Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(28), С. 19489 - 19498
Опубликована: Июль 8, 2024
High
oxidation
state
metal
cations
in
the
form
of
oxides,
oxoanions,
or
oxoperoxoanions
have
diverse
roles
carbon
dioxide
removal
(direct
air
capture
and
point
source).
Features
include
providing
basic
oxygens
for
chemisorption
reactions,
direct
binding
carbonate,
catalyzing
low-temperature
CO
ACS Environmental Au,
Год журнала:
2023,
Номер
3(5), С. 295 - 307
Опубликована: Июнь 29, 2023
Rising
CO2
emissions
are
responsible
for
increasing
global
temperatures
causing
climate
change.
Significant
efforts
underway
to
develop
amine-based
sorbents
directly
capture
from
air
(called
direct
(DAC))
combat
the
effects
of
However,
sorbents'
performances
have
usually
been
evaluated
at
ambient
(25
°C)
or
higher,
most
often
under
dry
conditions.
A
significant
portion
natural
environment
where
DAC
plants
can
be
deployed
experiences
below
25
°C,
and
always
contains
some
humidity.
In
this
study,
we
assess
adsorption
behavior
amine
(poly(ethyleneimine)
(PEI)
tetraethylenepentamine
(TEPA))
impregnated
into
porous
alumina
cold
(−20
humid
capacities
°C
400
ppm
highest
40
wt%
TEPA-incorporated
γ-Al2O3
samples
(1.8
mmol
CO2/g
sorbent),
while
wt
%
PEI-impregnated
exhibit
moderate
uptakes
(0.9
g–1).
both
PEI-
decrease
with
decreasing
content
temperatures.
The
20
TEPA
show
best
performance
−20
conditions
(1.6
1.1
g–1,
respectively).
Both
also
stable
high
working
1.2
g–1)
across
10
cycles
adsorption–desorption
(adsorption
desorption
conducted
60
°C).
Introducing
moisture
(70%
RH
improves
capacity
amine-impregnated
PEI,
TEPA,
good
results
presented
here
indicate
that
PEI
potential
materials
conditions,
further
opportunities
optimize
these
scalable
deployment
different
environmental
Energy & Environmental Science,
Год журнала:
2024,
Номер
17(13), С. 4544 - 4559
Опубликована: Янв. 1, 2024
A
direct
air
capture
(DAC)
economic
model
that
accounts
for
sorbent
degradation
is
developed.
Experimentally-measured
parameters
are
then
integrated
to
identify
and
process
features
minimize
both
the
DAC
carbon
footprint
cost.
JACS Au,
Год журнала:
2024,
Номер
4(5), С. 1883 - 1891
Опубликована: Май 1, 2024
The
cost
and
efficiency
of
direct
air
capture
(DAC)
carbon
dioxide
(CO2)
will
be
decisive
in
determining
whether
this
technology
can
play
a
large
role
decarbonization.
To
probe
the
meteorological
conditions
on
DAC
we
examine,
at
1
×
1°
resolution
for
continental
United
States
(U.S.),
impacts
temperature,
humidity,
atmospheric
pressure,
CO2
concentration
representative
amine-based
adsorption
process.
Spatial
temporal
variations
pressure
lead
to
strong
available
ambient
across
U.S.
specific
process
that
examine
is
described
by
model
accounts
both
temperature
humidity.
A
assumes
same
operating
choices
all
locations
shows
performance,
with
most
influential
variables
being
H2O
gas
phase
volume
fraction
which
are
negatively
correlated
productivity
consider.
also
moderate
positive
correlation
recovery.
We
show
optimizing
seven
reflect
spatial
significantly
improves
performance
and,
more
importantly,
would
different
sites
best
than
models
based
single
set
conditions.
Our
work
provides
framework
assessing
could
applied
any
indicates
these
have
important
implications
siting
facilities.
Accounts of Chemical Research,
Год журнала:
2023,
Номер
56(19), С. 2620 - 2630
Опубликована: Сен. 18, 2023
ConspectusSolid-supported
amines
are
a
promising
class
of
CO2
sorbents
capable
selectively
capturing
from
diverse
sources.
The
chemical
interactions
between
the
amine
groups
and
give
rise
to
formation
strong
adducts,
such
as
alkylammonium
carbamates,
carbamic
acids,
bicarbonates,
which
enable
capture
even
at
low
driving
force,
with
ultradilute
streams.
Among
various
solid-supported
sorbents,
oligomeric
infused
into
oxide
solid
supports
(noncovalently
supported)
widely
studied
due
their
ease
synthesis
cost.
This
method
allows
for
construction
amine-rich
while
minimizing
problems,
leaching
or
evaporation,
that
occur
supported
molecular
amines.Researchers
have
pursued
improved
by
tuning
physical
properties
phases.
In
terms
uptake,
efficiency,
moles
sorbed
per
mole
sites,
uptake
rate
(CO2
unit
time)
most
critical
factors
determining
effectiveness
material.
While
structure–property
relationships
been
developed
different
porous
supports,
interaction(s)
phase
support,
structure
distribution
organic
within
pores,
mobility
pores
not
well
understood.
These
important,
because
kinetics
sorption,
particularly
when
using
prototypical
oligomer
branched
poly(ethylenimine)
(PEI),
follow
an
unconventional
trend,
rapid
initial
followed
very
slow,
asymptotic
approach
equilibrium.
suggests
is
mass
transfer-limited.
Therefore,
improving
sorption
performance
can
be
facilitated
better
understanding
pores.In
this
context,
model
were
constructed
highly
ordered,
mesoporous
silica
SBA-15
array
techniques
was
used
probe
soft
matter
domains
these
hybrid
materials.
choice
support
based
on
its
ordered
arrangement
mesopores
tunable
properties,
including
pore
size,
particle
lengths,
surface
chemistries.
Branched
PEI─the
common
in
sorbents─and
linear,
weight
analogue,
tetraethylenepentamine
(TEPA),
deployed
Neutron
scattering
(NS),
small
angle
neutron
(SANS)
quasielastic
(QENS),
alongside
solid-state
NMR
(ssNMR)
dynamics
(MD)
simulations,
elucidate
phases
support.
Together,
tools,
previously
applied
materials,
provided
new
information
regarding
how
filled
loading
increased
those
Varying
surface-amine
led
unique
trends
distributions
mobility;
instance,
hydrophilic
walls
(i.e.,
attractive
amines)
resulted
hampered
motions
more
intimate
coordination
walls,
around
hydrophobic
grafted
chains
interrupt
amine-wall
showed
recovered
mobility,
being
liberated
walls.
By
correlating
structural
dynamic
novel
identified,
shedding
light
providing
valuable
guidance
design
effective
sorbents.