Nature Communications,
Год журнала:
2021,
Номер
12(1)
Опубликована: Июнь 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.
Nature Communications,
Год журнала:
2021,
Номер
12(1)
Опубликована: Май 17, 2021
Abstract
Electrochemically
converting
nitrate,
a
widespread
water
pollutant,
back
to
valuable
ammonia
is
green
and
delocalized
route
for
synthesis,
can
be
an
appealing
supplementary
alternative
the
Haber-Bosch
process.
However,
as
there
are
other
nitrate
reduction
pathways
present,
selectively
guiding
reaction
pathway
towards
currently
challenged
by
lack
of
efficient
catalysts.
Here
we
report
selective
active
on
Fe
single
atom
catalyst,
with
maximal
Faradaic
efficiency
~
75%
yield
rate
up
20,000
μg
h
−1
mg
cat.
(0.46
mmol
cm
−2
).
Our
catalyst
effectively
prevent
N-N
coupling
step
required
N
2
due
neighboring
metal
sites,
promoting
product
selectivity.
Density
functional
theory
calculations
reveal
mechanisms
potential
limiting
steps
atomically
dispersed
sites.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(7), С. 2215 - 2264
Опубликована: Янв. 1, 2020
This
review
summarized
the
fabrication
routes
and
characterization
methods
of
atomic
site
electrocatalysts
(ASCs)
followed
by
their
applications
for
water
splitting,
oxygen
reduction
selective
oxidation.
Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
60(9), С. 4448 - 4463
Опубликована: Апрель 21, 2020
Abstract
Single‐atom
catalysts
(SACs)
with
highly
active
sites
atomically
dispersed
on
substrates
exhibit
unique
advantages
regarding
maximum
atomic
efficiency,
abundant
chemical
structures,
and
extraordinary
catalytic
performances
for
multiple
important
reactions.
In
particular,
M–N–C
SACs
(M=transition
metal
atom)
demonstrate
optimal
electrocatalytic
activity
the
oxygen
reduction
reaction
(ORR)
have
attracted
extensive
attention
recently.
Despite
substantial
efforts
in
fabricating
various
SACs,
principles
regulating
intrinsic
of
their
not
been
sufficiently
studied.
this
Review,
we
summarize
regulation
strategies
promoting
ORR
by
modulation
center
atoms,
coordinated
environmental
guest
groups.
Theoretical
calculations
experimental
investigations
are
both
included
to
afford
a
comprehensive
understanding
structure–performance
relationship.
Finally,
future
directions
developing
advanced
other
analogous
reactions
proposed.
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(36), С. 19572 - 19590
Опубликована: Фев. 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.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(18), С. 6605 - 6631
Опубликована: Янв. 1, 2020
Recent
advances
in
the
design,
preparation,
and
applications
of
different
catalysts
for
electrochemical
photochemical
H2O2
production
are
summarized,
some
invigorating
perspectives
future
developments
also
provided.
Nature Communications,
Год журнала:
2020,
Номер
11(1)
Опубликована: Июль 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.
