Accounts of Chemical Research,
Journal Year:
2018,
Volume and Issue:
51(11), P. 2968 - 2977
Published: Oct. 30, 2018
Recent
years
have
witnessed
significant
development
of
electrocatalysis
for
clean
energy
and
related
potential
technologies.
The
precise
identification
toward
active
sites
catalysts
the
monitoring
product
information
are
highly
desirable
to
understand
how
materials
catalyze
a
specific
electrocatalytic
reaction.
For
long
period,
cognition
corresponding
catalytic
mechanisms
generally
based
on
various
ex
situ
characterization
methods
which
actually
could
not
capture
dynamic
structure
intermediate
during
processes.
With
recent
developments
in
operando
techniques,
it
has
been
extensively
observed
that
most
would
undergo
structural
self-reconstruction
as
result
electro-derived
oxidation
or
reduction
process
at
given
potential,
often
accompanied
by
increase
decrease
activity
well
change
selectivity.
In
fact,
such
self-change
does
make
difficult
identify
true
catalytically
efficiently,
thus
hindering
understanding
real
mechanism.
Therefore,
we
believe
combination
reliable
techniques
theoretical
calculations
holds
key
rational
design
advanced
catalysts.
this
Account,
provide
in-depth
insights
into
progress
regarding
electrocatalysts
several
typical
electrochemical
reactions
with
emphasis
fundamental
knowledge,
structure-property
relationships,
evolution
process,
modulation
self-reconstruction.
To
deliver
clear
understanding,
be
pointed
out
advance
these
drastic
processes
suggested
called
precatalysts
under
nonreaction
conditions.
restructured
components
realistic
reaction
conditions
bridges
behavior,
following
three
critical
aspects
will
carefully
disclosed
discussed
depth.
First,
origin
is
introduced.
It
noteworthy
atomic-level
correlations
between
behavior
intrinsic
emphasized
due
fact
even
if
some
congeneric,
they
exhibit
diverse
phenomenon
performance.
Second,
should
monitored
central
precisely
unveil
behavior.
characterizations
considered
judicious
track
self-reconstruction,
analyze
real-time
products.
Finally,
together
comprehensive
theory
calculations,
enhancement
degradation
mechanism
activities
can
unambiguously
clarified.
thoughtful
studies
complete
electrocatalysts,
feasible
tune
improve
performance
rationally
proposed.
Based
progress,
hope
new
insight
electrocatalysis,
particularly
then
offer
guidelines
electrocatalysts.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
33(31)
Published: June 12, 2021
Abstract
Hydrogen
economy
has
emerged
as
a
very
promising
alternative
to
the
current
hydrocarbon
economy,
which
involves
process
of
harvesting
renewable
energy
split
water
into
hydrogen
and
oxygen
then
further
utilization
clean
fuel.
The
production
by
electrolysis
is
an
essential
prerequisite
with
zero
carbon
emission.
Among
various
technologies,
alkaline
splitting
been
commercialized
for
more
than
100
years,
representing
most
mature
economic
technology.
Here,
historic
development
overviewed,
several
critical
electrochemical
parameters
are
discussed.
After
that,
advanced
nonprecious
metal
electrocatalysts
that
recently
negotiating
evolution
reaction
(OER)
(HER)
discussed,
including
transition
oxides,
(oxy)hydroxides,
chalcogenides,
phosphides,
nitrides
OER,
well
alloys,
carbides
HER.
In
this
section,
particular
attention
paid
catalyst
synthesis,
activity
stability
challenges,
performance
improvement,
industry‐relevant
developments.
Some
recent
works
about
scaled‐up
novel
electrode
designs,
seawater
also
spotlighted.
Finally,
outlook
on
future
challenges
opportunities
offered,
potential
directions
speculated.
Chemical Reviews,
Journal Year:
2020,
Volume and Issue:
120(15), P. 7642 - 7707
Published: July 8, 2020
Energy
and
water
are
of
fundamental
importance
for
our
modern
society,
advanced
technologies
on
sustainable
energy
storage
conversion
as
well
resource
management
in
the
focus
intensive
research
worldwide.
Beyond
their
traditional
biological
applications,
hydrogels
emerging
an
appealing
materials
platform
energy-
water-related
applications
owing
to
attractive
tailorable
physiochemical
properties.
In
this
review,
we
highlight
highly
tunable
synthesis
various
hydrogels,
involving
key
synthetic
elements
such
monomer/polymer
building
blocks,
cross-linkers,
functional
additives,
discuss
how
can
be
employed
precursors
templates
architecting
three-dimensional
frameworks
electrochemically
active
materials.
We
then
present
in-depth
discussion
structure–property
relationships
hydrogel
based
gelation
chemistry,
ultimately
targeting
properties
enhanced
ionic/electronic
conductivities,
mechanical
strength,
flexibility,
stimuli-responsiveness,
desirable
swelling
behavior.
