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Anthropogenic and biogenic influences on the oxidising capacity of the atmosphere

Research project EV/06 (Research action EV)


Persons :

  • Dr.  MÜLLER Jean-François - Royal Belgian Institute for Space Aeronomy (IASB-BIRA)
    Financed belgian partner
    Duration: 1/12/2000-28/2/2005
  • Prof. dr.  ARIJS Etienne - Royal Belgian Institute for Space Aeronomy (IASB-BIRA)
    Financed belgian partner
    Duration: 1/12/2000-28/2/2005
  • Prof. dr.  VINCKIER Chris - Katholieke Universiteit Leuven (K.U.Leuven)
    Financed belgian partner
    Duration: 1/12/2000-28/2/2005
  • Prof. dr.  PEETERS Jozef - Katholieke Universiteit Leuven (K.U.Leuven)
    Financed belgian partner
    Duration: 1/12/2000-28/2/2005

Description :

The composition of the troposphere is strongly affected by biogenic and anthropogenic emissions of chemical compounds, including hydrocarbons, carbon monoxide, and the nitrogen oxides. The emissions of non-methane hydrocarbons, in particular, have a large impact on the oxidizing capacity of the atmosphere (which determines the fate and lifetime of a large number of pollutants and greenhouse gases) and on the budget and distribution of tropospheric ozone and aerosols. In this project, we propose specifically to study their impact on the formation of oxidants (including the hydroxyl radical OH) and aerosols on the global scale. Laboratory data and theoretical results quantifying photochemical processes in the atmosphere will be integrated in chemistry/transport models of the global troposphere. These models simulate the distribution of key important compounds, including ozone and its precursors.

The first goal of this project is to reduce uncertainties in the processes (emissions, chemistry) that determine the global distribution of tropospheric constituents. For this purpose, a number of chemical and photochemical mechanisms which have been identified from model calculations to be potentially important will be studied though concerted laboratory, theoretical and modelling investigations. The degradation mechanisms of selected non-methane hydrocarbons will be established, and the potential formation of long-lived intermediates, including aerosols, will be identified. A special care will be devoted to the quantification of the remaining uncertainties in the emissions and atmospheric degradation of these compounds.

A second goal of the project is to quantify the impact of non-methane hydrocarbons on the oxidizing capacity of the atmosphere and on the chemistry of ozone in the upper troposphere. This region is of particular interest in the context of global change, because the injection of anthropogenic pollutants at these altitudes (through aircraft emissions or deep convection of polluted air) is known to have a strong influence on the budget of radicals and hence, ozone. For this purpose, a well-established chemical/transport model, which calculates the global climatological distributions of chemical constituents, the IMAGES model, will be used.

The third goal of the project is to determine the influence of human activity on the chemical composition and the oxidizing capacity of the atmosphere. For this purpose, scenarios accounting for future changes in population, energy consumption, changes in land-use, etc. will be introduced in the global model, in order to predict the possible future evolution of the atmospheric composition.

These assessment studies should help understanding the impact of global pollution on climate forcing and on the biosphere. They should provide to decision-makers indispensable scientific information that will contribute to ensure sustainable development.


Methodology

- use of the fast-flow reactor technique for the simulation of atmospheric chemistry processes at a laboratory scale;
- development and application of new analytical techniques for the determination of the terpenes oxidation products;
- development and application of theoretical techniques (quantum calculations, Structure-Activity Relationships, etc.) for the determination of the terpenes oxidation products, including aerosols;
- development of a comprehensive chemical mechanism for the oxidation of terpenes in atmospheric conditions, and validation of this mechanism by confrontation with laboratory results;
- determination of the global emissions of biogenic hydrocarbons, and investigation of their uncertainties.


Interactions between the different partners

- close collaboration between the teams of C. Vinckier (KULeuven) and E. Arijs (BIRA-IASB) for the application of the fast-flow reactor technique to the terpenes oxidation ;
- close collaboration between the teams of J.-F. Müller (IASB-BIRA) and J. Peeters (KULeuven) for the development and validation of the terpenes oxidation mechanism ;
- the mechanistic data obtained from the laboratory and theoretical studies will be integrated in a chemical model of the troposphere by the team of J. -F. Müller in order to determine their impact on the tropospheric composition.


