Abstract.
Clustering
of
gaseous
sulfuric
acid
(SA)
enhanced
by
dimethylamine
(DMA)
is
a
major
mechanism
for
new
particle
formation
(NPF)
in
polluted
atmospheres.
However,
uncertainty
remains
regarding
the
SA-DMA
nucleation
parameterization
that
reasonably
represents
cluster
dynamics
and
applicable
across
various
atmospheric
conditions.
This
hinders
accurate
three-dimensional
(3-D)
modeling
NPF
subsequent
assessment
its
environmental
climatic
impacts.
Here
we
extensively
compare
different
dynamics-based
parameterizations
identify
most
reliable
one
through
combination
box-model
simulations,
3-D
modeling,
in-situ
observations.
Results
show
derived
from
Atmospheric
Cluster
Dynamic
Code
(ACDC)
incorporating
latest
theoretical
insights
(DLPNO-CCSD(T)/aug-cc-pVTZ//ωB97X-D/6-311++G(3df,3pd)
level
theory)
adequate
representation
dynamics,
exhibits
dependable
performance
simulation
both
winter
summer
conditions
Beijing
shows
promise
application
diverse
Another
ACDC-derived
parameterization,
replacing
theory
with
RI-CC2/aug-cc-pV(T+d)Z//M06-2X/6–311++G(3df,3pd),
also
performs
well
at
relatively
low
temperatures
around
280
K
but
limitations
higher
due
to
inappropriate
thermodynamics.
Additionally,
previously
reported
simplifications
simulating
atmospheres
tends
overestimate
rates
under
elevated
temperature
(>
~300
K)
condensation
sink
(<
~3×10-3
s-1).
Our
findings
highlight
applicability
which
couples
holistic
modeling.
The
framework
provides
valuable
reference
developing
other
systems.
Photochemical & Photobiological Sciences,
Journal Year:
2022,
Volume and Issue:
21(3), P. 275 - 301
Published: Feb. 21, 2022
Abstract
The
Environmental
Effects
Assessment
Panel
of
the
Montreal
Protocol
under
United
Nations
Environment
Programme
evaluates
effects
on
environment
and
human
health
that
arise
from
changes
in
stratospheric
ozone
layer
concomitant
variations
ultraviolet
(UV)
radiation
at
Earth’s
surface.
current
update
is
based
scientific
advances
have
accumulated
since
our
last
assessment
(Photochem
Photobiol
Sci
20(1):1–67,
2021).
We
also
discuss
how
climate
change
affects
depletion
radiation,
change.
resulting
interlinking
depletion,
UV
are
assessed
terms
air
quality,
carbon
sinks,
ecosystems,
health,
natural
synthetic
materials.
further
highlight
potential
impacts
biosphere
extreme
events
occurring
with
increasing
frequency
as
a
consequence
These
other
interactive
examined
respect
to
benefits
its
Amendments
providing
life
Earth
by
controlling
production
various
substances
contribute
both
Environmental Science & Technology,
Journal Year:
2023,
Volume and Issue:
57(17), P. 6944 - 6954
Published: April 21, 2023
Iodic
acid
(IA)
has
recently
been
recognized
as
a
key
driver
for
new
particle
formation
(NPF)
in
marine
atmospheres.
However,
the
knowledge
of
which
atmospheric
vapors
can
enhance
IA-induced
NPF
remains
limited.
The
unique
halogen
bond
(XB)-forming
capacity
IA
makes
it
difficult
to
evaluate
enhancing
potential
(EP)
target
compounds
on
based
widely
studied
sulfuric
systems.
Herein,
we
employed
three-step
procedure
EP
nucleation
precursors
NPF.
First,
evaluated
63
by
simulating
free
energies
(ΔG)
IA-containing
dimer
clusters.
Among
all
clusters,
44
contained
XBs,
demonstrating
that
XBs
are
frequently
formed.
Based
calculated
ΔG
values,
quantitative
structure–activity
relationship
model
was
developed
evaluating
other
precursors.
Second,
amines
and
O/S-atom-containing
acids
were
found
have
high
EP,
with
diethylamine
(DEA)
yielding
highest
combining
both
concentration
considered
Finally,
studying
larger
(IA)1–3(DEA)1–3
IA-DEA
system
merely
0.1
ppt
(2.5×106
cm–3)
DEA
yields
comparable
rates
IA–iodous
system.
Photochemical & Photobiological Sciences,
Journal Year:
2024,
Volume and Issue:
23(6), P. 1087 - 1115
Published: May 19, 2024
Abstract
The
protection
of
Earth’s
stratospheric
ozone
(O
3
)
is
an
ongoing
process
under
the
auspices
universally
ratified
Montreal
Protocol
and
its
Amendments
adjustments.
