Nature Communications,
Год журнала:
2021,
Номер
12(1)
Опубликована: Фев. 22, 2021
Abstract
As
a
100%
atom-economy
process,
direct
oxidation
of
methane
into
methanol
remains
as
grand
challenge
due
to
the
dilemma
between
activation
and
over-oxidation
methanol.
Here,
we
report
that
water
enabled
mild
with
>99%
selectivity
over
Au
single
atoms
on
black
phosphorus
(Au
1
/BP)
nanosheets
under
light
irradiation.
The
mass
activity
/BP
reached
113.5
μmol
g
catal
−1
in
pressured
33
bar
mixed
gas
(CH
4
:O
2
=
10:1)
at
90
°C
irradiation
(1.2
W),
while
energy
was
43.4
kJ
mol
.
Mechanistic
studies
revealed
assisted
O
generate
reactive
hydroxyl
groups
•OH
radicals
Hydroxyl
reacted
form
CH
3
*
species,
followed
by
via
Considering
recycling
during
whole
can
also
regard
catalyst.
ACS Catalysis,
Год журнала:
2018,
Номер
8(5), С. 4064 - 4081
Опубликована: Март 28, 2018
H2O2
is
a
valuable,
environmentally
friendly
oxidizing
agent
with
wide
range
of
uses
from
the
provision
clean
water
to
synthesis
valuable
chemicals.
The
on-site
electrolytic
production
would
bring
chemical
applications
beyond
its
present
reach.
successful
commercialization
electrochemical
requires
cathode
catalysts
high
activity,
selectivity,
and
stability.
In
this
Perspective,
we
highlight
our
current
understanding
factors
that
control
performance.
We
review
influence
catalyst
material,
electrolyte,
structure
interface
at
mesoscopic
scale.
provide
original
theoretical
data
on
role
geometry
active
site
activity
selectivity.
have
also
conducted
series
experiments
(i)
effect
pH
glassy
carbon,
pure
metals,
metal–mercury
alloys,
(ii)
cell
mass
transport
in
liquid
half-cells
comparison
membrane
electrode
assemblies.
Science,
Год журнала:
2020,
Номер
367(6474), С. 193 - 197
Опубликована: Янв. 10, 2020
Confining
peroxide
to
make
methanol
In
principle,
hydrogen
would
be
an
efficient
oxidant
for
the
conversion
of
methane
under
mild
conditions.
practice,
however,
it
is
currently
too
expensive
produce
ahead
time
this
purpose.
Jin
et
al.
report
a
catalyst
system
that
generates
and
concentrates
immediate
reaction
with
methane.
A
hydrophobically
coated
zeolite
keeps
close
gold
palladium
active
site,
where
incoming
then
selectively
oxidized
methanol.
Science
,
issue
p.
193
Chemical Reviews,
Год журнала:
2020,
Номер
121(2), С. 882 - 961
Опубликована: Сен. 28, 2020
During
the
last
decades,
X-ray
absorption
spectroscopy
(XAS)
has
become
an
indispensable
method
for
probing
structure
and
composition
of
heterogeneous
catalysts,
revealing
nature
active
sites
establishing
links
between
structural
motifs
in
a
catalyst,
local
electronic
structure,
catalytic
properties.
Here
we
discuss
fundamental
principles
XAS
describe
progress
instrumentation
data
analysis
approaches
undertaken
deciphering
near
edge
(XANES)
extended
fine
(EXAFS)
spectra.
Recent
usages
field
catalysis,
with
emphasis
on
examples
concerning
electrocatalysis,
will
be
presented.
The
latter
is
rapidly
developing
immense
industrial
applications
but
also
unique
challenges
terms
experimental
characterization
restrictions
advanced
modeling
required.
This
review
highlight
new
insight
that
can
gained
complex
real-world
electrocatalysts
including
their
working
mechanisms
dynamic
processes
taking
place
course
chemical
reaction.
More
specifically,
situ
operando
to
probe
catalyst’s
interactions
environment
(support,
electrolyte,
ligands,
adsorbates,
reaction
products,
intermediates)
its
structural,
chemical,
transformations
as
it
adapts
conditions.
Chemical Reviews,
Год журнала:
2020,
Номер
120(8), С. 3890 - 3938
Опубликована: Март 30, 2020
In
this
review,
we
discuss
selected
examples
from
recent
literature
on
the
role
of
support
directing
nanostructures
Au-based
monometallic
and
bimetallic
nanoparticles.