Link with international programmes:

- EUROTRAC2 : contributions of the KULeuven teams to the subproject CMD (Chemical Mechanism Development) ;
- IPCC (Intergovernmental Panel on Climate Change) : contribution of J .-F. Müller to e.g. the 3d Assessment Report IPCC/TAR ;
- Integration in European research networks of the 5th Framework Programme.

Expected results

- new laboratory and theoretical techniques for investigating the oxidation of biogenic hydrocarbons (monoterpenes);
- new comprehensive mechanisms representing the oxidation of several important biogenic hydrocarbons (monoterpenes) in laboratory as well as in atmospheric conditions;
- better assessment of the role of these hydrocarbons on the global troposphere, in particular regarding the production of aerosols;
- better assessment of the impact of anthropogenic emissions on the composition of the global troposphere.

Partners

Activities

The groups of Vinckier and Arijs conduct laboratory studies of the oxidation of several monoterpenes by OH in the presence of NO. They benefit from the experience gained by Vinckier’s team during the previous PODO program. In addition, Arijs and Peeters’s teams investigate other selected organic reactions.

The groups of Peeters and Müller combine theoretical and modelling studies in order to construct an oxidation mechanism for monoterpenes in general conditions. Peeters’s team focuses on the gas-phase reaction steps, while Müller’s group works at their integration in a model that includes gas/particle-partitioning effects. The latter group also assesses the biogenic emissions as well as global impacts using a 3-dimensional chemical model.


Coordinates/Details

Project co-ordinator:

Jean-François Müller
Belgian Institute for Space Aeronomy (BIRA-IASB)
Avenue Circulaire 3, B-1180 Brussels
Tel: +32 (0)2 373 04 86; Fax: +32 (0)2 374 84 23
jfm@bira-iasb.oma.be

Project partners:
Jozef Peeters
Katholieke Universiteit Leuven - Chemistry Department
Celestijnenlaan 200F, B-3001 Heverlee
Tel: +32 (0)16 32 73 82; Fax: +32 (0)16 32 79 92
jozef.peeters@chem.kuleuven.ac.be

Christiaan Vinckier
Katholieke Universiteit Leuven - Chemistry Department
Celestijnenlaan 200F, B-3001 Heverlee
Tel: +32 (0)16 32 73 76; Fax: +32 (0)16 32 79 92
chris.vinckier@chem.kuleuven.ac.be

Etienne Arijs
Belgian Institute for Space Aeronomy (BIRA-IASB)
Ringlaan 3, B-1180 Brussels
Tel: +32 (0)2 373 04 76; Fax: +32 (0)2 374 84 23
earijs@bira-iasb.oma.be


Users Committee

Bob Nieuwejaers - AMINAL

Alex Guenther - National Center for Atmospheric Research

Guy Brasseur - Max-Planck-Institut für Meteorologie

Ulrich Schurath - Institut für Meteorologie und Klimaforschung, FZK


Documentation :

Anthropogenic and biogenic influences on the oxidation capacity of the atmosphere : final report  Muller, J.-F. - Vinckier, C. - Peeters, J. ... et al  Brussels : Belgian Science Policy, 2005 (SP1515)
[To download]  [To order

Antropogene en biogene invloeden op de oxiderende capaciteit van de atmosfeer : samenvatting    Brussel : Federaal Wetenschapsbeleid, 2005 (SP1516)
[To download

Influences anthropiques et biogéniques sur la capacité d'oxydation de l'atmosphère : résumé    Bruxelles : Politique scientifique fédérale, 2005 (SP1517)
[To download

Anthropogenic and biogenic influences on the oxidation capacity of the atmosphere : summary    Brussels : Belgian Science Policy, 2005 (SP1518)
[To download

Bibliografic references :

1,3-Cycloaddition of Ozone tEthylene, Benzene and Phenol: a Comparative Ab InitiStudy  HENDRICKX M.F.A. AND C. VINCKIER J. Chem. Phys., A 107, 2003 