A
critical
part
this
assessment
environmental
issues
related
to
changes
in
O
.
United
Nations
Environment
Programme’s
Environmental
Effects
Assessment
Panel
provides
annual
scientific
evaluations
some
key
arising
recent
collective
knowledge
base.
This
current
update
includes
a
comprehensive
incidence
rates
skin
cancer,
cataract
other
eye
diseases
observed
worldwide;
effects
UV
radiation
on
tropospheric
oxidants,
air
water
quality;
trends
breakdown
products
fluorinated
chemicals
information
their
toxicity;
technological
innovations
building
materials
for
greater
resistance
radiation.
These
span
wide
range
topics,
including
both
harmful
beneficial
exposure
radiation,
complex
interactions
with
climate
change.
While
has
succeeded
preventing
large
reductions
,
future
may
occur
due
number
natural
anthropogenic
factors.
Thus,
frequent
assessments
potential
impacts
are
essential
ensure
that
policies
remain
based
best
available
knowledge.
Graphical
abstract
Environmental Science & Technology,
Journal Year:
2024,
Volume and Issue:
58(45), P. 19925 - 19935
Published: Oct. 30, 2024
Trifluoroacetic
acid
(TFA)
is
a
persistent
and
mobile
substance
that
has
been
increasing
in
concentration
within
diverse
environmental
media,
including
rain,
soils,
human
serum,
plants,
plant-based
foods,
drinking
water.
Currently,
TFA
concentrations
are
orders
of
magnitude
higher
than
those
other
per-
polyfluoroalkyl
substances
(PFAS).
This
accumulation
due
to
many
PFAS
having
as
transformation
product,
several
fluorinated
gases
(F-gases),
pesticides,
pharmaceuticals,
industrial
chemicals,
addition
direct
release
industrially
produced
TFA.
Due
TFA's
extreme
persistence
ongoing
emissions,
irreversibly.
What
remains
less
clear
the
thresholds
where
irreversible
effects
on
local
or
global
scales
occur.
There
indications
from
mammalian
toxicity
studies
toxic
reproduction
it
exhibits
liver
toxicity.
Ecotoxicity
data
scarce,
with
most
being
for
aquatic
systems;
fewer
available
terrestrial
bioaccumulates
readily.
Collectively,
these
trends
imply
meets
criteria
planetary
boundary
threat
novel
entities
because
planetary-scale
exposure,
potential
disruptive
impacts
vital
earth
system
processes
could
The
rational
response
this
instigate
binding
actions
reduce
emissions
its
precursors.
Proceedings of the National Academy of Sciences,
Journal Year:
2021,
Volume and Issue:
118(35)
Published: Aug. 27, 2021
Recent
research
[Wang
et
al.,
Nature
581,
184-189
(2020)]
indicates
nitric
acid
(NA)
can
participate
in
sulfuric
(SA)-ammonia
(NH3)
nucleation
the
clean
and
cold
upper
free
troposphere,
whereas
NA
exhibits
no
obvious
effects
at
boundary
layer
with
relatively
high
temperatures.
Herein,
considering
that
an
SA-dimethylamine
(DMA)
mechanism
was
detected
megacities
[Yao
Science
361,
278-281
(2018)],
roles
of
SA-DMA
are
investigated.
Different
from
SA-NH3
nucleation,
we
found
enhance
SA-DMA-based
particle
formation
rates
polluted
atmospheric
layer,
such
as
Beijing
winter,
enhancement
up
to
80-fold.
Moreover,
promote
number
concentrations
clusters
(up
27-fold)
contribute
76%
cluster
pathways
280
K.
The
enhancements
on
by
critical
for
particulate
pollution
DMA
concentrations.
Atmospheric chemistry and physics,
Journal Year:
2025,
Volume and Issue:
25(5), P. 2829 - 2844
Published: March 7, 2025
Abstract.
Sulfamic
acid
(SFA)
significantly
impacts
atmospheric
pollution
and
poses
potential
risks
to
human
health.
Although
traditional
sources
of
SFA
their
role
in
sulfuric
acid–dimethylamine
new
particle
formation
(NPF)
have
received
increasing
attention,
the
mechanism
from
HNSO2
hydrolysis
with
methanesulfonic
(MSA)
its
enhancing
effect
on
MSA-methylamine
(MA)
NPF
not
been
studied,
which
will
limit
understanding
source
loss
agriculture-developed
coastal
industrial
areas.