The
unique
interconnected
porous
structures
enable
fast
charge/mass
transport
while
offering
large
surface
areas,
polymer–water
interactions
regulated
achieve
retention,
absorption,
evaporation
within
hydrogels.
Such
structure-derived
also
intimately
coordinated
realize
multifunctionality
stability
different
target
devices.
plethora
stimulating
examples
is
expounded
with
a
batteries,
supercapacitors,
electrocatalysts,
solar
purification,
atmospheric
harvesting,
which
showcase
unprecedented
technological
potential
enabled
by
hydrogel-derived
Finally,
study
challenges
ways
tackling
them
reveal
underlying
mechanisms
transform
current
development
into
technologies.
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(15), P. 8428 - 8469
Published: Jan. 1, 2021
The
recent
progress
in
activating
surface
reconstruction
by
integrating
advanced
characterizations
with
theoretical
calculations
for
high-efficiency
oxygen
evolution
reaction
is
reviewed.
Nature Communications,
Journal Year:
2019,
Volume and Issue:
10(1)
Published: Dec. 6, 2019
Abstract
Efficient
generation
of
hydrogen
from
water-splitting
is
an
underpinning
chemistry
to
realize
the
economy.
Low
cost,
transition
metals
such
as
nickel
and
iron-based
oxides/hydroxides
have
been
regarded
promising
catalysts
for
oxygen
evolution
reaction
in
alkaline
media
with
overpotentials
low
~200
mV
achieve
10
mA
cm
−2
,
however,
they
are
generally
unsuitable
reaction.
Herein,
we
show
a
Janus
nanoparticle
catalyst
nickel–iron
oxide
interface
multi-site
functionality
highly
efficient
comparable
performance
benchmark
platinum
on
carbon
catalyst.
Density
functional
theory
calculations
reveal
that
catalytic
activity
induced
by
strong
electronic
coupling
effect
between
iron
at
interface.
Remarkably,
also
exhibits
extraordinary
activity,
enabling
active
stable
bi-functional
whole
cell
with,
best
our
knowledge,
highest
energy
efficiency
(83.7%)
reported
date.
Advanced Materials,
Journal Year:
2019,
Volume and Issue:
31(17)
Published: Feb. 18, 2019
Electrochemical
water
splitting
driven
by
sustainable
energy
such
as
solar,
wind,
and
tide
is
attracting
ever-increasing
attention
for
production
of
clean
hydrogen
fuel
from
water.
Leveraging
these
advances
requires
efficient
earth-abundant
electrocatalysts
to
accelerate
the
kinetically
sluggish
oxygen
evolution
reactions
(HER
OER).
A
large
number
advanced
water-splitting
have
been
developed
through
recent
understanding
electrochemical
nature
engineering
approaches.
Specifically,
strain
offers
a
novel
route
promote
electrocatalytic
HER/OER
performances
splitting.
Herein,
theoretical
experimental
progress
on
applying
enhance
heterogeneous
both
HER
OER
are
reviewed
future
opportunities
discussed.
brief
introduction
fundamentals
reactions,
rationalization
utilizing
mechanical
tune
an
electrocatalyst
given,
followed
discussion
strain-promoted
OER,
with
special
emphasis
given
combined
approaches
determining
optimal
straining
effect
electrolysis,
along
creating
characterizing
in
nanocatalysts,
particularly
emerging
2D
nanomaterials.
Finally,
vision
community
based
electrolysis
proposed.
Chemical Reviews,
Journal Year:
2020,
Volume and Issue:
121(2), P. 567 - 648
Published: Sept. 17, 2020
Heterogeneous
catalysis
involves
solid-state
catalysts,
among
which
metal
nanoparticles
occupy
an
important
position.
Unfortunately,
no
two
from
conventional
synthesis
are
the
same
at
atomic
level,
though
such
regular
can
be
highly
uniform
nanometer
level
(e.g.,
size
distribution
∼5%).
In
long
pursuit
of
well-defined
nanocatalysts,
a
recent
success
is
atomically
precise
nanoclusters
protected
by
ligands
in
range
tens
to
hundreds
atoms
(equivalently
1–3
nm
core
diameter).
More
importantly,
have
been
crystallographically
characterized,
just
like
protein
structures
enzyme
catalysis.
Such
merge
features
homogeneous
catalysts
ligand-protected
centers)
and
enzymes
protein-encapsulated
clusters
few
bridged
ligands).
The
with
their
total
available
constitute
new
class
model
hold
great
promise
fundamental
research,
including
dependent
activity,
control
catalytic
selectivity
structure
surface
ligands,
structure–property
relationships
atomic-level,
insights
into
molecular
activation
mechanisms,
identification
active
sites
on
nanocatalysts.
This
Review
summarizes
progress
utilization
for
These
nanocluster-based
enabled
heterogeneous
research
single-atom
single-electron
levels.
Future
efforts
expected
achieve
more
exciting
understanding
tailoring
design
high
activity
under
mild
conditions.
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.