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Insitute of Physical Chemistry Polish Academy of Sciences. Laboratory research on aqueous reactions of isoprene with inorganic radicals. Inna Kuznietsova Lech Gmachowski, Krzysztof J. Rudzinski. Why ?. interaction and transformation of atmospheric trace compounds

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laboratory research on aqueous reactions of isoprene with inorganic radicals

Insitute of Physical Chemistry

Polish Academy of Sciences

Laboratory research on aqueous reactions of isoprene with inorganic radicals

Inna Kuznietsova

Lech Gmachowski, Krzysztof J. Rudzinski

slide2
Why ?
  • interaction and transformation of atmospheric trace compounds
  • formation of secondary organic aerosols

(SOA)

slide3
SO2
  • anthropogenic sources (80 TgS/year)

combustion of fossil fuels

vehicles, aircraft, ships,

power stations, industrial boilers

industry

ores smelting, scrubbing natural gas

  • natural sources (12 TgS/year)

volcanic eruptions

oxidation of organic materials in soils

atmospheric oxidation of dimethylsulfide

rainforests

autooxidation of s iv

SO2 + H2O

SO32- / HSO3-

Mn(III)

SIV, O2

Mn(II)

Mn(II) + SO3  -

Mn(III) + SO32-/HSO3-

SO3•-,SO4•- , SO5•-

2 SO32- /2 HSO3- + O2

2 SO42- /2 HSO42-

Autooxidation of SIV
isoprene
Isoprene

(2-methyl-1,3-butadien)

Sources:

  • Plants
  • Sea phytoplankton
  • Microbes
  • Animals and humans
  • Biomass burning
  • Combustion and evaporation of fuels
  • Cigarette smoking
  • Chemical technology
importance of isoprene
Importance of isoprene
  • Emission 500 TgC/year
  • High reactivity (OH•, NO3•, O3)
  • Precursor of Secondary Organic Aerosols
  • Influence on formation photochemical smog
  • Influence on autooxidation SIV
gas phase transformations of isoprene

•OH

NO3•

R•, O3

NO

R•

Cl•

SO3•

(....)

Gas-phase transformations of isoprene
typical gas phase products
Typical gas-phase products

aldehydes

ketones

3-methyl furan

diols

hydroxynitrates

dinitrates

peroxynitrates

peroxyacetyl nitrates (PAN)

methacrolyl nitrate (MPAN)

heterogeneous and aqueous phase transformations of isoprene
Heterogeneous and aqueous-phase transformations of isoprene

hydroxyacetons

2-methyltetraols

hydroxycarboxyl acids

dicarboxy acids

sulfate-nitrate esters

sulfate esters

nitrate esters

keto acids

slide10

Na2SO3 + Na2S2O5 + O2

Isoprene

MnSO4

[O2],pH

ESI-MS

(offline)

[iso], [S(IV)]

UV

25 oC

pH = 4.5÷8.6

Experimental setup

wavelength nm

Initial concentrations, mM:

MnSO4 SIV C5H8 O2 pH

0.01 1.04 0.07 0.25 6.7

Time, substrates

Time, products

Recorded UV spectra of a reacting solution

Wavelength, nm

Absorbance, a.u.

slide14

Identification of products

Intensity, cps

Mass / charge

slide17

Influence of isoprene on autooxidation of SIV

in solution of different acidity

2SO32- /2HSO3-+ O2

2SO42- /2HSO42-

experiments without isoprene (blue) and with isoprene (red)

Rudziński et.al.2007 Proc. 6th Conf. Urban Air Quality, Cyprus

take home messages
Take-Home-Messages
  • Aqueous-phase reactions of isoprene with sulfoxy radicals can be a source of atmospheric organosulfates and organosulfites
  • Influence of isoprene on aciditification of atmospheric waters
  • Interaction of biosphere and atmosphere
slide19
Thank you

for your attention

slide20

7

1

S2O82– → SO4•– + SO4•–

SO52– + SO32– → SO42– + SO42–

7a

2

HSO5– + HSO3– → SO42– + SO42– + 2 H+

Mn(II) (+ O2, S(IV))→ Mn(III)

8-1

SO5•– + Mn(II) → SO52– + Mn(III)

Mn(III) + SO32– → Mn(II) + SO3•–

3

8-2

SO5•– + Mn(II) → SO42– + Mn(III) (+ OH–)

4

SO3•– + O2 → SO5•–

9

SO5•– + SO32– → SO52– + SO3•–

SO4•– + Mn(II) → SO42– + Mn(III)

5-1

5-2

SO5•– + SO32– → SO42– + SO4•–

SO5•– + SO5•– → SO4•– + SO4•– + O2

10

5-1a

SO5•– + HSO3– → HSO5– + SO3•–

11

SO4•– + S2O82– → SO42– + S2O8•–

12

SO3•– + SO3•– → S2O62–

SO5•– + HSO3– → SO42– + SO4•– + H+

5-2a

13

SO4•– + SO32– → SO42– + SO3•–

SO4•– + SO4•– → S2O82–

6

14

SO5•– + SO5•– → S2O82– + O2

6a

SO4•– + HSO3– → SO42– + SO3•– + H+

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