A generalised structure-activity relationship for the decomposition of (substituted) alkoxy radicals  J. Peeters, G. Fantechi, L. Vereecken  Journal of Atmospheric Chemistry, 48, 2004 

A group contribution method for estimating the vapor pressures of α-pinene oxidation products  Capouet M., Müller J.-F.A group contribution method for estimating the vapor pressures of α-pinene oxidation products Environ. Sci. Technol, (Submitted) 

A highly sensitive method for time-resolved detection of O(1D) applied to precise determination of absolute O(1D) reaction rate constants and O(3P) yields.  S.A. Carl  Physical Chemistry - Chemical Physics, 7, 2005 

A selected ion flow tube study of the reactions of H3O+, NO+ and O2+ with a series of monoterpenes  N. Schoon, C. Amelynck, L. Vereecken, E. Arijs  International Journal of Mass Spectrometry, 229, 2003 

A selected ion flow tube study of the reactions of H3O+, NO+ and O2+ with some monoterpene oxidation products  N. Schoon, C. Amelynck, L. Vereecken, H. Coeckelberghs, E. Arijs  International Journal of Mass Spectrometry, 239, 2004 

A selected ion flow tube study of the reactions of H3O+, NO+ and O2+ with some monoterpene oxidation products  Schoon N., Amelynck C., Vereecken L., Coeckelberghs H., Arijs E.  International Journal of Mass Spectrometry, 239, 2004 

A selected ion flow tube study of the reactions of H3O+, NO+ and O2+ with some oxygenated biogenic volatile organic compounds  Amelynck C., Schoon N., Kuppens T., Arijs E. International Journal of Mass Spectrometry, (Submitted) 

A selected ion flow tube study of the reactions of H3O+, NO+ and O2+ with methyl vinyl ketone and some atmospherically important aldehydes  Michel E International Journal of Mass Spectrometry, 244/1, 2005 

Alpha-pinene oxidation by OH: Simulations of laboratory experiments  Capouet, M., J. Peeters, B. Nozière, and J.-F. Müller Atmos. Chem. Phys. 4, 2004 

Alpha-pinene oxidation by OH: simulations of laboratory experiments  M. Capouet, J. Peeters, B. Nozière, J.-F. Müller  Atmospheric Chemistry and Physics, 4, 2005 

Alpha-pinene oxidation by OH: Simulations of laboratory experiments  Capouet, M., J. Peeters, B. Nozière, and J.-F. Müller Atmos. Chem. Phys. 4, 2004 

Alpha-pinene oxidation by OH: simulations of laboratory experiments  Capouet M., Peeters J., Nozière B., Müller J.-F. Atmospheric Chemistry and Physics, 4, 2004 

Anthropogenic and biogenic influences on the oxidising capacity of the atmosphere   J.-F. Muller, M. Capouet, S. Wallens, T. Stavrakou, Vinckier, J . Peeters, F. Compernolle, H. Vankerckhoven, V. Van Den Bergh, H. Coeckelberghs, L. Vereecken, G. Fantechi, I. Hermans, C. Coeck, T.L. Nguyen, P.A. Jacobs, E. Arijs,C. Amelynck, N. Schoon  final report, 2005 

Computational study of the stability of á-hydroperoxyl- or á-alkylperoxyl substituted alkyl radicals  L. Vereecken, T.L. Nguyen, I. Hermans, J. Peeters  Chemical Physics Letters, 393, 2004 

Determination of the oxidation products of the reaction between α-pinene and OH radicals by High Performance Liquid Chromatography  Vanhees I., Van den Bergh V., Schildermans R., De Boer R., Compernolle F. and Vinckier C. J. Chromat. A, 915, 2001 

Enhanced H-atom abstraction from pinonaldehyde, pinonic acid, pinic acid and related compounds: theoretical study of the C-H bond strengths  Vereecken L., J. Peeters J. Phys. Chem. Chem. Phys., 4, 2002 

