Aerosol Formation from Natural Compounds Emitted by Vegetation

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• Langue: English
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Environment
Institute
Aerosol Formation from Natural
Compounds Emitted by Vegetation
Contribution to the NUCVOC project by:
Unit of Atmospheric Processes in Global Change
A PHAMA Activity
2000 EUR 19591 EN Aerosol Formation from Natural
Compounds Emitted by Vegetation
EC Joint Research Centre,
Environment Institute
Unit of Atmospheric Processes in Global Change
Contribution to the NUCVOC-Project
A PHAMA Activity
Prepared by
B. R. LARSEN, M. DUANE,
M. GLASIUS, AND D. KOTZIAS LEGAL NOTICE
Neither the European Commission nor any person
acting on behalf of the Commission is responsible for the use which
might be made of the following information.
EUR 19591 EN
© European Communities, 2000
Reproduction is authorised provided the source is acknowledged
Printed in Italy CONTENT
PREFACE 5
EXECUTIVE SUMMARY 9
1. INTRODUCTION TO AEROSOLS AND CLIMATE CHANGE 11
1.1 The global radiation budget 12
1.2. Chemistry of the troposphere5
1.3. Emission of terpenes from vegetation9
1.3. Atmospheric chemistry of terpenes 2
2. CHEMICAL ANALYSIS OF ORGANIC AEROSOL 31
2.1. GC-MS analysis 3
2.2. LC-MS analysis6
2.3. FT-IR ANALYSIS 4
3. REACTION CHAMBER EXPERIMENTS WITH OZONE 49
3.1. Smog chamber setup
3.3. Experimental results 52
3.4. Mechanistic considerations
4. REACTION CHAMBER EXPERIMENTS WITH OH 63
4.1. Smog Chamber setup 6
4.2. Sample collection and analysis5
4.3. Results on reaction products in the gas phase7
4.4. Results on reaction products in the particle phase9
4.6. Mechanistic considerations for compounds with an endocyclic C=C double bond 7
4.7.cs fors with anc C=C double bond 86
4.8. Mechanistic considerations for compounds with endocyclic and exocyclic C=C double bonds .... 92
4.9. Influence of the presence of ΝΟχ 93
4.10. Atmospheric implications4
5. CHAMBER EXPERIMENTS WITH PHOTOCHEMICAL REACTIONS (TERPENE + NOx + hv). 97
6. CONCLUSIONS 101
7. REFERENCESPREFACE
The European Commission Shared Cost Action Project "Nucleation Processes from
Oxidation of Biogenic Volatile Organic Compounds", NUCVOC, ENV CT97-039 has
been carried out during the period January 1998 to July 2000 under the Global Change
Programme, funded with 1025 kEuros. The project consortium was a multidisciplinary
mixture of research centres and universities
Institut für Spektrochemie, Dortmund, (D): T. Hoffmann, Co-ordinator
Max-Planck Institut für Chemie, Mainz, (D): G. Moortgat
Universität/Gesamthochschule Essen, (D): R. Zellner
Univesité Bordeaux I, (F): R. Lesclaux
Centre National de la Recherche Scientifique, Strassbourg, (F): P. Mirabel
AE A Technology, Culham, (UK): M. Jenkin
EC, Joint Research Centre, Ispra (I): B. R. Larsen / D. Kotzias
The goal of the project was to quantitatively evaluate aerosol formation from natural
sources with special emphasis on new particle formation processes and to gain
information about the organic component of tropospheric aerosols. Six specific tasks
were pursued:
(a) Laboratory investigations on the particle formation processes of selected biogenics
(model compounds) for the three relevant tropospheric oxidation pathways (O3, OH,
NO3).
(b) Construction of chemical mechanisms leading to condensable products.
(c) Detailed chemical characterisation of the oxidation products from biogenics,
focusing on the non-volatile fraction.
(d) Synthesis of reference compounds for most important oxidation products.
(e) Evaluation of missing physico-chemical parameters.
(f) Modelling of aerosol formation processes from terpenes.
