|Reference : Long-term study of biogenic volatile organic compound exchanges in a forest ecosystem|
|Dissertations and theses : Doctoral thesis|
|Physical, chemical, mathematical & earth Sciences : Multidisciplinary, general & others|
|Long-term study of biogenic volatile organic compound exchanges in a forest ecosystem|
|[fr] Etude des échanges à long-terme de composés organi-ques volatils d’origine biogénique par un écosystème forestier|
|Laffineur, Quentin [Université de Liège - ULg > Sciences et technologie de l'environnement > Physique des bio-systèmes >]|
|Université de Liège, Liège, Belgium|
|Docteur en sciences|
|[en] Eddy-covariance ; BVOC ; PTR-MS|
|[en] The terrestrial biosphere, especially forest ecosystems, emits large quantities of volatile organic compounds (VOCs) which have a significant impact on the atmosphere’s chemical and physical characteristics. In particular, VOCs are precursors in the formation of ozone and sec-ondary organic aerosols. Isoprene and monoterpenes dominate the total VOC emissions, and methanol is one of the most abundant atmospheric VOCs due to its longer half-life than the other two.
The main objective of this thesis was to investigate (using the eddy covariance technique and a proton-transfer-reaction mass spectrometer) the mechanisms of VOC (isoprene, monoterpene and methanol) emission and/or deposition at the scale of a temperate climate forest ecosystem (Vielsalm, Belgium) comprising several species (Fagus sylvatica, Abies alba, Picea Abies and Pseudotsuga menziessi).
The eddy covariance technique is very suitable for studying VOC emission/deposition mechanisms at ecosystem level as it does not interfere with the functioning of the ecosystem and it has very good temporal resolution (half an hour). It was used for several months at the Vielsalm site without any major interruption to the measurements.
The first measurement period ran from early July to late November 2009 and the second from late March to late November 2010. As well as measuring the VOC exchanges by eddy covari-ance, the climate parameters controlling the exchange mechanisms were also measured. During both these periods the methanol, acetaldehyde, acetone, isoprene, methyl vinyl ke-tone/methacrolein, monoterpene, acetic acid (2010) and formic acid (2010) fluxes were meas-ured. The highest emission levels observed were isoprene and monoterpenes along with methanol, which unlike the first two also showed depositions. The thesis therefore naturally focused on studying these three fluxes, in view of the important role played by these three compounds in atmospheric chemistry and hence the scientific community’s interest in refining the parametrisation of these compounds’ ecosystem/atmosphere exchange models. The study of the isoprene, monoterpene and methanol fluxes has been written up in three original articles which form the main body of this thesis.
Because of the heterogeneity of the ecosystem studied, the first essential study concerned the identification of VOC-emitting species. This was done with the aid of a flux footprint model combined with a map of the species occurring on the site. This analysis showed that the main monoterpene emitter was Fagus sylvatica followed, to a lesser extent, by Abies alba, Picea Abies and Pseudotsuga menziessi. In contrast to the literature, the analysis showed Abies alba to be a probable isoprene emitter but the presence of Picea Abies, a known isoprene emitter, ruled out absolute certainty on that point.
The isoprene fluxes were observed by day only, unlike the monoterpene fluxes which were observed both day and night. Diurnal flux analysis clearly showed temperature and light to be the two main variables controlling emissions. Combining this analysis with a study of the close relationship between isoprene/monoterpene emissions and photosynthesis revealed the plants’ de novo biosynthetic production mechanisms, an original aspect at ecosystem scale. From the occurrence of nocturnal monoterpene emissions it was possible to determine that de novo monoterpene production emitted directly into the atmosphere (as in the case of isoprene) was not the only source of the emissions observed. Withdrawals from monoterpene sinks located in plant organs or in the soil can also be monoterpene sources. Studying the relationship between isoprene/monoterpene fluxes and light, distinguishing between cloudy and sunny conditions, showed that for the same light intensity the emissions were higher in cloudy con-ditions than in sunshine. Similarly, a study of the relationship between isoprene fluxes and photosynthesis in cloudy/sunny conditions suggested that de novo isoprene production is greater in leaves above the canopy than in leaves within the canopy. Long-term measurement of isoprene and monoterpene emissions enabled seasonal changes in the mechanisms observed to be studied and more fully understood. As well as providing an understanding of the mechanisms, this research also resulted in quantification of the seasonal changes in the key parameters for modelling isoprene/monoterpene emissions.
Methanol exchanges were generally positive (emissions) by day and negative (depositions) at night. Overall, methanol depositions were predominant in summer and autumn but in the mi-nority in spring. On average, the Vielsalm site behaved like a methanol sink, which contradicts all the other research published to date. An original model was developed for identifying the mechanisms responsible for short-term and long-term methanol emissions/depositions. The consistency between the measurements and the model simulations suggested that the main processes controlling methanol exchanges in summer could be attributed, in the short term, to (water-soluble) methanol adsorption/desorption occurring in the films of water on leaf surfaces and/or on the soil surface and, in the long term, to methanol destruction by a biological and/or chemical degradation process also occurring on the surface of leaves and/or the soil. A study of the difference between the measurements and the model, in spring, indicated the possibility of biosynthetic methanol production by the plants. This production was apparently controlled mainly by temperature, but it could not be shown in summer when methanol adsorption/desorption processes dominated.
The literature on ecosystem-atmosphere exchanges of isoprene, monoterpenes and, to a lesser extent, methanol is extensive. Nevertheless, what makes this research original is the spatio-temporal scale used. We are in fact working at ecosystem scale, and not at leaf or branch scale as in most other cases. Moreover, our measurements cover a timescale from half an hour to a full growing season, which is rarely found in the literature. This has resulted in a better under-standing of these compounds’ production and exchange mechanisms. To be precise, the methanol flux study is currently unique in its description and understanding of the deposition mechanisms.
|Gembloux Agro-Bio Tech, Unité de Physique des Bio-systèmes|
|BELSPO, IMPECVOC, F.R.S.-FNRS|
|IMPECVOC: Impact of Phenology and Environmental Conditions on BVOC Emissions from Forest Ecosystems|
|Researchers ; Professionals ; Students|
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