Abstract

Abstract. Methanol exchanges over a mixed temperate forest in the Belgian Ardennes were measured for more than one vegetation season using disjunct eddy-covariance by a mass scanning technique and Proton Transfer Reaction Mass Spectrometry (PTR-MS). Half-hourly methanol fluxes were measured in the range of −0.6 μg m−2 s−1 to 0.6 μg m−2 s−1, and net daily methanol fluxes were generally negative in summer and autumn and positive in spring. On average, the negative fluxes dominated (i.e. the site behaved as a net sink), in contrast to what had been found in previous studies. An original model describing the adsorption/desorption of methanol in water films present in the forest ecosystem and the methanol degradation process was developed. Its calibration, based on field measurements, predicted a mean methanol degradation rate of −0.0074 μg m−2 s−1 and a half lifetime for methanol in water films of 57.4 h. Biogenic emissions dominated the exchange only in spring, with a standard emission factor of 0.76 μg m−2 s−1. The great ability of the model to reproduce the long-term evolution, as well as the diurnal variation of the fluxes, suggests that the adsorption/desorption and degradation processes play an important role in the global methanol budget. This result underlines the need to conduct long-term measurements in order to accurately capture these processes and to better estimate methanol fluxes at the ecosystem scale.

Highlights

  • Methanol is the second most abundant organic gas in the atmosphere after methane (Jacob et al, 2005; Singh et al, 2001)

  • Half-hourly methanol fluxes were measured in the range of −0.6 μg m−2 s−1 to 0.6 μg m−2 s−1, and net daily methanol fluxes were generally negative in summer and autumn and positive in spring

  • We present long-term ecosystem-scale measurements of methanol fluxes exchanged between a heterogeneous temperate forest and the atmosphere, obtained using the disjunct eddy-covariance by mass scanning

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Summary

Introduction

Methanol is the second most abundant organic gas in the atmosphere after methane (Jacob et al, 2005; Singh et al, 2001). Several modelling studies (Galbally and Kirstine, 2002; Heikes et al, 2002; Jacob et al, 2005; Singh et al, 2000; Stavrakou et al, 2011; Tie et al, 2003) have focused on the global methanol budget These studies show that the principal methanol source in the atmosphere is vegetation (60–80 %) and that the major sinks are the reaction with OH in gas-phase (40–70 %) and dry deposition on land (20–30 %). These modelling efforts, remain characterized by huge uncertainties.

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