Energy & Environmental Science,
Journal Year:
2020,
Volume and Issue:
13(8), P. 2275 - 2309
Published: Jan. 1, 2020
This
review
discusses
how
morphology
and
interface
engineering
promote
electrocatalytic
CO2
reduction,
providing
general
design
principles
to
fabricate
advanced
electrode
catalysts.
Journal of the American Chemical Society,
Journal Year:
2020,
Volume and Issue:
142(15), P. 7036 - 7046
Published: March 30, 2020
The
limitations
of
the
Haber-Bosch
reaction,
particularly
high-temperature
operation,
have
ignited
new
interests
in
low-temperature
ammonia-synthesis
scenarios.
Ambient
N2
electroreduction
is
a
compelling
alternative
but
impeded
by
low
ammonia
production
rate
(mostly
<10
mmol
gcat-1
h-1),
small
partial
current
density
(<1
mA
cm-2),
and
high-selectivity
hydrogen-evolving
side
reaction.
Herein,
we
report
that
room-temperature
nitrate
catalyzed
strained
ruthenium
nanoclusters
generates
at
higher
(5.56
mol
h-1)
than
process.
primary
contributor
to
such
performance
hydrogen
radicals,
which
are
generated
suppressing
hydrogen-hydrogen
dimerization
during
water
splitting
enabled
tensile
lattice
strains.
radicals
expedite
nitrate-to-ammonia
conversion
hydrogenating
intermediates
rate-limiting
steps
lower
kinetic
barriers.
nanostructures
can
maintain
nearly
100%
ammonia-evolving
selectivity
>120
cm-2
densities
for
100
h
due
robust
subsurface
Ru-O
coordination.
These
findings
highlight
potential
real-world,
synthesis.
Journal of the American Chemical Society,
Journal Year:
2021,
Volume and Issue:
143(20), P. 7819 - 7827
Published: May 13, 2021
Product
selectivity
in
multielectron
electrocatalytic
reactions
is
crucial
to
energy
conversion
efficiency
and
chemical
production.
However,
a
present
practical
drawback
the
limited
understanding
of
actual
catalytic
active
sites.
Here,
using
as
prototype
single-atom
catalysts
(SACs)
acidic
oxygen
reduction
reaction
(ORR),
we
report
structure–property
relationship
show
for
first
time
that
molecular-level
local
structure,
including
second
coordination
spheres
(CSs),
rather
than
individual
atoms,
synergistically
determines
response.
ORR
on
Co-SACs
can
be
tailored
from
four-electron
two-electron
pathway
by
modifying
(N
or/and
O
coordination)
(C–O–C
groups)
CSs.
Using
combined
theoretical
predictions
experiments,
X-ray
absorption
fine
structure
analyses
situ
infrared
spectroscopy,
confirm
unique
change
originates
structure-dependent
shift
sites
center
Co
atom
O-adjacent
C
atom.
We
this
optimizes
electronic
*OOH
adsorption
behavior
give
"best"
activity
>95%
H2O2
electrosynthesis.
Angewandte Chemie International Edition,
Journal Year:
2020,
Volume and Issue:
59(51), P. 22894 - 22915
Published: Feb. 3, 2020
Transforming
CO2
into
fuels
by
utilizing
sunlight
is
promising
to
synchronously
overcome
global
warming
and
energy-supply
issues.
It
crucial
design
efficient
photocatalysts
with
intriguing
features
such
as
robust
light-harvesting
ability,
strong
redox
potential,
high
charge-separation,
excellent
durability.
Hitherto,
a
single-component
photocatalyst
incapable
simultaneously
meet
all
these
criteria.
Inspired
natural
photosynthesis,
constructing
artificial
Z-scheme
provides
facile
way
conquer
bottlenecks.
In
this
review,
we
firstly
introduce
the
fundamentals
of
photocatalytic
reduction
systems.
Thereafter
discuss
state-of-the-art
reduction,
whereby
special
attention
placed
on
predominant
factors
that
affect
photoactivity.
Additionally,
further
modifications
are
important
for
photocatalysis
reviewed.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(36), P. 19572 - 19590
Published: Feb. 19, 2021
Abstract
Compared
to
modern
fossil‐fuel‐based
refineries,
the
emerging
electrocatalytic
refinery
(e‐refinery)
is
a
more
sustainable
and
environmentally
benign
strategy
convert
renewable
feedstocks
energy
sources
into
transportable
fuels
value‐added
chemicals.
A
crucial
step
in
conducting
e‐refinery
processes
development
of
appropriate
reactions
optimal
electrocatalysts
for
efficient
cleavage
formation
chemical
bonds.
However,
compared
well‐studied
primary
(e.g.,
O
2
reduction,
water
splitting),
mechanistic
aspects
materials
design
complex
are
yet
be
settled.
To
address
this
challenge,
herein,
we
first
present
fundamentals
heterogeneous
electrocatalysis
some
reactions,
then
implement
these
establish
framework
by
coupling
situ
generated
intermediates
(integrated
reactions)
or
products
(tandem
reactions).
We
also
set
principles
strategies
efficiently
manipulate
reaction
pathways.
Advanced Materials,
Journal Year:
2020,
Volume and Issue:
32(34)
Published: July 9, 2020
The
electrochemical
CO2
reduction
reaction
(CO2
RR)
is
of
great
importance
to
tackle
the
rising
concentration
in
atmosphere.
RR
can
be
driven
by
renewable
energy
sources,
producing
precious
chemicals
and
fuels,
with
implementation
this
process
largely
relying
on
development
low-cost
efficient
electrocatalysts.
Recently,
a
range
heterogeneous
potentially
single-atom
catalysts
(SACs)
containing
non-precious
metals
coordinated
earth-abundant
elements
have
emerged
as
promising
candidates
for
RR.
Unfortunately,
real
catalytically
active
centers
key
factors
that
govern
catalytic
performance
these
SACs
remain
ambiguous.
Here,
ambiguity
addressed
developing
fundamental
understanding
RR-to-CO
SACs,
CO
accounts
major
product
from
SACs.
mechanism,
rate-determining
steps,
control
activity
selectivity
are
analyzed
both
experimental
theoretical
studies.
Then,
synthesis,
characterization,
discussed.
Finally,
challenges
future
pathways
highlighted
hope
guiding
design
promote
understand