Here,
gaseous
interfacial
MSA
was
investigated
using
quantum
chemical
calculations
Born–Oppenheimer
molecular
dynamics
(BOMD)
simulations.
Furthermore,
MSA-MA
system
assessed
Atmospheric
Cluster
Dynamic
Code
(ACDC)
kinetic
model.
Our
simulation
results
indicate
that
can
be
competitive
catalyzed
by
H2O
within
an
altitude
5–15
km.
At
air–water
interface,
two
types
reactions,
ion-forming
proton
exchange
form
SFA−
…
H3O+
ion
pair,
were
observed
timescale
picoseconds.
Considering
overall
environment
emission
reduction,
present
findings
suggest
may
play
a
significant
growth
aerosol
particles,
as
(i)
directly
participate
MSA-MA-based
clusters
enhance
rate
these
approximately
103
times
at
278.15
K
(ii)
species
interface
attract
molecules
aqueous
surface
thus
promote
growth.
Atmospheric chemistry and physics,
Journal Year:
2024,
Volume and Issue:
24(7), P. 4029 - 4046
Published: April 4, 2024
Abstract.
The
reactions
between
SO3
and
atmospheric
acids
are
indispensable
in
improving
the
formation
of
aerosol
particles.
However,
relative
to
those
with
organic
acids,
reaction
inorganic
has
not
received
much
attention.
Here,
we
explore
H2SO4,
a
typical
acid,
gas
phase
at
air–water
interface
using
quantum
chemical
(QC)
calculations
Born–Oppenheimer
molecular
dynamics
simulations.
We
also
report
effect
H2S2O7,
product
on
new
particle
(NPF)
various
environments
Atmospheric
Cluster
Dynamics
Code
(ACDC)
kinetic
model
QC
calculations.
present
findings
show
that
gas-phase
+
H2SO4
without
water
molecules
both
low-energy-barrier
processes.
With
involvement
interfacial
molecules,
H2O
induced
S2O72-⋯H3O+
ion
pair,
HSO4-
mediated
HSO4-⋯H3O+
deprotonation
H2S2O7
was
observed
proceeded
picosecond
timescale.
suggest
potential
contribution
SO3–H2SO4
NPF
growth,
showing
(i)
although
is
easily
hydrolyzed
form
it
can
directly
participate
H2SO4–NH3-based
cluster
more
obvious
enhancement
SA–A-based
formation,
(ii)
formed
S2O72-
attract
candidate
species
from
surface
and,
thus,
accelerate
growth.
Atmospheric chemistry and physics,
Journal Year:
2022,
Volume and Issue:
22(3), P. 1951 - 1963
Published: Feb. 11, 2022
Abstract.
The
role
of
pyruvic
acid
(PA),
one
the
most
abundant
α-keto
carboxylic
acids
in
atmosphere,
was
investigated
both
SO3
hydrolysis
reaction
to
form
sulfuric
(SA)
and
SA-based
aerosol
particle
formation
using
quantum
chemical
calculations
a
cluster
dynamics
model.
We
found
that
PA-catalyzed
is
thermodynamically
driven
transformation
process,
proceeding
with
negative
Gibbs
free-energy
barrier,
ca.
−1
kcal
mol−1
at
298
K,
∼
6.50
lower
than
water-catalyzed
hydrolysis.
Results
indicated
can
potentially
compete
SA
production,
especially
dry
polluted
areas,
where
it
be
2
orders
magnitude
more
efficient
reaction.
Given
effective
stabilization
product
as
SA⚫PA
cluster,
we
proceeded
examine
PA
clustering
efficiency
sulfuric-acid–pyruvic-acid–ammonia
(SA-PA-NH3)
system.
Our
thermodynamic
data
used
Atmospheric
Cluster
Dynamics
Code
under
relevant
tropospheric
temperatures
concentrations
(106
molec.cm-3),
(1010
molec.cm-3)
NH3
(1011
5
×
1011
PA-enhanced
involves
clusters
containing
molecule.
Namely,
these
monomer
238
(SA)2⚫PA⚫(NH3)2
contribute
by
100
%
net
flux
formation.
At
higher
(258
278
K),
however,
dominated
pure
SA-NH3
clusters,
while
would
rather
evaporate
from
high
not
enhancing
effect
examined
evaluating
ratio
ternary
SA-PA-NH3
rate
binary
rate.
results
show
enhancement
factor
almost
insensitive
concentrations,
4.7
102
K
[NH3]
=
1.3
molec.cm-3.
This
indicates
may
actively
participate
formation,
only
cold
regions
troposphere
highly
NH3-polluted
environments.
inclusion
this
mechanism
models
reduce
uncertainties
prevail
modeling
impact
on
climate.