Nature Communications,
Journal Year:
2021,
Volume and Issue:
12(1)
Published: June 17, 2021
Abstract
Solar-driven
hydrogen
peroxide
(H
2
O
)
production
presents
unique
merits
of
sustainability
and
environmental
friendliness.
Herein,
efficient
solar-driven
H
through
dioxygen
reduction
is
achieved
by
employing
polymeric
carbon
nitride
framework
with
sodium
cyanaminate
moiety,
affording
a
rate
18.7
μmol
h
−1
mg
an
apparent
quantum
yield
27.6%
at
380
nm.
The
overall
photocatalytic
transformation
process
systematically
analyzed,
some
previously
unknown
structural
features
interactions
are
substantiated
via
experimental
theoretical
methods.
cyanamino
group
pyridinic
nitrogen-coordinated
soidum
in
the
promote
photon
absorption,
alter
energy
landscape
improve
charge
separation
efficiency,
enhance
surface
adsorption
dioxygen,
create
selective
2e
−
oxygen
reaction
surface-active
sites.
Particularly,
electronic
coupling
interaction
between
surface,
which
boosts
population
prolongs
lifetime
active
shallow-trapped
electrons,
experimentally
substantiated.
Chemical Society Reviews,
Journal Year:
2019,
Volume and Issue:
48(24), P. 5658 - 5716
Published: Jan. 1, 2019
Nitrogen
is
a
fundamental
constituent
for
all
living
creatures
on
the
Earth
and
modern
industrial
society.
The
current
nitrogen
industry
largely
powered
by
fossil
fuels
with
huge
energy
consumption
carbon
dioxide
emission,
pollution
in
surface
water
bodies
induced
indiscriminate
discharge
of
domestic
wastewater
has
become
worldwide
environmental
concern.
Electrochemical
techniques
fixation
transformation
under
mild
conditions
are
promising
approaches
to
meet
challenge
efficiently
managing
balancing
cycle,
where
rational
design
advanced
electrocatalysts
from
both
structural
compositional
aspects
down
nanoscale
plays
most
essential
role.
Herein,
important
species
including
dinitrogen
(N2),
ammonia
(NH3)
hydrazine
(N2H4),
their
processes
between
each
other
reduction
reaction
(NRR),
oxidation
(AOR)
(HzOR),
research
progress
development
related
systematically
summarized,
aiming
at
establishing
general
picture
whole
cycle
instead
certain
single
reaction.
Strategies
combining
theoretical
computations
experimental
optimizations
proposed
improve
catalytic
performance
activity,
efficiency,
selectivity
stability,
finally
contributing
self-sufficient
carbon-free
"green"
economy.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(38), P. 20627 - 20648
Published: April 17, 2021
Abstract
The
electrochemical
carbon
dioxide
reduction
reaction
(CO
2
RR)
provides
an
attractive
approach
to
convert
renewable
electricity
into
fuels
and
feedstocks
in
the
form
of
chemical
bonds.
Among
different
CO
RR
pathways,
conversion
is
considered
one
most
promising
candidate
reactions
because
its
high
technological
economic
feasibility.
Integrating
catalyst
electrolyte
design
with
understanding
catalytic
mechanism
will
yield
scientific
insights
promote
this
technology
towards
industrial
implementation.
Herein,
we
give
overview
recent
advances
challenges
for
selective
CO.
Multidimensional
engineering
are
also
summarized.
Furthermore,
studies
on
large‐scale
production
highlighted
facilitate
industrialization
.
To
conclude,
remaining
future
directions
application
generate
highlighted.
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 Energy Materials,
Journal Year:
2019,
Volume and Issue:
10(11)
Published: Dec. 13, 2019
Abstract
Selective
CO
2
reduction
to
formic
acid
or
formate
is
the
most
technologically
and
economically
viable
approach
realize
electrochemical
valorization.
Main
group
metal–based
(Sn,
Bi,
In,
Pb,
Sb)
nanostructured
materials
hold
great
promise,
but
are
still
confronted
with
several
challenges.
Here,
current
status,
challenges,
future
opportunities
of
main
for
reviewed.
Firstly,
fundamentals
presented,
including
technoeconomic
viability
different
products,
possible
reaction
pathways,
standard
experimental
procedure,
performance
figures
merit.
This
then
followed
by
detailed
discussions
about
types
electrocatalyst
materials,
an
emphasis
on
underlying
material
design
principles
promoting
activity,
selectivity,
stability.
Subsequently,
recent
efforts
flow
cells
membrane
electrode
assembly
reviewed
so
as
promote
density
well
mechanistic
studies
using
in
situ
characterization
techniques.
To
conclude
a
short
perspective
offered
directions
this
exciting
field.
Nature Communications,
Journal Year:
2020,
Volume and Issue:
11(1)
Published: July 20, 2020
Electrochemical
CO2
reduction
reaction
(CO2RR)
to
liquid
fuels
is
currently
challenged
by
low
product
concentrations,
as
well
their
mixture
with
traditional
electrolytes,
such
KHCO3
solution.
Here
we
report
an
all-solid-state
electrochemical
CO2RR
system
for
continuous
generation
of
high-purity
and
high-concentration
formic
acid
vapors
solutions.
The
cathode
anode
were
separated
a
porous
solid
electrolyte
(PSE)
layer,
where
electrochemically
generated
formate
proton
recombined
form
molecular
acid.
can
be
efficiently
removed
in
the
via
inert
gas
stream
flowing
through
PSE
layer.
Coupling
high
activity
(formate
partial
current
densities
~450
mA
cm-2),
selectivity
(maximal
Faradaic
efficiency
~97%),
stability
(100
hours)
grain
boundary-enriched
bismuth
catalyst,
demonstrated
ultra-high
concentrations
pure
solutions
(up
nearly
100
wt.%)
condensed
from
flexible
tuning
carrier
stream.