The JRC, Environment Institute played an active role under a), b), c), and d) focusing
on O3 and in particular OH. This report is a documentation of the fulfilment of the tasks that JRC was responsible
for. The methodology and obtained results are discussed in detail, preceded by a general
introduction to terpenes, aerosols and climate change. A presentation of all results
obtained within the NUCVOC project will be reported elsewhere by the co-ordinator of
the project.
The collaboration by many colleagues at JRC-EI, who at some point have contributed
with skilful technical assistance during the experiments and valuable discussions during
the reporting phase is gratefully acknowledged: A. Calogirou, D. Di Bella, M. Duane,
Y. Fiamegos, M. Glasius, J. Hjorth, N. R. Jensen, D. Kotzias, M. Lahaniati, B. Nicollin,
C. Ottobrini, S. Sørensen, R. Van Dingenen, and R. Winterhalter.
The scientific contribution of JRC-EI in the NUCVOC project has been fruitful. Early in
the project results were obtained, which clearly link emissions of volatile compounds
from vegetation to aerosol formation. The key to this link was the identification of
hereto-unknown compounds with extremely low vapour pressures as reaction products
in aerosol. This pioneer work received great attention from the society of aerosol
scientist at the fifth EUROTRAC Symposium in Garmish-Partenkirchen, 23-27 March,
1998 [1] and has since been further developed in a number of scientific papers
published in international peer-reviewed journals [2-6]. Based on this work M. Glasius
was awarded the Chemistry Gold Medal in the Danish Academic Prize Essay
Competition [7] and graduated as Ph. D. from the Southern Danish University [8].
[1] Carboxylic acids in secondary aerosols from O3 and OH oxidation of cyclic
monoterpenes (1999). Glasius, M., Lahaniati, M., Calogirou, Α., Di Bella, D.,
Jensen, Ν. R, Hjorth J., Duane, M., Kotzias, D., and Larsen, Β. R, Proceedings of
EUROTRAC Symposium 98', Garmisch-Partenkirchen, March 23-27, eds. P.M.
Borrel and P. Borrel, Witpress, Southampton, pp. 273-276.
[2] Gas phase terpene oxidation products: A review (1999). Calogirou, Α., Larsen, Β.
R., and Kotzias, D., Armos. Environ. 33A, 1352-2310.
[3] Atmospheric oxidation products of terpenes: A new nomenclature (1998), Larsen, Β.
R., Lahaniati, M., Calogirou, Α., and Kotzias, D.: Chemosphere 37, 1207-1220. [4] Analysis of polar terpene oxidation products in aerosols by liquid chromatography
ion trap multiple mass spectrometry (1999). Glasius, M., Duane, M., and Larsen,
B. R., : J. Chromatogr. 833, 121-135.
[5] Carboxylic acids in secondary aerosols from oxidation of cyclic monoterpenes by
ozone (2000). Glasius, M., Lahaniati, M., Calogirou, Α., Di Bella, D., Jensen, Ν.
R, Hjorth J., Kotzias, D., and Larsen, B. R.,: Environ. Sci. Technol. 34, 1001-
1010).
[6] Gas-Phase OH oxidation of monoterpenes: Gaseous and particulate products (2000).
Larsen, Β. R., Di Bella, D., Glasius, M., Winterhalter, R., Jensen, N., and Hjorth,
J. J. Atmos. Chem. (in press).
[7] Identification and characterisation of products from reactions between ozone and
terpenes (2000). Glasius, M. Gold Medal Winning Prize Essay from University of
Copenhagen.
[8] The relative contribution of natural and anthropogenic VOC to smog formation
(2000). Glasius, M. Ph. D. Thesis from the Southern Danish University, Denmark.
The main results obtained by JRC-EI in the NUCVOC project are summarised in the
following. For detailed discussions the reader is referred to the published material.
Ispra, Thursday, 15 June 2000
^
Bo R. Larsen
EC Joint Research Centre
Environment Institute, TP290
1-21020, Ispra(VA), Italy
Phone: [phone]
FAX: [phone]
e-mail: [e-mail]