Fresh air in the 21st century?   Prather M., Gauss M., Berntsen T., Isaksen I., Sundet J., Bey I., Brasseur G., Dentener F., Derwent R., Stevenson D., Lee Grenfell J., Hauglustaine D., Horowitz L., Jacob D., Mickley L., Lawrence M., von Kuhlmann M., Muller J.-F., Pitari G., Rogers H., va Geophys. Res. Lett., 1100, 2003 

Generation of Iron Atoms in the Gas Phase by a Microwave-Induced Plasma-Afterglow   VINCKIER C., K. CAPPAN Chem Phys Chem, 4, 2003 

H-Atom Abstraction by OH-Radicals from (Biogenic) (Poly)alkenes: CH bond strengths and abstraction rates  Vereecken L., Peeters J. Chem. Phys. Lett., 333, 2001 

HPLC-MS determination of the oxidation products of the reaction between a- and b-pinene and OH  Van den Bergh V., Coeckelberghs H., Vanhees I., DeBoer R., Compernolle F., Vinckier C. Anal. Bioanal. Chem., 372, 2002 

Inverse modeling of carbon monoxide surface emissions using CMDL network observations  Pétron G., Granier C., Khattatov B., Lamarque J.-F., Yudin V., Müller J.-F., Gille J. J. Geophys. Res., 107 (D24), 4761, doi:10.1029/2001JD001305, 2002 

Inverse modeling of ozone precursors using the adjoint model method  Müller J.-F., Stavrakou T. Proceedings IUGG meeting, Sapporo, Japan, 30/6-11/7, 2003 

Inversion of CO and NOx emissions using the adjoint of the IMAGES model  Müller J.-F., Stavrakou T. Atmospheric Chemistry and Physics, 5, 2005 

Kinetic Study in a Microwave Induced Plasma Afterglow of the Fe (a5D4) Reaction with NO2 from 303 t814 K  VINCKIER C. , K. CAPPAN Phys. Chem. Chem. Phys.,5, 2003 

Kinetics of alfa-hydroxy-alkylperoxyl radicals in oxidation processes. HO2-initiated oxidation of ketones/aldehydes near the tropopause
  I. Hermans, J.F. Müller, T.L. Nguyen, P.A. Jacobs, J. Peeters  The Journal of Physical Chemistry, A, 109, 2005 

Kinetics of alpha-hydroxy-alkylperoxyradicals in oxidation processes. HO2*-initiated oxidation of ketones/aldehydes near the tropopause  Hermans I., Müller J.-F., Nguyen T.L., Jacobs P.A., Peeters J. J. Phys. Chem. A., 109, 2005 

Modélisation des émissions de composes organiques volatils par la végétation. PhD Thesis, Université Libre de Bruxelles  Wallens, S. , 2004 

Multi-compound inverse modeling of emissions using the adjoint of the global CTM IMAGES  Müller J.-F., Stavrakou T. EGS-AGU Joint assembly, Nice, France, 2003 

Multi-model ensemble simulations of present-day and near-future tropospheric ozone, .   Stevenson D., and the IPCC-ACCENT modeling partners J. Geophys. Res., submitted 

Non-traditional (per)oxy ring-closure paths in the atmospheric oxidation of isoprene and monoterpenes  L. Vereecken, J. Peeters  The Journal of Physical Chemistry, A., 108, 2004 

Optimisation of surface emissions by inverse modeling  PETRON G., C. GRANIER, J.-F. MÜLLER, J. STAVRAKOU, POET POET, Report #4, EU project EVK2-1999-00011, 2003 

Photo-oxidation of alpha-pinene and its potential for aerosol production  CAPOUET M., G. FANTECHI, L. VEREECKEN, J. PEETERS, AND J.-F. MÜLLER EGS-AGU Joint assembly, Nice, France, 2003 

Photo-oxidation of alpha-pinene and its potential for aerosol production  CAPOUET, M., AND J.-F. MÜLLER Proceedings Organic Aerosol workshop, Belgirate, Italy, 2003 

Present and future surface emissions of atmospheric compounds  OLIVIER J. , J. PETERS, C. GRANIER, G. PETRON, J.-F. MÜLLER, S. WALLENS, POET POET, Report #2, EU project EVK2-1999-00011, 2003 

