
environments
performance.
This
review
offers
detailed
examination
internal
external
environmental
control
strategies
designed
to
enhance
efficiency.
fundamental
reaction
mechanisms
through
situ
operational
techniques,
paired
with
theoretical
analyses,
discussed
while
also
identifying
key
challenges
future
research
directions
technology.
By
delivering
overview
current
state
field,
this
highlights
critical
role
control,
mechanistic
insights,
practical
considerations
needed
successful
commercialization
National Science Review,
Год журнала:
2024,
Номер
11(8)
Опубликована: Июнь 22, 2024
ABSTRACT
Both
the
catalyst
and
electrolyte
strongly
impact
performance
of
CO2
electrolysis.
Despite
substantial
progress
in
catalysts,
it
remains
highly
challenging
to
tailor
compositions
understand
their
functions
at
interface.
Here,
we
report
that
ethylenediaminetetraacetic
acid
(EDTA)
its
analogs,
featuring
strong
Lewis
acid-base
interaction
with
metal
cations,
are
selected
as
additives
reshape
catalyst-electrolyte
interface
for
promoting
Mechanistic
studies
reveal
EDTA
molecules
dynamically
assembled
toward
regions
response
bias
potential
due
EDTA4–-K+.
As
a
result,
original
hydrogen-bond
network
among
interfacial
H2O
is
disrupted,
gap
layer
electrified
established.
The
EDTA-reshaped
K+
solvation
structure
promotes
protonation
*CO2
*COOH
suppressing
*H2O
dissociation
*H,
thereby
boosting
co-electrolysis
carbon-based
products.
In
particular,
when
5
mM
added
into
electrolytes,
Faradaic
efficiency
CO
on
commercial
Ag
nanoparticle
increased
from
57.0%
90.0%
an
industry-relevant
current
density
500
mA
cm−2.
More
importantly,
Lewis-base
ligand-reshaped
allows
range
catalysts
(Ag,
Zn,
Pd,
Bi,
Sn,
Cu)
deliver
substantially
selectivity
products
both
H-type
flow-type
electrolysis
cells.
Chemical Communications,
Год журнала:
2024,
Номер
60(21), С. 2887 - 2897
Опубликована: Янв. 1, 2024
This
feature
article
overviews
the
properties
of
green
solvent
systems
and
their
applications
in
framework
material
syntheses
CO
2
reduction
reactions.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
63(1)
Опубликована: Окт. 24, 2023
Abstract
Electrochemical
CO
2
reduction
(CO
RR)
on
copper
(Cu)
shows
promise
for
higher‐value
products
beyond
CO.
However,
challenges
such
as
the
limited
solubility,
high
overpotentials,
and
competing
hydrogen
evolution
reaction
(HER)
in
aqueous
electrolytes
hinder
practical
realization.
We
propose
a
functionalized
ionic
liquid
(IL)
which
generates
ion‐CO
adducts
bond
donor
(HBD)
upon
absorption
to
modulate
RR
Cu
non‐aqueous
electrolyte.
As
revealed
by
transient
voltammetry,
electrochemical
impedance
spectroscopy
(EIS),
situ
surface‐enhanced
Raman
(SERS)
complemented
with
image
charge
augmented
quantum‐mechanical/molecular
mechanics
(IC‐QM/MM)
computations,
unique
microenvironment
is
constructed.
In
this
microenvironment,
catalytic
activity
primarily
governed
IL
HBD
concentrations;
former
controlling
double
layer
thickness
latter
modulating
local
proton
availability.
This
translates
ample
availability,
reduced
overpotential,
suppressed
HER
where
C
4
are
obtained.
study
deepens
understanding
of
electrolyte
effects
role
ions
towards
electrocatalytic
design.
iScience,
Год журнала:
2024,
Номер
27(3), С. 109313 - 109313
Опубликована: Фев. 23, 2024
SummaryElectrocatalytic
CO2
reduction
reaction
(CO2RR)
has
emerged
as
a
focal
point
in
sustainable
energy
research,
offering
the
potential
for
closed
carbon
cycle.
Among
numerous
catalysts
designed
CO2RR,
two-dimensional
(2D)
Cu-based
stand
out
their
remarkable
performance
efficiently
converting
into
high-value-added
C1
and
C2+
chemicals.
Herein,
we
discuss
recent
progress
challenges
realm
of
CO2RR
utilizing
2D
catalysts.
The
first
section
introduces
various
synthetic
strategies,
emphasizing
features
advantages
different
techniques
proposing
solutions
to
existing
challenges.
second
part
outlines
mechanism
underlying
production
products
on
catalysts,
then
summarizes
applications
types
CO2RR.
Additionally,
evaluate
limitations
propose
improved
strategies.
Through
this
exploration
research
advances
challenges,
hope
illuminate
path
toward
developing
excellent
electrocatalysts.Graphical
abstract