The
is
then
discussed
in
relation
to
catalytic
properties
nanoparticles
using
different
gas
phase
liquid
reactions.
reactions
include
CO
oxidation,
aerobic
oxidation
monohydric
polyhydric
alcohols,
selective
hydrogenation
alkynes,
nitroaromatics,
CO2
hydrogenation,
C-C
coupling,
methane
oxidation.
Only
studies
where
has
been
explicitly
studied
detail
have
for
discussion.
However,
also
examined
involving
unsupported
metal
(i.e.,
colloidal
nanoparticles).
It
clear
that
functionality
can
play
a
crucial
tuning
activity
observed
advanced
theory
characterization
add
greatly
our
understanding
these
fascinating
catalysts.
Advanced Powder Materials,
Год журнала:
2021,
Номер
1(1), С. 100013 - 100013
Опубликована: Ноя. 15, 2021
Various
metal-based
electrocatalysts
from
nanocrystals,
to
clusters
and
single-atoms,
have
been
well-discovered
towards
high-efficient
power
devices
electrocatalytic
conversion.
To
accelerate
energy
transformation
materials
discovery,
developing
high-throughput
DFT
calculations
machine-learning
techniques
is
of
great
necessity.
This
review
comprehensively
outlines
the
latest
progress
theory-guided
design
advanced
materials.
Especially,
we
focus
on
study
single
atoms
in
various
devices,
such
as
fuel
cell
(oxygen
reduction
reaction,
ORR;
acid
oxidation
reaction;
alcohol
reaction),
other
reactions
for
energy-related
conversion
small
molecules,
H2O2
evolution
(2e−
ORR),
water
splitting
(H2
reaction/O2
HER/OER),
N2
reaction
(NRR),
CO2
(CO2RR).
Firstly,
electronic
structure,
interaction
mechanism,
activation
path
are
discussed
provide
an
overall
blueprint
electrocatalysis
batteries
mentioned
above.
Thereafter,
experimental
synthesis
strategies,
structural
recognition,
performance
figured
out.
Finally,
some
viewpoints
into
current
issues
future
concept
provided.
Angewandte Chemie International Edition,
Год журнала:
2019,
Номер
58(49), С. 17528 - 17551
Опубликована: Март 2, 2019
Abstract
Catalytic
C
1
chemistry
based
on
the
activation/conversion
of
synthesis
gas
(CO+H
2
),
methane,
carbon
dioxide,
and
methanol
offers
great
potential
for
sustainable
development
hydrocarbon
fuels
to
replace
oil,
coal,
natural
gas.
Traditional
thermal
catalytic
processes
used
transformations
require
high
temperatures
pressures,
thereby
carrying
a
significant
footprint.
In
comparison,
solar‐driven
catalysis
greener
more
pathway
manufacturing
other
commodity
chemicals,
although
conversion
efficiencies
are
currently
too
low
justify
industry
investment.
this
Review,
we
highlight
recent
advances
milestones
in
light‐driven
chemistry,
including
solar
Fischer–Tropsch
synthesis,
water‐gas‐shift
reaction,
CO
hydrogenation,
as
well
methane
reactions.
Particular
emphasis
is
placed
rational
design
catalysts,
structure–reactivity
relationships,
reaction
mechanisms.
Strategies
scaling
up
also
discussed.
Journal of the American Chemical Society,
Год журнала:
2019,
Номер
141(51), С. 20507 - 20515
Опубликована: Дек. 13, 2019
Direct
conversion
of
methane
into
methanol
and
other
liquid
oxygenates
still
confronts
considerable
challenges
in
activating
the
first
C-H
bond
inhibiting
overoxidation.
Here,
we
report
that
ZnO
loaded
with
appropriate
cocatalysts
(Pt,
Pd,
Au,
or
Ag)
enables
direct
oxidation
to
formaldehyde
water
using
only
molecular
oxygen
as
oxidant
under
mild
light
irradiation
at
room
temperature.
Up
250
micromoles
∼95%
selectivity
is
achieved
for
2
h
over
10
mg
0.1
wt
%
Au.
Experiments
isotopically
labeled
reveal
O2,
rather
than
water,
source
CH4
oxidation.
We
find
cocatalyst
could
concertedly
activate
O2
methyl
radical
mildly
oxidative
intermediate
(hydroperoxyl
radical)
which
are
two
key
precursor
intermediates
generating
oxygenated
products
Our
study
underlines
equally
significant
aspects
realizing
selective
photooxidation
oxygenates,
i.e.,
efficient
activation
controllable
O2.