Product yield determination of the OH-initiated oxidation of monoterpenes  AMELYNCK C. , N. SCHOON AND E. ARIJS Oral presentation at the Belgische Natuurkundige Vereniging, Gent, 2003 

Radiative forcing in the 21st century due tozone changes in the troposphere and the lower stratosphere  Gauss M., Myhre G., Pitari G., Prather M., Isaksen I., Berntsen T., Brasseur G., Dentener F., Derwent R., Hauglustaine D., Horowitz L., Jacob D., Johnson M., Law K., Mickley L., Muller J.-F., Plantevin P.-H., Pyle J., Rogers H., Stevenson D., Sundet J., v Res., 108, 4292, doi: 10.1029/2002JD002426, 2003 

Simulations of the future composition of the atmosphere  MÜLLER J.F., C. GRANIER, U. NIEMEIER, J. OLIVIER, J. PETERS, POET POET, Report #9, EU project EVK2-1999-00011, 2003 

Study of the carbonyl products of terpene/OH radical reactions: detection of the 2,4-DNPH derivatives by HPLC-MS  Van den Bergh V., Coeckelberghs H., Vankerckhoven H., Compernolle F., Vinckier C.  Anal. Bioanal. Chem., 379, 2004 

The 1,5-H-shift in 1-butoxy: a case study in the rigorous implementation of Transition State Theory for multi-rotamer systems
  L. Vereecken, J. Peeters Journal of Chemical Physics, 119, 2003 

The Acetic-Acid forming Channel in the Acetone + OH Reaction: a Combined Experimental and Theoretical Investigation  Vandenberk S., Vereecken L., Peeters J. Phys. Chem. Chem. Phys., 4, 2002 

The Detailed Mechanism of the OH-Initiated Atmospheric Oxidation of α-pinene: A Theoretical Study  Peeters J., Vereecken L., Fantechi G. Phys. Chem. Chem. Phys., 3, 2001 

The OH-initiated atmospheric oxidation of pinonaldehyde: detailed theoretical study and mechanism construction  Fantechi G., Vereecken L., Peeters J. Phys. Chem. Chem. Phys., 4, 2002 

The OH-initiated oxidation of alpha-pinene: quantification of acetone, pinonaldehyde and formaldehyde yields using a combined NFFR/CIMS instrument  AMELYNCK C., N. SCHOON, J. RIONDATO AND E. ARIJS Geophysical Research Abstracts, Vol. 5, EGS-AGU-EUG Joint Assembly,Nice, France, 2003 

The reaction of acetaldehyde and propionaldehyde with hydroxyl radicals: experimental determination of the primary H2O yield at room temperature  S. Vandenberk, J. Peeters Journal of Photochemistry and Photobiology, 157, 2003 

Theoretical and experimental study of the product branching in the reaction of acetic acid with OH radicals  De Smedt F., Bui X. V., Nguyen T. L., Peeters J., Vereecken L. J. Phys. Chem. A, 109, 2005 

Theoretical and experimental study of the product branching in the reaction of acetic acid with OH radicals.  F. De Smedt, X. V. Bui, T. L. Nguyen, J. Peeters, L. Vereecken  The Journal of Physical Chemistry A, 109, 2005 

Tropopause chemistry revisited: HO2-initiated oxidation as an efficient acetone sink  I. Hermans, T.L. Nguyen, P.J. Jacobs, J. Peeters  Journal of the American Chemical Society, 126, 2004 

Validation of the BVOC emissions fluxes – Development of a canopy environment model, IUGG meeting, Sapporo, Japan, 30/6-11/7  WALLENS S., J.-F. MÜLLER, A. GUENTHER, , 2003.  Proceedings IUGG meeting, Sapporo, Japan, 30/6-11/7, 2003 

Variation of the atmospheric composition over the 1990-2000 period  GRANIER C., U. NIEMEIR, J.-F. MÜLLER, J. OLIVIER, J. PETERS, A. RICHTER, H. NÜSS, J. BURROWS, POET POET, Report #6, EU project EVK2-1999-00011, 2003 

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